Sodium-Directed Photon-Induced Assembly Strategy for Preparing Multisite Catalysts with High Atomic Utilization Efficiency

Xiaoqiang An; Tingcha Wei; Peijia Ding; Li-Min Liu; Lunqiao Xiong; Junwang Tang; Jiani Ma; Feng Wang; Huijuan Liu; Jiuhui Qu

doi:10.1021/jacs.2c10690

Sodium-Directed Photon-Induced Assembly Strategy for Preparing Multisite Catalysts with High Atomic Utilization Efficiency

J Am Chem Soc. 2023 Jan 25;145(3):1759-1768. doi: 10.1021/jacs.2c10690. Epub 2023 Jan 6.

Authors

Xiaoqiang An¹, Tingcha Wei^{1

2}, Peijia Ding³, Li-Min Liu³, Lunqiao Xiong⁴, Junwang Tang⁴, Jiani Ma⁵, Feng Wang⁶, Huijuan Liu¹, Jiuhui Qu¹

Affiliations

¹ Center for Water and Ecology, State Key Joint Laboratory of Environment Simulation and Pollution Control, School of Environment, Tsinghua University, Beijing 100084, China.
² MIIT Key Laboratory of Aerospace Information Materials and Physics, College of Physics, Nanjing University of Aeronautics and Astronautics, Nanjing 211106, China.
³ School of Physics, Beihang University, Beijing 100191, China.
⁴ Department of Chemical Engineering, University College London, Torrington Place, London WC1E 7JE, U.K.
⁵ Key Laboratory of Applied Surface and Colloid Chemistry, Ministry of Education, School of Chemistry and Chemical Engineering, Shanxi Normal University, Xi'an 710119, China.
⁶ Department of Physics, Chemistry and Biology (IFM), Linköping University, Linköping 581 83, Sweden.

PMID: 36607337
DOI: 10.1021/jacs.2c10690

Abstract

Integrating different reaction sites offers new prospects to address the difficulties in single-atom catalysis, but the precise regulation of active sites at the atomic level remains challenging. Here, we demonstrate a sodium-directed photon-induced assembly (SPA) strategy for boosting the atomic utilization efficiency of single-atom catalysts (SACs) by constructing multifarious Au sites on TiO₂ substrate. Na⁺ was employed as the crucial cement to direct Au single atoms onto TiO₂, while the light-induced electron transfer from excited TiO₂ to Au(Na⁺) ensembles contributed to the self-assembly formation of Au nanoclusters. The synergism between plasmonic near-field and Schottky junction enabled the cascade electron transfer for charge separation, which was further enhanced by oxygen vacancies in TiO₂. Our dual-site photocatalysts exhibited a nearly 2 orders of magnitude improvement in the hydrogen evolution activity under simulated solar light, with a striking turnover frequency (TOF) value of 1533 h^-1 that exceeded other Au/TiO₂-based photocatalysts reported. Our SPA strategy can be easily extended to prepare a wide range of metal-coupled nanostructures with enhanced performance for diverse catalytic reactions. Thus, this study provides a well-defined platform to extend the boundaries of SACs for multisite catalysis through harnessing metal-support interactions.