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Cement-inspired readily fabricated water-strengthened polymeric materials

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Science China Chemistry 2024年第10期67卷 3458-3467页

作者： Han Zuo Luzhi Zhang Huixia Xuan Shijia Gu Xinxin Xu Rasoul Esmaeely Neisiany Qilin Wu 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 Key Laboratory of Lightweight CompositeShanghai Engineering Research Center of Nano-Biomaterials and Regenerative MedicineShanghai 201620China Zhejiang Hexin Science and Technology Co. Ltd.Jiaxing 314033China Biotechnology Centre Silesian University of TechnologyKrzywoustego 844-100 GliwicePoland Department of Polymer Engineering Hakim Sabzevari UniversitySabzevar ***Iran

Polymeric materials have penetrated all aspects of society and play an irreplaceable ***,there is an inherent contradiction between their mechanical properties and processing ***,inspired by cement,a crucial construction material renowned for its excellent fabricating behavior and self-strengthening properties,we have developed dynamic crosslinked poly(oxime-urethane)(CPOU).The synthesized CPOU showed good self-healing ability and 3D printability owing to the dynamic dissociation and re-association of oxime-carbamate *** objects printed through the fused deposition modeling technique were able to be readily assembled into complex architectures through intrinsic ***,the self-strengthening of CPOU was successfully realized through multiple-step tandem *** dissociation of dynamic oxime-carbamate bonds produced–NCO groups,which reacted with the surrounding water to form polar urea bonds in the polymer network,leading to an increase in the tensile strength of CPOU from 11.95 to 19.37 *** work not only develops the polymers with combined self-healing,facile fabricating,and self-strengthening properties but also provides a new molecular strategy to modulate the properties of polymers,which could be potentially applied in diverse areas.

关键词： dynamic bonds 3D printing self-strengthening self-healing

Interplay of Crosslinking Structures and Segmental dynamics in Solid-Liquid Elastomers

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Chinese Journal of Polymer Science 2022年第10期40卷 1297-1306,I0012页

作者： Hao Wang Wan-Su Peng Qi Wu Yan Zhao Shi-Tai Wang Yi Yang Jin-Rong Wu Xiao-Liang Wang Rong-Chun Zhang South China Advanced Institute for Soft Matter Science and Technology(AISMST) School of Emergent Soft MatterSouth China University of TechnologyGuangzhou 510640China Key Laboratory of High-Performance Polymer Materials and Technology of Ministry of Education Department of Polymer Science and EngineeringSchool of Chemistry and Chemical EngineeringNanjing UniversityNanjing 210093China State Key Laboratory of Polymer Materials Engineering College of Polymer Science and EngineeringSichuan UniversityChengdu 610065China Suzhou Niumag Analytical Instrument Corporation Chengdu 610065China Guangdong Provincial Key Laboratory of Functional and Intelligent Hybrid Materials and Devices South China University of TechnologyGuangzhou 510640China

There have been significant interests in recent years for incorporating dynamic bonds into polymer materials for achieving multiple functionalities,such as self-healing,recycling,stimuli-responsiveness,and so ***,the impact of dynamic bonds on the polymer dynamics is actually less *** this study,we investigate a self-healing solid-liquid elastomer(SLE),which is a dual-crosslinked network made by coupling a permanently crosslinked polydimethylsiloxane(PDMS)network with polyborosiloxane(PBS)via abundant dynamic boron/oxygen dative *** double-quantum(DQ)NMR reveals that the crosslinking degree is reduced while the structural heterogeneity of network is enhanced with increasing PBS content,i.e.,increasing the content of dynamic boron/oxygen dative *** experiments clearly reveal two chain relaxation modes in the SLE samples with a characteristic relaxation time of around 2.1 s and 11.8 s,corresponding to the relaxation of coupled PBS and PDMS chains,*** master curves obtained from variable-temperature frequency-dependent rheological experiments also reveal enhanced heterogeneity of chain relaxation with increasing PBS ***,the impact of boron/oxygen dative bonds on the Rouse dynamics is further revealed by fast-field-cycling(FFC)NMR experiments,where the spinlattice relaxation rate(R_(1))of all SLE samples follows the same power law of R_(1)(ω)∝ω^(-0.33).Nevertheless,the incorporation of PBS did slightly increase the energy barrier of Rouse *** study well demonstrates a combined use of rheology and solid-state NMR spectroscopy can provide piercing insights into the interplay of crosslinking structures and dynamics of polymer materials.

关键词： Fast-field-cycling NMR Multiple-quantum NMR Rheology dynamics dynamic bonds

dynamic Crosslinked Phosphorescent Poly(vinyl alcohol)-Terpyridine Films with Enhanced Mechanical Properties and Tunable Shape Memory

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Chinese Journal of Polymer Science 2024年第10期42卷 1595-1601,I0015页

作者： Meng Wei Wei-Hao Feng Chen Yu Zhen-Yi Jiang Guang-Qiang Yin Wei Lu Tao Chen Key Laboratory of Advanced Marine Materials Ningbo Institute of Materials Technology and EngineeringChinese Academy of SciencesNingbo315201China School of Chemical Sciences University of Chinese Academy of SciencesBeijing100049China School of Materials Science and Chemical Engineering Ningbo UniversityNingbo315211China

Achieving versatile room temperature phosphorescence(RTP)materials,especially with tunable mechanical properties and shape memory is attractive and essential but rarely ***,a strategy was reported to realize multi-functional RTP films with multicolor fluorescence,ultralong afterglow,adjustable mechanical properties,and shape memory through the synergistic dynamic interaction of lanthanide(Ln~Ⅲ)-terpyridine coordination,borate ester bonds,and hydrogen bondings in a poly(vinyl alcohol)(PVA)*** varying the amount of borax,the mechanical properties of the films could be finely controlled due to the change of crosslinking degree of dynamic borate ester bonds in *** assembly and disassembly of borate ester bonds upon the trigger of borax and acid were applied as reversible linkage to achieve programmable shape memory *** addition,the films displayed both fascinating multicolor fluorescence and ultralong afterglow characteristics due to the presence of Ln III doping and confinement of terpyridine in *** study provides a new avenue to impart modulable mechanical strength and shape memory to RTP materials.

关键词： Room temperature phosphorescence materials dynamic bonds Multicolor fluorescent Tunable mechanical properties Shape memory

Engineering the viscoelasticity of gelatin methacryloyl(GelMA)hydrogels via small“dynamic bridges”to regulate BMSC behaviors for osteochondral regeneration

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Bioactive Materials 2023年第7期25卷 445-459页

作者： Changjiang Liu Qifan Yu Zhangqin Yuan Qianping Guo Xiting Liao Feng Han Tao Feng Guoping Liu Runze Zhao Zhuang Zhu Haijiao Mao Caihong Zhu Bin Li College of Chemistry Chemical Engineering and Materials ScienceOrthopaedic InstituteDepartment of Orthopaedic SurgeryThe First Affiliated HospitalSuzhou Medical CollegeSoochow UniversitySuzhouJiangsuChina Department of Orthopaedic Surgery The Affiliated Hospital of Medical SchoolNingbo UniversityNingboZhejiangChina Collaborative Innovation Center of Hematology Soochow UniversitySuzhouJiangsuChina

The dynamic extracellular matrix(ECM)constantly affects the behaviors of *** mimic the dynamics of ECM with controllable stiffness and energy dissipation,this study proposes a strategy in which a small molecule,3,4-dihydroxybenzaldehyde(DB),was used as fast"dynamic bridges"to construct viscoelastic gelatin methacryloyl(GelMA)-based *** storage modulus and loss modulus of hydrogels were independently adjusted by the covalent crosslinking density and by the number of dynamic *** hydrogels exhibited self-healing property,injectability,excellent adhesion and mechanical ***,the in vitro results revealed that the viscous dissipation of hydrogels favored the spreading,proliferation,osteogenesis and chondrogenesis of bone marrow mesenchymal stem cells(BMSCs),but suppressed their ***-sequencing and immunofluorescence suggested that the viscous dissipation of hydrogels activated Yes-associated protein(YAP)by stabilizing integrinβ1,and further promoted nuclear translocation of smad2/3 andβ-catenin to enhance chondrogenesis and *** a result,the viscoelastic GelMA hydrogels with highest loss modulus showed best effect in cartilage and subchondral bone *** together,findings from this study reveal an effective strategy to fabricate viscoelastic hydrogels for modulating the interactions between cells and dynamic ECM to promote tissue regeneration.

关键词： Viscoelastic hydrogels dynamic bonds GelMA Dissipation Osteochondral regeneration

Mechanically skin-like and water-resistant self-healing bioelastomer for high-tension wound healing

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Bioactive Materials 2024年第9期39卷 443-455页

作者： Jinyi Huang Hongying Chen Zenghui Jia Xingqi Song Sinan Wang Baoshuai Bai Jian Wang Junfeng Zhang Guangdong Zhou Dong Lei Department of Plastic and Reconstructive Surgery Department of CardiologyShanghai Key Lab of Tissue EngineeringShanghai 9th People’s HospitalShanghai Jiao Tong University School of MedicineShanghai200011PR China Research Institute of Plastic Surgery Shandong Second Medical UniversityWeifangShandong261053PR China

The biomedical application of self-healing materials in wet or(under)water environments is quite challenging because the insulation and dissociation effects of water molecules significantly reduce the reconstruction of material–interface *** closure with uniform tension of high-tension wounds is often difficult,leading to further deterioration and ***,a new type of thermosetting water-resistant self-healing bioelastomer(WRSHE)was designed by synergistically incorporating a stable polyglycerol sebacate(PGS)covalent crosslinking network and triple hybrid dynamic networks consisting of reversible disulfide metathesis(SS),and dimethylglyoxime urethane(Dou)and hydrogen *** a resveratrol-loaded WRSHE(Res@WRSHE)was developed by a swelling,absorption,and crosslinked network locking *** exhibited skin-like mechanical properties in terms of nonlinear modulus behavior,biomimetic softness,high stretchability,and good elasticity,and they also achieved ultrafast and highly efficient self-healing in various liquid *** wound-healing applications of high-tension full-thickness skin defects,the convenient surface assembly by self-healing of WRSHEs provides uniform contraction stress to facilitate tight ***,Res@WRSHEs gradually release resveratrol,which helps inflammatory response reduction,promotes blood vessel regeneration,and accelerates wound repair.

关键词： Underwater self-healing dynamic bonds Bioelastomer High-tension wounds Resveratrol

dynamic chemistry in ionic liquid-based conductor

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Green Chemical Engineering 2021年第4期2卷 346-358页

作者： Zhiwu Chen Qinyuan Gui Yapei Wang Department of Chemistry Renmin University of ChinaBeijing100872China

Ionic liquids,as a kind of liquid conductors with the unique inherent abilities of rapid self-healing,highly adaptive deformation,reconstruction,as well as high ionic conductivity,have been highly praised and recommended as a new competitive conducting material for green ***,ionic liquids are likely encountered with the leakage problems when they are integrated into electronic *** issue as well as the need to develop intelligent electronics stimulate the innovation of ionic liquids with response characters besides conducting ***"innovative"or"functional"ionic liquids consisting dynamic chemical bonds can reversibly switch between different states in response to external *** specialized ionic liquids afford powerful supplements to minimize the issue of leakage of ionic liquid conductors from electrical circuits,and also exhibit the properties of self-healing,reprocessing,adaptive deformation,which accord with the forthcoming era of Internet of *** minireview systematically summarizes the progresses of ionic liquid-based conductors containing dynamic bonds,particularly highlighting their applicable merits in self-healing,stretchable,and recyclable *** also discuss the challenges in the next period and describe an unambiguous future of this research area.

关键词： Ionic liquid Conductor dynamic bonds Self-healing Recycle Stimuli-responsive

Skin-Inspired Electronics Enabled by Supramolecular Polymeric Materials

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CCS Chemistry 2019年第4期1卷 431-447页

作者： Kai Liu Yuanwen Jiang Zhenan Bao Xuzhou Yan School of Chemistry and Chemical Engineering Shanghai Jiao Tong UniversityShanghai 200240China Department of Chemical Engineering Stanford UniversityStanfordCA 94305United States

Next-generation electronics that intimately interact with the human body would play crucial roles in future health monitors and early disease ***-inspired electronics have been rapidly growing in the past decade to em... 详细信息

关键词： electronic skins supramolecular polymers mechanical adaptability conductive materials dynamic bonds

Self-healing materials enable free-standing seamless large-scale 3D printing

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Science China Materials 2021年第7期64卷 1791-1800页

作者： Han Zuo Zenghe Liu Luzhi Zhang Gengxin Liu Xikai Ouyang Qingbao Guan Qilin Wu Zhengwei You State Key Laboratory for Modification of Chemical Fibers and Polymer Materials Shanghai Belt and Road Joint Laboratory of Advanced Fiber and Low-Dimension Materials(Donghua University)College of Material Science and EngineeringDonghua UniversityShanghai 201620China Center for Advanced Low-Dimension Materials Donghua UniversityShanghai 201620China

Three-dimensional(3 D)printing has had a large impact on various fields,with fused deposition modeling(FDM)being the most versatile and cost-effective 3 D printing ***,FDM often requires sacrificial support structures,which significantly complicates the processing and increases the ***,poor layer-to-layer adhesion greatly affects the mechanical stability of 3D-printed ***,we present a new Print-Healing strategy to address the aforementioned challenges.A polymer ink(Cu-DOU-CPU)with synergetic triple dynamic bonds was developed to have excellent printability and room-temperature self-healing *** with various shapes were printed using a simple compact 3D printer,and readily assembled into large sophisticated architectures via *** dynamic bonds induce strong binding between ***,damaged printed objects can spontaneously heal,which significantly elongates their service *** work paves a simple and powerful way to solve the key bottlenecks in FDM 3D printing,and will have diverse applications.

关键词： dynamic bonds self-healing 3D printing support-free interlayer adhesion

Smart bistable coordination complexes

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Smart Molecules

Smart Molecules 2024年第2期2卷 15-62页

作者： Xiong Xiao Zong-Ju Chen Russell J.Varley Cheng-Hui Li State Key Laboratory of Coordination Chemistry School of Chemistry and Chemical EngineeringCollaborative Innovation Center of Advanced MicrostructuresNanjing UniversityNanjingChina Carbon Nexus at the Institute for Frontier Materials Deakin UniversityWaurn PondsVictoriaAustralia

Smart molecules have attracted increasing attention due to their transformative role in creating the next generation of smart structures and *** bistable coordination complexes are a class of functional complexes which have two stable states that can be reversibly switched in response to external *** bistable molecules play a vital role in various applications,such as sensors,data storage,spintronics,smart windows,optical switches,information encryption and decryption,displays,actuators,***,the recent research studies into the development of these smart bistable metal coordination complexes are *** to the different external stimuli,these smart bistable coordination systems have been classified and summarized,including light-responsive systems,thermally-responsive systems,electrically-responsive systems,mechanicallyresponsive systems,and some other *** systems are further subdivided according to the changes in signals(e.g.,color,fluorescence,spin state,crystalline phase)under external *** design principles of each type of smart bistable metal complexes as well as their broad and innovative applications are comprehensively ***,the challenges and opportunities in this field are briefly analyzed and discussed.

关键词： bistable coordination chemistry dynamic bonds smart molecules stimuli responsive