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硝酸盐、碳酸盐/碳酸氢盐、腐殖酸和 HO 对 UV 光解过程中双酚 A 的动力学和降解机制的影响。

Effect of nitrate, carbonate/bicarbonate, humic acid, and HO on the kinetics and degradation mechanism of Bisphenol-A during UV photolysis.

机构信息

Department of Environmental Health Sciences, School of Public Health, Seoul National University, Seoul, South Korea.

Department of Environmental Health Sciences, School of Public Health, Seoul National University, Seoul, South Korea.

出版信息

Chemosphere. 2018 Aug;204:148-155. doi: 10.1016/j.chemosphere.2018.04.015. Epub 2018 Apr 6.

Abstract

In this study, the effects of natural water components (nitrate, carbonate/bicarbonate, and humic acid) on the kinetics and degradation mechanisms of bisphenol A (BPA) during UV-C photolysis and UV/HO reaction were examined. The presence of NO (0.04-0.4 mM) and CO/HCO (0.4-4 mM) ions increased BPA degradation during UV photolysis. Humic acid less than 3 mg/L promoted BPA degradation, but greater than 3 mg/L of humic acid inhibited BPA degradation. During the UV/HO reaction, all water matrix components acted as radical scavengers in the order of humic acid > CO/HCO > NO. All of the degradation reactions agreed with the pseudo-first-order kinetics. While eight byproducts (m/z = 122, 136, 139, 164, 181, 244, 273, 289) were identified in UV-C/NO photolysis reaction, four (m/z = 122, 136, 164, 244) and three byproducts (m/z = 122, 136, 164) were observed during UV-C/NO/CO/HCO and UV-C/CO/HCO reactions. Nitrogenated and hydrogenated byproducts were first observed during the UV-C/NO photolysis, but only hydrogenated byproducts as adducts were detected during the UV-C/NO/CO/HCO photolysis. Nitrogenated and hydrogenated byproducts were formed in the early stage of degradation by OH or NO radicals, and these byproducts were subsequently degraded into smaller compounds with further reaction during UV-C/NO and UV-C/NO/CO/HCO reactions. In contrast, BPA was directly degraded into smaller compounds by β-scission of the isopropyl group by CO/HCO radicals during UV-C/CO/HCO reaction. Our results imply that the water components can change the degradation mechanism of BPA during UV photolysis.

摘要

在这项研究中,考察了天然水成分(硝酸盐、碳酸盐/碳酸氢盐和腐殖酸)对双酚 A(BPA)在 UV-C 光解和 UV/HO 反应中的动力学和降解机制的影响。NO(0.04-0.4 mM)和 CO/HCO(0.4-4 mM)离子的存在增加了 UV 光解过程中 BPA 的降解。小于 3mg/L 的腐殖酸促进了 BPA 的降解,但大于 3mg/L 的腐殖酸抑制了 BPA 的降解。在 UV/HO 反应中,所有水基质成分按腐殖酸>CO/HCO>NO 的顺序充当自由基清除剂。所有降解反应均符合准一级动力学。虽然在 UV-C/NO 光解反应中鉴定出了 8 种副产物(m/z=122、136、139、164、181、244、273、289),但在 UV-C/NO/CO/HCO 和 UV-C/CO/HCO 反应中仅观察到 4 种(m/z=122、136、164、244)和 3 种副产物(m/z=122、136、164)。在 UV-C/NO 光解过程中首次观察到氮化物和氢化副产物,但仅在 UV-C/NO/CO/HCO 光解过程中检测到作为加合物的氢化副产物。氮化物和氢化副产物是由 OH 或 NO 自由基在降解的早期形成的,并且这些副产物随后在 UV-C/NO 和 UV-C/NO/CO/HCO 反应中进一步降解成较小的化合物。相比之下,在 UV-C/CO/HCO 反应中,BPA 直接由 CO/HCO 自由基通过异丙基的β断裂降解成较小的化合物。我们的结果表明,水成分可以改变 UV 光解过程中 BPA 的降解机制。

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