A heteropore covalent organic framework(COF) integrating tetraphenylethene skeleton and catechol segment is designed and synthesized.It exhibits extremely high stability in water under different pH conditions,which ma...A heteropore covalent organic framework(COF) integrating tetraphenylethene skeleton and catechol segment is designed and synthesized.It exhibits extremely high stability in water under different pH conditions,which makes it an excellent material for adsorptive removal of Cd(Ⅱ) from aqueous solutions with very fast adsorption kinetics,high uptake capacity,and good recyclability.展开更多
Constructing two-dimensional(2D)supramolecular polymers with complicated hierarchical porosity significantly contributes to developing effective strategies to control delicate self-assembly architectures,thus facilita...Constructing two-dimensional(2D)supramolecular polymers with complicated hierarchical porosity significantly contributes to developing effective strategies to control delicate self-assembly architectures,thus facilitating the fabrication of advanced 2D organic functional materials.Here,we report utilizing cooperative cation-πand electrostatic interactions to construct a series of robust 2D heteropore supramolecular polymers(2D HPSPs)with hierarchical pore structures,in which hexagonal and rectangular pores are alternately and periodically arranged,and the pore sizes can be finely tuned.Remarkably,the as-prepared 2D HPSPs exhibit excellent iodine(I_(2))capture rate(a maximum K80%value is 2.25 g h^(-1)),and present a novel mechanism involving transport-adsorption spatiotemporal separation for rapid I_(2)capture.In this mechanism,the transport of free I_(2)is first conducted in large hexagonal pores,and then I_(2)can be preferentially adsorbed in small rectangular pores,thereby preventing the transfer channels from blocking and greatly improving the adsorption kinetics.展开更多
Designing metal covalent organic frameworks(MCOFs)to enhance ion transport and catalysis remains a significant challenge.In this study,a metal single crystal named Bpy-Cu is presynthesized,and subsequently a heteropor...Designing metal covalent organic frameworks(MCOFs)to enhance ion transport and catalysis remains a significant challenge.In this study,a metal single crystal named Bpy-Cu is presynthesized,and subsequently a heteroporous MCOF(Bpy-COF-Cu)is obtained directly by amulticomponent reaction.This approach avoids potential defects associated with postmodification methods and enables more controllable metal loading.Moreover,the structural properties of the framework position the metal catalytic sites uniformly distributed near two mesopores,significantly enhancing the photoelectric performance of imine-linked COFs and enabling synergistic ion transport and catalysis.As a result,Bpy-COF-Cu exhibits ultrafast photocatalytic uranium reduction with a rate constant(k)of 0.063 min^(−1) without requiring sacrificial reagents.This system achieves exceptionally high removal rates(>99%)in uraniumcontaining mine wastewater samples due to the recyclable catalysis metal sites.This strategy provides an innovative approach towards designing structurally complex MCOFs.展开更多
基金National Natural Science Foundation of China(No.21725404)Shanghai Scientific and Technological Innovation Project(No.18JC1410600)the Strategic Priority Research Program of the Chinese Academy of Sciences(No.XDB20000000)financial support。
文摘A heteropore covalent organic framework(COF) integrating tetraphenylethene skeleton and catechol segment is designed and synthesized.It exhibits extremely high stability in water under different pH conditions,which makes it an excellent material for adsorptive removal of Cd(Ⅱ) from aqueous solutions with very fast adsorption kinetics,high uptake capacity,and good recyclability.
基金supported by the National Natural Science Foundation of China(22022107,22071197)
文摘Constructing two-dimensional(2D)supramolecular polymers with complicated hierarchical porosity significantly contributes to developing effective strategies to control delicate self-assembly architectures,thus facilitating the fabrication of advanced 2D organic functional materials.Here,we report utilizing cooperative cation-πand electrostatic interactions to construct a series of robust 2D heteropore supramolecular polymers(2D HPSPs)with hierarchical pore structures,in which hexagonal and rectangular pores are alternately and periodically arranged,and the pore sizes can be finely tuned.Remarkably,the as-prepared 2D HPSPs exhibit excellent iodine(I_(2))capture rate(a maximum K80%value is 2.25 g h^(-1)),and present a novel mechanism involving transport-adsorption spatiotemporal separation for rapid I_(2)capture.In this mechanism,the transport of free I_(2)is first conducted in large hexagonal pores,and then I_(2)can be preferentially adsorbed in small rectangular pores,thereby preventing the transfer channels from blocking and greatly improving the adsorption kinetics.
基金support from the National Natural Science Foundation of China(grant nos.22036003,22176082,and 22376023)Natural Science Foundation of Jiangxi Province(grant no.20232BBE50031)Research Innovation Program for College Graduates of Jiangxi Province(grant no.YC2023-B019).
文摘Designing metal covalent organic frameworks(MCOFs)to enhance ion transport and catalysis remains a significant challenge.In this study,a metal single crystal named Bpy-Cu is presynthesized,and subsequently a heteroporous MCOF(Bpy-COF-Cu)is obtained directly by amulticomponent reaction.This approach avoids potential defects associated with postmodification methods and enables more controllable metal loading.Moreover,the structural properties of the framework position the metal catalytic sites uniformly distributed near two mesopores,significantly enhancing the photoelectric performance of imine-linked COFs and enabling synergistic ion transport and catalysis.As a result,Bpy-COF-Cu exhibits ultrafast photocatalytic uranium reduction with a rate constant(k)of 0.063 min^(−1) without requiring sacrificial reagents.This system achieves exceptionally high removal rates(>99%)in uraniumcontaining mine wastewater samples due to the recyclable catalysis metal sites.This strategy provides an innovative approach towards designing structurally complex MCOFs.