Issue 28, 2025

Multi-hydrogen adsorption of amorphous ReSx cocatalysts for boosting photocatalytic hydrogen evolution

Abstract

An ideal H2-evolution cocatalyst must achieve near-balanced hydrogen adsorption/desorption energetics at active sites to promote H2-evolution kinetics, yet existing cocatalysts typically exhibit imbalanced H adsorption (either too strong or too weak) that severely compromises their hydrogen-evolution performance. Moving beyond conventional electronic structure modulation approaches involving doping or heterojunctions, we demonstrate a synergistic hydrogen-evolution mechanism of multi-hydrogen adsorption, namely multi-hydrogen adsorption on cocatalyst surfaces can effectively balance H* adsorption/desorption, dramatically enhancing photocatalytic hydrogen production. For this purpose, the ReSx/TiO2 photocatalyst is prepared by loading sulfur-rich amorphous ReSx with multiple S active sites onto TiO2. The optimized ReSx/TiO2(1 : 10) achieves an exceptional photocatalytic hydrogen-evolution rate of 9.9 mmol g−1 h−1, which is 2.1 times higher than the crystalline c-ReS2/TiO2. Combined experimental and theoretical investigations reveal the multi-hydrogen adsorption mechanism: (1) the multi-hydrogen adsorption effectively lowers the p-band center of active S sites in the ReSx cocatalyst, increasing antibonding state occupancy, thereby greatly weakening S–Hads bond strength; (2) in situ XPS and KPFM verify efficient photogenerated electron transfer from TiO2 to ReSx for a rapid H2 evolution reaction. These findings fundamentally advance the understanding of multi-site adsorption effects in photocatalysis and establish new design principles for high-performance photocatalytic systems.

Graphical abstract: Multi-hydrogen adsorption of amorphous ReSx cocatalysts for boosting photocatalytic hydrogen evolution

Supplementary files

Article information

Article type
Paper
Submitted
07 May 2025
Accepted
14 Jun 2025
First published
24 Jun 2025

J. Mater. Chem. A, 2025,13, 23104-23112

Multi-hydrogen adsorption of amorphous ReSx cocatalysts for boosting photocatalytic hydrogen evolution

K. Gan, D. Gao, X. Yin, C. Bie, L. Zhang, J. Yu and H. Yu, J. Mater. Chem. A, 2025, 13, 23104 DOI: 10.1039/D5TA03629A

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