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Chinese Chemical Letters 2022年第5期33卷 2464-2468页

作者： Xiang-Hao Han Jia-qi Chu Wen-Zhuang Wang qiao-yan qi Xin Zhao Key Laboratory of Synthetic and Self-Assembly Chemistry for Organic Functional Molecules Center for Excellence in Molecular SynthesisShanghai Institute of Organic ChemistryUniversity of Chinese Academy of SciencesChinese Academy of SciencesShanghai 200032China Shanghai Normal University Shanghai 200234China

Covalent organic frameworks(COFs),as a novel class of functional polymers,exhibit versatile applica-tions due to their crystalline porous structures and conjugated ***,synthesis of COFs with high crystallinity still faces great challenges,especially for scale-up *** we report a two-step solvothermal process to improve crystallinity of *** first step focuses on polycondensa-tion of monomers with no need for optimizing crystallization *** the second step,appropriate solvothermal conditions are used to facilitate crystallization of the COFs through defects correction and structural ***,this strategy could also be applicable to scale-up synthesis of high qual-ity COFs,which lays a foundation for their practical applications.

关键词： Covalent organic frameworks Synthesis Solvothermal condensation High crystallinity Scale-up preparation

Designed Synthesis of a Two-Dimensional Covalent Organic Framework with Three-Level Hierarchical Porosity

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Chinese Journal of Chemistry 2020年第12期38卷 1676-1680页

作者： Xiang-Hao Han qiao-yan qi Zhi-Bei Zhou Xin Zhao Key Laboratory of Synthetic and Self-Assembly Chemistry for Organic Functional Molecules Center for Excellence in Molecular SynthesisShanghai Institute of Organic ChemistryUniversity of Chinese Academy of SciencesChinese Academy of Sciences345 Lingling RoodShanghai 200032China

of main observation and conclusion Covalent organic frameworks(COFs)with hierarchical porosity have drawn considerable attention very recently due to their advantages over the COFs with uniform porosity in some ***,the design strategies for the construction of this type of COFs,namely heteropore COFs,are quite *** herein report a facile approach to constructing a two-dimensional COF which possesses three different kinds of *** structure is confirmed by powder X-ray diffraction and nitrogen sorption *** successful construction of the triple-pore COF represents a new method to access COFs with high hierarchical porosity.

关键词： porosity valent constructing

Effects of connecting sequences of building blocks on reticular synthesis of covalent organic frameworks

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Nano Research 2021年第2期14卷 381-386页

作者： De-Li Ma Cheng qian qiao-yan qi Zhong-Ri Zhong Guo-Fang Jiang Xin Zhao State Key Lab of Chemo/Biosensing and Chemometrics College of Chemistry and Chemical EngineeringHunan Universityf Changsha 410082China Key Laboratory of Synthetic and Self-Assembly Chemistry for Organic Functional Molecules Center for Excellence in Molecular SynthesisShanghai Institute of Organic ChemistryChinese Academy of Sciences345 Lingling RoadShanghai 200032China

The principle of reticular chemistry has been widely used to guide the design of crystalline porous materials such as metal organic frameworks(MOFs)and covalent organic frameworks(COFs).While in the early strategies only the symmetries of the building blocks were considered for reticular synthesis of COFs,recently a few researches on COFs with hierarchical porosities indicate that connecting sequence of building blocks also plays a crucial role in determining crystalline structures of ***,this important phenomenon has not been systematically investigated *** this article,a model system has been established to demonstrate how different connecting sequences of two C_(2v)-symmetric building blocks lead to the formation of four two-dimensional(2D)COFs with distinct framework *** verify this concept,target synthesis was conducted to produce three COFs,whose structures were confirmed by powder X-ray diffraction and pore size distribution analysis.

关键词： reticular chemistry covalent organic framework connecting sequence building block

A heteropore covalent organic framework for adsorptive removal of Cd(Ⅱ) from aqueous solutions with high efficiency

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Chinese Chemical Letters 2020年第2期31卷 386-390页

作者： Na Liu Liangfeng Shi Xianghao Han qiao-yan qi Zong-Quan Wu Xin Zhao Department of Polymer Science and Engineering School of Chemistry and Chemical Engineeringand Anhui Key Laboratory of Advanced Catalytic Materials and Reaction EngineeringHefei University of TechnologyHefei 230009China CAS Key Laboratory of Synthetic and Self-Assembly Chemistry for Organic Functional Molecules Center for Excellence in Molecular SynthesisShanghai Institute of Organic ChemistryChinese Academy of SciencesShanghai 200032China

A heteropore covalent organic framework(COF) integrating tetraphenylethene skeleton and catechol segment is designed and *** 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.

关键词： Covalent organic frameworks Heteropore Hierarchical porosity Cd(Ⅱ)removal Water treatment

A luminescent one-dimensional covalent organic framework for organic arsenic sensing in water

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Chinese Chemical Letters 2024年第11期35卷 304-308页

作者： Chao Liu Chao Jia Shi-Xian Gan qiao-yan qi Guo-Fang Jiang Xin Zhao Advanced Catalytic Engineer Research Center of the Ministry of Education College of Chemistry and Chemical EngineeringHunan UniversityChangsha 410082China Key Laboratory of Synthetic and Self-Assembly Chemistry for Organic Functional Molecules Shanghai Institute of Organic ChemistryChinese Academy of SciencesShanghai 200032China

Roxarsone(ROX)is a commonly used antibacterial and growth-promoting additive to animal *** development of an effective method for detecting ROX and its conversion products is of importance because of their potential harm to human health and ***,we report the designed synthesis of a novel one-dimensional covalent organic framework(1D COF),named EP-COF,and its application as a fluorescent probe for ROX ***-COF is constructed based on imine linkages,exhibiting high crystallinity,strong fluorescence emission,and good dispersibility in *** displays a remarkable capability to efficiently detect ROX,with an impressive detection limit of 4.5 nmol/***,EP-COF also offers advantages of excellent selectivity,and high structural *** work not only presents a promising approach for the detection of harmful substances like ROX,but also serves as a valuable reference for exploring application of 1D COFs in chemical sensing.

关键词： One-dimensional Covalent organic framework Fluorescent probe Roxarsone Sensing

Converting Azine Linkage into Highly Stable(Thio)Urea-Based Bicyclic-Fused-Ring Connections in Covalent Organic Frameworks via Criss-Cross[3+2]Cycloaddition

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CCS Chemistry 2024年第9期6卷 2230-2240页

作者： Zhi-Bei Zhou Hui-Hui Sun qiao-yan qi Xin Zhao Key Laboratory of Synthetic and Self-Assembly Chemistry for Organic Functional Molecules Shanghai Institute of Organic ChemistryUniversity of Chinese Academy of SciencesChinese Academy of SciencesShanghai 200032

Exploring new linkage chemistry is of fundamental significance for covalent organic frameworks(COFs)to expand their structure and functional ***,we report a strategy for converting azine linkage into urea-and thiourea-based fused-ring connections in COFs by criss-cross[3+2]dipolar cycloaddition of azine with HNCO or *** as-prepared COFs with cyclized linkages exhibited enhanced chemical and thermal stability by locking the dynamic C=N linkages in the ***,functions could be introduced into the skeleton of COFs by this postsynthetic cyclization method,which enabled significant improvements in functionality,demonstrated by the studies on CO_(2)/N_(2) selective sorption,proton conduction,and Hg^(2+)*** use of this[3+2]cycloaddition strategy not only enriched the chemistry of linkage conversion for COFs but also offered a new way to fabricate fused-ring-linked COFs,thereby representing a high level of controllability on connectivity and functionality of COFs.

关键词： covalent organic frameworks linkage chemistry structural transformation [3+2]cycloaddition azine

A supramolecular bottlebrush polymer assembled on the basis of cucurbit[8]uril-encapsulation-enhanced donor-acceptor interaction

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Chinese Chemical Letters 2017年第6期28卷 1167-1171页

作者： Zhi-Jian Yin Zong-Quan Wu Feng Lin qiao-yan qi Xiao-Na Xu Xin Zhao Department of Polymer Science and Engineering School of Chemistry and Chemical EngineeringHefei University of Technology Key Laboratory of Synthetic and Self-assembly Chemistry for Organic Functional Molecules Shanghai Institute of Organic ChemistryChinese Academy of Sciences

A supramolecular bottlebrush polymer has been constructed in water through the self-assembly of a rigid electron-deficient building block and an electron-rich monomer which bears two tetraethylene glycol chains,driven by CB[8]-encapsulation-enhanced donor-acceptor *** as-formed supramolecular bottlebrush polymer has been characterized by -1H NMR titration experiment,UV-vis spectroscopy,DLS and 2D -1H NMR DOSY.

关键词： Self-assembly Supramolecular polymer Cucurbituril Donor-acceptor interaction Bottlebrush polymer

A Study on Constitutional Isomerism in Covalent Organic Frameworks:Controllable Synthesis,Transformation,and Distinct Difference in Properties

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CCS Chemistry 2020年第2期2卷 139-145页

作者： Rong-Ran Liang Fu-Zhi Cui Ru-Han A qiao-yan qi Xin Zhao Key Laboratory of Synthetic and Self-Assembly Chemistry for Organic Functional Molecules Center for Excellence in Molecular SynthesisShanghai Institute of Organic ChemistryChinese Academy of SciencesShanghai 200032China

Isomerism is an essential and widespread phenomenon in organic chemistry but rarely observed in covalent organic frameworks(COFs),a novel class of crystalline porous organic polymers with versatile ***,we give an account of the first example of a controllable synthesis of constitutional isomers of a *** two isomers exhibited marked differences in their gas/vapor adsorption behaviors and chemical stability in various ***,structure transformation from one isomer to the other was *** work not only paves the way for rational design and synthesis of COF isomers but also provides a vivid example of structure–property relationship in crystalline porous polymers.

关键词： covalent organic framework constitutional isomer controllable synthesis isomeric transformation adsorption behavior

Toward a Two-Dimensional Supramolecular Organic Framework with High Degree of Internal Order via Amphiphilic Modification

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CCS Chemistry 2022年第1期4卷 141-150页

作者： Zhi-Jian Yin Shu-yan Jiang Na Liu qiao-yan qi Zong-Quan Wu Tian-Guang Zhan Xin Zhao Key Laboratory of Synthetic and Self-Assembly Chemistry for Organic Functional Molecules Center for Excellence in Molecular SynthesisShanghai Institute of Organic ChemistryChinese Academy of SciencesShanghai 200032 Department of Polymer Science and Engineering School of Chemistry and Chemical EngineeringHefei University of TechnologyAnhui ProvinceHefei 230009 Key Laboratory of the Ministry of Education for Advanced Catalysis Materials College of Chemistry and Life SciencesZhejiang Normal UniversityJinhua 321004

Solution-phase self-assembly of two-dimensional(2D)networks with a high degree of internal order and long-range periodicity is a great ***,we report a rational design to improve 2D self-assembly in water through amphiphilic modification of the building *** amphiphilic tritopic molecule(1)is designed and synthesized by introducing three hydrophilic oligo(ethylene glycol)moieties and three hydrophobic hexyl *** assembly of 1 and cucurbit[8]uril(CB[8])leads to the formation of a Janus 2D supramolecular organic framework(SOF),which further creates unique bilayer supramolecular networks and exhibits an unprecedentedly high degree of internal order and long-range *** contrast,the assembly of a nonamphiphilic analog(2)with CB[8]only generates a 2D SOF with a lower degree of internal order,suggesting that the inherent amphiphilicity of 1 plays a crucial role in improving its 2D self-assembly in aqueous phase.

关键词： self-assembly supramolecular organic frameworks two-dimensional amphiphilicity internal order

A self-assembled framework that interpenetrates in crystal but does not interpenetrate in solution

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Science China Chemistry 2021年第7期64卷 1228-1234页

作者： Bo yang Jian-Wei Zhang Shang-Bo Yu Ze-Kun Wang Pan-qing Zhang Xiao-Di yang qiao-yan qi Guan-Yu yang Da Ma Zhan-Ting Li College of Chemistry Zhengzhou UniversityZhengzhou 450001China Innovation Research Institute of Traditional Chinese Medicine Shanghai University of Traditional Chinese MedicineShanghai 201203China Key Laboratory of Synthetic and Self-Assembly Chemistry for Organic Functional Molecules Shanghai Institute of Organic ChemistryChinese Academy of SciencesShanghai 200032China Department of Chemistry Fudan UniversityShanghai 200438China

A porous supramolecular framework has been for the first time revealed to undergo interpenetration in crystal and noninterpenetration in solution.A new supramolecular organic framework Bu-SOF has been constructed from the co-assembly of a tetracationic tetrahedral monomer and cucurbit[8]uril(CB[8])in water through the encapsulation of two anti-parallel n-butyl chains by CB[8].X-ray diffraction analysis reveals that Bu-SOF forms 3-fold interpenetrated networks in crystals grown by evaporation of its solution in water.1 H NMR,dynamic light scattering and isothermal titration calorimetric experiments confirm that Bu-SOF is also formed in *** samples,prepared by lyophilizing the aqueous solution of Bu-SOF,can adsorb nanoscaled organic dyes,supporting the porosity of the framework and thus non-interpenetration in *** avoidance of interpenetration of Bu-SOF in solution has been attributed to the filling of water inside the porous framework as well as the electrostatic repulsion of the appended bipyridinium units of the tetrahedral building block.

关键词： supramolecular organic framework cucurbituril crystal interpenetration non-interpenetration