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Developing Photosensitizer-Cobaloxime Hybrids for Solar-Driven H2 Production in Aqueous Aerobic Conditions

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Dynamic Valence-State-Adaptive Ta Single-Atom Sites for Artificial H₂O₂ Photosynthesis.

Xu Zhang¹, Ying Tao², Chenyu Yang³

¹Department of Materials Science and Engineering, City University of Hong Kong, Hong Kong SAR 999077, China.

Journal of the American Chemical Society

|July 1, 2026

Summary

Tantalum single-atom sites on carbon nitride efficiently catalyze hydrogen peroxide (H₂O₂) synthesis using visible light. This breakthrough in photocatalysis optimizes oxygen activation for clean H₂O₂ production.

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Probe Type II Band Alignment in One-Dimensional Van Der Waals Heterostructures Using First-Principles Calculations

Published on: October 12, 2019

Area of Science:

Photocatalysis
Green Chemistry
Materials Science

Background:

The synthesis of hydrogen peroxide (H₂O₂) via the two-electron oxygen reduction reaction (2e^- ORR) is crucial for sustainable chemical production.
Understanding the atomic-scale mechanisms of excited-state electron behavior and *in situ* oxygen activation in photocatalysis is essential but remains challenging.

Purpose of the Study:

To identify optimal single-atom catalysts for H₂O₂ photosynthesis.
To elucidate the dynamic interplay between active sites, excited-state electrons, and *in situ* O₂ activation at the atomic level.

Main Methods:

Mechanism-guided integrated strategy combining theoretical screening and experimental construction.
Utilizing *in situ* characterization techniques (e.g., spectroscopy) and theoretical calculations.
Identifying tantalum (Ta) single-atom sites on carbon nitride as active centers.

Main Results:

Achieved an apparent quantum yield of 14.53% at 420 nm and 1.12% solar-to-chemical efficiency for H₂O₂ production in pure water.
Demonstrated dynamic valence-state evolution of Ta single-atom sites (+4.16 → +4.37 → +3.14) facilitating O₂ adsorption and activation.
Revealed Ta 5d-O 2p orbital coupling driving end-on O₂ activation and *OOH-mediated H₂O₂ formation.

Conclusions:

Tantalum single-atom sites are optimal 5d metal centers on carbon nitride for H₂O₂ photosynthesis.
Dynamic active site adaptation is key to efficient photocatalytic H₂O₂ synthesis.
Established a framework for designing adaptive single-atom catalysts for artificial photosynthesis.