Effects of Lewis acid-base site and oxygen vacancy in MgAl minerals on peroxymonosulfate activation towards sulfamethoxazole degradation via radical and non-radical mechanism

被引:15
|
作者
Tian, Chen [1 ]
Dai, Chu [1 ]
Tian, Xike [1 ,2 ]
Nie, Yulun [1 ,2 ]
Yang, Chao [1 ,2 ]
Li, Yong [1 ]
机构
[1] China Univ Geosci, Fac Mat & Chem, Wuhan 430074, Peoples R China
[2] China Univ Geosci, State Key Lab Biogeol & Environm Geol, Wuhan 430074, Peoples R China
基金
中国国家自然科学基金;
关键词
Peroxymonosulfate; Radical; Non-Radical; Regulation; MgAl mineral; SINGLET OXYGEN; EFFICIENT DEGRADATION; FACILE SYNTHESIS; TRIPLET YIELDS; BISPHENOL-A; OXIDATION; XPS; CATALYSTS; SULFATE; WATER;
D O I
10.1016/j.seppur.2021.120437
中图分类号
TQ [化学工业];
学科分类号
0817 ;
摘要
Radicals of SO4 center dot-, OH center dot, non-radical of O-1(2) and even direct oxidation all occurred in peroxymonosulfate (PMS) activation process. Hence, to regulate the above radical or non-radical mechanism is of great significance for the treatment of organic pollutants in practical water. In this work, MgAl-minerals exhibited a satisfied performance in controlling the contribution of radicals (SO4 center dot-, OH center dot) and non-radical (O-1(2)) towards PMS activation based on results of reactive oxygen species scavenger experiments and electron spin resonance spectra. Compared with MgAl-1(61.8%) and MgAl-2 (61.4%) (Al/Mg = 1, 2), MgAl-3 (Al/Mg = 3) exhibited the highest sulfamethoxazole (SMX) removal efficiency (92.5%). Moreover, the contribution of radical and non-radical to SMX degradation were 56.7% and 30.1%, which was different from that of MgAl-1(7.8% and 39.5%) and MgAl-2 (5.2% and 41.6%). The roles of Lewis acid-base site and oxygen vacancies (OVs) in MgAl-minerals on radical and non-radical processes were detailed investigated. Lewis acid sites and OVs can enrich SMX and PMS at the solid-water interface. Simultaneously, OVs promote electron transfer from SMX to PMS acts as electron media, resulting in more SO4 center dot- and OH center dot generation. While the basic sites favored the generation of O-1(2) via PMS self-decomposition mechanism. Therefore, in PMS activation process over MgAl-minerals, the involved reactive oxygen species can be regulated via controlling the amounts of Lewis acid-base sites and oxygen vacancies. This finding provided new insights into PMS oxidation over non-transition metal-based catalysts and water remediation with complex water characteristics.
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页数:9
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