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作 者:Zhen Xue Shasha Wu Yujing Fu Lan Luo Min Li Zhenhua Li Mingfei Shao Lirong Zheng Ming Xu Haohong Duan
机构地区:[1]State Key Laboratory of Chemical Resource Engineering,Beijing University of Chemical Technology,Beijing 100029,China [2]Department of Chemistry,TsinghuaUniversity,Beijing 10084,China [3]Institute of High Energy Physics,The Chinese Academy of Sciences,Beijing 100049,China
出 处:《Journal of Energy Chemistry》2023年第1期239-248,I0007,共11页能源化学(英文版)
基 金:financially supported by the National Natural Science Foundation of China(202102007,21978147 and 21935001);the Fundamental Research Funds for the Central Universities(buctrc202112)。
摘 要:Selective reductive amination of carbonyl compounds with high activity is very essential for the chemical and pharmaceutical industry,but scarcely successful paradigm was reported via efficient photocatalytic reactions.Herein,the ultrasmall Ru nanoclusters(~0.9 nm)were successfully fabricated over P25 support with positive charged Ru^(δ+)species at the interface.A new route was developed to achieve the furfural(FAL)to furfurylamine(FAM)by coupling the light-driven reductive amination and hydrogen transfer of ethanol over this type catalyst.Strikingly,the photocatalytic activity and selectivity are strongly dependent on the particle size and electronic structure of Ruthenium.The Ru^(δ+)species at the interface promote the formation of active imine intermediates;moreover,the Ru nanoclusters facilitate the separation efficiency of electrons and holes as well as accelerate the further hydrogenation of imine intermediates to product primary amines.In contrast Ru particles in larger nanometer size facilitate the formation of the furfuryl alcohol and excessive hydrogenation products.In addition,the coupling byproducts can be effectively inhibited via the construction of sub-nanocluster.This study offers a new path to produce the primary amines from biomass-derived carbonyl compounds over hybrid semiconductor/metal-clusters photocatalyst via light-driven tandem catalytic process.
关 键 词:FURFURAL Reductive amination Ru nanoclusters Hydrogen transfer PHOTOCATALYSIS
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