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Interlocked covalent organic cages:Design,synthesis,and self-assembly
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作者 Bin Yao Yao Bu +3 位作者 Hongfei Sun Guowang Li Xianying Wu Wei Wang 《Chinese Chemical Letters》 2026年第1期92-105,共14页
Interlocked covalent organic cages have aesthetic skeletons endowed with structural and topological complexity.Their self-assembly provides a unique possibility to mimic the hierarchical self-assembly of biomacromolec... Interlocked covalent organic cages have aesthetic skeletons endowed with structural and topological complexity.Their self-assembly provides a unique possibility to mimic the hierarchical self-assembly of biomacromolecules.In recent years,significant progresses in interlocked covalent organic cages have been witnessed.Different topological structures have been fabricated via various non-template induced methods,and diverse weak interactions are demonstrated to play critical roles in guiding the formation of interlocked structures.Therefore,this article systematically summarizes the recent advances in interlocked covalent organic cages,especially their design,synthesis,and self-assembly properties.Depending on different types of chemical reactions,irreversible and reversible reactions are separately introduced.In each section,proper monomer selection,critical topology design,key driving forces as well as detailed interlocked mechanisms for the formation of interlocked structures,and their self-assembly behaviors in single crystals are discussed detailedly.Finally,the challenge and future development of interlocked covalent organic cages are briefly prospected. 展开更多
关键词 Mechanically interlocked molecules Chemical topology Dynamic covalent chemistry Non-covalent interactions Supramolecular chemistry
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Advances in electrocatalytic and photocatalytic CO_(2)conversion to value-added chemicals using copper-based covalent organic frameworks
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作者 LI Yue LIU Ziqi +7 位作者 FENG Ke LI Yingdan NING Yue SHEN Li LU Jitao MENG Qingguo WANG Min WANG Haiying 《无机化学学报》 北大核心 2026年第1期1-22,共22页
CO_(2)reduction technology can promote the resource utilization of carbon and help alleviate global warming and energy supply pressure.It is an effective way to achieve energy conversion and utilization.Covalent organ... CO_(2)reduction technology can promote the resource utilization of carbon and help alleviate global warming and energy supply pressure.It is an effective way to achieve energy conversion and utilization.Covalent organic frameworks(COFs)are porous crystalline materials formed by connecting organic monomers through covalent bonds.They have the characteristics of functional diversity and rich chemical properties.Their advantages,such as high porosity,a wide range of visible light absorption,and excellent charge separation efficiency,give them good potential in CO_(2)capture,separation,and conversion.Currently,Cu is a key metal in the catalytic CO_(2)reduction reaction(CO_(2)RR)for the preparation of high-value-added chemicals.The preparation of highly stable and large-pore Cu-based COFs using COFs as an ideal sacrificial template for loading Cu can be used to develop high-performance electrocatalysts and photocatalysts.In this review,we discuss the latest advancements in this field,including the development of various Cu-based COFs and their applications as catalysts for CO_(2)RR.Here,we mainly introduce the synthesis strategies,some important characterization information,and the applications of electrocatalytic and photocatalytic CO_(2)conversion using these previously reported Cu-based COFs. 展开更多
关键词 copper-based covalent organic frameworks CO_(2)reduction reactions electrocatalytic CO_(2)conversion photocatalytic CO_(2)conversion
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Facile and scale-up synthesis of cyano-functionalized covalent organic frameworks for selective gold recovery
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作者 Bo Li Yuanzhe Cheng +8 位作者 Xuyang Ma Dongxu Zhao Yang Zhang Yongxing Sun Jia Chen Li Wu Liang Zhao Hongdeng Qiu Yujian He 《Chinese Chemical Letters》 2026年第1期514-519,共6页
The recovery of gold from waste electronic and electric equipment(WEEE) has gained great attention with the increased number of WEEE,because it can largely alleviate the pressure on the environment and resources.Coval... The recovery of gold from waste electronic and electric equipment(WEEE) has gained great attention with the increased number of WEEE,because it can largely alleviate the pressure on the environment and resources.Covalent organic frameworks(COFs) are ideal adsorbents for gold recovery owing to their large surface area,good stability,easily functionalized ability,periodic structures,and definitive nanopores.Herein,a cyano-functionalized COF(COF-CN) with high crystallinity was large-scale prepared under mild conditions for the recovery of gold.The introduction of cyano groups enable COF-CN to exhibit excellent gold recovery performance,which possesses fast adsorption kinetics,high cycling stability,and adsorption capacity up to 663.67 mg/g.Excitingly,COF-CN showed extremely high selectivity for gold ions,even in the presence of various competing cations and anions.The COF-CN maintained excellent selectivity and removal efficiency in gold recovery experiments from WEEE.The facile synthesis of COF-CN and its outstanding selectivity in actual samples make it an attractive opportunity for practical gold recovery. 展开更多
关键词 Cyano functionalization Gold recovery covalent organic frameworks Waste electronic and electric equipment SELECTIVITY
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Construction of Modifiable Phthalocyanine-Based Covalent Organic Frameworks with Irreversible Linking for Efficient Photocatalytic CO_(2)Reduction
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作者 Xuefei Zhou Shaowei Yang +5 位作者 Zhengyang Hu Zhanwei Chen Ying Guo Tianshuai Wang Qiuyu Zhang Hepeng Zhang 《Nano-Micro Letters》 2026年第4期435-448,共14页
Covalent organic frameworks(COFs)are considered promising catalysts for photocatalytic CO_(2)reduction reaction(pCO_(2)RR)due to facilitated regulations.However,the instability of COFs with dynamic reversible covalent... Covalent organic frameworks(COFs)are considered promising catalysts for photocatalytic CO_(2)reduction reaction(pCO_(2)RR)due to facilitated regulations.However,the instability of COFs with dynamic reversible covalent bonds and the limited modifiability of COFs with irreversible covalent bonds restricted the enhancement of the pCO_(2)RR performance.Herein,three phthalocyanine-based COFs with ether-linked,CoOP,CoPOP,and CoBOP,were successfully prepared via in situ polycondensation using modifiable bis-phthalonitrile.CoBOP achieved a record of syngas performance in pCO_(2)RR systems with photosensitizers and sacrificial agents(CO 83.7 mmol g^(-1)h^(-1)and H_254.7 mmol g^(-1)h^(-1)),surpassing most COF photocatalysts.Additionally,CoOP,CoPOP,and CoBOP exhibit stabilities in extreme environments owing to their irreversible covalent bonds.Experimental and density functional theory analyses confirm that the optimally matched the lowest unoccupied molecular orbital of the linking unit between the photosensitizer and active unit endowed Co BOP with the highest photoelectron transfer efficiency among the three catalysts,boosting its pCO_(2)RR activity.This work is highly instructive for designing COFs with structure-adjustable and irreversible covalent bonds. 展开更多
关键词 Photocatalytic CO_(2)RR Phthalocyanine-based COF Irreversible covalent bond Electronic property modulation Photoelectron transfer
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Covalent organic framework ionomers enable synergistic efficient transport of protons and oxygen in medium-temperature proton exchange membrane fuel cells
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作者 Zijie Lin Qing Li 《Chinese Chemical Letters》 2026年第1期7-9,共3页
Covalent organic framework ionomers enable synergistic efficient transport of protons and oxygen in medium-temperature proton exchange membrane fuel cells Proton exchange membrane fuel cells(PEMFCs),as clean and effic... Covalent organic framework ionomers enable synergistic efficient transport of protons and oxygen in medium-temperature proton exchange membrane fuel cells Proton exchange membrane fuel cells(PEMFCs),as clean and efficient energy technologies,are constrained in their performance enhancement by the sluggish oxygen reduction reaction(ORR)kinetics at the cathode,anode CO poisoning(e.g.,from methanol crossover)and intricate water management dilemmas[1]. 展开更多
关键词 covalent organic framework ionomers proton exchange membrane fuel cells pemfcs proton exchange membrane fuel cells sluggish oxygen reduction reaction orr kinetics PROTONS water management dilemmas OXYGEN
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Covalent Organic Framework-Based Photocatalysts from Synthesis to Applications
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作者 Junxian Liu Kezhen Qi +3 位作者 Xianglin Xiang Abdollah Jamal Sisi Alireza Khataee Liqianyun Xu 《Energy & Environmental Materials》 2025年第6期263-293,共31页
Covalent organic frameworks have emerged as a hot spot in the field of photocatalysis due to their excellent structural tunability,high specific surface area,high porosity,and good chemical stability.Specifically,they... Covalent organic frameworks have emerged as a hot spot in the field of photocatalysis due to their excellent structural tunability,high specific surface area,high porosity,and good chemical stability.Specifically,they exhibit distinctive optoelectronic features by integrating different molecular building blocks with appropriate links,constructing an π-conjugated system,or introducing electron donor–acceptor units into the conjugated framework.The reasonably adjusted band structure yields excellent photocatalytic activity of covalent organic framework materials. 展开更多
关键词 covalent chemistry covalent organic frameworks functional ligands PHOTOCATALYSIS structure–property relationship
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In situ preparation of zincophilic covalent-organic frameworks with low surface work function and high rigidity to stabilize zinc metal anodes 被引量:3
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作者 Yunyu Zhao Kaiyong Feng Yingjian Yu 《Journal of Energy Chemistry》 2025年第3期524-533,共10页
Zinc-ion batteries(ZIBs)are inexpensive and safe,but side reactions on the Zn anode and Zn dendrite growth hinder their practical applications.In this study,1,3,5-triformylphloroglycerol(Tp)and various diamine monomer... Zinc-ion batteries(ZIBs)are inexpensive and safe,but side reactions on the Zn anode and Zn dendrite growth hinder their practical applications.In this study,1,3,5-triformylphloroglycerol(Tp)and various diamine monomers(p-phenylenediamine(Pa),benzidine(BD),and 4,4"-diamino-p-terphenyl(DATP))were used to synthesize a series of two-dimensional covalent-organic frameworks(COFs).The resulting COFs were named TpPa,TpBD,and TpDATP,respectively,and they showed uniform zincophilic sites,different pore sizes,and high Young's moduli on the Zn anode.Among them,TpPa and TpBD showed lower surface work functions and higher ion transfer numbers,which were conducive to uniform galvanizing/stripping zinc and inhibited dendrite growth.Theoretical calculations showed that TpPa and TpBD had wider negative potential region and greater adsorption capacity for Zn2+than TpDATP,providing more electron donor sites to coordinate with Zn^(2+).Symmetric cells protected by TpPa and TpBD stably cycled for more than 2300 h,whereas TpDATP@Zn and the bare zinc symmetric cells failed after around 150 and200 h.The full cells containing TpPa and TpBD modification layers also showed excellent cycling capacity at 1 A/g.This study provides comprehensive insights into the construction of highly reversible Zn anodes via COF modification layers for advanced rechargeable ZIBs. 展开更多
关键词 Zn ion batteries covalent organic framework DENDRITE Low surface work function High rigidity
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Pyridine-nitrogen conjugated covalent organic frameworks for high-efficiency gas-solid photocatalytic reduction of CO_(2)to CO 被引量:2
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作者 Haicheng Jiang Chi Cao +10 位作者 Wei Liu Hao Zhang Qianyu Li Siyuan Zhu Xiaoning Li Jinshuo Li Jinfa Chang Wei Hu Zihao Xing Xiaoqin Zou Guangshan Zhu 《Journal of Energy Chemistry》 2025年第5期127-135,共9页
The light-driven CO_(2)reduction reaction(CO_(2)RR)to CO is a very effective way to address global warming.To avoid competition with water photolysis,metal-free gas-solid CO_(2)RR catalysts should be investigated.Cova... The light-driven CO_(2)reduction reaction(CO_(2)RR)to CO is a very effective way to address global warming.To avoid competition with water photolysis,metal-free gas-solid CO_(2)RR catalysts should be investigated.Covalent organic frameworks(COFs)offer a promising approach for CO_(2)transformation but lack high efficiency and selectivity in the absence of metals.Here,we have incorporated a pyridine nitrogen component into the imine-COF conjugated structure(Tp Pym).This innovative system has set a record of producing a CO yield of 1565μmol g^(-1)within 6 h.The soft X-ray absorption fine structure measurement proves that Tp Pym has both better conjugation and electron cloud enrichment.The electronic structure distribution delays the charge-carrier recombination,as evidenced by femtosecond transient absorption spectroscopy.The energy band diagram and theoretical calculation show that the conduction-band potential of Tp Pym is lower and the reduction reaction of CO_(2)to CO is more likely to occur. 展开更多
关键词 Light-driven CO_(2)reduction Gas-solid reaction Conjugated pyridine nitrogen covalent organic framework CO_(2)catalysis to CO
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Superelastic and ultralight covalent organic framework composite aerogels modified with different functional groups for ultrafast adsorbing organic pollutants in water 被引量:1
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作者 Shiyan Ai Yaning Xu +3 位作者 Hui Zhou Ziwei Cui Tiantian Wu Dan Tian 《Chinese Chemical Letters》 2025年第10期478-487,共10页
Covalent organic frameworks(COFs)have great potential as adsorbents due to their customizable functionality,low density and high porosity.However,COFs powder exists with poor processing and recycling performance.Moreo... Covalent organic frameworks(COFs)have great potential as adsorbents due to their customizable functionality,low density and high porosity.However,COFs powder exists with poor processing and recycling performance.Moreover,due to the accumulation of COFs nanoparticles,it is not conducive to the full utilization of their surface functional groups.Currently,the strategy of COFs assembling into aerogel can be a good solution to this problem.Herein,we successfully synthesize composite aerogels(CSR)by in-situ self-assembly of two-dimensional COFs and graphene based on crosslinking of sodium alginate.Sodium alginate in the composite improves the mechanical properties of the aerogel,and graphene provides a template for the in-situ growth of COFs.Impressively,CSR aerogels with different COFs and sizes can be prepared by changing the moiety of the ligand and modulating the addition amount of COFs.The prepared CSR aerogels exhibit porous,low density,good processability and good mechanical properties.Among them,the density of CSR-N-1.6 is only 5 mg/cm3,which is the lowest density among the reported COF aerogels so far.Due to these remarkable properties,CSR aerogels perform excellent adsorption and recycling properties for the efficient and rapid removal of organic pollutants(organic dyes and antibiotics)from polluted water.In addition,it is also possible to visually recognize the presence of antibiotics by fluorescence detection.This work not only provides a new strategy for synthesizing COF aerogels,but also accelerates the practical application of COF aerogels and contributes to environmental remediation. 展开更多
关键词 covalent organic frameworks GRAPHENE AEROGELS ADSORPTION Sewage treatment
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Covalent modulation of mPGES1 activity via α,β-unsaturated aldehyde group: Implications for downregulating PGE2 expression and antipyretic response 被引量:1
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作者 Fuyun Chi Man Zhang +5 位作者 Yiman Han Fukui Shen Shijie Peng Bo Su Yuanyuan Hou Gang Bai 《Chinese Chemical Letters》 2025年第4期363-368,共6页
Prostaglandin E2(PGE2) serves as the ultimate mediator of fever induced by infiammatory factors. In contrast to cyclooxygenase inhibitors that suppress arachidonic acid metabolism, antipyretic herbs possess a well-est... Prostaglandin E2(PGE2) serves as the ultimate mediator of fever induced by infiammatory factors. In contrast to cyclooxygenase inhibitors that suppress arachidonic acid metabolism, antipyretic herbs possess a well-established clinical history in effectively managing fever. However, the specific mechanisms underlying their efficacy remain unclear. Following the screening for lead compounds that inhibit PGE2from antipyretic herbs, alkynylated active molecule probes were designed and synthesized to track and identify potential targets. The target investigation revealed that three antipyretic compounds, namely cinnamaldehyde, 2,4-decadienal, and perillaldehyde, containing α,β-unsaturated aldehyde groups irreversibly targeted the microsomal PGES1-TM4 helix(m PGES1-TM4) at Ser139. This specific interaction effectually inhibited PGE2 production in the cerebral vasculature, leading to exert potent antipyretic effects.α,β-Unsaturated aldehydes targeting m PGES1-TM4 offer a new approach for antipyretic effects with significant potential for various applications. 展开更多
关键词 α β-Unsaturated aldehyde covalent binding mPGES1 PGE2 ANTIPYRETIC
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Radiation reduction modification of sp^(2) carbon-conjugated covalent organic frameworks for enhanced photocatalytic chromium(Ⅵ) removal 被引量:1
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作者 Shouchao Zhong Yue Wang +6 位作者 Mingshu Xie Yiqian Wu Jiuqiang Li Jing Peng Liyong Yuan Maolin Zhai Weiqun Shi 《Chinese Chemical Letters》 2025年第5期277-282,共6页
A sp^(2) carbon-conjugated covalent organic framework (BDATN) was modified through γ-ray radiation reduction and subsequent acidification with hydrochloric acid to yield a novel functional COF (named rBDATN-HCl) for ... A sp^(2) carbon-conjugated covalent organic framework (BDATN) was modified through γ-ray radiation reduction and subsequent acidification with hydrochloric acid to yield a novel functional COF (named rBDATN-HCl) for Cr(Ⅵ) removal.The morphology and structure of rBDATN-HCl were analyzed and identified by SEM,FTIR,XRD and solid-state13C NMR.It is found that the active functional groups,such as hydroxyl and amide,were introduced into BDATN after radiation reduction and acidification.The prepared rBDATN-HCl demonstrates a photocatalytic reduction removal rate of Cr(Ⅵ) above 99%after 60min of illumination with a solid-liquid ratio of 0.5 mg/mL,showing outstanding performance,which is attributed to the increase of dispersibility and adsorption sites of r BDATN-HCl.In comparison to the cBDATN-HCl synthesized with chemical reduction,rBDATN-HCl exhibits a better photoreduction performance for Cr(Ⅵ),demonstrating the advantages of radiation preparation of rBDATN-HCl.It is expected that more functionalized sp^(2) carbon-conjugated COFs could be obtained by this radiation-induced reduction strategy. 展开更多
关键词 covalent organic framework Gamma radiation Photocatalytic reduction CHROMIUM Water purification
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Constructing S-scheme heterojunction between porphyrinyl covalent organic frameworks and Nb_(2)C MXene for photocatalytic H_(2)O_(2) production 被引量:1
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作者 Mingyang Xu Zhenzhen Li +4 位作者 Rongchen Shen Xin Zhang Zhihong Zhang Peng Zhang Xin Li 《Chinese Journal of Catalysis》 2025年第3期431-443,共13页
We have developed a novel S-scheme heterojunction photocatalyst for the photocatalytic production of hydrogen peroxide(H_(2)O_(2))via a two-electron(2e^(-))oxygen reduction reaction.This S-scheme heterojunction Tph-Dh... We have developed a novel S-scheme heterojunction photocatalyst for the photocatalytic production of hydrogen peroxide(H_(2)O_(2))via a two-electron(2e^(-))oxygen reduction reaction.This S-scheme heterojunction Tph-Dha-COF@Nb_(2)C was fabricated via the in-situ solvothermal growth of Tph-Dha-COF nanostructures on amino-functionalized Nb_(2)C MXene nanoflakes(Nb_(2)C-NH_(2)).The integration of Nb_(2)C significantly extended the visible light absorption of Tph-Dha-COF into the near-infrared region for photocatalytic H_(2)O_(2) production.The Tph-Dha-COF@Nb_(2)C composite demonstrated efficient charge separation,rapid electron transfer,and enhanced oxygen adsorption.Consequently,the Tph-Dha-COF@Nb_(2)C heterojunction exhibited a high H_(2)O_(2) production rate of 1833μmol g^(-1) h^(-1) without sacrificial agents.In-situ Fourier transformed infrared spectroscopy and density functional theory calculations revealed the photocatalytic H_(2)O_(2) production mechanism.The generated H_(2)O_(2) demonstrated enhanced antibacterial activity.This work presents the first application of Nb_(2)C in the photocatalytic synthesis of H_(2)O_(2) and provides a novel strategy for constructing COF-based heterojunctions for photocatalytic H_(2)O_(2) generation and wastewater treatment. 展开更多
关键词 Photocatalysis H_(2)O_(2) covalent organic framework Nb_(2)C MXene S-scheme heterojunction
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Design of Weldable and Recyclable Fluorine-containing Adhesives Utilizing Dynamic-covalent Boroxine Bonds
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作者 Hou-Li Zhang Yu-Quan Sun +6 位作者 Yao Xu Lu Wang Ying Li Jie Zhang Bing Geng Shu-Sheng Li Chuan-Yong Zong 《Chinese Journal of Polymer Science》 2025年第8期1433-1442,共10页
The advancement of functional adhesives featuring recyclable and repairable properties is of great significance in interfacial science and engineering.Herein,a series of high-strength,recyclable fluorine-containing ad... The advancement of functional adhesives featuring recyclable and repairable properties is of great significance in interfacial science and engineering.Herein,a series of high-strength,recyclable fluorine-containing adhesives(ESOx-FPF)were designed and synthesized by crosslinking two prepolymers,FPF-B(derived from side-chain fluorinated diol,isocyanate,and aminoboric acid)and ESO-B(synthesized from biobased epoxy soybean oil and aminoboric acid),through dynamic boro-oxygen bonds.The resulting adhesive exhibited an optimal tensile strength of 42 MPa and the shear strength on steel plates reached as high as 3.89 MPa.More importantly,benefiting from the dynamic reversibility of the boron-oxygen bonds along with the hydrogen bonds interaction,ESOx-FPF can be welded with the assistance of solvents and recycled for multiple cycles.The outstanding healing efficiency and excellent reprocessability of these functional adhesives were confirmed by mechanical testing.Moreover,the as-prepared adhesives demonstrated universal and remarkable adhesion to various substrates,such as aromatic polyamide,aluminum plates and polycarbonate,meanwhile,they could be easily disassembled and recycled using ethanol without damaging the substrates surface.This study not only provides a simple strategy for the synthesis of eco-friendly adhesives with weldable and recyclable properties,but also sheds light on the development of other functional materials utilizing dynamic covalent chemistry. 展开更多
关键词 Functional adhesive RECYCLABLE Dynamic covalent bonds Boroxines FLUORINE-CONTAINING
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Periodic Janus structure based on ionic covalent organic framework for selective removal of perfluoroalkyl substances
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作者 Xiaojuan Sun Ke Kong +3 位作者 Jun Liang Dan Wang Beibei Dong Ruihu Wang 《Chinese Journal of Structural Chemistry》 2025年第9期14-19,共6页
Per-and polyfluoroalkyl substances(PFAS)are persistent environmental contaminants that often show an adverse impact on human health.Rational design of porous adsorbents for selective and reversible removal of PFAS,suc... Per-and polyfluoroalkyl substances(PFAS)are persistent environmental contaminants that often show an adverse impact on human health.Rational design of porous adsorbents for selective and reversible removal of PFAS,such as perfluorooctane sulfonate(PFOS),is imperative and challenging.Herein,a Janus strategy based on an ionic covalent organic framework(iCOF-DGCl)composed of the alternately hydrophobic aromatic domains and hydrophilic guanidinium moieites has been proposed to meet the requirement of high-performance adsorbents.iCOF-DGCl shows fast adsorption kinetics(970.9 mg g^(−1)min^(−1))and ultrahigh uptake capacity(2491 mg g^(−1))toward PFOS,making it one of the most effective materials among the reported PFOS adsorbents.Moreover,the PFOS removal by iCOF-DGCl remains highly selective in the presence of disturbing anions,and the adsorbent could be well recovered for reuse.Mechanism studies have demonstrated that the Janus structure units of iCOF-DGCl form both hydrophobic and electrostatic interactions with the amphiphilic PFOS,thus achieving cooperative adsorption of PFOS.This work provides a facile approach based on Janus structure of COFs adsorbent for wastewater remediation. 展开更多
关键词 covalent organic framework Ionic polymer Perfluorooctane sulfonate Adsorption ADSORBENT
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Tumor-responsive covalent organic polymeric nanoparticles enhancing STING activation for cancer immunotherapy
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作者 Shuang Liang Jianjun Yao +3 位作者 Dan Liu Mengli Zhou Yong Cui Zhaohui Wang 《Chinese Chemical Letters》 2025年第3期357-362,共6页
The cyclic guanosine monophosphate-adenosine monophosphate synthase and the stimulator of interferon genes(cGAS-STING)has emerged as a promising target for cancer immunotherapy.However,the development of natural STING... The cyclic guanosine monophosphate-adenosine monophosphate synthase and the stimulator of interferon genes(cGAS-STING)has emerged as a promising target for cancer immunotherapy.However,the development of natural STING agonists is impeded by several challenges,including limited biostability,poor pharmacokinetics,and inefficient cytosolic delivery.Herein,we meticulously designed a doublelayer polyethylenimine(PEI)modified nanoscale covalent organic polymer(CPGP)for efficient delivery of 23cyclic guanosine monophosphate-adenosine monophosphate(cGAMP),a natural STING agonist.The double-layer PEI structured CPGP enhanced both the loading capacity and stability of cGAMP.Furthermore,CPGP improved the intracellular delivery efficiency and amplified the activation of STING pathway for the secretion of type-I interferon and pro-inflammatory cytokines.In contrast,single-layered nanoparticles failed to permit stable loading and intracellular delivery of cGAMP for immune response.The nano-STING agonist also mitigated the immunosuppressive tumor microenvironment(TME)by reducing regulatory T cells and polarizing M2 macrophages to the M1 phenotype,thereby creating an immune-supportive TME to enhance adaptive immune responses.The combination of CPGP and immune checkpoint blockers showed synergistic effect,further enhancing the inhibition effect on tumor growth.This double-layer PEI modified CPGP may offer a generalizable platform for other natural dinucleotide STING agonists to overcome the cascade delivery barriers,augmenting immune activation for tumor immunotherapy. 展开更多
关键词 IMMUNOTHERAPY covalent organic polymers Delivery STING agonists NANOPARTICLE
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Regulating local electron transfer environment of covalent triazine frameworks through F,N co-modification towards optimized oxygen reduction reaction
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作者 Quanyou Guo Yue Yang +6 位作者 Tingting Hu Hongqi Chu Lijun Liao Xuepeng Wang Zhenzi Li Liping Guo Wei Zhou 《Chinese Chemical Letters》 2025年第1期344-348,共5页
The high conductivity of electrocatalyst can eliminate the Schottky energy barrier at the interface of heterogeneous phases during an electrocatalytic reaction and accelerate the rapid electron transfer to the catalyt... The high conductivity of electrocatalyst can eliminate the Schottky energy barrier at the interface of heterogeneous phases during an electrocatalytic reaction and accelerate the rapid electron transfer to the catalytic active center.Therefore,the electronic conductivity is a vital parameter for oxygen reduction reaction(ORR).Covalent triazine frameworks(CTFs)have shown great potential application as electrocatalysts in ORR with a merit of the diverse building blocks.However,the intrinsic low conductivity and high impedance of CTFs could be significant setbacks in electrocatalytic application.Herein,CTFs were constructed by introducing F and N co-modification for efficient 2e^(-)ORR.Compared with the pristine CTF,the co-presence of F,N could increase the conductivity obviously by 1000-fold.As a result,F-N-CTF exhibits enhanced catalytic performance of H_(2)O_(2)generation and selectivity towards reaction pathways.This work reveals the importance of conductivity optimization for CTFs and provides guidance for designing high conductivity non-metallic organic semiconductor catalysts for 2e^(-)ORR. 展开更多
关键词 covalent triazine frameworks CONDUCTIVITY Co-modification ELECTROCATALYSIS Oxygen reduction reaction
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Facile scalable fabrication of triazine-based flexible covalent organic framework fiber film with multifunction at room temperature
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作者 Huimin Yan Yan Kou +4 位作者 Jiao Wang Shihui Zhang Nan Yin Wenhao Cui Quan Shi 《Journal of Energy Chemistry》 2025年第9期410-416,I0012,共8页
Flexible covalent organic framework(COF)film has drawn much attention as a promising functional material due to their unique molecular structure and self-supporting property.However,the traditional solvothermal method... Flexible covalent organic framework(COF)film has drawn much attention as a promising functional material due to their unique molecular structure and self-supporting property.However,the traditional solvothermal method of synthesizing flexible COF film is usually complicated,long-term duration and energy-consuming,making it unsuitable for scalable preparation.To address these limitations,a new method combining electrospinning and sacrificial template is proposed to quickly produce triazinebased COF fiber films at room temperature.The method is easy to operate and has a short reaction time(minimum 0.5 h)without dehydration and deoxygenation processes at room temperature,making it suitable for large-scale production(20 cm×30 cm).Different from the unprocessable of COF powder,COF films not only have good flexibility and mechanical properties,but also can be patterned with multiple functions to adapt to various application scenarios.Moreover,the functionality of triazine-structured COF is retained,enabling the use of the films in energy conversion and storage applications.Triazine-based COFs naturally have scalable conjugated structure,thus showing potential photocatalytic probability.Furthermore,the large pore structure of COF films enables loading of phase change materials endowing comprehensive properties of thermal management and flame retardance.This study proposes a strategy for the rapid synthesis of COF fiber films at room temperature and paves the way for multifunctional and high-performance COF based materials. 展开更多
关键词 covalent organic frameworks ELECTROSPINNING Photocatalysis Flame retardant Thermal management
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Covalent anchored Pd nanoclusters via a defect-mediated strategy for efficient alkaline hydrogen electrocatalysis
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作者 Guanghui Xia Huimin Xu +6 位作者 Yuchen Zhang Zhixiang Wang Ji Zhou Junyu Chen Yao Wang Yungui Chen Chaoling Wu 《Journal of Energy Chemistry》 2025年第12期346-353,I0010,共9页
The development of high-performance metal nanocluster catalysts is hindered by a fundamental stabilization-activity trade-off.Oxide supports often induce over-stabilization via insulating overlayers that block active ... The development of high-performance metal nanocluster catalysts is hindered by a fundamental stabilization-activity trade-off.Oxide supports often induce over-stabilization via insulating overlayers that block active sites,while conventional functionalized carbon supports suffer from thermodynamic instability and weak metal-support electronic coupling,leading to aggregation.Herein,a novel defectmediated covalent anchoring strategy is presented to immobilize transition metal(Pd,Ru,and Ir)NCs within ordered mesoporous carbon.This approach leverages intrinsic micropore defects to capture precursors and facilitate in-situ formation of direct metal-carbon covalent bonds.Controlled pyrolysis confines metal atom sintering into clusters within the mesopores,achieving high metal loading.This enrooted architectu re uniquely balances stability and activity:it avoids the excessive metal-carbon bonding detrimental to single-atom catalysts while maintaining sufficient,controllable interactions.The resulting Pd NCs catalyst exhibits exceptional hydrogen oxidation reaction activity,surpassing mass activity benchmarks of conventional Pt/C.Critically,this methodology decouples atomic-scale stabilization from catalytic site accessibility,resolving the long-standing activity-stability dilemma and providing a generalizable platform for fabricating stable,high-loading cluster catalysts with optimized electronic structures. 展开更多
关键词 NANO-CLUSTERS Metal-support interaction Alkaline hydrogen oxidation Palladium covalent anchoring
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Durable FEVE-based slippery coating for anti-corrosion/scaling:insights from covalent interpenetrating networks and multiple interfacial interactions
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作者 Xi-Guang Zhang Hao-Han Ning +6 位作者 Jing Jing Hao-Nan Liu Yu-Xin Fu Wei Zhang Chang Zhang Huai-Yuan Wang Zhan-Jian Liu 《Rare Metals》 2025年第9期6626-6642,共17页
Slippery liquid-infused porous surfaces(SLIPS)with exceptional liquid repellency and extremely low sliding angles demonstrate significant potential for applications in anti-corrosion,anti-fouling,and anti-scaling.Howe... Slippery liquid-infused porous surfaces(SLIPS)with exceptional liquid repellency and extremely low sliding angles demonstrate significant potential for applications in anti-corrosion,anti-fouling,and anti-scaling.However,the poor stability of the oil layer restricts its practical applications.Herein,a durable SLIPS coating with highly stable oil layer was developed by combining hierarchical porous structures with covalent interpenetrating networks and multiple interfacial interactions.The hierarchical porous structure was constructed via urea thermal decomposition with in situ hybridization of SiO_(2)and embedded carbon nanotubes(CNTs).Furthermore,the oil layer was chemically immobilized on the coating surface using methylenediphenyl diisocyanate(MDI)as a molecular bridge,leveraging interfacial covalent bonding andπ-OH interactions,which significantly enhanced its anti-corrosion properties,with an initial|Z|_(0.01 Hz)of1.22×10^(8)Ωcm^(2).Dynamic scaling experiments revealed a 96.47%improvement in scaling inhibition efficiency compared to conventional superhydrophobic coatings,showing its excellent anti-scaling properties.Owing to the durability and liquidity of oi layer,the prepared FEVE-SiO_(2)/CNTs@MDI SLIPS coating maintained outstanding slippery performance(water sliding angle<10°)even after 14 days of underwater immersion.Additionally,the coating also exhibited excellent thermal stability(120°C),remarkable shear resistance(5000 rpm),and ultraviolet resistance performance.Therefore,the prepared FEVE-SiO_(2)/CNTs@MDI SLIPS coating has broad practical application prospects in the field of industrial oilfield pipeline protection. 展开更多
关键词 covalent network Slippery surface SUPERHYDROPHOBICITY Anti-corrosion/scaling coating Durability
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Covalent organic framework/carbon black/molecularly imprinted polydopamine composites for the selective recognition and electrochemical detection of ciprofloxacin
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作者 Yufeng Sun Yongfeng Chen +3 位作者 Xiaomin Pang Geoffrey I.N.Waterhouse Xuguang Qiao Zhixiang Xu 《Food Science and Human Wellness》 2025年第7期2788-2796,共9页
In this work,a novel electrochemical sensor based on covalent organic framework@carbon black@molecularly imprinted polydopamine(COF@CB@MPDA)was developed for selective recognition and determination of ciprofloxacin(CF... In this work,a novel electrochemical sensor based on covalent organic framework@carbon black@molecularly imprinted polydopamine(COF@CB@MPDA)was developed for selective recognition and determination of ciprofloxacin(CF).COF@CB@MPDA possessed good water dispersibility and was synthesized by the selfpolymerization of dopamine under alkaline conditions in the presence of the COF,CB and CF.The high surface area COF enhanced the adsorption of CF,whilst CB gave the composites high electrical conductivity to improve the sensitivity of the proposed COF@CB@MPDA/glassy carbon electrode(GCE)sensor.The specific recognition of CF by COF@CB@MPDA involved hydrogen bonding and van der Waals interactions.Under optimized conditions,the sensor showed a good linear relationship with CF concentration over the range of 5.0×10^(–7)and 1.0×10^(–4)mol/L,with a limit of detection(LOD)of 9.53×10^(–8)mol/L.Further,the developed sensor exhibited high selectivity,repeatability and stability for CF detection in milk and milk powders.The method used to fabricate the COF@CB@MPDA/GCE sensor could be easily adapted for the selective recognition and detection of other antibacterial agents and organic pollutants in the environment. 展开更多
关键词 covalent organic framework Carbon black Molecular imprinted polydopamine Specific recognition Detection CIPROFLOXACIN
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