The development of efficient and sustainable methods to obtain spirocyclic compounds is of significance as these structures are widely found in pharmaceuticals and agrochemicals.Herein,we disclose an electrochemical d...The development of efficient and sustainable methods to obtain spirocyclic compounds is of significance as these structures are widely found in pharmaceuticals and agrochemicals.Herein,we disclose an electrochemical dearomative spirocyclization of N-acyl sulfonamides in a continuous-flow cell.The reaction is simple and efficient without external catalysts or supporting electrolytes and could be applied in a decagram-scale synthesis.展开更多
The discovery of new carbon nanomaterials such as fullerenes,carbon nanotubes,graphene,and graphyne has always driven the development of various fields of science[1].The arrangement of carbon atoms largely influences ...The discovery of new carbon nanomaterials such as fullerenes,carbon nanotubes,graphene,and graphyne has always driven the development of various fields of science[1].The arrangement of carbon atoms largely influences their properties.In the past decade,the atomic-precision synthesis and study of molecular nanocarbons,which is the sub-structures of larger carbon nanostructures,have attracted huge attention[2].Among them,the synthesis of cycloparaphenylene(CPP)(the substructure of carbon nanotubes)has been developed considerably since 2008[3].Recently,topologically complex nanocarbon[4]starting from CPP or oligoparaphenylene-derived carbon nanohoop has been explored as a new type of MIM,which undoubtedly revolutionizes a wide range of sciences,especially in the field of molecular machine(Fig.1)[5].展开更多
Both sulfur and fluorine play important roles in organic synthesis, the life science, and materials science.The direct incorporation of these elements into organic scaffolds with precise control of the oxidation state...Both sulfur and fluorine play important roles in organic synthesis, the life science, and materials science.The direct incorporation of these elements into organic scaffolds with precise control of the oxidation states of sulfur moieties is of great significance. Herein, we report the highly selective electrochemical vicinal fluorosulfenylation and fluorosulfoxidation reactions of alkenes, which were enabled by the unique ability of electrochemistry to dial in the potentials on demand. Preliminary mechanistic investigations revealed that the fluorosulfenylation reaction proceeded through a radical-polar crossover mechanism involving a key episulfonium ion intermediate. Subsequent electrochemical oxidation of fluorosulfides to fluorosulfoxides were readily achieved under a higher applied potential with the adventitious H;O in the reaction mixture.展开更多
A class of side-chain type ferrocene macrocycles with a radially conjugated system is introduced in this study.The stereo configurations of these ferrocene rings were determined through single-crystal X-ray diffractio...A class of side-chain type ferrocene macrocycles with a radially conjugated system is introduced in this study.The stereo configurations of these ferrocene rings were determined through single-crystal X-ray diffraction analysis.Notably,in the solid state,the ferrocene rings exhibit a distinctive herringbone stacking pattern imposed by a ferrocene-to-ring host−guest interaction.Through UV−vis absorption spectroscopy,electrochemical measurements,and theoretical calculations,valuable insights into the electronic properties of these rings were obtained.In addition,the single crystal of macrocycle A_(2)B demonstrates a second-order nonlinear optical response.As a class of organometallic nanorings,this work holds great potential for further exploration in the fields of organometallic chemistry,molecular electronics,and host−guest chemistry.展开更多
基金supported by the National Natural Science Foundation of China(No.22171046)the Hundred-Talent Project of Fujian(No.50021113).
文摘The development of efficient and sustainable methods to obtain spirocyclic compounds is of significance as these structures are widely found in pharmaceuticals and agrochemicals.Herein,we disclose an electrochemical dearomative spirocyclization of N-acyl sulfonamides in a continuous-flow cell.The reaction is simple and efficient without external catalysts or supporting electrolytes and could be applied in a decagram-scale synthesis.
基金supported by the National Natural Science Foundation of China(No.22071025).
文摘The discovery of new carbon nanomaterials such as fullerenes,carbon nanotubes,graphene,and graphyne has always driven the development of various fields of science[1].The arrangement of carbon atoms largely influences their properties.In the past decade,the atomic-precision synthesis and study of molecular nanocarbons,which is the sub-structures of larger carbon nanostructures,have attracted huge attention[2].Among them,the synthesis of cycloparaphenylene(CPP)(the substructure of carbon nanotubes)has been developed considerably since 2008[3].Recently,topologically complex nanocarbon[4]starting from CPP or oligoparaphenylene-derived carbon nanohoop has been explored as a new type of MIM,which undoubtedly revolutionizes a wide range of sciences,especially in the field of molecular machine(Fig.1)[5].
基金Financial support from the National Natural Science Foundation of China (Nos. 21901041 and 21772023)State Key Laboratory of Physical Chemistry of Solid Surfaces,Xiamen University (No.202008)Fuzhou University (No. 510841)。
文摘Both sulfur and fluorine play important roles in organic synthesis, the life science, and materials science.The direct incorporation of these elements into organic scaffolds with precise control of the oxidation states of sulfur moieties is of great significance. Herein, we report the highly selective electrochemical vicinal fluorosulfenylation and fluorosulfoxidation reactions of alkenes, which were enabled by the unique ability of electrochemistry to dial in the potentials on demand. Preliminary mechanistic investigations revealed that the fluorosulfenylation reaction proceeded through a radical-polar crossover mechanism involving a key episulfonium ion intermediate. Subsequent electrochemical oxidation of fluorosulfides to fluorosulfoxides were readily achieved under a higher applied potential with the adventitious H;O in the reaction mixture.
基金supported from National Natural Science Foundation of China(No.22071025)the Natural Science Fund of Fujian Province,China(No.2022J011152).
文摘A class of side-chain type ferrocene macrocycles with a radially conjugated system is introduced in this study.The stereo configurations of these ferrocene rings were determined through single-crystal X-ray diffraction analysis.Notably,in the solid state,the ferrocene rings exhibit a distinctive herringbone stacking pattern imposed by a ferrocene-to-ring host−guest interaction.Through UV−vis absorption spectroscopy,electrochemical measurements,and theoretical calculations,valuable insights into the electronic properties of these rings were obtained.In addition,the single crystal of macrocycle A_(2)B demonstrates a second-order nonlinear optical response.As a class of organometallic nanorings,this work holds great potential for further exploration in the fields of organometallic chemistry,molecular electronics,and host−guest chemistry.
