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Covalent organic framework with 3D Ordered Channel and Multi-Functional Groups Endows Zn Anode with Superior Stability

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Nano-Micro Letters 2024年第4期16卷 350-363页

作者： Bin Li Pengchao Ruan Xieyu Xu Zhangxing He Xinyan Zhu Liang Pan Ziyu Peng Yangyang Liu Peng Zhou Bingan Lu Lei Dai Jiang Zhou School of Chemical Engineering North China University of Science and TechnologyTangshan 063009People’s Republic of China School of Materials Science and Engineering Central South UniversityChangsha 410083People’s Republic of China State Key Laboratory for Mechanical Behavior of Materials Xi’an Jiaotong UniversityXi’an 710049People’s Republic of China Hunan Provincial Key Defense Laboratory of High Temperature Wear‑Resisting Materials and Preparation Technology Hunan University of Science and TechnologyXiangtan 411201People’s Republic of China School of Physics and Electronics Hunan UniversityChangsha 410082People’s Republic of China

Achieving a highly robust zinc(Zn)metal anode is extremely important for improving the performance of aqueous Zn-ion batteries(AZIBs)for advancing“carbon neutrality”society,which is hampered by the uncontrollable growth of Zn dendrite and severe side reactions including hydrogen evolution reaction,corrosion,and passivation,etc.Herein,an interlayer containing fluorinated zincophilic Covalent organic framework with sulfonic acid groups(COF-S-F)is developed on Zn metal(Zn@COF-S-F)as the artificial solid electrolyte interface(SEI).Sulfonic acid group(-SO_(3)H)in COF-S-F can effectively ameliorate the desolvation process of hydrated Zn ions,and the three-dimensional channel with fluoride group(-F)can provide interconnected channels for the favorable transport of Zn ions with ion-confinement effects,endowing Zn@COF-S-F with dendrite-free morphology and suppressed side reactions.Consequently,Zn@COF-S-F symmetric cell can stably cycle for 1,000 h with low average hysteresis voltage(50.5 m V)at the current density of 1.5 m A cm^(-2).Zn@COF-S-F|Mn O_(2)cell delivers the discharge specific capacity of 206.8 m Ah g^(-1)at the current density of 1.2 A g^(-1)after 800 cycles with high-capacity retention(87.9%).Enlightening,building artificial SEI on metallic Zn surface with targeted design has been proved as the effective strategy to foster the practical application of high-performance AZIBs.

关键词： Aqueous Zn ion batteries Covalent organic framework Interfacial modification Zn ion flux regulation Desolvation effect

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Quasi-Three-Dimensional Cyclotriphosphazene-Based Covalent organic framework Nanosheet for Efficient Oxygen Reduction

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Nano-Micro Letters 2023年第9期15卷 550-561页

作者： Jianhong Chang Cuiyan Li Xiaoxia Wang Daohao Li Jie Zhang Xiaoming Yu Hui Li Xiangdong Yao Valentin Valtchev Shilun Qiu Qianrong Fang State Key Laboratory of Inorganic Synthesis and Preparative Chemistry Jilin UniversityChangchun 130012People’s Republic of China State Key Laboratory of Bio-Fibers and Eco-Textiles College of Materials Science and EngineeringQingdao UniversityQingdao 266071People’s Republic of China Qingdao Institute of Bioenergy and Bioprocess Technology Chinese Academy of Sciences189 Song Ling RdQingdao 266101ShandongPeople’s Republic of China Laboratoire Catalyse et Spectrochimie CNRSENSICAENUNICAENNormandie Univ6 Marechal Juin14050 CaenFrance

Metal-free carbon-based materials are considered as promising oxygen reduction reaction(ORR)electrocatalysts for clean energy conversion,and their highly dense and exposed carbon active sites are crucial for efficient ORR.In this work,two unique quasi-three-dimensional cyclotriphosphazene-based Covalent organic frameworks(Q3CTP-COFs)and their nanosheets were successfully synthesized and applied as ORR electrocatalysts.The abundant electrophilic structure in Q3CTP-COFs induces a high density of carbon active sites,and the unique bilayer stacking of[6+3]imine-linked backbone facilitates the exposure of active carbon sites and accelerates mass diffusion during ORR.In particular,bulk Q3CTP-COFs can be easily exfoliated into thin COF nanosheets(NSs)due to the weak interlayerπ-πinteractions.Q3CTP-COF NSs exhibit highly efficient ORR catalytic activity(half-wave potential of 0.72 V vs.RHE in alkaline electrolyte),which is one of the best COF-based ORR electrocatalysts reported so far.Furthermore,Q3CTP-COF NSs can serve as a promising cathode for Zn-air batteries(delivered power density of 156 mW cm-2 at 300 mA cm^(-2)).This judicious design and accurate synthesis of such COFs with highly dense and exposed active sites and their nanosheets will promote the development of metal-free carbon-based electrocatalysts.

关键词： Covalent organic framework Quasi-three-dimensional structures Oxygen reduction reaction Metal-free electrocatalyst

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Bending Resistance Covalent organic framework Superlattice:“Nano‑Hourglass”‑Induced Charge Accumulation for Flexible In‑Plane Micro‑Supercapacitors

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Nano-Micro Letters 2023年第2期15卷 198-211页

作者： Xiaoyang Xu Zhenni Zhang Rui Xiong Guandan Lu Jia Zhang Wang Ning Shuozhen Hu Qingliang Feng Shanlin Qiao College of Chemistry and Pharmaceutical Engineering Hebei University of Science and TechnologyShijiazhuang 050018People’s Republic of China State Key Laboratory of Chemical Engineering East China University of Science and TechnologyShanghai 200237People’s Republic of China School of Chemistry and Chemical Engineering Northwestern Polytechnical UniversityXi’an 710072People’s Republic of China Hebei Electronic organic Chemicals Engineering Center Shijiazhuang 050018People’s Republic of China

Covalent organic framework(COF)film with highly exposed active sites is considered as the promising flexible selfsupported electrode for in-plane microsupercapacitor(MSC).Superlattice configuration assembled alternately by different nanofilms based on van der Waals force can integrate the advantages of each isolated layer to exhibit unexpected performances as MSC film electrodes,which may be a novel option to ensure energy output.Herein,a mesoporous free-standing A-COF nanofilm(pore size is 3.9 nm,averaged thickness is 4.1 nm)with imine bond linkage and a microporous B-COF nanofilm(pore size is 1.5 nm,averaged thickness is 9.3 nm)withβ-keto-enamine-linkages are prepared,and for the first time,we assembly the two lattice matching films into sandwich-type superlattices via layer-by-layer transfer,in which ABA–COF superlattice stacking into a“nano-hourglass”steric configuration that can accelerate the dynamic charge transportation/accumulation and promote the sufficient redox reactions to energy storage.The fabricated flexible MSC–ABA–COF exhibits the highest intrinsic CV of 927.9 F cm^(−3) at 10 mV s^(−1) than reported two-dimensional alloy,graphite-like carbon and undoped COF-based MSC devices so far,and shows a bending-resistant energy density of 63.2 mWh cm^(−3) even after high-angle and repeat arbitrary bending from 0 to 180°.This work provides a feasible way to meet the demand for future miniaturization and wearable electronics.

关键词： In-plane micro-supercapacitor Covalent organic framework Free-standing nanofilm Superlattice Bending resistance

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Monodispersed Covalent organic framework nanocrystals in aqueous solution for DNA inclusion

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Science China Chemistry 2023年第11期66卷 3161-3168页

作者： Xinheng Lyu Lezhi Yi Liang Zhang Jin Liu Hexiang Deng Key Laboratory of Biomedical Polymers-Ministry of Education College of Chemistry and Molecular SciencesWuhan UniversityWuhan 430072China Hubei Yangtze Memory Laboratories Wuhan 430205China Department of Chemistry The Hong Kong Branch of Chinese National Engineering Research Center for Tissue Resto-ration and ReconstructionThe Hong Kong University of Science and TechnologyHong Kong 999077China

Covalent organic framework(COF)nanocrystals are useful in biological applications;however,their hydrophobic nature makes them aggregate into clusters in aqueous media.In this work,we show that by modifying the crystal surface with hydrophilic functional groups,these nanocrystals can maintain in the monodispersed form in aqueous solution.Specifically,three COFs,TPB-DMTP COF,TAPB-PDA COF and TAPB-BPDA COF were synthesized using organic Lewis acid as the catalyst,to generate nanoparticles with the size ranging from 180 nm to 1μm.2-Aminoethanesulfonic acid(AESA)was applied to react with the terminal aldehyde functional groups exposed at the surface of COF nanocrystals.The resulting negatively charged surface keeps these nanocrystals apart from each other in aqueous solution for at least 48 h.The mesopore of these COF nanocrystals allows the entering of single-strand DNA molecules and the release in the presence of complementary DNA.

关键词： Covalent organic framework nanocrystals in aqueous solution DNA inclusion

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Porphyrin Covalent organic framework for photocatalytic synthesis of tetrahydroquinolines

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Chinese Chemical Letters 2022年第10期33卷 4559-4562页

作者： Chengjuan Wu Xinyu Li Mingzhen Shao Jinglan Kan Guangbo Wang Yan Geng Yu-Bin Dong College of Chemistry Chemical Engineering and Materials ScienceCollaborative Innovation Center of Functionalized Probes for Chemical Imaging in Universities of ShandongKey Laboratory of Molecular and Nano ProbesMinistry of EducationShandong Normal UniversityJi’nan 250014China

A metal-free porphyrin Covalent organic framework was employed as the heterogeneous photocatalyst for the synthesis of tetrahydroquinolines under aerobic conditions.With visible light irradiation of a catalytic amount of H_(2)P-Bph-COF at room temperature,various substituted N,N-dimethylanilines and N-aryl maleimides were transformed to tetrahydroquinoline derivatives in moderate to good yields.This was the first example of the synthesis of tetrahydroquinolines via the photocatalytic aerobic annulation reaction employing the metal-free COF as the heterogeneous photocatalyst.

关键词： Tetrahydroquinolines Photocatalytic oxidative annulation Covalent organic framework Heterogeneous photocatalyst Porphyrin

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Surface protection method for the magnetic core using Covalent organic framework shells and its application in As(Ⅲ)depth removal from acid wastewater

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Journal of Environmental Sciences 2022年第5期34卷 1-9页

作者： Wenjun Huang Haomiao Xu Xiaoshuang Liu Longlong Wang Shutang Li Leipeng Ji Zan Qu Naiqiang Yan School of Environmental Science and Engineering Shanghai Jiao Tong UniversityShanghai 200240China Shanghai Institute of Pollution Control and Ecological Security Shanghai 200092China

Fe_(3)O_(4)-based materials are widely used for magnetic separation from wastewater.However,they often suffer from Fe-leaching behavior under acidic conditions,decreasing their ac-tivity and limiting sustainable practical applications.In this study,covalent organic frame-works(COFs)were used as the shell to protect the Fe_(3)O_(4) core,and the Fe_(3)O_(4)@COF core-shell composites were synthesized for As(Ⅲ)removal from acid wastewater.The imine-linked COFs can in situ grow on the surface of the Fe_(3)O_(4) core layer by layer with[COFs/Fe_(3)O_(4)]mol ratio of up to 2∶1.The Fe-leaching behavior was weakened over a wide pH range of 1-13.Moreover,such composites keep their magnetic characteristic,making them favorable for nanomaterial separation.As(Ⅲ)batch adsorption experiments results indicated that,when COFs are used as the shell for the Fe_(3)O_(4) core,a balance between As(Ⅲ)removal efficiencies and the thickness of the COF shell exists.Higher As(Ⅲ)removal efficiencies are obtained when the[COFs/Fe_(3)O_(4)]mol ratios were<1.5∶1,but thicker COF shells were not beneficial for As(Ⅲ)removal.Such composites also exhibited better As(Ⅲ)removal performances in the pH range of 1-7.Over a wide pH range,the zeta potential of Fe_(3)O_(4)@COF core-shell compos-ites becomes more positive,which benefits the capture of negative arsenic ions.In addition,thinner surface COFs were favorable for mass transfer and facilitating the reaction of Fe and As elements.Our study highlights the promise of using COFs in nanomaterial surface protection and achieving As(Ⅲ)depth removal under acidic conditions.

关键词： Arsenic ions Covalent organic framework Core-shell structure Surface protectionLayer Thickness

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C2-phenyl-substituted benzimidazolium-based Covalent organic framework as efficient catalyst for CO_(2) conversion without solvents,metals,and cocatalysts

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Science China Chemistry 2024年第2期67卷 551-557页

作者： Zhenzhen Wu Jing Wang Lili Liu Shang Guo Juan Li Xianming Zhang Shanxi Institute for Functional Food Shanxi Agricultural UniversityTaiyuan030031China Institute of Crystalline Materials Shanxi UniversityTaiyuan030006China Key Laboratory of Interface Science and Engineering in Advanced Materials College of ChemistryTaiyuan University of TechnologyTaiyuan030024China

Covalent organic frameworks(COFs) are a potential platform for carbon dioxide(CO_(2)) conversion owing to their periodic permanent porosity,adjustable structure,and chemical stability.For good catalytic performance in CO_(2) conversion,collaborative multifunctions should be strategically integrated into the catalytic system design and construction.In this study,a four-in-one high-efficiency catalyst was synthesized and tested for CO_(2) cycloaddition to form cyclic carbonate.The obtained Tp-MPB-BrCOF had a high nitrogen content,which enhanced its CO_(2) affinity through substantial Lewis acid-base or dipole-quadrupole interactions;moreover,the acid(protons transferring from oxygen(–OH) to nitrogen(–NH)),hydrogen bond donor(hydroxyl group),and Br-(nucleophile group) served as three active sites,further improving the catalyst activity.These results provide a basis for designing efficient and stable CO_(2)-conversion catalysts.

关键词： Covalent organic framework C2-phenyl-substituted benzimidazolium CO_(2)conversion four-in-one catalyst

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A solubility limited pyrene-4,5,9,10-tetraone-based Covalent organic framework for high-performance aqueous zinc-organic batteries

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Nano Research 2024年第6期17卷 5095-5103页

作者： Min Cheng Shibing Zheng Tianjiang Sun Diantao Li Weijia Zhang Zhengtai Zha Qiong Sun Jing Tian Kai Zhang Zhanliang Tao Frontiers Science Center for New organic Matter State Key Laboratory of Advanced Chemical Power SourcesKey Laboratory of Advanced Energy Materials Chemistry(Ministry of Education)Collaborative Innovation Center of Chemical Science and Engineering(Tianjin)Renewable Energy Conversion and Storage CentreNankai UniversityTianjin 300071China Haihe Laboratory of Sustainable Chemical Transformations Tianjin 300192China

Pyrene-4,5,9,10-tetraone(PTO),with a high theoretical capacity of 408 mAh·g^(−1),is a promising candidate for rechargeable aqueous zinc-ion batteries(RAZIBs),but its zincated products during discharge process suffer from high solubility in electrolytes.Herein,aβ-ketoenamine-linked two-dimensional(2D)Covalent organic framework(COF)based on a 2,7-diaminopyrene-4,5,9,10-tetraone(4KT-BD)monomer and a 2,4,6-trihydroxy-benzene-1,3,5-tricarbaldehyde(Tp)node(4KT-Tp-COF)is synthesized to address the above issue.The well-designed 4KT-Tp-COF displays low solubility in 3 M Zn(CF3SO3)2 owing to the favorableπ-πstacking as well as extended structure.Besides,the ingenious structural design of the active molecule and the long-range ordered nano-channels alter the intramolecular electron distribution,which facilitates the ionic diffusion.Consequently,the 4KT-Tp-COF cathode exhibits a stable capacity of 181 mAh·g^(−1)at 0.2 A·g^(−1),superior rate capability of 139 mAh·g^(−1)at 20 A·g^(−1),and a long lifetime of 1000 cycles without capacity loss at 30 A·g^(−1).Even at a low temperature of−20°C,the electrode also performs an ultralong cycling life of 9000 cycles with a capacity of 106 mAh·g^(−1)at 5 A·g^(−1).The comprehensive characterizations of ex-situ analyses together with the theoretical calculations validate that the groups of C=O can contribute highly accessible redox-active sites for Zn^(2+)storage.The ultra-stable 4KT-Tp-COF cathode provides important insights for designing robust organic electrodes for sustainable and large-scale electrochemical energy storage.

关键词： pyrene-4,5,9,10-tetraone solubility limited Covalent organic framework zinc batteries

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Pyrenetetraone-based Covalent organic framework as an effective electrocatalyst for oxygen reduction reaction

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Nano Research 2022年第5期15卷 3907-3912页

作者： Paloma Garcia-Arroyo Emiliano Martinez-Perinan Jorge J.Cabrera-Trujillo Elena Salagre Enrique G.Michel Jose I.Martinez Encarnacion Lorenzo Jose L.Segura Departamento de Quimica organica I Facultad de CC.QuimicasUniversidad Complutense de Madrid28040 MadridSpain Departamento de Quimica Analitica y Analisis Instrumental Facultad de CienciasUniversidad Autónoma de Madrid28049 MadridSpain Departamento de Fisica de la Materia Condensada Universidad Autónoma de Madrid28049 MadridSpain Condensed Matter Physics Center(IFIMAC) Universidad Autónoma de Madrid28049 MadridSpain Departamento de Nanoestructuras SuperficiesRecubrimientos y Astrofisica MolecularInstituto de Ciencia de Materiales de Madrid(ICMMCSIC)28049 MadridSpain Instituto Madrileno de Estudios Avanzados en Nanociencia(IMDEA-Nanociencia) 28049 MadridSpain Institute for Advanced Research in Chemical Sciences(IAdChem) Universidad Autonoma de Madrid28049 MadridSpain

A novel porous and crystalline two-dimensional(2D)electrochemically active Covalent organic framework(COF)based on ortho-quinone units has been prepared as an innovative approach towards the development of organic cathode materials with multiple redox sites as an efficient electrocatalyst for the oxygen reduction reaction(ORR).In contrast with most of the previously reported COFs as electrocatalysts for the ORR,the electrocatalytic application of this material towards ORR has been investigated without adding any metal or conductive supporting material and avoiding any additional carbonization step.Additionally,the electrochemical properties of the COF material have been compared with two analogue amorphous frameworks with similar chemical composition,which points out the important role of the enhanced crystallinity and porosity of the COF network in its superior performance as an electrocatalyst towards ORR.

关键词： electrocatalysis oxygen reduction reaction metal free pyrenetetraone Covalent organic framework

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A novel 3D sp2 carbon-linked Covalent organic framework as a platform for efficient electro-extraction of uranium

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Science China Chemistry 2023年第2期66卷 562-569页

作者： Cheng-Rong Zhang Jia-Xin Qi Wei-Rong Cui Xiao-Juan Chen Xin Liu Shun-Mo Yi Cheng-Peng Niu Ru-Ping Liang Jian-Ding Qiu State Key Laboratory of Nuclear Resources and Environment East China University of TechnologyNanchang330013China College of Chemistry Nanchang UniversityNanchang330031China

Extracting uranium from seawater offers opportunities for sustainable nuclear fuel supply,but the task is quite challenging due to the low uranium concentration(~3 ppb)in seawater.Here,based on the Knoevenagel condensation reaction of aldehyde and acetonitrile groups,a novel stable sp^(2)carbon-linked three-dimensional Covalent organic framework(3D COF),TFPM-PDANAO was prepared as a porous platform for uranium extraction from seawater.The TFPM-PDAN-AO designed with regular 3D pore channel of 7.12 A provides a specific channel for uranyl diffusion,which exhibits high selectivity and fast kinetics for uranium adsorption.Meanwhile,the superior stability and optoelectronic properties enable it an excellent porous platform for uranium electroextraction.By applying alternating voltages between-5 and 0 V,uranyl ions can rapidly migrate and enrich into the porous structure of TFPM-PDAN-AO,then inducing the electrodeposition of uranium compounds to form the charge neutral species(Na_(2)O(UO_(3)H_(2)O)x)with an unprecedentedly high adsorption capacity of 4,685 mg g^(-1).This work not only expands the application prospects of functionalized 3D COFs,but also provides a technical support for the electrodeposition adsorption of uranium from seawater.

关键词： three-dimension Covalent organic framework uranium adsorption electrosorption

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