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Single‐Atom Co‐Ultrafine RuO<i><sub>x</sub></i> Clusters Codecorated TiO<sub>2</sub> Nanosheets Promote Photocatalytic Hydrogen Evolution: Modulating Charge Migration, H<sup>+</sup> Adsorption, and H<sub>2</sub> Desorption of Active Sites

Jiachao Shen, Chenghui Luo, Shanshan Qiao, Yuqing Chen, Kaixing Fu, Jieqiong Xu, Junjun Pei, Yanhong Tang, Xiaolong Zhang, Haifang Tang, Hao Zhang, Chengbin Liu

2023Advanced Functional Materials41 citationsDOIOpen Access PDF

Abstract

Abstract Ru 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 (H 2 ) 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 RuO x clusters codecorated TiO 2 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 RuO x , thereby enhancing the adsorption of H + . Moreover, the electronic state of the interaction between adjacent Co atoms and RuO x is conducive to the desorption of H 2 . 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 H 2 production from the in‐depth understanding of the electronic coupling effect of coupling active sites.

Topics & Concepts

Materials sciencePhotocatalysisDesorptionHydrogen productionPhotocatalytic water splittingCatalysisHydrogenCalcinationAdsorptionHydrogen atomWater splittingNanotechnologyPhysical chemistryChemistryOrganic chemistryAlkylBiochemistryAdvanced Photocatalysis TechniquesCopper-based nanomaterials and applicationsElectrocatalysts for Energy Conversion