Key Takeaways & Executive Findings
- •• • Achieved an atomically coherent heterointerface with an ultralow lattice mismatch of 0.05%, suppressing trap-mediated recombination and enabling efficient interfacial charge transfer, which is critical for high-performance heterojunction photocatalysts. • • Demonstrated synchronized electron-proton delivery via hydrogen spillover, yielding a photocatalytic H2 evolution rate of 70.3 mmol g−1 h−1, significantly outperforming conventional systems and addressing the bottleneck of asynchronous charge supply. • • Achieved selective oxidation of benzyl alcohol to aldehyde with a rate of 39.3 mmol g−1 h−1 and 93.6% selectivity, showcasing dual functionality for simultaneous H2 production and value-added chemical synthesis. • • Established that lattice matching and dual charge-proton management are essential design principles for efficient PCET, providing a roadmap for developing next-generation photocatalysts for solar-to-chemical energy conversion.
Abstract
Photocatalytic hydrogen production is fundamentally limited by inefficient charge separation and asynchronous supply of electrons and protons to active sites. Here, we designed a ZnIn2S4/ZnCo2S4 (ZIS/ZCS) heterojunction with an atomically coherent interface achieved via an ultralow lattice mismatch of 0.05%. This unique structure promotes rapid electron transfer through a built-in electric field and facilitates continuous proton migration via a hydrogen spillover effect, thereby synchronizing electron and proton delivery at the catalytic interface. This dual regulation of electrons and protons synergistically promotes proton-coupled electron transfer, resulting in a high hydrogen evolution rate of 70.3 mmol g−1 h−1 and selective oxidation of benzyl alcohol to aldehyde (39.3 mmol g−1 h−1) with 93.6% selectivity. This work demonstrates the critical importance of lattice match and dual charge-proton management in designing efficient photocatalysts for complex redox reactions.
1. Introduction
Photocatalytic hydrogen production offers a carbon-neutral route to sustainable fuels, yet its commercial viability is constrained by inefficient charge-carrier dynamics and sluggish surface reaction kinetics. A critical bottleneck is the asynchronous supply of electrons and protons to active sites, leading to charge recombination and parasitic reactions that severely limit hydrogen evolution efficiency. Conventional heterostructures often suffer from large lattice mismatches, creating incoherent interfaces with dangling bonds and trap states that promote non-radiative recombination and hinder interfacial charge transfer. This has stalled progress in achieving high-performance photocatalysts for practical solar fuel generation.
This work addresses these limitations by engineering a ZnIn2S4/ZnCo2S4 heterojunction with an atomically coherent interface, achieving an ultralow lattice mismatch of 0.05%. This precise atomic alignment minimizes defect density, suppresses trap-mediated recombination, and facilitates rapid electron transfer via a built-in electric field. Simultaneously, the hydrogen spillover effect enables continuous proton migration to the catalytic sites, synchronizing electron and proton delivery. This dual regulation of charge and proton transport promotes efficient proton-coupled electron transfer, resulting in exceptional hydrogen evolution rates and selective benzyl alcohol oxidation. The findings underscore the critical importance of lattice match and dual charge-proton management in designing efficient photocatalysts for complex redox reactions.
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Shuhan Sun, Yuxin Wang, Song Wang, Die Li, Yanxian Jin, Chenglin Wu, Gaowei Hu, Zhanfeng Li, Xiao Zhang, Xianqiang Xiong (2026). Interfacial hydrogen spillover and coherent lattice matching in ZnIn2S4/ZnCo2S4 enable synchronized electron-proton delivery for efficient photocatalytic H2 evolution. SCIENCE CHINA Materials. https://doi.org/10.1007/s40843-025-3889-6
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Frequently Asked Questions
What is the specific lattice mismatch value and how does it influence the interfacial charge transfer efficiency?
The ZIS/ZCS heterojunction achieves an ultralow lattice mismatch of 0.05%, which is critical for forming an atomically coherent interface. This minimizes dangling bonds and trap states, thereby suppressing non-radiative recombination and enabling rapid, directional electron transfer across the heterointerface, as evidenced by the high H2 evolution rate of 70.3 mmol g−1 h−1.
How does the hydrogen spillover effect contribute to the synchronized supply of protons and electrons?
The hydrogen spillover effect facilitates continuous proton migration from the hydrogen-adsorbing activator to the catalytic sites, ensuring a steady proton supply. This, combined with the built-in electric field that drives rapid electron transfer, synchronizes electron and proton delivery, which is essential for efficient proton-coupled electron transfer and high photocatalytic performance.
What are the measured rates for H2 evolution and benzyl alcohol oxidation, and what is the selectivity?
The ZIS/ZCS heterojunction exhibits a hydrogen evolution rate of 70.3 mmol g−1 h−1 and a benzyl alcohol oxidation rate of 39.3 mmol g−1 h−1, with 93.6% selectivity for aldehyde formation. These metrics demonstrate the catalyst's dual functionality and high efficiency for simultaneous H2 production and value-added chemical synthesis.
What are the potential scalability challenges for this photocatalyst system?
Scalability challenges include the need for precise control over the heterointerface lattice matching during large-scale synthesis, as well as the cost and availability of precursor materials. Additionally, maintaining the high selectivity and activity under continuous operation and real-world solar irradiation conditions requires further optimization. However, the demonstrated high rates and selectivity suggest promising potential for scale-up if these engineering challenges are addressed.
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