In-situ electrodeposition synthesis of Z-scheme rGO/g-C3N4/TNAs photoelectrodes and its degradation mechanism for oxytetracycline in dual-chamber photoelectrocatalytic system

Chengze Yu; Jiaqi Hou; Bin Zhang; Shiqi Liu; Xiangrui Pan; Heng Song; Xiangting Hou; Qinghua Yan; Chengzhi Zhou; Guocheng Liu; Yingjie Zhang; Yanjun Xin

doi:10.1016/j.jenvman.2022.114615

In-situ electrodeposition synthesis of Z-scheme rGO/g-C₃N₄/TNAs photoelectrodes and its degradation mechanism for oxytetracycline in dual-chamber photoelectrocatalytic system

J Environ Manage. 2022 Apr 15:308:114615. doi: 10.1016/j.jenvman.2022.114615. Epub 2022 Feb 4.

Authors

Chengze Yu¹, Jiaqi Hou², Bin Zhang³, Shiqi Liu³, Xiangrui Pan³, Heng Song³, Xiangting Hou³, Qinghua Yan³, Chengzhi Zhou³, Guocheng Liu³, Yingjie Zhang⁴, Yanjun Xin⁵

Affiliations

¹ 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.
² 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.
³ Qingdao Engineering Research Center for Rural Environment, College of Resources and Environment, Qingdao Agricultural University, Qingdao, 266109, China.
⁴ School of Marine Science and Technology, Sino-Europe Membrane Technology Research Institute Harbin Institute of Technology, Weihai, 264209, China.
⁵ Qingdao Engineering Research Center for Rural Environment, College of Resources and Environment, Qingdao Agricultural University, Qingdao, 266109, China. Electronic address: xintom2000@126.com.

PMID: 35131709
DOI: 10.1016/j.jenvman.2022.114615

Abstract

The dual-chamber photoelectrocatalytic (PEC) system possess advantages in the degradation efficiency and processing cost of organic contaminants. In this study, TiO₂ nanotube arrays modified by rGO and g-C₃N₄ (rGO/g-C₃N₄/TNAs) photoelectrodes were successfully prepared. The surface micromorphology, chemical structure, crystal structure, and basic element composition of rGO/g-C₃N₄/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-C₃N₄/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-C₃N₄/TNAs photoelectrodes. The results showed that rGO and g-C₃N₄ were successfully loaded on TNAs, and the separation efficiency of electrons and holes at rGO/g-C₃N₄/TNAs photoelectrodes was improved. The light absorption range of rGO/g-C₃N₄/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-C₃N₄/TNAs photoelectrodes exhibited excellent photocatalytic performance and have potential application prospects in water environmental remediation.

Keywords: Dual-chamber PEC system; Oxytetracycline; PEC degradation; RGO/g-C(3)N(4)/TNAs photoelectrodes.

MeSH terms

Catalysis
Electroplating
Graphite* / chemistry
Oxytetracycline*

Substances

graphene oxide
Graphite
Oxytetracycline