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Publications (10 of 11) Show all publications
Chen, T., Banda, H., Yang, L., Li, J., Zhang, Y., Parenti, R. & Dincă, M. (2023). High-rate, high-capacity electrochemical energy storage in hydrogen-bonded fused aromatics. Joule, 7(5), 986-1002
Open this publication in new window or tab >>High-rate, high-capacity electrochemical energy storage in hydrogen-bonded fused aromatics
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2023 (English)In: Joule, E-ISSN 2542-4351, Vol. 7, no 5, p. 986-1002Article in journal (Refereed) Published
Abstract [en]

Designing materials for electrochemical energy storage with short charging times and high charge capacities is a longstanding challenge. The fundamental difficulty lies in incorporating a high density of redox couples into a stable material that can efficiently conduct both ions and electrons. We report all-organic, fused aromatic materials that store up to 310 mAh g−1 and charge in as little as 33 s. This performance stems from abundant quinone/imine functionalities that decorate an extended aromatic backbone, act as redox-active sites, engage in hydrogen bonding, and enable a delocalized high-rate energy storage with stability upon cycling. The extended conjugation and hydrogen-bonding-assisted bulk charge storage contrast with the surface-confined or hydration-dependent behavior of traditional inorganic electrodes.

Place, publisher, year, edition, pages
Elsevier BV, 2023
Keywords
energy storage, intercalation, organic electrodes, pseudocapacitance, supercapacitors
National Category
Inorganic Chemistry Renewable Bioenergy Research
Identifiers
urn:nbn:se:kth:diva-331685 (URN)10.1016/j.joule.2023.03.011 (DOI)001137001100001 ()2-s2.0-85153908738 (Scopus ID)
Note

QC 20230713

Available from: 2023-07-13 Created: 2023-07-13 Last updated: 2024-02-06Bibliographically approved
Huang, X., Fu, S., Lin, C., Lu, Y., Wang, M., Zhang, P., . . . Dong, R. (2023). Semiconducting Conjugated Coordination Polymer with High Charge Mobility Enabled by "4+2" Phenyl Ligands. Journal of the American Chemical Society, 145(4), 2430-2438
Open this publication in new window or tab >>Semiconducting Conjugated Coordination Polymer with High Charge Mobility Enabled by "4+2" Phenyl Ligands
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2023 (English)In: Journal of the American Chemical Society, ISSN 0002-7863, E-ISSN 1520-5126, Vol. 145, no 4, p. 2430-2438Article in journal (Refereed) Published
Abstract [en]

Electrically conductive coordination polymers and metal-organic frameworks are attractive emerging electroactive materials for (opto-)electronics. However, developing semiconducting coordination polymers with high charge carrier mobility for devices remains a major challenge, urgently requiring the rational design of ligands and topological networks with desired electronic structures. Herein, we demonstrate a strategy for synthesizing high-mobility semiconducting conjugated coordination polymers (c-CPs) utilizing novel conjugated ligands with D2h symmetry, namely, "4 + 2" phenyl ligands. Compared with the conventional phenyl ligands with C6h symmetry, the reduced symmetry of the "4 + 2" ligands leads to anisotropic coordination in the formation of c-CPs. Consequently, we successfully achieve a single-crystalline three-dimensional (3D) c-CP Cu4DHTTB (DHTTB = 2,5-dihydroxy-1,3,4,6-tetrathiolbenzene), containing orthogonal ribbon-like pi-d conjugated chains rather than 2D conjugated layers. DFT calculation suggests that the resulting Cu4DHTTB exhibits a small band gap (similar to 0.2 eV), strongly dispersive energy bands near the Fermi level with a low electron-hole reduced effective mass (similar to 0.2m0*). Furthermore, the four-probe method reveals a semiconducting behavior with a decent conductivity of 0.2 S/cm. Thermopower measurement suggests that it is a p-type semiconductor. Ultrafast terahertz photoconductivity measurements confirm Cu4DHTTB's semiconducting nature and demonstrate the Drude-type transport with high charge carrier mobilities up to 88 +/- 15 cm2 V-1 s-1, outperforming the conductive 3D coordination polymers reported till date. This molecular design strategy for constructing high-mobility semiconducting c-CPs lays the foundation for achieving high-performance c-CP-based (opto-)electronics.

Place, publisher, year, edition, pages
AMER CHEMICAL SOC, 2023
National Category
Materials Chemistry
Identifiers
urn:nbn:se:kth:diva-324461 (URN)10.1021/jacs.2c11511 (DOI)000927671300001 ()36661343 (PubMedID)2-s2.0-85146912753 (Scopus ID)
Note

QC 20230315

Available from: 2023-03-15 Created: 2023-03-15 Last updated: 2023-06-08Bibliographically approved
Subramaniyam, C. M., Kang, M., Li, J., Mohammadi, A. V. & Hamedi, M. (2022). Additive-free red phosphorus/Ti3C2TxMXene nanocomposite anodes for metal-ion batteries. Energy Advances (12), 999-1008
Open this publication in new window or tab >>Additive-free red phosphorus/Ti3C2TxMXene nanocomposite anodes for metal-ion batteries
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2022 (English)In: Energy Advances, E-ISSN 2753-1457, no 12, p. 999-1008Article in journal (Refereed) Published
Abstract [en]

Herein, we report on scalable, environmentally benign, and additive-free, high-performance anodes for alkali-metal-ion batteries (MIBs, where M = Li+, Na+, K+). The intercalators in these anodes are the red phosphorus (RP) nanoparticles of uniform size (~40 nm), which are dispersible and blend with water-dispersed Ti3C2Tx MXene, forming a highly viscous aqueous slurry to fabricate additive-free nanocomposite electrodes. We further enhanced their performance using a very low weight percentage of various carbonaceous nanomaterials. Our RP-MWCNT/MXene nanocomposite anodes exhibited enhanced ion transport and low charge transfer resistance, delivering specific capacities of 1293.7 mA h g-1 at 500 mA g-1 and 263.3 mA h g-1 at 2600 mA g-1 for 10 000 cycles in Li+ cells, 371.6 mA h g-1 at 500 mA g-1 in Na+ cells, and 732.8 mA h g-1 at 50 mA g-1 in K+ cells. Our work shows a path towards fabricating nanoarchitectured electrodes using sustainable materials to eliminate inert polymer binders, toxic processing solvents, and rare earth elements from the battery fabrication process for next-generation alkali-metal-ion batteries.

Place, publisher, year, edition, pages
Royal Society of Chemistry (RSC), 2022
National Category
Materials Chemistry
Identifiers
urn:nbn:se:kth:diva-330971 (URN)10.1039/d2ya00168c (DOI)001105927300001 ()2-s2.0-85151304605 (Scopus ID)
Note

QC 20230705

Available from: 2023-07-05 Created: 2023-07-05 Last updated: 2023-12-11Bibliographically approved
Li, J., Lin, C., Ma, T. & Sun, J. (2022). Atomic-resolution structures from polycrystalline covalent organic frameworks with enhanced cryo-cRED. Nature Communications, 13(1), Article ID 4016.
Open this publication in new window or tab >>Atomic-resolution structures from polycrystalline covalent organic frameworks with enhanced cryo-cRED
2022 (English)In: Nature Communications, E-ISSN 2041-1723, Vol. 13, no 1, article id 4016Article in journal (Refereed) Published
Abstract [en]

The pursuit of atomic precision structure of porous covalent organic frameworks (COFs) is the key to understanding the relationship between structures and properties, and further developing new materials with superior performance. Yet, a challenge of how to determine their atomic structures has always existed since the first COFs reported seventeen years ago. Here, we present a universal method for ab initio structure determination of polycrystalline three-dimensional (3D) COFs at atomic level using enhanced cryo-continuous rotation electron diffraction (cryo-cRED), which combines hierarchical cluster analysis with cryo-EM technique. The high-quality datasets possess not only up to 0.79-angstrom resolution but more than 90% completeness, leading to unambiguous solution and precise refinement with anisotropic temperature factors. With such a powerful method, the dynamic structures with flexible linkers, degree of interpenetration, position of functional groups, and arrangement of ordered guest molecules are successfully revealed with atomic precision in five 3D COFs, which are almost impossible to be obtained without atomic resolution structure solution. This study demonstrates a practicable strategy for determining the structures of polycrystalline COFs and other beam-sensitive materials and to help in the future discovery of novel materials on the other.

Place, publisher, year, edition, pages
Springer Nature, 2022
National Category
Environmental Sciences
Identifiers
urn:nbn:se:kth:diva-316846 (URN)10.1038/s41467-022-31524-9 (DOI)35821216 (PubMedID)2-s2.0-85133946832 (Scopus ID)
Note

QC 20220901

Available from: 2022-09-01 Created: 2022-09-01 Last updated: 2023-03-28Bibliographically approved
Chen, T., Dou, J.-H., Yang, L., Sun, C., Oppenheim, J. J., Li, J. & Dinca, M. (2022). Dimensionality Modulates Electrical Conductivity in Compositionally Constant One-, Two-, and Three-Dimensional Frameworks. Journal of the American Chemical Society, 144(12), 5583-5593
Open this publication in new window or tab >>Dimensionality Modulates Electrical Conductivity in Compositionally Constant One-, Two-, and Three-Dimensional Frameworks
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2022 (English)In: Journal of the American Chemical Society, ISSN 0002-7863, E-ISSN 1520-5126, Vol. 144, no 12, p. 5583-5593Article in journal (Refereed) Published
Abstract [en]

We reveal here the construction of Ni-based metal-organic frameworks (MOFs) and conjugated coordination polymers (CCPs) with different structural dimensionalities, including closely pi-stacked 1D chains (Ni-1D), aggregated 2D layers (Ni-2D), and a 3D framework (Ni-3D), based on 2,3,5,6-tetraamino-1,4-hydroquinone (TAHQ) and its various oxidized forms. These materials have the same metal-ligand composition but exhibit distinct electronic properties caused by different dimensionalities and supramolecular interactions between SBUs, ligands, and structural motifs. The electrical conductivity of these materials spans nearly 8 orders of magnitude, approaching 0.3 S/cm.

Place, publisher, year, edition, pages
American Chemical Society (ACS), 2022
National Category
Materials Chemistry
Identifiers
urn:nbn:se:kth:diva-313502 (URN)10.1021/jacs.2c00614 (DOI)000799109400046 ()35290048 (PubMedID)2-s2.0-85127122662 (Scopus ID)
Note

QC 20220607

Available from: 2022-06-07 Created: 2022-06-07 Last updated: 2022-06-25Bibliographically approved
Cui, Y., Subramaniyam, C. M., Li, L., Han, T., Kang, M., Li, J., . . . Hamedi, M. (2022). Hierarchical soot nanoparticle self-assemblies for enhanced performance as sodium-ion battery anodes. Journal of Materials Chemistry A, 10(16), 9059-9066
Open this publication in new window or tab >>Hierarchical soot nanoparticle self-assemblies for enhanced performance as sodium-ion battery anodes
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2022 (English)In: Journal of Materials Chemistry A, ISSN 2050-7488, E-ISSN 2050-7496, Vol. 10, no 16, p. 9059-9066Article in journal (Refereed) Published
Abstract [en]

The drawbacks of amorphous hard carbon are its low conductivity and structural instability, due to its large volume change and the occurrence of side reactions with the electrolyte during cycling. Here, we propose a simple and rapid method to address these disadvantages; we used an emulsion solvent-evaporation method to create hierarchically structured microparticles of hard carbon nanoparticles, derived from soot, and multi-walled-carbon-nanotubes at a very low threshold of 2.8 wt%. These shrub-ball like microparticles have well-defined void spaces between different nanostructures of carbon, leading to an increased surface area, lower charge-resistance and side reactions, and higher electronic conductivity for Na+ insertion and de-insertion. They can be slurry cast to assemble Na+ anodes, exhibiting an initial discharge capacity of 713.3 mA h g(-1) and showing long-term stability with 120.8 mA h g(-1) at 500 mA g(-1) after 500 cycles, thus outperforming neat hard carbon nanoparticles by an order of magnitude. Our work shows that hierarchical self-assembly is attractive for increasing the performance of microparticles used for battery production.

Place, publisher, year, edition, pages
Royal Society of Chemistry (RSC), 2022
National Category
Materials Chemistry
Identifiers
urn:nbn:se:kth:diva-311641 (URN)10.1039/d1ta10889a (DOI)000780328500001 ()2-s2.0-85127876353 (Scopus ID)
Note

QC 20220502

Available from: 2022-05-02 Created: 2022-05-02 Last updated: 2022-11-29Bibliographically approved
Sun, L., Yang, L., Dou, J.-H. -., Li, J., Skorupskii, G., Mardini, M., . . . Rajh, T. (2022). Room-Temperature Quantitative Quantum Sensing of Lithium Ions with a Radical-Embedded Metal-Organic Framework. Journal of the American Chemical Society, 144(41), 19008-19016
Open this publication in new window or tab >>Room-Temperature Quantitative Quantum Sensing of Lithium Ions with a Radical-Embedded Metal-Organic Framework
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2022 (English)In: Journal of the American Chemical Society, ISSN 0002-7863, E-ISSN 1520-5126, Vol. 144, no 41, p. 19008-19016Article in journal (Refereed) Published
Abstract [en]

Recent advancements in quantum sensing have sparked transformative detection technologies with high sensitivity, precision, and spatial resolution. Owing to their atomic-level tunability, molecular qubits and ensembles thereof are promising candidates for sensing chemical analytes. Here, we show quantum sensing of lithium ions in solution at room temperature with an ensemble of organic radicals integrated in a microporous metal-organic framework (MOF). The organic radicals exhibit electron spin coherence and microwave addressability at room temperature, thus behaving as qubits. The high surface area of the MOF promotes accessibility of the guest analytes to the organic qubits, enabling unambiguous identification of lithium ions and quantitative measurement of their concentration through relaxometric and hyperfine spectroscopic methods based on electron paramagnetic resonance (EPR) spectroscopy. The sensing principle presented in this work is applicable to other metal ions with nonzero nuclear spin.

Place, publisher, year, edition, pages
American Chemical Society (ACS), 2022
Keywords
Electron spin resonance spectroscopy, Lithium, Magnetic moments, Metal ions, Metal-Organic Frameworks, Paramagnetic resonance, Qubits, Room temperature, Spectroscopic analysis, Spin dynamics, Analytes, Atomic levels, Detection technology, Embedded metals, High sensitivity, Lithium ions, Metalorganic frameworks (MOFs), Organic radicals, Spatial resolution, Tunabilities, Electrospinning, lithium ion, metal organic framework, adsorption, Article, chemical structure, concentration (parameter), electron spin resonance, reaction analysis, surface area, synthesis
National Category
Physical Chemistry
Identifiers
urn:nbn:se:kth:diva-328113 (URN)10.1021/jacs.2c07692 (DOI)000875645600001 ()36201712 (PubMedID)2-s2.0-85139474720 (Scopus ID)
Note

QC 20230602

Available from: 2023-06-02 Created: 2023-06-02 Last updated: 2023-06-02Bibliographically approved
Lu, Y., Zhong, H., Li, J., Dominic, A. M., Hu, Y., Gao, Z., . . . Dong, R. (2022). sp-Carbon Incorporated Conductive Metal-Organic Framework as Photocathode for Photoelectrochemical Hydrogen Generation. Angewandte Chemie International Edition, 61(39)
Open this publication in new window or tab >>sp-Carbon Incorporated Conductive Metal-Organic Framework as Photocathode for Photoelectrochemical Hydrogen Generation
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2022 (English)In: Angewandte Chemie International Edition, ISSN 1433-7851, E-ISSN 1521-3773, Vol. 61, no 39Article in journal (Refereed) Published
Abstract [en]

Metal-organic frameworks (MOFs) have attracted increasing interest for broad applications in catalysis and gas separation due to their high porosity. However, the insulating feature and the limited active sites hindered MOFs as photocathode active materials for application in photoelectrocatalytic hydrogen generation. Herein, we develop a layered conductive two-dimensional conjugated MOF (2D c-MOF) comprising sp-carbon active sites based on arylene-ethynylene macrocycle ligand via CuO4 linking, named as Cu3HHAE2. This sp-carbon 2D c-MOF displays apparent semiconducting behavior and broad light absorption till the near-infrared band (1600 nm). Due to the abundant acetylene units, the Cu3HHAE2 could act as the first case of MOF photocathode for photoelectrochemical (PEC) hydrogen generation and presents a record hydrogen-evolution photocurrent density of ≈260 μA cm−2 at 0 V vs. reversible hydrogen electrode among the structurally-defined cocatalyst-free organic photocathodes.

Place, publisher, year, edition, pages
Wiley, 2022
Keywords
Conductive 2D MOFs, Hydrogen Generation, Photocathode, Photoelectrocatalysis, sp-Carbon
National Category
Chemical Sciences
Identifiers
urn:nbn:se:kth:diva-335781 (URN)10.1002/anie.202208163 (DOI)000843769900001 ()35903982 (PubMedID)2-s2.0-85136518312 (Scopus ID)
Note

QC 20230908

Available from: 2023-09-08 Created: 2023-09-08 Last updated: 2023-09-08Bibliographically approved
Lin, Q.-F., Gao, Z. R., Lin, C., Zhang, S., Chen, J., Li, Z., . . . Chen, F.-J. (2021). A stable aluminosilicate zeolite with intersecting three-dimensional extra-large pores. Science, 374(6575), 1605-1608
Open this publication in new window or tab >>A stable aluminosilicate zeolite with intersecting three-dimensional extra-large pores
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2021 (English)In: Science, ISSN 0036-8075, E-ISSN 1095-9203, Vol. 374, no 6575, p. 1605-1608Article in journal (Refereed) Published
Abstract [en]

Zeolites are crystalline porous materials with important industrial applications, including uses in catalytic and adsorption-separation processes. Access into and out of their inner confined space, where adsorption and reactions occur, is limited by their pore apertures. Stable multidimensional zeolites with larger pores able to process larger molecules are in demand in the fine chemical industry and for the oil processing on which the world still relies for fuels. Currently known extra-large-pore zeolites display poor stability and/or lack pore multidimensionality, limiting their usefulness. We report ZEO-1, a robust, fully connected aluminosilicate zeolite with mutually intersecting three-dimensional extra-large plus three-dimensional large pores. ZEO-1 is stable up to 1000 degrees C, has an extraordinary specific surface area (1000 square meters per gram), and shows potential as a catalytic cracking catalyst.

Place, publisher, year, edition, pages
American Association for the Advancement of Science (AAAS), 2021
National Category
Inorganic Chemistry
Identifiers
urn:nbn:se:kth:diva-308670 (URN)10.1126/science.abk3258 (DOI)000736589300031 ()34941401 (PubMedID)2-s2.0-85122906841 (Scopus ID)
Note

QC 20220215

Available from: 2022-02-15 Created: 2022-02-15 Last updated: 2022-06-25Bibliographically approved
Villaescusa, L. A., Li, J., Mayoral, A., Gao, Z. R. & Camblor, M. A. (2021). Sandwich-Type Zeolite Intergrowths with MFI and the Novel Extra-Large Pore IDM-1 as Ordered End-Members. Chemistry of Materials, 33(19), 7869-7877
Open this publication in new window or tab >>Sandwich-Type Zeolite Intergrowths with MFI and the Novel Extra-Large Pore IDM-1 as Ordered End-Members
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2021 (English)In: Chemistry of Materials, ISSN 0897-4756, E-ISSN 1520-5002, Vol. 33, no 19, p. 7869-7877Article in journal (Refereed) Published
Abstract [en]

Stacking faults are two-dimensional planar defects frequently arising in zeolites, modifying their properties and potentially affecting their performance in catalysis and separation applications. In classical zeolite intergrowths, a topologically unique zeolite layer may often pile up after some spatial transformation (lateral translation, rotation, and/or reflection) that may occur in different amounts or directions with about similar probabilities, leading to a difficult to control disorder. Here, we present a new kind of zeolite intergrowth that requires an additional topologically distinct layer rather than a spatial transformation of a unique one. Stacking of the so-called pentasil layers produces the well-known medium pore zeolite MFI. Intercalation in strict alternation of a topologically distinct second layer sandwiched between pentasil layers expands the structure to produce the new extra-large pore IDM-1. Stacking disorder modulates the structural expansion along the stacking direction. The disordered materials have been studied by simulation of the X-ray diffraction patterns using the program DIFFaX and by Cs-corrected high-resolution electron microscopy. We show that disorder does not occur at random but in extended domains and can be controlled all the way from MFI to IDM-1 by just varying the concentration of the synthesis mixture.

Place, publisher, year, edition, pages
American Chemical Society (ACS), 2021
National Category
Chemical Process Engineering
Identifiers
urn:nbn:se:kth:diva-304717 (URN)10.1021/acs.chemmater.1c02631 (DOI)000708647800028 ()2-s2.0-85117094262 (Scopus ID)
Note

QC 20211110

Available from: 2021-11-10 Created: 2021-11-10 Last updated: 2022-06-28Bibliographically approved
Organisations
Identifiers
ORCID iD: ORCID iD iconorcid.org/0000-0003-2221-2285

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