Pd@MCM-48的壳层厚度对Suzuki偶联反应催化性能的影响  

Effect of Shell Thickness of Pd@MCM-48 on Catalytic Performance of Suzuki Coupling Reaction

作　　者：邓一蕾 张龙云 周港华 杨艳菊 宁欣 DENG Yi-lei;ZHANG Long-yun;ZHOU Gang-hua;YANG Yan-ju;NING Xin(School of Environmental Science and Engineering,Yangzhou University,Yangzhou 225000,China;State Key Laboratory of Pollution Control and Resource Reuse,School of the Environment,Nanjing University,Nanjing 210046,China)

机构地区：[1]扬州大学环境科学与工程学院,江苏扬州225000 [2]南京大学环境学院污染控制及资源化研究国家重点实验室,江苏南京210046

出　　处：《安徽师范大学学报(自然科学版)》2023年第6期531-537,共7页Journal of Anhui Normal University(Natural Science)

基　　金：江苏省高等学校自然科学研究面上项目(21KJB610003);污染控制与资源化研究国家重点实验室开放基金项目(PCRRF20006).

摘　　要：采用Stöber方法制备了以Pd纳米颗粒为核、介孔氧化硅(MCM-48)为壳的核壳型催化剂Pd@MCM-48。通过改变模板剂F127的投加量调节Pd@MCM-48壳层厚度。采用X射线衍射、N2-物理吸附、扫描/透射电子显微镜对催化剂的结构性质进行表征。研究催化剂壳层厚度对Suzuki偶联反应催化性能的影响。结果表明,核壳结构催化剂的平均壳层厚度在45.6~59.6 nm之间,随着壳层厚度增加,Suzuki偶联反应的催化活性逐渐降低,这可能由于较厚的壳层限制了反应物的有效扩散。然而,联苯的产率不受壳层厚度的影响。此外,催化剂可以通过简单回收并重复使用。在5次循环反应后,催化活性无明显下降且Pd浸出量可以忽略,主要归因于催化剂壳层的限域作用。A core-shell catalyst with Pd nanoparticles as the core and mesoporous silica(MCM-48)as the shell is prepared by Stöber method.The shell thickness of the catalysts are controlled by changing the addition amounts of template agent F127.The structure properties of the catalysts are characterized by X-ray diffraction,N2-physical adsorption,scanning electron microscopy and transmission electron microscopy.The effect of shell thickness on the catalytic performance of Suzuki coupling creation is studied.The results show that the shell thickness was in the range of 45.6-59.6 nm.The catalytic activity decreased gradually with the increase of shell thickness,probably because to thicker shells contribute to more severe diffusion limitations of the reactants.However,the yield of biphenyl is 99%and not influenced by the shell thickness.In addition,the catalyst could be simply recycled and reused.After 5 cycles,there was no significant reduction in catalytic activity and the leaching amount of Pd was negligible,which attributed to the confined effect of Pd@MS-x with core-shell structure.

关 键 词：核壳结构 Pd@MCM-48 壳层厚度 SUZUKI偶联反应 

分 类 号：O643[理学—物理化学]