Atomic-coherent covalent heterointerface enables full-spectrum photocatalytic H2 evolution coupled with selective organic oxidation

doi:10.1016/j.jmst.2025.07.005

Abstract

Abstract: Photocatalytic H₂ evolution coupled with selective benzyl alcohol oxidation represents a sustainable strategy for simultaneous energy storage and chemical production, yet its efficiency is fundamentally limited by interfacial charge dynamics and insufficient light utilization. We report a breakthrough in dual-functional photocatalysis through an atomic-function level engineered ZnIn₂S₄/ZnCo₂O₄ heterojunction with three key innovations: (1) atomically coherent interface (1.64 % lattice mismatch) via Zn-S-Zn covalent bridges, (2) strong built-in electric field for charge separation, and (3) ZnCo₂O₄-mediated photothermal NIR harvesting. This synergistic design achieves record-breaking performance (92.7 mmol g^-1 h^-1 H₂ + 72.9 mmol g^-1 h^-1 benzaldehyde) by simultaneously solving three fundamental limitations in conventional systems: charge recombination, narrow light absorption, and slow kinetics. Our work establishes new principles for solar-driven chemical synthesis through interfacial atomic control coupled with photothermal engineering.

Key words: Lattice-matched heterojunction, Photothermal photocatalysis, ZnIn₂S₄, ZnCo₂O₄, Solar-to-chemical conversion

Yuxin Wang, Shuhan Sun, Qianmin Fan, Nikolay Sirotkin, Alexander Agafonov, Huayue Zhu, Yuan Teng, Binbin Yu, Guijie Liang, Xianqiang Xiong. Atomic-coherent covalent heterointerface enables full-spectrum photocatalytic H₂ evolution coupled with selective organic oxidation[J]. J. Mater. Sci. Technol., 2026, 251: 135-148.

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Atomic-coherent covalent heterointerface enables full-spectrum photocatalytic H₂ evolution coupled with selective organic oxidation

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