Key Takeaways & Executive Findings
- •• • [email protected] achieves a photocatalytic hydrogen evolution rate of 3789.45 μmol g−1 h−1, which is 4.4 times higher than pristine ZIS (859.57 μmol g−1 h−1) and 264.4 times higher than FIR-125 (15.32 μmol g−1 h−1), demonstrating a significant performance leap for precious-metal-free photocatalysts. • • The heterojunction exhibits exceptional stability, retaining performance over five consecutive cycles and 16 hours of continuous reaction, with no significant loss of activity, color, or morphology, indicating robust structural integrity for long-term operation. • • The optimized [email protected] composition balances light absorption, carrier separation, and surface reaction, as evidenced by the lowest exciton binding energy (Eb) among the F@Z-X series, which directly correlates with the highest carrier separation efficiency (η2). • • The core-shell heterojunction design, with in-situ growth of ZIS nanosheets on FIR-125, creates abundant intimate contact interfaces and well-matched band structures, which are critical for efficient charge transfer and enhanced photocatalytic activity.
Abstract
Photocatalytic hydrogen evolution reaction (HER) from pure water is a promising strategy to address critical challenges in energy sustainability and environmental remediation. However, HER over single-component photocatalysts is intrinsically limited by inefficient carrier separation and relatively poor photostability. Forming abundant interfaces between two components is an effective approach for solving these issues. Herein, a series of hierarchical core-shell heterojunction photocatalysts, designated as F@Z-X, was rationally constructed by in situ growing ZnIn2S4 (ZIS) nanosheets on a Ti-based metal-organic framework (FIR-125), demonstrating remarkable structural stability. Due to the abundant intimate contact interfaces and well-matched band structure, the F@Z-X series exhibit enhanced HER performance. Among them, the optimized heterojunction [email protected] shows a photocatalytic hydrogen evolution rate of 3789.45 μmol g−1 h−1, which is about 4.4 and 264.4 times higher than that of pristine ZIS (859.57 μmol g−1 h−1) and FIR-125 (15.32 μmol g−1 h−1), respectively. Moreover, the photocatalyst manifests excellent reusability and durability, maintaining its performance over five consecutive cycles and sixteen hours of continuous reaction. The outstanding performance of [email protected] may be ascribed to an optimal balance among three fundamental photocatalytic processes: sufficient light absorption, exceptional carrier separation, and appropriate surface reaction. This work offers valuable insights into the rational design and controllable synthesis of novel heterojunction photocatalysts for efficient hydrogen evolution.
1. Introduction
Photocatalytic hydrogen evolution from pure water is a compelling route to renewable energy, yet its practical viability is constrained by thermodynamic and kinetic barriers. The decomposition of water requires a substantial energy input (ΔG° = 237.2 kJ mol−1), and catalysts must overcome overpotentials to drive the reaction. Single-component photocatalysts, such as metal oxides or sulfides, suffer from rapid recombination of photogenerated electron-hole pairs and poor photostability, limiting their efficiency. For instance, pristine ZnIn2S4 (ZIS), a promising ternary chalcogenide with a tunable bandgap (2.06–2.85 eV) suitable for visible-light absorption, still exhibits suboptimal hydrogen evolution rates due to inefficient carrier separation.
To address these bottlenecks, constructing heterojunctions between two semiconductors with well-matched band structures is an effective strategy to enhance charge separation and stability. This work presents a core-shell heterojunction by in-situ growing ZIS nanosheets on a Ti-based metal-organic framework (FIR-125). The intimate contact interfaces and synergistic effects between the two components aim to optimize light absorption, carrier dynamics, and surface reaction kinetics. The resulting F@Z-X series, particularly [email protected], demonstrates a remarkable hydrogen evolution rate of 3789.45 μmol g−1 h−1, far surpassing pristine components and many reported MOF-based heterojunctions, while maintaining excellent stability over extended operation.
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Hang Lei, Jieping Zhang, Zhiyuan Wu, Wenqiu Qi, Mengyue Zhang, Zhijia Li, Lian Chen, Maochun Hong (2026). In-situ growth of ZnIn2S4 nanosheets on a Ti-based MOF to form a core-shell heterojunction for enhanced photocatalytic hydrogen evolution. SCIENCE CHINA Materials. https://doi.org/10.1007/s40843-025-3875-1
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Frequently Asked Questions
What is the specific role of the Ti-based MOF (FIR-125) in enhancing the photocatalytic activity of the heterojunction?
FIR-125 acts as a structural support and participates in forming a type-II or Z-scheme heterojunction with ZIS, facilitating charge separation. The intimate contact interfaces reduce charge recombination, as evidenced by the lower exciton binding energy in [email protected], leading to enhanced carrier separation efficiency.
How does the [email protected] performance compare to state-of-the-art photocatalysts, and what are the advantages over Pt-based systems?
[email protected] achieves a hydrogen evolution rate of 3789.45 μmol g−1 h−1, which is superior to Pt/ZIS and many other MOF-ZIS heterojunctions. Being precious-metal-free, it offers a cost-effective alternative without compromising activity or stability.
What are the key factors contributing to the optimal performance at [email protected] composition?
The optimal balance among light absorption, carrier separation, and surface reaction is achieved at a medium FIR-125 to ZIS mass ratio. This composition exhibits the lowest exciton binding energy, indicating the highest carrier separation efficiency, while maintaining sufficient light absorption and surface active sites.
What is the long-term stability of [email protected] under continuous operation, and are there any signs of deactivation?
[email protected] maintains its performance over five consecutive cycles and 16 hours of continuous reaction without significant loss of activity, color, or morphology, indicating excellent photostability and structural integrity.
What are the potential scalability and cost implications of this synthesis method for industrial application?
The in-situ growth method is relatively simple and uses earth-abundant materials (Zn, In, S, Ti-based MOF), which are cost-effective compared to precious-metal catalysts. The high activity and stability suggest potential for scalable production, though further optimization of synthesis conditions and reactor design is needed.
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