物理化学学报 >> 2025, Vol. 41 >> Issue (11): 100136.doi: 10.1016/j.actphy.2025.100136

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ZIS1−x/UCN S型异质结界面的超快电子转移实现高效H2O2光合成耦合四环素降解

张淑敏1, 王亚琪1, 王泽林1, 王立博2, 安长胜1,*(), 许第发*,1()   

  1. 1 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
    2 中国地质大学(武汉)材料与化学学院太阳能燃料实验室, 湖北 武汉 430078
  • 收稿日期:2025-06-24 修回日期:2025-07-20 录用日期:2025-07-23 发布日期:2025-09-29
  • 通讯作者: Email: z20190628@ccsu.edu.cn. Tel: +86-18932463886 (安长胜)xudifa@sina.com. +86-13687382717 (许第发)
  • 基金资助:
    湖南省教育厅(24B0787); 国家自然科学基金(52204307); 国家自然科学基金(52202376)

Ultrafast electron transfer at the ZIS1−x/UCN S-scheme interface enables efficient H2O2 photosynthesis coupled with tetracycline degradation

Shumin Zhang1, Yaqi Wang1, Zelin Wang1, Libo Wang2, Changsheng An1,*(), Difa Xu*,1()   

  1. 1 Hunan Key Laboratory of Applied Environmental Photocatalysis, Changsha University, Changsha 410022, Hunan Province, China
    2 Laboratory of Solar Fuel, Faculty of Materials Science and Chemistry, China University of Geosciences, Wuhan 430078, Hubei Province, China
  • Received:2025-06-24 Revised:2025-07-20 Accepted:2025-07-23 Published:2025-09-29
  • Contact: Email: z20190628@ccsu.edu.cn. Tel: +86-18932463886 (Changsheng An)xudifa@sina.com. +86-13687382717 (Difa Xu)
  • Supported by:
    the Research Foundation Bureau of Hunan Province(24B0787); the National Natural Science Foundation of China(52204307); the National Natural Science Foundation of China(52202376)

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摘要：

将产过氧化氢与有机污染物降解相结合，不仅能有效克服水氧化反应动力学迟缓的问题，同时还能应对环境污染挑战。在这项工作中，通过在多孔超薄UCN上原位生长ZIS1−x纳米片，构建了一种富含S缺陷的ZnIn2S4/g-C3N4 (ZIS1−x/UCN) S型异质结光催化剂。设计的ZIS1−x/UCN光催化剂表现出增强的可见光吸收、丰富的活性位点和紧密的界面接触。优化后的ZIS1−x/UCN-1.0光催化剂表现出出色的双重功能，同时实现了2902.2 µmol·g−1·h−1的H2O2生成速率和91.3%的四环素(50 mg·L−1)降解效率。与在纯水中的活性(1777.0 µmol·g−1·h−1)相比，H2O2性能提高了1.63倍。通过飞秒瞬态吸收光谱(fs-TAS)、原位X射线光电子能谱(ISI-XPS)和原位X射线吸收精细结构光谱(XAFS)的综合表征，我们证实了S型异质结电荷转移机制。这种S型异质结诱导的独特电子结构不仅促进了界面上的超快电子转移(3.54 ps)，还显著增强了光生载流子的氧化还原能力。总体而言，这项工作为光催化技术在能源生产和环境修复领域的双重应用开辟了新的途径。

关键词: S型异质结, H2O2光合成, 四环素降解, 飞秒瞬态吸收光谱

Abstract:

Coupling H2O2 production with organic pollutant degradation can effectively overcome the sluggish kinetics of water oxidation while concurrently addressing environmental pollution challenges. In this work, an S-defect-rich ZnIn2S4/g-C3N4 (ZIS1−x/UCN) S-scheme heterojunction photocatalyst was constructed by in situ growing ZIS1−x nanosheets on porous ultrathin UCN. The designed ZIS1−x/UCN photocatalyst demonstrates enhanced visible light absorption, abundant active sites, and intimate interfacial contact. The optimized ZIS1−x/UCN-1.0 photocatalyst exhibits outstanding dual functionality, simultaneously achieving an H2O2 production rate of 2902.2 µmol·g−1·h−1 and 91.3% tetracycline (50 mg·L−1) degradation efficiency. This H2O2 performance represents a 1.63-fold enhancement compared to its activity in pure water (1777.0 µmol·g−1·h−1). Through comprehensive characterization including femtosecond transient absorption spectroscopy (fs-TAS), in situ irradiation X-ray photoelectron spectroscopy (ISI-XPS), and in situ X-ray absorption fine structure spectroscopy (XAFS), we unequivocally confirm the S-scheme charge transfer mechanism. This S-scheme induced unique electronic structure not only fosters ultrafast electron transfer at the interface (3.54 ps) but also significantly enhances the redox capacity of photogenerated carriers. Collectively, this work opens new avenues for the dual application of photocatalytic technology in both energy production and environmental remediation.

Key words: S-scheme heterojunction, H2O2 photosynthesis, Tetracycline degradation, fs-TA spectroscopy