Peroxymonosulfate activation using a composite of copper and nickel oxide coated on SBA-15 for the removal of sulfonamide antibiotics

被引:23
作者
Yu, Dan [1 ,2 ]
He, Jiahong [1 ]
Xie, Taiping [3 ]
Xu, Qiang [1 ]
Li, Guoqiang [1 ]
Du, Ling [1 ]
Huang, Junhao [1 ]
Yang, Jun [1 ]
Li, Wenpo [2 ]
Wang, Jiankang [3 ]
机构
[1] Chongqing Univ Arts & Sci, Coll Chem & Environm Engn, Chongqing Key Lab Environm Mat & Remediat Technol, Yongchuan 402160, Peoples R China
[2] Chongqing Univ, Sch Chem & Chem Engn, Chongqing 400044, Peoples R China
[3] Yangtze Normal Univ, Sch Mat Sci & Engn, Chongqing 408100, Peoples R China
基金
中国国家自然科学基金;
关键词
Peroxymonosulfate (PMS); Sulfonamide antibiotics; Active species; Heterogeneous catalysis; DEGRADATION; PERSULFATE; GENERATION; OXIDATION; GRAPHENE; SULFAMETHOXAZOLE; ADSORPTION;
D O I
10.1016/j.envres.2021.112301
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
The sluggish Ni(II)/Ni(III) redox cycle does not benefit perxymonosulfate (PMS) activation for recalcitrant pollutant degradation. To solve this problem, a heterogeneous catalyst, Cu0.2Ni0.8O/SBA-15 (CNS), was constructed to activate PMS for decomposing two sulfonamide antibiotics, sulfachlorpyridazine (SACP) and sulfapyridine (SAP). SACP and SAP were completely degraded over Cu0.2Ni0.8O/SBA-15/PMS (CNSP) after 90 min. O-2(center dot-) was the dominant active species involved in the degradation of SACP and SAP. Structural analysis and elemental valence state observations indicated that Cu(I) provided electrons through Cu-O-Ni bonds to realize the charge compensation for Ni(III) in the CNSP system. Thus, the in situ Cu(I)/Cu(II) promoting the Ni(II)/Ni (III) cycle could accelerate the PMS activation. This work provides new insights into the electron transfer between transition metals and the charge compensation mechanism for PMS activation. The degradation mechanism was proposed based on the XPS results before and after the reaction, a radical quenching test, and an EPR test. Combined with the SACP and SAP degradation intermediates identified by LC-MS, we suggest that the choice of treatment process depends on the occurrence of a steric hindrance effect between the molecular structure of the degradation target and free radicals.
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页数:11
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