化学学报 ›› 2013, Vol. 71 ›› Issue (03): 334-338.DOI: 10.6023/A12110977 上一篇    下一篇

研究通讯

包钯纳米颗粒的中空介孔硅铝酸盐纳米球的合成及其在多步催化反应和尺寸选择催化氢化中的应用

刘召辉, 方晓亮, 陈诚, 郑南峰   

  1. 厦门大学化学化工学院 固体表面物理化学国家重点实验室 厦门 361005
  • 投稿日期:2012-11-28 发布日期:2013-01-11
  • 通讯作者: 郑南峰 E-mail:nfzheng@xmu.edu.cn
  • 基金资助:

    项目受到科技部国家纳米重大科学研究计划(No.2011CB932403)、国家自然科学基金(Nos.21131005,21021061,20925103,20923004)和霍英东教育基金会青年教师基金(No.121011)资助.

Pd Nanoparticles Encapsulated in Hollow Mesoporous Aluminosilica Nanospheres as an Efficient Catalyst for Multistep Reactions and Size-Selective Hydrogenation

Liu Zhaohui, Fang Xiaoliang, Chen Cheng, Zheng Nanfeng   

  1. State Key Laboratory for Physical Chemistry of Solid Surfaces and Department of Chemistry, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, China
  • Received:2012-11-28 Published:2013-01-11
  • Supported by:

    Project supported by the Ministry of Science and Technology of China (No. 2011CB932403), the National Natural Science Foundation of China (Nos. 21131005, 21021061, 20925103, 20923004), and the Fok Ying Tung Education Foundation (No. 121011).

最近, 具有中空核壳结构的纳米材料在催化领域中有着深入的研究和广泛的应用. 在本文中, 我们使用一种简单易行的方法合成了一种包裹钯纳米颗粒的中空介孔硅铝酸盐纳米球(简写为Pd@HMAN). 首先, 通过一种先原位合成钯纳米粒子再对其进行二氧化硅包裹的方法, 在Brij56-环己烷-水的反相胶束中合成了具有核壳结构的包裹钯纳米颗粒的二氧化硅纳米球(简写为Pd@SiO2). 然后, 使用CTAB, Na2CO3和NaAlO2试剂, 通过简单的碱性条件下刻蚀Pd@SiO2的过程, 我们成功得到了具有多孔性能的中空核壳型Pd@HMAN纳米催化剂. 由于硅铝酸盐外壳具有酸催化作用, 并且内核钯纳米颗粒又是一种高活性的催化媒介, 因此, 这种复合的多功能纳米催化剂能够很好的应用于多步催化反应中. 此外, 通过一个简单的热处理的方法, 能够缩小硅铝酸盐外壳上的孔道, 我们发现这种孔道调节后的Pd@HMAN纳米催化剂在尺寸选择性氢化反应中有很好的应用前景.

关键词: 反相胶束, 核壳结构, 中空核壳结构, 钯, 多功能纳米催化剂, 尺寸选择性催化, 催化氢化

In this work, yolk-shell structured Pd@hollow mesoporous aluminosilica nanospheres (designated as Pd@HMAN) have been successfully fabricated by a straightforward synthetic route. Core-shell Pd@SiO2 nanospheres were firstly obtained by silica coating of in-situ synthesized Pd nanoparticles in a Brij56-cyclohexane-water reverse micelle system. Simply by alkaline etching of as-prepared Pd@SiO2 core-shell nanospheres in the presence of CTAB, Na2CO3 and NaAlO2, Pd@HMAN particles with high porosity were obtained. As the mesoporous aluminosilica shells can serve as acid catalysts, and the Pd yolks can be applied to catalytic hydrogenation, the as-prepared Pd@HMAN can be used as a stable multifunctional catalyst for multistep reactions. Moreover, due to their adjustable pore parameters, Pd@HMAN after simple thermal treatment can be further applied in the size-selective hydrogenation.

Key words: reverse micelle, core-shell structure, yolk-shell structure, palladium, multifunctional nanocatalyst, size-selective catalysis, hydrogenation