Shielding Protection by Mesoporous Catalysts for Improving Plasma-Catalytic Ambient Ammonia Synthesis

• Published in: Journal of the American Chemical Society 2022-07, Vol.144 (27), p.12020-12031
• Main Authors: Wang, Yaolin, Yang, Wenjie, Xu, Shanshan, Zhao, Shufang, Chen, Guoxing, Weidenkaff, Anke, Hardacre, Christopher, Fan, Xiaolei, Huang, Jun, Tu, Xin
• Format: Article
• Language: English
• ISSN: 0002-7863; 1520-5126; 1520-5126
• DOI: 10.1021/jacs.2c01950

Plasma catalysis is a promising technology for decentralized small-scale ammonia (NH3) synthesis under mild conditions using renewable energy, and it shows great potential as an alternative to the conventional Haber–Bosch process. To date, this emerging process still suffers from a low NH3 yield due to a lack of knowledge in the design of highly efficient catalysts and the in situ plasma-induced reverse reaction (i.e., NH3 decomposition). Here, we demonstrate that a bespoke design of supported Ni catalysts using mesoporous MCM-41 could enable efficient plasma-catalytic NH3 production at 35 °C and 1 bar with >5% NH3 yield at 60 kJ/L. Specifically, the Ni active sites were deliberately deposited on the external surface of MCM-41 to enhance plasma–catalyst interactions and thus NH3 production. The desorbed NH3 could then diffuse into the ordered mesopores of MCM-41 to be shielded from decomposition due to the absence of plasma discharge in the mesopores of MCM-41, that is, “shielding protection”, thus driving the reaction forward effectively. This promising strategy sheds light on the importance of a rational design of catalysts specifically for improving plasma-catalytic processes.