漆酶/ABTS介体系统催化氧化羟基化多溴联苯醚  

Transformation of hydroxylation polybrominateddiphenyl ethers in laccase-ABTS system

作　　者：张司雨 董仕鹏 高士祥[2] 卢坤 ZHANG Siyu;DONG Shipeng;GAO Shixiang;LU Kun(School of Computer Science and Information Engineering,Hefei University of Technology,Hefei,230601,China;State Key Laboratory of Pollution Control and Resource,School of the Environment,Nanjing University,Nanjing,210023,China)

机构地区：[1]合肥工业大学计算机与信息学院,合肥230601 [2]南京大学环境学院,污染控制与资源化研究国家重点实验室,南京210023

出　　处：《环境化学》2022年第12期3855-3865,共11页Environmental Chemistry

基　　金：国家自然科学基金(21906080);江苏省自然科学基金(BK20190318)资助.

摘　　要：本研究选取3-OH-BDE-7为典型的羟基化多溴联苯醚(OH-PBDEs),系统探究了3-OH-BDE-7在基于二(3-乙基-苯并噻唑-6-磺酸)二铵盐(ABTS)的漆酶介体系统中的转化动力学过程,考察了ABTS投加量、漆酶投加量、pH值和温度以及天然有机质对酶介体系统介导3-OH-BDE-7转化过程的影响.结果表明,3-OH-BDE-7在单一漆酶体系下去除率较低,加入2.0μmol·L^(−1)ABTS后,3-OH-BDE-7去除率提高了约20倍.3-OH-BDE-7在漆酶介体系统的转化过程符合假一级动力学过程,其假一级动力学常数分别与ABTS投加量和漆酶投加量呈正相关.漆酶介体系统催化氧化3-OH-BDE-7的适宜pH值范围为3—8,适宜的温度范围为25—35℃.此外,天然有机质能够抑制3-OH-BDE-7在漆酶介体系统中的转化过程,主要原因归结于天然有机质能够与底物有机自由基发生反应,使得底物有机自由基重新回到初始状态.本研究不仅对认识羟基化多溴联苯醚在自然环境中的转化过程具有重要意义,而且为合理设计基于漆酶介体系统的废水处理工艺具有重要参考价值.In this study,the transformation kinetics of 3-OH-BDE-7,a typical kind of hydroxylation polybrominateddiphenyl ethers(OH-PBDEs),in laccase-mediator-system(LMS)based on 2,2'-azinobis[3-ethyl-benzothiazoline-6-sulfonic acid]diammonium salt(ABTS)was systematically investigated.The influence of ABTS dosage,laccase dosage,solution pH,temperature and natural organism matter(NOM)on the transformation of 3-OH-BDE-7 was studied.The results showed the removal of 3-OH-BDE-7 in the system containing only laccase was very low,while with the presence of ABTS,the removal of 3-OH-BDE-7 increased about 20 times.Moreover,the removal of 3-OH-BDE-7 followed pseudo-first-order kinetics,and the first-order rate constant was proportional to the dosage of ABTS and laccase,respectively.The optimal pH was between 3 and 8,and the optimal temperature was between 25℃and 35℃.In addition,the presence of natural organic matter significantly inhibited the removal of 3-OH-BDE-7.This was mainly because NOM acted as the quenching agent of the radical intermediates and converted the intermediates back to their original forms.Taken together,this study is not only of key importance in understanding the significance of LMS catalyzed oxidation in the conversion of phenolic compounds in natural environment,but also of great value in the design of treatment processes based on LMS.

关 键 词：羟基化多溴联苯醚 漆酶 介体 动力学 环境因子 

分 类 号：X703[环境科学与工程—环境工程]