Regiodivergent catalysis provides an efficient strategic approach for the construction of architecturally different molecules from the same starting materials. In this field, the intermolecular regiodivergent 1,2-difu...Regiodivergent catalysis provides an efficient strategic approach for the construction of architecturally different molecules from the same starting materials. In this field, the intermolecular regiodivergent 1,2-difunctionalization of alkenes with two electrophiles is still a challenging task. A ligand-controlled, nickel-catalyzed regiodivergent dicarbofunctionalization of alkenes using both aryl/vinyl halides and acetals as electrophiles under mild reductive reaction conditions has been accomplished. This study provides a general approach to accessing both β-methoxyl esters and γ-methoxyl esters from readily available acrylates,aryl halides and acetals. Experimental mechanistic evidence supports that the difference in regioselective outcomes is attributed to the ligand tuning the reactivity of the nickel catalyst, which results in different catalytic cycles operating for these two reaction conditions.展开更多
1,1-Diaryl moieties are core structures in a wide range of bioactive and pharmaceutical compounds.Transition-metal catalysis is a convenient approach to accessing these invaluable compounds affording high yields and e...1,1-Diaryl moieties are core structures in a wide range of bioactive and pharmaceutical compounds.Transition-metal catalysis is a convenient approach to accessing these invaluable compounds affording high yields and enantioselectivities.This review summarizes 1,1-diarylalkanes synthesis through transition metal catalysis.Particular focus is given to recent developments,such as reductive cross-electrophile couplings,benzylic C–H bond arylation,transformations involving metal migration,asymmetric hydrogenation of 1,1-diarylalkenes and three-component coupling reactions.展开更多
A nickel-catalyzed 1,1-diarylation of electronically unbiased alkenes has been developed,providing straightforward access to diarylalkanes from readily available materials.Importantly,both the efficiency and the regio...A nickel-catalyzed 1,1-diarylation of electronically unbiased alkenes has been developed,providing straightforward access to diarylalkanes from readily available materials.Importantly,both the efficiency and the regioselectivity of this transformation are ensured by reaction conditions,rather than the coordinating group of substrates.We also demonstrate that under balloon pressure,ethylene and propylene can also be utilized as substrates.Preliminary mechanistic experiments suggest that this transformation involves a Ni(0)/Ni(Ⅱ)catalytic cycle rather than a Ni(Ⅰ)/Ni(Ⅲ)cycle.展开更多
基金supported by the National Natural Science Foundation of China (21871211, 21774029, 22122107)the Fundamental Research Funds for Central Universities (2042019kf0208)。
文摘Regiodivergent catalysis provides an efficient strategic approach for the construction of architecturally different molecules from the same starting materials. In this field, the intermolecular regiodivergent 1,2-difunctionalization of alkenes with two electrophiles is still a challenging task. A ligand-controlled, nickel-catalyzed regiodivergent dicarbofunctionalization of alkenes using both aryl/vinyl halides and acetals as electrophiles under mild reductive reaction conditions has been accomplished. This study provides a general approach to accessing both β-methoxyl esters and γ-methoxyl esters from readily available acrylates,aryl halides and acetals. Experimental mechanistic evidence supports that the difference in regioselective outcomes is attributed to the ligand tuning the reactivity of the nickel catalyst, which results in different catalytic cycles operating for these two reaction conditions.
基金supported by the National Natural Science Foundation of China(21702151,21871211)the Fundamental Research Funds for Central Universities(2042019kf0208)。
文摘1,1-Diaryl moieties are core structures in a wide range of bioactive and pharmaceutical compounds.Transition-metal catalysis is a convenient approach to accessing these invaluable compounds affording high yields and enantioselectivities.This review summarizes 1,1-diarylalkanes synthesis through transition metal catalysis.Particular focus is given to recent developments,such as reductive cross-electrophile couplings,benzylic C–H bond arylation,transformations involving metal migration,asymmetric hydrogenation of 1,1-diarylalkenes and three-component coupling reactions.
基金support from National Natural Science Foundation of China(21702151 and 21871211)the Fundamental Research Funds for Central Universities(2042019kf0208).
文摘A nickel-catalyzed 1,1-diarylation of electronically unbiased alkenes has been developed,providing straightforward access to diarylalkanes from readily available materials.Importantly,both the efficiency and the regioselectivity of this transformation are ensured by reaction conditions,rather than the coordinating group of substrates.We also demonstrate that under balloon pressure,ethylene and propylene can also be utilized as substrates.Preliminary mechanistic experiments suggest that this transformation involves a Ni(0)/Ni(Ⅱ)catalytic cycle rather than a Ni(Ⅰ)/Ni(Ⅲ)cycle.
