Photocatalytic degradation of tetracycline by UiO-66-S-FeS composites for visible light: Mechanistic on compact interfacial and degradation pathways

IF 4.7 3区 化学 Q2 CHEMISTRY, PHYSICAL Journal of Photochemistry and Photobiology A-chemistry Pub Date : 2025-02-14 DOI:10.1016/j.jphotochem.2025.116343
Huimin Wen , Xueyao Wang , Xin Zhang , Xinyang Yao , Lihui Huang , Ting Sun , Zhenhui Gao
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Abstract

Photocatalysis encounters a major challenge in developing catalysts that are capable of functioning stably and efficiently absorbing visible light. In this study, we designed and synthesized the UiO-66-S-FeS photocatalyst, which featured a type I heterojunction. Its successful synthesis was validated by characterization analyses. The UiO-66-S-FeS catalyst exhibited a “shell-core” structure, with FeS firmly anchored to the surface of UiO-66-SH2 via Fe-S bonds, creating a robust interface. The interface significantly enhanced the rate of photogenerated carrier transfer and separation during photocatalytic reactions. While retaining the original advantages of active site dispersion and high specific surface area of MOFs, the doping of FeS resulted in good visible light absorption performance. Ultraviolet–visible diffuse reflectance spectroscopy (UV–Vis DRS) revealed that the visible light absorption scope of UiO-66-S-FeS0.5 was effectively broadened compared to UiO-66-SH2. It resulted in a remarkable improvement in tetracycline degradation, achieving a degradation rate of 99.5 % under visible light. Electron spin resonance (ESR) and free radical scavenging experiments identified several reactive species, including ·O2, h+, ·OH and 1O2 playing roles in the degradation process. These findings supported the degradation mechanism as a type I heterojunction. This study demonstrated the potential of the UiO-66-S-FeS photocatalyst for effectively removing antibiotic contaminants.

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UiO-66-S-FeS复合材料在可见光下光催化降解四环素:致密界面和降解途径的机理
光催化面临的一个重大挑战是开发能够稳定有效地吸收可见光的催化剂。在本研究中,我们设计并合成了具有I型异质结的UiO-66-S-FeS光催化剂。通过表征分析验证了其成功合成。UiO-66-S-FeS催化剂呈现“壳核”结构,FeS通过Fe-S键牢固地锚定在UiO-66-SH2表面,形成坚固的界面。该界面显著提高了光催化反应中载流子转移和分离的速率。在保留mof原有的活性位点色散和高比表面积优势的同时,掺杂FeS获得了良好的可见光吸收性能。紫外-可见漫反射光谱(UV-Vis DRS)结果表明,与UiO-66-SH2相比,UiO-66-S-FeS0.5的可见光吸收范围得到有效拓宽。在可见光下,四环素的降解率达到了99.5%。电子自旋共振(ESR)和自由基清除实验发现了几种活性物质,包括·O2−、h+、·OH和1O2在降解过程中起作用。这些发现支持了I型异质结的降解机制。本研究证明了UiO-66-S-FeS光催化剂在有效去除抗生素污染物方面的潜力。
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来源期刊
CiteScore
7.90
自引率
7.00%
发文量
580
审稿时长
48 days
期刊介绍: JPPA publishes the results of fundamental studies on all aspects of chemical phenomena induced by interactions between light and molecules/matter of all kinds. All systems capable of being described at the molecular or integrated multimolecular level are appropriate for the journal. This includes all molecular chemical species as well as biomolecular, supramolecular, polymer and other macromolecular systems, as well as solid state photochemistry. In addition, the journal publishes studies of semiconductor and other photoactive organic and inorganic materials, photocatalysis (organic, inorganic, supramolecular and superconductor). The scope includes condensed and gas phase photochemistry, as well as synchrotron radiation chemistry. A broad range of processes and techniques in photochemistry are covered such as light induced energy, electron and proton transfer; nonlinear photochemical behavior; mechanistic investigation of photochemical reactions and identification of the products of photochemical reactions; quantum yield determinations and measurements of rate constants for primary and secondary photochemical processes; steady-state and time-resolved emission, ultrafast spectroscopic methods, single molecule spectroscopy, time resolved X-ray diffraction, luminescence microscopy, and scattering spectroscopy applied to photochemistry. Papers in emerging and applied areas such as luminescent sensors, electroluminescence, solar energy conversion, atmospheric photochemistry, environmental remediation, and related photocatalytic chemistry are also welcome.
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