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

Wang, Y ORCID: 0000-0003-1932-9810, Yang, W ORCID: 0000-0002-1013-2678, Xu, S, Zhao, S ORCID: 0000-0002-4595-1817, Chen, G, Weidenkaff, A ORCID: 0000-0002-7021-1765, Hardacre, C ORCID: 0000-0001-7256-6765, Fan, X ORCID: 0000-0002-9039-6736, Huang, J ORCID: 0000-0001-8704-605X and Tu, X ORCID: 0000-0002-6376-0897 (2022) Shielding Protection by Mesoporous Catalysts for Improving Plasma-Catalytic Ambient Ammonia Synthesis Journal of the American Chemical Society, 144 (27). pp. 12020-12031. ISSN 0002-7863, 1520-5126

Access the full-text of this item by clicking on the Open Access link.

Text jacs.2c01950.pdf - Published version Download (6MB) | Preview

Abstract

Plasma catalysis is a promising technology for decentralized small-scale ammonia (NH<inf>3</inf>) 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<inf>3</inf>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<inf>3</inf>decomposition). Here, we demonstrate that a bespoke design of supported Ni catalysts using mesoporous MCM-41 could enable efficient plasma-catalytic NH<inf>3</inf>production at 35 °C and 1 bar with >5% NH<inf>3</inf>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<inf>3</inf>production. The desorbed NH<inf>3</inf>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.

Item Type:	Article
Uncontrolled Keywords:	3402 Inorganic Chemistry, 34 Chemical Sciences, 7 Affordable and Clean Energy, 13 Climate Action
Divisions:	Faculty of Science & Engineering > School of Electrical Engineering, Electronics and Computer Science
Depositing User:	Symplectic Admin
Date Deposited:	23 Jun 2022 13:38
Last Modified:	13 Mar 2026 07:24
DOI:	10.1021/jacs.2c01950
Open Access URL:	https://doi.org/10.1021/jacs.2c01950
Related Websites:	Author Publisher
URI:	https://livrepository.liverpool.ac.uk/id/eprint/3157043
Disclaimer:	The University of Liverpool is not responsible for content contained on other websites from links within repository metadata. Please contact us if you notice anything that appears incorrect or inappropriate.