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

作者：Yaolin Wang, Wenjie Yang, Shanshan Xu, Shufang Zhao, Guoxing Chen, Anke Weidenkaff, Christopher Hardacre, Xiaolei Fan, Jun Huang, Xin Tu · 发表于：Journal of the American Chemical Society · 年份：2022 · DOI：10.1021/jacs.2c01950 · 被引用次数：254 · 研究领域：Ammonia Synthesis and Nitrogen Reduction、Catalytic Processes in Materials Science、Muon and positron interactions and applications

High Resolution Image Download MS PowerPoint Slide Plasma catalysis is a promising technology for decentralized small-scale ammonia (NH 3 ) 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 NH 3 yield due to a lack of knowledge in the design of highly efficient catalysts and the in situ plasma-induced reverse reaction (i.e., NH 3 decomposition). Here, we demonstrate that a bespoke design of supported Ni catalysts using mesoporous MCM-41 could enable efficient plasma-catalytic NH 3 production at 35 °C and 1 bar with >5% NH 3 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 NH 3 production. The desorbed NH 3 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.