Preparation of Graphite-UiO-66(Zr)/Ti electrode for efficient electrochemical oxidation of tetracycline in water.

Tetracycline (TC) is widely-used antibiotic pollutant with high toxicity, refractory, persistence and bacteriostasis, and its removal from water needs to be enhanced. In this work, a novel Graphite-UiO-66(Zr)/Ti electrode was successfully prepared and evaluated for electrochemical oxidation degradat...

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Main Authors: Bicun Jiang, Fuqiang Liu, Yang Pan, Yan Tan, Chendong Shuang, Aimin Li
Format: Article
Language:English
Published: Public Library of Science (PLoS) 2022-01-01
Series:PLoS ONE
Online Access:https://doi.org/10.1371/journal.pone.0271075
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author Bicun Jiang
Fuqiang Liu
Yang Pan
Yan Tan
Chendong Shuang
Aimin Li
author_facet Bicun Jiang
Fuqiang Liu
Yang Pan
Yan Tan
Chendong Shuang
Aimin Li
author_sort Bicun Jiang
collection DOAJ
description Tetracycline (TC) is widely-used antibiotic pollutant with high toxicity, refractory, persistence and bacteriostasis, and its removal from water needs to be enhanced. In this work, a novel Graphite-UiO-66(Zr)/Ti electrode was successfully prepared and evaluated for electrochemical oxidation degradation of TC. The electrochemical performance tests indicate the Graphite-UiO-66(Zr)/Ti electrode had higher electrochemical oxidation activity, which achieved higher TC removal efficiency (98.1% ± 1.5%) than Ti plate (65.2% ± 3.5%), Graphite-MIL-53(Al)/Ti electrode (79.5% ± 2.9%) and Graphite-MIL-100(Fe)/Ti electrode (89.0% ± 2.6%). The influence of operating condition was also systematically studied, and the optimized condition was pH 5.0, 20 mA/cm2 current density and 0.1 M electrolyte (Na2SO4). Through the liquid chromatography mass spectrometry (LC-MS), the TC degradation pathway by Graphite-UiO-66(Zr)/Ti electrode oxidation was proposed. Under the •OH free radical oxidative decomposition effect, the double bond, phenolic group and amine group of TC were attacked. TC was transformed into intermediate product ① (m/z = 447), then was further degraded to intermediates ② (m/z = 401) and ③ (m/z = 417). The latter was fragmented into small fractions ④ (m/z = 194), ⑤but-2-enedioic acid (m/z = 116) and ⑥oxalic acid (m/z = 90, the proposed intermediate). In addition, TC removal remained at 89.6% ± 2.7% in the sixth cycle of operation, which confirmed the efficient reusability and stability for antibiotics removal from water.
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spelling doaj.art-b80c660d72ff4565a59253cbb3c6588d2022-12-22T03:07:21ZengPublic Library of Science (PLoS)PLoS ONE1932-62032022-01-01178e027107510.1371/journal.pone.0271075Preparation of Graphite-UiO-66(Zr)/Ti electrode for efficient electrochemical oxidation of tetracycline in water.Bicun JiangFuqiang LiuYang PanYan TanChendong ShuangAimin LiTetracycline (TC) is widely-used antibiotic pollutant with high toxicity, refractory, persistence and bacteriostasis, and its removal from water needs to be enhanced. In this work, a novel Graphite-UiO-66(Zr)/Ti electrode was successfully prepared and evaluated for electrochemical oxidation degradation of TC. The electrochemical performance tests indicate the Graphite-UiO-66(Zr)/Ti electrode had higher electrochemical oxidation activity, which achieved higher TC removal efficiency (98.1% ± 1.5%) than Ti plate (65.2% ± 3.5%), Graphite-MIL-53(Al)/Ti electrode (79.5% ± 2.9%) and Graphite-MIL-100(Fe)/Ti electrode (89.0% ± 2.6%). The influence of operating condition was also systematically studied, and the optimized condition was pH 5.0, 20 mA/cm2 current density and 0.1 M electrolyte (Na2SO4). Through the liquid chromatography mass spectrometry (LC-MS), the TC degradation pathway by Graphite-UiO-66(Zr)/Ti electrode oxidation was proposed. Under the •OH free radical oxidative decomposition effect, the double bond, phenolic group and amine group of TC were attacked. TC was transformed into intermediate product ① (m/z = 447), then was further degraded to intermediates ② (m/z = 401) and ③ (m/z = 417). The latter was fragmented into small fractions ④ (m/z = 194), ⑤but-2-enedioic acid (m/z = 116) and ⑥oxalic acid (m/z = 90, the proposed intermediate). In addition, TC removal remained at 89.6% ± 2.7% in the sixth cycle of operation, which confirmed the efficient reusability and stability for antibiotics removal from water.https://doi.org/10.1371/journal.pone.0271075
spellingShingle Bicun Jiang
Fuqiang Liu
Yang Pan
Yan Tan
Chendong Shuang
Aimin Li
Preparation of Graphite-UiO-66(Zr)/Ti electrode for efficient electrochemical oxidation of tetracycline in water.
PLoS ONE
title Preparation of Graphite-UiO-66(Zr)/Ti electrode for efficient electrochemical oxidation of tetracycline in water.
title_full Preparation of Graphite-UiO-66(Zr)/Ti electrode for efficient electrochemical oxidation of tetracycline in water.
title_fullStr Preparation of Graphite-UiO-66(Zr)/Ti electrode for efficient electrochemical oxidation of tetracycline in water.
title_full_unstemmed Preparation of Graphite-UiO-66(Zr)/Ti electrode for efficient electrochemical oxidation of tetracycline in water.
title_short Preparation of Graphite-UiO-66(Zr)/Ti electrode for efficient electrochemical oxidation of tetracycline in water.
title_sort preparation of graphite uio 66 zr ti electrode for efficient electrochemical oxidation of tetracycline in water
url https://doi.org/10.1371/journal.pone.0271075
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AT yantan preparationofgraphiteuio66zrtielectrodeforefficientelectrochemicaloxidationoftetracyclineinwater
AT chendongshuang preparationofgraphiteuio66zrtielectrodeforefficientelectrochemicaloxidationoftetracyclineinwater
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