Organisch-Polyoxometallat-Co-Kristall-abgeleitete mesoporöse Metallcarbide/-nitride für die Wasserstofferzeugung aus Meerwasser
Herstellung und Eigenschaften von Funktionsmaterialien
Zusammenfassung der Projektergebnisse
This project dealt with the scalable synthesis of mesoporous metal carbide/nitride-based HER catalysts with high Mo/W content and crystallinity through the method of carbonization of organic-POM co-crystals and organic-POM-silica composites. Detailly, we developed a novel precipitation method and synthesized a series of organic-POM co-crystals and organic-POM-silica composites with well-defined and highly controllable single-crystal structures. By these well-designed co-crystal precursors, we obtained a series of mesoporous Mo/W carbides/nitrides and related materials as high-performance HER/OER catalysts through a simple carbonization process. In these co-crystal structures, the POM ensures a high Mo/W content while different amino functionalized benzene derivatives serve as coordination linkers and carbon/nitrogen sources. The corresponding (single-crystal) structures of the organic-POM crystals and their morphologies were fully explored. Specifically, four single crystals with different ligands with ammonium heptamolybdate were characterized, which revealed a stoichiometry of (Mo7O24)4(p-phenylenediamine)17, (Mo21O75)(m-phenylenediamine), (Mo8O26)(o-phenylenediamine)2, and (Mo12O40Cl)6(2-methylimidazole)11. Furthermore, the influence of the chosen synthetic conditions on the morphologies and nanostructures of these organic-POM-silica composites were elucidated. The corresponding electrochemical catalytic activities were measured in standard electrolytes and then applied to assemble water-splitting electrolyzers for hydrogen production from seawater. Overall, this project has accomplished several research objectives, including the selection of suitable organic molecules to obtain organic-POM co-crystals, controlling/optimizing their morphologies, compositions, and crystallinities, the analysis of the organic-POM co-crystals structures, the fabrication, and characterization of the final mesoporous Mo/W carbide/nitride, as well as the electrochemical tests and analysis for hydrogen production.
Projektbezogene Publikationen (Auswahl)
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Assembling and Regulating of Transition Metal‐Based Heterophase Vanadates as Efficient Oxygen Evolution Catalysts. Small, 18(7).
Shao, Wenjie; Xiao, Mingjun; Yang, Chengdong; Cheng, Menghao; Cao, Sujiao; He, Chao; Zhou, Mi; Ma, Tian; Cheng, Chong & Li, Shuang
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Oxygen-evolving catalytic atoms on metal carbides. Nature Materials, 20(9), 1240-1247.
Li, Shuang; Chen, Bingbing; Wang, Yi; Ye, Meng-Yang; van Aken, Peter A.; Cheng, Chong & Thomas, Arne
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Superstructures of Organic–Polyoxometalate Co‐crystals as Precursors for Hydrogen Evolution Electrocatalysts. Angewandte Chemie International Edition, 61(3).
Li, Shuang; Zhao, Zhenyang; Ma, Tian; Pachfule, Pradip & Thomas, Arne
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Crystalline Lattice‐Confined Atomic Pt in Metal Carbides to Match Electronic Structures and Hydrogen Evolution Behaviors of Platinum. Advanced Materials, 34(41).
Ma, Tian; Cao, Hao; Li, Shuang; Cao, Sujiao; Zhao, Zhenyang; Wu, Zihe; Yan, Rui; Yang, Chengdong; Wang, Yi; van Aken, Peter A.; Qiu, Li; Wang, Yang‐Gang & Cheng, Chong
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Interfacial Atom‐Substitution Engineered Transition‐Metal Hydroxide Nanofibers with High‐Valence Fe for Efficient Electrochemical Water Oxidation. Angewandte Chemie International Edition, 61(13).
Zhang, Ben; Wu, Zihe; Shao, Wenjie; Gao, Yun; Wang, Weiwen; Ma, Tian; Ma, Lang; Li, Shuang; Cheng, Chong & Zhao, Changsheng
