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β-环糊精功能化生物炭催化过二硫酸盐降解双酚A及其类似物的非自由基机制与毒性分析

Non-radical mechanism and toxicity analysis of β-cyclodextrin functionalized biochar catalyzing the degradation of bisphenol A and its analogs by peroxydisulfate.

作者信息

Pei Xuan-Yuan, Ren Hong-Yu, Liu Guo-Shuai, Cao Guang-Li, Xie Guo-Jun, Xing De-Feng, Ren Nan-Qi, Liu Bing-Feng

机构信息

State Key Laboratory of Urban Water Resource and Environment, School of Environment, Harbin Institute of Technology, Harbin 150090, China.

State Key Laboratory of Urban Water Resource and Environment, School of Environment, Harbin Institute of Technology, Harbin 150090, China.

出版信息

J Hazard Mater. 2022 Feb 15;424(Pt A):127254. doi: 10.1016/j.jhazmat.2021.127254. Epub 2021 Sep 22.

Abstract

Bisphenols (BPs) are distributed in worldwide as typical environmental hormones, which potentially harm the ecological environment and human health. In this study, four BPs, i.e., bisphenol A, bisphenol F, bisphenol S, and bisphenol AF, were used as prototypes to identify the intrinsic differences in degradation mechanisms correlated with the molecular structures in peroxydisulfate (PDS)-based advanced oxidation processes (AOPs). Electron transfer was the main way of modified biochar to trigger the heterogenous catalysis of PDS, which can cause the degradation of BPs. Phenolic hydroxyl groups on bisphenol pollutants were considered as possible active sites, and the existence of substituents was the main reason for the differentiation in the degradation efficiency of various bisphenols. Results of ecotoxicity prediction showed that most intermediates produced by the degradation of BPs in the β-SB/PDS system, which was dominated by the electron transfer pathway, had a lower toxicity than the parent molecules, while the toxicity of several ring cleavage intermediates was higher. This study presents a simple modification scheme for the conversion of biochar into functional catalysts and provides insights into the mechanism of heterogeneous catalytic degradation mediated by modified biochar as well as the degradation differences of bisphenol pollutants and their potential ecotoxicity.

摘要

双酚类物质(BPs)作为典型的环境激素在全球范围内广泛分布,对生态环境和人类健康具有潜在危害。本研究以双酚A、双酚F、双酚S和双酚AF这四种双酚类物质为原型,以识别基于过硫酸盐(PDS)的高级氧化过程(AOPs)中与分子结构相关的降解机制的内在差异。电子转移是改性生物炭触发PDS非均相催化从而导致双酚类物质降解的主要方式。双酚类污染物上的酚羟基被认为是可能的活性位点,取代基的存在是导致各种双酚类物质降解效率差异的主要原因。生态毒性预测结果表明,在以电子转移途径为主的β-SB/PDS体系中,双酚类物质降解产生的大多数中间产物的毒性低于母体分子,而几种开环中间产物的毒性较高。本研究提出了一种将生物炭转化为功能催化剂的简单改性方案,并深入探讨了改性生物炭介导的非均相催化降解机制以及双酚类污染物的降解差异及其潜在的生态毒性。

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