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Understand the Temperature Sensing Behavior of Solid-state Polymerized PEDOT Hybrid Based on X-ray Scattering Studies

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Chinese Journal of Polymer Science 2024年第1期42卷 105-112,I0010页

作者： Zhen-Hang He Guang-Feng Liu Ze-Kun Zhou Zhen Liu Yi-Shu Zeng Peng Zhang School of materials Science and Engineering Key Laboratory for Polymeric Composite and Functional Materials of Ministry of EducationSun Yat-sen UniversityGuangzhou 510275China shanghai advanced Research Institute(Zhangjiang laboratory) Chinese Academy of SciencesShanghai 201204China

Poly(3,4-ethylenedioxythiophene)(PEDOT) is one of the most successful conductive polymers that recently has been used in wearable sensors for human health monitoring. In this work, we prepared a series of PEDOT hybrids consisting of PEDOT, sodium poly(styrene sulfonate)(PSSNa) and polyethylene oxide(PEO), and their preparation could be scaled-up via an adapted solid-state polymerization process. The resistance of the as-prepared PEDOT:PSS/PEO hybrid shows clear temperature response, i.e., it decreases almost linearly with the temperature increase. To understand this phenomenon, the in situ synchrotron radiation wide-and small-angle X-ray scattering(WAXS/SAXS) characterizations were undertaken to study the temperature-dependent microstructure change of the PEDOT:PSS/PEO hybrid. It demonstrated that PEDOT formed conductive paths in the hybrids, which were not destroyed by the PEO crystallization. As temperature increased, the PEO crystals' melting and the accompanying reorganization of PEDOT chains endowed the hybrid sample temperature responsiveness. Based on these fundamental knowledges, the hybrid materials were used to fabricate flexible wearable sensor that showing temperature sensing performance with an accuracy of 1 ℃. These findings shed lights on the scalable manufacturing of wearable sensors for body temperature monitoring.

关键词： Solid-state polymerization PEDOT hybrid Structure-property correlation X-ray scattering

Nano-silica modified lightweight and high-toughness carbon fiber/phenolic ablator with excellent thermal insulation and ablation performance

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Defence Technology（防务技术） 2024年第1期31卷 192-199页

作者： Wenjie Xu Wenda Song Xianfeng Jia Cheng Ma Jitong Wang Wenming Qiao Licheng Ling State key laboratory of Chemical Engineering East China University of Science and TechnologyShanghai 200237China School of Chemical Engineering and materials Changzhou Institute of TechnologyChangzhou 213032China key laboratory of Specially Functional polymeric materials and Related Technology(ministry of education. School of Materials Science and EngineeringEast China University of Science and TechnologyShanghai 200237China

Lightweight and high-toughness carbon fiber/phenolic ablator(CFPA)is required as the Thermal Protection System(TPS)material of aerospace vehicles for next-generation space missions.To improve the ablative properties,silica sol with good particle size distribution prepared using tetramethoxysilane(TMOS)was blended with natural rubber latex and deposited onto carbon fiber felt,which was then integrated with phenolic aerogel matrix,introducing nano-silica into the framework of CFPA.The modified CFPA with a low density of 0.28—0.31 g/cm3exhibits strain-in-fracture as high as 31.2%and thermal conductivity as low as 0.054 W/(m·K).Furthermore,a trace amount of nano-silica could effectively protect CFPA from erosion of oxidizing atmosphere in different high-temperature environments.The oxyacetylene ablation test of 3000°C for 20 s shows a mass ablation rate of 0.0225 g/s,a linear ablation rate of 0.209 mm/s for the modified CFPA,which are 9.64%and 24.82%lower than the unmodified one.Besides,the long-time butane ablation test of 1200°C for 200 s shows an insignificant recession with mass and linear ablation rate of 0.079 g/s and 0.039 mm/s,16.84%and 13.33%lower than the unmodified one.Meanwhile,the fixed thermocouple in the test also demonstrates a good thermal insulation performance with a low peak back-face temperature of 207.7°C,12.25%lower than the unmodified one.Therefore,the nano-silica modified CFPA with excellent overall performance presents promising prospects in high-temperature aerospace applications.

关键词： Nano-silica Carbonfiber Phenolic aerogel Insulation Ablation

MIL-100(V) derived porous vanadium oxide/carbon microspheres with oxygen defects and intercalated water molecules as high-performance cathode for aqueous zinc ion battery

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Journal of Energy Chemistry 2024年第3期90卷 578-589,I0013页

作者： Yuexin Liu Jian Huang Xiaoyu Li Jiajia Li Jinhu Yang Kefeng Cai shanghai key laboratory of Development and Application for Metal-Functional materials Key Laboratory of Advanced Civil Engineering MaterialsMinistry of EducationSchool of Materials Science&EngineeringTongji UniversityShanghai 201804China State key laboratory of High Performance Ceramics and Superfine Microstructure Shanghai Institute of CeramicsChinese Academy of SciencesShanghai 201800China Research Center for Translational Medicine East HospitalTongji University School of MedicineShanghai 200092China

The development of aqueous zinc ion battery cathode materials with high capacity and high magnification is still a challenge.Herein,porous vanadium oxide/carbon(p-VO_(x)@C,mainly VO_(2) with a small amount of V_(2)O_(3)) core/shell microspheres with oxygen vacancies are facilely fabricated by using a vanadium-based metal-organic framework(MIL-100(V)) as a sacrificial template.This unique structure can improve the conductivity of the VO_(x),accelerate electrolyte diffusion,and suppress structural collapse during circulation.Subsequently,H_(2)O molecules are introduced into the interlayer of VO_(x) through a highly efficient in-situ electrochemical activation process,facilitating the intercalation and diffusion of zinc ions.After the activation,an optimal sample exhibits a high specific capacity of 464.3 mA h g^(-1) at0.2 A g^(-1) and 395.2 mA h g^(-1) at 10 A g^(-1),indicating excellent rate performance.Moreover,the optimal sample maintains a capacity retention of about 89.3% after 2500 cycles at 10 A g^(-1).Density functional theory calculation demonstrates that the presence of oxygen vacancies and intercalated water molecules can significantly reduce the diffusion barrier for zinc ions.In addition,it is proved that the storage of zinc ions in the cathode is achieved by reversible intercalation/extraction during the charge and discharge process through various ex-situ analysis technologies.This work demonstrates that the p-VO_(x)@C has great potential for applications in aqueous ZIBs after electrochemical activation.

关键词： Metal-organic frameworks Vanadium oxide Carbon Zn-ion batteries Electrochemical activation

Evaluating two stages of silicone-containing arylene resin oxidation via experiment and molecular simulation

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Chinese Journal of Chemical Engineering 2024年第2期66卷 189-202页

作者： Jiangtao Cai Qingfu Huang Huan Chen Tao Zhang Bo Niu Yayun Zhang Donghui Long key laboratory of Chemical Engineering East China University of Science and TechnologyShanghai 200237China key laboratory of Special Functional polymeric materials and Related Technology(ministry of education. School of Chemical EngineeringEast China University of Science and TechnologyShanghai 200237China

Silicon-containing aryl acetylene resin(PSA)is a new type of high-temperature resistant resin with excellent oxidation resistance,whereas antioxidant reaction mechanism of PSA resin under ultra-high temperatures still remains unclear.Herein,the oxidation behavior and mechanisms of PSA resin are systematically investigated combining kinetic analysis and Reax FF molecular dynamics(MD)simulations.Thermogravimetric analysis indicates that the oxidation process of PSA resin undergoes two main steps:oxidative mass gain and oxidative degradation.The distributed activation energy model(DAEM)is employed for describing oxidation processes and the best-fit one is obtained using genetic algorithms and differential evolution.DAEM model demonstrates that the oxidative weight gain stage is dominated by two virtual reactants and the oxidative degradation stage consists of three virtual reactants.Correspondingly,the observation of MD reaction pathways indicates that oxygen oxidation of unsaturated structures occurs in the initial stage,which results in the formation of PSA resin oxides.Furthermore,cracked pieces react with O_(2)to generate CO and other chemicals in the second step.The resin matrix's great antioxidation resilience is illustrated by the formation of SiO_(2).The analysis based on MD simulations exhibits an efficient computational proof with the experiments and DAEM methods.Based on the results,a two-stage reaction mechanism is proposed,which provides important theoretical support for the subsequent study of the oxidation behavior of silica-based resins.

关键词： PSA resin Oxidative degradation Thermogravimetric analysis DAEM reaction kinetics ReaxFF simulation

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Stress relaxation properties of calcium silicate hydrate:a molecular dynamics study

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Journal of Zhejiang University-Science A(Applied Physics & Engineering) 2024年第2期25卷 97-115页

作者： Zhicheng GENG Shengwen TANG Yang WANG Hubao A Zhen HE Kai WU Lei WANG State key laboratory of Water Resources Engineering and Management Wuhan UniversityWuhan430072China key laboratory of advanced Civil Engineering materials of ministry of education School of Materials Science and EngineeringTongji UniversityShanghai200092China College of materials Science and Engineering Xi’an University of Architecture and TechnologyXi’an710055China

The time-dependent viscoelastic response of cement-based materials to applied deformation is far from fully understood at the atomic level.Calcium silicate hydrate(C-S-H),the main hydration product of Portland cement,is responsible for the viscoelastic mechanism of cement-based materials.In this study,a molecular model of C-S-H was developed to explain the stress relaxation characteristics of C-S-H at different initial deformation states,Ca/Si ratios,temperatures,and water contents,which cannot be accessed experimentally.The stress relaxation of C-S-H occurs regardless of whether it is subjected to initial shear,tensile,or compressive deformation,and shows a heterogeneous characteristic.Water plays a crucial role in the stress relaxation process.A large Ca/Si ratio and high temperature reduce the cohesion between the calcium-silicate layer and the interlayer region,and the viscosity of the interlayer region,thereby accelerating the stress relaxation of C-S-H.The effect of the hydrogen bond network and the morphology of C-S-H on the evolution of the stress relaxation characteristics of C-S-H at different water contents was elucidated by nonaffine mean squared displacement.Our results shed light on the stress relaxation characteristics of C-S-H from a microscopic perspective,bridging the gap between the microscopic phenomena and the underlying atomic-level mechanisms.

关键词： Calcium silicate hydrate(C-S-H) Stress relaxation Ca/Si ratio Temperature Water content Atomic simulation

Combination of methylthio-chemistry with living crystallization-driven self-assembly toward uniformπ-conjugated nanostructures with antibacterial activity,surface tailorability,tunable morphology and dimension

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Science China Chemistry 2024年第7期67卷 2341-2352页

作者： Chuyu Duan Binbin Xu Ruru Li Xiaoyu Huang Shaoliang Lin Chun Feng shanghai key laboratory of advanced polymeric materials School of Materials Science and EngineeringEast China University of Science and TechnologyShanghai 200237China School of Chemistry and materials Science Hangzhou Institute for Advanced StudyUniversity of Chinese Academy of SciencesHangzhou 310024China key laboratory of Fluorine and Nitrogen Chemistry and advanced materials Shanghai Institute of Organic ChemistryChinese Academy of SciencesShanghai 200032China

Living crystallization-driven self-assembly(CDSA)provides robust access to uniformπ-conjugated nanostructures(CNSs)from block copolymers(BCPs)containing a crystallineπ-conjugated segment with controlled dimension,morphology and composition,which show appealing applications in biomedicine,photocatalysis and microelectronics.To further expand the application spectrum of these CNSs,the development of facile strategies toward diverse CNSs with varying structures/functionalities is highly desired.Herein,BCPs consisting of oligo(p-phenylene ethynylene)-b-poly(polypropyl-3-methanethiol acrylate)(OPE_(9)-bPMTPA35and OPE_(9)-b-PMTPA_(58);the subscript represents the number of repeat unit of each block)consisting of a crystallineπ-conjugated core-forming OPE_(9)segment and a corona-forming PMTPA block are synthesized.By efficient“click-type”alkylation of methylthio groups,OPE_(9)-b-PMTPA with varying contents of sulfonium unit is obtained.Uniform ribbon-like micelles with different widths and lengths can then be generated in a controlled manner via the self-seeding approach of living CDSA.Additionally,negatively charged polymeric and Ag nanoparticles can be immobilized on sulfonium/methylthio-containing shells by taking advantage of electrostatic attraction and coordination interaction,respectively.Interestingly,the ribbon-like micelles with positively charged shells exhibit antibacterial activity against E.coli.Given the ease of modification of PMTPA-based shell and attractive opto-electronic/photocatalytic properties ofπ-conjugated units,the combination of methylthio-chemistry and living CDSA opens a new avenue to generate multi-functional CNSs for widespread applications from biomedicine to photocatalysis.

关键词： crystallization-driven self-assembly block copolymer π-conjugated nanostructure methylthio-chemistry

Revisiting the sodium-ion storage capability of hard carbon in carbonate-based electrolytes via a sodium-metal-free protocol

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Science China Chemistry 2024年第7期67卷 2240-2247页

作者： Gaopan Liu Yanbing Mo Jiawei Chen Yu Peng Xiao Zhu Fei Wang Xiaoli Dong Yongyao Xia Department of Chemistry and shanghai key laboratory of Molecular Catalysis and Innovative materials Institute of New EnergyLaboratory of Advanced MaterialsFudan UniversityShanghai 200438China

Common evaluation methodology of sodium(Na)-containing two-electrode or three-electrode configurations overlooks the interference from highly reactive Na metal,leading to the underestimation or inconsistent performance of low-potential hard carbon(HC)electrodes.Herein,the trap of Na metal was systematically investigated with or without applied current,uncovering its inadequacy as the reference or counter electrode in different configurations.A Na-metal-free three-electrode protocol is proposed for evaluating the actual Na^(+)-storage capability of the typical low-potential HC electrode.By avoiding Na crosstalk and precisely controlling the working electrode's potential,the actual electrochemical performance of HC in the carbonate esterbased electrolyte can be recognized with high capacity of 222 mAh g^(-1)at 2 C and 113 mAh g^(-1)at 5 C,correcting the misunderstanding of the inferior performance of HC in coin-type half cells(68%and 50%undervaluation at 2 C and 5 C,respectively).The advanced protocol is expected to reduce misunderstandings or underestimation due to evaluation methods and to guide the development of high-performance battery materials.

关键词： highly reactive sodium potential drift carbonate ester sodium-metal-free protocol sodium storage capability

Intramolecular Hydrogen Bond Improved Durability and Kinetics for Zinc‑Organic Batteries

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Nano-Micro Letters 2024年第3期16卷 138-148页

作者： Tianjiang Sun Jun Pan Weijia Zhang Xiaodi Jiang Min Cheng Zhengtai Zha Hong Jin Fan Zhanliang Tao key laboratory of advanced Energy materials Chemistry(ministry of education. Renewable Energy Conversion and Storage CenterCollege of ChemistryNankai UniversityHaihe Laboratory of Sustainable Chemical TransformationsTianjin 300071People’s Republic of China School of Physical and Mathematical Sciences Nanyang Technological UniversitySingapore 637371Singapore shanghai key laboratory of Special Artificial Microstructure materials and Technology School of Physics Science and EngineeringTongji UniversityShanghai 200092People’s Republic of China

Organic compounds have the advantages of green sustainability and high designability,but their high solubility leads to poor durability of zinc-organic batteries.Herein,a high-performance quinone-based polymer(H-PNADBQ)material is designed by introducing an intramolecular hydrogen bonding(HB)strategy.The intramolecular HB(C=O⋯N-H)is formed in the reaction of 1,4-benzoquinone and 1,5-naphthalene diamine,which efficiently reduces the H-PNADBQ solubility and enhances its charge transfer in theory.In situ ultraviolet-visible analysis further reveals the insolubility of H-PNADBQ during the electrochemical cycles,enabling high durability at different current densities.Specifically,the H-PNADBQ electrode with high loading(10 mg cm^(-2))performs a long cycling life at 125 mA g^(-1)(>290 cycles).The H-PNADBQ also shows high rate capability(137.1 mAh g^(−1)at 25 A g^(−1))due to significantly improved kinetics inducted by intramolecular HB.This work provides an efficient approach toward insoluble organic electrode materials.

关键词： Zn-organic batteries H-PNADBQ polymer Intramolecular hydrogen bond Reduced solubility Improvedπ-conjugated level

Self assembled electron blocking and lithiophilic interface towards dendrite-free solid-state lithium battery

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Chinese Chemical Letters 2024年第4期35卷 220-225页

作者： Caixia Li Yi Qiu Yufeng Zhao Wuliang Feng Institute for Sustainable Energy&College of Sciences Shanghai UniversityShanghai 200444China key laboratory of advanced Energy materials Chemistry(ministry of education. Nankai UniversityTianjin 300071China

The poor interfacial contact is one of the biggest challenges that solid-state lithium batteries suffer from.Reducing the solid-state electrolyte surface energy by transforming the interface from lithiophobic to lithiophilic is effective to promote the interfacial contact, but electronic conductive interphases usually increase the risk of electron attack, thus leading to uncontrollable Li dendrite growth. Herein, we propose a self-assembled thermodynamic stable Li I interphase to simultaneously improve the interfacial contact between the garnet electrolyte Li_7La_(3)Zr_(2)O_(12)(LLZO) and Li anode, and prohibit the electron attack. The direct contact between LLZO and Li and the high temperature Li melting process was ascribed to Zr4+reduction, which facilitated Li dendrite formation and propagation. With the modification of the high lithiophilic I_(2) thin film, the area specific interfacial resistance of LLZO/Li was reduced from 1525 Ω/cm^(2) to 57 Ω/cm^(2). More importantly, LLZO was protected from being reduced due to the outstanding electronic insulativity of the Li I interphase, which leaded to a high critical current density of 1.2/7.0 m A/cm^(2) in the time/capacity-constant modes, respectively.

关键词： Li_7La_(3)Zr_(2)O_(12) LiI interphase Interfacial contact Li dendrite Thermodynamic stable