Photostable hollow core-shell ZnSe@PDA-7 type-II heterojunction with built-in electric field for efficient photocatalytic generation of H2O2

IF 5.7 2区材料科学 Q2 CHEMISTRY, PHYSICAL

Surfaces and Interfaces Pub Date : 2025-04-10 DOI:10.1016/j.surfin.2025.106427

Yubao Li , Guangyuan Chen , Shaowen Wu, Chenyang Lin, Tingting Tang, Qina Quan, Yunyun Lu, Shijian Zhou, Yan Kong

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Abstract

Various strategies have been developed to prevent electron-hole recombination and photocorrosion in sulfur-based semiconductors, improving catalyst efficiency and enabling high-activity, stable photocatalytic H₂O₂ generation. In this study, we construct a hollow core-shell catalyst by tightly coating hollow ZnSe microspheres with an organic semiconductor polydopamine (PDA) via a self-polymerization method, effectively reduces the impact of photocorrosion on ZnSe. DFT calculations confirmed the formation of a built-in electric field at the ZnSe/PDA interface, which, under its influence, promotes the creation of a type-II heterojunction favorable for photocatalytic H₂O₂ generation. The built-in electric field and type-II heterojunction enhance charge carrier transfer and separation. The PDA coating also improves O₂ adsorption and light utilization of ZnSe, further enhancing H₂O₂ photocatalytic performance. Results show that ZnSe@PDA-7, with optimal PDA loading, achieves an H₂O₂ generation rate of 1978.5 μmol g^-1 h^-1 under visible light irradiation in pure water. This method of organic polymer coating on chalcogenide semiconductors effectively mitigates photocorrosion effects and improves charge carrier separation, offering a sustainable solution for clean energy synthesis.

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光稳定的空心核壳ZnSe@PDA-7 ii型异质结，内置电场，用于高效光催化生成H2O2

为了防止硫基半导体中的电子-空穴复合和光腐蚀，提高催化剂效率，实现高活性、稳定的光催化H2O2生成，人们开发了各种策略。在本研究中，我们通过自聚合的方法将有机半导体聚多巴胺（PDA）紧密包裹在空心ZnSe微球上，构建了一种空心核壳催化剂，有效地降低了光腐蚀对ZnSe的影响。DFT计算证实，在ZnSe/PDA界面处形成了一个内置电场，在其影响下，促进了有利于光催化生成H2O2的ii型异质结的形成。内置电场和ii型异质结增强了载流子转移和分离。PDA涂层还提高了ZnSe对O2的吸附和光利用率，进一步提高了H2O2光催化性能。结果表明，在最佳PDA负载下，ZnSe@PDA-7在可见光照射下的H2O2生成速率为1978.5 μmol g-1 h-1。这种在硫系半导体上涂覆有机聚合物的方法有效地减轻了光腐蚀效应，改善了载流子的分离，为清洁能源合成提供了一种可持续的解决方案。

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来源期刊

Surfaces and Interfaces Chemistry-General Chemistry

CiteScore

8.50

自引率

6.50%

发文量

753

审稿时长

35 days

期刊介绍： The aim of the journal is to provide a respectful outlet for ''sound science'' papers in all research areas on surfaces and interfaces. We define sound science papers as papers that describe new and well-executed research, but that do not necessarily provide brand new insights or are merely a description of research results. Surfaces and Interfaces publishes research papers in all fields of surface science which may not always find the right home on first submission to our Elsevier sister journals (Applied Surface, Surface and Coatings Technology, Thin Solid Films)