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  Barium chromium nitride-hydride for ammonia synthesis

Guan, Y., Zhang, W., Wang, Q., Weidenthaler, C., Wu, A., Gao, W., et al. (2021). Barium chromium nitride-hydride for ammonia synthesis. Chem Catalysis, 1(5), 1042-1054. doi:10.1016/j.checat.2021.08.006.

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Guan, Yeqin1, 2, Autor
Zhang, Weijin1, 2, Autor
Wang, Qianru1, 2, Autor
Weidenthaler, Claudia3, Autor           
Wu, Anan4, Autor
Gao, Wenbo1, 2, Autor
Pei, Qijun1, Autor
Yan, Hanxue1, 2, Autor
Cui, Jirong1, 2, Autor
Wu, Han1, 2, Autor
Feng, Sheng1, 2, Autor
Wang, Runze1, 2, Autor
Cao, Hujun1, 2, Autor
Ju, Xiaohua1, Autor
Lui, Lin1, 2, Autor
He, Teng1, 2, Autor
Guo, Jianping1, 2, Autor
Chen, Ping1, 2, Autor
Affiliations:
1Dalian National Laboratory for Clean Energy, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, P. R. China, ou_persistent22              
2University of Chinese Academy of Sciences, Beijing 100049, P. R. China, ou_persistent22              
3Research Group Weidenthaler, Max-Planck-Institut für Kohlenforschung, Max Planck Society, ou_1950291              
4Department of Chemistry, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, P. R. China, ou_persistent22              

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Schlagwörter: ammonia synthesis; nitride-hydride; hydride; chromium; barium; nitrogen fixation; heterogeneous catalysis; early transition metal
 Zusammenfassung: Early 3d metals such as chromium can easily dissociate N2, but the subsequent hydrogenation to ammonia is difficult because they bind nitrogen too strongly. Hence, investigation of Cr-based catalysts for ammonia synthesis is very rare. Here we show that when Cr compounds with Ba, N, and H forming a nitride-hydride, effective ammonia synthesis catalysis can be achieved under mild conditions. Under 573 K and 10 bar, this catalyst has an ammonia synthesis rate (6.8 mmolNH3gcat−1h−1) that is about four times that of the Cs-Ru/MgO catalyst. With low apparent activation energy (50.1 kJ mol−1) and positive reaction orders of H2 and N2, it can produce observable ammonia at 373 K and 1 bar. The active phase has a Ba5CrN4H-like structure containing reactive hydrogen (H-) and nitrogen, which are involved in the ammonia formation. This work discloses a strategy to “activate” the inactive early transition metals for effective ammonia catalysis.

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Sprache(n): eng - English
 Datum: 2021-05-092021-08-112021-10-21
 Publikationsstatus: Online veröffentlicht
 Seiten: 13
 Ort, Verlag, Ausgabe: -
 Inhaltsverzeichnis: -
 Art der Begutachtung: Expertenbegutachtung
 Identifikatoren: DOI: 10.1016/j.checat.2021.08.006
 Art des Abschluß: -

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Titel: Chem Catalysis
  Kurztitel : Chem Catal.
Genre der Quelle: Zeitschrift
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Ort, Verlag, Ausgabe: New York : New York Elsevier Inc.
Seiten: - Band / Heft: 1 (5) Artikelnummer: - Start- / Endseite: 1042 - 1054 Identifikator: ISSN: 2667-1107
CoNE: https://pure.mpg.de/cone/journals/resource/3667-1107