【摘 要】
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Copper-hydrides have been intensively studied for a long time due to their utilization in a variety of technologically important chemical transformations.Nevertheless,poor stability of the species severely hinders its isolation,storage and operation,which
【机 构】
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State Key Laboratory for Physical Chemistry of Solid Surfaces,Collaborative Innovation Center of Che
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Copper-hydrides have been intensively studied for a long time due to their utilization in a variety of technologically important chemical transformations.Nevertheless,poor stability of the species severely hinders its isolation,storage and operation,which is worse for nano-sized ones.We report here an unprecedented strategy to access to ultrastable copper-hydride nanoclusters (NCs),namely,using bidentate N-heterocyclic carbenes as stabilizing ligands in addition to thiolates.In this work,a simple synthetic protocol was developed to synthesize the first large copper-hydride nanoclusters (NCs) stabilized by N-heterocyclic carbenes(NHCs).The NC,with the formula of Cu31(RS)25(NHC)3H6 (NHC =1,4-bis(1-benzyl-1H-benzimidazol-1-ium-3-yl) butane,RS =4-fluorothiophenol),was fully characterized by high resolution Fourier transform ion cyclotron resonance mass spectrum,nuclear magnetic resonance,ultra-violet visible spectroscopy,density functional theory (DFT) calculations and single-crystal X-ray crystallography.Structurally,the title cluster exhibits unprecedented Cu4 tetrahedron-based vertex-sharing (TBVS) superstructure(fusion of six Cu4 tetrahedra).Moreover,the ultrahigh thermal stability renders the cluster a model system to highlight the power of NHCs (even other carbenes) in controlling geometrical,electronic and surface structure of polyhydrido copper clusters.
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