Elucidating the formation and structural evolution of platinum single-site catalysts for the hydrogen evolution reaction

Tang, P, Lee, H, Hurlbutt, K ORCID: https://orcid.org/0000-0001-7494-0044, Huang, P, Narayanan, S, Wang, C, Gianolio, D ORCID: https://orcid.org/0000-0002-0708-4492, Arrigo, R ORCID: https://orcid.org/0000-0002-2877-8733, Chen, J, Warner, J and Pasta, M ORCID: https://orcid.org/0000-0002-2613-4555 2022, 'Elucidating the formation and structural evolution of platinum single-site catalysts for the hydrogen evolution reaction' , ACS Catalysis, 12 (5) , pp. 3173-3180.

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Abstract

Platinum single-site catalysts (SSCs) are a promising technology for the production of hydrogen from clean energy sources. They have high activity and maximal platinum-atom utilization. However, the bonding environment of platinum during operation is poorly understood. In this work, we present a mechanistic study of platinum SSCs using operando, synchrotron-X-ray absorption spectroscopy. We synthesize an atomically dispersed platinum complex with aniline and chloride ligands onto graphene and characterize it with ex-situ electron microscopy, X-ray diffractometry, X-ray photoelectron spectroscopy, X-ray absorption near-edge structure spectroscopy (XANES), and extended X-ray absorption fine structure spectroscopy (EXAFS). Then, by operando EXAFS and XANES, we show that as a negatively biased potential is applied, the Pt−N bonds break first followed by the Pt−Cl bonds. The platinum is reduced from platinum(II) to metallic platinum(0) by the onset of the hydrogen-evolution reaction at 0 V. Furthermore, we observe an increase in Pt−Pt bonding, indicating the formation of platinum agglomerates. Together, these results indicate that while aniline is used to prepare platinum SSCs, the single-site complexes are decomposed and platinum agglomerates at operating potentials. This work is an important contribution to the understanding of the evolution of bonding environment in SSCs and provides some molecular insights into how platinum agglomeration causes the deactivation of SSCs over time.

Item Type: Article
Additional Information: This document is the unedited Author's version of a Submitted Work that was subsequently accepted for publication in ACS Catalysis, copyright © 2022 American Chemical Society after peer review. To access the final edited and published work see https://pubs.acs.org/doi/abs/10.1021/acscatal.1c05958
Schools: Schools > School of Environment and Life Sciences
Journal or Publication Title: ACS Catalysis
Publisher: American Chemical Society (ACS)
ISSN: 2155-5435
Related URLs:
Funders: Jiangsu Industrial Technology Research Institute
SWORD Depositor: Publications Router
Depositing User: Publications Router
Date Deposited: 09 May 2022 16:55
Last Modified: 16 May 2022 16:46
URI: http://usir.salford.ac.uk/id/eprint/63558

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