化学
激进的
路易斯酸
羟基自由基
电子顺磁共振
氧气
电子转移
光化学
基础(拓扑)
催化作用
无机化学
有机化学
物理
核磁共振
数学分析
数学
作者
Chen Tian,Chu Dai,Xike Tian,Yulun Nie,Chao Yang,Yong Li
标识
DOI:10.1016/j.seppur.2021.120437
摘要
• Non-transition metal MgAl minerals exhibits excellent activity towards SMX removal. • Radical and non-radical are involved in MgAl/PMS system. • Mechanism dominated by radical and non-radical is realized by adjusting MgAl ratio. • Interaction of acid sites and OVs contributes to the generation of • OH and SO 4 •- . • The basic sites are beneficial for the self-decomposition of PMS to produce 1 O 2 . Radicals of SO 4 •- , OH • , non-radical of 1 O 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 (SO 4 •- , OH • ) and non-radical ( 1 O 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 SO 4 •- and OH • generation. While the basic sites favored the generation of 1 O 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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