一个物理化学综合实验设计
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摘要
设计了一个双核铜配合物合成及其催化性能研究的综合实验。合成了N,N'-双(N-羟乙基乙二胺基)草酰胺合二铜,并研究了铜配合物作为模拟过氧化物酶催化氧化过氧化氢降解苯酚的反应。利用紫外-可见分光光度计检测反应过程中苯酚浓度的变化,建立了准一级反应动力学模型。综合实验有利于提高学生的综合操作能力和应用能力,增强了学生的创新能力和团队协作意识。
A comprehensive experiment,the synthesis and catalytic properties of a dinuclear copper complex,was designed. The dinuclear copper complex,Cu2( oxheel),was synthesized and employed as mimetic peroxidase to catalyze the oxidation of phenol with hydrogen peroxide. The concentration of phenol during the reaction was detected by using UV-visible spectrophotometer. A pseudo first order reaction kinetic mathematic model was constructed. Comprehensive experiment is conducive to improve students' comprehensive operational ability and application ability,and enhance the students' innovative ability and team collaboration consciousness.
A comprehensive experiment,the synthesis and catalytic properties of a dinuclear copper complex,was designed. The dinuclear copper complex,Cu2( oxheel),was synthesized and employed as mimetic peroxidase to catalyze the oxidation of phenol with hydrogen peroxide. The concentration of phenol during the reaction was detected by using UV-visible spectrophotometer. A pseudo first order reaction kinetic mathematic model was constructed. Comprehensive experiment is conducive to improve students' comprehensive operational ability and application ability,and enhance the students' innovative ability and team collaboration consciousness.
引文
[1]欧丽娟,孙爱明,刘开建.一个分析化学综合实验[J].广州化工,2016,44(8):181-182.
[2]张逢星,李珺,郭慧林.以创新培养为主线构建综合化学实验与科研训练体系[J].大学化学,2009,24(3):18-21.
[3]金燕仙.一个全新的材料化学专业综合设计性实验[J].广东化工,2012,39(5):257-259.
[4]王韬,李鑫钢,杜启云.含酚废水治理技术研究进展[J].化工进展,2008,27(2):231-235.
[5]S Kobayashi,H Higashimura.Oxidative polymerization of phenols revisited[J].Prog Polym Sci,2003,28:1015-1048.
[6]D López-Molina,ANP Hiner,J Tudela.Enzymatic removal of phenols from aqueous solution by artichoke(Cynara scolymus L)extracts[J].Enzyme and Microbial Technology,2003,33(5):738-742.
[7]褚衍洋,邓肖丽,王蒙.钛基氧化物阳极氧化降解水中2,4-二氯酚[J].环境科学学报,2010,30(7):1425-1430.
[8]MENG Xiang Guang,ZHU Jie,YAN Jie,et al.Studies on the oxidation of phenols catalyzed by a copper(Ⅱ)-Schiff base complex inaqueous solution under mild conditions[J].Journal of Chemical Technology and Biotechnology,2006,81:2-7.
[9]A Santos,P Yustos,A Quintanilla,et al.Route of the catalytic oxidation of phenol in aqueous phase[J].Appl Catal B(Environ),2002,39:97-113.
[10]JF Akyurtlu,A Akyurtlu,S Kovenklioglu.Catalytic oxidation of phenol in aqueous solutions[J].Catal Today,1998,40:343-352.
[11]宋继梅,张小霞,焦剑,等.三氧化钨纳米片的制备及其光催化性质研究[J].安徽大学学报(自然科学版),2009,33(03):73-77.
[12]HE Zhiqiao,XIE Lei,TU Jinjun.Visible Light-Induced Degradation of Phenol over Iodine-Doped Titanium Dioxide Modied with Platinum:Role of Platinum and the Reaction Mechanism[J].Phys.Chem.C,2010,114:526-532.
[13]ZENG Jian,LIU Shilin,CAI Jie,et al.Ti O2Immobilized in Cellulose Matrix for Photocatalytic Degradation of Phenol under Weak UV Light Irradiation[J].Phys.Chem.C,2010,114:7806-7811.
[14]C Comninellis,A Nerini.Anodic-oxidation of phenol in the presence of Na Cl for waster-water treatment[J].Appl Electrochem,1995,25:23-28.
[15]JL Boudenne,O Cerclier,J Galéa,et al.Electrochemical oxidation of aqueous phenol at a carbonblack slurry electrode[J].Appl Catal A(General),1996,143:185-202.
[16]TD Thornton,PE Savage.Kinetics of phenol oxidation in supercritical water[J].AICh E,1992,38(3):321-327.
[17]X Zhang,PE Savage.Fast catalytic oxidation of phenol in supercritical water[J].Catal Today,1998,40:333-342.
[18]S Gopalan,PE Savage.A reaction network model for phenol oxidation in supercritical water[J].AICh E,1995,41(8):1864-1873.
[19]AM Gizir,AA Clifford,KD Bartle.The catalytic role of transition metal salts on supercritical water oxidation of phenol and chlorophenols in a titanium reactor[J].React Kinet Catal Lett,2003,78(1):175-182.
[20]谢斌,王莹,李志成,等.N,N'-(N-羟乙基乙二胺基)草酰胺合二铜催化过氧化氢氧化对苯二酚的动力学研究[J].四川大学学报(自然科学版),2006,43(2):403-410.
[21]XIE Jiaqing,LI Jianzhang,MENG Xiangguang,et al.A kinetic study of phenolic oxidation by H2O2using the Schiff base complexes as mimetic peroxidases[J].Transition Metal Chemistry,2004,29:388-393.
[22]IU Castro,DC Sherrington,A Fortuny,et al.Synthesis of polymersupported copper complexes and their evaluation in catalytic phenol oxidation[J].Catalysis Today,2010,157:66-70.
[23]WC Ellis,CT Tran,MA Denardo,et al.Design of More Powerful Iron-TAML Peroxidase Enzyme Mimics[J].J.AM.CHEM.SOC,2009,131:18052-18053.
[2]张逢星,李珺,郭慧林.以创新培养为主线构建综合化学实验与科研训练体系[J].大学化学,2009,24(3):18-21.
[3]金燕仙.一个全新的材料化学专业综合设计性实验[J].广东化工,2012,39(5):257-259.
[4]王韬,李鑫钢,杜启云.含酚废水治理技术研究进展[J].化工进展,2008,27(2):231-235.
[5]S Kobayashi,H Higashimura.Oxidative polymerization of phenols revisited[J].Prog Polym Sci,2003,28:1015-1048.
[6]D López-Molina,ANP Hiner,J Tudela.Enzymatic removal of phenols from aqueous solution by artichoke(Cynara scolymus L)extracts[J].Enzyme and Microbial Technology,2003,33(5):738-742.
[7]褚衍洋,邓肖丽,王蒙.钛基氧化物阳极氧化降解水中2,4-二氯酚[J].环境科学学报,2010,30(7):1425-1430.
[8]MENG Xiang Guang,ZHU Jie,YAN Jie,et al.Studies on the oxidation of phenols catalyzed by a copper(Ⅱ)-Schiff base complex inaqueous solution under mild conditions[J].Journal of Chemical Technology and Biotechnology,2006,81:2-7.
[9]A Santos,P Yustos,A Quintanilla,et al.Route of the catalytic oxidation of phenol in aqueous phase[J].Appl Catal B(Environ),2002,39:97-113.
[10]JF Akyurtlu,A Akyurtlu,S Kovenklioglu.Catalytic oxidation of phenol in aqueous solutions[J].Catal Today,1998,40:343-352.
[11]宋继梅,张小霞,焦剑,等.三氧化钨纳米片的制备及其光催化性质研究[J].安徽大学学报(自然科学版),2009,33(03):73-77.
[12]HE Zhiqiao,XIE Lei,TU Jinjun.Visible Light-Induced Degradation of Phenol over Iodine-Doped Titanium Dioxide Modied with Platinum:Role of Platinum and the Reaction Mechanism[J].Phys.Chem.C,2010,114:526-532.
[13]ZENG Jian,LIU Shilin,CAI Jie,et al.Ti O2Immobilized in Cellulose Matrix for Photocatalytic Degradation of Phenol under Weak UV Light Irradiation[J].Phys.Chem.C,2010,114:7806-7811.
[14]C Comninellis,A Nerini.Anodic-oxidation of phenol in the presence of Na Cl for waster-water treatment[J].Appl Electrochem,1995,25:23-28.
[15]JL Boudenne,O Cerclier,J Galéa,et al.Electrochemical oxidation of aqueous phenol at a carbonblack slurry electrode[J].Appl Catal A(General),1996,143:185-202.
[16]TD Thornton,PE Savage.Kinetics of phenol oxidation in supercritical water[J].AICh E,1992,38(3):321-327.
[17]X Zhang,PE Savage.Fast catalytic oxidation of phenol in supercritical water[J].Catal Today,1998,40:333-342.
[18]S Gopalan,PE Savage.A reaction network model for phenol oxidation in supercritical water[J].AICh E,1995,41(8):1864-1873.
[19]AM Gizir,AA Clifford,KD Bartle.The catalytic role of transition metal salts on supercritical water oxidation of phenol and chlorophenols in a titanium reactor[J].React Kinet Catal Lett,2003,78(1):175-182.
[20]谢斌,王莹,李志成,等.N,N'-(N-羟乙基乙二胺基)草酰胺合二铜催化过氧化氢氧化对苯二酚的动力学研究[J].四川大学学报(自然科学版),2006,43(2):403-410.
[21]XIE Jiaqing,LI Jianzhang,MENG Xiangguang,et al.A kinetic study of phenolic oxidation by H2O2using the Schiff base complexes as mimetic peroxidases[J].Transition Metal Chemistry,2004,29:388-393.
[22]IU Castro,DC Sherrington,A Fortuny,et al.Synthesis of polymersupported copper complexes and their evaluation in catalytic phenol oxidation[J].Catalysis Today,2010,157:66-70.
[23]WC Ellis,CT Tran,MA Denardo,et al.Design of More Powerful Iron-TAML Peroxidase Enzyme Mimics[J].J.AM.CHEM.SOC,2009,131:18052-18053.