Theoretical insight into the relevance between the oxidation states of CeO2 supported Pt4+/2+/1+/0/2− and their HER performance

Hongxian Liu; Changling Liu; Chao Ma; Dunhua Hong; Zhenxing Fang; Haitao Zhao; Tongwei Wu; Yanning Zhang

doi:10.1039/D2CE01246D

Theoretical insight into the relevance between the oxidation states of CeO₂ supported Pt^{4+/2+/1+/0/2−} and their HER performance†

Hongxian Liu,‡^ab Changling Liu,‡^c Chao Ma,^b Dunhua Hong,^a Zhenxing Fang,

*^a Haitao Zhao,^e Tongwei Wu

*^d and Yanning Zhang

*^b

Author affiliations

* Corresponding authors

^a School of Physics and Electronic Science, Zunyi Normal University, Zunyi 563000, Guizhou, China

^b Institute of Fundamental and Frontier Sciences, University of Electronic Science and Technology of China, Chengdu 610054, Sichuan, China
E-mail: yanningz@uestc.edu.cn

^c College of Materials Science and Engineering, Jilin Institute of Chemical Technology, Jilin City 132022, Jilin Province, China

^d State Key Laboratory of Electronic Thin Films and Integrated Devices, University of Electronic Science and Technology of China, Chengdu 610054, Sichuan, China

^e Materials Interfaces Center, Shenzhen Institutes of Advanced Technology, Chinese Academy of Sciences, Shenzhen 440305, China

Abstract

The oxidation states (OSs) of Pt catalysts play a key role in the hydrogen evolution reaction (HER), which has become a focus in recent years. As for Pt/CeO₂ catalysts, we have systematically explored the effect of Pt^{4+/2+/1+/0/2−} OSs on the HER. H atoms could not adsorb on the Pt⁴⁺ and Pt_4c²⁺ sites, and they prefer to locate on the adjacent O atoms (labeled as Pt⁴⁺–O and Pt_4c²⁺–O). As for the other OSs, the adsorption ability of H atoms follows the order Pt⁰ > Pt_3c²⁺ > Pt¹⁺ > Pt²⁻. The electron-enriched Pt²⁻ is the most suitable oxidation state for the HER, no matter the reaction mechanism, which is the Volmer–Heyrovsky or Volmer–Tafel mechanism. The Pt OSs would greatly affect the electronic structures of Pt catalysts, which will further impact their overall catalytic properties. Our study could shed light on the research of Pt-based catalysts for the HER.

This article is part of the themed collection: Data Driven Crystal Engineering

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Article information

DOI: https://doi.org/10.1039/D2CE01246D
Article type: Communication
Submitted: 08 Sep 2022
Accepted: 17 Nov 2022
First published: 17 Nov 2022

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CrystEngComm, 2023,25, 40-47

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Theoretical insight into the relevance between the oxidation states of CeO₂ supported Pt^{4+/2+/1+/0/2−} and their HER performance

H. Liu, C. Liu, C. Ma, D. Hong, Z. Fang, H. Zhao, T. Wu and Y. Zhang, CrystEngComm, 2023, 25, 40 DOI: 10.1039/D2CE01246D

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