富含氧空位S型MIL-101(Fe)/BiOCl异质结增强光催化去除Cr(Ⅵ)

doi:10.3866/PKU.WHXB202307045

物理化学学报 >> 2024, Vol. 40 >> Issue (7): 2307045.doi: 10.3866/PKU.WHXB202307045

富含氧空位S型MIL-101(Fe)/BiOCl异质结增强光催化去除Cr(Ⅵ)

王春春¹^,†, 游常俊¹^,†, 戎珂¹, 申楚琦¹, 杨方², 李世杰¹^,*()

¹ 浙江海洋大学海洋科学与技术学院, 国家海洋设施养殖工程技术研究中心, 浙江省海产品健康危害因素关键技术研究重点实验室, 浙江舟山 316022
² 上海工程技术大学机械与汽车工程学院, 上海 201620

收稿日期:2023-07-23 修回日期:2023-08-25 录用日期:2023-08-25 发布日期:2023-12-01
通讯作者: Email: lishijie@zjou.edu.cn; Tel: +86-580-2551319 (李世杰)
作者简介:
^†These authors contributed equally to this work.
基金资助:
国家自然科学基金(U1809214); 国家自然科学基金(51708504); 浙江省自然科学基金(LY20E080014); 舟山科技项目(2022C41011)

An S-Scheme MIL-101(Fe)-on-BiOCl Heterostructure with Oxygen Vacancies for Boosting Photocatalytic Removal of Cr(Ⅵ)

Chunchun Wang¹, Changjun You¹, Ke Rong¹, Chuqi Shen¹, Fang Yang², Shijie Li¹^,*()

¹ Key Laboratory of Health Risk Factors for Seafood of Zhejiang Province, National Engineering Research Center for Marine Aquaculture, College of Marine Science and Technology, Zhejiang Ocean University, Zhoushan 316022, Zhejiang Province, China
² School of Mechanical and Automotive Engineering, Shanghai University of Engineering Science, Shanghai 201620, China

Received:2023-07-23 Revised:2023-08-25 Accepted:2023-08-25 Published:2023-12-01
Contact: Email: lishijie@zjou.edu.cn; Tel: +86-580-2551319 (Shijie Li)
Supported by:
National Natural Science Foundation of China(U1809214); National Natural Science Foundation of China(51708504); the Natural Science Foundation of Zhejiang Province of China(LY20E080014); the Science and Technology Project of Zhoushan of China(2022C41011)

1. 附件.pdf(734KB)

摘要/Abstract

摘要：

Cr(Ⅵ)污染物有毒有害且不可生物降解，会对环境造成严重破坏。光催化技术可实现Cr(Ⅵ)的有效去除，在解决环境污染问题方面具有良好前景。因此，本文通过在富含氧空位(OV)的BiOCl微球表面原位生长MIL-101(Fe)晶体，构建了一种新型富氧缺陷MOF基S型异质结催化剂-MIL-101(Fe)/BiOCl。这种催化剂在高浓度Cr(Ⅵ)的光催化还原中表现出优异活性，60 min内对Cr(Ⅵ)溶液(10 mg∙L^-1]，100 mL)的光还原效率达到88.5%，其光催化效率分别是BiOCl和MIL-101(Fe)的4.4和9.0倍。而且，MIL-101(Fe)/BiOCl还表现出良好的抗环境干扰性、稳定性和可重复使用性，显示出令人印象深刻的实际应用前景。实验结果表明，富含氧空位的S型MIL-101(Fe)/BiOCl异质结构暴露了大量活性位点，促进了界面电荷分离，提高了光生载流子的氧化还原能力，从而增强了光催化性能。另外，经过活性自由基检测发现，e^-和∙O₂^-是光催化反应过程中的主要活性物种。这些研究结果将为开发用于环境治理的缺陷半导体/MOF S型光催化剂开辟新的途径。

关键词: MOF, S型异质结, MIL-101(Fe), BiOCl, Cr(Ⅵ)光还原, 氧空位

Abstract:

Hexavalent chromium (Cr(Ⅵ)) may be a hazardous and non-biodegradable waste matter which will cause substantial environmental damage. Fabricating powerful photosystems to achieve efficacious elimination of Cr(Ⅵ) holds eminent promise in solving environmental issues. Thanks to their outstanding photo/electrical properties, large surface area, and customizable structure, metal-organic framework (MOF) catalysts have attracted widespread attention within the field of pollutant degradation and reduction. Nevertheless, due to the recombination of photo-generated charge carriers, pristine semiconductor MOFs' photocatalytic performance is inadequate. To overcome this challenge, one of the most typical and effective strategies is to create heterojunctions by combining MOFs with another semiconductor. Among these strategies, the innovative step-scheme (S-scheme) heterojunction has gained increasing prominence. Unlike traditional type Ⅱ and Z-scheme heterojunctions, the built-in electric field at the S-scheme heterojunction boundary enhances spatial charge separation and boosts redox capacity, thereby improving photocatalytic performance. In this study, a creative MOF-based S-scheme architecture with oxygen vacancies (OV) was built via in situ growth of MIL-101(Fe) crystals on the surface of OV-rich BiOCl microspheres. The optimized MIL-101(Fe)/BiOCl heterojunction exhibited exceptional photocatalytic performance in photo-reducing high concentrations of Cr(Ⅵ) and 88.5% of Cr(Ⅵ) solution (10 mg∙L^-1], 100 mL) can be removed within 60 min, which is about 4.4 and 9.0 times that of BiOCl and MIL-101(Fe). Besides, the MIL-101(Fe)/BiOCl manifests impressive practical implementation prospect due to its high anti-interference property, robustness and reusability. Photoelectron spectroscopy results validated that built-in electric field, bending band, and Coulomb attraction facilitated the transition of photoelectrons from the conduction band (CB) of BiOCl to the valence band (VB) of MIL-101(Fe), where they recombined with the photo-created holes. This suggests an S-scheme interfacial photo-carrier detachment mechanism at the MIL-101(Fe)/BiOCl interface. In addition, BET measurements indicated a notable increase in surface area with the introduction of MIL-101(Fe). The OV-rich S-scheme MIL-101(Fe)/BiOCl heterostructure boasts more reactive sites, enhanced interfacial charge separation, and optimal redox ability of photo-carriers, leading to enhanced photocatalytic properties. Measurements of active radical scavenging and electron spin resonance (ESR) confirm that e^- and ∙O₂^- are the primary active species during photocatalysis. These discoveries would open up new avenues for developing defective semiconductor/MOF S-scheme photocatalyst for environmental purification.

Key words: MOF, S-scheme heterojunction, MIL-101(Fe), BiOCl, Cr(Ⅵ) photoreduction, Oxygen vacancy

王春春, 游常俊, 戎珂, 申楚琦, 杨方, 李世杰. 富含氧空位S型MIL-101(Fe)/BiOCl异质结增强光催化去除Cr(Ⅵ)[J]. 物理化学学报, 2024, 40(7), 2307045. doi: 10.3866/PKU.WHXB202307045

Chunchun Wang, Changjun You, Ke Rong, Chuqi Shen, Fang Yang, Shijie Li. An S-Scheme MIL-101(Fe)-on-BiOCl Heterostructure with Oxygen Vacancies for Boosting Photocatalytic Removal of Cr(Ⅵ)[J]. Acta Phys. -Chim. Sin. 2024, 40(7), 2307045. doi: 10.3866/PKU.WHXB202307045

链接本文: https://www.whxb.pku.edu.cn/CN/10.3866/PKU.WHXB202307045

https://www.whxb.pku.edu.cn/CN/Y2024/V40/I7/2307045

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富含氧空位S型MIL-101(Fe)/BiOCl异质结增强光催化去除Cr(Ⅵ)

An S-Scheme MIL-101(Fe)-on-BiOCl Heterostructure with Oxygen Vacancies for Boosting Photocatalytic Removal of Cr(Ⅵ)

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