紫外/二氯异氰尿酸盐体系对水中抗病毒药物降解路径及降解产物毒性分析  

Analysis of degradation pathways and toxicity of degradation products of antiviral drugs in water by UV/Dichloroisocyanurate process

作　　者：黄鹏程 许泽平 郭雨欣 王菲凤[1,2,3] 蔡开聪 孙启元[1,2,3] HUANG Pengcheng;XU Zeping;GUO Yuxin;WANG Feifeng;CAI Kaicong;SUN Qiyuan(College of Environmental and Resource Sciences,College of Carbon Neutral Modern Industry,Fujian Normal University,Fuzhou,350108,China;Fujian Key Laboratory of Pollution Control and Resource Reuse,Fuzhou,350108,China;Research Center of Urban Waste Resource Recycling Technology and Management Engineering in Universities of Fujian Province,Fuzhou,350108,China;College of Chemistry and Materials Science,Fujian Normal University,Fuzhou,350108,China)

机构地区：[1]福建师范大学环境与资源学院、碳中和现代产业学院,福州350108 [2]福建省污染控制与资源循环利用重点实验室,福州350108 [3]福建省高校城市废物资源化技术与管理工程研究中心,福州350108 [4]福建师范大学化学与材料学院,福州350108

出　　处：《环境化学》2024年第6期2058-2068,共11页Environmental Chemistry

基　　金：福建省自然科学基金(2021J06022)资助.

摘　　要：紫外/二氯异氰尿酸盐体系(UV/NaDCC)是一种新兴的高级氧化工艺,通过产生羟基自由基(·OH)和含氯自由基(Cl·,ClO·和Cl_(2)·^(−))等活性物质降解水中持久性有机污染物.莫诺拉韦和巴瑞替尼是用于治疗新冠肺炎等的抗病毒类药物,大量生产和使用导致其通过各环境介质排放进入天然水体,威胁水环境和水质安全.因此,迫切需要探索高效绿色降解莫诺拉韦和巴瑞替尼的新技术.本研究采用密度泛函理论,通过福井函数、简缩双描述符预测了UV/NaDCC体系中莫诺拉韦和巴瑞替尼易发生反应的位点及其降解路径;通过ECOSAR和T.E.S.T程序预测降解产物毒性变化.结果表明,莫诺拉韦中O21、N20及巴瑞替尼中C20、C21更易受到UV/NaDCC产生的含氯自由基和·OH攻击.ECOSAR预测结果显示,部分降解产物表现出比母体物质更高的毒性水平,因此在UV/NaDCC实际应用于抗病毒药物的降解中应关注有毒中间产物的去除.T.E.S.T预测结果表明,多数降解产物生物蓄积性和发育毒性均有所降低.研究成果对UV/NaDCC高级氧化技术对水中抗病毒药物的无害化去除机制和实际应用提供理论依据.UV/Dichloroisocyanurate(UV/NaDCC)process is an emerging advanced oxidation process for degrading persistent organic pollutants in aquatic environments by efficiently generating various reactive species such as hydroxyl radicals(·OH)and reactive chlorine species(including Cl·,ClO·,and Cl_(2)·^(−)).Monoravir and Baricitinib are antiviral drugs used to treat COVID-19 pneumonia,which could be inevitably released into natural water via various environmental media due to their extensive production and usage,and then threaten the aquatic environment and water quality safety.Therefore,it is urgent to develop new technologies for efficiently degrading Monolavir and Baricitinib.In this study,the susceptible reaction sites and degradation pathways of Molnupiravir and Baricitinib were investigated and proposed on the basis of density functional theory,Fukui function,and Condensed dual descriptor,and the toxicity changes of the degradation products were evaluated by ECOSAR and T.E.S.T.programs.The results showed that O21 and N20 in Molnupiravir and C20 and C21 in Baricitinib were more susceptible to attack by RCSs and·OH produced by UV/NaDCC.ECOSAR predictions showed that some degradation products exhibited higher toxicity than their parent substance,so the removal of toxic intermediates should be concerned in the application of UV/NaDCC for the degradation of antiviral medications.T.E.S.T predictions indicated that the Bioconcentration factor and Developmental Toxicity of most degradation products were reduced.The results provide a theoretical basis for the harmless removal mechanism and practical application of UV/NaDCC advanced oxidation technology to antiviral medications in water.

关 键 词：紫外/二氯异氰尿酸盐体系 降解路径 产物毒性 密度泛函理论 莫诺拉韦 巴瑞替尼 

分 类 号：X-1[环境科学与工程] O6[理学—化学]