Tetralin-1-carboxamides are frequently incorporated in myriad medicinally important molecules.However,their existing synthetic routes not only suffer from some drawbacks such as tedious procedures,harsh reaction condi...Tetralin-1-carboxamides are frequently incorporated in myriad medicinally important molecules.However,their existing synthetic routes not only suffer from some drawbacks such as tedious procedures,harsh reaction conditions,narrow substrate scope,low yields,and environmental problems,but are also based upon the elaboration of uneasily available non-linear tetralin derivatives.Herein,we describe a metal-and additive-free visible light-induced[4+2]annulation of two simple linear starting materials,namely acrylamides and 2-benzyl-2-bromocarbonyls,through a cascade C(sp^(3))-Br/C(sp^(2))-H bond cleavage,double C-C bond formation,and aromatization sequence.The developed protocol provides a convenient,efficient,and green approach to a variety of tetralin-1-carboxamide derivatives with good functional group compatibility.Importantly,the resulting products could also undergo the Licl-mediated mono-decarboxylative cyclization process to further furnish the architecturally novel bridged polycyclic imides with excellentcis-diastereoselectivities.展开更多
As one of the most common structural motifs in natural products,cyclopentenones usually can be fabricated by Nazarov cyclization using divinyl ketones or functionalized tertiary divinyl carbinols(TDCs)as substrates.Ho...As one of the most common structural motifs in natural products,cyclopentenones usually can be fabricated by Nazarov cyclization using divinyl ketones or functionalized tertiary divinyl carbinols(TDCs)as substrates.However,straightforward method for transforming unfunctionalized TDCs to their corresponding cyclopentenones is currently lacking.Herein,we wish to report the total syntheses of four structurally distinct terpenoids,namely laurane-type marine sesquiterpenoids isolaurene,debromoaplysin and aplysin,and guaiane sesquiterpenoid guaiadienone A,all using a novel synthetic method,named oxidative Nazarov cyclization,as the key step.This work demonstrated our robust method is suitable for synthesizing various highly substituted cyclopentenones.展开更多
Single-atom catalysts (SACs) have garnered extensive attention in the field of catalysis due to their exceptional inherent reaction activity, optimal utilization of metal atoms, etc. Controlled synthesis plays a cruci...Single-atom catalysts (SACs) have garnered extensive attention in the field of catalysis due to their exceptional inherent reaction activity, optimal utilization of metal atoms, etc. Controlled synthesis plays a crucial role in elucidating the structure-activity relationship of SACs. This paper reviews various synthetic strategies for SACs, encompassing defect engineering, metal-organic frameworks (MOFs) pyrolysis, and ion exchange. With specific examples, the significance of constructing catalysts at the atomic level is discussed, aiming to comprehensively understand the synthetic strategies of SACs. Finally, it addresses the challenges and prospects associated with controlled synthesis techniques for SACs as well as their future applications.展开更多
基金supported by the National Natural Science Foundation of China(Nos.22101237,22171233)the Science and Technology Program of Sichuan Province(Nos.2022YFS0608,2022NSFSC1219)+1 种基金the Open Project Program of Nuclear Medicine and Molecular Imaging Key Laboratory of Sichuan Province(Nos.HYX21003,HYX22008)the research fund of Southwest Medical University(2021ZKMS042).
文摘Tetralin-1-carboxamides are frequently incorporated in myriad medicinally important molecules.However,their existing synthetic routes not only suffer from some drawbacks such as tedious procedures,harsh reaction conditions,narrow substrate scope,low yields,and environmental problems,but are also based upon the elaboration of uneasily available non-linear tetralin derivatives.Herein,we describe a metal-and additive-free visible light-induced[4+2]annulation of two simple linear starting materials,namely acrylamides and 2-benzyl-2-bromocarbonyls,through a cascade C(sp^(3))-Br/C(sp^(2))-H bond cleavage,double C-C bond formation,and aromatization sequence.The developed protocol provides a convenient,efficient,and green approach to a variety of tetralin-1-carboxamide derivatives with good functional group compatibility.Importantly,the resulting products could also undergo the Licl-mediated mono-decarboxylative cyclization process to further furnish the architecturally novel bridged polycyclic imides with excellentcis-diastereoselectivities.
基金support from the National Natural Science Foundation of China(Nos.21971104,22001114 and 22271136)Shenzhen Science,Technology and Innovation Commission(JCYJ20220814203252001)+5 种基金Shenzhen Key Laboratory of Small Molecule Drug Discovery and Synthesis(ZDSYS20190902093215877)Guangdong Provincial Key Laboratory of Catalysis(No.2020B121201002)Guangdong Innovative Program(No.2019BT02Y335)Education Department of Guangdong Province,Key Research Projects in Colleges and Universities in Guangdong Province(2021ZDZX2035)Shenzhen Nobel Prize Scientists Laboratory Project(C17783101),Innovative Team of Universities in Guangdong Province(2020KCXTD016)Guangdong Natural Science Foundation(2022A1515010456)is greatly appreciated.
文摘As one of the most common structural motifs in natural products,cyclopentenones usually can be fabricated by Nazarov cyclization using divinyl ketones or functionalized tertiary divinyl carbinols(TDCs)as substrates.However,straightforward method for transforming unfunctionalized TDCs to their corresponding cyclopentenones is currently lacking.Herein,we wish to report the total syntheses of four structurally distinct terpenoids,namely laurane-type marine sesquiterpenoids isolaurene,debromoaplysin and aplysin,and guaiane sesquiterpenoid guaiadienone A,all using a novel synthetic method,named oxidative Nazarov cyclization,as the key step.This work demonstrated our robust method is suitable for synthesizing various highly substituted cyclopentenones.
基金This work was supported by the National Natural Science Foundation of China(No.52172208)the Taishan Scholar Young Talent Program,China(No.tsqn202306216)the Taishan Scholar Talent Program,China(No.ts20190402).
文摘Single-atom catalysts (SACs) have garnered extensive attention in the field of catalysis due to their exceptional inherent reaction activity, optimal utilization of metal atoms, etc. Controlled synthesis plays a crucial role in elucidating the structure-activity relationship of SACs. This paper reviews various synthetic strategies for SACs, encompassing defect engineering, metal-organic frameworks (MOFs) pyrolysis, and ion exchange. With specific examples, the significance of constructing catalysts at the atomic level is discussed, aiming to comprehensively understand the synthetic strategies of SACs. Finally, it addresses the challenges and prospects associated with controlled synthesis techniques for SACs as well as their future applications.
