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通过醇还原法合成的用于肉桂醛加氢的高活性负载型铂纳米催化剂:金属价态与羟基的协同作用

Highly Active Supported Pt Nanocatalysts Synthesized by Alcohol Reduction towards Hydrogenation of Cinnamaldehyde: Synergy of Metal Valence and Hydroxyl Groups.

作者信息

Wang Yanyan, He Wanhong, Wang Liren, Yang Junjiao, Xiang Xu, Zhang Bing, Li Feng

机构信息

State Key Laboratory of Chemical Resource Engineering, Beijing University of Chemical Technology, Beijing, 100029, PR China.

School of Chemical Engineering, Zhengzhou University, Zhengzhou, 450001, PR China.

出版信息

Chem Asian J. 2015 Jul;10(7):1561-70. doi: 10.1002/asia.201500188. Epub 2015 May 12.

Abstract

The hydrogenation of α,β-unsaturated aldehydes to allylic alcohols or saturated aldehydes provides a typical example to study the catalytic effect on structure-sensitive reactions. In this work, supported platinum nanocatalysts over hydrotalcite were synthesized by an alcohol reduction method. The Pt catalyst prepared by the reduction with a polyol (ethylene glycol) outperforms those prepared with ethanol and methanol in the hydrogenation of cinnamaldehyde. The selectivity towards the C=O bond is the highest over the former, although its mean size of Pt particles is the smallest. The hydroxyl groups on hydrotalcite could act as an internally accessible promoter to enhance the selectivity towards the C=O bond. The optimal Pt catalyst showed a high activity with an initial turnover frequency (TOF) of 2.314 s(-1). This work unveils the synergic effect of metal valence and in situ promoter on the chemoselective hydrogenation, which could open up a new direction in designing hydrogenation catalysts.

摘要

将α,β-不饱和醛氢化为烯丙醇或饱和醛为研究对结构敏感反应的催化作用提供了一个典型例子。在本工作中,采用醇还原法合成了水滑石负载的铂纳米催化剂。用多元醇(乙二醇)还原制备的铂催化剂在肉桂醛氢化反应中比用乙醇和甲醇制备的催化剂表现更优。尽管其铂颗粒平均尺寸最小,但对C=O键的选择性在前者上最高。水滑石上的羟基可作为内部可及的促进剂来提高对C=O键的选择性。最优铂催化剂表现出高活性,初始周转频率(TOF)为2.314 s(-1)。本工作揭示了金属价态和原位促进剂对化学选择性氢化的协同作用,这可为设计氢化催化剂开辟新方向。

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