Local environmental engineering for highly stable single-atom Pt1/CeO2catalysts: first-principles insights

Jiasi Yan; Wei Xiao; Rong Zeng; Zheng Zhao; Xiaowu Li; Ligen Wang

doi:10.1088/1361-6528/acf3f2

Local environmental engineering for highly stable single-atom Pt₁/CeO₂catalysts: first-principles insights

Nanotechnology. 2023 Oct 4;34(50). doi: 10.1088/1361-6528/acf3f2.

Authors

Jiasi Yan^{1

2

3

4}, Wei Xiao^{1

2

3}, Rong Zeng^{1

2

3}, Zheng Zhao⁵, Xiaowu Li⁴, Ligen Wang^{1

2

3}

Affiliations

¹ State Key Laboratory of Nonferrous Metals and Processes & National Engineering Research Center of Nonferrous Metals Materials and Products for New Energy, China GRINM Group Co., Ltd, Beijing 100088, People's Republic of China.
² GRIMAT Engineering Institute Co., Ltd, Beijing 101407, People's Republic of China.
³ General Research Institute for Nonferrous Metals, Beijing 100088, People's Republic of China.
⁴ Department of Materials Physics and Chemistry, School of Materials Science and Engineering, Key Laboratory for Anisotropy and Texture of Materials, Ministry of Education, Northeastern University, Shenyang, 110819, People's Republic of China.
⁵ National Engineering Research Center for Rare Earth, GRINM Group Corporation Limited, Beijing 100088, People's Republic of China.

PMID: 37789667
DOI: 10.1088/1361-6528/acf3f2

Abstract

Single-atom Pt₁/CeO₂catalysts may cope with the high cost and durability issues of fuel cell electrocatalysts. In the present study, the stability and underlying interaction mechanisms of the Pt₁/CeO₂system are systematically investigated using first-principles calculations. The Pt adsorption energy on CeO₂surfaces can be divided into chemical interaction and surface deformation parts. The interaction energy, mainly associated with the local chemical environment, i.e. the number of Pt-O bonds, plays a major role in Pt₁/CeO₂stability. When forming a Pt-4O configuration, the catalytic system has the highest stability and Pt is oxidized to Pt²⁺. An electronic metal-support interaction mechanism is proposed for understanding Pt₁/CeO₂stability. In addition, our calculations show that the Pt₁/CeO₂(100) system is dynamically stable, and the external O environment can promote the further oxidation of Pt to Ptⁿ⁺(2 ≤n< 4). The present study provides useful guidance for the experimental development of highly stable and efficient electrocatalysts for fuel cell applications.

Keywords: Pt1/CeO2 catalysts; first-principles calculations; local environment; stability; valence change mechanism.