A comparative analysis of the mechanisms of ammonia synthesis on various catalysts using density functional theory

Zeinalipour-Yazdi, C. D., Hargreaves, J. S.J. , Laassiri, S. and Catlow, C. R. A. (2021) A comparative analysis of the mechanisms of ammonia synthesis on various catalysts using density functional theory. Royal Society Open Science, 8(11), 210952. (doi: 10.1098/rsos.210952)

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In this review, we present the recent progress in ammonia synthesis research using density functional theory (DFT) calculations on various industrial catalysts, metal nitrides and nano-cluster-supported catalysts. The mechanism of ammonia synthesis on the industrial Fe catalyst is generally accepted to be a dissociative mechanism. We have recently found, using DFT techniques, that on Co3Mo3N (111) surfaces, an associative mechanism in the synthesis of ammonia can offer a new low-energy pathway that was previously unknown. In particular, we have shown that metal nitrides that are also known to have high activity for ammonia synthesis can readily form nitrogen vacancies which can activate dinitrogen, thereby promoting the associative mechanism. These fundamental studies suggest that a promising route to the discovery of low-temperature ammonia synthesis catalysts will be to identify systems that proceed via the associative mechanism, which is closer to the nitrogen-fixation mechanism occurring in nitrogenases.

Item Type:Articles
Additional Information:The authors acknowledge financial support from EPSRC (grant nos. EP/L026317/1 and EP/L02537X/1). The authors acknowledge EPSRC-funded computer resources (grant no. EP/L000202/1) at ARCHER UK National Supercomputing Service (http://www.archer.ac.uk) received via our membership of the UK's HPC Materials Chemistry Consortium.
Glasgow Author(s) Enlighten ID:Laassiri, Dr Said and Hargreaves, Professor Justin
Authors: Zeinalipour-Yazdi, C. D., Hargreaves, J. S.J., Laassiri, S., and Catlow, C. R. A.
College/School:College of Science and Engineering > School of Chemistry
Journal Name:Royal Society Open Science
Publisher:Royal Society
ISSN (Online):2054-5703
Published Online:03 November 2021
Copyright Holders:Copyright © 2021 The Authors
First Published:First published in Royal Society Open Science
Publisher Policy:Reproduced under a Creative Commons Licence

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Project CodeAward NoProject NamePrincipal InvestigatorFunder's NameFunder RefLead Dept
170245First principles design of novel ammonia synthesis catalystsJustin HargreavesEngineering and Physical Sciences Research Council (EPSRC)EP/L02537X/1Chemistry