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作 者:Shixiang Feng Qi Yu Xinbin Ma Xiaohu Yu Ning Yan
机构地区:[1]Joint School of National University of Singapore and Tianjin University,International Campus of Tianjin University,Binhai New City,Fuzhou 350207,China [2]School of Materials Science and Engineering,Shaanxi Laboratory of Catalysis,Shaanxi University of Technology,Hanzhong 723001,China [3]School of Chemical Engineering and Technology,Tianjin University,Tianjin 300072,China [4]Department of Chemical&Biomolecular Engineering,National University of Singapore,Singapore 117580,Singapore
出 处:《National Science Open》2023年第2期161-174,共14页国家科学进展(英文)
基 金:supported by the National Natural Science Foundation of China(92061109 and 22273053);the Natural Science Basic Research Program of Shaanxi(2021JCW-20 and 2022KJXX-18).
摘 要:Atomic dispersion of Rh on phosphotungstic acid(PTA)salts was achieved by a self-assembled precipitation method using alkali metal ions as coprecipitation reagents.During styrene hydroformylation,the supported Rh single-atom catalyst(Rh1/M-PTA,M refers to an alkali metal ion)demonstrated an optimum turnover frequency(TOF)of 1076 h−1.With increasing ionic radius,the pore size of the catalysts increased in the following order:Rh1/K-PTA<Rh1/Rb-PTA<Rh1/Cs-PTA.The catalytic activity showed the same trend,suggesting a positive correlation between pore size and hydroformylation perfor-mance.Further experimental data suggested that temperature is an important factor affecting not only the activity but also the selectivity.This study enriches the understanding of the structure and catalytic properties of PTA-supported single-atom materials.The cation-controlled synthesis of catalysts may also be applied to prepare other single-atom catalysts with tunable pore size distributions.
关 键 词:POLYOXOMETALATES Rh single-atom HYDROFORMYLATION SELF-ASSEMBLY STYRENE
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