摘要
邻苯二甲酸酯(PAEs)是典型的环境内分泌干扰物,广泛用作塑料增塑剂,具有生态和健康风险.本研究结合分子对接和分子动力学模拟(MD)技术,考察了PAEs结构与酶解性能的关系,深入探究了漆酶降解PAEs的分子机制.研究结果表明,PAEs与漆酶的亲和力随其烷基链长度和酯基数量增加而降低,但受链结构(直链/支链)影响较小.通过30 ns的MD模拟分析发现,漆酶-PAEs复合物具有较高的结合稳定性(结合能(-75.684±4.068)kJ·mol^(-1)),其中范德华力为主导作用力,且复合物间最多可形成2个氢键.关键残基分析表明,Ala80、Phe81、Leu112、Pro346和Glu460在漆酶催化PAEs过程中起核心作用.本研究为漆酶介导的PAEs降解机制提供了分子层面的理论依据,对环境污染修复技术的开发具有指导意义.
Phthalates(PAEs),widely used as plasticizers,are typical environmental endocrinedisrupting chemicals that pose significant ecological and human health risks.In this study,molecular docking and molecular dynamics(MD)simulations were employed to elucidate the structure-activity relationship of PAEs and to investigate the molecular mechanism underlying their enzymatic degradation by laccase.The results indicated that the binding affinity of PAEs to laccase decreased with increasing alkyl chain length and the number of ester groups,while the chain structure(linear vs.branched)had a negligible effect.A 30 ns MD simulation revealed that the laccase-PAEs complexes exhibited high binding stability,with an average binding energy of(-75.684±4.068)kJ·mol^(-1).The interaction was predominantly governed by van der Waals forces,and up to two hydrogen bonds were formed within the complexes.Key residue analysis identified Ala80,Phe81,Leu112,Pro346,and Glu460 as critical amino acids involved in the catalytic degradation of PAEs.These findings provide molecular-level insights into the laccase-mediated degradation pathway of PAEs and offer theoretical guidance for the development of enzyme-based strategies for environmental pollutant remediation.
作者
王丹
朱若斐
WANG Dan;ZHU Ruofei(College of Textiles&Clothing,Xinjiang University,Urumqi,830017,China;Key Laboratory for Smart&Green Textiles of Xinjiang,Urumqi,830017,China)
出处
《环境化学》
2025年第8期3073-3081,共9页
Environmental Chemistry
基金
新疆维吾尔自治区自然科学基金青年基金(2024D01C213,2024D01C214)
新疆大学博士启动基金(620323015,620323016)
新疆维吾尔自治区高校基本科研业务(XJEDU2024P028)资助.
作者简介
通信联系人:朱若斐,E-mail:ruofeizhu@xju.edu.cn。
