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Molecular Chain Flexibility and Dielectric Loss at High-Frequency:Impact of Ester Bond Arrangement in Poly(ester imide)s

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Chinese Journal of Polymer Science 2024年第8期42卷 1122-1133页

作者： Ya-Dong Li Hong Li Lu-Kun Feng Feng Bao Ming-Liang Wang Cai-Zhen Zhu Zhao-Hui Zheng Xiao-Bin Ding Jian Xu Chengdu institute of Organic chemistry Chinese Academy of SciencesChengdu 610041China University of Chinese Academy of Sciences Beijing 100081China institute of low-dimensional materials genome initiative College of Chemistry and Environmental EngineeringShenzhen UniversityShenzhen 518060China

The evolution of high-frequency communication has accentuated the significance of controlling dielectric properties in polymer ***,it has been theorized that rigid molecular chains lead to lower dielectric ***,the validity of this proposition at high frequencies remains *** scrutinize the correlation between chain flexibility and dielectric properties,we synthesized six poly(ester imide)s(PEIs)with systematically varied molecular chain flexibilities by modifying the ester's substitution on the aromatic *** introduction of ester bonds bestowed all PEI films with a low dielectric dissipation factor(D_(f)),ranging from 0.0021 to 0.0038 at 10 GHz in dry *** dry D_(f)displayed a pattern consistent with volume polarizability(P/V).Unexpectedly,PI-mmm-T,featu ring the most flexible molecular chain,exhibited the lowest dielectric loss under both dry(0.0021@10 GHz)and hygroscopic(0.0029@10 GHz)***,the observed increase in D_(f)after humidity absorption suggests that the high dielectric loss of PEI in applications may be attributed to its hygroscopic *** simulations and characterization of the aggregation structure revealed that the smaller cavities within flexible molecular chains,after close stacking,impede the entry of water *** sacrificing high-temperature resistance,the precursor exhibited enhanced solubility properties and could be processed into high-quality *** research unveils new insights into the relationship between flexibility and highfrequency dielectric loss,offering innovative perspectives on synthesizing aromatic polymers with exceptional dielectric properties.

关键词： 5G communications Poly(ester imide)s Molecular chain flexibility Dielectric properties Humidity absorption

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High-Performance Recyclable Furan-based Epoxy Resin and Its Carbon Fiber Composites with Dense Hydrogen Bonding

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Chinese Journal of Polymer Science 2024年第1期42卷 73-86,I0008页

作者： Chang-Bo Zhao Lu-Kun Feng Hui Xie Ming-Liang Wang Bing Guo Zhi-Yong Xue Cai-Zhen Zhu Jian Xu Advanced materials Research institute North China Electric Power UniversityBejing 102206China institute of low-dimensional materials genome initiative College of Chemistry and Environmental EngineeringShenzhen UniversityShenzhen 518060China Chengdu institute of Organic chemistry Chinese Academy of SciencesChengdu 610041China School of Science and Shenzhen Key Laboratory of Flexible Printed Electronics Technology and Shenzhen Key Laboratory of Advanced Functional Carbon Materials Research and Comprehensive ApplicationHarbin Institute of TechnologyShenzhen 518055China

The emerging biomass-based epoxy vitrimers hold great potential to fulfill the requirements for sustainable development of *** the existence of dynamic chemical bonds in vitrimers often reduces both the thermal and mechanical properties of epoxy resins, it is challenging to produce recyclable epoxy vitrimers with both excellent mechanical properties and good thermal stability. Herein, a monomer 4-(((5-(hydroxymethyl)furan-2-yl)methylene)amino)phenol(FCN) containing furan ring with potential to form high density of hydrogen bonding among repeating units is designed and copolymerized with glycerol triglycidyl ether to yield epoxy resin(FCN-GTE), which intrinsically has dual hydrogen bond networks, dynamic imine structure and resultant high performance. Importantly, as compared to the BPA-GTE, the FCN-GTE exhibits significantly improved mechanical properties owing to the increased density of hydrogen bond network and physical crosslinking interaction. Furthermore, density functional theory(DFT) calculation and in situ FTIR analysis is conducted to decipher the formation mechanism of hydrogen bond network. In addition, the FCN-GTE possesses superior UV shielding, chemical degradation, and recyclability because of the existence of abundant imine bonds. Notably, the FCN-GTE-based carbon fiber composites could be completely recycled in an amine *** study provides a facile strategy for synthesizing recyclable biomass-based high-performance epoxy vitrimers and carbon fiber composites.

关键词： Furan Hydrogen bond network Dynamic Schiff base Carbon fiber composites Recycling

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Novel Quasi Solid-State Succinonitrile-based Electrolyte with low-flammability for Lithium-ion Battery

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Chinese Journal of Polymer Science 2023年第11期41卷 1695-1705,I0005页

作者： Yan-Kun Xie Lu-Kun Feng Dong-Dong Li Yin Tang Cai-Zhen Zhu Ming-Liang Wang Jian Xu institute of low-dimensional materials genome initiative College of Chemistry and Environmental EngineeringShenzhen UniversityShenzhen 518060China

Quasi solid-state succinonitrile(SN)-based polymer electrolytes have emerged for lithium-metal batteries due to their excellent ionconductivity at room temperature,wide electrochemical stability window(ESW,usually>5 V).However,the practical application of these solid SN-based polymer electrolytes is hampered by the flammability and the inherent instability of SN to Li-metal *** this work,solid SN-based polymer electrolytes were prepared with succinonitrile,ethoxylated trimethylolpropane triacrylate(ETPTA),triethyl phosphate(TEP)and fluoroethylene carbonate for Li-metal battery via in situ polymerization *** SN-based polymer electrolytes with 5 wt%triethyl phosphate and FEC showed good nonflammability,superior ion-conductivity as high as 1.01×10^(-3)S/cm,and wide ESW of 5.41 *** SN-based polymer electrolyte also exhibited excellent interfacial compatibility to lithium metal *** it also delivered a high specific capacity of 156m Ah/g at 0.2 C at ambient temperature,and presented stable cycling at 1.0 C with a specific capacity retention of 98.4%after 1000 *** work provides an alternative and simple strategy to realize the practical application of the solid-state SN-based polymer electrolyte.

关键词： Solid polymer electrolyte Succinonitrile Solid-state battery In situ polymerization low-flammability

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Wireless Autonomous Soft Crawlers for Adjustable Climbing Actuation

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Chinese Journal of Polymer Science 2023年第3期41卷 405-413,I0008页

作者： Lei Tian Ji-Ji Tan Wei-Liang Dong Bo Yang Cui-Hua Li Dai Wang Hai-Yu Huang Xin-Tong Li Cai-Zhen Zhu Jian Xu institute of low-dimensional materials genome initiative College of Chemistry and Environmental EngineeringShenzhen UniversityShenzhen 518060China

Artificial soft actuators,featured with non-equilibrium internal circumstance and fast,programmable shape transformations,have attracted strong research interest recently due to their flexibility,highly controllable,and ***,wireless soft actuators,achieving the locomotion on different large slopes with multiple energy conversion,have been rarely ***,we create a asymmetric bilayer strategy to construct autonomous soft crawler via“breathing”moisture to motivate the mechanical *** soft crawlers present conspicuous performances including periodic tumbler locomotion predicted via improved Timoshenko’s equation,multiple reversible shape-morphing(circle,helix,despiralization,etc.)determined by their fiber orientation,controlled drive mode(front drive and rear drive)and rapid climb speed(4.76 cm/min)at wide slope *** architecture design,they can be series-wound or shunt-wound to construct multijoint complex *** climbing,a intelligent soft ring-pull with admirable cycle performance for preventing overheating or something untouchable,has been *** soft crawlers also realize multiple energy conversion to be actuated by light *** envision that this soft crawler system has an enormous potential in intelligent machine,microscopic diagnosis and treatment,biosensing,energy harvesting and conversion.

关键词： Soft crawler Tumbler locomotion Reversible shape-morphing Autonomous Energy conversion

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Controlling the Balance of Photoluminescence and Photothermal Effect in Cyanostilbene-Based Luminescent Liquid Crystals

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Chinese Journal of chemistry 2022年第8期40卷 902-910页

作者： Xiang-Jian Cao Wei Li Jiahua Li Lin Zou Xing-Wang Liu Xiang-Kui Ren Zhen-Qiang Yu School of Chemical engineering and Technology State Key Laboratory of Chemical EngineeringTianjin UniversityTianjin 300350China college of chemistry and environmental engineering Institute of Low-dimensional Materials Genome InitiativeShenzhen UniversityShenzhenGuangdong 518071China

Molecular motions of the luminescent liquid crystals(LLCs)show a significant effect on fluorescent emission and heat *** this article,a series of cyanostilbene-based LLCs(CSs:CS1-6,CS1-12,CS2-6 and CS2-12)are synthesized to investigate how the pho-toluminescence and photothermal effect *** these materials,the mesogens peripheried by single alkyl chains formed enantiotropic nematic(CS1-6)or smectic C(CS1-12)phase with different alkyl tail *** the single aliphatic chain is re-placed by mini-dendrons,room temperature(RT)monotropic hexagonal columnar phase(CS2-12)or molecular liquid(CS2-6)is *** results revealed that all these materials exhibited high efficiency emission with the highest quantum yield reaching 59.0%.The photoluminescence and photothermal effect can be effectively tuned by dispersing CSs into a commercially available RT liquid crystal matrix 8CB,which output significantly improved photothermal conversion efficiency of 63.2%.Furthermore,the pho-tothermal can rapidly trigger the Smectic A-Nematic-Isotropic sequence transitions of 8CB doped with *** work paves a way of adjusting the balance of photoluminescence and photothermal properties of the LLC materials.

关键词： Aggregation-induced emission Liquid crystals Molecular motions Photothermal effect Phase transitions

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Freestanding and Ultra‑flexible PAN/ZIF‑67 Hybrid Membrane with Controlled Porosity for High‑Performance and High‑Safety Lithium Batteries Separator

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Advanced Fiber materials 2022年第6期4卷 1511-1524页

作者： Mao Guo Hangyi Zhu Pengfei Wan Feng Xu Caihong Wang Shengjun Lu Yufei Zhang Haosen Fan Jian Xu college of materials Science and Metallurgy engineering Guizhou UniversityGuiyang 550025China School of Chemical engineering and Light Industry Guangdong University of TechnologyGuangzhou 510006China institute of low‑dimensional materials genome initiative College of Chemistry and Environmental EngineeringShenzhen UniversityShenzhen 518060China

Herein,a flexible ZIF-67/PAN hybrid membrane was successfully prepared by the incorporation of ZIF-67 nanoparticles and PAN nanofibers through electrospinning *** hybrid membrane presented tomatoes on sticks structures with one single PAN fiber stringing series of ZIF-67 *** morphology,electrolyte wettability,heat resistance,flexibility,and electrochemical properties of the electrospun ZIF-67/PAN membranes were *** the membranes prepared with different percentage of ZIF-67,the 30% ZIF-67/PAN membrane exhibited outstanding heat shrinkage resistance(remained intact at 200℃ for 1 h),excellent electrolyte uptake(556.39%),wide electrochemical window(~5.25 V)and high ionic conductivity(2.98 mS cm^(−1)).When used as lithium-ion batteries(LIBs)separators,the cells assembled by 30% ZIF-67/PAN membrane presented excellent rate capacity and high capacity retention of 86.9% after 300 cycles at *** importantly,the cells assembled with ZIF-67/PAN membranes repeated bent for 1000 times also exhibited high rate performance and maintained capacity retention of 92% after 100 cycles at 1 *** characterization and the electrochemical testing suggest the electrospinning prepared ZIF-67/PAN flexible membranes can be expected to be used as potential separator for advanced batteries with high safety and high performance.

关键词： ZIF-67/PAN Hybrid membrane Ultra-flexible High safety Separator

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AIEgen containing side-chain liquid crystalline polymers: Photoluminecence or photothermal, which dominate?

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Nano Research 2022年第10期15卷 9334-9340页

作者： Lei Tao He-Lou Xie Xin Qi Jun Song Hong Xin Zhen-Qiang Yu college of chemistry and environmental engineering Institute of Low-dimensional Materials Genome InitiativeShenzhen UniversityShenzhen 518060China Key Laboratory of Optoelectronic Devices and Systems of Ministry of Education and Guangdong Province College of Optoelectronic EngineeringShenzhen UniversityShenzhen 518071China Key Lab of Environment-friendly chemistry and Application in Ministry of Education College of ChemistryXiangtan UniversityXiangtan 411105China

Why many luminescent liquid crystalline polymers(LLCPs)containing aggregation-induced emission luminogen(AIEgen)show weak emission is a question still to be ***,a series of LLCPs(α-Pns,n=4,8,and 12)with polynorbornene as main chain and twoα-dicyanodistyrylbenzene(α-DCS)as side chain are successfully synthesized to solve this *** scanning calorimetry(DSC),polarized light microscopy(PLM),one-dimentional(1D),two-dimentional(2D)middle-angle and wide-angle X-ray scattering(MAXS and WAXS)results demonstrate that the polymers form smectic A(SmA)phase with the side chains interdigitated packed within the smectic ***,the photophysical properties ofα-Pns were investigated by ultraviolet-visible(UV-vis)absorption,steady state and time-resolved spectroscopy,and photothermal *** show that the polymers are AIE active,but emit weak *** emission peak ofα-Pns film red-shift from 473 to 531 nm,the quantum yield gradually increases from around 1.6%to 14.7%,and the photothermal conversion efficiency decreases from 39%to 19%with the alkyl tail length *** photothermal effect,but not photoluminescence,dominates the excited state relaxation.

关键词： luminescent liquid crystalline polymers dicyanodistyrylbenzene smectic A structure alkyl tail dependence photothermal conversion

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水溶液介质中氰基苯乙烯衍生物的可逆手性光驱动自组装

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Science China materials 2022年第5期65卷 1413-1416页

作者：曾晓璇吴玥邹林刘兴旺祁鑫余振强 college of chemistry and environmental engineering Institute of Low-dimensional Materials Genome InitiativeShenzhen UniversityShenzhen 518071China

人工手性自组装一直是分子化学与材料化学的前沿挑战性课题.但由于缺少合适的手性光响应结构单元,构造具有光控、可逆、手性专一性响应的分子体系具有很大的挑战性.本工作通过合理的分子设计:以氰基二苯乙烯作为光致异构基团,磺酸基作... 详细信息

人工手性自组装一直是分子化学与材料化学的前沿挑战性课题.但由于缺少合适的手性光响应结构单元,构造具有光控、可逆、手性专一性响应的分子体系具有很大的挑战性.本工作通过合理的分子设计:以氰基二苯乙烯作为光致异构基团,磺酸基作为亲水基团,胆固醇作为疏水手性基团,构造了独特的光响应组装体系.当氰基二苯乙烯处于反式构型时,在水相中组装形成规则的球状组装体且具有较强的手性信号.通过365 nm光照后,反式构型转变为顺式构型,球状组装体解组装,同时手性信号消失;当采用254 nm光照后,重新形成具有手性信号的球状组装体.核磁共振和吸收光谱结果表明光致异构转化率达到90%,并且具有良好的光致异构重复性(抗疲劳性)及热稳定性.本研究成功实现了水相介质中光控、手性专一性响应的可逆光调控,在构建双稳态光控手性开关方面表现出潜在的应用前景.

关键词：光致异构顺式构型分子体系双稳态组装体分子化学材料化学抗疲劳性

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Surface modification of MoS_(2) nanosheets by single Ni atom for ultrasensitive dopamine detection

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Nano Research 2023年第1期16卷 917-924页

作者： Xuejiao Sun Cai Chen Can Xiong Congmin Zhang Xusheng Zheng Jin Wang Xiaoping Gao Zhen-Qiang Yu Yuen Wu college of chemistry and environmental engineering Institute of Low-dimensional Materials Genome InitiativeShenzhen UniversityShenzhen 518071China School of chemistry and materials Science University of Science and Technology of ChinaHefei 230026China college of materials Science and engineering Shenzhen UniversityShenzhen 518071China Dalian National Laboratory for Clean Energy Dalian 116023China National Synchrotron Radiation Laboratory University of Science and Technology of ChinaHefei 230029China

Single atom catalysts have been recognized as potential catalysts to fabricate electrochemical biosensors,due to their unexpected catalytic selectivity and ***,we designed and fabricated an ultrasensitive dopamine(DA)sensor based on the flower-like MoS_(2) embellished with single Ni site catalyst(Ni-MoS_(2)).The limit of detection could achieve 1 pM in phosphate buffer solution(PBS,pH=7.4),1 pM in bovine serum(pH=7.4),and 100 pM in artificial urine(pH=6.8).The excellent sensing performance was attributed to the Ni single atom axial anchoring on the Mo atom in the MoS_(2) basal plane with the Ni-S_(3) *** the experiment and density functional theory(DFT)results certify that this structural feature is more favorable for the adsorption and electron transfer of DA on Ni *** high proportion of Ni active sites on MoS_(2) basal plane effectively enhanced the intrinsic electronic conductivity and electrochemical activity toward *** successful establishment of this sensor gives a new guide to expand the field of single atom catalyst in the application of biosensors.

关键词： single atom catalysts MoS_(2) dopamine(DA)sensor serum urine

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RuO_(2) clusters derived from bulk SrRuO_(3):Robust catalyst for oxygen evolution reaction in acid

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Nano Research 2022年第3期15卷 1959-1965页

作者： Muwei Ji Xin Yang Shengding Chang Wenxing Chen Jin Wang Dongsheng He Yao Hu Qian Deng You Sun Bo Li Jingyu Xi Tomoaki Yamada Jiatao Zhang Hai Xiao Caizhen Zhu Jia Li Yadong Li college of materials Science and engineering Shenzhen UniversityShenzhen 518060China institute of low-dimensional materials genome initiative College of Chemistry and Environmental Engineering of Shenzhen UniversityShenzhen 518060China Tsinghua Shenzhen International Graduate School Tsinghua UniversityShenzhen 518055China Beijing Key Laboratory of Construction Tailorable Advanced Functional materials and Green Applications School of Materials Science and EngineeringBeijing Institute of TechnologyBeijing 100081China materials Characterization and Preparation Center Southern University of Science and TechnologyShenzhen 518055China Department of Energy engineering Nagoya UniversityFuro-choChikusa-kuNagoya 464-8603Japan Department of chemistry Tsinghua UniversityBeijing 100084China

Developing highly efficient oxygen evolution reaction(OER)catalyst for the acidic corrosive operating conditions is a challenging ***,we report the synthesis of uniform RuO_(2)clusters with~2 nm in size via electrochemical leaching of Sr from SrRuO_(3) ceramic in *** RuO_(2)clusters exhibit ultrahigh OER activity with overpotential of~160 mV at 10 mA·cm_(geo)^(−2) in 1.0 M HClO4 solution for 30-h *** extended X-ray absorption fine structure measurement reveals enlarged Jahn-Teller distortion of Ru-O octahedra in the RuO_(2)clusters compared to its bulk *** function theory calculations show that the enhanced Jahn-Teller distortion can improve the intrinsic OER activity of RuO_(2).

关键词： oxygen evolution reaction RuO_(2)cluster electrochemical leaching acid solution

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