超细钴纳米粒子催化1-己烯低压氢甲酰化反应的原位红外光谱研究(英文)  

In situ FTIR study of low-pressure hydroformylation of 1-hexene catalyzed by ultrafine cobalt nanoparticles

作　　者：王航[1] 蔡志鹏[1] 钟梦琦 姚思宇[1] 寇元[1] 

机构地区：[1]北京大学化学与分子工程学院分子科学国家实验室绿色化学中心,北京100871

出　　处：《催化学报》2013年第4期781-788,共8页

基　　金：supported by the National Natural Science Foundation of China(21176221);the National Basic Research Program of China(973 Program,2011CB201402)~~

摘　　要：利用原位透射红外光谱研究了2.8nm超细钴纳米粒子在2~3MPa合成气(CO:H2=1:1)和100℃条件下催化的1-己烯氢甲酰化反应.结果表明,在反应中出现与Co2(CO)8类似的红外吸收峰(2071,2041和2022cm-1),被证明是不同Co位点端式吸附CO.首次观测到了位于2054cm-1处吸收峰处的物种,可能归属为RCH2CH2COCo.通过此中间物种,产物醛可以在钴催化剂表面经由结合一个氢原子脱除反应而获得.The hydroformylation of 1-hexene in syngas (CO:H2 = 1) under 2–3 MPa at 100 ℃ was catalyzed using 2.8 nm ultrafine cobalt nanoparticles and investigated by in situ Fourier transform infrared spectroscopy (FTIR). A group of bands observed in the in situ FTIR spectra at 2071, 2041, and 2022 cm–1 are assigned to terminal CO adsorptions distributed over different Co sites. A band at 2054 cm–1 is attributed to the intermediate, RCH2CH2 COCo, which has been observed for the first time. Through this intermediate, the catalytic reaction proceeds via the elimination of RCH2CH2 COCo to leave a single H atom on the surface of each 2.8-nm Co nanoparticle.

关 键 词：钴纳米粒子 氢甲酰化反应 原位红外光谱 汞中毒实验 1-己烯 

分 类 号：O643.36[理学—物理化学]