催化臭氧氧化降解邻苯二甲酸二甲酯中催化剂构效关系  

Relationship between the structure and activity of ruthenium catalysts in the catalytic ozonation of dimethyl phthalate

作　　者：王建兵[1] 王灿[1] 杨春丽[1] 王国庆[1] 祝万鹏[2] 

机构地区：[1]中国矿业大学(北京)化学与环境工程学院,北京100083 [2]清华大学环境学院,北京100084

出　　处：《催化学报》2013年第2期313-321,共9页

基　　金：国家自然科学基金(20907072)~~

摘　　要：采用传统焙烧和微波辐射制备了不同活性炭(AC)负载Ru催化剂,并用于催化臭氧氧化降解邻苯二甲酸二甲酯(DMP)反应中,探讨了催化剂的构效关系.结果表明,所有AC和催化剂均能提高臭氧氧化DMP过程中TOC(总有机碳)去除率,其活性顺序为Ru/coal-AC>nutshell-AC>Ru/nutshell-AC>Ru/coconut-AC≈coal-AC>coconut-AC.负载的Ru颗粒扩散到AC大孔中,增加了反应的传质阻力,使得反应物与AC内表面的活性位和金属Ru的接触机会减少,这是Ru/nutshell-AC和Ru/coconut-AC活性低于Ru/coal-AC的一个原因;催化剂表面Ru分散度也是导致其活性差别的原因之一.微波加热引起nutshell-AC表面活性官能团发生变化,从而导致其负载的Ru催化活性降低.相对于传统焙烧,微波辐射热处理能够提高coal-AC表面Ru的分散度,从而提高催化剂活性.Ruthenium catalysts on various activated carbon (AC) supports were prepared using conventional calcination and microwave irradiation. Their activity in the catalytic ozonation of dimethyl phthalate was studied. The relationship between the structure and activity was investigated. All the supports and catalysts increased total organic carbon removal. The activity order wasRu/coal-AC > nutshell-AC > Ru/nutshell-AC > Ru/coconut-AC ≈coal-AC > coconut-AC. The supported Ruparticles diffused into the macropores, which increased mass transfer resistance in catalytic ozonation and decreased the probability that the reactants can contact the active phase on the interior surface. This was one reason why the activity of nutshell-AC and Ru/nutshell-AC was lower than that of Ru/coal-AC. A difference in Ru dispersion on the surface of the catalyst also caused the activity difference. The active phase on the surface of nutshell-AC can be changed by microwave irradiation, which caused Ru/nutshell-AC to even be less active than the corresponding support. As compared to the use of conventional calcination, the use of microwave irradiation enhanced the metal dispersion and catalytic activity of Ru/coal-AC.

关 键 词：催化臭氧氧化 邻苯二甲酸二甲酯 钌 活性炭 

分 类 号：O643.32[理学—物理化学]