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单双核铜配合物催化H2O2氧化3,4-二甲氧基苯乙酮动力学研究

发表时间:2013-04-15  浏览量:1313  下载量:326
全部作者: 李晓丽,崔刚,唐少坚,彭雨,孟祥光
作者单位: 四川大学化学学院
摘 要: 制备了2种单核金属铜配合物和一种双核金属铜配合物。系统地研究了水溶液中3种铜配合物催化氧化木质素模型底物3,4-二甲氧基苯乙酮的反应动力学,计算了反应速率常数。研究表明,单核铜配合物只在较高温度下对H2O2氧化3,4-二甲氧基苯乙酮表现出了好的催化活性,而双核铜配合物则表现了在常温下很好的催化能力。研究还发现,这些铜配合物的催化活性与反应体系的pH值有关,在研究的pH值范围内随pH值的增大而增加。提出的催化反应机理合理地解释了铜配合物催化活性的pH值效应。催化剂的碱式氧化物种被认为是催化体系的有效氧化物种。
关 键 词: 物理化学;催化氧化;木质素;3,4-二甲氧基苯乙酮;过氧化氢;动力学
Title: Oxidation kinetics of 1-(3,4-dimethoxyphenyl)ethanone by H2O2 with catalyzation of mononucleonic and binucleonic copper complexes
Author: LI Xiaoli, CUI Gang, TANG Shaojian, PENG Yu, MENG Xiangguang
Organization: College of Chemistry, Sichuan University
Abstract: Two mononucleonic copper complexes and one binucleonic copper complex were prepared. The oxidation kinetics of 1-(3,4-dimethoxyphenyl)ethanone catalyzed by three coper complexes in water solution were investigated, and the reaction rate constants were also obtained. The results showed that the mononucleonic complexes displayed good catalytic activity for 1-(3,4-dimethoxyphenyl)ethanone oxidation by H2O2 only at relatively high temperature, while the binucleoniccomplex could display good catalytic ability at ambient temperature. Furthermore, the catalytic activity of the complexes were correlated with pH of reaction solution, and it increased with increasing pH value within the experimental pH range. In addition, the proposed catalytic reaction mechanism explained the pH effect on catalytic activity of copper complexes. Therefore, the alkaline oxidative form of catalyst was belived as the real active species.
Key words: physical chemistry; catalytic oxidation; lignin; 1-(3,4-dimethoxyphenyl)ethanone; hydrogen peroxide; kinetics
发表期数: 2013年4月第7期
引用格式: 李晓丽,崔刚,唐少坚,等. 单双核铜配合物催化H2O2氧化3,4-二甲氧基苯乙酮动力学研究[J]. 中国科技论文在线精品论文,2013,6(7):667-672.
 
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