Revealing the reconstruction mechanism of AgPd nanoalloys under fluorination based on a multiscale deep learning potential

Author:

Guo Longfei12ORCID,Shan Shuang12,Liu Xiaoqing2,Zhang Wanxuan2,Xu Peng1,Ma Fanzhe1,Li Zhen12ORCID,Wang Chongyang2,Wang Junpeng2ORCID,Chen Fuyi12ORCID

Affiliation:

1. State Key Laboratory of Solidification Processing, Northwestern Polytechnical University 1 , Xi’an 710072, China

2. School of Materials Science and Engineering, Northwestern Polytechnical University 2 , Xi’an 710072, China

Abstract

The design of heterogeneous catalysts generally involves optimizing the reactivity descriptor of adsorption energy, which is inevitably governed by the structure of surface-active sites. A prerequisite for understanding the structure–properties relationship is the precise identification of real surface-active site structures, rather than relying on conceived structures derived from bulk alloy properties. However, it remains a formidable challenge due to the dynamic nature of nanoalloys during catalytic reactions and the lack of accurate and efficient interatomic potentials for simulations. Herein, a generalizable deep-learning potential for the Ag–Pd–F system is developed based on a dataset encompassing the bulk, surface, nanocluster, amorphous, and point defected configurations with diverse compositions to achieve a comprehensive description of interatomic interactions, facilitating precise prediction of adsorption energy, surface energy, formation energy, and diffusion energy barrier and is utilized to investigate the structural evolutions of AgPd nanoalloys during fluorination. The structural evolutions involve the inward diffusion of F, the outward diffusion of Ag in Ag@Pd nanoalloys, the formation of surface AgFx species in mixed and Janus AgPd nanoalloys, and the shape deformation from cuboctahedron to sphere in Ag and Pd@Ag nanoalloys. Moreover, the effects of atomic diffusion and dislocation formation and migration on the reconstructing pathway of nanoalloys are highlighted. It is demonstrated that the stress relaxation upon F adsorption serves as the intrinsic driving factor governing the surface reconstruction of AgPd nanoalloys.

Funder

National Natural Science Foundation of China

Research Fund of State Key Laboratory of Solidification Processing in China

Aeronautic Science Foundation Program of China

Project of Transformation of Scientific and Technological Achievements of NWPU

Open Fund of State Key Laboratory of Advanced Technology for Materials Synthesis and Processing

Publisher

AIP Publishing

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