COx-free hydrogen production from ammonia – mimicking the activity of Ru catalysts with unsupported Co-Re alloys

Kirste, K., McAulay, K., Bell, T. E., Stoian, D., Laassiri, S., Daisley, A., Hargreaves, J. S.J. , Mathisen, K. and Torrente-Murciano, L. (2021) COx-free hydrogen production from ammonia – mimicking the activity of Ru catalysts with unsupported Co-Re alloys. Applied Catalysis B: Environmental, 280, 119405. (doi: 10.1016/j.apcatb.2020.119405)

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Abstract

On-demand production of hydrogen from ammonia is a challenge limiting the implementation of ammonia as a long term hydrogen vector to overcome the difficulties associated with hydrogen storage. Herein, we present the development of catalysts for the on-demand production of hydrogen from ammonia by combining metals with high and low N-adatom adsorption energies. In this way, cobalt-rhenium (Co-Re) catalysts show high activity mimicking that of ruthenium. EXAFS/XANES analyses demonstrate that the bimetallic Co-Re contribution is responsible for the activity and the stability of the catalysts in consecutive runs with no observable formation of nitrides (Co-N and Re-N) occurring under the ammonia atmosphere. While cobalt is partially re-oxidised under ammonia, re-reduction in the presence of rhenium is observed at higher temperatures, coinciding with the on-set of catalytic activity which is accompanied by minor structural changes. These results provide insight for the development of highly active alloy based ammonia decomposition catalysts.

Item Type:Articles
Additional Information:Also funded by UK Engineering and Physical Science Research Council (EPSRC grant numbers EP/L020432/2, EP/N013778/1, and EP/L026317/1).
Status:Published
Refereed:Yes
Glasgow Author(s) Enlighten ID:Daisley, Miss Angela and McAulay, Dr Kate and Laassiri, Dr Said and Hargreaves, Professor Justin
Creator Roles:
McAulay, K.Investigation, Writing – review and editing
Laassiri, S.Investigation, Writing – review and editing
Daisley, A.Investigation, Writing – review and editing
Hargreaves, J.Supervision, Funding acquisition, Writing – review and editing
Authors: Kirste, K., McAulay, K., Bell, T. E., Stoian, D., Laassiri, S., Daisley, A., Hargreaves, J. S.J., Mathisen, K., and Torrente-Murciano, L.
College/School:College of Science and Engineering > School of Chemistry
Journal Name:Applied Catalysis B: Environmental
Publisher:Elsevier
ISSN:0926-3373
ISSN (Online):1873-3883
Published Online:07 August 2020
Copyright Holders:Copyright © 2020 The Authors
First Published:First published in Applied Catalysis B: Environmental 280:119405
Publisher Policy:Reproduced under a Creative Commons license

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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