Pd@Cu(II)-MOF-Catalyzed Aerobic Oxidation of Benzylic Alcohols in Air with High Conversion and Selectivity
Pd@Cu(II)-MOF-Catalyzed Aerobic Oxidation of Benzylic Alcohols in Air with High Conversion and Selectivity
复制标题
Pd@Cu(II)-MOF 催化空气中苯甲醇的高转化率和选择性有氧氧化
DOI：
10.1021/acs.inorgchem.5b02973
复制
发表时间：
2016-03-21
影响因子：
4.6
通讯作者：
Dong, Yu-Bin
中科院分区：
文献类型：
--
作者：
Chen, Gong-Jun;Wang, Jing-Si;Dong, Yu-Bin
以吡啶取代双酮配体和Cu（OAc）（2）为原料，在溶液中合成了一种新型的三维多孔Cu（II）-MOF（1），X射线衍射分析表明，该材料具有三维NbO结构.在此基础上，采用溶液浸渍法制备了Pd纳米粒子负载的杂化材料Pd@Cu（II）-MOF（2），并通过高分辨透射电镜（HRTEM）、扫描电镜（SEM）、X射线粉末衍射（XRPD）、气体吸附-脱附、等离子体发射光谱（ICP）等手段对其结构进行了表征。2对空气中的各种苯甲醇底物（苯甲醇及其具有吸电子和供电子基团的衍生物）氧化反应表现出优异的催化活性（转化率从93%到>99%）和选择性（对苯甲醛>99%）。此外，2是一种典型的多相催化剂，热溶液浸出实验证实了这一点，并且它至少可以循环使用6次而其催化活性和选择性没有明显损失。
A new 3D porous Cu(II)-MOF (1) was synthesized based on a ditopic pyridyl substituted diketonate ligand and Cu(OAc)(2) in solution, and it features a 3D NbO motif which is determined by the X-ray crystallography. Furthermore, the Pd NPs-loaded hybrid material Pd@Cu(II)-MOF (2) was prepared based on 1 via solution impregnation, and its structure was confirmed by HRTEM, SEM, XRPD, gas adsorption-desorption, and ICP measurement. 2 exhibits excellent catalytic activity (conversion, 93% to >99%) and selectivity (>99% to benzaldehydes) for various benzyl alcohol substrates (benzyl alcohol and its derivatives with electron-withdrawing and electron-donating groups) oxidation reactions in air. In addition, 2 is a typical heterogeneous catalyst, which was confirmed by hot solution leaching experiment, and it can be recycled at least six times without significant loss of its catalytic activity and selectivity.