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Fabrication of a permeable SnO2-Sb reactive anodic filter for high-efficiency electrochemical oxidation of antibiotics in wastewater

Journal 2021 · IF 9.621 · 发表于 2021 年 8 月 18 日
作者: Chao Yang,Yiang Fan,Shanshan Shang,Pu Li,Xiao-yan Li
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摘要

Electrochemical oxidation (ECO) is an appealing technology for treating emerging organic pollutants in wastewater. However, the conventional flow-by ECO process is expensive with a low energy efficiency owing to the limitations of mass transport of contaminants to the limited surface area of the anode. In this study, a novel freestanding porous and permeable SnO 2 -Sb anode was fabricated by one-step sintering using micrometer-sized (NH 4 ) 2 CO 3 grains as the pore-forming agents. This permeable SnO 2 -Sb anode without Ti substrate functioned as a reactive anodic filter (RAF) in an ECO cell to treat wastewater containing ciprofloxacin (CIP). Forcing the wastewater through the porous RAF depth-wise improved the mass transport and vastly enlarged the electroactive surface area. Compared with the conventional flow-by configuration, the flow-through RAF exhibited a 12-fold increase in the mass transfer rate constant (60.7 × 10 −6 m s −1 ) and a 5-fold increase in the CIP degradation rate constant (0.077 min −1 ). At a cell potential of 4.0 V, more than 92% of the CIP was degraded in a single-pass operation at a filtration flux of 54 L m −2 h −1 and a short retention time of 1.7 min through the RAF. The robustness and stability of the RAF were demonstrated by its remarkable CIP degradation efficacy of 99% during 200 h of operation. The mechanism of CIP degradation was examined using probe molecules and density functional theory calculations and found to be a combined effect of direct electron transfer and oxidation by generated radicals ( OH and SO 4 − ). The great potential of RAF in flow-through ECO was further validated by its effective removal (>92%) of various organic pollutants in actual municipal wastewater at a low energy consumption of 0.33 kWh m −3 . The RAF-based ECO process thus provides an advanced environmental technology for the oxidation of toxic and recalcitrant organic pollutants in wastewater treatment.

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