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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

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A Strong,Tough,and Self-Healing Strengthening Thioctic Acid-based Elastomer for Highly Reliable Flexible Strain Sensor

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Chinese Journal of polymer Science 2024年第10期42卷 1610-1618,I0016页

作者： Xin-Yu Chen Yu-Bing Fu Xue-Ling Yan Lan Liu School of Materials Science and Engineering Key Lab of Guangdong Province for High Property and Functional Polymer MaterialsSouth China University of TechnologyGuangzhou510641China

Elastomers with high strength and toughness,excellent self-healing properties,and biocompatibility have broad application prospects in wearable electronics and other fields,but preparing it remains a *** this work,we propose a highly adaptable strategy by introducing the small molecule crosslinking agent of triethanolamine(TEA)to the poly(thioctic acid)(PTA)chains and preparing the PAx Ey elastomers using a simple synthesis *** strategy stabilizes the PTA chains by constructing multiple non-covalent cross-linked dynamic networks,endowing materials with excellent strength and toughness(tensile strength of 288 kPa,toughness of 278.2 kJ/m3),admirable self-healing properties(self-healing efficiency of 121.6%within 7 h at 70℃),and good *** PAx Ey elastomers can also be combined with MWNTs to become flexible strain sensors,which can be used to monitor human joint movements with high sensitivity,repeatable responses,and stability.

关键词： Thioctic acid Ion clusters Multiple dynamic networks Self-healing strengthening Flexible strain sensor

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Study on Catalytic Behavior of Iron-based Catalyst with IITP as Electron Donor in the polymerization of Butadiene

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Chinese Journal of polymer Science 2024年第5期42卷 612-619,I0007页

作者： Shi-Liang Xu Ying-Nan Zhao Yao Yu Qi Yang Li-Hua Na Heng Liu Chun-Yu Zhang Xue-Quan Zhang Key laboratory of Advanced Rubber Material Ministry of EducationSchool of Polymer Science and EngineeringQingdao University of Science&TechnologyQingdao266042China Shandong Provincial College laboratory of Rubber Material and Engineering School of Polymer Science and EngineeringQingdao University of Science&TechnologyQingdao266042China Key lab of Rubber-Plastics Ministry of Education/Shandong Provincial Key Lab of Rubber-plasticsSchool of Polymer Science and EngineeringQingdao University of Science&TechnologyQingdao266042China

In this study,a novel iron-based catalyst system,Fe(acac)3/(isocyanoimino)triptenylphosphorane(IITP)/AlR3,was employed for the synthesis of syndiotactic 1,2-polybutadiene in *** catalyst system exhibits remarkably high catalytic activity,achieving a polymerization activity of 762 kgpolymer·molcatalyst^(-1)·h^(-1)at 50℃with a[BD]/[Fe]molar ratio of ***,living polymerization characteristic were observed during the investigation of the polymerization kinetics of 1,3-butadiene *** characteristics were well demonstrated by a narrow molecular weight distribution(PDI≈2.0)of the resulting polybutadiene and a linear relationship between-ln(1-c)and polymerization time as well as number average molecular weight and polymer *** resultant polymer showed a 1,2-selectivity of approximately 76%and stereoregularity ranging from 62%to 73%(rrrr).Additionally,through kinetic studies on polymerization reaction,an apparent activation energy Ea value of this catalytic system was calculated to be 84.98 kJ·mol^(-1),which suggests that high polymerization temperature favors efficient polymerization.

关键词： Iron catalyst Syndiotactic 1,2-polybutadiene Elastomers Donor Selectivity

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Synthesis,Characterization of Polyethylene Ionomers and Their Antibacterial Properties

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Chinese Journal of polymer Science 2024年第8期42卷 1077-1084页

作者： Jia-Jia Wu Fei Wang Peng-Qi Wan Li Pan Chun-Sheng Xiao Zhe Ma Yue-Sheng Li Tianjin Key lab Composite&Functional Materials School of Materials Science and EngineeringTianjin UniversityTianjin 300350China Key lab polymer Ecomaterials Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China

Owing to its high production volume and wide range of application s,polyethylene has gained a great deal of attention,but its low surface energy and non-polar nature have limited its application in some important *** this study,ethylene/11-iodo-1-undecene copolymers were prepared and used as the intermediates to afford a series of imidazolium-based ionomers bearing methanesulfonate(CH_(3)SO_(3)^(-)),trifluoromethanesulfonate(CF_(3)SO_(3)^(-)),or bis(trifluoromethane)sulfonimide(Tf_(2)N^(-))*** tensile test results showed that the stress-at-break(7.8-25.6 MPa)and the elongation-at-break(445%-847%)of the ionomers could be adjusted by changing the counterion species and the ionic group *** importantly,the ionomers exhibited marvelous antibacterial activities against Staphylococcus aureus(***)and Escherichia coli(***).The ionomers bearing Tf_(2)N^(-)exhibited antibacterial activities>99%against both *** and *** when ionic content reached 9.1%.The imidazolium-based ionomers prepared in this work demonstrated excellent comprehensive properties,especially highefficient and broad-spectrum antibacterial ability,exhibiting the potential fo r the application as the antibacterial materials in packaging,medical,and other fields.

关键词： Polyethylene Ionomer polymerization catalysis Imidazolium Antibacterial material

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Lightweight,Strong and High Heat-Resistant Poly(lactide acid)Foams via Microcellular Injection Molding with Self-Assembly Nucleating Agent

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Chinese Journal of polymer Science 2024年第6期42卷 739-750页

作者： Xiao-Hu Bing Wen-Yu Ma Ming-Hui Wu Peng Gao Xiao Zhou Hai-Bin Luo Long Wang Wen-Ge Zheng School of materials Science and Engineering Shanghai UniversityShanghai200444China Ningbo Key lab of polymer Materials Ningbo Institute of Material Technology and EngineeringChinese Academy of SciencesNingbo315201China University of Chinese Academy of Sciences Beijing100049China

Poly(lactide acid)(PLA)foams have shown considerable promise as eco-friendly alternatives to nondegradable plastic foams,such as polystyrene(PS)***,PLA foam typically suffers from low heat-resistance and poor cellular structure stemming from its inherent slow crystallization rate and low melt *** this study,a high-performance PLA foam with well-defined cell morphology,exceptional strength and enhanced heat-resistance was successfully fabricated via a core-back microcellular injection molding(MIM)*** scanning calorimetry(DSC)results revealed that the added hydrazine-based nucleating agent(HNA)significantly increased the crystallization temperature and accelerated the crystallization process of ***,the addition of a 1.5 wt%of HNA led to a significant reduction in PLA’s cell size,from 43.5µm to 2.87µm,and a remarkable increase in cell density,from 1.08×10^(7)cells/cm^(3)to 2.15×10^(10)cells/cm^(3).This enhancement resulted in a final crystallinity of approximately 55.7%for the PLA blend foam,a marked improvement compared to the pure PLA ***,at 1.5 wt%HNA concentration,the tensile strength and tensile toughness of PLA blend foams demonstrated remarkable improvements of 136%and 463%,***,the Vicat softening temperature of PLA blend foam increased significantly to 134.8°C,whereas the pure PLA foam exhibited only about 59.7℃.These findings underscore the potential for the preparation of lightweight injection-molded PLA foam with enhanced toughness and heat-resistance,which offers a viable approach for the production of high-performance PLA foams suitable for large-scale applications.

关键词： Poly(lactide acid) Nucleating agent Microcellular injection molding Heat-resistance Toughness

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Tunable Phase Structure of Side-chain Liquid Crystalline polymers Enabled by Molecular Engineering of Dual Mesogenic Cores

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Chinese Journal of polymer Science 2024年第10期42卷 1459-1469,I0009页

作者： Wen-Huan Yao Lan-Sheng Liu Jie Zhao Yan-Xia Wang An-Zhi Ma Zheng-Rui Ma Lan-Ying Zhang Ruo-Chen Lan College of Chemistry and Chemical Engineering Hunan UniversityChangsha410082China Key laboratory of Eco-Functional polymer Materials of the Ministry of Education Key Laboratory of Eco-Environmental Polymer Materials of Gansu ProvinceCollege of Chemistry and Chemical EngineeringNorthwest Normal UniversityLanzhou730070China Department of Materials Science and Engineering College of EngineeringPeking UniversityBeijing100871China Institute of Advanced Materials&Key lab of Fluorine and Silicon for Energy Materials and Chemistry of Ministry of Education College of Chemistry and Chemical EngineeringJiangxi Normal UniversityNanchang330022China

A series of novel side-chain liquid crystalline(SCLC)copolymers were synthesized by attaching two distinct mesogenic units,namely a chiral cholesteryl-based monomer(M1)and an achiral biphenyl-based monomer(M2),to a poly(3-mercaptopropylmethylsiloxane)(PMMS)backbone via thiol-ene click *** influence of side chain composition on the self-assembly behavior and phase structures of these SCLC copolymers was systematically investigated using different *** indicate that three distinct liquid crystalline phases and four unique molecular configurations were identified within the polymer series,with the emergence of the liquid crystalline phase being a synergistic outcome of the two distinct side *** study underscores the critical influence of side chain dimensions,rigidity,and spatial volume on the self-assembly structures and phase characteristics of liquid crystalline polymers,providing valuable insights for the rational design and development of advanced functional materials with tailored properties.

关键词： Liquid crystalline copolymers Self-assembly Phase structure Chiral molar ratio

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Lightweight foam-like nitrogen-doped carbon nanotube complex achieving highly efficient electromagnetic wave absorption

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Journal of Materials Science & Technology 2024年第1期168卷 114-123页

作者： Zongcheng Li Jin Liang Zhiheng Wei Xin Cao Jiahui Shan Chunwei Li Xiaoyi Chen Dong Zhou Ruizhe Xing Chunjia Luo Jie Kong MOE Key lab of Materials Physics and Chemistry in Extraordinary Conditions Shaanxi Key Laboratory of Macromolecular Science and TechnologySchool of Chemistry and Chemical EngineeringNorthwestern Polytechnical UniversityXi’an 710072China Key laboratory of Flexible Electronics of Zhejiang Province Ningbo Institute of Northwestern Polytechnical UniversityNingbo 315103China polymer Materials and Engineering Department School of Materials Science and EngineeringChang’an UniversityXi’an 710064China

With the increased electromagnetic wave(EMW)threat to military and human health,the develop-ment of EMW-absorbing materials is ***-organic framework derivatives containing magnetic nanoparticles and a carbon matrix are potential candidates for designing efficient EMW-absorbing ***,a zeolitic imidazolate framework-67(ZIF-67)-embedded three-dimensional melamine foam is pyrolyzed to afford carbon foam-based nitrogen-doped carbon nanotube composites,named 3D foam-like CoO/Co/*** CoO/Co particles are confined in the dielectric carbon nanotube *** carbon nanotubes provide considerable conductive loss,while CoO/Co magnetic particles are con-ducive to providing magnetic loss and adjusting impedance ***,the numerous defect structures introduced by heteroatomic doping(nitrogen)cause dipole polarization and simultaneously adjust impedance ***,the unique porous nanotube structure promotes multiple re-flections and scattering of EMWs,further optimizing impedance ***/Co/N-CNTs composites exhibit a minimum reflection loss of−52.3 dB at a matching thickness of 2.0 mm,while the correspond-ing effective absorption bandwidth is 5.28 GHz at a matching thickness of 2.2 *** study reports a novel approach to fabricating a lightweight high-performance EMW-absorbing material.

关键词： Lightweight porous carbon materials Carbon nanotubes CoO/Co magnetic particles Electromagnetic synergistic effect Impedance matching

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A Simple Urea Approach to N-Dopedα-Mo_(2)C with Enhanced Superconductivity

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Chinese Physics Letters 2024年第10期41卷 103-111页

作者： Longfu Li Lei Shi Lingyong Zeng Kuan Li Peifeng Yu Kangwang Wang Chao Zhang Rui Chen Zaichen Xiang Yunwei Zhang Huixia Luo School of Materials Science and Engineering State Key Laboratory of Optoelectronic Materials and TechnologiesGuangdong Provincial Key Laboratory of Magnetoelectric Physics and DevicesKey Lab of Polymer Composite&Functional MaterialsSun Yat-Sen UniversityGuangzhou 510275China School of Physics Guangdong Provincial Key Laboratory of Magnetoelectric Physics and DevicesSun Yat-Sen UniversityGuangzhou 510275China

Chemical doping is a critical factor in the development of new superconductors or optimizing the superconducting transition temperature(T_(c))of the parent superconducting ***,a new simple urea approach is developed to synthesize the N-dopedα-Mo_(2)*** from the simple urea method,a broad superconducting dome is found in the Mo_(2)C1−xNx(0≤x≤0.49)compositions.X-ray diffraction results show that the structure of𝛼α-Mo_(2)C remains unchanged and there is a variation of lattice parameters with nitrogen ***,magnetic susceptibility,and heat capacity measurement results confirm that T_(c)was strongly increased from 2.68K(x=0)to 7.05K(x=0.49).First-principles calculations and our analysis indicate that increasing nitrogen doping leads to a rise in the density of states at the Fermi level and doping-induced phonon softening,which enhances electron–phonon *** results in an increase in𝑇T_(c)and a sharp rise in the upper critical *** findings provide a promising strategy for fabricating transition metal carbonitrides and provide a material platform for further study of the superconductivity of transition metal carbides.

关键词： softening doping critical

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Phase-stable wide-bandgap perovskites enabled by suppressed ion migration

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Journal of Energy Chemistry 2024年第9期96卷 120-128页

作者： Zhiyu Gao Yu Zhu Jingwei Zhu Cong Chen Zongjin Yi Yi Luo Yuliang Xu Kai Wu Tianshu Ma Fangfang Cao Zijun Chen Fang Yao Juncheng Wang Wenwu Wang Chuanxiao Xiao Hao Huang Hongxiang Li Qianqian Lin Pei Cheng Changlei Wang Xia Hao Guanggen Zeng Dewei Zhao College of Materials Science and Engineering&Institute of New Energy and Low-Carbon Technology&Engineering Research Center of Alternative Energy Materials and Devices Ministry of EducationSichuan UniversityChengdu 610065SichuanChina School of Optoelectronic Science and Engineering&Collaborative Innovation Center of Suzhou Nano Science and Technology Key Lab of Advanced Optical Manufacturing Technologies of Jiangsu Province&Key Lab of Modern Optical Technologies of Education Ministry of ChinaSoochow UniversitySuzhou 215006JiangsuChina Ningbo Institute of Materials Technology and Engineering Chinese Academy of SciencesNingbo 315201ZhejiangChina Ningbo New Materials Testing and Evaluation Center Co.Ltd Ningbo 315201ZhejiangChina State Key laboratory of Featured Metal Materials and Life-cycle Safety for Composite Structure&School of Resources Environment and MaterialsGuangxi UniversityNanning 530004GuangxiChina Key lab of Artificial Micro-and Nano-Structures of Ministry of Education of China School of Physics and TechnologyWuhan UniversityWuhan 430072HubeiChina College of polymer Science and Engineering State Key Laboratory of Polymer Materials EngineeringSichuan UniversityChengdu 610065SichuanChina

Wide-bandgap(>1.7 eV)perovskites suffer from severe light-induced phase segregation due to high bromine content,causing irreversible damage to devices ***,the strategies of suppressing photoinduced phase segregation and related mechanisms have not been fully ***,we report a new passivation agent 4-aminotetrahydrothiopyran hydrochloride(4-ATpHCl)with multifunctional groups for the interface treatment of a 1.77-eV wide-bandgap perovskite film.4-ATpH^(+)impeded halogen ion migration by anchoring on the perovskite surface,leading to the inhibition of phase segregation and thus the passivation of defects,which is ascribed to the interaction of 4-ATpH^(+)with perovskite and the formation of low-dimensional ***,the champion device achieved an efficiency of 19.32%with an open-circuit voltage(V_(OC))of 1.314 V and a fill factor of 83.32%.Moreover,4-ATpHCl modified device exhibited significant improved stability as compared with control *** target device maintained 80%of its initial efficiency after 519 h of maximum power output(MPP)tracking under 1 sun illumination,however,the control device showed a rapid decrease in efficiency after 267 ***,an efficiency of 27.38%of the champion 4-terminal all-perovskite tandem solar cell was achieved by mechanically stacking this wide-bandgap top subcell with a 1.25-eV low-bandgap perovskite bottom subcell.

关键词： Wide-bandgap perovskite Phase segregation lon migration Interface post-treatment All-perovskite tandems

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Simultaneously optimizing exciton diffusion length and nonradiative energy loss in organic solar cells via ternary strategy

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Science China Chemistry 2024年第9期67卷 3004-3011页

作者： Huanxiang Jiang Hao Lu Zezhou Liang Yonghai Li Guangliu Ran Chenyu Han Yuqiang Liu Hongxiang Li Xichang Bao Zhishan Bo College of Textiles and Clothing State Key Laboratory of Bio-fibers and Eco-textilesQingdao UniversityQingdao 266071China Qingdao Institute of Bioenergy and Bioprocess Technology Chinese Academy of SciencesQingdao 266101China Key laboratory for Physical Electronics and Devices of the Ministry of Education&Shaanxi Key Lab of Photonic Technique for InformationSchool of Electronics Science&EngineeringFaculty of Electronic and Information EngineeringXi’an Jiaotong UniversityXi’an 710049China Department of Physics and Applied Optics Beijing Area Major laboratory Center for Advanced Quantum StudiesBeijing Normal UniversityBeijing 100875China College of polymer Science and Engineering State Key Laboratory of Polymer Materials EngineeringSichuan UniversityChengdu 610065China laboratory of Solar Energy Shandong Energy InstituteQingdao 266101China

Significant nonradiative energy loss and short exciton diffusion length in organic solar cells(OSCs)are two major obstacles to achieving state-of-the-art *** is crucial to conduct a study on the intensive mechanism and improvement strategies for future breakthroughs in the efficiency of *** this work,nonradiative energy loss and exciton diffusion length are optimized simultaneously by incorporating a guest acceptor(LA15)to construct ternary OSC(D18:L8-BO:LA15).Firstly,LA15 exhibits excellent compatibility with the host acceptor L8-BO,and effectively improves the fluorescence quantum efficiency(FLQY),resulting in suppressed non-radiative energy ***,LA15 effectively prolongs the fluorescent lifetime of the acceptor phase from 0.85 to 1.12 ns,leading to larger exciton diffusion length,which is beneficial for reducing geminate ***,the addition of LA15 optimizes the crystallinity of the active layer with amplified charge transport *** a result,the optimized D18:L8-BO:LA15 device achieves ultralow nonradiative energy loss of 0.18 e V and improved fill factor(FF)with high efficiency up to 19.13%.These results highlight the crucial roles of regulating FLQYand exciton lifetime in achieving highefficiency OSCs.

关键词： organic solar cells nonradiative energy loss exciton lifetime exciton diffusion length

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