The two-electron oxygen reduction reaction(ORR)for H_(2)O_(2) photosynthesis is often hindered by sluggish charge kinetics and a limited number of activation sites.Theoretical predictions based on dipole moment analys...The two-electron oxygen reduction reaction(ORR)for H_(2)O_(2) photosynthesis is often hindered by sluggish charge kinetics and a limited number of activation sites.Theoretical predictions based on dipole moment analysis indicate that introducing pyrazine units enhances charge migration,leading to increased accumulation of photoinduced electrons on these units,thereby facilitating the two-site,two-electron ORR.Inspired by these theoretical insights,this work designed and fabricated a triazine-pyrazine-based covalent organic framework materials(TTDN-COFs)for H_(2)O_(2) photosynthesis via a polarity-functionalization strategy.The TTDN-COFs demonstrate a significant improvement in the photocatalytic H_(2)O_(2) production rate,reaching 2757.6μmol h^(-1) g^(-1) in pure water–3.2 times higher than that of the triazine-based COFs(TTPH-COFs).Experimental results and theoretical calculations confirm that the incorporation of pyrazine units not only enhances polarization,promoting the separation and migration of charge carriers,but also facilitates the formation of endoperoxide at both the triazine and pyrazine units.The dual adsorption activation sites lower the activation energy barrier for O_(2),thereby accelerating the overall reaction kinetics.These findings highlight the potential of functional-group-mediated polarization engineering as a promising strategy for developing COFs-based H_(2)O_(2) photosynthesis with dual activation sites.展开更多
Two-dimensional covalent organic frameworks(COFs)with specific morphologies including nanofibers and nanoplates are highly desired in both nanoscience research and practical applications.Thus far,however,morphology en...Two-dimensional covalent organic frameworks(COFs)with specific morphologies including nanofibers and nanoplates are highly desired in both nanoscience research and practical applications.Thus far,however,morphology engineering for COFs remains challenging because the mechanism underlying the morphology formation and evolution of COFs is not well understood.Herein,we propose a strategy of surfactant mediation coupled with acid adjustment to engineer the morphology of aβ-ketoenamine-linked COF,TpPa,during solvothermal synthesis.The surfactants function as stabilizers that can encapsulate monomers and prepolymers to create micelles,enabling the formation of fiber-like and plate-like morphologies of TpPa rather than irregularly shaped aggregates.It is also found that acetic acid is important in regulating such morphologies,as the amino groups inside the prepolymers can be precisely protonated by acid adjustment,leading to an inhibited ripening process for the creation of specific morphologies.Benefitting from the synergistic enhancement of surfactant mediation and acid adjustment,TpPa nanofibers with a diameter down to~20 nm along with a length of up to a few microns and TpPa nanoplates with a thickness of~18 nm are created.Our work sheds light on the mechanism underlying the morphology formation and evolution of TpPa,providing some guidance for exquisite control over the growth of COFs,which is of great significance for their practical applications.展开更多
Metal-free carbon catalysts with excellent conduction performance have drawn much research attention in reduction reactions.Herein,a N,B co-doped carbon catalyst with high pyrrolic N proportion(35.75%)and excellent su...Metal-free carbon catalysts with excellent conduction performance have drawn much research attention in reduction reactions.Herein,a N,B co-doped carbon catalyst with high pyrrolic N proportion(35.75%)and excellent surface area(1409 m^(2)/g)was successfully prepared via carbonizing covalent organic framework materials(COFs)containing N and B atoms assisted by ZnCl_(2)molten salt.The presence of ZnCl_(2)maintains the micropore structure of COFs to provide high specific surface areas and abundant lattice defects for carbon materials.In addition,electron-withdrawing B heteroatom further facilitates the formation of pyrrolic N at defect sites by modifying the electronic structure of carbon network.The tuning of surface areas and active N species in carbon catalysts successfully improve the selective hydrogenation of nitrobenzene to aniline.The optimized carbon material exhibits excellent nitrobenzene conversion(99.9%)and aniline selectivity(>99%)within 15 min,as well as excellent substrate suitability.This work provides a certain guiding for the design and application of metal-free catalysis.展开更多
Covalent organic frameworks(COFs)are an emerging class of photoactive materials,solely composed of light elements.Their ordered structure,crystallinity,and high porosity led to enormous worldwide attention in many res...Covalent organic frameworks(COFs)are an emerging class of photoactive materials,solely composed of light elements.Their ordered structure,crystallinity,and high porosity led to enormous worldwide attention in many research fields.The extensiveπ-electron conjugation,light-harvesting and charge transport characteristics make them a fascinating polymer for photocatalytic systems.Versatile selection of building blocks and innumerable synthetic methodologies enable them to be a robust platform for solar energy production.In this mini-review,we summarized recent progress and challenges of the design,construction,and applications of COFs-based photocatalysts,and also presented some perspectives on challenges.展开更多
Covalent organic frameworks(COFs)are an emerging class of porous crystalline materials formed by the precise assembly of organic molecular building blocks into extended periodic structures via strong covalent bonds.Th...Covalent organic frameworks(COFs)are an emerging class of porous crystalline materials formed by the precise assembly of organic molecular building blocks into extended periodic structures via strong covalent bonds.They feature well-defined pore structure,high specific surface area,and tunable physicochemical properties,endowing them with broad application prospects in gas storage,molecular separation.展开更多
Traditional fossil fuels significantly contribute to energy supply,economic development,and advancements in science and technology.However,prolonged and extensive use of fossil fuels has resulted in increasingly sever...Traditional fossil fuels significantly contribute to energy supply,economic development,and advancements in science and technology.However,prolonged and extensive use of fossil fuels has resulted in increasingly severe environmental pollution.Consequently,it is imperative to develop new,clean,and pollution-free energy sources with high energy density and versatility as substitutes for conventional fossil fuels,although this remains a considerable challenge.Simultaneously,addressing water pollution is a critical concern.The development,design,and optimization of functional nanomaterials are pivotal to advancing new energy solutions and pollutant remediation.Emerging porous framework materials such as metal-organic frameworks(MOFs)and covalent organic frameworks(COFs),recognized as exemplary crystalline porous materials,exhibit potential in energy and environmental applications due to their high specific surface area,adjustable pore sizes and structures,permanent porosity,and customizable functionalities.This work provides a comprehensive and systematic review of the applications of MOFs,COFs,and their derivatives in emerging energy technologies,including the oxygen reduction reaction,oxygen evolution reaction,hydrogen evolution reaction,lithium-ion batteries,and environmental pollution remediation such as the carbon dioxide reduction reaction and environmental pollution management.In addition,strategies for performance adjustment and the structure-effect relationships of MOFs,COFs,and their derivatives for these applications are explored.Interaction mechanisms are summarized based on experimental discussions,theoretical calculations,and advanced spectroscopy analyses.The challenges,future prospects,and opportunities for tailoring these materials for energy and environmental applications are presented.展开更多
MXenes,a class of two-dimensional(2D)transition metal carbides,and covalent organic frameworks(COFs)deliver unique structural and electrochemical properties,making them promising candidates for energy storage and conv...MXenes,a class of two-dimensional(2D)transition metal carbides,and covalent organic frameworks(COFs)deliver unique structural and electrochemical properties,making them promising candidates for energy storage and conversion applications.MXenes exhibit excellent conductivity and tunable surface chemistries,whereas the COFs provide high porosity and structural versatility.Recent advances in integrating MXene-COF composites have revealed their potential to enhance charge transfer and energy storage/conversion properties.The work highlights key developments in MXene-COF integration,offering insights into their applications in batteries(Li-ion,K-ion,Na-ion,and Li-S),supercapacitors,and electrocatalysis(HER,OER,RR,NRR,and ORRCO2),while also addressing current challenges and future directions for not only energy conversion but also other electronic devices.展开更多
Fabricating macroscale smart actuators that can convert light energy into other forms of energy,especially mechanical and electrical energy,is of great significance.Herein,a simple and efficient 4D printed method for ...Fabricating macroscale smart actuators that can convert light energy into other forms of energy,especially mechanical and electrical energy,is of great significance.Herein,a simple and efficient 4D printed method for fabricating photomechanical actuators based on micro/nano-scale crystals is developed.The high versatility and generality of this method are successfully demonstrated using nine different types of photoresponsive crystalline actuators,including acylhydrazone-,anthracene-,olefin-,and azobenzene-based molecular crystals and covalent organic frameworks(COFs).The low-cost neutral silicone sealant elastomer is first chosen as the photomechanical 4D printing matrix.Notably,these actuators can be used to perform bionic motions(the first windmills spin using crystalline material,dragonflies fly,and sunflowers bloom)under the stimulation of visible light and can realize energy conversion from mechanical energy into electricity when coupled with a piezoelectric membrane.This work provides new insights into the design and manufacturing of smart photomechanical actuators and electricity generators and expands the application scope of COFs.展开更多
Photoelectrochemical CO_(2)reduction to multi-carbon products fuels remains challenged by inefficient C–C coupling and competing proton reduction reaction.Herein,we designed a cationic covalent organic framework(COF+...Photoelectrochemical CO_(2)reduction to multi-carbon products fuels remains challenged by inefficient C–C coupling and competing proton reduction reaction.Herein,we designed a cationic covalent organic framework(COF+)to create an electrostatic microenvironment that synergizes with CuPt alloy nanoparticles for selective ethylene/ethane production.By spatially decoupling CO_(2)enrichment from proton exclusion,the COF^(+)/CuPt interface simultaneously facilitates CO_(2)accessibility while impeding H+migration,suppressing the hydrogen evolution reaction(HER).This unique microenvironment stabilizes key anionic intermediates(*COO^(−),*OCCO^(−))and promotes*CO dimerization,steering electron transfer toward C–C coupling.The optimized system achieves a record-high Faradaic efficiency of 51.5%±5.3%for ethane and 10.6%±2.5%for ethylene with a total C2+yield exceeding 62%at−0.25 V vs.RHE and high stability(>300 min),representing the highest performance for photoelectrochemical CO_(2)reduction to ethane.The combined analyses of in situ spectroscopy and theoretical calculations reveal that electrostatic field effects lower the energy barrier for*OCCO formation while accelerating hydrogenation kinetics.Therefore,this work demonstrates that microenvironment modification of the active site by cationic covalent organic framework is a versatile strategy for solar-driven CO_(2)conversion into value-added hydrocarbons.展开更多
In the past decades,metal-organic frameworks(MOFs)and covalent organic frameworks(COFs)basically enjoy the coordination chemistry and covalent chemistry,respectively,and such uniqueness has become the major obstacle h...In the past decades,metal-organic frameworks(MOFs)and covalent organic frameworks(COFs)basically enjoy the coordination chemistry and covalent chemistry,respectively,and such uniqueness has become the major obstacle hampering their further scope diversity and application multi-functionalization.Inspired from the principle of organic retrosynthesis,combining coordination bond and covalent bond together offers additional opportunities for constructing novel MOFs,COFs and MOF@COF hybrids as well as confer on them superior performances in versatile application fields.In this review,we firstly classify and summarize the recently reported synthesis strategies based on the integration of metal-ligand coordination and dynamic covalent bonds.Then,the application performances of as-constructed MOFs,COFs as well as MOF@COF hybrids are discussed and highlighted in the fields of adsorption,separation,catalysis,biosensing,energy storage and so on.Last,our personal insights of the remaining challenges and further prospects are also provided,in order to trigger much more inspirations and endeavors for this hot research field.展开更多
The lack of macro-continuity and mechanical strength of covalent organic frameworks(COFs)has significantly limited their practical applications.Here,we propose an“alcohol-triggered defect cleavage”strategy to precis...The lack of macro-continuity and mechanical strength of covalent organic frameworks(COFs)has significantly limited their practical applications.Here,we propose an“alcohol-triggered defect cleavage”strategy to precisely regulate the growth and stacking of COF grains through a moderate reversed Schiff base reaction,realizing the direct synthesis of COF nanofibers(CNFs)with high aspect ratio(L/D=103.05)and long length(>20μm).An individual CNF exhibits a biomimetic scale-like architecture,achieving superior flexibility and fatigue resistance under dynamic bending via a multiscale stress dissipation mechanism.Taking advantages of these structural features,we engineer CNF aerogels(CNF-As)with programmable porous structures(e.g.,honeycomb,lamellar,isotropic)via directional ice-template methodology.CNF-As demonstrate 100%COF content,high specific surface area(396.15 m^(2)g^(-1))and superelasticity(~0%elastic deformation after 500 compression cycles at 50%strain),outperforming most COF-based counterparts.Compared with the conventional COF aerogels,the unique structural features of CNF-A enable it to perform outstandingly in uranium extraction,with an 11.72-fold increment in adsorption capacity(920.12 mg g^(-1))and adsorption rate(89.9%),and a 2.48-fold improvement in selectivity(U/V=2.31).This study provides a direct strategy for the development of next-generation COF materials with outstanding functionality and structural robustness.展开更多
文摘The two-electron oxygen reduction reaction(ORR)for H_(2)O_(2) photosynthesis is often hindered by sluggish charge kinetics and a limited number of activation sites.Theoretical predictions based on dipole moment analysis indicate that introducing pyrazine units enhances charge migration,leading to increased accumulation of photoinduced electrons on these units,thereby facilitating the two-site,two-electron ORR.Inspired by these theoretical insights,this work designed and fabricated a triazine-pyrazine-based covalent organic framework materials(TTDN-COFs)for H_(2)O_(2) photosynthesis via a polarity-functionalization strategy.The TTDN-COFs demonstrate a significant improvement in the photocatalytic H_(2)O_(2) production rate,reaching 2757.6μmol h^(-1) g^(-1) in pure water–3.2 times higher than that of the triazine-based COFs(TTPH-COFs).Experimental results and theoretical calculations confirm that the incorporation of pyrazine units not only enhances polarization,promoting the separation and migration of charge carriers,but also facilitates the formation of endoperoxide at both the triazine and pyrazine units.The dual adsorption activation sites lower the activation energy barrier for O_(2),thereby accelerating the overall reaction kinetics.These findings highlight the potential of functional-group-mediated polarization engineering as a promising strategy for developing COFs-based H_(2)O_(2) photosynthesis with dual activation sites.
基金the National Natural Science Foundation of China(No.21921006).
文摘Two-dimensional covalent organic frameworks(COFs)with specific morphologies including nanofibers and nanoplates are highly desired in both nanoscience research and practical applications.Thus far,however,morphology engineering for COFs remains challenging because the mechanism underlying the morphology formation and evolution of COFs is not well understood.Herein,we propose a strategy of surfactant mediation coupled with acid adjustment to engineer the morphology of aβ-ketoenamine-linked COF,TpPa,during solvothermal synthesis.The surfactants function as stabilizers that can encapsulate monomers and prepolymers to create micelles,enabling the formation of fiber-like and plate-like morphologies of TpPa rather than irregularly shaped aggregates.It is also found that acetic acid is important in regulating such morphologies,as the amino groups inside the prepolymers can be precisely protonated by acid adjustment,leading to an inhibited ripening process for the creation of specific morphologies.Benefitting from the synergistic enhancement of surfactant mediation and acid adjustment,TpPa nanofibers with a diameter down to~20 nm along with a length of up to a few microns and TpPa nanoplates with a thickness of~18 nm are created.Our work sheds light on the mechanism underlying the morphology formation and evolution of TpPa,providing some guidance for exquisite control over the growth of COFs,which is of great significance for their practical applications.
基金National Natural Science Foundation of China(Nos.21776129 and 21706121)Natural Science Foundation of Jiangsu Province(No.BK20170995)+1 种基金Postgraduate Research&Practice Innovation Program of Jiangsu Province(No.KYCX211171)the Project of Priority Academic Program Development of Jiangsu Higher Education Institutions(PAPD)。
文摘Metal-free carbon catalysts with excellent conduction performance have drawn much research attention in reduction reactions.Herein,a N,B co-doped carbon catalyst with high pyrrolic N proportion(35.75%)and excellent surface area(1409 m^(2)/g)was successfully prepared via carbonizing covalent organic framework materials(COFs)containing N and B atoms assisted by ZnCl_(2)molten salt.The presence of ZnCl_(2)maintains the micropore structure of COFs to provide high specific surface areas and abundant lattice defects for carbon materials.In addition,electron-withdrawing B heteroatom further facilitates the formation of pyrrolic N at defect sites by modifying the electronic structure of carbon network.The tuning of surface areas and active N species in carbon catalysts successfully improve the selective hydrogenation of nitrobenzene to aniline.The optimized carbon material exhibits excellent nitrobenzene conversion(99.9%)and aniline selectivity(>99%)within 15 min,as well as excellent substrate suitability.This work provides a certain guiding for the design and application of metal-free catalysis.
基金This work was financially supported by the National Natural Science Foundation of China(No.21975086)the International S&T Cooperation Program of China(No.2018YFE010498)+2 种基金the HUST Innovation Funding(No.2018JYCXJJ041)Science and Technology Department of Hubei Province(Nos.2019CFA008 and 2018AAA057)the Program for HUST Interdisciplinary Innovation Team(No.2016JCTD104).
文摘Covalent organic frameworks(COFs)are an emerging class of photoactive materials,solely composed of light elements.Their ordered structure,crystallinity,and high porosity led to enormous worldwide attention in many research fields.The extensiveπ-electron conjugation,light-harvesting and charge transport characteristics make them a fascinating polymer for photocatalytic systems.Versatile selection of building blocks and innumerable synthetic methodologies enable them to be a robust platform for solar energy production.In this mini-review,we summarized recent progress and challenges of the design,construction,and applications of COFs-based photocatalysts,and also presented some perspectives on challenges.
文摘Covalent organic frameworks(COFs)are an emerging class of porous crystalline materials formed by the precise assembly of organic molecular building blocks into extended periodic structures via strong covalent bonds.They feature well-defined pore structure,high specific surface area,and tunable physicochemical properties,endowing them with broad application prospects in gas storage,molecular separation.
基金supported by the National Natural Science Foundation of China(22327807,U2067215,U2341289,22341602,22006036,U2167218,22276054).
文摘Traditional fossil fuels significantly contribute to energy supply,economic development,and advancements in science and technology.However,prolonged and extensive use of fossil fuels has resulted in increasingly severe environmental pollution.Consequently,it is imperative to develop new,clean,and pollution-free energy sources with high energy density and versatility as substitutes for conventional fossil fuels,although this remains a considerable challenge.Simultaneously,addressing water pollution is a critical concern.The development,design,and optimization of functional nanomaterials are pivotal to advancing new energy solutions and pollutant remediation.Emerging porous framework materials such as metal-organic frameworks(MOFs)and covalent organic frameworks(COFs),recognized as exemplary crystalline porous materials,exhibit potential in energy and environmental applications due to their high specific surface area,adjustable pore sizes and structures,permanent porosity,and customizable functionalities.This work provides a comprehensive and systematic review of the applications of MOFs,COFs,and their derivatives in emerging energy technologies,including the oxygen reduction reaction,oxygen evolution reaction,hydrogen evolution reaction,lithium-ion batteries,and environmental pollution remediation such as the carbon dioxide reduction reaction and environmental pollution management.In addition,strategies for performance adjustment and the structure-effect relationships of MOFs,COFs,and their derivatives for these applications are explored.Interaction mechanisms are summarized based on experimental discussions,theoretical calculations,and advanced spectroscopy analyses.The challenges,future prospects,and opportunities for tailoring these materials for energy and environmental applications are presented.
基金Hong Kong Innovation and Technology Commission,Grant/Award Number:GHP/247/22GD。
文摘MXenes,a class of two-dimensional(2D)transition metal carbides,and covalent organic frameworks(COFs)deliver unique structural and electrochemical properties,making them promising candidates for energy storage and conversion applications.MXenes exhibit excellent conductivity and tunable surface chemistries,whereas the COFs provide high porosity and structural versatility.Recent advances in integrating MXene-COF composites have revealed their potential to enhance charge transfer and energy storage/conversion properties.The work highlights key developments in MXene-COF integration,offering insights into their applications in batteries(Li-ion,K-ion,Na-ion,and Li-S),supercapacitors,and electrocatalysis(HER,OER,RR,NRR,and ORRCO2),while also addressing current challenges and future directions for not only energy conversion but also other electronic devices.
基金the National Natural Science Foundation of China(22175099,22205116,22301147)National Key Research and Development Program of China(2021YFC2102100)+1 种基金Frontiers Science Center for New Organic Matter of Nankai University(63181206)111 Project(B12015).
文摘Fabricating macroscale smart actuators that can convert light energy into other forms of energy,especially mechanical and electrical energy,is of great significance.Herein,a simple and efficient 4D printed method for fabricating photomechanical actuators based on micro/nano-scale crystals is developed.The high versatility and generality of this method are successfully demonstrated using nine different types of photoresponsive crystalline actuators,including acylhydrazone-,anthracene-,olefin-,and azobenzene-based molecular crystals and covalent organic frameworks(COFs).The low-cost neutral silicone sealant elastomer is first chosen as the photomechanical 4D printing matrix.Notably,these actuators can be used to perform bionic motions(the first windmills spin using crystalline material,dragonflies fly,and sunflowers bloom)under the stimulation of visible light and can realize energy conversion from mechanical energy into electricity when coupled with a piezoelectric membrane.This work provides new insights into the design and manufacturing of smart photomechanical actuators and electricity generators and expands the application scope of COFs.
基金financial support from the National Natural Science Foundation of China(No.52273187)the Guangdong Basic and Applied Basic Research Foundation(2022A1515110372,2023A1515011306,2023A1515240077)+1 种基金the National Key Research and Development Program of China(2022YFA1502900)the Guangdong-Hong Kong Joint Laboratory for Preparation and Application of Ordered Structural Materials of Guangdong Province(2023B1212120011).
文摘Photoelectrochemical CO_(2)reduction to multi-carbon products fuels remains challenged by inefficient C–C coupling and competing proton reduction reaction.Herein,we designed a cationic covalent organic framework(COF+)to create an electrostatic microenvironment that synergizes with CuPt alloy nanoparticles for selective ethylene/ethane production.By spatially decoupling CO_(2)enrichment from proton exclusion,the COF^(+)/CuPt interface simultaneously facilitates CO_(2)accessibility while impeding H+migration,suppressing the hydrogen evolution reaction(HER).This unique microenvironment stabilizes key anionic intermediates(*COO^(−),*OCCO^(−))and promotes*CO dimerization,steering electron transfer toward C–C coupling.The optimized system achieves a record-high Faradaic efficiency of 51.5%±5.3%for ethane and 10.6%±2.5%for ethylene with a total C2+yield exceeding 62%at−0.25 V vs.RHE and high stability(>300 min),representing the highest performance for photoelectrochemical CO_(2)reduction to ethane.The combined analyses of in situ spectroscopy and theoretical calculations reveal that electrostatic field effects lower the energy barrier for*OCCO formation while accelerating hydrogenation kinetics.Therefore,this work demonstrates that microenvironment modification of the active site by cationic covalent organic framework is a versatile strategy for solar-driven CO_(2)conversion into value-added hydrocarbons.
基金This work was supported by the National Natural Science Foundation of China(Nos.21905195 and 22103055)the Natural Science Foundation of Tianjin City(No.20JCYBJC00800)PEIYANG Young Scholars Program of Tianjin University(No.2020XRX-0023).
文摘In the past decades,metal-organic frameworks(MOFs)and covalent organic frameworks(COFs)basically enjoy the coordination chemistry and covalent chemistry,respectively,and such uniqueness has become the major obstacle hampering their further scope diversity and application multi-functionalization.Inspired from the principle of organic retrosynthesis,combining coordination bond and covalent bond together offers additional opportunities for constructing novel MOFs,COFs and MOF@COF hybrids as well as confer on them superior performances in versatile application fields.In this review,we firstly classify and summarize the recently reported synthesis strategies based on the integration of metal-ligand coordination and dynamic covalent bonds.Then,the application performances of as-constructed MOFs,COFs as well as MOF@COF hybrids are discussed and highlighted in the fields of adsorption,separation,catalysis,biosensing,energy storage and so on.Last,our personal insights of the remaining challenges and further prospects are also provided,in order to trigger much more inspirations and endeavors for this hot research field.
基金supported by the National Natural Science Foundation of China(No.52403035)the Shanghai Sailing Program(23YF1400300)+1 种基金the Fundamental Research Funds for the Central Universities(2232023D-05)the Weiqiao Teaching and Research Innovation Program.
文摘The lack of macro-continuity and mechanical strength of covalent organic frameworks(COFs)has significantly limited their practical applications.Here,we propose an“alcohol-triggered defect cleavage”strategy to precisely regulate the growth and stacking of COF grains through a moderate reversed Schiff base reaction,realizing the direct synthesis of COF nanofibers(CNFs)with high aspect ratio(L/D=103.05)and long length(>20μm).An individual CNF exhibits a biomimetic scale-like architecture,achieving superior flexibility and fatigue resistance under dynamic bending via a multiscale stress dissipation mechanism.Taking advantages of these structural features,we engineer CNF aerogels(CNF-As)with programmable porous structures(e.g.,honeycomb,lamellar,isotropic)via directional ice-template methodology.CNF-As demonstrate 100%COF content,high specific surface area(396.15 m^(2)g^(-1))and superelasticity(~0%elastic deformation after 500 compression cycles at 50%strain),outperforming most COF-based counterparts.Compared with the conventional COF aerogels,the unique structural features of CNF-A enable it to perform outstandingly in uranium extraction,with an 11.72-fold increment in adsorption capacity(920.12 mg g^(-1))and adsorption rate(89.9%),and a 2.48-fold improvement in selectivity(U/V=2.31).This study provides a direct strategy for the development of next-generation COF materials with outstanding functionality and structural robustness.
