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二氧化硅微球负载钌催化剂的制备及其在苯乙酮不对称氢转移反应中的应用

徐晓宁 曹发海

化工学报2016,Vol.67Issue(6):2340-2348,9.
化工学报2016,Vol.67Issue(6):2340-2348,9.DOI:10.11949/j.issn.0438-1157.20151895

二氧化硅微球负载钌催化剂的制备及其在苯乙酮不对称氢转移反应中的应用

Preparation of mesoporous silica microsphere supported ruthenium catalysts for asymmetric transfer hydrogenation of acetophenone

徐晓宁 1曹发海1

作者信息

  • 1. 华东理工大学大型工业反应器工程教育部工程研究中心,上海 200237
  • 折叠

摘要

Abstract

Supported ruthenium catalyst, complexes of TsDPEN supported with mesoporous silica microspheres of various morphologies and structures, which were synthesized by a simple one-stepin situ polymerization- induced precipitation procedure, were prepared for the asymmetric transfer hydrogenation of acetophenone. The mesoporous structure of silica microspheres were observed by the nitrogen adsorption/desorption isotherms and field emission scanning electron microscopy (FESEM), ruthenium complex well distributed on silica microspheres by transmission electrum microscopy (TEM), and the existence of hydrogen bonds between catalyst and regents by infrared spectrometry (IR). Effect of support structure and reaction conditions such as reaction temperature and time, and reactant concentration on catalytic performances for the asymmetric transfer hydrogenation of acetophenone were investigated. It showed that the interaction between ruthenium complexes with supports of small pore size and high specific surface area promoted the asymmetric transfer hydrogenation and channel stereo-confinement of mesoporous silica microspheres, resulting in significant enhancement of the activity and optical selectivity of the reaction. Under the optimum of 40℃, 16 h and 0.2 mlacetophenone of reaction conditions, the catalyst achieved its highest 64.1% and 93.4% of acetophenone conversion and enantio selectivity ofR-α-phenethyl alcohol for asymmetric transfer hydrogenation of acetophenone, respectively.

关键词

催化剂/载体/聚合诱导沉淀法/二氧化硅/限域效应

Key words

catalyst/support/polymerization-induced colloid aggregation procedure/silica/channel stereo- confinement

分类

化学化工

引用本文复制引用

徐晓宁,曹发海..二氧化硅微球负载钌催化剂的制备及其在苯乙酮不对称氢转移反应中的应用[J].化工学报,2016,67(6):2340-2348,9.

化工学报

OA北大核心CSCDCSTPCD

0438-1157

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