Single‐Atom Co‐Ultrafine RuOx Clusters Codecorated TiO2 Nanosheets Promote Photocatalytic Hydrogen Evolution: Modulating Charge Migration, H+ Adsorption, and H2 Desorption of Active Sites

Author:

Shen Jiachao1,Luo Chenghui1,Qiao Shanshan2,Chen Yuqing1,Fu Kaixing1,Xu Jieqiong1,Pei Junjun1,Tang Yanhong2,Zhang Xiaolong3,Tang Haifang1,Zhang Hao4,Liu Chengbin1ORCID

Affiliation:

1. State Key Laboratory of Chemo/Biosensing and Chemometrics Advanced Catalytic Engineering Research Center of the Ministry of Education College of Chemistry and Chemical Engineering Hunan University Changsha 410082 P. R. China

2. College of Materials Science and Engineering Hunan University Changsha 410082 P. R. China

3. Division of Nanomaterials & Chemistry Hefei National Laboratory for Physical Sciences at the Microscale University of Science and Technology of China Hefei Anhui 230026 P. R. China

4. Institute of Functional Nano & Soft Materials (FUNSOM) Jiangsu Key Laboratory for Carbon‐Based Functional Materials & Devices Collaborative Innovation Center of Suzhou Nano Science & Technology Soochow University Suzhou Jiangsu 215123 P. R. China

Abstract

AbstractRu as a cocatalyst has attracted wide attention as a substitute for Pt precious metal. However, the strong interaction between Ru and H atoms reduces the efficiency of hydrogen (H2) desorption and slows the overall hydrogen evolution reaction (HER) efficiency. How to further improve the efficiency of Ru‐based cocatalyst is challenging. Herein, single‐atom Co‐ultrafine RuOx clusters codecorated TiO2 nanosheets for photocatalytic HER are synthesized using a simple hydrothermal–calcination method. Experiments and theoretical calculations demonstrate that Co atoms can serve as a specific electronic medium, promoting electron enrichment at RuOx, thereby enhancing the adsorption of H+. Moreover, the electronic state of the interaction between adjacent Co atoms and RuOx is conducive to the desorption of H2. As a result, the proposed photocatalyst system gives a classy photocatalytic HER performance. The hydrogen production rate at stationary point reaches up to 20.20 mmol g−1 h−1, and the apparent quantum yield at 365 nm is 86.5%. It is worth noting that the hydrogen production rate in seawater is as high as 9.83 mmol g−1 h−1. This work offers precise guidance to design catalysts for efficient photocatalytic H2 production from the in‐depth understanding of the electronic coupling effect of coupling active sites.

Publisher

Wiley

Subject

Electrochemistry,Condensed Matter Physics,Biomaterials,Electronic, Optical and Magnetic Materials

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