The integration of experiment and computational modelling in heterogeneously catalysed ammonia synthesis over metal nitrides

Zeinalipour-Yazdi, C. D., Hargreaves, J. S.J. , Laassiri, S. and Catlow, C. R. A. (2018) The integration of experiment and computational modelling in heterogeneously catalysed ammonia synthesis over metal nitrides. Physical Chemistry Chemical Physics, 20(34), pp. 21803-21808. (doi: 10.1039/C8CP04216K) (PMID:30112528)

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Abstract

In this perspective we present recent experimental and computational progress in catalytic ammonia synthesis research on metal nitrides involving a combined approach. On this basis, it suggested that the consideration of nitrogen vacancies in the synthesis of ammonia can offer new low energy pathways that were previously unknown. We have shown that metal nitrides that are also known to have high activity for ammonia synthesis can readily form nitrogen vacancies on their surfaces. These vacancies adsorb dinitrogen much more strongly than the defect-free surfaces and can efficiently activate the strong N–N triple bond. These fundamental studies suggest that heterogeneously catalysed ammonia synthesis over metal nitrides is strongly affected by bulk and surface defects and that further progress in the discovery of low temperature catalysts relies on more careful consideration of nitrogen vacancies. The potential occurrence of an associative pathway in the case of the Co3Mo3N catalytic system provides a possible link with enzymatic catalysis, which will be of importance in the design of heterogeneous catalytic systems operational under process conditions of reduced severity which are necessary for the development of localised facilities for the production of more sustainable “green” ammonia.

Item Type:Articles
Additional Information:Also funded by EPSRC grants EP/L026317/1 and EP/K014714/1.
Status:Published
Refereed:Yes
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:Physical Chemistry Chemical Physics
Publisher:Royal Society of Chemistry
ISSN:1463-9076
ISSN (Online):1463-9084
Published Online:03 August 2018
Copyright Holders:Copyright © 2018 The Authors
First Published:First published in Physical Chemistry Chemical Physics 20(34):21803-21808
Publisher Policy:Reproduced under a Creative Commons License

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Project CodeAward NoProject NamePrincipal InvestigatorFunder's NameFunder RefLead Dept
652781First principles design of novel ammonia synthesis catalystsJustin HargreavesEngineering and Physical Sciences Research Council (EPSRC)EP/L02537X/1CHEM - CHEMISTRY