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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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 Creators:
Guan, Yeqin1, 2, Author
Zhang, Weijin1, 2, Author
Wang, Qianru1, 2, Author
Weidenthaler, Claudia3, Author              
Wu, Anan4, Author
Gao, Wenbo1, 2, Author
Pei, Qijun1, Author
Yan, Hanxue1, 2, Author
Cui, Jirong1, 2, Author
Wu, Han1, 2, Author
Feng, Sheng1, 2, Author
Wang, Runze1, 2, Author
Cao, Hujun1, 2, Author
Ju, Xiaohua1, Author
Lui, Lin1, 2, Author
He, Teng1, 2, Author
Guo, Jianping1, 2, Author
Chen, Ping1, 2, Author
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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Free keywords: ammonia synthesis; nitride-hydride; hydride; chromium; barium; nitrogen fixation; heterogeneous catalysis; early transition metal
 Abstract: 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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Language(s): eng - English
 Dates: 2021-05-092021-08-112021-10-21
 Publication Status: Published online
 Pages: 13
 Publishing info: -
 Table of Contents: -
 Rev. Type: Peer
 Identifiers: DOI: 10.1016/j.checat.2021.08.006
 Degree: -

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Title: Chem Catalysis
  Abbreviation : Chem Catal.
Source Genre: Journal
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Affiliations:
Publ. Info: New York : New York Elsevier Inc.
Pages: - Volume / Issue: 1 (5) Sequence Number: - Start / End Page: 1042 - 1054 Identifier: ISSN: 2667-1107
CoNE: https://pure.mpg.de/cone/journals/resource/3667-1107