Synthetic chemistry enables constructing molecular complexity using simple substrates through simple processes.We disclose an unprecedented Al-atom transfer strategy for the synthesis of aluminum heterocycles with hig...Synthetic chemistry enables constructing molecular complexity using simple substrates through simple processes.We disclose an unprecedented Al-atom transfer strategy for the synthesis of aluminum heterocycles with high atom economy.This strategy involves an effective cycloaddition of a free carbazolyl-aluminylene with unsaturated hydrocarbons,followed by facile cleavage of the N-Al bond.The aluminylene formally behaves as a tetra-active ambiphilic[Al+]cation transfer reagent in a two-step manner,and the only byproduct is a carbazolide salt that can be utilized to regenerate the aluminylene.The carbazolyl Al-heterocycles show unique luminescent properties,in which one exhibits dual emission.Our approach not only has a significant impact on the future design of single-atom addition reactions but also paves the way for emissive materials based on Al-heterocycles.展开更多
基金financial support from the National Natural Science Foundation of China(grant nos.22271132,22101114,and 22201122)Guangdong Basic and Applied Basic Research Foundation(grant no.2022A1515011717)+2 种基金Guangdong Provincial Key Laboratory of Catalysis(grant no.2020B121201002)X.Z.thanks China Postdoctoral Science Foundation(CPSF)for financial support(grant no.2022T150289)Y.M.thanks CPSF for financial support(grant nos.2021 M691420 and 2022T150288).
文摘Synthetic chemistry enables constructing molecular complexity using simple substrates through simple processes.We disclose an unprecedented Al-atom transfer strategy for the synthesis of aluminum heterocycles with high atom economy.This strategy involves an effective cycloaddition of a free carbazolyl-aluminylene with unsaturated hydrocarbons,followed by facile cleavage of the N-Al bond.The aluminylene formally behaves as a tetra-active ambiphilic[Al+]cation transfer reagent in a two-step manner,and the only byproduct is a carbazolide salt that can be utilized to regenerate the aluminylene.The carbazolyl Al-heterocycles show unique luminescent properties,in which one exhibits dual emission.Our approach not only has a significant impact on the future design of single-atom addition reactions but also paves the way for emissive materials based on Al-heterocycles.
