Subject Code:H07 With the support from the National Natural Science Foundation of China and HGZ-CAS,a collaborative study by the research groups led by Prof.Chen Ping(陈萍)from Dalian Institute of Chemical Physics,Chi...Subject Code:H07 With the support from the National Natural Science Foundation of China and HGZ-CAS,a collaborative study by the research groups led by Prof.Chen Ping(陈萍)from Dalian Institute of Chemical Physics,Chinese Academy of Sciences and Prof.M.Dornheim,Helmholtz-Zentrum Geesthacht,Germany展开更多
Converting low-concentration carbon dioxide(CO_(2))into value-added chemicals meets the demand of carbonneutral technologies,yet efficient and stable catalysts for CO_(2)absorption and activation are urgently desired....Converting low-concentration carbon dioxide(CO_(2))into value-added chemicals meets the demand of carbonneutral technologies,yet efficient and stable catalysts for CO_(2)absorption and activation are urgently desired.Singleatom(-site)catalysts(SACs)supported by molecule-based porous materials offer new catalyst platforms that enable the integration of enrichment,activation,and conversion through multisite cooperation.Herein,we report the synthesis of the first N-heterocyclic olefin(NHO)coordinated Pd SAC through a facile precursor-partial metallization of a methyl-modified porous imidazolium-based polymer,which exhibits the highest turnover frequency of 117.7±1.4 h^(−1) for Pd-catalyzed one-pot tri-component reactions of propargylamines,aryl iodides,and CO_(2)in simulated flue gas,and is approximately 58 times higher than that of N-heterocyclic carbene coordinated analogues and outperforms all reported catalysts.Various spectroscopic technologies and density functional theory calculations unveiled the NHO-assisted dual-site catalysis through the formation of NHO–CO_(2)adducts and intramolecular cyclization intermediates.These findings showcase the significant potential of coupling inorganic single atoms and functional organic sites for multicomponent catalytic reactions.展开更多
文摘Subject Code:H07 With the support from the National Natural Science Foundation of China and HGZ-CAS,a collaborative study by the research groups led by Prof.Chen Ping(陈萍)from Dalian Institute of Chemical Physics,Chinese Academy of Sciences and Prof.M.Dornheim,Helmholtz-Zentrum Geesthacht,Germany
基金financially supported by the National Natural Science Foundation of China(grant nos.22161021,22261002,21890382,and 22375079)the Key Project of Jiangxi Provincial Department of Science and Technology(grant nos.S2023ZRZDL0164,20232ACB203016,and S2023ZRMSL0668)+2 种基金the Key Laboratory of Jiangxi University for Functional Materials Chemistry(grant no.FMC21702)the Education Department of Jiangxi Province(grant nos.GJJ201427 and SZUGSHX2022-1043)C.-T.H.acknowledges the support of Jiangxi Province(grant no.20224ACB214001).
文摘Converting low-concentration carbon dioxide(CO_(2))into value-added chemicals meets the demand of carbonneutral technologies,yet efficient and stable catalysts for CO_(2)absorption and activation are urgently desired.Singleatom(-site)catalysts(SACs)supported by molecule-based porous materials offer new catalyst platforms that enable the integration of enrichment,activation,and conversion through multisite cooperation.Herein,we report the synthesis of the first N-heterocyclic olefin(NHO)coordinated Pd SAC through a facile precursor-partial metallization of a methyl-modified porous imidazolium-based polymer,which exhibits the highest turnover frequency of 117.7±1.4 h^(−1) for Pd-catalyzed one-pot tri-component reactions of propargylamines,aryl iodides,and CO_(2)in simulated flue gas,and is approximately 58 times higher than that of N-heterocyclic carbene coordinated analogues and outperforms all reported catalysts.Various spectroscopic technologies and density functional theory calculations unveiled the NHO-assisted dual-site catalysis through the formation of NHO–CO_(2)adducts and intramolecular cyclization intermediates.These findings showcase the significant potential of coupling inorganic single atoms and functional organic sites for multicomponent catalytic reactions.
