Novel Cu(II)–EDTA Decomplexation by Discharge Plasma Oxidation and Coupled Cu Removal by Alkaline Precipitation: Underneath Mechanisms

Strong complexation between heavy metals and organic complexing agents makes the heavy metals difficult to be removed by classical chemical precipitation. In this study, a novel decomplexation method was developed using discharge plasma oxidation, which was followed by alkaline precipitation to trea...

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Published in	Environmental science & technology Vol. 52; no. 14; pp. 7884 - 7891
Main Authors	Wang, Tiecheng, Cao, Yang, Qu, Guangzhou, Sun, Qiuhong, Xia, Tianjiao, Guo, Xuetao, Jia, Hanzhong, Zhu, Lingyan
Format	Journal Article
Language	English
Published	United States American Chemical Society 17.07.2018
Subjects	Acetic acid ammonium Carbon Chemical precipitation Coordination compounds Copper cupric oxide Discharge Edetic acid EDTA (chelating agent) Energy efficiency Ethylenediaminetetraacetic acids Fluorescence Fourier transform infrared spectroscopy Heavy metals hydroxyl radicals Intermediates nitrates Organic acids Organic carbon Organic chemistry Oxidation ozone Plasma Precipitates singlet oxygen superoxide anion Total organic carbon ultraviolet-visible spectroscopy Water treatment
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Abstract	Strong complexation between heavy metals and organic complexing agents makes the heavy metals difficult to be removed by classical chemical precipitation. In this study, a novel decomplexation method was developed using discharge plasma oxidation, which was followed by alkaline precipitation to treat water containing heavy metal–organic complex, that is, Cu–ethylenediaminetetraacetic acid (Cu–EDTA). The decomplexation efficiency of Cu complex reached up to nearly 100% after 60 min’s oxidation by discharge plasma, which was accompanied by 82.1% of total organic carbon removal and energy efficiency of 0.62 g kWh–1. Presence of free Cu2+ favored Cu–EDTA decomplexation, whereas the presence of excessive EDTA depressed this process. Cu–EDTA decomplexation was mainly driven by the produced 1O2, O2 •–, O3, and •OH by discharge plasma. Cu–EDTA decomplexation process was characterized by UV–vis, ATR–FTIR, total organic carbon, and three-dimensional fluorescence diagnosis. The main intermediates including Cu–EDDA, Cu–IDA, Cu–NTA, small organic acids, NH4 +, and NO3 – were identified, accompanied by Cu2+ releasing. The followed precipitation process removed 78.1% of Cu2+, and Cu-associated precipitates included CuCO3, Cu2CO3(OH)2, CuO, and Cu(OH)2. A possible pathway of Cu complex decomplexation and Cu2+ removal in such a system was proposed.
AbstractList	Strong complexation between heavy metals and organic complexing agents makes the heavy metals difficult to be removed by classical chemical precipitation. In this study, a novel decomplexation method was developed using discharge plasma oxidation, which was followed by alkaline precipitation to treat water containing heavy metal–organic complex, that is, Cu–ethylenediaminetetraacetic acid (Cu–EDTA). The decomplexation efficiency of Cu complex reached up to nearly 100% after 60 min’s oxidation by discharge plasma, which was accompanied by 82.1% of total organic carbon removal and energy efficiency of 0.62 g kWh–1. Presence of free Cu2+ favored Cu–EDTA decomplexation, whereas the presence of excessive EDTA depressed this process. Cu–EDTA decomplexation was mainly driven by the produced 1O2, O2 •–, O3, and •OH by discharge plasma. Cu–EDTA decomplexation process was characterized by UV–vis, ATR–FTIR, total organic carbon, and three-dimensional fluorescence diagnosis. The main intermediates including Cu–EDDA, Cu–IDA, Cu–NTA, small organic acids, NH4 +, and NO3 – were identified, accompanied by Cu2+ releasing. The followed precipitation process removed 78.1% of Cu2+, and Cu-associated precipitates included CuCO3, Cu2CO3(OH)2, CuO, and Cu(OH)2. A possible pathway of Cu complex decomplexation and Cu2+ removal in such a system was proposed. Strong complexation between heavy metals and organic complexing agents makes the heavy metals difficult to be removed by classical chemical precipitation. In this study, a novel decomplexation method was developed using discharge plasma oxidation, which was followed by alkaline precipitation to treat water containing heavy metal–organic complex, that is, Cu–ethylenediaminetetraacetic acid (Cu–EDTA). The decomplexation efficiency of Cu complex reached up to nearly 100% after 60 min’s oxidation by discharge plasma, which was accompanied by 82.1% of total organic carbon removal and energy efficiency of 0.62 g kWh–1. Presence of free Cu2+ favored Cu–EDTA decomplexation, whereas the presence of excessive EDTA depressed this process. Cu–EDTA decomplexation was mainly driven by the produced 1O2, O2•–, O3, and •OH by discharge plasma. Cu–EDTA decomplexation process was characterized by UV–vis, ATR–FTIR, total organic carbon, and three-dimensional fluorescence diagnosis. The main intermediates including Cu–EDDA, Cu–IDA, Cu–NTA, small organic acids, NH4+, and NO3– were identified, accompanied by Cu2+ releasing. The followed precipitation process removed 78.1% of Cu2+, and Cu-associated precipitates included CuCO3, Cu2CO3(OH)2, CuO, and Cu(OH)2. A possible pathway of Cu complex decomplexation and Cu2+ removal in such a system was proposed. Strong complexation between heavy metals and organic complexing agents makes the heavy metals difficult to be removed by classical chemical precipitation. In this study, a novel decomplexation method was developed using discharge plasma oxidation, which was followed by alkaline precipitation to treat water containing heavy metal–organic complex, that is, Cu–ethylenediaminetetraacetic acid (Cu–EDTA). The decomplexation efficiency of Cu complex reached up to nearly 100% after 60 min’s oxidation by discharge plasma, which was accompanied by 82.1% of total organic carbon removal and energy efficiency of 0.62 g kWh–¹. Presence of free Cu²⁺ favored Cu–EDTA decomplexation, whereas the presence of excessive EDTA depressed this process. Cu–EDTA decomplexation was mainly driven by the produced ¹O₂, O₂•–, O₃, and •OH by discharge plasma. Cu–EDTA decomplexation process was characterized by UV–vis, ATR–FTIR, total organic carbon, and three-dimensional fluorescence diagnosis. The main intermediates including Cu–EDDA, Cu–IDA, Cu–NTA, small organic acids, NH₄⁺, and NO₃– were identified, accompanied by Cu²⁺ releasing. The followed precipitation process removed 78.1% of Cu²⁺, and Cu-associated precipitates included CuCO₃, Cu₂CO₃(OH)₂, CuO, and Cu(OH)₂. A possible pathway of Cu complex decomplexation and Cu²⁺ removal in such a system was proposed. Strong complexation between heavy metals and organic complexing agents makes the heavy metals difficult to be removed by classical chemical precipitation. In this study, a novel decomplexation method was developed using discharge plasma oxidation, which was followed by alkaline precipitation to treat water containing heavy metal-organic complex, that is, Cu-ethylenediaminetetraacetic acid (Cu-EDTA). The decomplexation efficiency of Cu complex reached up to nearly 100% after 60 min's oxidation by discharge plasma, which was accompanied by 82.1% of total organic carbon removal and energy efficiency of 0.62 g kWh-1. Presence of free Cu2+ favored Cu-EDTA decomplexation, whereas the presence of excessive EDTA depressed this process. Cu-EDTA decomplexation was mainly driven by the produced 1O2, O2•-, O3, and •OH by discharge plasma. Cu-EDTA decomplexation process was characterized by UV-vis, ATR-FTIR, total organic carbon, and three-dimensional fluorescence diagnosis. The main intermediates including Cu-EDDA, Cu-IDA, Cu-NTA, small organic acids, NH4+, and NO3- were identified, accompanied by Cu2+ releasing. The followed precipitation process removed 78.1% of Cu2+, and Cu-associated precipitates included CuCO3, Cu2CO3(OH)2, CuO, and Cu(OH)2. A possible pathway of Cu complex decomplexation and Cu2+ removal in such a system was proposed.Strong complexation between heavy metals and organic complexing agents makes the heavy metals difficult to be removed by classical chemical precipitation. In this study, a novel decomplexation method was developed using discharge plasma oxidation, which was followed by alkaline precipitation to treat water containing heavy metal-organic complex, that is, Cu-ethylenediaminetetraacetic acid (Cu-EDTA). The decomplexation efficiency of Cu complex reached up to nearly 100% after 60 min's oxidation by discharge plasma, which was accompanied by 82.1% of total organic carbon removal and energy efficiency of 0.62 g kWh-1. Presence of free Cu2+ favored Cu-EDTA decomplexation, whereas the presence of excessive EDTA depressed this process. Cu-EDTA decomplexation was mainly driven by the produced 1O2, O2•-, O3, and •OH by discharge plasma. Cu-EDTA decomplexation process was characterized by UV-vis, ATR-FTIR, total organic carbon, and three-dimensional fluorescence diagnosis. The main intermediates including Cu-EDDA, Cu-IDA, Cu-NTA, small organic acids, NH4+, and NO3- were identified, accompanied by Cu2+ releasing. The followed precipitation process removed 78.1% of Cu2+, and Cu-associated precipitates included CuCO3, Cu2CO3(OH)2, CuO, and Cu(OH)2. A possible pathway of Cu complex decomplexation and Cu2+ removal in such a system was proposed. Strong complexation between heavy metals and organic complexing agents makes the heavy metals difficult to be removed by classical chemical precipitation. In this study, a novel decomplexation method was developed using discharge plasma oxidation, which was followed by alkaline precipitation to treat water containing heavy metal-organic complex, that is, Cu-ethylenediaminetetraacetic acid (Cu-EDTA). The decomplexation efficiency of Cu complex reached up to nearly 100% after 60 min's oxidation by discharge plasma, which was accompanied by 82.1% of total organic carbon removal and energy efficiency of 0.62 g kWh . Presence of free Cu favored Cu-EDTA decomplexation, whereas the presence of excessive EDTA depressed this process. Cu-EDTA decomplexation was mainly driven by the produced O , O , O , and •OH by discharge plasma. Cu-EDTA decomplexation process was characterized by UV-vis, ATR-FTIR, total organic carbon, and three-dimensional fluorescence diagnosis. The main intermediates including Cu-EDDA, Cu-IDA, Cu-NTA, small organic acids, NH , and NO were identified, accompanied by Cu releasing. The followed precipitation process removed 78.1% of Cu , and Cu-associated precipitates included CuCO , Cu CO (OH) , CuO, and Cu(OH) . A possible pathway of Cu complex decomplexation and Cu removal in such a system was proposed.
Author	Xia, Tianjiao Sun, Qiuhong Qu, Guangzhou Cao, Yang Wang, Tiecheng Jia, Hanzhong Zhu, Lingyan Guo, Xuetao
AuthorAffiliation	Key Laboratory of Plant Nutrition and the Agri-environment in Northwest China College of Natural Resources and Environment Institute of Soil and Water Conservation Northwest A&F University Ministry of Agriculture
AuthorAffiliation_xml	– name: Ministry of Agriculture – name: Northwest A&F University – name: Institute of Soil and Water Conservation – name: Key Laboratory of Plant Nutrition and the Agri-environment in Northwest China – name: College of Natural Resources and Environment
Author_xml	– sequence: 1 givenname: Tiecheng orcidid: 0000-0003-1085-9946 surname: Wang fullname: Wang, Tiecheng organization: Ministry of Agriculture – sequence: 2 givenname: Yang surname: Cao fullname: Cao, Yang organization: Ministry of Agriculture – sequence: 3 givenname: Guangzhou surname: Qu fullname: Qu, Guangzhou organization: Ministry of Agriculture – sequence: 4 givenname: Qiuhong surname: Sun fullname: Sun, Qiuhong organization: Northwest A&F University – sequence: 5 givenname: Tianjiao surname: Xia fullname: Xia, Tianjiao organization: Ministry of Agriculture – sequence: 6 givenname: Xuetao surname: Guo fullname: Guo, Xuetao organization: Ministry of Agriculture – sequence: 7 givenname: Hanzhong orcidid: 0000-0002-9838-2881 surname: Jia fullname: Jia, Hanzhong email: jiahz@nwafu.edu.cn organization: Ministry of Agriculture – sequence: 8 givenname: Lingyan orcidid: 0000-0001-9318-7940 surname: Zhu fullname: Zhu, Lingyan organization: Ministry of Agriculture
BackLink	https://www.ncbi.nlm.nih.gov/pubmed/29928796$$D View this record in MEDLINE/PubMed
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Snippet	Strong complexation between heavy metals and organic complexing agents makes the heavy metals difficult to be removed by classical chemical precipitation. In...
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SubjectTerms	Acetic acid ammonium Carbon Chemical precipitation Coordination compounds Copper cupric oxide Discharge Edetic acid EDTA (chelating agent) Energy efficiency Ethylenediaminetetraacetic acids Fluorescence Fourier transform infrared spectroscopy Heavy metals hydroxyl radicals Intermediates nitrates Organic acids Organic carbon Organic chemistry Oxidation ozone Plasma Precipitates singlet oxygen superoxide anion Total organic carbon ultraviolet-visible spectroscopy Water treatment
Title	Novel Cu(II)–EDTA Decomplexation by Discharge Plasma Oxidation and Coupled Cu Removal by Alkaline Precipitation: Underneath Mechanisms
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