N-羟基邻苯二甲酰亚胺与负载型铁氧化物催化氧化环己烷研究  

Catalytic oxidation of cyclohexane with N-hydroxyphthalimide/supported iron oxides and its mechanism

作　　者：张延路[1,2] 赵文军[1] 杨丹红[1,2] 陈勇[1,2] 高林[1] 

机构地区：[1]中国科学院新疆理化技术研究所,新疆乌鲁木齐830011 [2]中国科学院研究生院,北京100049

出　　处：《工业催化》2009年第2期55-59,共5页Industrial Catalysis

摘　　要：考察了N-羟基邻苯二甲酰亚胺与负载型铁氧化物相组合时催化氧化环已烷的效果以及可能存在的机理。用浸渍法制备了多种负载型铁氧化物催化剂,研究了用不同载体和不同铁来源制备的催化剂与N-羟基邻苯二甲酰亚胺共同催化氧化环己烷,比普通的三价铁盐与N-羟基邻苯二甲酰亚胺相组合催化氧化环己烷好。N-羟基邻苯二甲酰亚胺与Fe/ZrO_2在100℃和氧压0.6MPa下反应6 h,环己烷转化率可达53%。通过穆斯堡尔谱图等实验手段提供的信息提出可能的催化机理,负载型铁氧化物晶体缺陷产生的Fe^(4+)是激发N-羟基邻苯二甲酰亚胺为PINO自由基的来源。N-hydroxyphthalimide（NHPI） and supported ic oxidation of cyclohexane and the catalytic effects and iron oxides were used as the catalysts for catalytpossible mechanisms were investigated. Different kinds of supported iron oxides containing different supports and iron precursors were prepared, which, when combined with N-hydroxyphthalimide, had catalytic properties superior to those of conventional Fe （ Ⅲ ） salts/N-hydroxyphthalimide. Cyclohexane conversion of 53% was obtained over N-hydroxyphthalimide/Fe/ZrO2 under 100 ℃, O2 pressure of 0. 6 MPa and reaction time of 6 h. Mossbauer spectra showed that Fe^4＋ generated from the crystal defects was the PINO radical initiator.

关 键 词：催化化学 环己烷 N-羟基邻苯二甲酰亚胺 负载铁氧化物 穆斯堡尔谱 超交换相互作用 晶体缺陷 

分 类 号：O643.31[理学—物理化学] O624.1[理学—化学]