Factors and mechanisms that influence the reactivity of trivalent copper: A novel oxidant for selective degradation of antibiotics

被引:96
作者
Feng, Yong [1 ]
Qing, Weihua [1 ]
Kong, Lingjun [1 ,2 ]
Li, Hailong [1 ,3 ]
Wu, Deli [4 ,5 ]
Fan, Yiang [1 ]
Lee, Po-Heng [6 ]
Shih, Kaimin [1 ]
机构
[1] Univ Hong Kong, Dept Civil Engn, Pokfulam, Hong Kong, Peoples R China
[2] Guangzhou Univ, Sch Environm Sci & Engn, Guangdong Prov Key Lab Radionuclides Pollut Contr, Guangzhou 510006, Guangdong, Peoples R China
[3] Cent S Univ, Sch Energy Sci & Engn, Changsha 410083, Hunan, Peoples R China
[4] Tongji Univ, Sch Environm Sci & Engn, State Key Lab Pollut Control & Resources Reuse, Shanghai 200092, Peoples R China
[5] Shanghai Inst Pollut Control & Ecol Secur, Shanghai 200092, Peoples R China
[6] Hong Kong Polytech Univ, Dept Civil & Environm Engn, Hung Hom, Hong Kong, Peoples R China
关键词
Trivalent copper; Cu3+; Cupryl species; Copper(III) periodate; Selective oxidation; Antibiotics; HYDROGEN-PEROXIDE; RATE CONSTANTS; WASTE-WATER; HYDRATED ELECTRONS; HYDROXYL RADICALS; PULSE-RADIOLYSIS; OXIDATION; PEROXYMONOSULFATE; ACTIVATION; STABILITY;
D O I
10.1016/j.watres.2018.10.090
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
Trivalent copper complexes are active intermediates in aquatic redox reactions that involve copper ions or structural copper, but their reactivity and selectivity toward pollutants remain unknown. We characterized copper(III) periodate, a representative trivalent copper compound, with phenol and several antibiotics as model contaminants. The results show that Cu(III) is highly reactive to phenol degradation; near-complete degradation was achieved after 10 min at a molar ratio of 3:1 (COM: phenol). Common alcohols, including methanol and 2-propanol, showed pH-dependent reactivity for Cu(III). In contrast to aquo trivalent copper ions that react rapidly with tert-butanol, Cu(Ill) showed limited reactivity toward tert-butanol. A mechanistic investigation showed that the degradation was caused by direct oxidation by Cu(Ill) and that no hydroxyl radicals were involved. Common water components such as chloride ions did not influence the reaction, which suggests that the use of Cu(III) may help mitigate the generation of chlorinated products. As a one-electron oxidant, Cu(III) showed high reactivity to degrade electron-rich compounds; the concentrations of sulfamethazine, sulfamethoxazole, and sulfadiazine (100 mu g/L) were reduced to 1.8, 7.5, and 42.5 ng/L, respectively, after 2 min of reaction with 10 mu M Cu(III). These results demonstrate a novel and highly efficient oxidant for selective removal of ubiquitous micropollutants from water bodies. (C) 2018 Elsevier Ltd. All rights reserved.
引用
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页码:1 / 8
页数:8
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