Catalytic four-component radical carbonylation of unactivated alkenes has recently been recognized as a robust protocol for rapid construction of various structurally diverse carbonyl compounds.Given the significance ...Catalytic four-component radical carbonylation of unactivated alkenes has recently been recognized as a robust protocol for rapid construction of various structurally diverse carbonyl compounds.Given the significance of fluorine-containing groups,this reaction class has been extensively applied to assembly of a variety of perfluoroalkyl carboxylic acid derivatives by transition metal catalysis.Herein,we report a visible-light-driven radical relay 1,2-perfluoroalkylation aminocarbonylation of unactivated alkenes using CO gas as carbonyl source and 4CzIPN as organic photocatalyst.A wide range of alkenes and amines were well tolerated,providing the valuableβ-perfluoroalkylated amides with generally good yields and high chemoselectivity.展开更多
α,β-Unsaturated primary amides are important intermediates and building blocks in organic synthesis.Herein,we report a ligand-free iron-catalyzed hydroaminocarbonylation of alkynes using NH_(4)HCO_(3)as the ammonia ...α,β-Unsaturated primary amides are important intermediates and building blocks in organic synthesis.Herein,we report a ligand-free iron-catalyzed hydroaminocarbonylation of alkynes using NH_(4)HCO_(3)as the ammonia source,enabling the highly efficient and regioselective synthesis of linearα,β-unsaturated primary amides.Various aromatic and aliphatic alkynes are transformed into the desired linearα,β-unsaturated primary amides in good to excellent yields.Further studies show that using NH_(4)HCO_(3)as the ammonia source is key to obtain good yields and selectivity.The utility of this route is demonstrated with the synthesis of linearα,β-unsaturated amides including vanilloid receptor-1 antagonist TRPV-1.展开更多
The discovery of a rearrangement reaction of 5-amino-1-arylaminocarbonyl-1,2,triazole(pyrszole)to 5-arylureylene-1,2,4-trazole and the mechanism for thisrearrangement reaction are presented. The rearrangement reaction...The discovery of a rearrangement reaction of 5-amino-1-arylaminocarbonyl-1,2,triazole(pyrszole)to 5-arylureylene-1,2,4-trazole and the mechanism for thisrearrangement reaction are presented. The rearrangement reaction could be attributed to athermodynamic energy preference leading to the predominant formation of 5-aryluretjlene1,2,4-triazole,as shown by molecular mechanics calculation with MMX Program.展开更多
A hydrogen storage system was developed via heterogeneous catalysis,employing the dehydrogenative coupling of methanol and N,N′-dimethylethylenediamine to efficiently produce high-purity H_(2).In this process,the Cu/...A hydrogen storage system was developed via heterogeneous catalysis,employing the dehydrogenative coupling of methanol and N,N′-dimethylethylenediamine to efficiently produce high-purity H_(2).In this process,the Cu/ZnO/Al_(2)O_(3) catalyst displayed superior activity in hydrogen production,with Cu+identified as the major active site through comprehensive characterization.展开更多
基金the financial support from the National Natural Science Foundation of China(21971081,22171099,21820102003,91956201,22203034,and 92256301)the Double-Thousand Talents Plan of Jiangxi Province(jxsq2023102004)+1 种基金the Open Research Fund of School of Chemistry and Chemical Engineering,Henan Normal University(2021YB02)and the Program of Introducing Talents of Discipline to Universities of China(111 Program,B17019).
文摘Catalytic four-component radical carbonylation of unactivated alkenes has recently been recognized as a robust protocol for rapid construction of various structurally diverse carbonyl compounds.Given the significance of fluorine-containing groups,this reaction class has been extensively applied to assembly of a variety of perfluoroalkyl carboxylic acid derivatives by transition metal catalysis.Herein,we report a visible-light-driven radical relay 1,2-perfluoroalkylation aminocarbonylation of unactivated alkenes using CO gas as carbonyl source and 4CzIPN as organic photocatalyst.A wide range of alkenes and amines were well tolerated,providing the valuableβ-perfluoroalkylated amides with generally good yields and high chemoselectivity.
基金financial supports from the National Natural Science Foundation of China(Nos.21772035,22022204,22072167,21202206)Natural Science Foundation of Hunan Province(Nos.2021JJ40147)。
文摘α,β-Unsaturated primary amides are important intermediates and building blocks in organic synthesis.Herein,we report a ligand-free iron-catalyzed hydroaminocarbonylation of alkynes using NH_(4)HCO_(3)as the ammonia source,enabling the highly efficient and regioselective synthesis of linearα,β-unsaturated primary amides.Various aromatic and aliphatic alkynes are transformed into the desired linearα,β-unsaturated primary amides in good to excellent yields.Further studies show that using NH_(4)HCO_(3)as the ammonia source is key to obtain good yields and selectivity.The utility of this route is demonstrated with the synthesis of linearα,β-unsaturated amides including vanilloid receptor-1 antagonist TRPV-1.
文摘The discovery of a rearrangement reaction of 5-amino-1-arylaminocarbonyl-1,2,triazole(pyrszole)to 5-arylureylene-1,2,4-trazole and the mechanism for thisrearrangement reaction are presented. The rearrangement reaction could be attributed to athermodynamic energy preference leading to the predominant formation of 5-aryluretjlene1,2,4-triazole,as shown by molecular mechanics calculation with MMX Program.
基金supported by the National Key R&D Program of China(2021YFA1501100)the National Natural Science Foundation of China(22005007)+1 种基金the New Cornerstone Science Foundation,and Liaoning Binhai Laboratory Project(LBLF-202306)the Tencent Foundation through the XPLORER PRIZE.
文摘A hydrogen storage system was developed via heterogeneous catalysis,employing the dehydrogenative coupling of methanol and N,N′-dimethylethylenediamine to efficiently produce high-purity H_(2).In this process,the Cu/ZnO/Al_(2)O_(3) catalyst displayed superior activity in hydrogen production,with Cu+identified as the major active site through comprehensive characterization.
