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  • 1.
    Ahmad, Shargeel
    et al.
    Dalian Univ Technol, Inst Artificial Photosynth, State Key Lab Fine Chem, Dalian 116024, Peoples R China..
    Liu, Jinxuan
    Dalian Univ Technol, Inst Artificial Photosynth, State Key Lab Fine Chem, Dalian 116024, Peoples R China..
    Gong, Chenghuan
    Dalian Univ Technol, Inst Artificial Photosynth, State Key Lab Fine Chem, Dalian 116024, Peoples R China..
    Zhao, Jianzhang
    Dalian Univ Technol, Inst Artificial Photosynth, State Key Lab Fine Chem, Dalian 116024, Peoples R China..
    Sun, Licheng
    KTH, School of Chemical Science and Engineering (CHE), Centres, Centre of Molecular Devices, CMD. KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Organic chemistry. Dalian Univ Technol, Inst Artificial Photosynth, State Key Lab Fine Chem, Dalian 116024, Peoples R China..
    Photon Up-Conversion via Epitaxial Surface-Supported Metal-Organic Framework Thin Films with Enhanced Photocurrent2018In: ACS Applied Energy Materials, E-ISSN 2574-0962, Vol. 1, no 2, p. 249-253Article in journal (Refereed)
    Abstract [en]

    We report a new triplet-triplet annihilation photon up-conversion (TTA-UC) system using an epitaxial Zn-perylene surface-supported metal-organic framework (SURMOF) grown on metal oxide surface as "emitter", and a platinum octaethylporphyrin (PtOEP) as "sensitizer" in [Co(bpy)(3)](2+/3+) acetonitrile solution. It has been demonstrated that the photocurrent can be significantly enhanced relative to epitaxial Zn-perylene SURMOF due to the TTA-UC mechanism. This initial result holds promising applications toward SURMOF-based solar energy conversion devices.

  • 2. An, J.
    et al.
    Tian, Z.
    Zhang, L.
    Yang, X.
    Cai, B.
    Yu, Z.
    Hagfeldt, A.
    Sun, Licheng
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Organic chemistry. State Key Laboratory of Fine Chemicals, Institute of Artificial Photosynthesis, DUT-KTH Joint Education and Research Center on Molecular Devices, Dalian University of Technology (DUT), Dalian 116024, China.
    Supramolecular Co-adsorption on TiO2to enhance the efficiency of dye-sensitized solar cells2021In: Journal of Materials Chemistry A, ISSN 2050-7488, E-ISSN 2050-7496, Vol. 9, no 23, p. 13697-13703Article in journal (Refereed)
    Abstract [en]

    Three novel push-pull dyes, with carbazole donors, codedAJ502,TZ101andTZ102are synthesized and applied as co-sensitizers in dye-sensitized solar cells (DSSCs).TZ101andTZ102have similar structures except for two fluorine atoms introduced on the benzotriazole (BTZ) unit.AJ502shows a near-IR absorption spectrum that is suitable for co-sensitization withTZ101andTZ102. The co-sensitized DSSC device based onCO-1(AJ502 : TZ101= 3 : 4 (0.075 mM : 0.1 mM)) achieves a power conversion efficiency (PCE) of 10.3% under AM 1.5G irradiation, with 1.06 V open-circuit voltage (Voc), 13.75 mA cm−2short-circuit photocurrent density (Jsc), and 70.8% fill factor (FF), a significant improvement compared to the single dye, 6.0% forAJ502and 5.1% forTZ101with a copper(i/ii)-based redox electrolyte. A PCE of 8.9% is also obtained by devices based onCO-2(AJ502 : TZ102= 3 : 4). ForCO-1, the fluorine atoms inTZ101play a critical role by widening the active light capturing bands of bothTZ101andAJ502on the TiO2film whileTZ102andAJ502show weaker interaction under the same conditions. The UV-vis spectrum and Raman spectrum revealed thatAJ502can form supramolecules withTZ101andTZ102formed on the TiO2film. 

  • 3.
    An, Jincheng
    et al.
    State Key Laboratory of Fine Chemicals, Institute of Artificial Photosynthesis, DUT−KTH Joint Education and Research Center on Molecular Devices, Dalian University of Technology (DUT), Dalian 116024, China.
    Yang, Xichuan
    State Key Laboratory of Fine Chemicals, Institute of Artificial Photosynthesis, DUT−KTH Joint Education and Research Center on Molecular Devices, Dalian University of Technology (DUT), Dalian 116024, China.
    Cai, Bin
    State Key Laboratory of Fine Chemicals, Institute of Artificial Photosynthesis, DUT−KTH Joint Education and Research Center on Molecular Devices, Dalian University of Technology (DUT), Dalian 116024, China.
    Zhang, Li
    State Key Laboratory of Fine Chemicals, Institute of Artificial Photosynthesis, DUT−KTH Joint Education and Research Center on Molecular Devices, Dalian University of Technology (DUT), Dalian 116024, China.
    Yang, Kaiyuan
    State Key Laboratory of Fine Chemicals, Institute of Artificial Photosynthesis, DUT−KTH Joint Education and Research Center on Molecular Devices, Dalian University of Technology (DUT), Dalian 116024, China.
    Yu, Ze
    State Key Laboratory of Fine Chemicals, Institute of Artificial Photosynthesis, DUT−KTH Joint Education and Research Center on Molecular Devices, Dalian University of Technology (DUT), Dalian 116024, China.
    Wang, Xiuna
    State Key Laboratory of Fine Chemicals, Institute of Artificial Photosynthesis, DUT−KTH Joint Education and Research Center on Molecular Devices, Dalian University of Technology (DUT), Dalian 116024, China.
    Hagfeldt, Anders
    Laboratory of Photomolecular Science, Institute of Chemical Sciences and Engineering, École Polytechnique Fédérale de Lausanne, Lausanne CH-1015, Switzerland.
    Sun, Licheng
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Organic chemistry. State Key Laboratory of Fine Chemicals, Institute of Artificial Photosynthesis, DUT−KTH Joint Education and Research Center on Molecular Devices, Dalian University of Technology (DUT), Dalian 116024, China.
    Fine-Tuning by Triple Bond of Carbazole Derivative Dyes to Obtain High Efficiency for Dye-Sensitized Solar Cells with Copper Electrolyte2020In: ACS Applied Materials and Interfaces, ISSN 1944-8244, E-ISSN 1944-8252, Vol. 12, no 41, p. 46397-46405Article in journal (Refereed)
    Abstract [en]

    Three novel dyes consisting of a 5,8,15-tris(2-ethylhexyl)-8,15-dihydro-5H-benzo[1,2-b:3,4-b':6,5-b″]tricarbazole (BTC) electron-donating group and a 4,7-bis(4-hexylthiophen-2-yl)benzo[c][1,2,5]thiadiazole (BTBT) π-bridge with an anchoring group of phenyl carboxyl acid were synthesized and applied in dye-sensitized solar cells (DSCs).The AJ202 did not contain any triple bonds, the AJ201's ethynyl group was inserted between the BTC and BTBT units, and the AJ206's ethynyl group was introduced between the BTBT moiety and the anchor group. The inclusion and position of the ethynyl linkage in the sensitizer molecules significantly altered the electrochemical properties of these dyes, which can fine-tune the energy levels of the dyes. The best performing devices contained AJ206 as a sensitizer and a Cu(I/II) redox couple, which resulted in a power conversion efficiency (PCE) up to 10.8% under the standard AM 1.5 G illumination, which obtained PCEs higher than those from the devices that contained AJ201 (9.2%) and AJ202 (9.7%) under the same conditions. The highest occupied molecular orbital and lowest unoccupied molecular orbital levels of the sensitizers were tuned to be well-suited for the Cu(I/II) redox potential and the Fermi level of TiO2. The innovative synthesis of a tricarbazole-based donor moiety in a sensitizer used in combination with a Cu(I/II) redox couple has resulted in relatively high PCEs.

  • 4.
    An, Jincheng
    et al.
    Dalian Univ Technol DUT, DUT KTH Joint Educ & Res Ctr Mol Devices, Inst Artificial Photosynth, State Key Lab Fine Chem, Dalian 116024, Peoples R China..
    Yang, Xichuan
    Dalian Univ Technol DUT, DUT KTH Joint Educ & Res Ctr Mol Devices, Inst Artificial Photosynth, State Key Lab Fine Chem, Dalian 116024, Peoples R China..
    Tian, Zhifeng
    Dalian Univ Technol DUT, DUT KTH Joint Educ & Res Ctr Mol Devices, Inst Artificial Photosynth, State Key Lab Fine Chem, Dalian 116024, Peoples R China..
    Cai, Bin
    Dalian Univ Technol DUT, DUT KTH Joint Educ & Res Ctr Mol Devices, Inst Artificial Photosynth, State Key Lab Fine Chem, Dalian 116024, Peoples R China..
    Zhang, Li
    Dalian Univ Technol DUT, DUT KTH Joint Educ & Res Ctr Mol Devices, Inst Artificial Photosynth, State Key Lab Fine Chem, Dalian 116024, Peoples R China..
    Yu, Ze
    Dalian Univ Technol DUT, DUT KTH Joint Educ & Res Ctr Mol Devices, Inst Artificial Photosynth, State Key Lab Fine Chem, Dalian 116024, Peoples R China..
    Wang, Xiuna
    Dalian Univ Technol DUT, DUT KTH Joint Educ & Res Ctr Mol Devices, Inst Artificial Photosynth, State Key Lab Fine Chem, Dalian 116024, Peoples R China..
    Hagfeldt, Anders
    Ecole Polytech Fed Lausanne, Lab Photomol Sci, Inst Chem Sci & Engn, CH-1015 Lausanne, Switzerland..
    Sun, Licheng
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Organic chemistry. Dalian Univ Technol DUT, DUT KTH Joint Educ & Res Ctr Mol Devices, Inst Artificial Photosynth, State Key Lab Fine Chem, Dalian 116024, Peoples R China..
    Thiophene-fused carbazole derivative dyes for high-performance dye-sensitized solar cells2021In: Tetrahedron, ISSN 0040-4020, E-ISSN 1464-5416, Vol. 88, article id 132124Article in journal (Refereed)
    Abstract [en]

    Two novel dyes that are similar in chemical structure, except for different donor units, AJ301and AJ303 were synthesized, characterized and applied as sensitizers in dye-sensitized solar cells (DSSCs). Both dyes exhibited a wide absorption of visible sunlight. The introduction of fused rings on the donor unit of AJ303 presented an appropriate energy level, less recombination and longer electron lifetime to achieve a power conversion efficiency (PCE) of 10.2%, far above that achieved for AJ301 of 6.2% with a [Co(bpy)(3)](2+/3+)-based electrolyte under standard AM1.5G solar irradiation (100 mW cm(-2)). The DSSCs based on AJ303 and AJ301 with [Cu(tmby)(2)](2+/+)-based electrolyte showed a lower PCE of 8.2% and 5.4%, respectively. Therefore, the results indicated that the introduction of a fused-ring in the donor group is a meaningful synthetic strategy to improve the photovoltaic performance.

  • 5.
    Ananikov, Valentine
    et al.
    Zelinsky Institute of Organic Chemistry, Russian Academy of Sciences, Leninsky Prospect, 47, Moscow 119991, Russia.
    Gevorgyan, Vladimir
    Department of Chemistry and Biochemistry, The University of Texas at Dallas, Richardson, Texas 75080-3021, United States.
    Moberg, Christina
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Organic chemistry.
    Suginome, Michinori
    Department of Synthetic Chemistry and Biological Chemistry, Graduate School of Engineering, Kyoto University, Katsura, Nishikyo-ku, Kyoto 615-8510, Japan.
    Trzeciak, Anna
    Faculty of Chemistry, University of Wrocław, 14 F. Joliot-Curie St., 50-383 Wrocław, Poland.
    Irina Beletskaya: Chemistry Excellence in Scientific Endeavors2023In: Organometallics, ISSN 0276-7333, E-ISSN 1520-6041, Vol. 42, no 18, p. 2415-2425Article in journal (Other academic)
  • 6.
    Avetyan, David L.
    et al.
    Tomsk Polytech Univ, Lenin Ave 30, Tomsk 634050, Russia..
    Shatskiy, Andrey
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Organic chemistry.
    Kärkäs, Markus D.
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Organic chemistry.
    Stepanova, Elena, V
    Tomsk Polytech Univ, Lenin Ave 30, Tomsk 634050, Russia..
    Scalable total synthesis of natural vanillin-derived glucoside omega-esters2022In: Carbohydrate Research, ISSN 0008-6215, E-ISSN 1873-426X, Vol. 522, p. 108683-, article id 108683Article in journal (Refereed)
    Abstract [en]

    The first total synthesis of vanilloloside, calleryanin, and a series of naturally occurring omega-esters of vanilloloside was realized through direct glycosylation of vanillin-based aglycones or late-stage derivatization of vanilloloside. All aglycones and their fragments were synthesized from vanillin as the sole aromatic precursor. Subsequently, these intermediates were used to construct various vanillin-derived glucoside omega-esters using a mild acidic deacetylation as the key synthetic step, providing the final products in the total yields of 10-50% and general purity of >95%. Additionally, the first operationally simple and sustainable synthesis of litseafoloside B was realized on large scale, avoiding the use of toxic solvents and reagents, providing an attractive alternative to isolation of this and other similar compounds from plant sources.

  • 7.
    Axelsson, Karolin
    et al.
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Organic chemistry.
    Zendegi-Shiraz, Amene
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH). Ferdowsi Univ Mashhad, Dept Chem, Fac Sci, Mashhad, Razavi Khorasan, Iran..
    Swedjemark, Gunilla
    Skogforsk, Ekebo, Svalov, Sweden..
    Borg-Karlson, Anna-Karin
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Organic chemistry. Mid Sweden Univ, Dept Chem Engn, Sundsvall, Sweden..
    Zhao, Tao
    Örebro Univ, Sch Sci & Technol, SE-70182 Örebro, Sweden..
    Chemical defence responses of Norway spruce to two fungal pathogens2020In: Forest Pathology, ISSN 1437-4781, E-ISSN 1439-0329, Vol. 50, no 6, article id e12640Article in journal (Refereed)
    Abstract [en]

    Constitutive and inducible terpene production is involved in conifer resistance against insects and fungal infestations. To gain knowledge about local defence responses of Norway spruce bark against pathogens and to find potential chemical markers for resistance breeding, we inoculated the stem of 8-year-old Norway spruce (Picea abies) clonal trees with bothEndoconidiophora polonica(Ep, a common fungal pathogen associated with the spruce bark beetleIps typographus) andHeterobasidion parviporum(Hp, a severe pathogen causing root and stem rot disease). Three weeks after inoculation, the fungal-inoculated and intact bark from each tree was sampled. The terpenes in tree bark were extracted with hexane and characterized by gas chromatography-mass spectrometry (GC-MS). The two fungi induced varied terpene responses in the four spruce clones used. Three of the clones showed a 2.3-fold to 5.7-fold stronger terpene response to Hp relative to Ep inoculation, while one clone responded similarly to inoculation with the two fungal pathogens. The amount of the diterpenes thunbergol and geranyllinalool varied between the clones. The level of thunbergol was higher in both intact and fungal-inoculated bark from the less susceptible clones compared with the more susceptible clones. Geranyllinalool was present in higher amounts in the susceptible clones and is thus a possible marker for susceptibility. Our observations show that Norway spruce employs a similar chemical mechanism against the two fungal pathogens. Based on the present and earlier published data, we suggest that certain Norway spruce genotypes have a strong defence reaction against these two pathogens. The diterpenes thunbergol and geranyllinalool might be useful markers of susceptibility in tree-breeding programmes and should be the focus of further detailed investigations.

  • 8.
    Azeem, Muhammad
    et al.
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry. Department of Chemistry, COMSATS University Islamabad, Abbottabad Campus, Abbottabad 22060, Pakistan.
    Barba Aliaga, Marina
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Industrial Biotechnology.
    Borg-Karlson, Anna-Karin
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Organic chemistry. Division of Organic Chemistry, Institute of Technology, Tartu University, Tartu 50411, Estonia.
    Terenius, O.
    Broberg, A.
    Rajarao, Gunaratna Kuttuva
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Industrial Biotechnology.
    Heterobasidion-growth inhibiting Bacillus subtilis A18 exhibits medium- and age-dependent production of lipopeptides2019In: Microbiological Research, ISSN 0944-5013, E-ISSN 1618-0623, Vol. 223-225, p. 129-136Article in journal (Refereed)
    Abstract [en]

    Heterobasidion annosum s.s. and H. parviporum are severe pathogens of conifers causing butt rot and root rot thus reducing the economic value of timber. Here, the antifungal activity of Bacillus subtilis isolate A18 against these two Heterobasidion species was investigated. Five different culture media with different culture age were investigated to study the effect of substrate composition and culture age for metabolite production. Bacterial cultures and cell-free culture filtrates were tested for antifungal activity. Inhibition of fungal growth was analysed using the agar disc-diffusion method. MALDI-TOF and LC-HRMS analyses were used to identify the antifungal metabolites. Substrate composition and age of culture were found to be active variables with direct effect on the antifungal activity of bacterial culture extracts. High anti-fungal activity was observed when B. subtilis was cultured in PDB, SGB and LB media for four days. Mass-spectrometry analysis showed the presence of lipopeptides in culture filtrates identified as members of the surfactins, polymixins, kurstakins and fengycins. A culture filtrate containing fengycin-type lipopeptides showed the highest bioactivity against Heterobasidion species. Bacterial cultures had higher bioactivity compared to their respective cell free culture filtrates. The results of the present study suggest that B. subtilis A18 is a powerful biocontrol agent against Heterobasidion infections of tree wounds and stumps.

  • 9.
    Azeem, Muhammad
    et al.
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry.
    Iqbal, Z.
    Emami, S. N.
    Nordlander, G.
    Nordenhem, H.
    Mozūratis, R.
    El-Seedi, Hesham
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry.
    Borg-Karlson, Anna-Karin
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Organic chemistry.
    Chemical composition and antifeedant activity of some aromatic plants against pine weevil (Hylobius abietis)2020In: Annals of Applied Biology, ISSN 0003-4746, E-ISSN 1744-7348Article in journal (Refereed)
    Abstract [en]

    The pine weevil Hylobius abietis is an important pest causing severe damage to conifer seedlings in reforestation areas in Europe and Asia. Plants that have no evolutionary history with the pine weevil are of special interest in the search for compounds with a strong antifeedant activity. Thus, the essential oils of nine aromatic plants, viz Amomum subulatum, Cinnamomum tamala, Curcuma longa, Laurus nobilis, Ocimum basilicum, Origanum majorana, Origanum vulgare, Syzygium aromaticum and Trachyspermum ammi were extracted by hydrodistillation. The essential oil constituents were identified by gas chromatography–mass spectrometry, and antifeedant properties towards the pine weevil were assessed using choice feeding bioassay. The essential oils of C. longa, O. majorana, S. aromaticum and T. ammi showed an excellent antifeedant activity towards the pine weevil for 24 hr, whereas the essential oil of other plants showed the activity for 6 hr. There was a positive correlation between the amount of benzenoid compounds and the antifeedant activity of the essential oils. This study suggests that pine weevil non-host plant compounds have potential to be used for the protection of seedlings against pine weevil feeding. However, further study will be needed to explore the antifeedant activity of individual components and oils in the laboratory as well as in the field. 

  • 10.
    Baroffio, C. A.
    et al.
    Agroscope, Rte Eterpys 18, CH-1964 Conthey, Switzerland..
    Sigsgaard, L.
    Univ Copenhagen, Dept Plant & Environm Sci, Thorvaldsensvej 40, DK-1871 Frederiksberg C, Denmark..
    Ahrenfeldt, E. J.
    Univ Copenhagen, Dept Plant & Environm Sci, Thorvaldsensvej 40, DK-1871 Frederiksberg C, Denmark..
    Borg-Karlson, Anna-Karin
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Organic chemistry.
    Bruun, S. A.
    NIBIO Norwegian Inst Bloecon Res, NO-1431 As, Norway.;NMBU Norwegian Univ Life Sci, Fac Environm Sci & Nat Resource Management, NO-1432 As, Norway..
    Cross, J. V.
    NIAB EMR, New Rd, Kent ME19 6BJ, England..
    Fountain, M. T.
    NIAB EMR, New Rd, Kent ME19 6BJ, England..
    Hall, D.
    Univ Greenwich, Nat Resources Inst, Cent Ave, Chatham ME4 4TB, Kent, England..
    Mozuraitis, R.
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry.
    Ralle, B.
    LPPRC Latvian Plant Protect Res Ctr, Struktoru Lela 14 A, LV-1039 Riga, Latvia..
    Trandem, N.
    NIBIO Norwegian Inst Bloecon Res, NO-1431 As, Norway.;NMBU Norwegian Univ Life Sci, Fac Environm Sci & Nat Resource Management, NO-1432 As, Norway..
    Wibe, A.
    NORSOK Norwegian Ctr Organ Agr, Gunnars Vei 6, NO-6630 Tingvoll, Norway..
    Combining plant volatiles and pheromones to catch two insect pests in the same trap: Examples from two berry crops2018In: Crop Protection, ISSN 0261-2194, E-ISSN 1873-6904, Vol. 109, p. 1-8Article in journal (Refereed)
    Abstract [en]

    Most horticultural crops are attacked by more than one insect pest. As broad-spectrum chemical control options are becoming increasingly restricted, there is a need to develop novel control methods. Semiochemical attractants are available for three important horticultural pests, strawberry blossom weevil, Anthonomus rubi Herbst (Coleoptera: Curculionidae), European tarnished plant bug, Lygus rugulipennis Poppius (Hemiptera: Miridae) and raspberry beetle, Byturus tomentostts deGeer (Coleoptera: Byturidae). Traps targeting more than one pest species would be more practical and economical for both monitoring and mass trapping than traps for single-species. In this study we aimed to (1) improve the effectiveness of existing traps for insect pests in strawberry and raspberry crops by increasing catches of each species, and (2) test if attractants for two unrelated pest species could be combined to capture both in the same trap without decreasing the total catches. Field tests were carried out in four European countries and different combinations of semiochemicals were compared. A volatile from strawberry flowers, 1,4 dimethoxybenzene (DMB), increased the attractiveness of the aggregation pheromone to both sexes of A. rubi. The host-plant volatile, phenylacetaldehyde (PAA), increased the attraction of female L. rugulipennis to the sex pheromone, and, in strawberry, there was some evidence that adding DMB increased catches further. Traps baited with the aggregation pheromone of A. rubi, DMB, the sex pheromone of L rugulipennis and PAA attracted both target species to the same trap with no significant difference in catches compared to those single-species traps. In raspberry, catches in traps baited with a combination of A. rubi aggregation pheromone, DMB and the commercially available lure for B. tomentosus, based on raspberry flower volatiles, were similar to those in single-species traps. In both crops the efficiency of the traps still needs improvement, but the multi species traps are adequate for monitoring and should not lead to confusion for the user as the target species are easy to distinguish from each other.

  • 11.
    Beeren, Sophie R.
    et al.
    Tech Univ Denmark, Dept Chem, Kemitorvet Bldg 207, DK-2800 Lyngby, Denmark..
    McTernan, Charlie T.
    Francis Crick Inst, Artificial Mol Machinery Lab, 1 Midland Rd, London NW1 1AT, England.;Kings Coll London, Dept Chem, Britannia House,7 Trinity St, London SE1 1DB, England..
    Schaufelberger, Fredrik
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Organic chemistry.
    The mechanical bond in biological systems2023In: Chem, ISSN 2451-9308, E-ISSN 2451-9294, Vol. 9, no 6, p. 1378-1412Article, review/survey (Refereed)
    Abstract [en]

    The field of mechanically interlocked molecules (MIMs) has advanced rapidly in recent years, with much work focused on their use in materials, sensing, and catalysis. However, the use of MIMs in biology and biomedicine has been limited, despite the identifica-tion of naturally occurring MIMs in DNA and proteins and the poten-tial advantages of the mechanical bond in fields such as nanomedi-cine and tissue engineering. Difficulties in the synthesis of MIMs, along with their limited solubility and stability in biological media, have until recently impeded their wider application in biology. Contemporary advances have, however, enabled a broader integra-tion of the mechanical bond in biology; the mechanical interlocking endows these systems with unique functional advantages. Herein, we summarize recent advances in the application of small-molecule, biologically derived, and polymeric MIMs in biology, highlighting synergies ripe for future exploration.

  • 12.
    Blomkvist, Björn
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Organic chemistry.
    Green Chemistry in Chemical Education and Synthetic Applications of Sulfinamides2020Doctoral thesis, comprehensive summary (Other academic)
    Abstract [en]

    The preparation of chiral molecules, i.e. compounds that are not identical to their mirror image, is of great interest in the field of organic chemistry. The preparation of a enantiomerically pure molecules is crucial in the development of new pharmaceuticals, agrochemicals and more, since the building blocks of life are chiral and the interactions between enantiomers and receptor are different. Furthermore, an important aspect of chemistry is sustainability, developing new synthetic procedures where green chemistry has been incorporated.

    In chapter 2, the use of Brønsted acid catalysis as well as a combined Brønsted acid and aminocatalytic procedure for the preparation of the chiral synthon tert-butane N-sulfinyl imine. Using HBF4•DEE as a catalyst gave the sulfinylimine in high yields in 2 h. Changing the catalyst to HBF4•DEE and aniline both improved the yields and shortened the reaction time to only 30 min. Furthermore, DFT-calculations were performed for both catalytic systems, providing a proposed mechanism suggesting a six-membered cyclic transition state as the key transition state.

    In chapter 3 a light-assisted method for the preparation of chiral unnatural amino acids is presented. Via a photoredox-catalyzed decarboxylation of carboxylic acids, a carbon radical is generated that adds stereoselectively to an N-sulfinyl imine. This method allows for green synthesis of non-natural amino acids, and compared to previous methods, we have extended the radical source to include carboxylic acids.

    In chapter 4, the use of green chemistry in B.Sc. level teaching is explored through an experimental design project for third-year students, using green chemistry as basis for analysis of literature procedures. Following this, the procedure is implemented in a first-year B.Sc. course. This is proven to be an efficient way to increase the students understanding of organic chemistry, as well as an efficient way to teach green chemistry.

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  • 13.
    Blomkvist, Björn
    et al.
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Organic chemistry.
    Dinér, Peter
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Organic chemistry.
    Mild and Rapid Aniline/HBF4 center dot DEE-Catalysed Formation of Sulfinyl Imines2019In: ChemistrySelect, ISSN 2365-6549, Vol. 4, no 25, p. 7431-7436Article in journal (Refereed)
    Abstract [en]

    The combination of anline and tetrafluoroboric acid diethyl etherate (2.5 mol% and 5 mol%, respectively) significantly accelerates the formation of sulfinyl imines in dichloromethane and isopropylacetate at room temperature compared to previous procedures. A DFT and NMR spectroscopic study shows that the anilinium tetrafluoroborate complex is solvated by sulfinamide molecules in the initial state and that the rate-limiting step of the reaction is the addition of the sulfinamide molecule to the protonated aniline-based imine. In addition, the catalytic system was also utilised in a one-pot, two step reaction, where the in situ formed sulfinyl imine was arylated in a rhodium catalysed reaction with high diastereoselectivity.

  • 14.
    Cai, Bin
    et al.
    DUT, DUT KTH Joint Educ & Res Ctr Mol Devices, Inst Artificial Photosynth, State Key Lab Fine Chem, Dalian 116024, Peoples R China..
    Yang, Xichuan
    DUT, DUT KTH Joint Educ & Res Ctr Mol Devices, Inst Artificial Photosynth, State Key Lab Fine Chem, Dalian 116024, Peoples R China..
    Jiang, Xiaoqing
    DUT, DUT KTH Joint Educ & Res Ctr Mol Devices, Inst Artificial Photosynth, State Key Lab Fine Chem, Dalian 116024, Peoples R China..
    Yu, Ze
    DUT, DUT KTH Joint Educ & Res Ctr Mol Devices, Inst Artificial Photosynth, State Key Lab Fine Chem, Dalian 116024, Peoples R China..
    Hagfeldt, Anders
    Ecole Polytech Fed Lausanne, Inst Chem Sci & Engn, Lab Photomol Sci, CH-1015 Lausanne, Switzerland..
    Sun, Licheng
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Organic chemistry.
    Boosting the power conversion efficiency of perovskite solar cells to 17.7% with an indolo[3,2-b]carbazole dopant-free hole transporting material by improving its spatial configuration2019In: Journal of Materials Chemistry A, ISSN 2050-7488, Vol. 7, no 24, p. 14835-14841Article in journal (Refereed)
    Abstract [en]

    The development of facilely synthesized, dopant-free hole-transporting materials (HTMs) with high efficiency is of great significance for the potential application of perovskite solar cells (PSCs). Herein, we report two novel indolo[3,2-b]carbazole (ICZ) based small molecules obtained via a three-step reaction in a high yield without using expensive catalysts, namely C201 and C202, and further apply them as dopant-free HTMs in PSCs. Compared with C201, C202 contains two additional biphenylamino groups to improve its spatial configuration. It is found that the interplay between the molecular geometry and the aggregation behavior can exert a great influence on the film formation property and thus on the device performance. Strikingly, the champion devices employing C202 as the HTM deliver a much higher PCE of up to 17.7%, which is substantially higher than that of devices containing C201 (8.7%) under 100 mW cm(-2) illumination (AM 1.5G). It is revealed that the C202 capping layer exhibits a more homogeneous and uniform surface morphology as compared to that of C201, which effectively reduces the charge recombination losses and facilitates charge extraction, leading to a much-enhanced photovoltaic performance. This is the first example of ICZ core-based small molecules as dopant-free HTMs in PSCs. Moreover, the PSCs containing C202 as the HTM also exhibited good long-term stability under ambient conditions (40% RH) as compared to devices with doped spiro-OMeTAD, due largely to the hydrophobic nature of C202 which prevented moisture from destroying the perovskite film. This work offers a new avenue for developing cost-effective and stable HTMs for PSCs and other optoelectronic devices.

  • 15. Cao, S.
    et al.
    Wu, Y.
    Hou, J.
    Zhang, B.
    Li, Z.
    Nie, X.
    Sun, Licheng
    KTH, School of Chemical Science and Engineering (CHE), Centres, Centre of Molecular Devices, CMD. KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Organic chemistry.
    3D Porous Pyramid Heterostructure Array Realizing Efficient Photo-Electrochemical Performance2019In: Advanced Energy Materials, ISSN 1614-6832, E-ISSN 1614-6840, article id 1902935Article in journal (Refereed)
    Abstract [en]

    Direct photo-electrochemical (PEC) water splitting is of great practical interest for developing a sustainable energy systems, but remains a big challenge owing to sluggish charge separation, low efficiency, and poor stability. Herein, a 3D porous In2O3/In2S3 pyramid heterostructure array on a fluorine-doped tin oxide substrate is fabricated by an ion exchange–induced synthesis strategy. Based on the synergistic structural and electronic modulations from density functional theory calculations and experimental observations, 3D porous In2O3/In2S3 photoanode by the protective layer delivers a low onset potential of ≈0.02 V versus reversible hydrogen electrode (RHE), the highest photocurrent density of 8.2 mA cm−2 at 1.23 V versus RHE among all the In2S3 photoanodes reported to date, an incident photon-to-current efficiency of 76% at 400 nm, and high stability over 20 h for PEC water splitting are reported. This work provides an alternative promising prototype for the design and construction of novel heterostructures in robust PEC water splitting applications.

  • 16.
    Chang, Qingyan
    et al.
    State Key Laboratory of Fine Chemicals, Dalian University of Technology (DUT), Dalian 116024, Liaoning, China, Liaoning.
    An, Yidan
    Department of Materials Science and Engineering, City University of Hong Kong, Kowloon 999077, Hong Kong, China.
    Cao, Huaiman
    State Key Laboratory of Fine Chemicals, Dalian University of Technology (DUT), Dalian 116024, Liaoning, China, Liaoning.
    Pan, Yuzhen
    School of Chemical and Engineering, Dalian University of Technology (DUT), Dalian 116024, Liaoning, China, Liaoning.
    Zhao, Liangyu
    State Key Laboratory of Fine Chemicals, Dalian University of Technology (DUT), Dalian 116024, Liaoning, China, Liaoning.
    Chen, Yulong
    State Key Laboratory of Fine Chemicals, Dalian University of Technology (DUT), Dalian 116024, Liaoning, China, Liaoning.
    We, Yi
    Key Laboratory of Materials Modification by Laser, Ion, and Electron Beams (Ministry of Education), Dalian University of Technology (DUT), Dalian 116024 Liaoning, China, Liaoning.
    Tsang, Sai Wing
    Department of Materials Science and Engineering, City University of Hong Kong, Kowloon 999077, Hong Kong, China.
    Yip, Hin Lap
    Department of Materials Science and Engineering, City University of Hong Kong, Kowloon 999077, Hong Kong, China; School of Energy and Environment, City University of Hong Kong, Kowloon 999077, Hong Kong, China.
    Sun, Licheng
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Organic chemistry. State Key Laboratory of Fine Chemicals, Dalian University of Technology (DUT), Dalian 116024, Liaoning, China, Liaoning; Center of Artificial Photosynthesis for Solar Fuels and Department of Chemistry, School of Science, Westlake University, Hangzhou 310024, Zhejiang, China, Zhejiang.
    Yu, Ze
    State Key Laboratory of Fine Chemicals, Dalian University of Technology (DUT), Dalian 116024, Liaoning, China, Liaoning.
    Precursor engineering enables high-performance all-inorganic CsPbIBr2 perovskite solar cells with a record efficiency approaching 13%2024In: Journal of Energy Chemistry, ISSN 2095-4956, E-ISSN 2096-885X, Vol. 90, p. 16-22Article in journal (Refereed)
    Abstract [en]

    All-inorganic CsPbIBr2 perovskite has attracted widespread attention in photovoltaic and other optoelectronic devices because of its superior thermal stability. However, the deposition of high-quality solution-processed CsPbIBr2 perovskite films with large thicknesses remains challenging. Here, we develop a triple-component precursor (TCP) by employing lead bromide, lead iodide, and cesium bromide, to replace the most commonly used double-component precursor (DCP) consisting of lead bromide and cesium iodide. Remarkably, the TCP system significantly increases the solution concentration to 1.3 M, leading to a larger film thickness (∼390 nm) and enhanced light absorption. The resultant CsPbIBr2 films were evaluated in planar n-i-p structured solar cells, which exhibit a considerably higher optimal photocurrent density of 11.50 mA cm−2 in comparison to that of DCP-based devices (10.69 mA cm−2). By adopting an organic surface passivator, the maximum device efficiency using TCP is further boosted to a record efficiency of 12.8% for CsPbIBr2 perovskite solar cells.

  • 17. Chen, C.
    et al.
    Zhang, P.
    Wang, M.
    Zheng, D.
    Chen, J.
    Li, F.
    Wu, X.
    Fan, K.
    Sun, Licheng
    KTH, School of Chemical Science and Engineering (CHE), Centres, Centre of Molecular Devices, CMD. KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Organic chemistry.
    Boosting Electrocatalytic Water Oxidation by Creating Defects and Lattice-Oxygen Active Sites on Ni-Fe Nanosheets2020In: ChemSusChem, ISSN 1864-5631, E-ISSN 1864-564X, Vol. 13, no 18, p. 5067-5072Article in journal (Refereed)
    Abstract [en]

    Layered nickel-iron oxide/hydroxide nanosheets have proven to be the most efficient catalyst for the water oxidation reaction. Introducing structural defects to the nanosheets is a particularly attractive method for increasing the number of active sites and tailoring the intrinsic electronic properties. Herein, defects were introduced on Ni−Fe nanosheets through sequentially electrodoping and dedoping the surface of the material with tetramethylammonium ions. The as-prepared defect-rich Ni−Fe nanosheets showed an enhanced catalytic performance for the oxygen evolution reaction (OER) compared with conventional NiFe layered double hydroxides (LDHs), exhibiting an overpotential of only 172 mV at the current density of 10 mA cm−2. The relationship between pH and OER activity indicated that the lattice oxygens participated in the catalytic OER process as active sites. This work provides new insights into the understanding of the structure-activity relationship of layered materials and helps to develop new methods to implement defects on such frameworks aided by organic molecules.

  • 18. Chen, X.
    et al.
    Shatskiy, Andrey
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Organic chemistry.
    Liu, Jianquan
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry.
    Kärkäs, Markus D.
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Organic chemistry.
    Wang, X. -S
    Synthesis of Sulfonylated Heterocycles via Copper-Catalyzed Heteroaromatization/Sulfonyl Transfer of Propargylic Alcohols2021In: Chemistry - An Asian Journal, ISSN 1861-4728, E-ISSN 1861-471X, Vol. 16, no 1, p. 30-33Article in journal (Refereed)
    Abstract [en]

    An unprecedented copper-catalyzed heteroaromatization/sulfonyl transfer of propargylic alcohols with isocyanide has been developed. 3-Sulfonyl benzofurans and indoles were produced under Cu(I) catalysis in good to high yields. The developed catalytic methodology provides controlled, modular, and facile access to sulfonyl benzoheterocycle scaffolds.

  • 19. Chen, Y.
    et al.
    Wu, Y.
    Shatskiy, Andrey
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Organic chemistry.
    Kan, Y.
    Kärkäs, Markus D.
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Organic chemistry.
    Liu, J. -Q
    Wang, X. -S
    Cooperative Silver- and Base-Catalyzed Diastereoselective Cycloaddition of Nitrones with Methylene Isocyanides: Access to 2-Imidazolinones2020In: European Journal of Organic Chemistry, ISSN 1434-193X, E-ISSN 1099-0690Article in journal (Refereed)
    Abstract [en]

    A protocol involving cooperative silver- and base-catalyzed diastereoselective cycloaddition of nitrones with isocyanides is described, providing access to a wide range of 2-imidazolinone derivatives with various functional groups as single diastereomers. Varying the base and temperature of the reaction allowed selective access to both diastereomers of the product. A plausible reaction mechanism is proposed and supported by DFT calculations. 

  • 20.
    Chen, Yan
    et al.
    Jiangsu Normal Univ, Sch Chem & Mat Sci, Xuzhou 221116, Jiangsu, Peoples R China..
    Shatskiy, Andrey
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Organic chemistry.
    Liu, Jianquan
    Jiangsu Normal Univ, Sch Chem & Mat Sci, Xuzhou 221116, Jiangsu, Peoples R China..
    Kärkäs, Markus D.
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Organic chemistry.
    Wang, Xiang-Shan
    Jiangsu Normal Univ, Sch Chem & Mat Sci, Xuzhou 221116, Jiangsu, Peoples R China..
    Silver-Promoted (4+1) Annulation of Isocyanoacetates with Alkylpyridinium Salts: Divergent Regioselective Synthesis of 1,2-Disubstituted Indolizines2021In: Organic Letters, ISSN 1523-7060, E-ISSN 1523-7052, Vol. 23, no 19, p. 7555-7560Article in journal (Refereed)
    Abstract [en]

    An unprecedented silver-promoted regioselective (4 + 1) annulation of isocyanoacetates with pyridinium salts is reported. The established protocol provides controlled, facile, and modular access to a range of synthetically useful N-fused heterocyclic scaffolds containing indolizines, pyrrolo[1,2-a]quinolines, pyrrolo[2,1-a]isoquinolines, and 1H-imidazo[4,5-a]indolizin-2(3H)-ones. A mechanistic pathway involving nucleophilic addition/protonation/elimination/cydoisomerization is proposed.

  • 21.
    Cuartero, Maria
    et al.
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Applied Physical Chemistry.
    Chai, Lijun
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Applied Physical Chemistry.
    Zhang, Biaobiao
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Organic chemistry.
    De Marco, Roland
    Univ Sunshine Coast, Fac Sci Hlth Educ & Engn, 90s Sippy Downs Dr, Sippy Downs, Qld 4556, Australia.;Univ Queensland, Sch Chem & Mol Biosci, Brisbane, Qld 4072, Australia.;Curtin Univ, Fuels & Energy Technol Inst, Perth, WA 6102, Australia..
    Crespo, Gaston A.
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Applied Physical Chemistry.
    Ferrocene self assembled monolayer as a redox mediator for triggering ion transfer across nanometer-sized membranes2019In: Electrochimica Acta, ISSN 0013-4686, E-ISSN 1873-3859, Vol. 315, p. 84-93Article in journal (Refereed)
    Abstract [en]

    Modulation of ion-transfer processes across nanometer-sized voltammetry membranes by ferrocene-based self-assembled monolayer on regular glassy carbon electrode is herein demonstrated. The composition of the membrane is advantageously tuned to promote either cation or anion transfer: the presence of an exchangeable cation results in cation transfer, whereas a lipophilic salt induces anion transfer through the fulfilment of the electroneutrality of the system. When an anodic scan oxidizes ferrocene moieties in the monolayer, these are stabilized by the pairing of lipophilic anions present in the membrane. As a result, either, hydrophilic cations present in the membrane are expelled into the solution or anions enter from the solution generating hence reversible and voltammetric waves for these transfers. The use of a redox active monolayer rather than a conducting polymer film or a redox active compound into the membrane overcomes a number of drawbacks previously manifested by these systems. The confinement of the redox process in a thin film at the immediate vicinity of the membrane allows to avoid the need of elevated number of redox moieties to be sued in the membrane, therefore suppressing its acute leaching and being compatible with the incorporation of both cation and anion ionophores for the first time. In this sense, assisted transfer of lithium and chloride are shown as proof-of-concept. Here, the peak potential of the associated voltammetric waves shifts according to the Nernst equation, in analogy to potentiometric sensors. Analytical detection of lithium and chloride ions in real samples is additionally presented.

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  • 22.
    Danielsson, Marie
    et al.
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry.
    Zhao, Tao
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Organic chemistry. Department of Science and Technology, Örebro University, Örebro, Sweden.
    Borg-Karlson, Anna-Karin
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Organic chemistry.
    Arthropod infestation sites and induced defence can be traced by emission from single spruce needles2019In: Arthropod-Plant Interactions, ISSN 1872-8855, E-ISSN 1872-8847, Vol. 13, no 2, p. 253-259Article in journal (Refereed)
    Abstract [en]

    Emissions of defence chemicals from Norway spruce seedlings can be induced by feeding arthropods or by exogenous hormonal application. Some defence chemicals may attract or repel associated arthropods. The aim of this study was to show that it is possible to detect and collect stress-induced volatiles from micro sites, such as at the scale of a single needle, in vivo by using SPME. Methyl jasmonate application on the stem of Norway spruce seedlings induced emission of (E)-beta-farnesene only from the needles closest to the application site. Emissions of (E)-beta-farnesene, (E,E)-alpha-farnesene and (E)-alpha-bisabolene were only detected from needles infested by the spider mite Oligonychus ununguis. The total volatile amount detected by SPME-GC-MS reached a considerable mass of 14 ng/needle/24 h, suggesting that emission from damaged and stressed conifers might have a larger impact on the macro climate than previously estimated.

  • 23.
    Das, Biswanath
    et al.
    Stockholm Univ, Dept Organ Chem, Arrhenius Lab, SE-10691 Stockholm, Sweden..
    Rahaman, Ahibur
    Stockholm Univ, Dept Organ Chem, Arrhenius Lab, SE-10691 Stockholm, Sweden..
    Shatskiy, Andrey
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Organic chemistry.
    Verho, Oscar
    Uppsala Univ, Biomedicinskt Ctr BMC, Dept Med Chem Drug Design & Discovery, SE-10044 Uppsala, Sweden..
    Kärkäs, Markus D.
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Organic chemistry.
    Åkermark, Björn
    Stockholm Univ, Dept Organ Chem, Arrhenius Lab, SE-10691 Stockholm, Sweden..
    The Impact of Ligand Carboxylates on Electrocatalyzed Water Oxidation2021In: Accounts of Chemical Research, ISSN 0001-4842, E-ISSN 1520-4898, Vol. 54, no 17, p. 3326-3337Article, review/survey (Refereed)
    Abstract [en]

    Fossil fuel shortage and severe climate changes due to global warming have prompted extensive research on carbon-neutral and renewable energy resources. Hydrogen gas (H-2), a clean and high energy density fuel, has emerged as a potential solution for both fulfilling energy demands and diminishing the emission of greenhouse gases. Currently, water oxidation (WO) constitutes the bottleneck in the overall process of producing H-2 from water. As a result, the design of efficient catalysts for WO has become an intensively pursued area of research in recent years. Among all the molecular catalysts reported to date, ruthenium-based catalysts have attracted particular attention due to their robust nature and higher activity compared to catalysts based on other transition metals. Over the past two decades, we and others have studied a wide range of ruthenium complexes displaying impressive catalytic performance for WO in terms of turnover number (TON) and turnover frequency (TOF). However, to produce practically applicable electrochemical, photochemical, or photo-electrochemical WO reactors, further improvement of the catalysts' structure to decrease the overpotential and increase the WO rate is of utmost importance. WO reaction, that is, the production of molecular oxygen and protons from water, requires the formation of an O-O bond through the orchestration of multiple proton and electron transfers. Promotion of these processes using redox noninnocent ligand frameworks that can accept and transfer electrons has therefore attracted substantial attention. The strategic modifications of the ligand structure in ruthenium complexes to enable proton-coupled electron transfer (PCET) and atom proton transfer (APT; in the context of WO, it is the oxygen atom (metal oxo) transfer to the oxygen atom of a water molecule in concert with proton transfer to another water molecule) to facilitate the O-O bond formation have played a central role in these efforts. In particular, promising results have been obtained with ligand frameworks containing carboxylic acid groups that either are directly bonded to the metal center or reside in the close vicinity. The improvement of redox and chemical properties of the catalysts by introduction of carboxylate groups in the ligands has proven to be quite general as demonstrated for a range of mono- and dinudear ruthenium complexes featuring ligand scaffolds based on pyridine, imidazole, and pyridazine cores. In the first coordination sphere, the carboxylate groups are firmly coordinated to the metal center as negatively charged ligands, improving the stability of the complexes and preventing metal leaching during catalysis. Another important phenomenon is the reduction of the potentials required for the formation of higher valent intermediates, especially metal-oxo species, which take active part in the key O-O bond formation step. Furthermore, the free carboxylic acid/carboxylate units in the proximity to the active center have shown exciting proton donor/acceptor properties (through PCET or APT, chemically noninnocent) that can dramatically improve the rate as well as the overpotential of the WO reaction.

  • 24.
    Das, Biswanath
    et al.
    Department of Organic Chemistry, Arrhenius Laboratory Stockholm University, Svante Arrhenius väg 16C Stockholm 10691 Sweden, Svante Arrhenius väg 16C.
    Toledo-Carrillo, Esteban Alejandro
    KTH, School of Engineering Sciences (SCI), Applied Physics, Materials and Nanophysics.
    Li, Guoqi
    School of Physical Science and Technology, ShanghaiTech University, Shanghai 201210 China.
    Ståhle, Jonas
    Department of Organic Chemistry, Arrhenius Laboratory Stockholm University, Svante Arrhenius väg 16C Stockholm 10691 Sweden, Svante Arrhenius väg 16C.
    Thersleff, Thomas
    Department of Materials and Environmental Chemistry, Stockholm University, Svante Arrhenius väg 16C Stockholm 10691 Sweden, Svante Arrhenius väg 16C.
    Chen, Jianhong
    Department of Materials and Environmental Chemistry, Stockholm University, Svante Arrhenius väg 16C Stockholm 10691 Sweden, Svante Arrhenius väg 16C.
    Li, Lin
    School of Physical Science and Technology, ShanghaiTech University, Shanghai 201210 China.
    Fei, Ye
    KTH, School of Engineering Sciences (SCI), Applied Physics, Materials and Nanophysics.
    Slabon, Adam
    Inorganic Chemistry, University of Wuppertal Gaußstr. 20, Wuppertal 42119 Germany.
    Göthelid, Mats
    KTH, School of Engineering Sciences (SCI), Applied Physics, Materials and Nanophysics.
    Weng, Tsu Chien
    School of Physical Science and Technology, ShanghaiTech University, Shanghai 201210 China.
    Yuwono, Jodie A.
    School of Chemical Engineering, University of New South Wales, Sydney 2052 Australia.
    Kumar, Priyank V.
    School of Chemical Engineering, University of New South Wales, Sydney 2052 Australia.
    Verho, Oscar
    Department of Medicinal Chemistry, Biomedicinskt Centrum BMC, Uppsala University, SE-75123 Uppsala Sweden.
    Kärkäs, Markus D.
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Organic chemistry.
    Dutta, Joydeep
    KTH, School of Engineering Sciences (SCI), Applied Physics, Materials and Nanophysics.
    Åkermark, Björn
    Department of Organic Chemistry, Arrhenius Laboratory Stockholm University, Svante Arrhenius väg 16C Stockholm 10691 Sweden, Svante Arrhenius väg 16C.
    Bifunctional and regenerable molecular electrode for water electrolysis at neutral pH2023In: Journal of Materials Chemistry A, ISSN 2050-7488, E-ISSN 2050-7496, Vol. 11, no 25, p. 13331-13340Article in journal (Refereed)
    Abstract [en]

    The instability of molecular electrodes under oxidative/reductive conditions and insufficient understanding of the metal oxide-based systems have slowed down the progress of H2-based fuels. Efficient regeneration of the electrode's performance after prolonged use is another bottleneck of this research. This work represents the first example of a bifunctional and electrochemically regenerable molecular electrode which can be used for the unperturbed production of H2 from water. Pyridyl linkers with flexible arms (-CH2-CH2-) on modified fluorine-doped carbon cloth (FCC) were used to anchor a highly active ruthenium electrocatalyst [RuII(mcbp)(H2O)2] (1) [mcbp2− = 2,6-bis(1-methyl-4-(carboxylate)benzimidazol-2-yl)pyridine]. The pyridine unit of the linker replaces one of the water molecules of 1, which resulted in RuPFCC (ruthenium electrocatalyst anchored on -CH2-CH2-pyridine modified FCC), a high-performing electrode for oxygen evolution reaction [OER, overpotential of ∼215 mV] as well as hydrogen evolution reaction (HER, overpotential of ∼330 mV) at pH 7. A current density of ∼8 mA cm−2 at 2.06 V (vs. RHE) and ∼−6 mA cm−2 at −0.84 V (vs. RHE) with only 0.04 wt% loading of ruthenium was obtained. OER turnover of >7.4 × 103 at 1.81 V in 48 h and HER turnover of >3.6 × 103 at −0.79 V in 3 h were calculated. The activity of the OER anode after 48 h use could be electrochemically regenerated to ∼98% of its original activity while it serves as a HE cathode (evolving hydrogen) for 8 h. This electrode design can also be used for developing ultra-stable molecular electrodes with exciting electrochemical regeneration features, for other proton-dependent electrochemical processes.

  • 25.
    Das, Satyajit
    et al.
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Organic chemistry.
    Schaufelberger, Fredrik
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Organic chemistry.
    Interlocked structures on active duty2023In: Nature Chemistry, ISSN 1755-4330, E-ISSN 1755-4349, Vol. 15, no 2, p. 160-162Article in journal (Refereed)
    Abstract [en]

    Interlocking macrocyclic carbon nanomaterials is an exciting way to tune their molecular properties, but all-conjugated catenanes and rotaxanes are extremely challenging to make. Now, fully π-conjugated [2]- and [3]catenanes as well as a [3]rotaxane have been prepared through an ‘active metal template’ approach.

  • 26.
    Deng, Zijian
    et al.
    Dalian Univ Technol DUT, State Key Lab Fine Chem, Inst Artificial Photosynth, Dalian 116024, Peoples R China..
    Yang, Xichuan
    Dalian Univ Technol DUT, State Key Lab Fine Chem, Inst Artificial Photosynth, Dalian 116024, Peoples R China..
    Yang, Kaiyuan
    Dalian Univ Technol DUT, State Key Lab Fine Chem, Inst Artificial Photosynth, Dalian 116024, Peoples R China..
    Zhang, Li
    Dalian Univ Technol DUT, State Key Lab Fine Chem, Inst Artificial Photosynth, Dalian 116024, Peoples R China..
    Wang, Haoxin
    Dalian Univ Technol DUT, State Key Lab Fine Chem, Inst Artificial Photosynth, Dalian 116024, Peoples R China..
    Wang, Xiuna
    Dalian Univ Technol DUT, State Key Lab Fine Chem, Inst Artificial Photosynth, Dalian 116024, Peoples R China..
    Sun, Licheng
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Organic chemistry. Dalian Univ Technol DUT, State Key Lab Fine Chem, Inst Artificial Photosynth, Dalian 116024, Peoples R China.;Westlake Univ, Ctr Artificial Photosynth Solar Fuels, Sch Sci, Hangzhou 310024, Peoples R China..
    Helical Copper Redox Mediator with Low Electron Recombination for Dye-Sensitized Solar Cells2021In: ACS Sustainable Chemistry and Engineering, E-ISSN 2168-0485, Vol. 9, no 15, p. 5252-5259Article in journal (Refereed)
    Abstract [en]

    Redox mediators play a major role in determining the photocurrent and photovoltage in dye-sensitized solar cells (DSSCs). Copper complexes are a good option for redox mediators but suffer from electron recombination. The traditional method is to add 4-(tert-butyl)pyridine (TBP) to the electrolyte, which is coordinated with the empty orbit of Ti, thereby slowing down the oxidized mediator's ability to capture electrons. However, this strategy will result in competitive coordination between the redox mediator and TBP, decreasing the stability of the device. In this study, two helical copper(I) complexes are synthesized and applied to TBP-free solar cells. La (1,3-bis(2,2'-bipyridin-6-yloxy)propane) and Lb (1,3-bis[(6'-methyl-2,2'-bipyridin-6-yl)oxy]propane) tend to form double-stranded helicates ([Cu-2(Ln)(2)](2+), n = a, b) rather than mononuclear complexes ([Cu(Ln)](+), n = a, b). To facilitate quantitative analysis of the complexes, Cu(I)Ln and Cu(II)Ln (n = a, b) are used as molecular formulae. (CuLa)-La-I and Cu(I)Lb are characterized by electrospray mass spectroscopy, H-1 NMR spectroscopy, and electrochemistry. J-V measurement shows that both V-oc and J(sc) increase with the increase of (CuLa)-La-I concentration (below 0.1 M), and the best power conversion efficiency is 8.2%. The relationship between Cu(I) concentration and recombination for further study was measured by IMVS.

  • 27.
    Dieguez, Montserrat
    et al.
    Univ Rovira & Virgili, Dept Quim Fis & Inorgan, Tarragona 43007, Spain..
    Pamies, Oscar
    Univ Rovira & Virgili, Dept Quim Fis & Inorgan, Tarragona 43007, Spain..
    Moberg, Christina
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Organic chemistry.
    Self-Adaptable Tropos Catalysts2021In: Accounts of Chemical Research, ISSN 0001-4842, E-ISSN 1520-4898, Vol. 54, no 16, p. 3252-3263Article, review/survey (Refereed)
    Abstract [en]

    Biological systems have often served as inspiration for the design of synthetic catalysts. The lock and key analogy put forward by Emil Fischer in 1894 to explain the high substrate specificity of enzymes has been used as a general guiding principle aimed at enhancing the selectivity of chemical processes by optimizing attractive and repulsive interactions in molecular recognition events. However, although a perfect fit of a substrate to a catalytic site may enhance the selectivity of a specific catalytic reaction, it inevitably leads to a narrow substrate scope, exduding substrates with different sizes and shapes from efficient binding. An ideal catalyst should instead be able to accommodate a wide range of substrates-it has indeed been recognized that enzymes also are often highly promiscuous as a result of their ability to change their conformation and shape in response to a substrate-and preferentially be useful in various types of processes. In biological adaptation, the process by which species become fitted to new environments is crucial for their ability to cope with changing environmental conditions. With this in mind, we have been exploring catalytic systems that can adapt their size and shape to the environment with the goal of developing synthetic catalysts with wide scope. In this Account, we describe our studies aimed at elucidating how metal catalysts with flexible structural units adapt their binding pockets to the reacting substrate. Throughout our studies, ligands equipped with tropos biaryl units have been explored, and the palladium-catalyzed allylic alkylation reaction has been used as a suitable probe to study the adaptability of the catalytic systems. The conformations of catalytically active metal complexes under different conditions have been studied by both experimental and theoretical methods. By the design of ligands incorporating two flexible units, the symmetry properties of metal complexes could be used to facilitate conformational analysis and thereby provide valuable insight into the structures of complexes involved in the catalytic cycle. The importance of flexibility was convincingly demonstrated when a phosphine group in a privileged ligand that is well-known for its versatility in a number of processes was exchanged for a tropos biaryl phosphite unit: the result was a truly self-adaptive ligand with dramatically increased scope.

  • 28. Du, Jian
    et al.
    Li, Fei
    Sun, Licheng
    KTH, School of Chemical Science and Engineering (CHE), Centres, Centre of Molecular Devices, CMD. KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Organic chemistry. Dalian Univ Technol, DUT KTH Joint Educ & Res Ctr Mol Devices, State Key Lab Fine Chem, Dalian 116024, Peoples R China.;Westlake Univ, Sch Sci, Ctr Artificial Photosynth Solar Fuels, Hangzhou 310024, Peoples R China.;KTH Royal Inst Technol, Sch Engn Sci Chem Biotechnol & Hlth, Dept Chem, S-10044 Stockholm, Sweden..
    Metal-organic frameworks and their derivatives as electrocatalysts for the oxygen evolution reaction2021In: Chemical Society Reviews, ISSN 0306-0012, E-ISSN 1460-4744, Vol. 50, no 4, p. 2663-2695Article, review/survey (Refereed)
    Abstract [en]

    Electrochemical water splitting is an appealing and promising approach for energy conversion and storage. As a key half-reaction of electricity-driven water splitting, the oxygen evolution reaction (OER) is a sluggish process due to the transfer of four protons and four electrons. Therefore, development of low-cost and robust OER electrocatalysts is of great importance for improving the efficiency of water splitting. Based on the merits of high surface area, rich pore structure, diverse composition and well-defined metal centers, metal-organic frameworks (MOFs) and their derivatives have been widely exploited as OER electrocatalysts. Herein, the current progress on MOFs and their derivatives for OER electrolysis is summarized, highlighting the design principle, synthetic methods and performance for MOF-based materials. In addition, the structure-performance relationships of MOFs and their derivatives toward the OER are discussed, providing valuable insights into rationally developing OER catalysts with high efficiency. The current scientific and technological challenges and future perspectives towards the purpose of sustainable industrial applications are addressed at the end.

  • 29.
    Du, Jian
    et al.
    Dalian Univ Technol, State Key Lab Fine Chem, DUT KTH Joint Educ & Res Ctr Mol Devices, Dalian 116024, Peoples R China..
    Li, Fei
    Dalian Univ Technol, State Key Lab Fine Chem, DUT KTH Joint Educ & Res Ctr Mol Devices, Dalian 116024, Peoples R China..
    Wang, Yong
    Dalian Univ Technol, State Key Lab Fine Chem, DUT KTH Joint Educ & Res Ctr Mol Devices, Dalian 116024, Peoples R China..
    Zhu, Yong
    Dalian Univ Technol, State Key Lab Fine Chem, DUT KTH Joint Educ & Res Ctr Mol Devices, Dalian 116024, Peoples R China..
    Sun, Licheng
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Organic chemistry. Dalian Univ Technol, State Key Lab Fine Chem, DUT KTH Joint Educ & Res Ctr Mol Devices, Dalian 116024, Peoples R China..
    Cu3P/CuO Core-Shell Nanorod Arrays as High-Performance Electrocatalysts for Water Oxidation2018In: ChemElectroChem, E-ISSN 2196-0216, Vol. 5, no 15, p. 2064-2068Article in journal (Refereed)
    Abstract [en]

    Earth-abundant transition-metal-based oxides are potential candidates to replace the state-of-the-art noble-metal-based oxygen evolution catalysts (OECs) such as IrO2 and RuO2. Despite the low cost and large abundance, copper-based OER catalysts have been less frequently studied, mainly owing to the low electrical conductivity of copper oxides that results in large overpotential and sluggish kinetics for oxygen evolution. We report here the insitu fabrication of semi-metallic Cu3P nanorod arrays on commercial copper foam via a template approach; the resulting self-supported core-shell Cu-Cu3P/CuO electrode has the merits of high electrical conductivity, large active area, and short diffusion paths for electrolyte and evolved oxygen, exhibiting a low overpotential of 315mV and high durability over 50h at a current density of 10mAcm(-2) for OER in 1.0 M KOH. The remarkable OER performance reported here is not only superior to that of analogous Cu-CuO foam electrode, but also outperforms those of copper-based OER electrocatalysts in the literature.

  • 30.
    Du, Jian
    et al.
    Dalian Univ Technol, DUT KTH Joint Educ & Res Ctr Mol Devices, State Key Lab Fine Chem, Dalian 116024, Peoples R China..
    Liu, Guoquan
    Dalian Univ Technol, DUT KTH Joint Educ & Res Ctr Mol Devices, State Key Lab Fine Chem, Dalian 116024, Peoples R China..
    Li, Fei
    Dalian Univ Technol, DUT KTH Joint Educ & Res Ctr Mol Devices, State Key Lab Fine Chem, Dalian 116024, Peoples R China..
    Zhu, Yong
    Dalian Univ Technol, DUT KTH Joint Educ & Res Ctr Mol Devices, State Key Lab Fine Chem, Dalian 116024, Peoples R China..
    Sun, Licheng
    KTH, School of Chemical Science and Engineering (CHE), Centres, Centre of Molecular Devices, CMD. KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Organic chemistry.
    Iron-Salen Complex and Co2+ Ion-Derived Cobalt-Iron Hydroxide/Carbon Nanohybrid as an Efficient Oxygen Evolution Electrocatalyst2019In: Advanced Science, E-ISSN 2198-3844, Vol. 6, no 12, article id 1900117Article in journal (Refereed)
    Abstract [en]

    Metal-salen complexes are widely used as catalysts in numerous fundamental organic transformation reactions. Here, CoFe hydroxide/carbon nanohybrid is reported as an efficient oxygen evolution electrocatalyst derived from the in situ formed molecular Fe-salen complexes and Co2+ ions at a low temperature of 160 degrees C. It has been evidenced that Fe-salen as a molecular precursor facilitates the confined-growth of metal hydroxides, while Co2+ plays a critical role in catalyzing the transformation of organic ligand into nanocarbons and constitutes an essential component for CoFe hydroxide. The resulting Co1.2Fe/C hybrid material requires an overpotential of 260 mV at a current density of 10 mA cm(-2) with high durability. The high activity is contributed to uniform distribution of CoFe hydroxides on carbon layer and excellent electron conductivity caused by intimate contact between metal and nanocarbon. Given the diversity of molecular precursors, these results represent a promising approach to high-performance carbon-based water splitting catalysts.

  • 31.
    Du, Jian
    et al.
    Dalian Univ Technol, DUT KTH Joint Educ & Res Ctr Mol Devices, State Key Lab Fine Chem, Dalian 116024, Peoples R China..
    Xu, Suxian
    Dalian Univ Technol, DUT KTH Joint Educ & Res Ctr Mol Devices, State Key Lab Fine Chem, Dalian 116024, Peoples R China..
    Sun, Licheng
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Organic chemistry.
    Li, Fei
    Dalian Univ Technol, DUT KTH Joint Educ & Res Ctr Mol Devices, State Key Lab Fine Chem, Dalian 116024, Peoples R China..
    Iron carbonate hydroxide templated binary metal-organic frameworks for highly efficient electrochemical water oxidation2019In: Chemical Communications, ISSN 1359-7345, E-ISSN 1364-548X, Vol. 55, no 98, p. 14773-14776Article in journal (Refereed)
    Abstract [en]

    Metal-organic frameworks (MOFs) are promising catalysts for electrochemical reactions. Herein, self-supported NiFe-MOF nanoplates grown on Ni foam (NF) were prepared with iron carbonate hydroxide nanosheets (FeCH NSs) as a semisacrificial template and evaluated for the electrocatalytic oxygen evolution reaction (OER). In this approach, the porous FeCH NSs not only serve as the iron source of NiFe-MOF, but also slow down the leaching of Ni ions from the substrate, thus playing a unique role in regulating the morphology of NiFe-MOF with reduced thickness and sizes, enabling rapid electron transfer and mass transport. The resultant NiFe-MOF/FeCH-NF electrode showed higher activity than FeCH template-free electrodes and superior OER performance over other MOF based binder-free OER electrodes. A current density of 10 mA cm(-2) was obtained at a low overpotential of 200 mV with excellent durability in alkaline solution. Raman and TEM measurements reveal the partial transformation of NiFe-MOF to hydroxide during water oxidation.

  • 32.
    Du, Jian
    et al.
    Institute of Natural Sciences, Westlake Institute for Advanced Study, China; Center of Artificial Photosynthesis for Solar Fuels, School of Science, Westlake University, China.
    Yang, Hao
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Organic chemistry.
    Sun, Licheng
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Organic chemistry. Institute of Natural Sciences, Westlake Institute for Advanced Study, China; Center of Artificial Photosynthesis for Solar Fuels, School of Science, Westlake University, China; State Key Laboratory of Fine Chemicals, DUT-KTH Joint Education and Research Centre on Molecular Devices, Dalian University of Technology, China.
    2D materials for solar fuels via artificial photosynthesis2022In: National Science Review, ISSN 2095-5138, Vol. 9, no 5, article id nwab116Article in journal (Refereed)
  • 33.
    Elawad, Mohammed
    et al.
    Dalian Univ Technol DUT, DUT KTH Joint Educ & Res Ctr Mol Devices, Inst Artificial Photosynth, State Key Lab Fine Chem, Dalian 116024, Peoples R China.;Omdurman Islamic Univ, Dept Chem, Fac Sci, POB 382, Omdurman, Sudan..
    Lee, Husileng
    Dalian Univ Technol DUT, DUT KTH Joint Educ & Res Ctr Mol Devices, Inst Artificial Photosynth, State Key Lab Fine Chem, Dalian 116024, Peoples R China..
    Yu, Ze
    Dalian Univ Technol DUT, DUT KTH Joint Educ & Res Ctr Mol Devices, Inst Artificial Photosynth, State Key Lab Fine Chem, Dalian 116024, Peoples R China..
    Sun, Licheng
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Organic chemistry. Dalian Univ Technol DUT, DUT KTH Joint Educ & Res Ctr Mol Devices, Inst Artificial Photosynth, State Key Lab Fine Chem, Dalian 116024, Peoples R China..
    Ionic liquid doped organic hole transporting material for efficient and stable perovskite solar cells2020In: Physica. B, Condensed matter, ISSN 0921-4526, E-ISSN 1873-2135, Vol. 586, article id 412124Article in journal (Refereed)
    Abstract [en]

    As a hole transporting material (HTM), N2,N2,N2',N2',N7,N7,N7',N7'-octakis (4-methoxyphenyl) spiro [fluorene-9,9'-xanthene]-2,2',7,7'-tetraamine (X60) in mesoscopic perovskite solar cells (PSCs) has been widely utilized for substitution of the 2,2',7,7'-tetrakis (N,N-di-p-methoxyphenylamine)-9,9'-spiro-bi-fluorene (spiroOMeTAD). In this study, we have introduced an ionic liquid N-butyl-N'-(4-pyridylheptyl) imidazolium bis (trifluoromethane) sulfonamide (BuPyIm-TFSI) as a p-dopant to increase the hole conductivity and stability of the X60 based perovskite solar cells. As a result, based on the different concentrations of BuPyIm-TFSI in mesoscopic PSCs, the optimal condition (4.85 mM) showed the best power conversion efficiency (PCE) of 14.65%, which is extremely higher than the device without BuPyIm-TFSI. Moreover, the device based on X60: BuPyIm-TFSI composite HTM at ambient conditions with humidity of similar to 40% exhibited good PSCs performance with the long-term stability of 840 h. Hence, the use of BuPyIm-TFSI as a p-dopant for X60 played a significant role in enhancing the electrical properties, stability and efficiency of PSCs.

  • 34.
    Elmhalli, Fawzeia
    et al.
    Uppsala Univ, Dept Systemat Biol, Evolutionary Biol Ctr, Norbyvagen 18D, S-75536 Uppsala, Sweden.;Univ Benghazi, Fac Publ Hlth, Dept Environm Hlth, Benghazi, Libya..
    Garboui, Samira S.
    Univ Benghazi, Fac Publ Hlth, Dept Environm Hlth, Benghazi, Libya..
    Borg-Karlson, Anna-Karin
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Organic chemistry.
    Mozuraitis, Raimondas
    Stockholm Univ, Dept Zool, Svante Arrhenius Vag 18B, S-11418 Stockholm, Sweden..
    Baldauf, Sandra L.
    Uppsala Univ, Dept Systemat Biol, Evolutionary Biol Ctr, Norbyvagen 18D, S-75536 Uppsala, Sweden..
    Grandi, Giulio
    Swedish Univ Agr Sci SLU, Dept Biomed Sci & Vet Publ Hlth, Box 7036,Ulls Vag 26, S-75651 Uppsala, Sweden.;Natl Vet Inst SVA, Dept Microbiol, Ulls Vag 2B, S-75651 Uppsala, Sweden..
    Acaricidal activity against Ixodes ricinus nymphs of essential oils from the Libyan plants Artemisia herba alba, Origanum majorana and Juniperus phoenicea2021In: Veterinary Parasitology: Regional Studies and Reports, E-ISSN 2405-9390, Vol. 24, article id 100575Article in journal (Refereed)
    Abstract [en]

    Ixodes ricinus (L.) (Acari: Ixodidae) is a major vector for the transmission of several important human pathogens. The aim of the present study was to evaluate the in vitro efficacy of different concentrations of essential oils (Eos) on I. ricinus tick nymphs. Oils were obtained from the leaves of three plants native to Libya: white wormwood (Artemisia herba alba Asso), marjoram (Origanum majorana L.) and Arar (Juniperus phoenicea L., English common name Phoenician juniper). Assays were done using the "open filter paper method". Two concentrations from each oil, 0.5 and 1 mu l/cm, were tested. The acaricidal effect was measured in terms of the lethal concentrations (LC50, LC95) and lethal time (LT50, LT95). Mortality rates were obtained by counting the surviving nymphs every 30 min for the first five hours and then at 24, 48 and 72 h. A mortality of 100% was recorded at the higher concentration of oils (1 mu l/cm(2)) from A. herba alba and J. phoenicea at the first 2 h of exposure. Exposure to O. majorana led to 100% mortality on the third day (72 h), and this effect decreased noticeably with 0.5 mu l/cm(2) oil at the same exposure time. However, 50% of ticks showed a paralysis effect and less movement after 2 h. The LC50 of mortality was reached within the first 24 h of exposure time at 0.5 mu l/cm(2) of O. majorana, which produced 60% tick's mortality. Chemical composition of the essential oils was elucidated by gas chromatography-mass spectrometry analyses. These results suggest that essential oils deserve further investigation as components of alternative approaches for I. ricinus tick control.

  • 35. Elmhalli, Fawzeia
    et al.
    Garboui, Samira S.
    Borg-Karlson, Anna-Karin
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Organic chemistry.
    Mozuraitis, Raimondas
    Baldauf, Sandra L.
    Grandi, Giulio
    The repellency and toxicity effects of essential oils from the Libyan plants Salvadora persica and Rosmarinus officinalis against nymphs of Ixodes ricinus2019In: Experimental & applied acarology, ISSN 0168-8162, E-ISSN 1572-9702, Vol. 77, no 4, p. 585-599Article in journal (Refereed)
    Abstract [en]

    Essential oils extracted from the leaves of Libyan Rosemary (Rosmarinus officinalis L.), and Miswak (Salvadora persica L.) were evaluated for their acaricidal and repellent effects on Ixodes ricinus L. nymphs (Acari: Ixodidae) using a bioassay based on an open filter paper method'. Rosmarinus officinalis leaf essential oil diluted to 0.5 and 1 mu l/cm(2) in acetone exhibited, respectively, 20 and 100% tick mortality after about 5h of exposure. A total of 50 and 95% of I. ricinus nymphs were killed by direct contact with the oil when exposed to lethal concentrations (LC)of 0.7 mu l/cm(2) (LC50) and 0.95 mu l/cm(2) (LC95), respectively. The LC50 (0.5 mu l/cm(2)) was reached before the end of the first 24h of exposure time (ET), as tick mortality at 24h was 60%. Salvadora persica leaf essential oil at 1 mu l/cm(2) showed a significant repellency effect against I. ricinus nymphs at 1.5h ET. A 95% repellency was observed at a repellent concentration (RC95) of 1 mu l/cm(2) of S. persica, but no significant mortality was recorded at this dose of S. persica oil. Gas chromatography-mass spectrometry analyses showed that the main monoterpenes in both oils were 1,8-cineol, -pinene, and -pinene, although in markedly different proportions. These results suggest that essential oils have substantial potential as alternative approaches for I. ricinus tick control.

  • 36.
    Fan, Ke
    et al.
    Wuhan Univ Technol, State Key Lab Adv Technol Mat Synth & Proc, Wuhan 430070, Peoples R China.;DUT, DUT KTH Joint Educ & Res Ctr Mol Devices, Inst Energy Sci & Technol, State Key Lab Fine Chem,Inst Artificial Photosynt, Dalian 116024, Peoples R China..
    He, Min
    Wuhan Univ Technol, State Key Lab Adv Technol Mat Synth & Proc, Wuhan 430070, Peoples R China..
    Dharanipragada, N. V. R. Aditya
    Stockholm Univ, Dept Mat & Environm Chem, S-10691 Stockholm, Sweden..
    Kuang, Panyong
    Wuhan Univ Technol, State Key Lab Adv Technol Mat Synth & Proc, Wuhan 430070, Peoples R China..
    Jia, Yufei
    Wuhan Univ Technol, State Key Lab Adv Technol Mat Synth & Proc, Wuhan 430070, Peoples R China..
    Fan, Lizhou
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Organic chemistry.
    Inge, A. Ken
    Stockholm Univ, Dept Mat & Environm Chem, S-10691 Stockholm, Sweden..
    Zhang, Biaobiao
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Organic chemistry.
    Sun, Licheng
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Organic chemistry. DUT, DUT KTH Joint Educ & Res Ctr Mol Devices, Inst Energy Sci & Technol, State Key Lab Fine Chem,Inst Artificial Photosynt, Dalian 116024, Peoples R China..
    Yu, Jiaguo
    Wuhan Univ Technol, State Key Lab Adv Technol Mat Synth & Proc, Wuhan 430070, Peoples R China..
    Amorphous WO3 induced lattice distortion for a low-cost and high-efficient electrocatalyst for overall water splitting in acid2020In: Sustainable Energy & Fuels, E-ISSN 2398-4902, Vol. 4, no 4, p. 1712-1722Article in journal (Refereed)
    Abstract [en]

    The development of highly active and durable catalysts for water oxidation under acidic conditions is necessary but challenging for renewable energy conversion. Ir-based catalysts are highly efficient for water oxidation in acid, but their large scale application is hindered by the high cost and scarcity of iridium. Herein, we use an amorphous WO3 induced lattice distortion (AWILD) strategy to reduce the Ir content to only 2 wt% in the final material. The optimized hybrid nitrogen-doped carbon (NC)/WO3/IrO2 can efficiently catalyze water oxidation with a low overpotential of 270 mV at 10 mA cm(-2) current density (eta (10)) and a high turnover frequency of over 2 s(-1) at 300 mV overpotential in 0.5 M H2SO4, a performance that surpasses that of commercial IrO2 significantly. Introducing the layer of amorphous WO3 between IrO2 nanoparticles and NC can distort the lattice of IrO2, exposing more highly active sites for water oxidation. The AWILD effect compensates for the lower Ir content and dramatically reduces the cost of the catalyst without sacrificing the catalytic activity. Additionally, this catalyst also exhibits high activity in acid for hydrogen evolution with only 65 mV of eta (10) attributed to the AWILD effect, exhibiting efficient bifunctionality as a Janus catalyst for overall water splitting. The AWILD approach provides a novel and efficient strategy for low-cost and highly efficient electrocatalysts for acidic overall water splitting with an extremely low content of noble metals.

  • 37.
    Fan, Ke
    et al.
    State Key Laboratory of Fine Chemicals, Institute of Artificial Photosynthesis, DUT-KTH Joint Education and Research Centre on Molecular Devices, Institute for Energy Science and Technology, Dalian University of Technology, Dalian, 116024, China.
    Zou, H.
    Dharanipragada, N. V. R. A.
    Fan, L.
    Inge, A. K.
    Duan, L.
    Zhang, Biaobiao
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Organic chemistry.
    Sun, Licheng
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Organic chemistry. State Key Laboratory of Fine Chemicals, Institute of Artificial Photosynthesis, DUT-KTH Joint Education and Research Centre on Molecular Devices, Institute for Energy Science and Technology, Dalian University of Technology, Dalian, 116024, China; Center of Artificial Photosynthesis for Solar Fuels, School of Science, Westlake University, Hangzhou, 310024, China.
    Surface and bulk reconstruction of CoW sulfides during pH-universal electrocatalytic hydrogen evolution2021In: Journal of Materials Chemistry A, ISSN 2050-7488, E-ISSN 2050-7496, Vol. 9, no 18, p. 11359-11369Article in journal (Refereed)
    Abstract [en]

    Electrocatalytic water splitting is an efficient means of producing energy carriers, such as H2. The hydrogen evolution reaction (HER) requires high-efficiency electrocatalysts. Understanding the active site structures of the HER electrocatalysts is essential for the rational design and development of water splitting devices. In this study, porous CoW sulfides were employed as model electrocatalysts for pH-universal HER. Multiple characterization studies, such as X-ray photoelectron spectroscopy, X-ray absorption spectroscopy and operando X-ray diffraction, were systematically used to investigate the reconstruction of the active species at the surface and in the bulk. The results show that during the HER, the structural transformation of the species CoW sulfides is strongly dependent on the pH of the electrolyte. Electrolytes of varying pH lead to varied reconstruction and influence the true catalytically active species responsible for the HER. The surface and the bulk of the electrocatalysts transform to different oxides/hydroxides when subjected to the HER. This is the first time that the pH-dependent bulk and surface structural evolution in the HER has been revealed. This study reveals the reconstruction and potential active site evolution of mixed-metal sulfides for the HER. We believe that the present study not only provides an idealized "pre-catalyst"for pH-universal highly-efficient HER, but also provides a thorough understanding about the identification of the real active sites and the mechanism of the structural evolution of the electrocatalysts during hydrogen evolution.

  • 38.
    Fan, Ke
    et al.
    Dalian Univ Technol, Inst Energy Sci & Technol, DUT KTH Joint Educ & Res Ctr Mol Devices, State Key Lab Fine Chem, Dalian 116024, Peoples R China..
    Zou, Haiyuan
    Southern Univ Sci & Technol, Shenzhen Grubbs Inst, Dept Chem, Shenzhen 518055, Peoples R China.;Southern Univ Sci & Technol, Guangdong Prov Key Lab Energy Mat Elect Power, Shenzhen 518055, Peoples R China..
    Ding, Yunxuan
    Dharanipragada, N. V. R. Aditya
    Stockholm Univ, Dept Mat & Environm Chem, S-10691 Stockholm, Sweden..
    Fan, Lizhou
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Organic chemistry. Center of Artificial Photosynthesis for Solar Fuels, School of Science, Westlake University, Hangzhou, 310024, China.
    Inge, A. Ken
    Stockholm Univ, Dept Mat & Environm Chem, S-10691 Stockholm, Sweden..
    Duan, Lele
    Southern Univ Sci & Technol, Shenzhen Grubbs Inst, Dept Chem, Shenzhen 518055, Peoples R China.;Southern Univ Sci & Technol, Guangdong Prov Key Lab Energy Mat Elect Power, Shenzhen 518055, Peoples R China..
    Zhang, Biaobiao
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Organic chemistry.
    Sun, Licheng
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Organic chemistry. State Key Laboratory of Fine Chemicals, Institute of Artificial Photosynthesis, DUT-KTH Joint Education and Research Centre on Molecular Devices, Institute for Energy Science and Technology, Dalian University of Technology, Dalian, 116024, China; Center of Artificial Photosynthesis for Solar Fuels, School of Science, Westlake University, Hangzhou, 310024, China.
    Sacrificial W Facilitates Self-Reconstruction with Abundant Active Sites for Water Oxidation2022In: Marine and Petroleum Geology, ISSN 0264-8172, E-ISSN 1873-4073, Vol. 138, article id 2107249Article in journal (Refereed)
    Abstract [en]

    Water oxidation is an important reaction for multiple renewable energy conversion and storage-related devices and technologies. High-performance and stable electrocatalysts for the oxygen evolution reaction (OER) are urgently required. Bimetallic (oxy)hydroxides have been widely used in alkaline OER as electrocatalysts, but their activity is still not satisfactory due to insufficient active sites. In this research, A unique and efficient approach of sacrificial W to prepare CoFe (oxy)hydroxides with abundant active species for OER is presented. Multiple ex situ and operando/in situ characterizations have validated the self-reconstruction of the as-prepared CoFeW sulfides to CoFe (oxy) hydroxides in alkaline OER with synchronous W etching. Experiments and theoretical calculations show that the sacrificial W in this process induces metal cation vacancies, which facilitates the in situ transformation of the intermediate metal hydroxide to CoFe-OOH with more high-valence Co(III), thus creating abundant active species for OER. The Co(III)-rich environment endows the in situ formed CoFe oxyhydroxide with high catalytic activity for OER on a simple flat glassy carbon electrode, outperforming those not treated by the sacrificial W procedure. This research demonstrates the influence of etching W on the electrocatalytic performance, and provides a low-cost means to improve the active sites of the in situ self-reconstructed bimetallic oxyhydroxides for OER.

  • 39.
    Fan, Lizhou
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Organic chemistry.
    Towards Artificial Photosynthesis: Exploration of Efficient First-Row Transition Metal-Based Water Oxidation Catalysts2020Doctoral thesis, comprehensive summary (Other academic)
    Abstract [en]

    Artificial photosynthesis provides a promising strategy for sustainable energy harvesting, yet its overall efficiency is limited by the water oxidation reaction. The subject of this thesis focuses on the exploration of highly efficient cost-effective heterogeneous catalysts for water oxidation, and the investigation of essential catalyst structure-activity relationships.

    Chapters 1 and 2 present a brief introduction on heterogeneous catalysts for water oxidation, including selected state-of-the-art catalysts, methodologies for activity improvement, and mechanistic investigations. The characterization methods used in this thesis are also demonstrated.

    In chapter 3, a molecular functionalization approach is developed to rationally modify the electronic structure of NiO catalyst, by which the water oxidation activity is systematically tailored. These studies correspond to the question: “How to rationally adjust the catalytic performance of heterogeneous catalysts?

    In chapter 4, to lower the catalyst cost, a Fe-based Fe0.65Cr0.35Ox nanocatalyst is fabricated by structural and electronic modulation, which shows considerable water oxidation activity. These studies target the question: “How to fabricate an efficient Fe-based water oxidation catalyst?

    In chapter 5, a bio-inspired Mn-based catalyst is presented. The catalyst successfully imitates the key features of the natural oxygen evolving complex, achieving dramatically improved water oxidation activity. These studies correspond to the question: “How to improve the catalytic activity of Mn-based water oxidation catalysts?

    Finally, in chapter 6, a 3D NiFeCr/Cu nanoarray electrode is constructed by structural engineering, which exhibits extremely high water oxidation activity. These studies correspond to the question: “How to fabricate an efficient catalytic electrode for water oxidation?

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  • 40.
    Fan, Lizhou
    et al.
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Organic chemistry.
    Song, Yuxiang
    Center of Artificial Photosynthesis for Solar Fuels and Department of Chemistry, School of Science and Research Center for Industries of the Future, Westlake University, Zhejiang, Hangzhou, 310024, China.
    Zhang, Fan
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Surface and Corrosion Science.
    Timmer, Brian
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Organic chemistry.
    Kravberg, Alexander
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Organic chemistry.
    Zhang, Biaobiao
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Organic chemistry. Center of Artificial Photosynthesis for Solar Fuels and Department of Chemistry, School of Science and Research Center for Industries of the Future, Westlake University, Zhejiang, Hangzhou, 310024, China.
    Sun, Licheng
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Organic chemistry. State Key Laboratory of Fine Chemicals, Institute of Artificial Photosynthesis, DUT-KTH Joint Education and Research Center on Molecular Devices, Dalian University of Technology (DUT), Dalian, 116024, China;Center of Artificial Photosynthesis for Solar Fuels and Department of Chemistry, School of Science and Research Center for Industries of the Future, Westlake University, Zhejiang, Hangzhou, 310024, China.
    Holistic functional biomimetics: a key to make an efficient electrocatalyst for water oxidation2023In: Journal of Materials Chemistry A, ISSN 2050-7488, E-ISSN 2050-7496, Vol. 11, no 20, p. 10669-10676Article in journal (Refereed)
    Abstract [en]

    Water oxidation is the holy grail reaction of natural and artificial photosynthesis. How to design an efficient water-oxidation catalyst remains a long-term challenge for solar fuel production. The rate of water oxidation in photosystem II by the oxygen-evolving complex (OEC) Mn4CaO5 cluster is as high as 100-400 s−1. Mimicking the structures of the OEC is a straightforward strategy to design water-oxidation catalysts. However, the high efficiency of the OEC relies on not only its highly active site but also its holistic system for well-organized electron transfer and proton transport. Lacking such a holistic functional system makes δ-MnO2 a poor water-oxidation catalyst, although the local structure of δ-MnO2 is similar to that of the Mn4CaO5 cluster. Electrocatalysts simultaneously imitating the catalytically active sites, fast electron transfer, and promoted proton transport in a natural OEC have been rarely reported. The significance of the synergy of a holistic system is underrated in the design of water-oxidation catalysts. In this work, we fabricated holistic functional biomimetic composites of two-dimensional manganese oxide nanosheets and pyridyl-modified graphene (MnOx-NS/py-G) for electrocatalytic water oxidation. MnOx-NS/py-G simultaneously imitates the synergy of catalytically active sites, fast electron transfer, and promoted proton transport in a natural OEC, resulting in overall 600 times higher activity than that of typical δ-MnO2. This work demonstrates the significance of holistic functional biomimetic design and guides the development of highly active electrocatalysts for small molecule activation related to solar energy storage.

  • 41.
    Fan, Lizhou
    et al.
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Organic chemistry.
    Zhang, Biaobiao
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Organic chemistry.
    Qiu, Zhen
    Dharanipragada, N. V. R. Aditya
    Timmer, Brian
    Zhang, Fuguo
    Sheng, Xia
    Liu, Tianqi
    Meng, Qijun
    Inge, A. Ken
    Edvinsson, Tomas
    Sun, Licheng
    KTH, School of Chemical Science and Engineering (CHE), Centres, Centre of Molecular Devices, CMD. KTH, Superseded Departments (pre-2005), Chemistry. KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Organic chemistry.
    Molecular functionalization of NiO nanocatalyst for enhanced water oxidation by electronic structure engineeringIn: ChemSusChem, ISSN 1864-5631, E-ISSN 1864-564XArticle in journal (Refereed)
    Abstract [en]

    Tuning the local environment of nanomaterial-based catalysts has emerged as an effective approach to optimize their oxygen evolution reaction (OER) performance, yet the controlled electronic modulation around surface active sites remains a grand challenge. Herein, we achieve directed electronic modulation of NiO nanoparticles by simple surface molecular modification with small organic molecules. By adjusting the electronic properties of modifying molecules, the local electronic structure is rationally tailored and a close electronic structure-activity relationship is discovered: the increasing electron-withdrawing modification readily decreases the electron density around surface Ni sites, accelerating the reaction kinetics and improving OER activity, and vice versa. Detailed investigation by operando Raman spectroelectrochemistry revealed that the electron-withdrawing modification facilitates the charge transfer kinetics, stimulates the catalyst reconstruction, and promotes abundant high-valent γ-NiOOH reactive species generation. The NiO-C6F5 catalyst, with the optimized electronic environment, exhibits superior performance towards water oxidation. This work provides a well-designed and effective approach for heterogeneous catalyst fabrication under the molecular level.

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  • 42.
    Fan, Lizhou
    et al.
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Organic chemistry. KTH Royal Inst Technol, Dept Chem, S-10044 Stockholm, Sweden..
    Zhang, Biaobiao
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Organic chemistry. KTH Royal Inst Technol, Dept Chem, S-10044 Stockholm, Sweden..
    Timmer, Brian
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Organic chemistry.
    Dharanipragada, N. V. R. Aditya
    Stockholm Univ, Dept Mat & Environm Chem, S-10691 Stockholm, Sweden..
    Sheng, Xia
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Organic chemistry.
    Tai, Cheuk-Wai
    Stockholm Univ, Dept Mat & Environm Chem, S-10691 Stockholm, Sweden..
    Zhang, Fuguo
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry. KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Fibre- and Polymer Technology, Coating Technology.
    Liu, Tianqi
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Organic chemistry.
    Meng, Qijun
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Glycoscience.
    Inge, A. Ken
    Stockholm Univ, Dept Mat & Environm Chem, S-10691 Stockholm, Sweden..
    Sun, Licheng
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry. KTH Royal Inst Technol, Dept Chem, S-10044 Stockholm, Sweden.;Dalian Univ Technol DUT, DUT KTH Joint Educ & Res Ctr Mol Devices, Inst Artificial Photosynth, State Key Lab Fine Chem, Dalian 116024, Peoples R China..
    Promoting the Fe(VI) active species generation by structural and electronic modulation of efficient iron oxide based water oxidation catalyst without Ni or Co2020In: Nano Energy, ISSN 2211-2855, E-ISSN 2211-3282, Vol. 72, article id 104656Article in journal (Refereed)
    Abstract [en]

    Fe is considered as a promising alternative for OER catalysts owing to its high natural abundance and low cost. Due to the low conductivity and sluggish catalytic kinetics, the catalytic efficiency of Fe-rich catalysts is far from less abundant Ni, Co-rich alternatives and has been hardly improved without the involvement of Ni or Co. The lower activity of Fe-rich catalysts renders the real active center of state-of-the-art NiFe, CoFe catalyst in long-term scientific debate, despite of detection of Fe-based active intermediates in these catalysts during catalytic process. In the present work, we fabricated a series of sub-5 nm Fe1-yCryOx nanocatalysts via a simple solvothermal method, achieving systematically promoted high-valent Fe(VI) species generation by structural and electronic modulation, displaying highly active OER performance without involvement of Ni or Co. Detailed investigation revealed that the high OER activity is related to the ultrasmall nanoparticle size that promotes abundant edge- and corner-site exposure at catalyst surface, which involves in OER as highly reactive site; and the incorporated Cr ions that remarkably accelerate the charge transfer kinetics, providing an effective conduit as well as suitable host for high-valent active intermediate. This work reveals the structural prerequisites for efficient Fe-rich OER catalyst fabrication, inspiring deeper understanding of the structure-activity relationship as well as OER mechanism of Fe-based catalysts.

  • 43.
    Fan, Lizhou
    et al.
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Organic chemistry.
    Zhang, Biaobiao
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Organic chemistry.
    Zhang, Fan
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Surface and Corrosion Science.
    Timmer, Brian
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Organic chemistry.
    Kravchenko, Oleksandr
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Organic chemistry.
    Sun, Licheng
    KTH, School of Chemical Science and Engineering (CHE), Centres, Centre of Molecular Devices, CMD. KTH, Superseded Departments (pre-2005), Chemistry. KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Organic chemistry.
    2D MnOx composite catalysts inspired by natural OEC for efficient catalyticwater oxidationManuscript (preprint) (Other academic)
    Abstract [en]

    Birnessite MnOx is a close inorganic model of natural oxygen-evolving complex (OEC) that hasbeen widely investigated for catalytic water oxidation, yet its activity is limited by the pooractive site exposure and sluggish charge transfer. Herein, starting from typical birnessite MnOx,we fabricated a hybrid of 2D manganese oxide nanosheets and pyridyl modified graphene(MnOx-NS/py-G) for electrocatalytic water oxidation. Benefiting from the synergy of structuralexfoliation, graphene substrate and molecular pyridyl modification, the MnOx-NS/py-G exhibitsabundant catalytically active sites exposure, fast electron transport, and promoted proton transferat catalyst surface, which imitates the key features of natural OEC. Consequently, theMnOx-NS/py-G reached over 600 times higher activity compared to the typical birnessite MnOx.Inspired by nature, this work provides a well-designed and effective strategy to develop highlyactive manganese oxide-based water oxidation catalysts.

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  • 44.
    Fan, Yanmiao
    et al.
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Fibre- and Polymer Technology, Coating Technology.
    Chen, Chao
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Fibre- and Polymer Technology.
    Fu, Ying
    KTH, School of Engineering Sciences (SCI), Applied Physics.
    Ek, Monica
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Fibre- and Polymer Technology.
    Ramström, Olof
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Organic chemistry.
    Fluorescent silicon nanoparticles as a potential capaturing and imaging agent for Staphylococcus aureusManuscript (preprint) (Other academic)
    Abstract [en]

    Nanomaterials, with various shapes and specific physicochemical properties, have attracted a lot of interest in the biomedical fields. Fluorescent silicon nanoparticles (SiNPs) have shown promise as immunofluorescent cellular imaging agents. In this study, SiNPs were synthesized to explore their potential as bacterial imaging agents. Silicon nanoparticles with amino groups on the surface were prepared using microwave-assisted synthesis method using trisodium citrate as the reducing agent. The obtained SiNPs were characterized using dynamic light scattering (DLS), UV−vis absorption spectroscopy and fluorescence spectrophotometer. And SiNPs were used to study their interactions with both Gram-negative Escherichia coli (E. coli) and Gram-positive Staphylococcus aureus (S. aureus). The interactions between the prepared SiNPs and bacteria were monitored by the fluorescence microscope, and SiNPs showed a strong interaction with S. aureus. SEM was used to study the morphological changes of S. aureus, and we found that the cell membranes of S. aureus became damaged after the interaction with SiNPs. The amino groups on the surfaces of SiNPs could also be functionalized with other functional groups for other applications. 

  • 45.
    Fan, Yanmiao
    et al.
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Fibre- and Polymer Technology, Coating Technology.
    Chen, Chao
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Fibre- and Polymer Technology.
    Ren, Yansong
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Organic chemistry.
    Ek, Monica
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Fibre- and Polymer Technology.
    Ramström, Olof
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Organic chemistry.
    Detection of gemcitabine metabolism using 19F-NMR and its impacts on E. coli morphologyManuscript (preprint) (Other academic)
    Abstract [en]

    19F-NMR spectroscopy is a sensitive analytical method to detect the metabolism of fluorine-containing drugs by bacteria. In this study, 19F-NMR was used to achieve the real time detection of metabolic process of gemcitabine (2′, 2′-difluorodeoxycytidine) by Escherichia Coli (E. coli) in the nutrient broth. Both E. coli and Staphylococcus aureus (S. aureus) were used in the metabolism study. E. coli can metabolize gemcitabine, while gemcitabine cannot be metabolized by S. aureus. Our results showed that gemcitabine can be totally metabolized to its inactive form 2′, 2′-difluorodeoxyuridine (dFdU) by E. coli both in Mueller-Hinton broth and M9 minimal salt. The metabolic rate of gemcitabine has a positive correlation with the bacterial concentrations. The metabolism is due to the presence of bacterial cytidine deaminase, and the enzyme inhibitor tetrahydrouridine (THU) can inhibit the gemcitabine metabolism. Scanning electron microscope (SEM) was used to study the effects of gemcitabine metabolism on E. coli morphological changes, and the treated E. coli was 2-3 times longer than the normal bacteria. 19F–NMR was capable to achieve real time detection of gemcitabine metabolism process considering there was no need to separate the bacterial cells from the nutrient medium, this study provided a fast and facile way to detect fluorine-containing drug metabolism by bacteria.

  • 46.
    Fan, Zhaozhong
    et al.
    State Key Laboratory of Fine Chemicals, Frontiers Science Center for Smart Materials Oriented Chemical Engineering, School of Chemical Engineering, Dalian University of Technology, Dalian, 116024, P. R. China.
    Luo, Ruichun
    School of Physical Sciences and CAS Key Laboratory of Vacuum Physics, University of Chinese Academy of Sciences, Beijing, 100049, P. R. China; CAS Center for Excellence in Topological Quantum Computation, University of Chinese Academy of Sciences, Beijing, 100049, P. R. China.
    Zhang, Yanxue
    Laboratory of Materials Modification by Laser, Ion and Electron Beams, Ministry of Education, Dalian University of Technology, Dalian, 116024, P. R. China.
    Zhang, Bo
    State Key Laboratory of Fine Chemicals, Frontiers Science Center for Smart Materials Oriented Chemical Engineering, School of Chemical Engineering, Dalian University of Technology, Dalian, 116024, P. R. China.
    Zhai, Panlong
    State Key Laboratory of Fine Chemicals, Frontiers Science Center for Smart Materials Oriented Chemical Engineering, School of Chemical Engineering, Dalian University of Technology, Dalian, 116024, P. R. China.
    Zhang, Yanting
    State Key Laboratory of Fine Chemicals, Frontiers Science Center for Smart Materials Oriented Chemical Engineering, School of Chemical Engineering, Dalian University of Technology, Dalian, 116024, P. R. China.
    Wang, Chen
    State Key Laboratory of Fine Chemicals, Frontiers Science Center for Smart Materials Oriented Chemical Engineering, School of Chemical Engineering, Dalian University of Technology, Dalian, 116024, P. R. China.
    Gao, Junfeng
    Laboratory of Materials Modification by Laser, Ion and Electron Beams, Ministry of Education, Dalian University of Technology, Dalian, 116024, P. R. China.
    Zhou, Wu
    School of Physical Sciences and CAS Key Laboratory of Vacuum Physics, University of Chinese Academy of Sciences, Beijing, 100049, P. R. China; CAS Center for Excellence in Topological Quantum Computation, University of Chinese Academy of Sciences, Beijing, 100049, P. R. China.
    Sun, Licheng
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Organic chemistry. Center of Artificial Photosynthesis for Solar Fuels, School of Science, Westlake University, Hangzhou, 310024, P. R. China.
    Hou, Jungang
    State Key Laboratory of Fine Chemicals, Frontiers Science Center for Smart Materials Oriented Chemical Engineering, School of Chemical Engineering, Dalian University of Technology, Dalian, 116024, P. R. China.
    Oxygen-Bridged Indium-Nickel Atomic Pair as Dual-Metal Active Sites Enabling Synergistic Electrocatalytic CO2 Reduction2023In: Angewandte Chemie International Edition, ISSN 1433-7851, E-ISSN 1521-3773, Vol. 62, no 7, article id e202216326Article in journal (Refereed)
    Abstract [en]

    Single-atom catalysts offer a promising pathway for electrochemical CO2 conversion. However, it is still a challenge to optimize the electrochemical performance of dual-atom catalysts. Here, an atomic indium-nickel dual-sites catalyst bridged by an axial oxygen atom (O-In-N6-Ni moiety) was anchored on nitrogenated carbon (InNi DS/NC). InNi DS/NC exhibits superior CO selectivity with Faradaic efficiency higher than 90 % over a wide potential range from −0.5 to −0.8 V versus reversible hydrogen electrode (vs. RHE). Moreover, an industrial CO partial current density up to 317.2 mA cm−2 is achieved at −1.0 V vs. RHE in a flow cell. In situ ATR-SEIRAS combined with theory calculations reveal that the synergistic effect of In-Ni dual-sites and O atom bridge not only reduces the reaction barrier for the formation of *COOH, but also retards the undesired hydrogen evolution reaction. This work provides a feasible strategy to construct dual-site catalysts towards energy conversion.

  • 47.
    Fang, Zhiyong
    et al.
    Dalian Univ Technol, DUT KTH Joint Educ & Res Ctr Mol Devices, Inst Artificial Photosynth, State Key Lab Fine Chem, Dalian 116024, Peoples R China..
    Zhang, Peili
    Dalian Univ Technol, DUT KTH Joint Educ & Res Ctr Mol Devices, Inst Artificial Photosynth, State Key Lab Fine Chem, Dalian 116024, Peoples R China..
    Wang, Mei
    Dalian Univ Technol, DUT KTH Joint Educ & Res Ctr Mol Devices, Inst Artificial Photosynth, State Key Lab Fine Chem, Dalian 116024, Peoples R China..
    Li, Fusheng
    Dalian Univ Technol, DUT KTH Joint Educ & Res Ctr Mol Devices, Inst Artificial Photosynth, State Key Lab Fine Chem, Dalian 116024, Peoples R China..
    Wu, Xiujuan
    Dalian Univ Technol, DUT KTH Joint Educ & Res Ctr Mol Devices, Inst Artificial Photosynth, State Key Lab Fine Chem, Dalian 116024, Peoples R China..
    Fan, Ke
    Dalian Univ Technol, DUT KTH Joint Educ & Res Ctr Mol Devices, Inst Artificial Photosynth, State Key Lab Fine Chem, Dalian 116024, Peoples R China..
    Sun, Licheng
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Organic chemistry. Dalian Univ Technol, DUT KTH Joint Educ & Res Ctr Mol Devices, Inst Artificial Photosynth, State Key Lab Fine Chem, Dalian 116024, Peoples R China.;Westlake Univ, Ctr Artificial Photosynth Solar Fuels, Sch Sci, Hangzhou 310024, Peoples R China..
    Selective Electro-oxidation of Alcohols to the Corresponding Aldehydes in Aqueous Solution via Cu(III) Intermediates from CuO Nanorods2021In: ACS Sustainable Chemistry and Engineering, E-ISSN 2168-0485, Vol. 9, no 35, p. 11855-11861Article in journal (Refereed)
    Abstract [en]

    Electrochemical oxidation using renewable energy is an attractive strategy that provides a sustainable and mild approach for biomass transformation. Herein, the electrocatalytic oxidation of furfuryl alcohol in an aqueous solution was investigated using CuO nanorods. Two kinds of Cu-III intermediates, namely, (CuO2)(-) and (Cu2O6)(6-), were detected on the surface of the working electrode. (Cu2O6)(6-), generated in the potential range of 1.35-1.39 V versus the reversible hydrogen electrode (RHE), induced the oxidation of furfuryl alcohol to furaldehyde with a yield of >= 98%. (CuO2)(-), generated at a potential greater than 1.39 V versus RHE, which led to the oxidation of furfuryl alcohol to 2-furoic acid with a yield of >= 99%. Furthermore, the Cu-III-catalyzed system exhibited a measure of universal applicability, wherein (Cu2O6)(6-) and (CuO2)(-) induced the highly selective electro-oxidation of benzyl alcohol, vanillyl alcohol, and 4-pyridinemethanol to yield the corresponding aldehydes and acids, respectively.

  • 48.
    Fedorova, Dariya D.
    et al.
    Tomsk Polytech Univ, Tomsk 634050, Russia..
    Nazarova, Dariya S.
    Tomsk Polytech Univ, Tomsk 634050, Russia..
    Avetyan, David L.
    Tomsk Polytech Univ, Tomsk 634050, Russia.;Siberian State Med Univ, Tomsk 634050, Russia..
    Shatskiy, Andrey
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Organic chemistry. Tomsk Polytech Univ, Tomsk 634050, Russia..
    Belyanin, Maxim L.
    Tomsk Polytech Univ, Tomsk 634050, Russia..
    Kärkäs, Markus D.
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Organic chemistry.
    Stepanova, Elena, V
    Tomsk Polytech Univ, Tomsk 634050, Russia.;Russian Acad Sci, ND Zelinsky Inst Organ Chem, Moscow 119991, Russia..
    Divergent Synthesis of Natural Benzyl Salicylate and Benzyl Gentisate Glucosides2020In: Journal of Natural Products, ISSN 0163-3864, E-ISSN 1520-6025, Vol. 83, no 10, p. 3173-3180Article in journal (Refereed)
    Abstract [en]

    Herein is reported the first total synthesis of benzyl salicylate and benzyl gentisate glucosides present in various plant species, in particular the Salix genus, such as Populus balsamifera and P. trichocarpa. The method permits the synthesis of several natural phenolic acid derivatives and their glucosides starting from salicylic or gentisic acid. The divergent approach afforded access to three different acetylated glucosides from a common synthetic intermediate. The key step in the total synthesis of naturally occurring glycosides-the selective deacetylation of the sugar moiety-was achieved in the presence of a labile benzyl ester group by employing mild deacetylation conditions. The protocol permitted synthesis of trichocarpine (4 steps, 40% overall yield), isotrichocarpine (3 steps, 51% overall yield), trichoside (6 steps, 40% overall yield), and deoxytrichocarpine (3 steps, 42% overall yield) for the first time (>95% purity). Also, the optimized mild deacetylation conditions allowed synthesis of 2-O-acetylated derivatives of all four glycosides (5-17% overall yield, 90-95% purity), which are rare plant metabolites.

  • 49.
    Franchi, Daniele
    et al.
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Organic chemistry. KTH Royal Inst Technol, Dept Chem, SE-10044 Stockholm, Sweden.;Ist Chim Composti Organometall CNR ICCOM, Consiglio Nazl Ric, I-50019 Florence, Italy..
    Amara, Zacharias
    HESAM Univ, Equipe Chim Mol, Conserv Natl Arts & Metiers, Lab GBCM,EA7528, F-75003 Paris, France..
    Applications of Sensitized Semiconductors as Heterogeneous Visible-Light Photocatalysts in Organic Synthesis2020In: ACS Sustainable Chemistry and Engineering, E-ISSN 2168-0485, Vol. 8, no 41, p. 15405-15429Article in journal (Refereed)
    Abstract [en]

    The industrial transition to more-sustainable chemical manufacturing requires the development of a variety of high-performance heterogeneous catalysts. Recently, new classes of heterogeneous and recyclable catalysts that exploit visible-light activation have emerged in the field of organic synthesis. Among these systems, sensitized semiconductors occupy a strategic place as they are able to initiate single electron transfer processes under heterogeneous conditions and using medium-to-low energy light activation. This technology can promote a range of synthetically useful reactions, such as oxidations, reductions, or additions, including C-C bond formation, under very mild conditions and with high selectivity. Sensitized semiconductors have been known for decades in solar cell technologies (the so-called "Dye-Sensitized Solar Cells") but applications in organic synthesis are only very recent. This Review provides a comprehensive overview of the mechanisms, reactivity, and scope of this technology, with a focus on their new and promising synthetic applications.

  • 50.
    Franchi, Daniele
    et al.
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Organic chemistry. Univ Firenze, Dipartimento Chim Ugo Schiff, Via Lastruccia 13, I-50019 Sesto Fiorentino, Italy.;CNR Ist Chim Composti Organometall CNR ICCOM, Via Madonna Piano 10, I-50019 Sesto Fiorentino, Italy..
    Calamante, Massimo
    Univ Firenze, Dipartimento Chim Ugo Schiff, Via Lastruccia 13, I-50019 Sesto Fiorentino, Italy.;CNR Ist Chim Composti Organometall CNR ICCOM, Via Madonna Piano 10, I-50019 Sesto Fiorentino, Italy..
    Coppola, Carmen
    Univ Siena, R2ES Lab, Dipartimento Biotecnol Chim & Farm, Via A Moro 2, I-53100 Siena, Italy.;Consorzio Sviluppo Sistemi Grande Interfase, CSGI, Via Lastruccia 3, I-50019 Sesto Fiorentino, Italy..
    Mordini, Alessandro
    Univ Firenze, Dipartimento Chim Ugo Schiff, Via Lastruccia 13, I-50019 Sesto Fiorentino, Italy.;CNR Ist Chim Composti Organometall CNR ICCOM, Via Madonna Piano 10, I-50019 Sesto Fiorentino, Italy..
    Reginato, Gianna
    CNR Ist Chim Composti Organometall CNR ICCOM, Via Madonna Piano 10, I-50019 Sesto Fiorentino, Italy..
    Sinicropi, Adalgisa
    CNR Ist Chim Composti Organometall CNR ICCOM, Via Madonna Piano 10, I-50019 Sesto Fiorentino, Italy.;Univ Siena, R2ES Lab, Dipartimento Biotecnol Chim & Farm, Via A Moro 2, I-53100 Siena, Italy.;Consorzio Sviluppo Sistemi Grande Interfase, CSGI, Via Lastruccia 3, I-50019 Sesto Fiorentino, Italy..
    Zani, Lorenzo
    CNR Ist Chim Composti Organometall CNR ICCOM, Via Madonna Piano 10, I-50019 Sesto Fiorentino, Italy..
    Synthesis and Characterization of New Organic Dyes Containing the Indigo Core2020In: Molecules, ISSN 1431-5157, E-ISSN 1420-3049, Vol. 25, no 15, p. 3377-Article in journal (Refereed)
    Abstract [en]

    A new series of symmetrical organic dyes containing an indigo central core decorated with different electron donor groups have been prepared, starting from Tyrian Purple and using the Pd-catalyzed Stille-Migita coupling process. The effect of substituents on the spectroscopic properties of the dyes has been investigated theoretically and experimentally. In general, all dyes presented intense light absorption bands, both in the blue and red regions of the visible spectrum, conferring them a bright green color in solution. Using the same approach, an asymmetrically substituted D-A-pi-A green dye, bearing a triarylamine electron donor and the cyanoacrylate acceptor/anchoring group, has been synthesized for the first time and fully characterized, confirming that spectroscopic and electrochemical properties are consistent with a possible application in dye-sensitized solar cells (DSSC).

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