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Design and synthesis of thiol-terminated imidothioether oligomer as thermally latent hardener and modifier for high-performance epoxy/thiol thermosets

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Science China Chemistry 2024年第2期67卷 632-641页

作者： Xing Liu Jianjun Zhou Shumei Liu Jianqing Zhao School of Materials Science and engineering South China University of TechnologyGuangzhou510640China Key Lab Guangdong High Property&Functional polymer Materials Key Laboratory of Polymer Processing EngineeringMinistry of EducationGuangzhou510640China

Conventional base-catalyzed epoxy/aliphatic thiol systems have a poor storage stability,and are impossible to be one-pot systems.A widely accepted solution is to use the latent catalysts,which are usually insoluble anionic initiators sensitive to impurities and moisture,and have many limitations in practical *** this work,a soluble thiol-terminated imidothioether oligomer(TPI) was synthesized and used as a latent hardener and modifier to prepare one-pot epoxy/thiol systems without the latent *** latent behavior and curing mechanism of epoxy systems(EP/TPI series),consisted of bisphenol A diglycidyl ether(DGEBA),pentaerythritol tetrakis(mercaptoacetate)(PETMP) and TPI,were *** thiol exchange reaction between TPI and PETMP preceded the curing reaction of DGEBA,and produced aromatic thiols,which were unreactive at ambient conditions and reacted with DGEBA to form the thermosets at temperatures above 130 ℃.At the loading of 24.4 wt%TPI,the epoxy system(EP/TPI-3) had a shelf life of 13 days and was completely cured within 20 min at 180 ℃.Meanwhile,the catalyst-free curing process of EP/TPI-3 system was insensitive to impurities and ***,the thermal and mechanical properties of EP/TPI-3 thermoset were simultaneously improved,thereinto,the glass transition temperature,Young's modulus and ultimate tensile strength were increased by 16.7 ℃,12.9%,and 13.6%,respectively,compared with those of the commercial DGEBA/PETMP *** work shows that TPI has the potential to be a powerful alternative to commercial latent catalysts,and EP/TPI thermosets with high performance have broad application prospects.

关键词： thiol-terminated imidothioether oligomer epoxy systems thiol exchange reaction thermal latency high performance

In situ protonation in a locally flexible porous coordination polymer for enhancing proton-carrier loading and proton conductivity

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Science China Chemistry 2024年第10期67卷 3432-3437页

作者： Xianzhe Wei Jincheng Liu Yan Su Weitao Wang Guixiang Wang Gen Zhang Ping Wang Cheng Gu State Key Laboratory of Luminescent Materials and Devices Institute of Polymer Optoelectronic Materials and DevicesSouth China University of TechnologyGuangzhou 510640China College of polymer Science and engineering State Key Laboratory of Polymer Materials EngineeringSichuan UniversityChengdu 610065China Key Laboratory for Soft Chemistry and Functional Materials of Ministry of Education School of Chemistry and Chemical EngineeringNanjing University of Science and TechnologyNanjing 210094China

Designing efficient proton-conductive materials is crucial in fuel ***,it remains a substantial challenge because of the issues in proton mobility,proton-carrier amount,and orientation of proton host ***,we report an in-situ protonation strategy to produce a locally flexible porous coordination polymer(PCP)to enhance the proton-carrier loading and proton *** local dipole flipping of the ligand allows effective proton exchange with low activation energy,promoting interpore proton transport through the pore apertures and pore *** protonation induces substantial charges to the frameworks and enhances the interaction with proton carriers,thereby increasing the loading of the proton *** this design strategy,the resulting PCP exhibits enhanced phosphoric acid loading and extraordinary proton conductivities under both aqueous and anhydrous conditions compared to its isoreticular analog that features rigidity without proton-exchange *** work provides a new avenue for designing proton-conductive materials that combine structural dynamics with performance merits.

关键词： porous coordination polymers in-situ protonation local flexibility proton-exchange mechanism proton conduction

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Multifunctional photothermal hydrogels: Design principles, various functions, and promising biological applications

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Chinese Chemical Letters 2024年第10期35卷 79-88页

作者： Zikang Hu Hengjie Zhang Zhengqiu Li Tianbao Zhao Zhipeng Gu Qijuan Yuan Baoshu Chen School of Materials Science and engineering Xihua University College of polymer Science and engineering State Key Laboratory of Polymer Materials Engineering Sichuan University

Photothermal hydrogels with excellent photo responsive and thermal conversion ability had attract a great deal of attention from researchers to explore their biological applications. This review aimed to provide a comprehensive overview of photothermal hydrogels, focusing on their design principles, various functions, and biological applications. Firstly, several classifications of photothermal hydrogels were given according to different photothermal agents(metal, metal sulfide/oxide, MXene, carbon-based, dyes, black phosphorus, and polymer) utilized in hydrogel construction. The photothermal conversion mechanism and hydrogel fabrication were also discussed in detail. Then, the relationship between their photothermal conversion property and functions, together with some indispensable property such as biocompatibility,adhesion, mechanical properties, and self-healing properties was fully introduced. Furthermore, the applications of photothermal hydrogels in the biomedical(i.e., wound healing, antibacterial treatments, controlled drug release, bone repair, and tumor treatment) was summarized. Finally, the future opportunities and challenges of photothermal hydrogels were proposed. We believe that this review could provide a new horizon for further preparation of photothermal hydrogels, and could promote their applications in wider fields.

关键词： Multifunctional hydrogels Photothermal agents Photothermal conversion Tissue repair Wound healing

Understanding the Thermal Impedance of Silicone Rubber/Hexagonal Boron Nitride Composites as Thermal Interface Materials

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Chinese Journal of polymer Science 2024年第3期42卷 352-363,I0008页

作者： Yuan Ji Shi-Da Han Hong Wu Shao-Yun Guo Feng-Shun Zhang Jian-Hui Qiu The State Key Laboratory of polymer Materials engineering Sichuan Provincial Engineering Laboratory of Plastic/Rubber Complex Processing TechnologyPolymer Research InstituteSichuan UniversityChengdu 610065China Institute of Chemical Materials China Academy of Engineering PhysicsMianyang 621900China Department of Mechanical engineering Faculty of Systems Science and TechnologyAkita Prefectural UniversityAkita 015-0055Japan

Silicone rubber(SR) composites are most widely used as thermal interface materials(TIMs) for electronics heat dissipation. Thermal impedance as the main bottleneck limiting the performance of TIMs is usually neglected. Herein, the thermal impedance of SR composites loaded with different levels of hexagonal boron nitride(h-BN) as TIMs was elaborated for the first time by the ASTM D 5470 standard test and finite element analysis. It was found that elastic modulus and surface roughness of SR composites increased with the increase of h-BN content, indicating that the conformity was reduced. When the assembly pressure was 0.69 MPa, there existed an optimal h-BN content at which the contact resistance was minimum(0.39 K·cm^(2)·W^(-1)). Although the decreased bond line thickness(BLT) by increasing the assembly pressure was beneficial to reduce the thermal impedance, the proper assembly pressure should be selected to prevent the warpage of the contact surfaces and the increase in contact resistance, according to the compression properties of the SR composites. This study provides valuable insights into fabrication of high-performance TIMs for modern electronic device applications.

关键词： Thermal interface materials Hexagonal boron nitride Thermal impedance Surfaces

A Self-Healing Elastomer with Extremely High Toughness Achieved by Acylsemicarbazide Hydrogen Bonding and Cu^(2+)-Neocuproine Coordination Interactions

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Chinese Journal of polymer Science 2024年第10期42卷 1425-1434,I0007页

作者： Xiao-Ming An Yi-Ping Wang Tang-Song Zhu Chong Xing Xu-Dong Jia Qiu-Hong Zhang Key Laboratory of High Performance polymer Material and technology of MOE Department of Polymer Science and EngineeringSchool of Chemistry and Chemical EngineeringNanjing UniversityNanjing210093China State Key Laboratory of Coordination Chemistry Nanjing UniversityNanjing210093China

Elastomers with high mechanical toughness can guarantee their durability during service ***-healing ability,as well as recyclability,can also extend the life of materials and save the consuming cost of the *** efforts have been dedicated to promoting the mechanical toughness as well as the self-healing capability of elastomers at the same time,while it remains a challenge to balance the trade-off between the above properties in one *** we proposed a molecular design driven by dual interactions of acylsemicarbazide hydrogen bonding and Cu^(2+)-neocuproine coordination *** introducing the reversible multiple hydrogen bonds and strong coordination bonds,we successfully fabricated an extremely tough and self-healing *** elastomer can achieve an impressive top-notch toughness of 491 MJ/m^(3).Furthermore,it boasted rapid elastic restorability within 10 min and outstanding crack tolerance with high fracture energy(152.6kJ/m^(2)).Benefiting from the combination of dynamic interactions,the material was able to self-repair under 80℃conveniently and could be reprocessed to restore the exceptional mechanical properties.

关键词： Metal-ligand coordination Hydrogen bond Ultra-tough elastomer Self-healing

Recent Advances in Asymmetric Structural Composites for Excellent Electromagnetic Interference Shielding: A Review

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Chinese Journal of polymer Science 2024年第6期42卷 693-710页

作者： Ying Zhou Bai Xue Lan Xie Chang-Mei Wu Qiang Zheng Department of polymer Materials and engineering College of Materials and Metallurgy Guizhou University National engineering Research Center for Compounding and Modification of polymer Materials National and Local Joint Engineering Research Center for Functional Polymer Membrane Materials and Membrane Processes State Key Laboratory of Public Big Data Guizhou University Department of polymer Science and engineering Zhejiang University

Since electromagnetic pollution is detrimental to human health and the environment, numerous efforts have been successively made to achieve excellent electromagnetic interference shielding effectiveness(EMI SE) via designing the hierarchical structures for electromagnetic interference(EMI) shielding polymer composites. Among the plentiful structures, the asymmetric structures are currently a hot spot, principally categorizing into multi-layered, porous, fibrous, and segregated asymmetric structures, which endows the high EMI shielding performance for polymer composites incorporated with magnetic, conductive, and/or dielectric micro/nano-fillers, due to the “absorption-reflection-reabsorption” shielding mechanism. Therefore, this review provides the retrospection and summary of the efforts with respect to abundant asymmetric structures and multifunctional micro/nano-fillers for enhancing EMI shielding properties, which is conducive to the booming development of polymeric EMI shielding materials for the promising prospect in modern electronics and 5-generation(5G) technology.

关键词： Asymmetric structure Microano functional filler polymer composite Electromagnetic interference shielding

Dual-functional poly(2-methyl-2-oxazoline)/poly(2-(dimethylamine)ethyl methacrylate)mixed brushes with switchable protein adsorption and antibacterial properties

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Chinese Journal of Chemical engineering 2024年第2期66卷 19-30页

作者： Kang He Liangyu Zhu Yanmei Wang CAS Key Laboratory of Soft Matter Chemistry Department of Polymer Science and EngineeringUniversity of Science and Technology of ChinaHefei 230026China

Herein,binary mixed brushes consisting of poly(2-methyl-2-oxazoline)(PMOXA)and poly(2-(dimethylamine)ethyl methacrylate)(PDMAEMA)with different chain lengths were fabricated by successive grafting of NH_(2)-terminated PMOXA and SH-terminated PDMAEMA onto polydopamine-anchored *** mixed-brush coating was characterized by variable-angle spectroscopic ellipsometry,X-ray photoelectron spectroscopy,Fourier transform infrared spectroscopy,zeta potential measurements,water contact angle,and atomic force *** mixed brushes showed tunable surface charge,wettability,and surface roughness,depending on the degree of PDMAEMA swelling under varying pH and ionic strength(Ⅰ).Then the adsorption behaviors of pepsin,bovine serum albumin(BSA),γ-globulin,and lysozyme,four very different proteins with regard to isoelectric point,on the mixed brushes coating were studied by using fluorescence microscopy and surface plasmon *** the chain length of PDMAEMA was about twice as long as PMOXA,the mixed brushes not only had high adsorption capacity for pepsin,BSA,and y-globulin but also had a desorption efficiency of 86.9%,87.1%,and 93.5%,*** is explained that electrostatic attraction between the protonated PDMAEMA and positively charged acidic proteins(pepsin and BSA,whose isoelectric points were below the pK_(a) of PDMAEMA)would drive the intensive adsorption(at pH 3,I=10^(-3)mol·L^(-1)for pepsin,and pH 5,I=10^(-5)mol·L^(-1)for BSA),while desorption was dominated by the hydrophilic PMOXA when PDMAEMA was shrinking(at pH 7,I=10^(-1)mol·L^(-1)for pepsin,and pH 9,I=10^(-1)mol·L^(-1)for BSA).Furthermore,the isoelectric precipitation led to the adsorption of neutral protein(γ-globulin,whose isoelectric point was near the pK_a of PDMAEMA)at pH 7,I=10^(-5)mol·L^(-1),while electrostatic repulsion and antifouling PMOXA triggered the desorption of y-globulin at pH 3,I-10^(-1)mol·L^(-1).However,alkaline protein(lysozyme,whose isoelectric point was higher than

关键词： Switchable conformation transition Controllable protein adsorption Mixed brushes Isoelectric point Antibacterial surface

3D printing encouraging desired in-situ polypyrrole seed-polymerization for ultra-high energy density supercapacitors

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Journal of Energy Chemistry 2024年第8期95卷 117-125,I0004页

作者： Tiantian Zhou Shangwen Ling Shuxian Sun Ruoxin Yuan Ziqin Wu Mengyuan Fu Hanna He Xiaolong Li Chuhong Zhang State Key Laboratory of polymer Materials engineering Polymer Research InstituteSichuan UniversityChengdu 610065SichuanChina

The tireless pursuit of supercapacitors with high energy density entails the parallel advancement of wellsuited electrode materials and elaborately engineered ***(PPy)emerges as an exceedingly conductive polymer and a prospective pseudocapacitive materials for supercapacitors,yet the inferior cyclic stability and unpredictable polymerization patterns severely impede its real-world ***,for the first time,an innovative seed-induced in-situ polymerization assisted 3D printing strategy is proposed to fabricate PPy-reduced graphene oxide/poly(vinylidene difluoride-cohexafluoropropylene)(PVDF-HFP)(PPy-rGO/PH)electrodes with controllable polymerization behavior and exceptional areal mass *** preferred active sites uniformly pre-planted on the 3D-printed graphene substrates serve as reliable seeds to induce efficient polypyrrole deposition,achieving an impressive mass loading of 185.6 mg cm^(-2)(particularly 79.2 mg cm^(-2)for polypyrrole)and a superior areal capacitance of 25.2 F cm^(-2)at 2 mA cm^(-2)for a 12-layer *** agreement with theses appealing features,an unprecedented areal energy density of 1.47 mW h cm^(-2)for a symmetrical device is registered,a rarely achieved value for other PPy/rGO-based *** work highlights a promising route to preparing high energy density energy storage modules for real-world applications.

关键词： 3D printing Seed-induced polymerization Supercapacitor Polypyrrole High energy density

Cyclic-acyclic monomers metathesis polymerization to access photodegradable polydicyclopentadiene and polyethylene-like materials

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Science China Chemistry 2024年第4期67卷 1311-1315页

作者： Wu Li Daohong Liao Yougui Li Guifu Si Changle Chen School of Chemistry and Chemical engineering Hefei University of TechnologyHefei 230009China Key Laboratory of Precision and Intelligent Chemistry Department of Polymer Science and EngineeringUniversity of Science and Technology of ChinaHefei 230026China

The development of degradable and recyclable polymers is an attractive strategy to tackle the post-consumption pollution issue of commercial ***-acyclic monomers metathesis polymerization(CAMMP)has been recently reported to produce degradable thermoset,thermoplastic and elastomeric polymers,and their degradability is enabled with addition of various *** this contribution,we demonstrate that the utilization of diene comonomers containing photodegradable moiety can give access to thermoset and thermoplastic materials bearing photo-degradation *** copolymerization of a series easily accessible diene comonomers bearing photodegradable ortho-nitrobenzyl moieties with dicyclopentadiene(DCPD)or cyclooctene(COE)leads to the formation of photodegradable p DCPD thermosets and p COE thermoplastic polymers with mechanical properties comparable to their non-degradable *** importantly,their photo-degradation properties can be efficiently tuned with the addition of ultraviolet absorber during in-situ polymerization.

关键词： metathesis polymerization photodegradable polydicyclopentadiene polyethylene-like materials