Topochemical Synthesis of Ca3CrN3H Involving a Rotational Structural Transformation for Catalytic Ammonia Synthesis
Angew Chem Int Ed - 2022 - Cao - Topochemical Synthesis of Ca3CrN3H Involving a Rotational Structural Transformation for_removed.pdf
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Rai, Rohit Kumar
KAUST DepartmentImaging and Characterization Department, Core Labs, King Abdullah University of Science and Technology Thuwal 23955, Saudi Arabia
KAUST Catalysis Center (KCC)
Physical Science and Engineering (PSE) Division
Imaging and Characterization Core Lab
Chemical Science Program
Embargo End Date2023-08-05
Permanent link to this recordhttp://hdl.handle.net/10754/680151
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AbstractTopochemical reactions have led to great progress in the discovery of new metastable compounds with novel chemical and physical properties. With these reactions, the overall crystal structure of the host material is generally maintained. Here we report a topochemical synthesis of a hexagonal nitride hydride, h-Ca3CrN3H, by heating an orthorhombic nitride, o-Ca3CrN3, under hydrogen at 673 K, accompanied by a rotational structural transformation. The hydrogen intercalation modifies the Ca-N rock-salt-like atomic packing in o-Ca3CrN3 to a face-sharing octahedral chain in h-Ca3CrN3H, mimicking a 'hinged tessellation' movement. In addition, the h-Ca3CrN3H exhibited stable ammonia synthesis activity when used as a catalyst.
CitationCao, Y., Kirsanova, M., Ochi, M., Almaksoud, W., Zhu, T., Rai, R., Gao, S., Tsumori, T., Kobayashi, S., Kawaguchi, S., Abou-Hamad, E., Kuroki, K., Tassel, C., Abakumov, A., Kobayashi, Y., & Kageyama, H. (2022). Topochemical Synthesis of Ca3CrN3H Involving a Rotational Structural Transformation for Catalytic Ammonia Synthesis. Angewandte Chemie International Edition. Portico. https://doi.org/10.1002/anie.202209187
SponsorsThis work was supported by the Japan Society for Promotion of Science (JSPS) the Grant-in-Aid for Specially Promoted Research (22H04914), JSPS Core-to-Core Program (Grant JPJSCCA20200004), CREST (JPMJCR20R2) and JSPS KAKENHI (21J15834). The financial support for this work was also provided by the King Abdullah University of Science and Technology (KAUST). The synchrotron-diffraction measurements were carried out by the project approval (nos. 2021A1595 and 2021B1815).