Evaluating tetracycline degradation pathway and intermediate toxicity during the electrochemical oxidation over a Ti/Ti4O7 anode
Tetracycline (TC) is one of the most widely used antibiotics with significant impacts on human health and thus it needs appropriate approaches for its removal. In the present study, we evaluated the performance and complete pathway of the TC electrochemical oxidation on a Ti/Ti4O7 anode prepared by...
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| Published in | Water research (Oxford) Vol. 137; pp. 324 - 334 |
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| Main Authors | , , , , |
| Format | Journal Article |
| Language | English |
| Published |
Elsevier Ltd
15.06.2018
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| Subjects | |
| Online Access | Get full text |
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| Abstract | Tetracycline (TC) is one of the most widely used antibiotics with significant impacts on human health and thus it needs appropriate approaches for its removal. In the present study, we evaluated the performance and complete pathway of the TC electrochemical oxidation on a Ti/Ti4O7 anode prepared by plasma spraying. Morphological data and composition analysis indicated a compact coating layer on the anode, which had the characteristic peaks of Ti4O7 as active constituent. The TC electrochemical oxidation on the Ti/Ti4O7 anode followed a pseudo-first-order kinetics, and the TC removal efficiency reached 95.8% in 40 min. The influential factors on TC decay kinetics included current density, anode-cathode distance and initial TC concentration. This anode also had high durability and the TC removal efficiency was maintained over 95% after five times reuse. For the first time, we unraveled the complete pathway of the TC electrochemical oxidation using high-performance liquid chromatograph (HPLC) and gas chromatograph (GC) coupled with mass spectrometer (MS). ·OH radicals produced from electrochemical oxidation attack the double bond, phenolic group and amine group of TC, forming a primary intermediate (m/z = 461), secondary intermediates (m/z = 432, 477 and 509) and tertiary intermediates (m/z = 480, 448 and 525). The latter were further oxidized to the key downstream intermediate (m/z = 496), followed by further downstream intermediates (m/z = 451, 412, 396, 367, 351, 298 and 253) and eventually short-chain carboxylic acids. We also evaluated the toxicity change during the electrochemical oxidation process with bioluminescent bacteria. The bioluminescence inhibition ratio peaked at 10 min (55.41%), likely owing to the high toxicity of intermediates with m/z = 461, 432 and 477 as obtained from quantitative structure activity relationship (QSAR) analysis. The bioluminescence inhibition ratio eventually decreased to 16.78% in 40 min due to further transformation of TC and intermediates. By comprehensively analyzing the influential factors and complete degradation pathway of TC electrochemical oxidation on the Ti/Ti4O7 anode, our research provides deeper insights into the risk assessment of intermediates and their toxicity, assigning new perspectives for practical electrochemical oxidation to effectively eliminate the amount and toxicity of TC and other antibiotics in wastewater.
[Display omitted]
•Satisfactory tetracycline degradation (95.8%) on a Ti/Ti4O7 anode.•The tetracycline electrochemical oxidation follows a pseudo-first order kinetics.•First complete pathway of tetracycline electrochemical oxidation.•Toxicity evaluation of 25 intermediates by QSAR explains toxicity reduction delay. |
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| AbstractList | Tetracycline (TC) is one of the most widely used antibiotics with significant impacts on human health and thus it needs appropriate approaches for its removal. In the present study, we evaluated the performance and complete pathway of the TC electrochemical oxidation on a Ti/Ti4O7 anode prepared by plasma spraying. Morphological data and composition analysis indicated a compact coating layer on the anode, which had the characteristic peaks of Ti4O7 as active constituent. The TC electrochemical oxidation on the Ti/Ti4O7 anode followed a pseudo-first-order kinetics, and the TC removal efficiency reached 95.8% in 40 min. The influential factors on TC decay kinetics included current density, anode-cathode distance and initial TC concentration. This anode also had high durability and the TC removal efficiency was maintained over 95% after five times reuse. For the first time, we unraveled the complete pathway of the TC electrochemical oxidation using high-performance liquid chromatograph (HPLC) and gas chromatograph (GC) coupled with mass spectrometer (MS). ·OH radicals produced from electrochemical oxidation attack the double bond, phenolic group and amine group of TC, forming a primary intermediate (m/z = 461), secondary intermediates (m/z = 432, 477 and 509) and tertiary intermediates (m/z = 480, 448 and 525). The latter were further oxidized to the key downstream intermediate (m/z = 496), followed by further downstream intermediates (m/z = 451, 412, 396, 367, 351, 298 and 253) and eventually short-chain carboxylic acids. We also evaluated the toxicity change during the electrochemical oxidation process with bioluminescent bacteria. The bioluminescence inhibition ratio peaked at 10 min (55.41%), likely owing to the high toxicity of intermediates with m/z = 461, 432 and 477 as obtained from quantitative structure activity relationship (QSAR) analysis. The bioluminescence inhibition ratio eventually decreased to 16.78% in 40 min due to further transformation of TC and intermediates. By comprehensively analyzing the influential factors and complete degradation pathway of TC electrochemical oxidation on the Ti/Ti4O7 anode, our research provides deeper insights into the risk assessment of intermediates and their toxicity, assigning new perspectives for practical electrochemical oxidation to effectively eliminate the amount and toxicity of TC and other antibiotics in wastewater. Tetracycline (TC) is one of the most widely used antibiotics with significant impacts on human health and thus it needs appropriate approaches for its removal. In the present study, we evaluated the performance and complete pathway of the TC electrochemical oxidation on a Ti/Ti4O7 anode prepared by plasma spraying. Morphological data and composition analysis indicated a compact coating layer on the anode, which had the characteristic peaks of Ti4O7 as active constituent. The TC electrochemical oxidation on the Ti/Ti4O7 anode followed a pseudo-first-order kinetics, and the TC removal efficiency reached 95.8% in 40 min. The influential factors on TC decay kinetics included current density, anode-cathode distance and initial TC concentration. This anode also had high durability and the TC removal efficiency was maintained over 95% after five times reuse. For the first time, we unraveled the complete pathway of the TC electrochemical oxidation using high-performance liquid chromatograph (HPLC) and gas chromatograph (GC) coupled with mass spectrometer (MS). ·OH radicals produced from electrochemical oxidation attack the double bond, phenolic group and amine group of TC, forming a primary intermediate (m/z = 461), secondary intermediates (m/z = 432, 477 and 509) and tertiary intermediates (m/z = 480, 448 and 525). The latter were further oxidized to the key downstream intermediate (m/z = 496), followed by further downstream intermediates (m/z = 451, 412, 396, 367, 351, 298 and 253) and eventually short-chain carboxylic acids. We also evaluated the toxicity change during the electrochemical oxidation process with bioluminescent bacteria. The bioluminescence inhibition ratio peaked at 10 min (55.41%), likely owing to the high toxicity of intermediates with m/z = 461, 432 and 477 as obtained from quantitative structure activity relationship (QSAR) analysis. The bioluminescence inhibition ratio eventually decreased to 16.78% in 40 min due to further transformation of TC and intermediates. By comprehensively analyzing the influential factors and complete degradation pathway of TC electrochemical oxidation on the Ti/Ti4O7 anode, our research provides deeper insights into the risk assessment of intermediates and their toxicity, assigning new perspectives for practical electrochemical oxidation to effectively eliminate the amount and toxicity of TC and other antibiotics in wastewater. [Display omitted] •Satisfactory tetracycline degradation (95.8%) on a Ti/Ti4O7 anode.•The tetracycline electrochemical oxidation follows a pseudo-first order kinetics.•First complete pathway of tetracycline electrochemical oxidation.•Toxicity evaluation of 25 intermediates by QSAR explains toxicity reduction delay. Tetracycline (TC) is one of the most widely used antibiotics with significant impacts on human health and thus it needs appropriate approaches for its removal. In the present study, we evaluated the performance and complete pathway of the TC electrochemical oxidation on a Ti/Ti4O7 anode prepared by plasma spraying. Morphological data and composition analysis indicated a compact coating layer on the anode, which had the characteristic peaks of Ti4O7 as active constituent. The TC electrochemical oxidation on the Ti/Ti4O7 anode followed a pseudo-first-order kinetics, and the TC removal efficiency reached 95.8% in 40 min. The influential factors on TC decay kinetics included current density, anode-cathode distance and initial TC concentration. This anode also had high durability and the TC removal efficiency was maintained over 95% after five times reuse. For the first time, we unraveled the complete pathway of the TC electrochemical oxidation using high-performance liquid chromatograph (HPLC) and gas chromatograph (GC) coupled with mass spectrometer (MS). ·OH radicals produced from electrochemical oxidation attack the double bond, phenolic group and amine group of TC, forming a primary intermediate (m/z = 461), secondary intermediates (m/z = 432, 477 and 509) and tertiary intermediates (m/z = 480, 448 and 525). The latter were further oxidized to the key downstream intermediate (m/z = 496), followed by further downstream intermediates (m/z = 451, 412, 396, 367, 351, 298 and 253) and eventually short-chain carboxylic acids. We also evaluated the toxicity change during the electrochemical oxidation process with bioluminescent bacteria. The bioluminescence inhibition ratio peaked at 10 min (55.41%), likely owing to the high toxicity of intermediates with m/z = 461, 432 and 477 as obtained from quantitative structure activity relationship (QSAR) analysis. The bioluminescence inhibition ratio eventually decreased to 16.78% in 40 min due to further transformation of TC and intermediates. By comprehensively analyzing the influential factors and complete degradation pathway of TC electrochemical oxidation on the Ti/Ti4O7 anode, our research provides deeper insights into the risk assessment of intermediates and their toxicity, assigning new perspectives for practical electrochemical oxidation to effectively eliminate the amount and toxicity of TC and other antibiotics in wastewater.Tetracycline (TC) is one of the most widely used antibiotics with significant impacts on human health and thus it needs appropriate approaches for its removal. In the present study, we evaluated the performance and complete pathway of the TC electrochemical oxidation on a Ti/Ti4O7 anode prepared by plasma spraying. Morphological data and composition analysis indicated a compact coating layer on the anode, which had the characteristic peaks of Ti4O7 as active constituent. The TC electrochemical oxidation on the Ti/Ti4O7 anode followed a pseudo-first-order kinetics, and the TC removal efficiency reached 95.8% in 40 min. The influential factors on TC decay kinetics included current density, anode-cathode distance and initial TC concentration. This anode also had high durability and the TC removal efficiency was maintained over 95% after five times reuse. For the first time, we unraveled the complete pathway of the TC electrochemical oxidation using high-performance liquid chromatograph (HPLC) and gas chromatograph (GC) coupled with mass spectrometer (MS). ·OH radicals produced from electrochemical oxidation attack the double bond, phenolic group and amine group of TC, forming a primary intermediate (m/z = 461), secondary intermediates (m/z = 432, 477 and 509) and tertiary intermediates (m/z = 480, 448 and 525). The latter were further oxidized to the key downstream intermediate (m/z = 496), followed by further downstream intermediates (m/z = 451, 412, 396, 367, 351, 298 and 253) and eventually short-chain carboxylic acids. We also evaluated the toxicity change during the electrochemical oxidation process with bioluminescent bacteria. The bioluminescence inhibition ratio peaked at 10 min (55.41%), likely owing to the high toxicity of intermediates with m/z = 461, 432 and 477 as obtained from quantitative structure activity relationship (QSAR) analysis. The bioluminescence inhibition ratio eventually decreased to 16.78% in 40 min due to further transformation of TC and intermediates. By comprehensively analyzing the influential factors and complete degradation pathway of TC electrochemical oxidation on the Ti/Ti4O7 anode, our research provides deeper insights into the risk assessment of intermediates and their toxicity, assigning new perspectives for practical electrochemical oxidation to effectively eliminate the amount and toxicity of TC and other antibiotics in wastewater. |
| Author | He, Xuwen Zhi, Dan Wang, Jianbing Zhou, Hao Zhang, Dayi |
| Author_xml | – sequence: 1 givenname: Jianbing orcidid: 0000-0003-2755-1403 surname: Wang fullname: Wang, Jianbing email: wangjb@cumtb.edu.cn organization: School of Chemical and Environmental Engineering, Beijing Campus, China University of Mining and Technology, Beijing 100083, PR China – sequence: 2 givenname: Dan surname: Zhi fullname: Zhi, Dan organization: School of Chemical and Environmental Engineering, Beijing Campus, China University of Mining and Technology, Beijing 100083, PR China – sequence: 3 givenname: Hao surname: Zhou fullname: Zhou, Hao organization: School of Chemical and Environmental Engineering, Beijing Campus, China University of Mining and Technology, Beijing 100083, PR China – sequence: 4 givenname: Xuwen surname: He fullname: He, Xuwen organization: School of Chemical and Environmental Engineering, Beijing Campus, China University of Mining and Technology, Beijing 100083, PR China – sequence: 5 givenname: Dayi orcidid: 0000-0002-4175-5982 surname: Zhang fullname: Zhang, Dayi email: zhangdayi@tsinghua.org.cn organization: School of Environment, Tsinghua University, Beijing 100084, PR China |
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| ContentType | Journal Article |
| Copyright | 2018 Elsevier Ltd Copyright © 2018 Elsevier Ltd. All rights reserved. |
| Copyright_xml | – notice: 2018 Elsevier Ltd – notice: Copyright © 2018 Elsevier Ltd. All rights reserved. |
| DBID | AAYXX CITATION 7X8 7S9 L.6 |
| DOI | 10.1016/j.watres.2018.03.030 |
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| DeliveryMethod | fulltext_linktorsrc |
| Discipline | Engineering |
| EISSN | 1879-2448 |
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| Snippet | Tetracycline (TC) is one of the most widely used antibiotics with significant impacts on human health and thus it needs appropriate approaches for its removal.... |
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| SubjectTerms | anodes bacteria bioluminescence carboxylic acids chemical bonding Degradation pathway durability Electrochemical oxidation electrochemistry free radicals gas chromatography high performance liquid chromatography human health hydroxyl radicals oxidation quantitative structure-activity relationships spectrometers spraying Tetracycline Ti/Ti4O7 anode toxicity Toxicity assessment wastewater |
| Title | Evaluating tetracycline degradation pathway and intermediate toxicity during the electrochemical oxidation over a Ti/Ti4O7 anode |
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