Construction of highly dispersed Pt single sites and high-efficiencyheterocatalysis silylation of alcohols with silanes  

作　　者：Qiulian Wei Yunqiang Sun Shan Wang Zunfu Hu Qingyun Liu Xiuwen Zheng 

机构地区：[1]School of Chemical and Biological Engineering,Shandong University of Science and Technology,Qingdao 266510,China [2]Key Laboratory of Functional Nanomaterials and Technology in Universities of Shandong,College of Chemistry and Chemical Engineering,Linyi University,Linyi 276000,China

出　　处：《Nano Research》2023年第4期4643-4649,共7页纳米研究（英文版）

基　　金：supported by the National Natural Science Foundation of China(Nos.22075122 and 21971152);the Natural Science Foundation of Shandong Province(Nos.ZR2019BB038,ZR2020QB170,and ZR2020MB003).

摘　　要：The construction of silicon-oxygen bonds has been highlighted as an exciting achievement in organosilicon and green chemistry,but their synthetic efficiency has great improvement potential,so it is crucial to explore and achieve an effective approach for synthesizing such compounds.In this study,we successfully prepared the highly dispersed platinum single-atom catalyst(Pt SAC/N-C)through a coordination-assisted strategy with a mixture of ligands(H2bpdc and H2bpydc),which were used for the Osilylation of alcohols with silanes.The strong coordination between Pt2+and the Pyridine N at the skeleton of UiO-67 plays a critical role in accessing the atomically isolated dispersion of Pt sites.Without the assistance of the H2bpydc ligands,the Pt/UiO-67-bpdc precursor is prone to aggregation during the pyrolysis process,resulting in the formation of Pt nanoparticles.Aided by advanced characterization techniques of high-angle annular dark-field scanning transmission electron microscopy(HAADFSTEM)and X-ray absorption fine structure(XAFS)spectroscopy,it has been demonstrated that atomically dispersed Pt was formed on the UiO-67 through a local structure of four-coordinated Pt-N4,exhibiting a high actual Pt loading content(0.6962 wt.%).In the oxidation of silanes,the Pt SAC/N-C catalyst showed a high turnover frequency(TOF)value(up to 9,920 h−1)when the catalyst loading decreased to 0.005%.Excellent performance was maintained during recycling experiments,indicating high stability of the catalyst.

关 键 词：high-dispersion single-atom catalysis O-silylation heterogeneous catalysis 

分 类 号：O64[理学—物理化学]