MIL-101(Fe)/BiOBr S-scheme photocatalyst for promoting photocatalytic abatement of Cr(VI) and enrofloxacin antibiotic: Performance and mechanism

光催化 双功能 催化作用 电子顺磁共振 异质结 材料科学 人体净化 化学工程 降级(电信) 光化学 化学 纳米技术 废物管理 光电子学 有机化学 计算机科学 电信 物理 工程类 核磁共振
作者
Shijie Li,Chunchun Wang,Kexin Dong,Peng Zhang,Xiaobo Chen,Xin Li
出处
期刊:Chinese Journal of Catalysis [China Science Publishing & Media Ltd.]
卷期号:51: 101-112 被引量:280
标识
DOI:10.1016/s1872-2067(23)64479-1
摘要

The development of highly active, economical, and robust bifunctional photocatalysts is a priority for sustainable photocatalytic water remediation. Inadequately available reactive sites and sluggish interface photocarrier transfer and separation remain significant challenges in the photoreaction progress. In this study, the Fe-containing metal-organic framework (MOF) MIL-101(Fe) was integrated with BiOBr microspheres to form a competent S-scheme heterostructure for the photocatalytic mitigation of Cr(VI) and enrofloxacin (ENR) antibiotics. The optimal MIL-101(Fe)/BiOBr exhibited the highest photoactivity, with 99.4% of Cr(VI) and 84.4% of ENR eliminated upon visible-light illumination in a single-pollutant system. The photoactivity of MIL-101(Fe)/BiOBr in the decontamination of the Cr(VI)-ENR co-existence system exhibited a substantial enhancement when compared to that in a single system, owing to the improved utilization of electrons and holes resulting from the synergism between Cr(VI), ENR, and the photocatalyst. The enhanced photoactivity is attributed to two aspects: (1) the incorporation of MIL-101(Fe) results in an increased number of available reactive sites and improved solar harvesting properties; and (2) the S-scheme mechanism enables the effective spatial disassociation of photoexcited carriers and optimization of the photo-redox capability of the system. Through scavenging experiments, electron spin resonance characterization, liquid chromatography-tandem mass spectrometry analysis, and T.E.S.T. theoretical estimation, the catalytic mechanism, antibiotic degradation process, and biotoxicities of the degraded products were analyzed and confirmed. This study provides a viable strategy for building competent MOF-inorganic semiconductor S-scheme photocatalysts with superior photocatalytic decontamination performance.
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