Li Yuan, Pei Biao, Chen Junjie, Bing Shaosuo, Hou Linxiao, Sun Qi, Xu Gang, Yao Zhikan, Zhang Lin
Key Laboratory of Biomass Chemical Engineering, College of Chemical and Biological Engineering, Zhejiang University, Hangzhou 310027, P.R. China.
Key Laboratory of Biomass Chemical Engineering, College of Chemical and Biological Engineering, Zhejiang University, Hangzhou 310027, P.R. China; Ningbo Research Institute, Zhejiang University, Ningbo 315100, P.R. China.
J Colloid Interface Sci. 2021 Jun;591:273-280. doi: 10.1016/j.jcis.2021.01.105. Epub 2021 Feb 3.
A novel catalyst with a yolk-shell structure was designed to overcome the leaching of noble metals in heterogeneous catalysis. Through a template method, palladium (Pd) nanoparticles were encapsulated by hollow spherical covalent organic frameworks (COFs) consisting of 2,4,6-trihydroxybenzene-1,3,5-tricarbaldehyde (Tp) and p-phenylenediamine (Pa). The final catalyst with a yolk-shell structure was denoted as (Pd/C)@TpPa COFs. The unique morphology and chemical structure of this novel composite (Pd/C)@TpPa COFs were confirmed by a transmission electron microscope (TEM), a laser particle analyzer, X-ray diffraction (XRD), and N adsorption and desorption. Subsequently, to demonstrate its catalytic performance brought by structural design, this novel catalyst was applied to catalyze the Suzuki reaction. Interestingly, this catalyst exhibited a brilliant size cutoff efficiency for aryl benzene amounting to 100% and achieved a high conversion with only 0.05 mol% Pd loading. Besides, this catalyst could be readily recovered via filtration and reused for at least five consecutive cycles without any significant loss in its activity.
设计了一种具有核壳结构的新型催化剂，以克服多相催化中贵金属的浸出问题。通过模板法，钯（Pd）纳米颗粒被由2,4,6-三羟基苯-1,3,5-三甲醛（Tp）和对苯二胺（Pa）组成的中空球形共价有机框架（COF）包裹。具有核壳结构的最终催化剂被标记为（Pd/C）@TpPa COF。通过透射电子显微镜（TEM）、激光粒度分析仪、X射线衍射（XRD）以及N吸附-脱附对这种新型复合材料（Pd/C）@TpPa COF独特的形态和化学结构进行了确认。随后，为了证明其结构设计带来的催化性能，将这种新型催化剂应用于催化铃木反应。有趣的是，该催化剂对芳基苯表现出出色的尺寸截留效率，达到100%，并且在钯负载量仅为0.05 mol%时就实现了高转化率。此外，该催化剂可通过过滤轻松回收，并可连续重复使用至少五个循环，其活性没有任何显著损失。
