Efficient Holes Abstraction by Precisely Decorating Ruthenium Single Atoms and RuO_x Clusters on ZnIn₂S₄ for Photocatalytic Pure Water Splitting

Shuangzhi Wu ¹, Shengyu Zhang ¹, Qingsheng Zhang ¹

⁰National & Local Joint Engineering Research Center for Applied Technology of Hybrid Nanomaterials, Henan University, Kaifeng, Henan, 475004, China.

Small (weinheim an Der Bergstrasse, Germany) +

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July 23, 2024

View abstract on PubMed

Summary

This study introduces a novel photocatalyst, RuO<sub>x</sub>/Ru-ZIS, for efficient two-electron water splitting. It significantly enhances hydrogen (H<sub>2</sub>) and hydrogen peroxide (H<sub>2</sub>O<sub>2</sub>) generation by improving charge utilization.

Area Of Science

Materials Science
Photocatalysis
Green Chemistry

Background

Two-electron water splitting for H<sub>2</sub>O<sub>2</sub> and H<sub>2</sub> generation is promising but limited by poor charge utilization, especially slow hole transfer.
Developing efficient photocatalysts is crucial for practical applications in clean energy and chemical production.

Purpose Of The Study

To design and synthesize a novel photocatalyst for efficient two-electron water splitting.
To enhance the utilization of photogenerated charges, particularly holes, for improved water oxidation.
To investigate the synergistic effects of single Ru atoms and RuO<sub>x</sub> clusters on ZnIn<sub>2</sub>S<sub>4</sub> for photocatalysis.

Main Methods

Co-decoration of Ru single atoms and RuO<sub>x</sub> clusters on ZnIn<sub>2</sub>S<sub>4</sub> (RuO<sub>x</sub>/Ru-ZIS).
Investigation of electronic structure modification by Ru doping for enhanced hole abstraction.
Utilizing interfacial electric fields from RuO<sub>x</sub> clusters to promote hole migration.
Evaluation of photocatalytic performance under visible light irradiation.

Main Results

Ru single atoms enhance hole abstraction by regulating the electronic structure of ZnIn<sub>2</sub>S<sub>4</sub>.
RuO<sub>x</sub> clusters create an interfacial electric field promoting out-of-plane hole migration.
RuO<sub>x</sub>/Ru-ZIS exhibits excellent H<sub>2</sub> and H<sub>2</sub>O<sub>2</sub> evolution rates of 581.9 and 464.4 µmol g<sup>-1</sup> h<sup>-1</sup>.
Achieved an apparent quantum efficiency (AQE) of 4.36% at 400 nm.

Conclusions

The co-decoration strategy effectively enhances charge utilization and surface water oxidation.
RuO<sub>x</sub>/Ru-ZIS demonstrates superior performance for simultaneous H<sub>2</sub> and H<sub>2</sub>O<sub>2</sub> production via photocatalytic water splitting.
This work offers a new approach to manipulate photocatalysts using single atoms and clusters for improved efficiency.

Keywords:

Ru single atom RuOx cluster ZnIn2S4 holes abstraction pure water splitting