Cu(Ⅱ)-席夫碱配合物的合成及其催化活性  

Synthesis of Cu(Ⅱ)-Schiff base complex and its catalytic activity evaluation in aqueous solution

作　　者：彭建彪 顾梦瑶 卞伟 贺冰冰 张耀宗 张超男 孙芊芊 刘海津 高士祥[3] Peng Jianbiao;Gu Mengyao;Bian Wei;He Bingbing;Zhang Yaozong;Zhang Chaonan;Sun Qianqian;Liu Haijin;Gao Shixiang(School of Environment,Key Laboratory for Yellow River and Huai River Water Environment and Pollution Control,Ministry of Education,Henan Key Laboratory for Environmental Pollution Control,Henan Normal University,Xinxiang 453007,China;China Energy Investment Group CO.,LTD.,Beijing 100011,China;School of the Environment,State Key Laboratory of Pollution Control and Resource Reuse,Nanjing University,Nanjing 210023,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,河南新乡453007 [2]国家能源投资集团有限责任公司,北京100011 [3]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：《河南师范大学学报（自然科学版）》2021年第1期57-63,共7页Journal of Henan Normal University(Natural Science Edition)

基　　金：中国博士后科学基金(2018M632783,2019M660589);河南师范大学博士启动基金(5101219170124);河南师范大学博士后科研经费(5101219470210);河南师范大学青年科学基金(5101219170307);河南师范大学大学生创新训练项目(20190132);污染控制与资源化研究国家重点实验室开放基金(PCRRF18028).

摘　　要：在乙醇溶剂中,3,5-二溴水杨醛为母体,与乙醇胺反应合成了席夫碱,随后与铜离子进一步反应生成铜配合物,用元素分析、紫外光谱、红外光谱和X射线光电子能谱等手段来表征其结构和组成,用液相色谱-高分辨飞行时间-质谱联用仪测定了席夫碱的分子量.以铜配合物为催化剂在水相近中性条件下催化H_(2)O_(2)氧化酚类污染物,以苯酚为底物探讨了溶液pH、H_(2)O_(2)用量、反应温度和反应时间等因素对氧化反应的影响.结果表明,在酚类浓度为1.00mmol/L,铜配合物浓度为0.05mmol/L,H_(2)O_(2)浓度为30mmol/L,pH7.6,50℃,5h等条件下,2,4-二氯酚的去除率最大,达84.8%(矿化率7.8%),五氯酚的去除率最小,为29.1%(无矿化).淬灭实验结果表明羟基自由基是该反应体系中的主要活性氧物质.A Schiff base was synthesized from the reaction between 3,5-dibromosalicylaldehyde and ethanolamine;then its Cu^(2+)-complex was prepared from the reaction between the Schiff base and copper ion.Their structure and chemical composition were characterized by elemental analysis(EA),ultraviolet spectroscopy(UV),Fourier-transform infrared spectro-scopy(FT-IR),and X-ray photoelectron spectroscopy(XPS).The molecular weight of the Schiff base was confirmed by the high resolution liquid chromatograph-time of flight-mass spectrometry(LC-TOF-MS).Catalytic oxidation of phenols by the Cu^(2+)-complex activated hydrogen peroxide(H_(2)O_(2))was evaluated at neutral conditions.To optimize the reaction condition,effects of solution pH,H_(2)O_(2) concentration,reaction temperature,and reaction time were investigated by using phenol as the model contaminant.Under the optimal reaction condition of[Phenols]0=1.00 mmol/L,[Cu^(2+)-complex]0=0.05 mmol/L,[H_(2)O_(2)]0=30 mmol/L,pH 7.6,and 50℃,the removal of PCP was the lowest 29.1%(TOC removal=0),and that of 2.4-DCP was the highest 84.8%(TOC removal=7.8%)within 5 h.Radical quenching experiment results showed that hydroxyl radical(·OH)was the dominant reactive oxygen species(ROS)in the reaction system.

关 键 词：3 5-二溴水杨醛 铜配合物 H_(2)O_(2) 酚类污染物 

分 类 号：O413[理学—理论物理]