以聚酰胺—胺为模板剂一些无机功能材料的制备及催化性能研究
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摘要
聚酰胺-胺型(PAMAM)树枝状大分子是一类新型纳米级大分子化合物，其分子大小约1～10nm，高度枝化而呈树枝状，分子外面携带大量活性的官能团，在材料、医学、催化等许多领域特别是无机功能材料的合成方面有实际应用价值，成为相关领域的研究热点之一。同时，由于能够在分子水平上对分子的大小、形状，以及表面官能团进行严格地控制与设计，极大地推动了分子设计理论向前发展。
本论文以PAMAM树枝状大分子为模板剂，研究一些无机功能材料的制备及催化性能。
采用树状聚酰胺-胺(PAMAM)大分子化合物与同多酸阴离子[Mo_6O_(19)]~(2-)，基于静电组装得到新颖的同多金属氧酸盐／树型分子超分子化合物。用元素分析、FTIR、UV-Vis、TG／DTA、荧光光谱等测试技术分别对样品进行了结构表征及性能测试。并利用其作为电极修饰剂，制得化学体修饰的碳糊电极(CMCPE)，用循环伏安法研究了同多金属氧酸盐／树型分子超分子化合物修饰碳糊电极的电化学行为和电催化性能。
以3.5代端酯基PAMAM树型分子为模板，制备了颗粒均匀的纳米氧化锌，采用TEM、XRD及UV-Vis等手段对合成样品的形貌和结构进行表征，初步探讨了纳米ZnO形成的可能模板机理，并研究了其在紫外光作用下光催化降解罗丹明B的性能。
以聚酰胺-胺(PAMAM)树形分子为模板，制备了颗粒细、分散性好的ZnO-SnO_2纳米复合氧化物，采用XRD、DRS、EDS、TEM等手段对合成样品的形貌和结构进行了表征，测试其在可见光作用下光催化降解罗丹明B的性能，讨论了罗丹明B溶液的初始浓度、ZnO-SnO_2纳米复合氧化物的用量、ZnO-SnO_2纳米复合氧化物合成过程中的焙烧时间以及焙烧温度对降解罗丹明B光催化活性的影响，并探讨了PAMAM树形分子的代数、浓度对合成复合氧化物颗粒形貌及光催化性能的影响。
Dendritic polymer, a class of new macromolecule, appeared in the middle of eighty years of twenty centuries. Dendrimers have a hyper-branched, well defined and monodisperse structures and can be formed by reiterative reaction sequences starting from smaller molecules named "initiator core". And its molecular weight, size, shape and functional group over surface can be controlled by the reactions and synthetic building blocks used. Great attention has been paid to dendrimers, especially poly(amidoamine) dendrimers, in a number of potential applications in supramobecular chemistry, nanosciences, biology, medicine, catalysis and so on.
A novel supramolecular compound [Mo_6O_(19)]~(2-)/PAMAM assembled by ionic bonding was synthesized by Poly(amide amine)dendrimer(PAMAM) and [Mo_6P_(19)]~(2-) polyanion, and characterized by element analysis, FTIR, UV-Vis absorption, TG/DTA, Fluorescence spectrum. Electrochemical behavior and electrocatalytic activity of the carbon paste electrode(CPE) modified by the title compound was studied in H_2SO_4 aqueous solution.
ZnO nanoparticles were prepared in the presence of generation 3.5 poly (amidoamine) with surface ester groups (G3.5-COOCH_3 PAMAM dendrimer) and characterized by TEM, XRD, UV-Vis. The forming mechanism of ZnO nanoparticles was discussed. The degradation of methyl Rhodamine B in aqueous solution was also investigated using ZnO nanoparticles as photochemical catalyst under UV irradiation.
ZnO-SnO_2 nanocomposite oxides with Zn/Sn molar ratio of 2 were prepared in the presence of poly (amidoamine) dendrimer and characterized by XRD, DRS, EDS, TEM. The degradation of methyl Rhodamine B in aqueous solution was investigated using ZnO-SnO_2 nanocomposite oxides as photochemical catalyst under visible light irradiation. Effect of initial concentration of Rhodamine B, amount of catalyst, calcining time,calcining temperature, template concentration and tempate generation on decolour rate were also studied.
本论文以PAMAM树枝状大分子为模板剂，研究一些无机功能材料的制备及催化性能。
采用树状聚酰胺-胺(PAMAM)大分子化合物与同多酸阴离子[Mo_6O_(19)]~(2-)，基于静电组装得到新颖的同多金属氧酸盐／树型分子超分子化合物。用元素分析、FTIR、UV-Vis、TG／DTA、荧光光谱等测试技术分别对样品进行了结构表征及性能测试。并利用其作为电极修饰剂，制得化学体修饰的碳糊电极(CMCPE)，用循环伏安法研究了同多金属氧酸盐／树型分子超分子化合物修饰碳糊电极的电化学行为和电催化性能。
以3.5代端酯基PAMAM树型分子为模板，制备了颗粒均匀的纳米氧化锌，采用TEM、XRD及UV-Vis等手段对合成样品的形貌和结构进行表征，初步探讨了纳米ZnO形成的可能模板机理，并研究了其在紫外光作用下光催化降解罗丹明B的性能。
以聚酰胺-胺(PAMAM)树形分子为模板，制备了颗粒细、分散性好的ZnO-SnO_2纳米复合氧化物，采用XRD、DRS、EDS、TEM等手段对合成样品的形貌和结构进行了表征，测试其在可见光作用下光催化降解罗丹明B的性能，讨论了罗丹明B溶液的初始浓度、ZnO-SnO_2纳米复合氧化物的用量、ZnO-SnO_2纳米复合氧化物合成过程中的焙烧时间以及焙烧温度对降解罗丹明B光催化活性的影响，并探讨了PAMAM树形分子的代数、浓度对合成复合氧化物颗粒形貌及光催化性能的影响。
Dendritic polymer, a class of new macromolecule, appeared in the middle of eighty years of twenty centuries. Dendrimers have a hyper-branched, well defined and monodisperse structures and can be formed by reiterative reaction sequences starting from smaller molecules named "initiator core". And its molecular weight, size, shape and functional group over surface can be controlled by the reactions and synthetic building blocks used. Great attention has been paid to dendrimers, especially poly(amidoamine) dendrimers, in a number of potential applications in supramobecular chemistry, nanosciences, biology, medicine, catalysis and so on.
A novel supramolecular compound [Mo_6O_(19)]~(2-)/PAMAM assembled by ionic bonding was synthesized by Poly(amide amine)dendrimer(PAMAM) and [Mo_6P_(19)]~(2-) polyanion, and characterized by element analysis, FTIR, UV-Vis absorption, TG/DTA, Fluorescence spectrum. Electrochemical behavior and electrocatalytic activity of the carbon paste electrode(CPE) modified by the title compound was studied in H_2SO_4 aqueous solution.
ZnO nanoparticles were prepared in the presence of generation 3.5 poly (amidoamine) with surface ester groups (G3.5-COOCH_3 PAMAM dendrimer) and characterized by TEM, XRD, UV-Vis. The forming mechanism of ZnO nanoparticles was discussed. The degradation of methyl Rhodamine B in aqueous solution was also investigated using ZnO nanoparticles as photochemical catalyst under UV irradiation.
ZnO-SnO_2 nanocomposite oxides with Zn/Sn molar ratio of 2 were prepared in the presence of poly (amidoamine) dendrimer and characterized by XRD, DRS, EDS, TEM. The degradation of methyl Rhodamine B in aqueous solution was investigated using ZnO-SnO_2 nanocomposite oxides as photochemical catalyst under visible light irradiation. Effect of initial concentration of Rhodamine B, amount of catalyst, calcining time,calcining temperature, template concentration and tempate generation on decolour rate were also studied.
引文
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