A descriptor guiding the selection of catalyst supports for ammonia synthesis

Weilhard, Andreas, Popov, Ilya, Kohlrausch, Emerson C., Aliev, Gazi N., Blankenship, L. Scott, Norman, Luke T., Ghaderzadegh, Sadegh, Smith, Louise R., Isaacs, Mark Andrew, O'Shea, James, Lanterna, Anabel, Theis, Wolfgang, Morgan, David ORCID: https://orcid.org/0000-0002-6571-5731, Hutchings, Graham J. ORCID: https://orcid.org/0000-0001-8885-1560, Besley, Elena, Khlobystov, Andrei and Alves Fernandes, Jesum 2025. A descriptor guiding the selection of catalyst supports for ammonia synthesis. Chemical Science 10.1039/D4SC08253B

PDF - Published Version Available under License Creative Commons Attribution. Download (887kB)

Abstract

The efforts to increase the active surface area of catalysts led to reduction of metal particle size, down to single metal atoms. This results in increasing importance of support–metal interactions. We demonstrate the mechanisms through which the support influences catalytic activity of nanoclusters: the support electronics, described by the O 2p energy level, and the support surface chemistry, determined by the density of Lewis base sites. Using Ru nanoclusters, our study shows that these parameters can be effectively captured within a single catalyst support descriptor (CSD). The apparent activation energy and turnover frequency (TOF) for the ammonia synthesis correlates strongly with CSD measured for the series Ru/MgO, Ru/Sc2O3, Ru/CeO2, Ru/La2O3, and Ru/Y2O3. Furthermore, the study demonstrates that CSD correlates linearly with the binding strength of N–Ru in nanocluster, thereby providing a direct link between the catalyst's surface chemistry and the nature of the support. The catalyst support descriptor developed in this study serves as a simple yet powerful tool for selecting the optimal support material to maximise the activity of metal nanoclusters without altering the metal itself.

Item Type:	Article
Status:	In Press
Schools:	Schools > Chemistry Research Institutes & Centres > Cardiff Catalysis Institute (CCI)
Publisher:	Royal Society of Chemistry
ISSN:	2041-6520
Funders:	EPSRC
Date of First Compliant Deposit:	7 February 2025
Date of Acceptance:	27 January 2025
Last Modified:	19 Feb 2025 12:45
URI:	https://orca.cardiff.ac.uk/id/eprint/176036

Actions (repository staff only)

Edit Item