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可见光促有机物诱导铁还原的多相类芬顿体系强化效能与机制
摘要点击 479  全文点击 87  投稿时间:2021-08-31  修订日期:2021-10-25
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中文关键词  Fe3+还原  过硫酸盐高级氧化  可见光催化  电子传递  双酚A
英文关键词  Fe3+reduction  advanced oxidation of persulfate  visible light catalysis  electron transfer  bisphenol A
作者单位E-mail
曹丝雨 西安建筑科技大学环境与市政工程学院, 西安 710055 734709675@qq.com 
许路 西安交通大学人居环境与建筑工程学院, 西安 710049  
付权超 西安建筑科技大学环境与市政工程学院, 西安 710055  
金鑫 西安交通大学人居环境与建筑工程学院, 西安 710049  
石烜 西安交通大学人居环境与建筑工程学院, 西安 710049  
金鹏康 西安建筑科技大学环境与市政工程学院, 西安 710055
西安交通大学人居环境与建筑工程学院, 西安 710049 
pkjin@hotmail.com 
中文摘要
      近年来,亚铁离子活化过硫酸盐的类芬顿(Fe2+-PMS/PS)高级氧化技术发展日趋成熟,但因Fe3+无法还原导致反应停止的问题仍制约其大规模应用.结果发现,当把以双酚A (BPA)为代表的某些有机物与Fe3+和TiO2混合,所形成的某种络合物可以拓宽TiO2光响应范围捕获可见光,通过TiO2将光生电子传递给Fe3+进行还原,从而实现Fe3+/Fe2+的无限循环.依据上述原理,构建了可见光下BPA-TiO2-Fe3+-PS复合体系来降解BPA,并对其催化性能、催化机制和影响因素进行探讨.结果表明,该体系具有突出的催化性能,60 min内BPA (50 mg·L-1)降解率达到93.1%,矿化度达到70%.同时验证该体系可以通过双酚A自生光电子还原Fe3+,60 min还原得到的Fe2+稳态浓度为3.5 μmol·L-1.体系中主要的活性氧化物质为硫酸根自由基(SO4-·)和羟基自由基(·OH),其中·OH贡献率超过60%.适当提高TiO2、Fe3+和PS投加量以及光照强度可以提高BPA的降解效果.该体系在弱酸性条件下处理效果最好,降解率达到96.5%,在中性条件下也有很好的效果;CO32-、H2PO4-和SO42-对体系有一定抑制作用.
英文摘要
      In recent years, the Fenton-like (Fe2+-PMS/PS) advanced oxidation technology of persulfate activated by ferrous ions has been increasingly developed, but the difficulty of Fe3+ reduction, which stops the reaction, still restricts its large-scale application. In this study, it was found that when some organic compounds represented by bisphenol A (BPA) were mixed with Fe3+ and pristine TiO2, some surface structures could broaden the light response range of TiO2, capture visible light, and transfer the photoelectrons to Fe3+ through TiO2 for reduction, so as to achieve an infinite cycle of Fe3+/Fe2+. According to the above principle, a BPA-TiO2-Fe3+-PS composite system under visible light was constructed to degrade BPA, and its catalytic performance, catalytic mechanism, and influencing factors were discussed. The results showed that the system had outstanding catalytic performance, the degradation efficiency of BPA (50 mg·L-1) reached 93.1%, and the mineralization efficiency reached 70% within 60 min. At the same time, it verified that the system could reduce Fe3+ by the authigenic photoelectron of bisphenol A, and the steady-state concentration of Fe2+ obtained by 60 min reduction was 3.5 μmol·L-1. The main active oxidizing species in the system were sulfate radicals (SO4-[KG-*2/3]·) and hydroxyl radicals (·OH), of which the contribution rate of·OH was more than 60%. An appropriate increase in TiO2, Fe3+, and PS dosage and light intensity could improve the degradation effect. The system had the best treatment efficiency under weak acid conditions, and the degradation efficiency reached 96.5%. It also had a good effect under neutral conditions. CO32-, H2PO4-, and SO42- had a certain inhibitory effect on the system.

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