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

引用本文: 张淑敏, 王亚琪, 王泽林, 王立博, 安长胜, 许第发. ZIS_1−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[J]. 物理化学学报, 2025, 41(11): 100136. doi: 10.1016/j.actphy.2025.100136 shu

Citation: Shumin Zhang, Yaqi Wang, Zelin Wang, Libo Wang, Changsheng An, Difa Xu. Ultrafast electron transfer at the ZIS_1−x/UCN S-scheme interface enables efficient H₂O₂ photosynthesis coupled with tetracycline degradation[J]. Acta Physico-Chimica Sinica, 2025, 41(11): 100136. doi: 10.1016/j.actphy.2025.100136 shu

ZIS_1−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.
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

通讯作者: 安长胜, z20190628@ccsu.edu.cn; 许第发, xudifa@sina.com

基金项目:
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

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ZIS_1−x纳米片，构建了一种富含S缺陷的ZnIn₂S₄/g-C₃N₄ (ZIS_1−x/UCN) S型异质结光催化剂。设计的ZIS_1−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ZIS_1−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:

English

Ultrafast electron transfer at the ZIS_1−x/UCN S-scheme interface enables efficient H₂O₂ photosynthesis coupled with tetracycline degradation

Shumin Zhang ^1, ,
Yaqi Wang ^1, ,
Zelin Wang ^1, ,
Libo Wang ^2, ,
Changsheng An ^{1,
,} ,
Difa Xu ^{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

Corresponding author: Email: z20190628@ccsu.edu.cn (C.A.). Tel: +86-18932463886 (C.A.); Email: xudifa@sina.com (D.X.). +86-13687382717. (D.X.)

Received Date: 24 June 2025
Accepted Date: 23 July 2025
Revised Date: 20 July 2025
Available Online: 15 November 2025
Fund Project:
the Research Foundation Bureau of Hunan Province

the National Natural Science Foundation of China

the National Natural Science Foundation of China

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 (ZIS_1−x/UCN) S-scheme heterojunction photocatalyst was constructed by in situ growing ZIS_1−x nanosheets on porous ultrathin UCN. The designed ZIS_1−x/UCN photocatalyst demonstrates enhanced visible light absorption, abundant active sites, and intimate interfacial contact. The optimized ZIS_1−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.

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1.
沈阳化工大学材料科学与工程学院沈阳 110142

ZIS_1−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

通讯作者: 安长胜, z20190628@ccsu.edu.cn; 许第发, xudifa@sina.com

English

Ultrafast electron transfer at the ZIS_1−x/UCN S-scheme interface enables efficient H₂O₂ photosynthesis coupled with tetracycline degradation

Corresponding author: Email: z20190628@ccsu.edu.cn (C.A.). Tel: +86-18932463886 (C.A.); Email: xudifa@sina.com (D.X.). +86-13687382717. (D.X.)

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