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  • 1. Agrell, J.
    et al.
    Birgersson, H.
    Boutonnet, Magali
    KTH, Superseded Departments, Chemical Engineering and Technology.
    Melian-Cabrera, I.
    Navarro, R. M.
    Fierro, J. L. G.
    Production of hydrogen from methanol over Cu/ZnO catalysts promoted by ZrO2 and Al2O32003In: Journal of Catalysis, ISSN 0021-9517, E-ISSN 1090-2694, Vol. 219, no 2, p. 389-403Article in journal (Refereed)
    Abstract [en]

    Production of H-2 from methanol by steam reforming, partial oxidation, or a combination thereof was studied over Cu/ZnO-based catalysts. The catalysts were characterized by a variety of techniques, including N2O chemisorption, X-ray photoelectron spectroscopy, X-ray diffraction, and temperature-programmed reduction/oxidation. The influence of feed composition, reaction temperature, and catalyst formulation on H-2 production rate, product distribution, and catalyst lifetime was investigated. Distinct differences between the processes were observed with respect to catalyst behavior. ZrO2-containing catalysts, especially Cu/ZnO/ZrO2/Al2O3, exhibit the best performance in the steam reforming reaction. During partial oxidation, however, a binary Cu/ZnO catalyst exhibits the lowest light-off temperature and the lowest level of CO by-product. The redox properties of the catalyst appear to play a key role in determining the pathway for H-2 production. In particular. the extent of methanol and/or H-2 combustion at differential O-2 conversion is strongly dependent on the ease of copper oxidation in the catalyst.

  • 2. Christoffersen, E.
    et al.
    Liu, P.
    Ruban, Andrei V.
    Skriver, H. L.
    Norskov, J. K.
    Anode materials for low-temperature fuel cells: A density functional theory study2001In: Journal of Catalysis, ISSN 0021-9517, E-ISSN 1090-2694, Vol. 199, no 1, p. 123-131Article in journal (Refereed)
    Abstract [en]

    Based on density functional calculations, we discuss the effect of alloying Pt with other metals for use as anode catalyst materials in low-temperature fuel cells. We discuss why a few parts per million of CO in the H-2 fuel can poison Pt surfaces and how this problem can be alleviated by alloying, and an extensive data base of the effect of alloying on the reactivity that includes all binary combinations of the transition metals to the right in the periodic table is given. We also discuss the effect of surface segregation and give a calculated data base of segregation energies of binary transition metal alloys. Based on extensive Monte Carlo simulations we show that while the adsorbate-free surface of a Ru0.5Pt0.5 alloy has no Ru in the first layer, the presence of CO can move some Ru to the surface, but all these Ru atoms are covered by CO.

  • 3. Fashandi, Hossein
    et al.
    Soldemo, Markus
    KTH, School of Information and Communication Technology (ICT), Materials- and Nano Physics, Material Physics, MF.
    Weissenrieder, Jonas
    KTH, School of Industrial Engineering and Management (ITM), Materials Science and Engineering.
    Gothelid, Mats
    KTH, School of Industrial Engineering and Management (ITM), Materials Science and Engineering, Materials Technology.
    Eriksson, Jens
    Eklund, Per
    Spetz, Anita Lloyd
    Andersson, Mike
    Applicability of MOS structures in monitoring catalytic properties, as exemplified for monolayer-iron-oxide-coated porous platinum films2016In: Journal of Catalysis, ISSN 0021-9517, E-ISSN 1090-2694, Vol. 344, p. 583-590Article in journal (Refereed)
    Abstract [en]

    Metal Oxide Semiconductor (MOS) capacitor devices comprised of monolayer iron oxide-coated as well as non-coated polycrystalline Pt deposited on oxidized silicon carbide substrates have been fabricated and their usefulness as realistic model systems in catalyst studies development was evaluated. The CO oxidation characteristics of both iron oxide- and non-coated Pt catalysts were investigated using mass spectrometry, monitoring the carbon dioxide production rate for different combinations of carbon monoxide (CO) and oxygen concentrations at various temperatures. Additionally, the output capacitance of the MOS model catalysts was recorded for each individual CO oxidation activity. A low-temperature shift in CO oxidation characteristics for the monolayer-coated compared to the non-coated Pt catalysts was observed, similar to that previously reported for monolayer iron oxide grown on single-crystalline Pt substrates. A strong correlation between the output capacitance of the MOS structures and the CO oxidation characteristics was found for both monolayer- and non-coated model catalysts. Furthermore, the devices exhibit retained MOS electrical output and CO oxidation characteristics as well as an unaffected catalyst surface composition, as confirmed by photoelectron spectroscopy, even after 200 h of continuous model catalyst operation. In addition to the implications on practical applicability of monolayer iron oxide coating on widely used polycrystalline Pt films in real-world catalysts and sensors, the findings also point to new possibilities regarding the use of MOS model systems for in situ characterization, high throughput screening, and tailoring of e.g. catalyst- and fuel-cell-electrode materials for specific applications.

  • 4.
    Janin, Emmanuelle
    et al.
    KTH, Superseded Departments, Microelectronics and Information Technology, IMIT.
    von Schenck, Hans
    KTH, Superseded Departments, Microelectronics and Information Technology, IMIT.
    Ringler, Sandrine
    KTH, Superseded Departments, Microelectronics and Information Technology, IMIT.
    Weissenrieder, Jonas
    KTH, Superseded Departments, Microelectronics and Information Technology, IMIT.
    Åkermark, Torbjörn
    KTH, Superseded Departments, Microelectronics and Information Technology, IMIT.
    Göthelid, Mats
    KTH, Superseded Departments, Microelectronics and Information Technology, IMIT.
    Adsorption and bonding of 2-butenal on Sn/Pt surface alloys2003In: Journal of Catalysis, ISSN 0021-9517, E-ISSN 1090-2694, Vol. 215, no 2, p. 245-253Article in journal (Refereed)
    Abstract [en]

    The adsorption of 2-butenal on the Pt(111), Pt(111)Sn-(2 x 2), and Pt(111)Sn-(root3 x root3)R30degrees surfaces has been studied by high-resolution photoelectron spectroscopy and DFT calculations. On Pt(111) 2-butenal adsorbs at a threefold hollow in a eta(3)(C,C,O) configuration. A similar geometry is observed for Pt(111)Sn-(2 x 2), although the oxygen coordinates to tin instead of platinum. As the surface coverage of tin increases, as for Pt(111)Sn-(root3 x root3)R30degrees, the most stable adsorption geometry changes to eta(1)(O), where the carbonyl oxygen once again coordinates to tin. The carbonyl bond thus retains an activated character as Pt/Sn alloys are formed. The alkene/surface interaction is, however, dramatically influenced at increasing surface concentrations of tin.

  • 5.
    Jiang, Xue
    et al.
    KTH, School of Industrial Engineering and Management (ITM), Materials Science and Engineering, Applied Material Physics.
    Nisar, Jawad
    Pathak, Biswarup
    Zhao, Jijun
    Ahuja, Rajeev
    KTH, School of Industrial Engineering and Management (ITM), Materials Science and Engineering, Applied Material Physics.
    Graphene oxide as a chemically tunable 2-D material for visible-light photocatalyst applications2013In: Journal of Catalysis, ISSN 0021-9517, E-ISSN 1090-2694, Vol. 299, p. 204-209Article in journal (Refereed)
    Abstract [en]

    To elucidate the usage of graphene oxide (GO) as a photocatalysis material, we have studied the effect of epoxy and hydroxyl functionalization on the electronic structure, work function, CBM/VBM position, and optical absorption spectra of GO using density functional theory calculations. By varying the coverage and relative ratio of the surface epoxy (-O-) and hydroxyl (-OH) groups, both band gap and work function of the GO materials can be tuned to meet the requirement of photocatalyst. Interestingly, the electronic structures of GO materials with 40-50% (33-67%) coverage and OH:O ratio of 2:1(1:1) are suitable for both reduction and oxidation reactions for water splitting. Among of these systems, the GO composition with 50% coverage and OH:O (1:1) ratio can be very promising materials for visible-light-driven photocatalyst. Our results not only explain the recent experimental observations about 2-D graphene oxide as promising visible-light-driven photocatalyst materials but can also be very helpful in designing the optimal composition for higher performance.

  • 6.
    Lögdberg, Sara
    et al.
    KTH, School of Chemical Science and Engineering (CHE), Chemical Engineering and Technology, Chemical Technology.
    Lualdi, Matteo
    KTH, School of Chemical Science and Engineering (CHE), Chemical Engineering and Technology, Chemical Technology.
    Järås, Sven
    KTH, School of Chemical Science and Engineering (CHE), Chemical Engineering and Technology, Chemical Technology.
    Walmsley, John C.
    Blekkan, Edd A.
    Rytter, Erling
    Holmen, Anders
    On the selectivity of cobalt-based Fischer-Tropsch catalysts: Evidence for a common precursor for methane and long-chain hydrocarbons2010In: Journal of Catalysis, ISSN 0021-9517, E-ISSN 1090-2694, Vol. 274, no 1, p. 84-98Article in journal (Refereed)
    Abstract [en]

    A total of 36 cobalt-based supported catalysts were investigated in the Fischer-Tropsch reaction at industrially relevant process conditions: 483 K, 20 bar, molar H-2/CO ratio = 2.1, pellet size: 53-90 mu m. The effect of adding water vapour to the feed was investigated for 20 of the catalysts, and a H-2/CO ratio of 1.0 was used for a few catalysts. The catalysts differed in support material, Co loading, promoters, Cl content, Co particle size (larger than similar to 6 nm), morphology, degree of reduction and preparation technique and showed a large variation in selectivity. For each set of process conditions, a linear relationship seems to exist between the selectivity to methane (and other light products) and C5+ indicating a common precursor, i.e. a common monomer pool, for all hydrocarbon products. A high selectivity to C5+ is mainly an effect of a high intrinsic chain-growth probability and unlikely to be a result of an enhanced cc-olefin readsorption. The universal effect of external water addition on the hydrocarbon selectivities is limited to a decrease in the methane selectivity. A small proportion of the catalysts developed "pure methanation" sites upon exposure to high partial pressures of water.

  • 7.
    Lögdberg, Sara
    et al.
    KTH, School of Chemical Science and Engineering (CHE), Chemical Engineering and Technology, Chemical Technology.
    Yang, J.
    Lualdi, Matteo
    KTH, School of Chemical Science and Engineering (CHE), Chemical Engineering and Technology, Chemical Technology.
    Walmsley, J. C.
    Järås, Sven
    KTH, School of Chemical Science and Engineering (CHE), Chemical Engineering and Technology, Chemical Technology.
    Boutonnet, Magali
    KTH, School of Chemical Science and Engineering (CHE), Chemical Engineering and Technology, Chemical Technology.
    Blekkan, E. A.
    Rytter, E.
    Holmen, A.
    Further insights into methane and higher hydrocarbons formation over cobalt-based catalysts with γ-Al2O3, α-Al2O3 and TiO2 as support materials2017In: Journal of Catalysis, ISSN 0021-9517, E-ISSN 1090-2694, Vol. 352, p. 515-531Article in journal (Refereed)
    Abstract [en]

    A range of cobalt-based catalysts varying in Co loading and prepared by incipient wetness impregnation of traditional support materials (γ-Al2O3, α-Al2O3 and TiO2), have been studied in the Fischer-Tropsch reaction at industrially relevant process conditions (483 K, 20 bar, H2/CO = 2.1). A high selectivity to C5+ hydrocarbons (SC5+) is to a great extent connected with a high site activity, but not exclusively. We propose that the ratio of monomer-production rate to C–C coupling rate of a catalyst determines chain-growth probability by means of governing the coverage of the monomer on the cobalt surface. We speculate that this ratio depends on e.g. shape, strain and size of the Co crystallites and, therefore, is highly dependent on the choice of support material. No general relationship between Co particle size and SC5+ is found, but individual correlations exist for each support material. Within each support material, there are indications of negative correlations between the chain-growth probability of the C1 ∗ surface intermediate (αC1) and the higher αCn values. This can be rationalized by assuming that the majority of methane is formed by a different mechanism, separate from chain growth, but connected with chain growth through a common carbon pool. We propose that the monomers and the majority of methane are produced at sites different from the ones involved in chain growth. There is no general correlation between αC1 and SC5+ for catalysts with different support materials, possibly due to small differences in cobalt surface coverage of hydrogen. For the TiO2-supported catalysts, a dramatically increased αC1 value observed for catalysts with Co particles smaller than approx. 15 nm, is probably associated with strong metal-support interactions (SMSI). This phenomenon apparently limits the effect (reduction) on the SC5+ when moving toward smaller Co particles.

  • 8.
    Persson, Katarina
    et al.
    KTH, School of Chemical Science and Engineering (CHE), Chemical Engineering and Technology.
    Ersson, Anders
    KTH, School of Chemical Science and Engineering (CHE), Chemical Engineering and Technology.
    Jansson, K.
    Iverlund, N
    Järås, Sven
    KTH, School of Chemical Science and Engineering (CHE), Chemical Engineering and Technology.
    Influence of co-metals on bimetallic palladium catalysts for methane combustion2005In: Journal of Catalysis, ISSN 0021-9517, E-ISSN 1090-2694, Vol. 231, p. 139-150Article in journal (Refereed)
    Abstract [en]

    The catalytic combustion of methane has been investigated over eight different bimetallic palladium catalysts, comprising the co-metals Co, Rh, Ir, Ni, Pt, Cu, Ag, or An. The catalysts were characterized by TEM, EDS, PXRD, and temperature-programmed oxidation (TPO). It was found that a catalyst containing both Pd and Pt was the most promising, as it had a high activity that did not decline with time. The catalyst containing Pd and Ag was also a promising candidate, but its activity was slightly lower. For PdCo and PdNi, the co-metals formed spinel structures with the alumina support, with the result that the co-metals did not affect the combustion performance of palladium. For PdRh, PdIr, PdCu, and PdAg, the co-metals formed separate particles consisting of the corresponding metal oxide. These catalysts, except PdRh, showed a stable activity. For PdPt and PdAu, the co-metals formed alloys with palladium, and both catalysts showed a stable activity.

  • 9.
    Persson, Katarina
    et al.
    KTH, School of Chemical Science and Engineering (CHE), Chemical Engineering and Technology.
    Jansson, Kjell
    Järås, Sven G.
    KTH, School of Chemical Science and Engineering (CHE), Chemical Engineering and Technology.
    Characterisation and microstructure of Pd and bimetallic Pd-Pt catalysts duirng methane oxidation2007In: Journal of Catalysis, ISSN 0021-9517, E-ISSN 1090-2694, Vol. 245, no 2, p. 401-414Article in journal (Refereed)
    Abstract [en]

    The catalytic oxidation of methane was studied over Pd/Al2O3 and Pd-Pt/Al2O3. It was found that the activity of Pd/Al2O3 gradually decreases with time at temperatures well below that of PdO decomposition. The opposite was observed for Pd-Pt/Al2O3, of which the activity decreases slightly with time. Morphological studies of the two catalysts showed major changes during operation. The palladium particles in Pd/Al2O3 are initially composed of smaller, randomly oriented crystals of both PdO and Pd. In oxidising atmospheres, the crystals become more oxidised and form larger crystals. The activity increase of Pd-PuAl2O3 is probably related to more PdO being formed during operation. The particles in Pd-Pt/Al2O3 are split into two different domains: one with PdO and the other likely consisting of an alloy between Pd and Pt. The alloy is initially rich in palladium, but the composition changes to a more equalmolar Pd-Pt structure during operation. The ejected Pd is oxidised into PdO, which is more active than its metallic phase. The amount of PdO formed depends on the oxidation time and temperature.

  • 10. Thevenin, P. O.
    et al.
    Alcalde, A.
    Pettersson, Lars J.
    KTH, Superseded Departments, Chemical Engineering and Technology.
    Järås, Sven G.
    KTH, Superseded Departments, Chemical Engineering and Technology.
    Fierro, J. L. G.
    Catalytic combustion of methane over cerium-doped palladium catalysts2003In: Journal of Catalysis, ISSN 0021-9517, E-ISSN 1090-2694, Vol. 215, no 1, p. 78-86Article in journal (Refereed)
    Abstract [en]

    Various Pd-supported catalysts have been prepared using three different types of alumina as support material: (a) gamma-alumina, (b) Ba-stabilized alumina, and

  • 11. Thevenin, P. O.
    et al.
    Pocoroba, E.
    Pettersson, Lars J.
    KTH, Superseded Departments, Chemical Engineering and Technology.
    Karhu, H.
    Vayrynen, I. J.
    Järås, Sven G.
    KTH, Superseded Departments, Chemical Engineering and Technology.
    Characterization and activity of supported palladium combustion catalysts2002In: Journal of Catalysis, ISSN 0021-9517, E-ISSN 1090-2694, Vol. 207, no 1, p. 139-149Article in journal (Refereed)
    Abstract [en]

    The catalytic activity of Pd supported on gamma-Al2O3, Ba-Al2O3, and La-Al2O3 has been examined in complete oxidation of methane when operating in excess of oxygen. Two different sizes of I'd particles have been considered. Foreign ions have a strong influence with respect to the stabilization of alumina when submitted to a temperature as high as 1000 degrees C. In contrast, no specific effect can be detected when the samples are calcined at 500 degreesC. Interaction with the supported palladium particles, observed during the combustion reaction, has been investigated by X-ray photoelectron Spectroscopy and temperature-programmed oxidation. The difference in combustion activity is attributed to the difference in surface oxidation states of the Pd particles. The presence of foreign ions in the alumina structure results in surface PdO only. When supported on gamma-Al2O3, small amounts of metallic Pd can be detected, resulting in a lower ignition temperature.

  • 12. Wang, D. P.
    et al.
    Wang, M.
    Wang, X. N.
    Chen, Y. G.
    Gao, A. P.
    Sun, Licheng C.
    Asymmetric epoxidation of styrene and chromenes catalysed by chiral (salen)Mn(III) complexes with a pyrrolidine backbone2006In: Journal of Catalysis, ISSN 0021-9517, E-ISSN 1090-2694, Vol. 237, no 2, p. 248-254Article in journal (Refereed)
    Abstract [en]

    A series of chiral (pyrrolidine salen)Mn(III) complexes were synthesized front N-aza-substituted (R,R)-N,N'-bis(3,5-di-tert-butylsalicylidene)-3.4-diaminopyrrolidine salen ligands. High yields and comparable enantioselectivity relative to Jacobsen's catalyst were achieved in asymmetric epoxidation of styrene and chromenes using NaClO/PPNO and m-CPBA/NMO as the oxidant systems. Complexes 1-3, featuring a tertiary airline unit, displayed higher activity than complex 4, bearing ail amide unit and Jacobsen's catalyst in the NaClO/PPNO aqueous/organic biphasic system. The influence of CH3I on epoxidation of 6-nitro-2,2-dimethylchromene catalysed by 1-4 in the biphasic medium was Studied to explore the catalysts with built-in phase-transfer capability. The alkenes' access pathway is discussed on the basis of the steric effect of the N-aza-substituent in the pyrrolidine backbone of complexes 1-3 on the enantioselectivity of epoxidation.

  • 13.
    Wang, Lei
    et al.
    KTH, School of Chemical Science and Engineering (CHE), Chemistry.
    Duan, Lele
    KTH, School of Chemical Science and Engineering (CHE), Chemistry.
    Tong, Lianpeng
    KTH, School of Chemical Science and Engineering (CHE), Chemistry.
    Sun, Licheng
    KTH, School of Chemical Science and Engineering (CHE), Chemistry, Organic Chemistry.
    Visible light-driven water oxidation catalyzed by mononuclear ruthenium complexes2013In: Journal of Catalysis, ISSN 0021-9517, E-ISSN 1090-2694, Vol. 306, p. 129-132Article in journal (Refereed)
    Abstract [en]

    A series of mononuclear ruthenium water oxidation catalysts (WOCs) [Ru(bda)L-2] (H(2)bda = 2,2'-bipyridine-6,6'-dicarboxylic acid; L = N-cyclic aromatic ligands) were investigated in three-component light-driven water oxidation systems composed of photosensitizers, a sacrificial electron acceptor, and WOCs. A high turnover number of 579 for water oxidation was achieved in the homogeneous system using complex 4 ([Ru(bda)(4-Br-pyridine)(2)]) as the WOC, and a high quantum efficiency of 17% was found which is a new record for visible light-driven water oxidation in homogeneous systems.

  • 14. Wang, M.
    et al.
    Zhu, H. J.
    Jin, K.
    Dai, D.
    Sun, Licheng C.
    Ethylene oligomerization by salen-type zirconium complexes to low-carbon linear alpha-oletins2003In: Journal of Catalysis, ISSN 0021-9517, E-ISSN 1090-2694, Vol. 220, no 2, p. 392-398Article in journal (Refereed)
    Abstract [en]

    A series of zirconium salen-type complexes were prepared by using ZrCl4 and sodium salts of the tetradentate Schiff base ligands. In combination with Et2AlCl, they displayed moderate to high catalytic activities in ethylene oligomerization under a pressure of 1.0-1.8 MPa at 150 degreesC in toluene. The main products are C-4-C-10 olefins with good selectivity to linear alpha-olefins. The turnover frequency (TOF) of catalyst system Zr(salen)Cl-2 (.) THF/Et2AlCl, under a pressure of 1.8 MPa and in an Al/Zr molar ratio of 300, was 4.93 x 10(4) h(-1) with a satisfactory selectivity to C-4-C-10 olefins (89%), and linear alpha-olefins accounted for 95%. The steric and conjugate effects of the ligands on ethylene oligomerization, as well as the effects of cocatalysts, the Al/Zr molar ratios, the reaction temperature, the ethylene pressure, and the lifetime of the catalysts were studied.

  • 15. Wang, Ying
    et al.
    Wang, Mei
    Wang, Yu
    Wang, Xiuna
    Wang, Lin
    Sun, Licheng
    KTH, School of Chemical Science and Engineering (CHE), Chemistry, Organic Chemistry.
    Highly enantioselective sulfoxidation with vanadium catalysts of Schiff bases derived from bromo- and iodo-functionalized hydroxynaphthaldehydes2010In: Journal of Catalysis, ISSN 0021-9517, E-ISSN 1090-2694, Vol. 273, no 2, p. 177-181Article in journal (Refereed)
    Abstract [en]

    Two series of chiral Schiff bases, 4a-e and 5a-e, prepared from the condensation of the mono-, di-, trib-romohydroxynaphthaldehyde or monoiodohydroxynaphthaldehyde with chiral amino alcohols, were used in combination with VO(acac)(2) for the asymmetric oxidation of aryl methyl sulfides using H2O2 as terminal oxidant. Among these Schiff bases, dibromo-functionalized 4d and iodo-functionalized 5e gave high yields (91-93%) with good enantioselectivities (80-82% ee) for the oxidation of thioanisole in dichloromethane. The asymmetric oxidation of thioanisole in toluene using these Schiff bases gave methyl phenyl sulfoxide in satisfactory isolated yields (48-62%) with high enantioselectivities (91-94% ee), which were further improved by a modified procedure with the ee value up to 98% in 62% yield. The oxidations of other aryl methyl sulfides in toluene with dibromo- and iodo-functionalized Schiff bases 5d and 5e as ligands using the modified procedure afforded the corresponding sulfoxides in 55-67% isolated yields with 95-99% ee. (C) 2010 Elsevier Inc. All rights reserved.

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