原位电沉积合成 Z 型 rGO/g-CN/TNAs 光电极及其在双室光电化学催化体系中对土霉素的降解机制。
In-situ electrodeposition synthesis of Z-scheme rGO/g-CN/TNAs photoelectrodes and its degradation mechanism for oxytetracycline in dual-chamber photoelectrocatalytic system.
机构信息
Qingdao Engineering Research Center for Rural Environment, College of Resources and Environment, Qingdao Agricultural University, Qingdao, 266109, China; State Key Laboratory of Environmental Criteria and Risk Assessment, Chinese Research Academy of Environmental Sciences, Beijing, 100012, China; State Environmental Protection Key Laboratory of Simulation and Control of Groundwater Pollution, Chinese Research Academy of Environmental Sciences, Beijing, 100012, China.
State Key Laboratory of Environmental Criteria and Risk Assessment, Chinese Research Academy of Environmental Sciences, Beijing, 100012, China; State Environmental Protection Key Laboratory of Simulation and Control of Groundwater Pollution, Chinese Research Academy of Environmental Sciences, Beijing, 100012, China.
出版信息
J Environ Manage. 2022 Apr 15;308:114615. doi: 10.1016/j.jenvman.2022.114615. Epub 2022 Feb 4.
The dual-chamber photoelectrocatalytic (PEC) system possess advantages in the degradation efficiency and processing cost of organic contaminants. In this study, TiO nanotube arrays modified by rGO and g-CN (rGO/g-CN/TNAs) photoelectrodes were successfully prepared. The surface micromorphology, chemical structure, crystal structure, and basic element composition of rGO/g-CN/TNAs photoelectrodes were studied by SEM, FTIR, XRD, Raman, and XPS. UV-vis absorption, photoluminescence (PL) spectra, and photoelectrochemical (PECH) tests were used to explore the photoelectrochemical characteristics of rGO/g-CN/TNAs photoelectrodes. Under simulated sunlight illumination, the dual-chamber PEC system with external bias voltage was used to investigate the degradation of oxytetracycline (OTC) on rGO/g-CN/TNAs photoelectrodes. The results showed that rGO and g-CN were successfully loaded on TNAs, and the separation efficiency of electrons and holes at rGO/g-CN/TNAs photoelectrodes was improved. The light absorption range of rGO/g-CN/TNAs photoelectrodes extends to the visible light region and has better light absorption performance. Compared with the photocatalytic process, when 1.2 V bias voltage was applied, the degradation efficiency of OTC in anode and cathode chambers in PEC were increased by 3.28% and 44.01% within 60 min, respectively. In addition, the anode and cathode chambers have different degradation effects on OTC. Both the external bias voltage and initial pH have significant effects in cathode chamber, but have little effect in photoanode chamber. The fluorescence excitation-emission matrix spectra and liquid chromatography-tandem mass spectrometry showed that there were different intermediates in the degradation process of OTC. This study indicated that for the dual-chamber PEC system, rGO/g-CN/TNAs photoelectrodes exhibited excellent photocatalytic performance and have potential application prospects in water environmental remediation.
双室光电催化（PEC）系统在降解有机污染物的效率和处理成本方面具有优势。在本研究中，成功制备了 rGO 和 g-CN（rGO/g-CN/TNAs）修饰的 TiO 纳米管阵列光电电极。通过 SEM、FTIR、XRD、拉曼和 XPS 研究了 rGO/g-CN/TNAs 光电电极的表面微观形貌、化学结构、晶体结构和基本元素组成。通过 UV-vis 吸收、光致发光（PL）光谱和光电化学（PECH）测试研究了 rGO/g-CN/TNAs 光电电极的光电化学特性。在模拟太阳光照射下，采用带外偏压的双室 PEC 系统研究了 rGO/g-CN/TNAs 光电电极对土霉素（OTC）的降解。结果表明，rGO 和 g-CN 成功负载在 TNAs 上，rGO/g-CN/TNAs 光电电极中电子和空穴的分离效率提高。rGO/g-CN/TNAs 光电电极的光吸收范围扩展到可见光区域，具有更好的光吸收性能。与光催化过程相比，当施加 1.2 V 偏压时，在 60 min 内，PEC 中阳极室和阴极室中 OTC 的降解效率分别提高了 3.28%和 44.01%。此外，阳极室和阴极室对 OTC 有不同的降解效果。外加偏压和初始 pH 值对阴极室均有显著影响，但对光阳极室影响较小。荧光激发-发射矩阵光谱和液相色谱-串联质谱表明，OTC 降解过程中有不同的中间产物。本研究表明，对于双室 PEC 系统，rGO/g-CN/TNAs 光电电极表现出优异的光催化性能，在水环境修复方面具有潜在的应用前景。
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