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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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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

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Sequence-controlled dynamic covalent units enable decoupling of mechanical and self-healing performance of polymers

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Science China Chemistry 2024年

作者： Luzhi Zhang Hongfei Huang Lijie Sun Xiaopeng Ma Hui Tan zhengwei you Respiratory Department Shenzhen Children's Hospital Affiliated to Shantou University Medical College State Key Laboratory for Modification of Chemical Fibers and Polymer Materials College of Materials Science and EngineeringInstitute of Functional MaterialsShanghai Key Laboratory of Lightweight CompositeShanghai Engineering Research Center of Nano-Biomaterials and Regenerative MedicineDonghua University Yangtze Delta Region Institute (Huzhou) University of Electronic Science and Technology of China

Sequence regulation provides an effective approach to controlling the properties of polymer ***,this approach remains an open question in the field of dynamic polymers,which emerge as more and more important new generation ***,we systematically investigate the effect of sequence control of dynamic covalent units in tuning the properties of *** sequence-controlled poly(oxime-urethanes) are *** dynamic oxime-urethane groups are relatively dispersed (SCP-1) or concentrated (SCP-2) distributed in their molecular *** sequence control strategy provides an efficient way to decouple the mechanical and self-healing performance of polymers,which is one of the most pressing challenges in the *** relatively dispersed oxime-urethane groups in SCP-1 not only facilitate the reorganization of the dynamic covalent bonds but also increase the probability of the reformation of hydrogen *** reversible dissociation/reassociation of dynamic bonds is conducive to dissipating energy to enhance mechanical performance and promote self-healing *** a result,SCP-1 exhibits much faster self-healing than SCP-2,and its tensile strength is nearly twice that of *** addition,energy dissipation capacity and degradation behavior also show significant sequence ***,this work reveals a new molecular structure-property relationship and provides a powerful strategy to construct high-performance polymers.

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Long-Range Electronic Effect-Promoted Ring-Opening Polymerization of Thioctic Acid to Produce Biomimetic Ionic Elastomers for Bioelectronics

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CCS Chemistry 2024年第3期6卷 761-773页

作者： Hongfei Huang Huijing Wang Lijie Sun Ruohan Zhang Luzhi Zhang ZekaiWu Yaxuan Zheng Yang Wang Wei Fu youwei Zhang Rasoul Esmaeely Neisiany zhengwei you State Key Laboratory for Modification of Chemical Fibers and Polymer Materials College of Materials Science and EngineeringInstitute of Functional MaterialsDonghua 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 201620 Institute of Pediatric Translational Medicine Shanghai Children’s Medical CenterSchool of MedicineShanghai Jiao Tong UniversityShanghai 200127 Department of Materials and Polymer Engineering Faculty of EngineeringHakim Sabzevari UniversitySabzevar ***

Poly(disulfide)s have been widely used in flexible wearable electronics,smart materials,and drug *** synthesis of poly(disulfide)s usually utilizes external stimuli or toxic initiators to promote the ***,we indicated that the long-range electronic effect can significantly alter the reactivity of the disulfide ***,we established deprotonation-promoted ring-opening polymerization of thioctic acid(TA)as a highly effective and simple method to synthesize poly(disulfide)s due to the long-range electronic effect and nucleophilic *** external stimuli and initiators,simple mixing of TA and deprotonation reagent,choline bicarbonate,in different ratios at room temperature rapidly produced a series of high molecular weight(up to 772 kDa)ionic liquid crystal poly(disulfide)s elastomers with room temperature self-healing ability,adjustable conductivity(2.39×10^(−2)∼0.28×10^(−2)S m^(−1)),degradability,biocompatibility,antibacterial property,and tissue-like softness(young’s moduli ranging from 18.2±6.0 to 111.1±36.7 kPa).The experiments and density functional theory calculations also revealed the principle of long-range electronic effect to establish a new synthetic strategy of poly(disulfide)s with superior properties favorable for bioelectronics.

关键词： self-healing elastomers thioctic acid ionic liquid bioelectronics

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基于多重氢键的自修复超分子聚氨酯弹性体

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中国材料进展 2024年第2期43卷 136-141页

作者：何宇飞游正伟东华大学材料科学与工程学院纤维材料改性国家重点实验室、中国纺织工程学会柔性电子生物医用纺织材料科研基地、上海纳米生物材料与再生医学工程技术研究中心上海201600

多重氢键是一类具有较高结合强度及动态可逆性质的超分子作用,在线型聚合物中可形成物理交联网络,提高材料机械强度的同时赋予材料良好的自修复能力。以聚四氢呋喃、六亚甲基二异氰酸酯、2,4-二氨基-6-羟基嘧啶为原料,合成了具有多重氢... 详细信息

多重氢键是一类具有较高结合强度及动态可逆性质的超分子作用,在线型聚合物中可形成物理交联网络,提高材料机械强度的同时赋予材料良好的自修复能力。以聚四氢呋喃、六亚甲基二异氰酸酯、2,4-二氨基-6-羟基嘧啶为原料,合成了具有多重氢键物理交联结构的聚氨酯。当聚四氢呋喃与扩链剂2,4-二氨基-6-羟基嘧啶的物质的量的比为7∶3及5∶5时,可得到兼具力学强度与自愈能力的超分子聚氨酯弹性体。利用核磁共振氢谱、红外光谱、凝胶渗透色谱、差示扫描量热分析、流变测试表征了弹性体的结构和基本性质。通过对2组弹性体力学性能及自愈性能的比较发现,不同的组成比例改变了多重氢键形成的物理交联强度及分子链的运动能力,聚四氢呋喃与扩链剂物质的量的比为7∶3时,材料具有较高的断裂伸长率(1280%);物质的量的比为5∶5时,材料在循环拉伸中具有更好的形变回复能力,应力松弛更慢;两组弹性体在60℃环境下均表现出一定的自修复能力。

关键词：多重氢键聚氨酯自修复超分子弹性体

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Dynamic Oxime-Urethane Bonds, a Versatile Unit of High Performance Self-healing Polymers for Diverse Applications

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Chinese Journal of Polymer Science 2021年第10期39卷 1281-1291,I0006页

作者： Luzhi Zhang 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 Materials Science and EngineeringShanghai Engineering Research Center of Nano-Biomaterials and Regenerative MedicineDonghua UniversityShanghai 201620China

Oxime-urethane bond featuring with high reversibility even at room temperature and multiple reactivity is an emerging dynamic covalent bond,and has shown great potential for self-healing polymers,which are one of the most attractive development directions for next generation of polymeric *** this review,recent progresses on the oxime-urethane-based self-healing polymers,including their designs and applications in diverse fields such as biomedicine,flexible electronics,soft robots,3D printing,protective materials,and adhesives,are summarized,and outlooks on the future development of this field are discussed.

关键词： Self-healing Dynamic covalent bonds Polyurethane Covalent adaptable networks Metal coordination

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面向高性能柔性电子的强韧、可修复和优异抗穿刺的氟化弹性体

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Science Bulletin 2024年第12期69卷 1875-1886页

作者：贾宇杰管清宝储成臻张璐之 Rasoul Esmaeely Neisiany 顾士甲孙俊芬游正伟 State Key Laboratory for Modification of Chemical Fibers and Polymer Materials Institute of Functional MaterialsCollege of Materials Science and EngineeringResearch Base of Textile Materials for Flexible Electronics and Biomedical Applications(China Textile Engineering Society)Shanghai Engineering Research Center of Nano-Biomaterials and Regenerative MedicineDonghua UniversityShanghai 201620China Biotechnology Centre Silesian University of TechnologyGliwice 44-100Poland Department of Polymer Engineering Hakim Sabzevari UniversitySabzevar ***Iran

There is usually a trade-off between high mechanical strength and dynamic self-healing because the mechanisms of these properties are mutually ***,we design and fabricate a fluorinated phenolic polyurethane(FPPU)elastomer based on octafluoro-4,4'-biphenol to overcome this *** fluorine-based motif not only tunes interchain interactions throughπ-πstacking between aromatic rings and free-volume among polymer chains but also improves the reversibility of phenol-carbamate bonds via electron-withdrawing effect of fluorine *** developed FPPU elastomer shows the highest recorded puncture energy(648.0 m J),high tensile strength(27.0 MPa),as well as excellent selfhealing efficiency(92.3%),along with low surface energy(50.9 MJ m^(-2)),notch-insensitivity,and reprocessability compared with non-fluorinated counterpart biphenolic polyurethane(BPPU)*** advantage of the above-mentioned merits of FPPU elastomer,we prepare an anti-fouling triboelectric nanogenerator(TENG)with a self-healable,and reprocessable elastic *** from stronger electron affinity of fluorine atoms than hydrogen atoms,this electronic device exhibits ultrahigh peak open-circuit voltage of 302.3 V compared to the TENG fabricated from BPPU ***,a healable and stretchable conductive composite is *** research provides a distinct and general pathway toward constructing high-performance elastomers and will enable a series of new applications.

关键词： Fluorinated elastomer Polyurethane Phenol-carbamate bonds Self-healing Reprocessable

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生物基半芳香族共聚酰胺PA5T/56与脂肪族聚酰胺PA56的性能对比

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东华大学学报（自然科学版） 2024年第3期50卷 39-44页

作者：张海洋郭小炜宋云鹤田卫东管清宝游正伟东华大学材料科学与工程学院上海东华大学纤维材料改性国家重点实验室上海黑龙江伊品新材料有限公司黑龙江大庆成都升宏新材料科技有限公司四川成都

生物基聚酰胺PA56凭借其绿色低碳的原料来源以及与商业化PA66相近的综合性能而受到关注,但受限于脂肪族的柔性主链结构,无法满足高温场景下的使用需求。为解决上述问题,引入对苯二甲酸构筑生物基半芳香族共聚酰胺PA5T/56,对PA5T/56的结... 详细信息

生物基聚酰胺PA56凭借其绿色低碳的原料来源以及与商业化PA66相近的综合性能而受到关注,但受限于脂肪族的柔性主链结构,无法满足高温场景下的使用需求。为解决上述问题,引入对苯二甲酸构筑生物基半芳香族共聚酰胺PA5T/56,对PA5T/56的结构及性能进行系统研究,并与生物基脂肪族聚酰胺PA56进行对比分析。红外光谱与核磁共振氢谱的表征结果验证了PA5T/56与PA56结构上的差异;相比PA56,PA5T/56具有更高的玻璃化转变温度(t_(g)=113℃)、更优的热稳定性(t_(d,5%)=392℃,t_(dmax)=423℃),以及更佳的热机械性能,同时其在高温下具有适宜加工的熔体黏度(<10^(3)Pa·s),这些优势赋予生物基半芳香族PA5T/56广阔的应用前景。

关键词：生物基聚酰胺半芳香族聚酰胺脂肪族聚酰胺熔融结晶行为热稳定性热机械性能流变行为

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Supertough spontaneously self-healing polymer based on septuple dynamic bonds integrated in one chemical group

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Science China Chemistry 2022年第2期65卷 363-372页

作者： Luzhi Zhang Qingbao Guan Ao Shen Rasoul Esmaeely Neisiany zhengwei you Meifang Zhu 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 Materials Science and EngineeringShanghai Engineering Research Center of Nano-Biomaterials and Regenerative MedicineInstitute of Functional MaterialsDonghua UniversityResearch Base of Textile Materials for Flexible Electronics and Biomedical ApplicationsChina Textile Engineering SocietyShanghai 201620China Department of Materials and Polymer Engineering Hakim Sabzevari UniversitySabzevar ***Iran

The development of spontaneously self-healing materials with excellent mechanical properties remains a formidable challenge despite the extensive interest in such *** is because the self-healing and mechanical properties of a material are usually optimized via contradictory *** present study demonstrated a supertough spontaneously self-healing polymer,Fe-(2,6-diacetylpyridine dioxime)-urethane-based polyurethane(Fe-PPOU)based on septuple dynamic bonds integrated in one chemical group.A synergistic effect was induced by the presence of multiple dynamic crosslinking points,which comprised the integrated dynamic interactions,and the hidden lengths of the folded polymeric chains in ***,the mechanical and self-healing properties of the polymer were simultaneously ***-PPOU demonstrated the highest reported toughness(139.8 MJ m^(-3))among all the room-temperature spontaneously self-healing polymers with a nearly 100%healing ***-PPOU exhibited instant(30 s)self-healing to reach a strength of 1.6 MPa that was higher than the original strength of numerous recently reported self-healing polymers.

关键词： oxime-urethane bonds hydrogen bonds metal-coordination bonds 2 6-diacetylpyridine dioxime self-healing

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含酮羰基热固性液晶聚芳酯的设计合成与性能

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东华大学学报（自然科学版） 2024年第4期50卷 68-75页

作者：韩雨菲刘萍庄耀中胡兴其姚敏刚管清宝游正伟东华大学材料科学与工程学院纤维材料改性国家重点实验室上海新凤鸣集团股份有限公司浙江桐乡

液晶聚芳酯(LCPs)具有优异的热稳定性和力学性能,被广泛应用于航空航天、电子工业等前沿领域,但LCPs面临高熔点(t_(m)>350℃)所带来的加工难题。利用活性端基苯炔基封端LCPs主链,在不破坏液晶性的基础上有效调控分子量并降低聚合物熔点... 详细信息

液晶聚芳酯(LCPs)具有优异的热稳定性和力学性能,被广泛应用于航空航天、电子工业等前沿领域,但LCPs面临高熔点(t_(m)>350℃)所带来的加工难题。利用活性端基苯炔基封端LCPs主链,在不破坏液晶性的基础上有效调控分子量并降低聚合物熔点,获得综合性能优异的液晶聚芳酯固化物(LCTs);调控的主链结构可进一步调控LCTs的热学性能。通过一步熔融缩聚法合成由对羟基苯甲酸(HBA)、对苯二甲酸(TA)、对苯二酚(HQ)、4,4'-二羟基二苯甲酮(DHBP)和2,6-萘二甲酸(NDA)构成主链并由苯炔基封端的LCTs。为进一步研究酮羰基与LCTs热学性能的关系,调节HQ与DHBP的比例合成一系列LCTs。结果表明:制得的LCTs均具有高热稳定性(t_(d,5%)>470℃)、典型向列相液晶纹影织构与取向微纤形貌;酮羰基的引入影响分子链的规整度及软硬段比例,随着酮羰基含量增多,LCTs的玻璃化转变温度降低。

关键词：液晶聚芳酯酮羰基苯炔基熔融缩聚高性能聚合物

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