Wang, Yaolin ; Yang, Wenjie ; Xu, Shanshan ; Zhao, Shufang ; Chen, Guoxing ; Weidenkaff, Anke ; Hardacre, Christopher ; Fan, Xiaolei ; Huang, Jun ; Tu, Xin (2022)
Shielding Protection by Mesoporous Catalysts for Improving Plasma-Catalytic Ambient Ammonia Synthesis.
In: Journal of the American Chemical Society, 144 (27)
doi: 10.1021/jacs.2c01950
Artikel, Bibliographie

Kurzbeschreibung (Abstract)

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 degrees 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.

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