Combination of theoretical and in-situ experimental investigations of the role of lithium dopant in manganese nitride: a two-stage reagent for ammonia synthesis

Laassiri, S., Zeinalipour-Yazdi, C. D., Bion, N., Catlow, R. C. A. and Hargreaves, J. (2021) Combination of theoretical and in-situ experimental investigations of the role of lithium dopant in manganese nitride: a two-stage reagent for ammonia synthesis. Faraday Discussions, 229, pp. 281-296. (doi: 10.1039/C9FD00131J) (PMID:33729220)

Abstract

Manganese nitride related materials are of interest as two-stage reagents for ammonia synthesis via nitrogen chemical looping. However, unless doped with a co-cation, manganese nitrides are thermochemically stable and high temperature is required to produce ammonia under reducing conditions, thereby hindering their use as nitrogen transfer materials. Nevertheless, when lithium is used as dopant, ammonia generation can be observed at a reaction temperature as low as 300°C. In order to develop strategies for the improvement of the reactivity of nitride materials in the context of two-stage reagents, it is necessary to understand the intrinsic role of the dopant in the mechanism of ammonia synthesis. To this end, we have investigated the role of lithium in increasing the manganese nitride reactivity by in-situ neutron diffraction studies and N2 and H2 isotopic exchange reactions supplemented by DFT calculations.

• Item Type: Articles
• Additional Information: The authors acknowledge the support of PRESTIGE H2020 program and the financial support of MOPGA and region haut de France research funding program. This study was supported by EPSRC funding (EP/L026317/1, EP/L02537X/1). Via our membership of the UK's HEC Materials Chemistry Consortium, which is funded by EPSRC (EP/L000202/1)
• Status: Published
• Refereed: Yes
• Glasgow Author(s) Enlighten ID: Laassiri, Dr Said and Hargreaves, Professor Justin
• Authors: Laassiri, S., Zeinalipour-Yazdi, C. D., Bion, N., Catlow, R. C. A., and Hargreaves, J.
• College/School: College of Science and Engineering > School of Chemistry
• Journal Name: Faraday Discussions
• Publisher: Royal Society of Chemistry
• ISSN: 1359-6640
• ISSN (Online): 1364-5498
• Published Online: 28 January 2020
• Copyright Holders: Copyright © 2020 Royal Society of Chemistry
• First Published: First published in Faraday Discussions 229:281-296
• Publisher Policy: Reproduced under a Creative Commons License

Project Code	Award No	Project Name	Principal Investigator	Funder's Name	Funder Ref	Lead Dept
170245		First principles design of novel ammonia synthesis catalysts	Justin Hargreaves	Engineering and Physical Sciences Research Council (EPSRC)	EP/L02537X/1	Chemistry