Kinetic and mechanistic analysis of NH3 decomposition on Ru(0001), Ru(111) and Ir(111) surfaces

Lu, Xiuyuan, Zhang, Jing, Chen, Wenkai and Roldan, Alberto ORCID: https://orcid.org/0000-0003-0353-9004 2021. Kinetic and mechanistic analysis of NH3 decomposition on Ru(0001), Ru(111) and Ir(111) surfaces. Nanoscale Advances 3 (6) , pp. 1624-1632. 10.1039/D1NA00015B

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Abstract

We investigated the NH3 catalytic decomposition on Ru and Ir metal surfaces using density functional theory. The reaction mechanisms were unraveled on both metals, considering that, at nano-scale, Ru particles may also present an fcc structure, hence, leading to three energy profiles. We implemented thermodynamic and kinetic parameters obtained from DFT into microkinetic simulations. Batch reactor simulations suggest that hydrogen generation starts at 400 K, 425 K and 600 K on Ru(111), Ru(0001) and Ir(111) surfaces respectively, in excellent agreement with experiments. During the reaction, the main surface species on Ru are NH, N and H, whereas, on Ir(111), it is mainly NH. The rate-determining step for all surfaces is the formation of molecular nitrogen. We also performed temperature-programmed reaction simulations and inspected the desorption spectra of N2 and H2 as a function of the temperature, which highlighted the importance of N coverage on the desorption rate.

Item Type:	Article
Date Type:	Publication
Status:	Published
Schools:	Chemistry Cardiff Catalysis Institute (CCI) Advanced Research Computing @ Cardiff (ARCCA)
Publisher:	Royal Society of Chemistry
ISSN:	2516-0230
Funders:	EPSRC
Date of First Compliant Deposit:	10 February 2021
Date of Acceptance:	8 February 2021
Last Modified:	08 Dec 2023 15:03
URI:	https://orca.cardiff.ac.uk/id/eprint/138411

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