Cu(I)-catalyzed azide-alkyne cycloadditions(CuAAC)have gained increasing interest in the selective labeling of living cells and organisms with biomolecules.However,their application is constrained either by the high c...Cu(I)-catalyzed azide-alkyne cycloadditions(CuAAC)have gained increasing interest in the selective labeling of living cells and organisms with biomolecules.However,their application is constrained either by the high cytotoxicity of Cu(I)ions or the low activity of CuAAC in the internal space of living cells.This paper reports the design of a novel Cu-based nanocatalyst,watersoluble thiolated Cu30 nanoclusters(NCs),for living cell labeling via CuAAC.The Cu30 NCs offer good biocompatibility,excellent stability,and scalable synthesis(e.g.,gram scale),which would facilitate potential commercial applications.By combining the highly localized Cu(I)active species on the NC surface and good structural stability,the Cu30 NCs exhibit superior catalytic activities for a series of Huisgen cycloaddition reactions with good recyclability.More importantly,the biocompatibility of the Cu30 NCs enables them to be a good catalyst for CuAAC,whereby the challenging labeling of living cells can be achieved via CuAAC on the cell membrane.This study sheds light on the facile synthesis of atomically precise Cu NCs,as well as the design of novel Cu NCs-based nanocatalysts for CuAAC in intracellular bioorthogonal applications.展开更多
The traditional approach to utilizing an ion-relay mechanism for ion transport requires three or more ion-relay stations.Herein,we describe a novel strategy,incorporating a swing action to realize a minimal ion-relay ...The traditional approach to utilizing an ion-relay mechanism for ion transport requires three or more ion-relay stations.Herein,we describe a novel strategy,incorporating a swing action to realize a minimal ion-relay mechanism via only two relay stations.This swing-relay mechanism was achieved using a class of crown ether-appended,long-armed molecular tetrahedrons(MTs).These MTs comprise ion-relaying crown units attached to a rigid tetrahedral core via flexible alkyl linkers,which act as the mobile arms and endow the crown units with great mobility to swing.展开更多
基金This work was supported by the National Natural Science Foundation of China(No.22071127)Taishan Scholar Foundation(No.tsqn201812074)+1 种基金the Natural Science Foundation of Shandong Province(No.ZR2019YQ07)the NanoBio Lab(IMRE,A*STAR,Singapore).
文摘Cu(I)-catalyzed azide-alkyne cycloadditions(CuAAC)have gained increasing interest in the selective labeling of living cells and organisms with biomolecules.However,their application is constrained either by the high cytotoxicity of Cu(I)ions or the low activity of CuAAC in the internal space of living cells.This paper reports the design of a novel Cu-based nanocatalyst,watersoluble thiolated Cu30 nanoclusters(NCs),for living cell labeling via CuAAC.The Cu30 NCs offer good biocompatibility,excellent stability,and scalable synthesis(e.g.,gram scale),which would facilitate potential commercial applications.By combining the highly localized Cu(I)active species on the NC surface and good structural stability,the Cu30 NCs exhibit superior catalytic activities for a series of Huisgen cycloaddition reactions with good recyclability.More importantly,the biocompatibility of the Cu30 NCs enables them to be a good catalyst for CuAAC,whereby the challenging labeling of living cells can be achieved via CuAAC on the cell membrane.This study sheds light on the facile synthesis of atomically precise Cu NCs,as well as the design of novel Cu NCs-based nanocatalysts for CuAAC in intracellular bioorthogonal applications.
基金Northwestern Polytechnical University and the NanoBio Lab(Biomedical Research Council,Agency for Science,Technology,and Research).
文摘The traditional approach to utilizing an ion-relay mechanism for ion transport requires three or more ion-relay stations.Herein,we describe a novel strategy,incorporating a swing action to realize a minimal ion-relay mechanism via only two relay stations.This swing-relay mechanism was achieved using a class of crown ether-appended,long-armed molecular tetrahedrons(MTs).These MTs comprise ion-relaying crown units attached to a rigid tetrahedral core via flexible alkyl linkers,which act as the mobile arms and endow the crown units with great mobility to swing.
