一种席夫碱铜配合物催化过氧化氢氧化降解三氯生  

Oxidative removal of triclosan with hydrogen peroxide catalyzed by a Schiff base Cu(Ⅱ)-complex

作　　者：彭建彪 张耀宗 张亚 陈敏 张慧 李静华 刘海津 高士祥[2] PENG Jianbiao;ZHANG Yaozong;ZHANG Ya;CHEN Min;ZHANG Hui;LI Jinghua;LIU Haijin;GAO Shixiang(Henan Key Laboratory for Environmental Pollution Control, Key Laboratory for Yellow River and Huai River Water Environment and Pollution Control, Ministry of Education, School of Environment, Henan Normal University. Xinxiang, 453007 , China;State Key Laboratory of Pollution Control and Resource Reuse, School of the Environment, Nanjing University, Nanjing, 210023 , China;Nanjing Institute of Environmental Sciences, Ministry of Ecology and Environment of the People s Republic of China, Nanjing, 210042, China)

机构地区：[1]河南师范大学环境学院,黄淮水环境污染与防治教育部重点实验室,河南省环境污染控制重点实验室,新乡453007 [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 [3]生态环境部南京环境科学研究所,南京210042

出　　处：《环境化学》2019年第5期977-984,共8页Environmental Chemistry

基　　金：中国博士后科学基金(2018M632783);河南师范大学科学基金(5101219170124,5101219170307,5101219470210);国家自然科学基金(21577059,41807129);中央级公益性科研院所基本科研业务专项(GYZX180210);污染控制与资源化研究国家重点实验室开放基金(PCRRF18028)资助~~

摘　　要：利用溶液法,合成了5-硝基水杨醛缩N-苯基邻苯二胺席夫碱及其铜配合物,通过元素分析、紫外可见吸收光谱、红外吸收光谱和X射线电子能谱等技术进行了结构表征和确认.考察了不同条件下该配合物催化过氧化氢氧化降解三氯生的反应,结果表明该配合物能迅速催化过氧化氢氧化降解三氯生.催化反应速度与配合物的用量、过氧化氢的用量和反应温度等因素有关,在起始三氯生浓度0.02 mmol·L^-1,铜配合物0.05 mmol·L^-1,过氧化氢1.0 mmol·L^-1,pH=7.6,反应温度50℃,反应时间为30 min条件下,三氯生的去除率高达80.5%.通过反应过程中反应活性物质的测定,发现降解过程主要涉及羟基自由基的氧化机理.综上结果表明,席夫碱金属配合物可以作为催化剂催化过氧化氢在近中性条件下氧化降解水中三氯生.A Schiff base from the condensation of 5-nitrosalicylaldehyde with N-phenyl-o-phenylenediamine and its Cu(Ⅱ)-complex were synthesized by solution method. The structure and chemical composition of the Schiff base and its Cu(Ⅱ)-complex were characterized with various techniques including elemental analysis(EA), UV-Vis absorption spectroscopy(UV), Fourier-transform infrared spectroscopy(FT-IR), and X-ray photoelectron spectroscopy(XPS). Catalytic degradation of triclosan(TCS) by hydrogen peroxide in the presence of the Cu(Ⅱ)-complex was evaluated under various conditions. The results revealed that the Cu(Ⅱ)-complex showed good catalytic performance on the degradation of TCS. The TCS removal efficiency increased with the increase of Cu(Ⅱ)-complex concentration, H2O2 concentration, and reaction temperature. At optimal reaction conditions of 0.05 mmol·L^-1 Cu(Ⅱ)-complex0, 1.0 mmol·L^-1 H2O2, 0.02 mmol·L^-1 TCS, pH 7.6, and at temperature 50 ℃, TCS was removed by 80.5% within 30 min. The dominant reactive oxygen species(ROS) involved in the reaction was identified as ·OH radical using 2-propanol, sodium azide, and nitro blue tetrazolium as scavengers for ·OH, 1O2 and O2^-, respectively. The results suggested that the Cu(Ⅱ)-complex is a promising catalyst for catalyzing oxidative degradation of TCS by H2O2 in aqueous solution under neutral condition.

关 键 词：5-硝基水杨醛缩N-苯基邻苯二胺席夫碱 过氧化氢 铜配合物 三氯生 

分 类 号：X505[环境科学与工程—环境工程]