Mn(Ⅲ)TPP-Au/SiO_2复合催化剂催化空气氧化环己烷的性能  

Catalytic Activity of Mn(Ⅲ)TPP-Au/SiO_2 Composite Catalyst for Aerobic Oxidation of Cyclohexane

作　　者：谢娟[1,2] 王延吉[1] 边丽[2] 魏雨[3] 

机构地区：[1]河北工业大学化工学院,天津300130 [2]河北工程大学理学院,河北邯郸056038 [3]河北师范大学化学与材料科学学院,河北石家庄050016

出　　处：《石油学报（石油加工）》2011年第2期207-212,共6页Acta Petrolei Sinica(Petroleum Processing Section)

基　　金：国家自然科学基金重点项目(20636030);科技部重大基础研究前期研究专项项目(2005CCA06100);天津市自然科学基金重点项目(07JCZDJC00100)资助

摘　　要：以包含巯基和吡啶基官能团的巯基吡啶为桥联剂,实现了四苯基锰卟啉(Mn(Ⅲ)TPP)在5%Au/SiO2催化剂上的固载化,合成了新型复合催化剂Mn(Ⅲ)TPP-Au/SiO2。利用傅里叶变换红外光谱、元素分析及X-射线光电子能谱对该催化剂进行表征。以空气氧化环己烷制环己酮和环己醇为探针反应,在不加入任何溶剂或助催化剂的条件下,考察了催化剂用量、反应压力、温度、时间等对Mn(Ⅲ)TPP-Au/SiO2催化性能的影响。结果表明,Mn(Ⅲ)TPP-Au/SiO2复合催化剂与未固载金属卟啉的5%Au/SiO2催化剂相比,在空气氧化环己烷反应中具有更高的催化活性;在最优化反应条件下,环己烷转化率与酮醇总选择性分别为5.39%和88.74%。此外,该催化剂还具有可重复使用的特点。A new type of composite catalyst Mn（Ⅲ）TPP-Au/SiO2 was obtained by immobilizing manganese tetrayphenylporphrin on 5%Au/SiO2 catalyst,with mercaptopyridine as bridging agent,which has sulfhydryl and pyridyl groups.The as-prepared catalyst was characterized by Fourier transform infrared spectroscopy（FT-IR）,elemental analysis（EA）,and X-ray photoelectron spectroscopy（XPS）.The catalytic oxidation of cyclohexane to cyclohexanone（One） and cyclohexanol（Ol） in air was performed as probe reaction without any solvent or promotor,and the influences of the Mn（Ⅲ）TPP-Au/SiO2 amount,reaction pressure,reaction temperature and reaction time on its catalytic performance were investigated.It was found that the activity of Mn（Ⅲ）TPP-Au/SiO2 catalyst was higher than that of pure 5%Au/SiO2 catalyst in the catalytic oxidation of cyclohexane.Under optimum reaction conditions,the conversion of cyclohexane and the total selectivity of cyclohexanone and cyclohexanol were 5.39% and 88.74%,respectively.Furthermore,the catalyst can be used repeatedly.

关 键 词：四苯基锰卟啉 Au/SiO2 空气 氧化 环己烷 

分 类 号：O621[理学—有机化学]