Hydrogenation of aromatic rings can be used not only for synthesis of fine chemicals,but also for hydrogen storage and transportation using organic hydrides.In this paper,a yolk–shell structured SiO_(2)@Ru@NC catalys...Hydrogenation of aromatic rings can be used not only for synthesis of fine chemicals,but also for hydrogen storage and transportation using organic hydrides.In this paper,a yolk–shell structured SiO_(2)@Ru@NC catalyst,which was successfully synthesized by a strategy combining a modified Stöber method and vacuum-assisted impregnation,revealed excellent catalytic activity in dimethyl terephthalate(DMT)hydrogenation to dimethyl 1,4-cyclohexanedicarboxylate(DMCD),which is a green chemical reagent and precursor for high-value chemicals.Characterization results showed that highly dispersed Ru NPs with subnanometer size distribution were encapsulated in the yolk–shell nanoarchitecture and the mesoporous shell could ensure unhindered diffusion of reactant molecules.Moreover,yolk–shell structure-induced interaction of Ru and the carbon shell allowed for tuning the electronic structure of the Ru species,which in turn could regulate the catalytic properties.The yolk–shell nanoarchitecture catalyst offers advantages of low active metal loading,and excellent activity and stability,and thus can expand applications of ultra-low loaded precious metal catalysts in catalytic conversion of aromatic compounds.展开更多
基金financially supported by the National Natural Science Foundation of China(Grant No.52072371,51871209)Key Technologies Research and Development Program of Anhui Province(202004a06020056)+2 种基金Special Foundation of President of HFIPS(No.YZJJ202102)HFIPS Director’s Fund(No.GGZX-GTCX-2023-07,YZJJ-GGZX-2022-01)HFIPS Director’s Fund(No.2023YZGH05)。
文摘Hydrogenation of aromatic rings can be used not only for synthesis of fine chemicals,but also for hydrogen storage and transportation using organic hydrides.In this paper,a yolk–shell structured SiO_(2)@Ru@NC catalyst,which was successfully synthesized by a strategy combining a modified Stöber method and vacuum-assisted impregnation,revealed excellent catalytic activity in dimethyl terephthalate(DMT)hydrogenation to dimethyl 1,4-cyclohexanedicarboxylate(DMCD),which is a green chemical reagent and precursor for high-value chemicals.Characterization results showed that highly dispersed Ru NPs with subnanometer size distribution were encapsulated in the yolk–shell nanoarchitecture and the mesoporous shell could ensure unhindered diffusion of reactant molecules.Moreover,yolk–shell structure-induced interaction of Ru and the carbon shell allowed for tuning the electronic structure of the Ru species,which in turn could regulate the catalytic properties.The yolk–shell nanoarchitecture catalyst offers advantages of low active metal loading,and excellent activity and stability,and thus can expand applications of ultra-low loaded precious metal catalysts in catalytic conversion of aromatic compounds.
