Comparative study on bisphenols oxidation via TiO2 photocatalytic activation of peroxymonosulfate: Effectiveness, mechanism and pathways

Comparative study on bisphenols oxidation via TiO2 photocatalytic activation of peroxymonosulfate: Effectiveness, mechanism and pathways
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DOI:
10.1016/j.jhazmat.2021.127434
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发表时间:
2021-10-23
影响因子:
13.6
通讯作者:
Tian, Jiayu
Tian, Jiayu
中科院分区:
环境科学与生态学1区
文献类型:
--
作者:
Jia, Jialin;Liu, Dongmei;Tian, Jiayu

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本文首次研究了模拟太阳光照射下,过氧单硫酸盐(PMS)负载TiO 2纳米管阵列(TiO 2 NTAs)对双酚F(BPF)、双酚AF(BPAF)和双酚S(BPS)的降解效果,并进行了比较。三种双酚的降解顺序为BPS < BPAF < BPF,酸性条件更有利于它们的降解。在三种双酚降解过程中均发现了SO 4中心点-、.OH、h+和中心点O2-。其中,SO 4中心点-和中心点O2-在BPF氧化过程中起主导作用,而SO 4中心点-和h+是BPAF和BPS去除的主要反应物种。由于在不同的双酚降解过程中起作用的活性物种不同,无机阴离子对三种双酚降解的影响也不同。通过对三种双酚氧化中间产物的分析,发现三种双酚的氧化降解有一些共同的途径,包括键断裂和苯环羟基化。此外,还发现了一些特定的降解途径,如BPF和BPS降解过程中存在自偶联,而BPAF转化过程中只存在苯环裂解
In this work, degradation of bisphenol F (BPF), bisphenol AF (BPAF) and bisphenol S (BPS) by perox-ymonosulfate (PMS) with TiO2 nano-tubes arrays (TiO2NTAs) under simulated sunlight irradiation was inves-tigated and compared for the first time. All three bisphenols exhibited appreciable degradation following the order of BPS < BPAF < BPF, and acidic conditions were more conducive to their degradation. The SO4 center dot-, .OH, h+ and center dot O2-were all identified in three bisphenols degradation processes. Among these, SO4 center dot-and center dot O2-were proven to play a dominant role in BPF oxidation process, but SO4 center dot-and h+ were confirmed as the main reactive species for BPAF and BPS removal. Owing to the different reactive species worked in different bisphenols degradation processes, the influences of inorganic anions on three bisphenols degradation were also different. By analyzing the oxidation intermediates of the three bisphenols, it was found that there were some common degradation pathways including bond-cleavage and hydroxylation of the benzene ring shared by three bisphenols. Besides, some specific degradation pathways were also identified, for example, the self-coupling was found in BPF and BPS degradation process, while the benzene ring splitting was occurred only in BPAF transformation process