Issue 21, 2022

Towards the rational design of Pt-based alloy catalysts for the low-temperature water-gas shift reaction: from extended surfaces to single atom alloys

Abstract

The rational design of Pt-based catalysts for the low-temperature water-gas-shift (LT-WGS) reaction is an active research field because of its important role played in the fuel cell-based hydrogen economy, especially in mobile applications. Previous theoretical analyses have suggested that Pt alloys, leading to a weaker CO binding affinity than the Pt metal, could help alleviate CO poisoning and thus should be promising catalysts of the LT-WGS reaction. However, experimental research along this line was rather ineffective in the past decade. In the present work, we employed the state-of-the-art kinetic Monte Carlo (KMC) simulations to examine the influences of the electronic effect by introducing sub-surface alloys and/or core–shell structures, and the synergetic effect by introducing single atom alloys on the catalytic performance of Pt-alloy catalysts. Our KMC simulations have highlighted the importance of the OH binding affinity on the catalyst surfaces to reduce the barrier of water dissociation as the rate determining step, instead of the CO binding affinity as has been emphasized before in conventional mean-field kinetic models. Along this new direction of catalyst design, we found that Pt–Ru synergetic effects can significantly increase the activity of the Pt metal, leading to Ru1–3@Pt alloys with a tetrahedron site of one surface-three subsurface Ru atoms on the Pt host, showing a turnover frequency of about five orders of magnitude higher than the Pt metal.

Graphical abstract: Towards the rational design of Pt-based alloy catalysts for the low-temperature water-gas shift reaction: from extended surfaces to single atom alloys

Supplementary files

Article information

Article type
Edge Article
Submitted
25 3 2022
Accepted
04 5 2022
First published
05 5 2022
This article is Open Access

All publication charges for this article have been paid for by the Royal Society of Chemistry
Creative Commons BY-NC license

Chem. Sci., 2022,13, 6385-6396

Towards the rational design of Pt-based alloy catalysts for the low-temperature water-gas shift reaction: from extended surfaces to single atom alloys

Y. Yang, T. Shen and X. Xu, Chem. Sci., 2022, 13, 6385 DOI: 10.1039/D2SC01729F

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