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过氧氢(H2O2)和过硫酸钠(SPS)引发的双酚 A(BPA)光氧化反应的机理研究。

Mechanistic study of photo-oxidation of Bisphenol-A (BPA) with hydrogen peroxide (H2O2) and sodium persulfate (SPS).

机构信息

Department of Chemical Engineering, Indian Institute of Technology, Roorkee, Roorkee, 247667, India.

Department of Chemical Engineering, Indian Institute of Technology, Roorkee, Roorkee, 247667, India; Department of Chemical Engineering, Indian School of Mines, Dhanbad, Jharkhand, India.

出版信息

J Environ Manage. 2016 Jan 15;166:12-22. doi: 10.1016/j.jenvman.2015.09.043. Epub 2015 Oct 24.

Abstract

The removal of Bisphenol-A (BPA) from contaminated water using advanced oxidation methods such as UV-C assisted oxidation by hydrogen peroxide (H2O2) and sodium persulfate (SPS) has been reported by the authors earlier (Sharma et al., 2015a). In the present study, the authors report the removal of BPA from aqueous solution by the above two methods and its degradation mechanism. UV-C light (254 nm wavelength, 40 W power) was applied to BPA contaminated water at natural pH (pHN) under room temperature conditions. Experiments were carried out with the initial BPA concentration in the range of 0.04 mM-0.31 mM and the oxidant/BPA molar ratio in the range of 294:1-38:1 for UV-C/H2O2 and 31.5-4.06:1 for UV-C/SPS systems. The removal of BPA enhanced with decreasing BPA concentration. The total organic carbon also decreased with the UV-C irradiation time under optimum conditions ([H2O2]0 = 11.76 mM; [SPS]0 = 1.26 mM; temperature (29 ± 3 °C). Competition of BPA for reaction with HO or [Formula: see text] radicals at its higher concentrations results in a decrease in the removal of BPA. The intermediates with smaller and higher molecular weights than that of BPA were found in the treated water. Based on GC-MS and FTIR spectra of the reaction mixture, the formation of hydroxylated by-products testified the HO mediated oxidation pathway in the BPA degradation, while the formation of quinones and phenoxy phenols pointed to the [Formula: see text] dominating pathway through the formation of hydroxycyclohexadienyl (HCHD) and BPA phenoxyl radicals. The main route of BPA degradation is the hydroxylation followed by dehydration, coupling and ring opening reactions.

摘要

作者之前曾报道过(Sharma 等人,2015a)使用高级氧化方法(如过氧化氢(H2O2)和过硫酸钠(SPS)辅助的 UV-C 氧化)从受污染的水中去除双酚 A(BPA)。在本研究中,作者报告了通过上述两种方法从水溶液中去除 BPA 及其降解机制。在室温条件下,在自然 pH(pHN)下将 UV-C 光(254nm 波长,40W 功率)应用于受 BPA 污染的水中。实验在初始 BPA 浓度为 0.04mM-0.31mM 和氧化剂/BPA 摩尔比为 294:1-38:1 的范围内进行UV-C/H2O2 系统和 31.5-4.06:1 的 UV-C/SPS 系统。随着 BPA 浓度的降低,BPA 的去除率增加。在最佳条件下([H2O2]0=11.76mM;[SPS]0=1.26mM;温度(29±3°C),随着 UV-C 辐照时间的增加,总有机碳也减少。在较高浓度下,BPA 与 HO 或[Formula: see text]自由基竞争反应导致 BPA 去除率降低。在处理水中发现了分子量小于和大于 BPA 的中间体。基于反应混合物的 GC-MS 和 FTIR 谱,羟基化副产物的形成证明了 BPA 降解中 HO 介导的氧化途径,而醌和苯氧基苯酚的形成则表明[Formula: see text]主导途径通过形成羟基环己二烯基(HCHD)和 BPA 苯氧基自由基。BPA 降解的主要途径是羟化,随后是脱水、偶联和开环反应。

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