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

Yaolin Wang, Wenjie Yang, Shanshan Xu, Shufang Zhao, Guoxing Chen, Anke Weidenkaff, Christopher Hardacre, Xiaolei Fan, Jun Huang, Xin Tu

Research output: Journal PublicationArticlepeer-review

114 Citations (Scopus)

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 NH3yield due to a lack of knowledge in the design of highly efficient catalysts and the in situ plasma-induced reverse reaction (i.e., NH3decomposition). Here, we demonstrate that a bespoke design of supported Ni catalysts using mesoporous MCM-41 could enable efficient plasma-catalytic NH3production at 35 °C and 1 bar with >5% NH3yield 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 NH3production. The desorbed NH3could 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.

Original languageEnglish
Pages (from-to)12020-12031
Number of pages12
JournalJournal of the American Chemical Society
Volume144
Issue number27
DOIs
Publication statusPublished - 13 Jul 2022
Externally publishedYes

ASJC Scopus subject areas

  • Catalysis
  • General Chemistry
  • Biochemistry
  • Colloid and Surface Chemistry

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