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 mar 2022
Accepted
04 maj 2022
First published
05 maj 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

This article is licensed under a Creative Commons Attribution-NonCommercial 3.0 Unported Licence. You can use material from this article in other publications, without requesting further permission from the RSC, provided that the correct acknowledgement is given and it is not used for commercial purposes.

To request permission to reproduce material from this article in a commercial publication, please go to the Copyright Clearance Center request page.

If you are an author contributing to an RSC publication, you do not need to request permission provided correct acknowledgement is given.

If you are the author of this article, you do not need to request permission to reproduce figures and diagrams provided correct acknowledgement is given. If you want to reproduce the whole article in a third-party commercial publication (excluding your thesis/dissertation for which permission is not required) please go to the Copyright Clearance Center request page.

Read more about how to correctly acknowledge RSC content.

Social activity

Spotlight

Advertisements