The large-scale preparation ofmonolayer two-dimensional(2D)material remains a great challenge,which hinders its real-world applications.Herein,we report a novel layered metal–organic framework(MOF),IPM-1,whichwas syn...The large-scale preparation ofmonolayer two-dimensional(2D)material remains a great challenge,which hinders its real-world applications.Herein,we report a novel layered metal–organic framework(MOF),IPM-1,whichwas synthesized froma cage-like organic linker,with extremely weak interlaminar interaction.When subjected to external disturbance,IPM-1 degenerated into an intermediate state between the crystalline and amorphous phase,in which the layers retain the inplane two-dimensional periodic structure but aremisaligned in the third dimension,leading to the loss of apparent porosity and crystallinity.This amorphous IPM-1 is readily exfoliated at gramscale into crystalline 2D nanosheets with a thickness of 1.15 nm,excellent thickness homogeneity,lateral size up to 10μm,and restored microporosity.IPM-1 nanosheets exhibit high chemical stability and catalytic activity in the oxidation of alcohol,combining the advantages of both homogeneous and heterogeneous catalyst.This work underscores that MOFs without apparent crystallinity can be ideal precursors for the successful preparation of 2D crystalline monolayer nanosheets.展开更多
文摘The large-scale preparation ofmonolayer two-dimensional(2D)material remains a great challenge,which hinders its real-world applications.Herein,we report a novel layered metal–organic framework(MOF),IPM-1,whichwas synthesized froma cage-like organic linker,with extremely weak interlaminar interaction.When subjected to external disturbance,IPM-1 degenerated into an intermediate state between the crystalline and amorphous phase,in which the layers retain the inplane two-dimensional periodic structure but aremisaligned in the third dimension,leading to the loss of apparent porosity and crystallinity.This amorphous IPM-1 is readily exfoliated at gramscale into crystalline 2D nanosheets with a thickness of 1.15 nm,excellent thickness homogeneity,lateral size up to 10μm,and restored microporosity.IPM-1 nanosheets exhibit high chemical stability and catalytic activity in the oxidation of alcohol,combining the advantages of both homogeneous and heterogeneous catalyst.This work underscores that MOFs without apparent crystallinity can be ideal precursors for the successful preparation of 2D crystalline monolayer nanosheets.