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Boosting thermal stability and crystallization of closed-loop-recyclable biodegradable poly(p-dioxanone) by end-group regulation

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Science China Chemistry 2024年第2期67卷 642-651页

作者： Jin Lei Zhu-Xin Gui Wan-Ting Xiong Gang Wu Si-Chong Chen Yu-Zhong Wang The Collaborative Innovation Center for Eco-Friendly and Fire-Safety polymeric Materials(MoE) National Engineering Laboratory of Eco-Friendly Polymeric Materials(Sichuan)State Key Laboratory of Polymer Materials EngineeringCollege of ChemistrySichuan UniversityChengdu610064China

A chemically closed-loop-recyclable biodegradable polymer,poly(p-dioxanone)(PPDO),is one of the ideal candidates for single-use plastic products due to its suitability for different application ***,when PPDO wastes can be collected,its monomer p-dioxanone(PDO) will be obtained through chemical recycling of these wastes;when cannot be collected,the wastes are able to be biodegraded into harmless ***,unsatisfied thermal stability and low crystallization rate of PPDO restrict its wider ***,based on end-group regulation,we simultaneously realized the significant enhancement of thermal stability and crystallization of PPDO through the simple melt processing with tributyl phosphite(TBP) or triphenyl phosphite(TPP).The model reactions were conducted to investigate the reaction mechanism and theoretical products during the preparation of PPDO/phosphite *** kinds of phosphites were proved to act as the end-capped reagent and chain extender in the melt processing,while TBP presented better *** a result,the activation energy of thermal decomposition was largely elevated,and the unprecedented T_(5%)(the temperature at a weight loss of 5%) and Tmax(the temperature at a maximum rate of weight loss) of PPDO were obtained,i.e.,T_(5%)of ~330 ℃ and Tmaxof ~385 ℃ in N_(2) atmosphere,T_(5%)of ~240 ℃ and Tmaxof ~317 ℃ in air atmosphere,***,the increased crystallization rate,crystallinity,crystalline orderliness,and realizable monomer recovery(yield >90%,purity >99.9%) of PPDO/phosphite compounds were confirmed.

关键词： poly(p-dioxanone) phosphite thermal stability crystallization end-group regulation

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Phosphorus-silicon-integrated electrolyte additive boosts cycling performance and safety of high-voltage lithium-ion batteries

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Chinese Chemical Letters 2024年第8期35卷 418-424页

作者： Mei-Chen Liu Qing-Song Liu Yi-Zhou Quan Jia-Ling Yu Gang Wu Xiu-Li Wang Yu-Zhong Wang The Collaborative Innovation Center for Eco-Friendly and Fire-Safety polymeric Materials(MoE) National Engineering Laboratory of Eco-Friendly Polymeric Materials(Sichuan)State Key Laboratory of Polymer Materials EngineeringCollege of ChemistrySichuan UniversityChengdu 610064China

Safety and energy density are significant for lithium-ion batteries(LIBs),and the flammable organic elec-trolyte is one of the most critical causes of the safety problem of *** LiNi0.8 Co 0.1 Mn 0.1 O 2(NCM811)cathode with high capacity can improve the energy density,the interface stability between NCM811 cathode and electrolytes needs to be ***,we report a multifunctional additive,diethyl(2-(triethoxysilyl)ethyl)phosphonate(DETSP),which can suppress the flammability of the elec-trolyte and enhance the cycling stability of NCM811 cathode with a capacity retention of 89.9%after 400 cycles at 1 C,while that of the blank electrolyte is merely 61.3%.In addition,DETSP is compati-ble well with the graphite anode without impairing the electrochemical ***,the performance and safety of NCM811/graphite full cells are also *** and theoretical re-sults demonstrate that DETSP can scavenge acidic byproducts and is beneficial to form a stable cathode-electrolyte interface(CEI).Accordingly,DETSP can potentially be an effective solution to ameliorating the safety of the commercial electrolyte and improving the stability of high-voltage cathodes.

关键词： Electrolyte additive NCM Lithium-ion batteries Safety Cathode-electrolyte interface

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In situ thermoresponsive supramolecular assembly for switchable circularly polarized luminescence

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Science China Chemistry 2024年第7期67卷 2362-2372页

作者： Menghan Pan Gong Zhang Haotian Ma Xiaoxiao Cheng Jieai Li Wei Zhang State and Local Joint Engineering laboratory for Novel Functional polymeric Materials Jiangsu Engineering Laboratory of Novel Functional Polymeric MaterialsSuzhou Key Laboratory of Macromolecular Design and Precision SynthesisCollege of ChemistryChemical Engineering and Materials ScienceSoochow UniversitySuzhou 215123China School of Chemical and Environmental Engineering Anhui Polytechnic UniversityWuhu 241000China

The dynamic regulation of circularly polarized luminescence(CPL)holds profound significance in various fields,such as highlevel information storage and *** we developed a chiral amphiphilic molecule,CPSB-GLU-PEG350(CGP),composed of aggregation-induced emission(AIE)chromophores(Z)-4-(1-cyano-2-phenylvinyl)benzoic acid(CPSB),a chiral linker Glutamic acid and polyethylene glycol(PEG)thermoresponsive *** the self-assembled supramolecular system formed by CGP,we have achieved in-situ temperature-responsive chiral structures,facilitating the thermal control switch of the CPL *** dynamics simulations demonstrate the distinct behaviors of AIE and PEG units during the temperature-variable assembly ***,by co-assembling achiral dye molecules with CGP,we have expanded the color range of the temperature-responsive CPL assembly system in situ and confirmed the occurrence of circularly polarizedF?rster resonance energy transfer(C-FRET)phenomenon in this process,which successfully enriched the strategies for in-situ CPL control in aqueous *** addition,the contactless radiative energy transfer of CPL can also be realized in this system,exhibiting more flexible temperature regulation of the CPL *** study provides a convenient and universal strategy for the construction of dynamically smart chiroptical materials.

关键词： circularly polarized luminescence in-situ thermoresponsive supramolecular assembly energy transfer

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Upcycling of Poly(butylene adipate-co-terephthalate)into Dual Covalent Adaptable Networks through Chain Breaking-Crosslinking Strategy

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Chinese Journal of Polymer Science 2024年第10期42卷 1505-1513,I0011页

作者： Bin-Bo Wang Rong Huang Xin Wang Tao Jiang Yi Wang Shuai Du Fa-Lin Li Jin Zhu Song-Qi Ma Key laboratory of Synthetic and Biological Colloids Ministry of EducationSchool of Chemical and Material EngineeringJiangnan UniversityWuxi214122China Key laboratory of Bio-based polymeric Materials Technology and Application of Zhejiang Province Divisions of Polymers and CompositesNingbo Institute of Materials Technology and EngineeringChinese Academy of SciencesNingbo315201China University of Chinese Academy of Sciences Beijing100049China

Poly(butylene adipate-co-terephthalate)(PBAT),a widely studied biodegradable material,has not effectively addressed the problem of plastic *** into consideration the cost-effectiveness,upcycling PBAT should take precedence over direct composting *** present work adopts a chain breaking-crosslinking strategy,upcycling PBAT into dual covalent adaptable networks(CANs).During the chainbreaking stage,the ammonolysis between PBAT and polyethyleneimine(PEI)established the primary crosslinked ***,styrene maleic anhydride copolymer(SMA)reacted with the hydroxyl group,culminating in the formation of dual covalent adaptable *** contrast to PBAT,the PBAT-dual-CANs exhibited a notable Young's modulus of 239 MPa,alongside an inherent resistance to creep and *** to catalysis from neighboring carboxyl group and excess hydroxyl groups,the PBAT-dual-CANs exhibited fast stress ***,they could be recycled through extrusion and hot-press reprocessing,while retaining their *** straightforward strategy offers a solution for dealing with plastic waste.

关键词： Poly(butylene adipate-co-terephthalate) Dynamic crosslinked networks Chain breaking-crosslinking strategy Upcycle Recycle

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Highly Transparent Fire-resistant Coatings with Intumescent Three-source Integration

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Chinese Journal of Polymer Science 2024年第7期42卷 907-915,I0005页

作者： Xiao-Liang Zeng Xin-Sheng Lan Yan Wang Lin Zhang De-Ming Guo Hai-Bo Zhao State Grid Sichuan Electric Power Research Institute Chengdu610041China The Collaborative Innovation Center for Eco-Friendly and Fire-Safety polymeric Materials(Ministry of Education) National Engineering Laboratory of Eco-Friendly Polymeric Materials(Sichuan)State Key Laboratory of Polymer Materials EngineeringCollege of ChemistrySichuan UniversityChengdu610064China

Wood,a readily available and sustainable natural resource,has found widespread use in construction and ***,its inherent flammability poses a potential fire *** intumescent fire-retardant coatings effectively mitigate this risk,achieving high transparency in such coatings presents a significant *** our approach,we employed a cross-linked network of phytic acid anion and N-[3-(trimethoxysilyl)propyl]-N,N,N-trimethylammonium cation to create a transparent"three-in-one"intumescent *** collaborative P/N/Si flame-retardant effect markedly improved the intumescent char-forming capability,preventing the wood from rapid *** resulted in a substantial reduction in heat release(13.9%decrease in THR)and an increased limiting oxygen index(LOI)value of 35.5%.Crucially,the high transparency of the coating ensured minimal impact on the wood's appearance,allowing the natural wood grains to remain clearly *** innovative approach provides a straightforward method for developing transparent intumescent flame-retardant coatings suitable for wooden *** potential applications extend to preserving ancient buildings and heritage conservation efforts.

关键词： Fire-resistant coating Flame retardancy Wood Transparency

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Rheological Behaviors of Polymers with Nanoparticles Tethered at Each End

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Chinese Journal of Polymer Science 2024年第3期42卷 400-406,I0009页

作者： Song-Qi Zhang Wen-Qing Wang Jia-Ping Lin Li-Quan Wang Shanghai Key laboratory of Advanced polymeric Materials Key Laboratory for Ultrafine Materials of Ministry of EducationSchool of Materials Science and EngineeringEast China University of Science and TechnologyShanghai 200237China

The polymer with nanoparticles tethered at each end is a unique model for unraveling the effect of chain ends on the polymer dynamics. We investigated the rheological behavior of this kind of polymer by using nonequilibrium molecular dynamics simulation. The effect of polymer lengths and nanoparticle radii on the complex moduli and viscosity was examined. The dependence of complex moduli on the frequency becomes less pronounced as the polymer is short or the nanoparticle is large. The shear thinning behavior was revealed for these systems, and the scaling exponent of complex viscosity with respect to the frequency was found to change from-1/2 to-3/4 as the polymer shortens or the nanoparticle enlarges. The rheological behavior was further explained by analyzing the mean square distance of nanoparticles. The simulation results were compared with the existing experimental finding, showing an agreement. The work provides information for understanding the chain end effect on polymer rheology.

关键词： Polymer rheology Modulus Viscosity Molecular dynamics

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Effect of samarium doping on the activity and sulfur resistance of Ce/MnFeO_(x) catalyst for low-temperature selective catalytic reduction of NO_(x) by ammonia

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Chinese Journal of Chemical Engineering 2024年第7期71卷 272-282页

作者： Qiyao Zhang Shuangshuang Zhang Xu Hu Yongmin Huang Key laboratory of Specially Functional polymeric Materials and Related Technology School of Chemistry and Molecular EngineeringEast China University of Science and TechnologyShanghai 200237China

The self-made MnFeO_(x) catalysts doped with cerium and samarium were prepared by impregnation method for low-temperature selective catalytic reduction(SCR)by *** this work,the surface properties of the series of MnFe-based catalysts were *** results indicate Sm-modified catalyst have superior low-temperature SCR activity;NO_(x) conversion maintained at nearby to 100%at 90℃ to 240℃.In addition,The N_(2) selectivity of Sm doping remains above 80%in the range of 60℃ to 150℃.In SO_(2) poisoning test,the NO_(x) conversion can be remained>90%after 10 h of *** XPS,NH_(3)-TPD and H_(2)-TPR results show the catalyst with Sm doping enhances the acid sites and oxidation catalytic sites of mixed oxides serves for improving oxygen vacancies and transfer *** situ diffuse reflaxions infrared Fourier transformations spectroscopy(DRIFTS)results show that NO_(x) is more easily adsorbed on the surface after Sm doping,which provided favorable conditions for the NH_(3)-SCR reaction to *** reaction at the catalyst surface will follow the L-H reaction mechanism by transient reaction test.

关键词： SCR Sm doping Catalyst Sulfur resistance In situ DRIFTS Selectivity

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Injection molding of highly filled microcrystalline cellulose/polycaprolactone composites with the aid of reversible Diels-Alder reaction

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Journal of Materials Science & Technology 2024年第3期170卷 246-254页

作者： Ze Pu Wang WenHong Ruan MinZhi Rong MingQiu Zhang Key laboratory for polymeric Composite and Functional Materials of MOE GD HPPC LabIGCMESchool of ChemistrySun Yat-Sen UniversityGuangzhou 510275China

To tackle the challenge of producing highly filled polymer composites using the traditional injection molding technique,which is characterized by the fairly high melt viscosity that makes mold filling difficult,the authors propose a solution based on dynamic covalent *** demonstrated by the proof-of-concept experiments,the 4-arm starshaped polycaprolactone(PCL)oligomers and microcrystalline cel-lulose(MCC)are crosslinked by the reversible Diels-Alder(DA)*** flowability of the compounds greatly decreases due to the dissociation of the intercomponent DA bonds at the retro-reaction tempera-ture,and the networked architecture is reconstructed during cooling as a result of the forward DA ***,the high-loading MCC fillers are well distributed in the matrix and covalently bonded to the nearby PCL,forming a striking contrast to the control in which linear PCL acts as the *** DA bonds crosslinked biodegradable PCL composites exhibit decent mechanical strength(20.7 MPa)even at the MCC fraction of 65 wt%,which is superior to those(5-12.2 MPa)of the highly filled PCL composites(with filler contents of 50-63.8 wt%)reported so *** proposed approach has sufficient expansibility for the fabrication of the highly filled polymer composites constructed by other types of matrix and fillers.

关键词： Polymer composites Microcrystalline cellulose Polycaprolactone Injection molding Dynamic reversible chemistry

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A tree-growing graphic model for asymmetrical phantom networks in polymeric gels undergoing dynamic mechanochemical coupling

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Science China(Technological Sciences) 2024年第2期67卷 558-567页

作者： SHI WeiLin ZHOU Jian LU HaiBao ELMARAKBI Ahmed FU Yong-Qing National Key laboratory of Science and Technology on Advanced composites in Special Environments Harbin Institute of TechnologyHarbin 150080China College of Mechanical and Vehicle Engineering Hunan UniversityChangsha 410082China Faculty of Engineering and Environment University of NorthumbriaNewcastle upon Tyne NEI 8STUK

Network structures of various polymers have significant effects on their mechanical properties;therefore,numerous studies have investigated the constitutive relationship between symmetrical network structures and their rubber elasticity in ***,few studies have focused on asymmetrical network structures in polymers that undergo bond exchange reactions,selfassembly,or mechanochemical coupling—all of which are induced by transition probabilities of chemical bonding *** this study,an extended constraint junction and phantom network model is formulated using the tree-growing theory to establish a constitutive relationship between asymmetrical network structures and their rubber elasticity in polymers.A free-energy equation is further developed to explore working principles of configurational transitions on the dynamic rubber elasticity of symmetrical and asymmetrical network *** constitutive relationship between dynamic rubber elasticity and symmetrical and asymmetrical network structures has also been proposed for the gels undergoing mechanochemical and hydromechanical ***,the effectiveness of this newly proposed tree-growing model has been verified by comparing with the classical affine network model,finite element analysis,and the experimental results of gels reported in literature.

关键词： gel polymer network rubber elasticity asymmetric

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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

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