Comprehensive Summary The development of carbon dioxide(CO_(2))capture and utilization is of vital importance.However,previous photocatalytic reduction reactions for converting CO_(2)into chemicals(e.g.,CO,HCOOH,CH_(4...Comprehensive Summary The development of carbon dioxide(CO_(2))capture and utilization is of vital importance.However,previous photocatalytic reduction reactions for converting CO_(2)into chemicals(e.g.,CO,HCOOH,CH_(4),or CH_(3)OH)rely heavily on sacrificial reagents.Herein,we disclose a visible light photoredox-catalyzed 1,2-difunctionalization of terminal alkynes by using CO_(2)as an ideal quenching reagent and the xanthene dye Rhodamine 6G(Rh-6G)as a photocatalyst(PC)via consecutive photoinduced electron transfer(ConPET)process.展开更多
α-Azaarene quaternary carbon centers are prevalent in drug molecules,making the development of efficient synthetic approaches of great interest.Herein,we describe an unprecedented method for constructingα-all-carbon...α-Azaarene quaternary carbon centers are prevalent in drug molecules,making the development of efficient synthetic approaches of great interest.Herein,we describe an unprecedented method for constructingα-all-carbon quaternary carbon-centered azaarenes by employing photocatalytic reductive coupling of various 2,2-disubstituted cycloproarylketones with readily available cyanoazaarenes.The reaction proceeds with high efficiency,displaying excellent compatibility with various functional groups and demonstrating high chemo-and regioselectivity.Mechanistic investigations suggest that consecutive photo-induced electron transfer(ConPET)plays a crucial role in the formation of photocatalyst with greater reducing capability,ultimately enabling the direct reductive conversion of unreactiveπ-bonds under mild and transition-metal-free conditions.展开更多
基金supported by the National Natural Science Foundation of China(Nos.22471045,U2001222)the Science and Technology Planning Project of Guangdong Province(No.2021A0505030069)。
文摘Comprehensive Summary The development of carbon dioxide(CO_(2))capture and utilization is of vital importance.However,previous photocatalytic reduction reactions for converting CO_(2)into chemicals(e.g.,CO,HCOOH,CH_(4),or CH_(3)OH)rely heavily on sacrificial reagents.Herein,we disclose a visible light photoredox-catalyzed 1,2-difunctionalization of terminal alkynes by using CO_(2)as an ideal quenching reagent and the xanthene dye Rhodamine 6G(Rh-6G)as a photocatalyst(PC)via consecutive photoinduced electron transfer(ConPET)process.
基金Grants from the National Natural Science Foundation of China(22271077,21925103,21901062)the Natural Science Foundation of Henan(232300421078,222301420046)+2 种基金the Program for Science&Technology Innovation Talents in Universities of Henan Province(24HASTIT001)the China Postdoctoral Science Foundation(2021M690890)Henan University are gratefully acknowledged.
文摘α-Azaarene quaternary carbon centers are prevalent in drug molecules,making the development of efficient synthetic approaches of great interest.Herein,we describe an unprecedented method for constructingα-all-carbon quaternary carbon-centered azaarenes by employing photocatalytic reductive coupling of various 2,2-disubstituted cycloproarylketones with readily available cyanoazaarenes.The reaction proceeds with high efficiency,displaying excellent compatibility with various functional groups and demonstrating high chemo-and regioselectivity.Mechanistic investigations suggest that consecutive photo-induced electron transfer(ConPET)plays a crucial role in the formation of photocatalyst with greater reducing capability,ultimately enabling the direct reductive conversion of unreactiveπ-bonds under mild and transition-metal-free conditions.