高活性Au/SnO2催化剂的制备及其在1,4-丁二醇氧化制γ-丁内酯反应中的催化应用

doi:10.1016/S1872-2067(12)60534-8

催化学报 ›› 2013, Vol. 34 ›› Issue (5): 1013-1019.DOI: 10.1016/S1872-2067(12)60534-8

高活性Au/SnO₂催化剂的制备及其在1,4-丁二醇氧化制γ-丁内酯反应中的催化应用

李娴^a, 郑嘉旻^a, 杨新丽^b, 戴维林^a, 范康年^a

a 复旦大学化学系, 上海市分子催化和功能材料重点实验室, 上海 200433;<;
b r>;
b 河南工业大学化学化工学院, 河南郑州 450001

收稿日期:2012-11-26 修回日期:2013-05-20 出版日期:2013-05-06 发布日期:2013-05-06
通讯作者: 戴维林

Preparation and application of highly efficient Au/SnO₂ catalyst in the oxidative lactonization of 1,4-butanediol to γ-butyrolactone

LI Xian^a, ZHENG Jiamin^a, YANG Xinli^b, DAI Weilin^a, FAN Kangnian^a

a Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Department of Chemistry, Fudan University, Shanghai 200433, China;
b College of Chemistry and Chemical Engineering, Henan University of Technology, Zhengzhou 450001, Henan, China

Received:2012-11-26 Revised:2013-05-20 Online:2013-05-06 Published:2013-05-06

摘要/Abstract

摘要：

采用沉积沉淀法制备了一系列商业SnO₂负载的纳米Au催化剂, 通过电感耦合等离子体发射光谱、X射线粉末衍射、透射电镜和X射线光电子能谱等方法研究了溶液酸碱性、沉淀剂种类、Au负载量和焙烧温度等对催化剂性质的影响.结果表明, Au的负载量以及催化剂的焙烧温度对Au颗粒状态有较大影响.其中, 于573 K焙烧的3%Au/SnO₂催化剂在1,4-丁二醇氧化制备γ-丁内酯反应中的催化活性最好, TOF值是Au/TiO₂催化剂的15倍.这主要是由于SnO₂载体独特的性质对所负载的Au颗粒的影响.

null

关键词: 金催化, 二氧化锡, 沉积沉淀法, 1,4-丁二醇, 氧化内酯化, 焙烧温度, 金负载量

Abstract:

A series of gold catalysts supported on commercial SnO₂ were synthesized by deposition-precipitation while accurately controlling pH and precipitant species. The supported catalysts were characterized by X-ray diffraction, inductively coupled plasma atomic emission spectrometry, transmission electron microscopy, and X-ray photoelectron spectroscopy. Gold loading and calcination temperature both affected the dispersion and nature of gold species on SnO₂. The performance of the catalysts in the oxidative lactonization of 1,4-butanediol to g-butyrolactone was investigated. The catalyst with 3% gold that was calcined at 573 K exhibited the highest activity, which was 15 times higher than that of Au/TiO₂. The excellent catalytic performance was attributed to the high dispersion of gold particles and adequate Au⁰ and Au^δ^- species formed because of the strong interaction between Au and SnO₂ and the intrinsic properties of SnO₂.

Key words: Gold catalyst, Tin dioxide, Deposition-precipitation method, 1,4-Butanediol, Oxidative lactonization, Calcination temperature, Gold loading

李娴, 郑嘉旻, 杨新丽, 戴维林, 范康年. 高活性Au/SnO₂催化剂的制备及其在1,4-丁二醇氧化制γ-丁内酯反应中的催化应用[J]. 催化学报, 2013, 34(5): 1013-1019.

LI Xian, ZHENG Jiamin, YANG Xinli, DAI Weilin, FAN Kangnian. Preparation and application of highly efficient Au/SnO₂ catalyst in the oxidative lactonization of 1,4-butanediol to γ-butyrolactone[J]. Chinese Journal of Catalysis, 2013, 34(5): 1013-1019.

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高活性Au/SnO₂催化剂的制备及其在1,4-丁二醇氧化制γ-丁内酯反应中的催化应用

Preparation and application of highly efficient Au/SnO₂ catalyst in the oxidative lactonization of 1,4-butanediol to γ-butyrolactone

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