用于高效光催化产H2O2的S型In2S3/HOF异质结

doi:10.1016/S1872-2067(26)65018-8

催化学报 ›› 2026, Vol. 84: 261-273.DOI: 10.1016/S1872-2067(26)65018-8

用于高效光催化产H₂O₂的S型In₂S₃/HOF异质结

张勇^a, 朱文君^a(), 赵艳艳^b, 张淑敏^c

^a 湖北理工学院新材料与绿色化工学院, 高分子材料化学助剂湖北省工程研究中心, 湖北黄石 435003
^b 商洛学院生物医药与食品工程学院, 陕西商洛 726000
^c 长沙学院环境光催化应用技术湖南省重点实验室, 湖南长沙 410022

收稿日期:2026-01-15 接受日期:2026-02-02 出版日期:2026-05-18 发布日期:2026-04-16
通讯作者: *电子信箱: wjzhu2000@163.com (朱文君).
基金资助:
国家自然科学基金(22378103);国家自然科学基金(22409128);国家自然科学基金(22508019);湖南省教育厅科学研究项目(24B0787);湖北省科技厅黄石发展创新联合基金重点项目(2025AFD004)

In₂S₃/HOF S-scheme heterojunction for enhanced photocatalytic H₂O₂ production

Yong Zhang^a, Wenjun Zhu^a(), Yanyan Zhao^b, Shumin Zhang^c

^a School of Advanced Materials and Green Chemical Engineering, Hubei Provincial Engineering Research Center for Chemical Additives of Polymeric Materials, Hubei polytechnic University, Huangshi 435003, Hubei, China
^b College of Biology Pharmacy and Food Engineering, Shangluo University, Shangluo 726000, Shaanxi, China
^c Hunan Key Laboratory of Applied Environmental Photocatalysis, Changsha University, Changsha 410022, Hunan, China

Received:2026-01-15 Accepted:2026-02-02 Online:2026-05-18 Published:2026-04-16
Contact: *E-mail: wjzhu2000@163.com (W. Zhu).
Supported by:
National Natural Science Foundation of China(22378103);National Natural Science Foundation of China(22409128);National Natural Science Foundation of China(22508019);Research Foundation Bureau of Hunan Province(24B0787);Hubei Provincial Natural Science Foundation Innovation and Development Joint Fund Key Project of Huangshi(2025AFD004)

摘要/Abstract

摘要：

作为一种多功能绿色氧化剂, 过氧化氢(H₂O₂)广泛应用于有机合成、消毒、废水处理等众多领域. 工业上大规模制备H₂O₂多采用蒽醌氧化法, 但该方法能耗高、污染大,不符合绿色化工生产理念. 半导体光催化产H₂O₂是一种绿色和可持续的技术, 对其进行开发具有重要的环境、经济与能源战略意义. 氢键有机框架(HOF)是一种新兴的多孔有机晶体材料, 被认为是光催化产H₂O₂的理想候选催化剂之一. 然而, 由于氢键等分子间作用力较弱, 导致大多数HOF稳定性欠佳, 且单组分HOF存在光生载流子快速复合等弊端, 严重限制了它在光催化产H₂O₂领域中的应用. 选用高稳定性的HOF材料与无机物复合, 构建S型异质结光催化剂, 可有效解决上述问题.

本文采用湿化学方法在高度稳定的HOF(PFC-1)纳米棒表面原位生长了In₂S₃纳米片, 得到了一种新型的无机/有机S型异质结In₂S₃/PFC-1(IP). 在可见光照射下, 以苯甲醇为牺牲剂, 最优复合材料IP-40实现了3.78 mmol g^‒1 h^‒1的光催化产H₂O₂速率, 分别是In₂S₃和PFC-1的2.9倍和3.7倍. IP-40不仅具有较高的热稳定性, 而且在光催化循环测试中表现出良好的化学稳定性. IP-40还具有增强的可见光吸收能力、丰富的活性位点和高效的电荷分离和转移效率，这使得其获得了显著提升的光催化性能. 此外, IP-40的优异氧气吸附能力、适中的质子亲和力和疏水性协同优化了表面反应动力学, 这也有助于提高其光催化产H₂O₂的性能. 通过原位辐照X射线光电子能谱和飞秒瞬态吸收光谱阐明了S型异质结IP的电荷转移机理. 电子顺磁共振光谱和原位红外光谱均检测到了IP-40在光催化过程中的超氧阴离子自由基的信号, 旋转圆盘电极实验测得其电子转移数约为2.11, 这证实了IP-40在光催化产H₂O₂过程中经历了两步单电子氧气还原路径. IP-40在不同条件下光催化产H₂O₂的对比实验表明, 氧气在光催化产H₂O₂的过程中是不可或缺的, 光生电子和超氧阴离子自由基在光催化过程中起着至关重要的作用, 它们是参与H₂O₂生成的主要活性物种. 密度泛函理论计算揭示, 在光催化产H₂O₂的反应路径中, 氧气吸附和两步质子化过程在热力学上是有利的, 而H₂O₂在IP-40催化剂表面上的解吸是光催化反应中的决速步骤.

综上, 合理构建S型异质结是提高其光催化性能的行之有效策略. 本文详细研究了一种无机/有机S型异质结, 该材料在增强光催化过氧化氢生产方面表现出优异性能. 这项工作为设计高效稳定的HOF基光催化剂提供了重要参考.

关键词: 氢键有机框架, 三硫化二铟, S型光催化剂, 氧气还原, 光催化产过氧化氢

Abstract:

As an emerging crystalline porous material, hydrogen bonded organic frameworks (HOFs) have enormous potential in photocatalytic field. However, poor stability and rapid recombination of photogenerated charges hinder their practical application in photocatalytic H₂O₂ production. To address the above challenges, this work employs a wet chemical method to grow In₂S₃ nanosheets in situ on the surface of highly stable HOF nanorods (PFC-1), resulting in a novel inorganic/organic In₂S₃/PFC-1 (IP) S-scheme heterojunction. The optimal IP composite achieves a significantly improved photocatalytic H₂O₂ evolution rate of 3.78 mmol g^‒1 h^‒1, which is 2.9- and 3.7-fold than that of In₂S₃ and PFC-1, respectively. The elevated visible-light absorption, abundant active sites, and effective charge separation of IP S-scheme heterojunction result in the improvement in photocatalytic performance. Additionally, photocatalytic H₂O₂ production of IP goes through a two-electron O₂ reduction reaction pathway. This work offers a novel strategy for the fabrication of efficient HOF-based S-scheme heterostructures and their application in photocatalytic field.

Key words: Hydrogen-bonded organic frameworks, In₂S₃, S-scheme photocatalyst, O₂ reduction, Photocatalytic H₂O₂ production

张勇, 朱文君, 赵艳艳, 张淑敏. 用于高效光催化产H₂O₂的S型In₂S₃/HOF异质结[J]. 催化学报, 2026, 84: 261-273.

Yong Zhang, Wenjun Zhu, Yanyan Zhao, Shumin Zhang. In₂S₃/HOF S-scheme heterojunction for enhanced photocatalytic H₂O₂ production[J]. Chinese Journal of Catalysis, 2026, 84: 261-273.

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链接本文: https://www.cjcatal.com/CN/10.1016/S1872-2067(26)65018-8

https://www.cjcatal.com/CN/Y2026/V84/I5/261

图/表 8

Fig. 1. (a) Schematics for the fabrication of IP S-scheme heterostructure. TEM images of In2S3 (b), PFC-1 (c), and IP-40 (d). (e) HRTEM image of IP-40 in the selected area. (f) EDS mapping images of IP-40.

Fig. 2. XRD patterns (a), FTIR spectra (b), and TGA curves (c) of the samples. (d) N2 adsorption-desorption isotherms of In2S3, PFC-1, and IP-40, the inset shows pore size distribution.

Fig. 3. (a) UV-vis DRS spectra of the as-prepared samples. Mott-Schottky plots of In2S3 (b) and PFC-1 (c). (d) Band diagrams of In2S3 and PFC-1.

Fig. 4. (a) ISI-XPS spectra of In 3d for In2S3 and IP-40. (b) ISI-XPS spectra of O 1s for PFC-1 and IP-40. DFT calculated work functions of In2S3 (c) and PFC-1 (d). (e) Schematics of IP S-scheme heterojunction mechanism.

Fig. 5. Pseudocolor fs-TAS plots of In2S3 (a), PFC-1 (b), and IP-40 (c) using a 380 nm pump pulse. Normalized fs-TAS decay kinetics of In2S3 and IP-40 at 460 nm (d), and PFC-1 and IP-40 at 540 nm (e). (f) Schematic for the decay pathways of photogenerated electrons in IP S-scheme heterojunction.

Fig. 6. (a) Photocatalytic H2O2 production In2S3, PFC-1, and IP composites. (b) Cyclic measurements of IP-40 for photocatalytic H2O2 evolution. (c) H2O2 decomposition of In2S3, PFC-1, and IP composites. (d) Kf and Kd for photocatalytic H2O2 production.

Fig. 7. Photocurrent curves (a), EIS spectra (b), and TRPL spectra (c) of PFC-1, In2S3 and IP-40. (d) Photocatalytic H2O2 evolution rate of IP-40 under different conditions. (e) DMPO-?O2- signals of PFC-1, In2S3 and IP-40 in methanol after 5 min irradiation. (f) Koutechy-Levich plots of PFC-1, In2S3 and IP-40 at -1 V versus Ag/AgCl.

Fig. 8. In-situ DRIFTS on IP-40 under dark (a) and irradiation (b) for 60 min. (c) The free energy diagram of ORR pathway toward H2O2 production over IP S-scheme heterojunction. (d) Proposed mechanism of photocatalytic H2O2 production by IP S-scheme heterojunction.

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用于高效光催化产H₂O₂的S型In₂S₃/HOF异质结

In₂S₃/HOF S-scheme heterojunction for enhanced photocatalytic H₂O₂ production

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