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Chinese Chemical Letters 2016年第12期27卷 1740-1744页

作者： Tian-Nan Wang Guang Yang Li-Bin Wu Guo-Song Chen The State Key Laboratory of Molecular Engineering of Polymers and Department of Macromolecular Science Fudan University

In this paper, dynamic covalent bond has been employed to construct supra-amphiphile of carbohydrate for the first time. In neutral environment, the molecule was fabricated by reacting a hydrophobic building block bearing benzoic aldehyde with a hydrophilic building block bearing hydrazine to form a sugar-containing supra-amphiphile based on acylhydrazone bond, The obtained azobenzene- galactopyranoside （Azo-Gal） supra-amphiphile self-assembled to fibrillar structure in water, which showed dual responses to UV light and pH.

关键词： Supra-amphiphile Self-assembly dynamic covalent bond Carbohydrate Dual responses

Cancer Therapy by Targeting Thioredoxin Reductase Based on Selenium-Containing dynamic covalent bond

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CCS Chemistry 2020年第3期2卷 225-235页

作者： Shuojiong Pan Jichun Yang Shaobo Ji Tianyu Li Shiqian Gao Chenxing Sun Huaping Xu Key Laboratory of Organic Optoelectronics and Molecular Engineering Department of ChemistryTsinghua UniversityBeijing 100084

Thioredoxin Reductase(TrxR)plays a pivotal role in defending cells against reactive oxygen species(ROS)and maintaining a reduced intracellular *** has been discovered that TrxR is elevated significantly in human cancer,evidenced by its association with the promotion of tumor cell proliferation,inhibiting tumor cell apoptosis,as well as enhancing tumor drug ***,finding highly selective inhibitors of TrxR is urgently ***,we developed a selenium-containing small molecule(EbD),which had two Se–N *** reduction conditions,the two Se–N bonds reacted with Se–H bond and S–H bond in TrxR to form new Se–Se bond and Se–S bonds,***,the newly formed bonds were able to disrupt the thioredoxin(Trx)reduction catalytic cycle,and thus,inhibited the TrxR activity irreversibly,which resulted in the collapse of the antioxidant *** a consequence,ROS levels elevated that triggered cancer cell *** strategy,based on selenium-containing dynamic covalent bonds,provides a new avenue for cancer therapy via targeting TrxR.

关键词： cancer therapy TrxR Selenium dynamic covalent bond ROS

A dynamic covalent bonding-based Nanoplatform for Intracellular Co-Delivery of Protein Drugs and Chemotherapeutics with Enhanced Anti-Cancer Effect

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Chinese Journal of Polymer Science 2024年第5期42卷 559-569,I0005页

作者： Sai-Nan Liu Jia-Hui Meng Li-Yun Cui Hua Chen Lin-Qi Shi Ru-Jiang Ma Key Laboratory of Functional Polymer Materials of Ministry of Education Institute of Polymer ChemistryTianjin Key Laboratory of Functional Polymer MaterialsState Key Laboratory of Medicinal Chemical BiologyFrontiers Science Center for New Organic MatterCollege of ChemistryNankai UniversityTianjin300071China Haihe Laboratory of Sustainable Chemical Transformations Tianjin300192China

Efficient intracellular delivery of protein drugs is critical for protein *** combination of protein drugs with chemotherapeutics represents a promising strategy in enhancing anti-cancer ***,co-delivery systems for efficient delivery of these two kinds of drugs are still lacking because of their different ***,we show a well-designed delivery system based on dynamic covalent bond for efficient intracellular co-delivery of ribonuclease A(RNase A)and doxorubicin(DOX).Two polymers,PEG-b-P(Asp-co-AspDA)and PAE-b-P(Asp-co-AspPBA),and two 2-acetylphenylboronic acid(2-APBA)-functionalized drugs,2-APBA-RNase A and 2-APBA-DOX,self-assemble into mixed-shell nanoparticles(RNase A/DOX@MNPs)via dynamic phenylboronic acid(PBA)-catechol bond between PBA and dopamine(DA)*** PBA-catechol bond endows the nanoparticles with high stability and excellent stimulus-responsive drug release *** the slight acidic environment at tumor tissue,RNase A/DOX@MNPs are positively charged,promoting their *** cellular uptake into endosome,further protonation of PAE chains leads to the rupture of endosomes because of the proton sponge effect and the cleavage of PBA-catechol bond promotes the release of two *** cytoplasm,the high level of GSH removed the modification of 2-APBA on *** restored RNase A and DOX show a synergistic and enhanced antic-cancer *** system may be a promising platform for intracellular co-delivery of protein drugs and chemotherapeutics.

关键词： Drug co-delivery Combination therapy dynamic covalent bond

An interfacial robust and entire self-healing ionogel-elastomer hybrid for elastic electronics enables discretionary assembly and reconfiguration

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Science China Chemistry 2024年第4期67卷 1316-1323页

作者： Lei Yang Lijie Sun Hongfei Huang Rasoul Esmaeely Neisiany Zhengwei You State Key Laboratory for Modification of Chemical Fibers and Polymer Materials Institute of Functional MaterialsCollege of Materials Science and EngineeringDonghua UniversityResearch Base of Textile Materials for Flexible Electronics and Biomedical Applications(China Textile Engineering Society)Shanghai Engineering Research Center of Nano-Biomaterials and Regenerative MedicineShanghai 201620China Department of Polymer Engineering Hakim Sabzevari UniversitySabzevar ***Iran Biotechnology Centre Silesian University of TechnologyGliwice 44-100Poland

Inspired by the multi-layer architecture of mammal skins,interfacial robust,stretchable,and entirely healable gel-elastomer hybrids hold great potential in diverse fields including biomedical devices,wearable electrical devices,and soft ***,existing gel-elastomer hybrids have numerous limitations including low interfacial bonding toughness,complex and time-consuming preparation process,unhealable,and ***,we propose a simple and general chemical strategy through the interfacial dynamic bonding between gel and elastomer to simultaneously address the abovementioned *** covalent bonds readily and repeatably covalent bonding ionogel and elastomer(interfacial toughness:390 J m^(-2)),endowed the hybrids with entire self-healing features like skin and enabled discretionary assembly and ***,this strategy resolved the troublesome contradiction between interfacial stability and *** advantage of the aforementioned features,we readily constructed a multi-module,self-healing,self-powered,and realtime monitoring of personal status integrated elastic electronics,which could simply reconfigure the output signal of elastic electronics into an input signal of the devices-braille keyboard.

关键词： ionogel elastomer interface bonding self-healing dynamic covalent bond

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Aggregates of fluorescent gels assembled by interfacial dynamic bonds

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聚集体(英文)

聚集体(英文) 2023年第2期4卷 83-101页

作者： Ziqing Hu Shaoyu Xu Hanwei Zhang Xiaofan Ji Key Laboratory of Materials Chemistry for Energy Conversion and Storage Ministry of EducationHubei Key Laboratory of Materials Chemistry and Service FailureSchool of Chemistry and Chemical EngineeringHuazhong University of Science and TechnologyWuhanChina

Life,defined as the specific form of substance,is an integration of aggregates at various scales,ranging from single molecules to ***,these building blocks of common aggregates are usually recognized as confining at the microscopic level,while there are few studies focusing on macroscopic building blocks for *** gels,as the important macroscopic building blocks,are drawing researchers’attention on account of their extraordinary fluorescence as well as soft material *** by nature,fluorescent gels can be aggregated through interfacial *** to the driving forces for interfacial adhesion,a series of aggregates of fluorescent gels(AFGs)was summarized,including H-bond,metal coordinations,host-guest interactions,hydrophobic interactions,electrostatic interactions,dynamic covalent bonds as well as multiple driving *** AFGs own dynamic assembled behaviors and rich stimuli responsiveness,which could be applied to information storage,sensing,biomedical systems,and so *** authors anticipate this review can accelerate the development of aggregate science,especially based on macroscopic building blocks.

关键词： aggregation-induced emission assembly dynamic covalent bond fluorescent gel interfacial adhesion noncovalent interactions

Detachable and hierarchical assemblies for recyclable and highly efficient oil-fouling removal

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Nano Research 2023年第2期16卷 2551-2562页

作者： Tengda Wang Shaoying Dai Jie Wang Bin Liu Meiwen Cao Bo Guan Yuchun Han Yilin Wang CAS Key Laboratory of Colloid Interface and Chemical ThermodynamicsBeijing National Laboratory for Molecular Sciences(BNLMS)CAS Research/Education Center for Excellence in Molecular SciencesInstitute of ChemistryChinese Academy of SciencesBeijing 100190China University of Chinese Academy of Sciences Beijing 100049China State Key Laboratory of Heavy Oil Processing Department of Biological and Energy Chemical EngineeringCollege of Chemical EngineeringChina University of Petroleum(East China)Qingdao 266580China

Large-scale use of detergents to remove oil-fouling in industry continuously generates tremendous amounts of wastewater and thus leads to both economic and environmental *** develop recyclable oil-fouling removal strategy is an appealing solution but a challenging ***,a kind of dynamic imine-based surfactant has been constructed by 2-formylbenzenesulfonic acid sodium salt(FBSS)and linear amines(CnNH_(2),n=6,7,8,10,and 12).Owing to high interfacial activity and strong assembly ability,dynamic FBSS/C8NH_(2)system can remove oil-fouling on multiple substrates for at least 10 cycles,largely reducing the toxicity to *** basic pH,the hierarchical assemblies(from vesicle to network and hollow sphere)are formed and boost surfactant molecule enrichment around oil-fouling,leading to highly efficient *** pH is changed to acidic condition,the surfactant molecules dissociate due to the breaking of imine bonds,and accordingly the emulsion is destroyed and the released oil droplets float to the top *** removing the oil-fouling and adjusting the solution back to basic pH,the surfactant assemblies are reconstructed and used for the next oil-fouling cleaning *** study provides a recyclable,efficient and eco-friendly oil-fouling removal approach,satisfying the need of sustainable development.

关键词： dynamic covalent bond hierarchical assembly oil-fouling removal emulsion oil/water separation

Configurational Selectivity Study of Two-dimensional covalent Organic Frameworks Isomers Containing D2h and C2 Building Blocks

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Chemical Research in Chinese Universities 2022年第2期38卷 639-642页

作者： ZHENG Xuhan ZHANG Lin XIE Chenxiao WANG Hui LIU Hui PAN Qingyan ZHAO Yingjie College of Polymer Science and Engineering Qingdao University of Science and TechnologyQingdao 266042P.R.China

The isomerization of covalent organic frameworks(COFs) materials is still a mysterious and attractive topic. Diversified monomer structures are still urgently needed to explore the in-depth mechanism of isomerization in these special COFs. This work provides a new D2h monomer for the construction of [D2h+C2] 2D COFs isomers. A new D2h monomer adopted here was proven to tend to form a single pore framework structure.

关键词： covalent organic framework Isomerization Kagome dynamic covalent bond

Thermal- and Light-driven Metathesis Reactions Between Different Diselenides

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Chemical Research in Chinese Universities 2022年第2期38卷 516-521页

作者： KANG Xiaoying YUAN Yuan XU Huaping CHEN Yulan Tianjin Key Laboratory of Molecular Optoelectronic Science Department of ChemistryTianjin UniversityTianjin 300354P.R.China Key Laboratory of Organic Optoelectronics and Molecular Engineering Department of ChemistryTsinghua UniversityBeijing 100084P.R.China

Thermal- and light-driven diselenide metathesis reactions with different types of diselenides are investigated systematically. Their exchange reaction rates and equilibrium conversions are compared in the aspects of the different diselenide structures, activation conditions and solvents. As a result, the metathesis reactions between diselenide small molecules are demonstrated with high dynamic and sensitive features, which can be broadly tuned by varying the electron affinity and aromaticity of the diselenide substituents and external conditions(e.g., solvent, stimulus mode). The current work thus will not only advance our understanding on diselenide metathesis chemistry, but also promote concrete and impactful studies in selenium-containing materials.

关键词： dynamic covalent bond Metathesis Diselenide

Self-assembly behavior of disaccharide-containing supra-amphiphiles

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Chinese Chemical Letters 2023年第1期34卷 373-377页

作者： Zhenfei Gao Tiannan Wang Zikun Rao Hui Yan Ran Zhang Guosong Chen The State Key Laboratory of Molecular Engineering of Polymers and Department of Macromolecular Science Fudan UniversityShanghai 200433China Changchun Institute of Applied Chemistry Chinese Academy of SciencesChangchun 130022China School of Pharmaceutical Sciences Liaocheng UniversityLiaocheng 252059China

In this paper,supra-amphiphilic compounds containing disaccharides and azobenzene ends have been constructed via dynamic covalent *** was found that the slight structural difference of the disaccharides made significant difference in the self-assembled ***,three kinds of azodisaccharide supra-amphiphiles were found to assemble into different morphologies,with the only difference in chemical structure from the *** importantly,the structural difference between the disaccharides,including lactoside,maltoside and cellobioside was *** simulation revealed the packing of molecules was due to the different contribution from hydrogen *** above results clearly indicated the contribution of saccharide packing,especially the related hydrogen bonding,to the final morphology of the assembled structures.

关键词： Supra-amphiphile Disaccharide Self-assembly dynamic covalent bond Molecular dynamics simulation

"Solid-Liquid" Vitrimers Based on dynamic Boronic Ester Networks

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Chinese Journal of Polymer Science 2021年第10期39卷 1292-1298,I0006页

作者： Sheng Wang Lu-Lu Xue Xiao-Zhuang Zhou Jia-Xi Cui INM-Leibniz Institute for New Materials Campus D22 Saarbrucken 66123Germany Beijing National Laboratory for Molecular Sciences Key Laboratory of Polymer Chemistry and Physics of Ministry of EducationCollege of Chemistry and Molecular EngineeringPeking UniversityBeijing 100871China Institute of Fundamental and Frontier Sciences University of Electronic Science and Technology of ChinaChengdu 610054China

The"solid-liquid"behavior of vitrimers have not been systematically ***,a series of"solid-liquid"vitrimers bearing varying contents of dynamic boronic ester bonds were synthesized via thiol-ene click *** vitrimers allow for flexibile modulation of their network structures and thus show a range of intriguing properties including high stretchability,flexible transition from elasticity to plasticity,strong strain rate dependence,and solid-liquid *** dynamic association rate of boronic ester bonds within these vitrimers could be apparently accelerated via increasing the content of boronic ester,which could be used to shape-program the flat vitrimer films into various complex 3D structures just with external *** with such versatile dynamic behavior may open up a range of new applications.

关键词： Solid-liquid dynamic covalent bond Boronic ester bond Strain-rate dependent High stretchability