S型共价有机框架/Ni-ZIF-8异质结的构筑及其光催化制氢性能

doi:10.1016/S1872-2067(25)64826-1

催化学报 ›› 2026, Vol. 80: 200-212.DOI: 10.1016/S1872-2067(25)64826-1

S型共价有机框架/Ni-ZIF-8异质结的构筑及其光催化制氢性能

张璇^,¹, 周林^,¹, 闫腾, 张晓虎(), 陈浩()

华中农业大学化学学院, 湖北武汉 430070

收稿日期:2025-05-19 接受日期:2025-07-24 出版日期:2026-01-18 发布日期:2026-01-05
通讯作者: 张晓虎,陈浩
作者简介:第一联系人：¹共同第一作者
基金资助:
国家自然科学基金(52372081);国家自然科学基金(52073110);中央高校基本科研业务费(2662024JC013);中央高校基本科研业务费(2662023LXPY002)

Fabrication of S-scheme heterojunction between covalent organic frameworks and Ni-ZIF-8 and its photocatalytic hydrogen production performance

Xuan Zhang^,¹, Lin Zhou^,¹, Teng Yan, Xiaohu Zhang(), Hao Chen()

College of Chemistry, Huazhong Agricultural University, Wuhan 430070, Hubei, China

Received:2025-05-19 Accepted:2025-07-24 Online:2026-01-18 Published:2026-01-05
Contact: Xiaohu Zhang, Hao Chen
About author:First author contact:¹These authors contributed equally.
Supported by:
National Natural Science Foundation of China(52372081);National Natural Science Foundation of China(52073110);Fundamental Research Funds for the Central Universities(2662024JC013);Fundamental Research Funds for the Central Universities(2662023LXPY002)

摘要/Abstract

摘要：

随着能源危机与环境污染问题日益严峻, 发展高效光催化制氢技术对实现碳中和目标具有重要意义. 共价有机框架(COFs)因其可调能带结构、高比表面积和优异光吸收能力成为理想光催化剂, 但其光生载流子复合率高的问题严重制约实际应用. 金属有机框架(MOFs)衍生物虽具结构可调性, 却面临导电性差和稳定性不足的挑战. 本文巧妙的将COF与镍掺杂沸石咪唑酯框架(Ni-ZIF-8), 成功构建S型异质结, 并对其光催化制氢性能进行研究.

本研究通过静电自组装策略构建了芘基共价有机框架(Py-COF)与镍掺杂沸石咪唑酯框架(Ni(30%)-ZIF-8)的S型异质结(Py-COF-[Ni(30%)-ZIF8]-10: 1). 创新设计依托于材料表面Zeta电位差异(Py-COF: -13.3 mV; Ni-ZIF8: +16.9 mV)驱动自组装, 实现紧密界面结合. X射线衍射(XRD)等表征证实了溶剂热法合成的高结晶度Py-COF (AA堆叠, 比表面积1373.4 m²·g^‒1)与表面选择性镍掺杂的Ni-ZIF-8成功复合, 异质结同时保留Py-COF与Ni-ZIF-8的晶面结构. 复合材料的比表面积提升至1731.5 m²·g^‒1. 光催化制氢性能测试表明异质结的最高产氢速率达162.77 mmol·g^-1·h^-1, 表观量子效率在450 nm处达4.18%, 且循环12 h后活性无衰减. 红外光谱与XRD证实反应后复合催化材料的化学结构与晶型保持完整, 紫外-可见光漫反射光谱显示光吸收特性保持稳定. 通过原位X射线光电子能谱揭示了S型异质结的电子转移方向, 光照下Py-COF的N 1s结合能升高, 而Ni-ZIF-8的Zn 2p结合能降低, 直接证实电子从Py-COF迁移向Ni-ZIF-8. 该过程促使Py-COF的光生电子与Ni-ZIF-8的空穴复合, 同时保留Ni-ZIF-8导带中的高能电子参与H⁺还原, Py-COF价带空穴则被抗坏血酸消耗. 荧光光谱显示异质结荧光强度显著降低, 瞬态荧光光谱证实载流子寿命延长, 结合电化学阻抗谱揭示的电荷转移电阻降低, 多种表征共同验证了S型异质结通过定向电荷分离提高电子利用率的核心机制.

综上, 本工作设计了双金属MOF/COF基S型异质结光催化剂, 为突破有机半导体电荷分离瓶颈提供了新范式. 未来可进一步拓展至多元金属掺杂体系及全光谱响应材料设计, 推动光催化制氢技术向实际应用转化. 该研究为开发高效、稳定的清洁能源转换材料奠定了重要科学基础.

关键词: 共价有机框架, 镍掺杂沸石咪唑酯框架, S型异质结, 光催化, 制氢

Abstract:

Covalent organic frameworks (COFs) have garnered significant attention in photocatalysis owing to their exceptional light absorption capacities, tunable band structures, and high specific surface areas. However, the rapid recombination of photogenerated carriers in COFs remains a critical bottleneck limiting their practical application. In this study, a novel S-scheme heterojunction was constructed by integrating a Ni-doped zeolitic imidazolate framework-8 (Ni-ZIF-8) with Py-COF, effectively addressing this challenge. Through precisely controlled synthesis, the heterojunction achieves efficient and stable material combination, which not only significantly enhances photogenerated charge separation efficiency and markedly reduces recombination rates, but also demonstrates outstanding catalytic performance (162.77 mmol·h^-1·g^-1) and cycling stability in hydrogen evolution reaction. This study provides new insights into the design of efficient ZIF/COF-based heterojunction catalysts. This study provides an important theoretical foundation for the design of high-performance photocatalytic materials with broad application prospects.

Key words: Covalent organic frameworks, Ni-doped zeolitic imidazolate framework, S-scheme heterojunction, Photocatalytic, Hydrogen production

张璇, 周林, 闫腾, 张晓虎, 陈浩. S型共价有机框架/Ni-ZIF-8异质结的构筑及其光催化制氢性能[J]. 催化学报, 2026, 80: 200-212.

Xuan Zhang, Lin Zhou, Teng Yan, Xiaohu Zhang, Hao Chen. Fabrication of S-scheme heterojunction between covalent organic frameworks and Ni-ZIF-8 and its photocatalytic hydrogen production performance[J]. Chinese Journal of Catalysis, 2026, 80: 200-212.

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链接本文: https://www.cjcatal.com/CN/10.1016/S1872-2067(25)64826-1

https://www.cjcatal.com/CN/Y2026/V80/I1/200

图/表 13

Fig. 1. Synthesis of Py-COF.

Fig. 2. Synthesis of Ni-ZIF-8.

Fig. 3. Schematic diagram of Py-COF-[Ni(x%)-ZIF8]-y:z.

Fig. 4. (a) FT-IR spectra of Py-COF, TFPPY and BD. (c) 13C SS NMR of Py-COF (b), PXRD patterns and refined profiles of Py-COF. (d) XRD patterns of Ni-ZIF-8, Ni(15%)-ZIF8, Ni(30%)-ZIF8 and Ni(45%)-ZIF8. XRD patterns (e) and FT-IR spectra (f) of Py-COF, Ni(30%)-ZIF8 and Py-COF-[Ni(30%)-ZIF8]-10:1.

Fig. 5. (a) The SEM images of Py-COF. (b) The SEM images and TEM-mapping of Ni(30%)-ZIF8. (c) The SEM images of Py-COF-[Ni(30%)-ZIF8]-10:1. The TEM images of Py-COF (d), Ni(30%)-ZIF8 (e), and Py-COF-[Ni(30%)-ZIF8]-10:1 (f).

Fig. 6. The XPS survey spectrum (a), high-resolution XPS spectra of C 1s (b) and N 1s (c) for Py-COF, Ni(30%)-ZIF8 and Py-COF-[Ni(30%)-ZIF8]-10:1. (d) XPS spectra of Zn 2p for Ni(30%)-ZIF8 and Py-COF-[Ni(30%)-ZIF8]-10:1.

Fig. 7. (a) Comparison of photocatalytic H2 production activity of Py-COF, ZIF-8, Ni-ZIF-8, Ni(45%)-ZIF8, Py-COF-ZIF8]-10:1 and Py-COF-[Ni(45%)-ZIF8]-10:1. The effects of COF/Ni-ZIF-8 mass ratio (b) and Ni loading (c) on the performance of Py-COF-[Ni(30%)-ZIF8]-10:1. Influence of sacrificial reagent types (d), the influence of catalyst quality (e) and AA concentration (f) on the hydrogen production performance of Py-COF-[Ni(30%)-ZIF8]-10:1.

Fig. 8. (a) AQY test of Py-COF-[Ni(30%)-ZIF8]-10:1. (b) Comparison of properties of COFs-based heterojunctions in the literature.

Fig. 9. Cyclic stability tests (a), FT-IR (b), XRD (c) and UV-vis DRS (d) before and after reaction of Py-COF-[Ni(30%)-ZIF8]-10:1.

Fig. 10. UV-vis DRS spectra of Ni(30%)-ZIF8 (a) and, Py-COF and Py-COF-[Ni(30%)-ZIF8]-10:1 (b). (c) Tauc images of Py-COF. M-S images of Ni(30%)-ZIF8 (d) and Py-COF (e). (f) The suitable bandgap between the Py-COF and Ni(30%)-ZIF8 rendered it possible to build up S-schemed heterojunction.

Fig. 11. Transient photocurrent test (a) and EIS Nyquist plots (b) of Ni(30%)-ZIF8, Py-COF, Py-COF-[Ni(30%)-ZIF8]-10:1. (c) PL spectra of Py-COF and hybrid samples comprising Py-COF combined with [Ni(15%)-ZIF-8], [Ni(30%)-ZIF-8], and [Ni(45%)-ZIF-8] at varying ratios.

Fig. 12. In-situ XPS spectra of N 1s (a) and Zn 2p (b) over Py-COF-[Ni(30%)-ZIF8]-10:1.

Fig. 13. Schematic diagram of the photocatalytic hydrogen production mechanism of Py-COF-[Ni(30%)-ZIF8]-10:1.

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S型共价有机框架/Ni-ZIF-8异质结的构筑及其光催化制氢性能

Fabrication of S-scheme heterojunction between covalent organic frameworks and Ni-ZIF-8 and its photocatalytic hydrogen production performance

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