期刊
CHINESE JOURNAL OF CATALYSIS
卷 43, 期 8, 页码 2183-2192出版社
ELSEVIER
DOI: 10.1016/S1872-2067(22)64129-9
关键词
N-2-to-NH3 conversion; Scaling relations; Heterogeneous catalyst design; First-principles calculations
资金
- National Natural Science Foundation of China [22122304, 21903047, 22033005, 22038002]
- Guangdong Basic and Applied Basic Research Foundation [2020A1515110282]
- Guangdong Provincial Key Laboratory of Catalysis [2020B121201002]
- Center for Computational Science and Engineering (SUSTech)
The catalytic mechanisms of N-2-to-NH3 conversion on the lanthanide intermetallic electride catalyst LaRuSi were investigated, revealing the presence of a bowl active site that can break the scaling relations and enable highly efficient catalysis.
The design of optimal heterogeneous catalysts for N-2-to-NH3 conversion is often dictated by the scaling relations, which result in a volcano curve that poses a limit on the catalytic performance. Herein, we reveal a bowl active site that can break the scaling relations, through investigating the catalytic mechanisms of N-2-to-NH3 conversion on the lanthanide intermetallic electride catalyst LaRuSi by first-principles modeling. This bowl active site, composed of four surface La cations and one subsurface Si atom rich in electrons, plays the key role in enabling efficient catalysis. With adaptive electrostatic and orbital interactions, the bowl active site promotes the adsorption and activation of N-2 that delivers facile cleavage of N.N bond, while destabilizes the adsorptions of *NHx (x = 1, 2, 3) species, which facilitates the release of the final NH3 product. By comparison with other electride catalysts isostructural to LaRuSi, we confirm the breaking of scaling relations between the adsorptions of *NHx species and that of *N on the bowl active site. Thus, this bowl active site presents a design concept that breaks the scaling relations for highly efficient heterogeneous catalysis of N-2-to-NH3 conversion. (c) 2022, Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by Elsevier B.V. All rights reserved.
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