Mechanistic Insight into the Synergy between Platinum Single Atom and Cluster Dual Active Sites Boosting Photocatalytic Hydrogen Evolution

Author:

Zhang Jiankang1ORCID,Pan Yukun23,Feng Dan4,Cui Lin1,Zhao Shichao3,Hu Jinlong5,Wang Sen3,Qin Yong13

Affiliation:

1. Interdisciplinary Research Center of Biology & Catalysis School of Life Sciences Northwestern Polytechnical University Xi'an 710072 P. R. China

2. College of Chemical Engineering Xiangtan University Xiangtan 411105 P. R. China

3. State Key Laboratory of Coal Conversion Institute of Coal Chemistry Chinese Academy of Sciences Taiyuan 030001 P. R. China

4. Analytical & Testing Center Northwestern Polytechnical University Xi'an 710072 P. R. China

5. Key Laboratory of Renewable Energy Guangdong Key Laboratory of New and Renewable Energy Research and Development Guangzhou Institute of Energy Conversion Chinese Academy of Sciences Guangzhou 510640 P. R. China

Abstract

AbstractIn the energy transition context, the design and synthesis of high‐performance Pt‐based photocatalysts with low Pt content and ultrahigh atom‐utilization efficiency for hydrogen production are essential. Herein, a facile approach for decorating atomically dispersed Pt cocatalysts having single‐atom (SA) and atomic cluster (C) dual active sites on CdS nanorods (PtSA+C/CdS) via atomic layer deposition is reported. The size of the cocatalyst and the spatial intimacy of the cocatalyst active sites are precisely engineered at the atomic scale. The PtSA+C/CdS photocatalysts show the optimized photocatalytic hydrogen evolution activity, achieving a reaction rate of 80.4 mmol h−1 g−1, which is 1.6‐ and 7.3‐fold higher than those of the PtSA/CdS and PtNP/CdS photocatalysts, respectively. Thorough characterization and theoretical calculations reveal that the enhanced photocatalytic activity is due to a remarkable synergy between SAs and atomic clusters as dual active sites, which are responsible for water adsorption–dissociation and hydrogen desorption, respectively. A similar synergetic effect is found in a representative Pt/TiO2 system, indicating the generality of the strategy. This study demonstrates the significance of the synergy between active sites for enhancing the reaction efficiency, opening a new avenue for the rational design of atomically dispersed photocatalysts with high efficiency.

Funder

National Science Fund for Distinguished Young Scholars

Natural Science Foundation of Shanxi Province

Youth Innovation Promotion Association of the Chinese Academy of Sciences

Fundamental Research Funds for the Central Universities

Publisher

Wiley

Subject

Mechanical Engineering,Mechanics of Materials,General Materials Science

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