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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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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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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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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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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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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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Reversibly Cross-Linking Polyimide and Cyclophosphazene Toward Closed-Loop Recyclable Plastics with High Mechanical Strength,Excellent Flame Retardancy,and Chemical Resistance

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CCS Chemistry 2024年第4期6卷 976-987页

作者： Tingting Guan Xiaohan Wang Xi Zhao Xingyuan Lu Xiu-Li Wang Yu-Zhong Wang Junqi Sun State Key laboratory of Supramolecular Structure and materials College of ChemistryJilin UniversityChangchun 130012 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 610064

Traditional flame-retardant plastics are technically difficult to chemically *** development of newtypes of flame-retardant plastics that are intrinsically capable of being closed-loop recycled and are sufficiently robust and stable to satisfy their practical application is urgently *** this study,closed-loop recyclable flame-retardant plastics with high mechanical strength and excellent chemical resistance are fabricated by cross-linking amino-terminated polyimide(PI-NH_(2))and aldehyde-terminated cyclophosphazene(CP-CHO)with imine *** resultant flame-retardant plastic,which is denoted as PI-CP,exhibits a tensile strength of∼115.6 MPa,Young’s modulus of∼2.5 GPa,and glass transition temperature of 316°*** the PI-CP plastic,the imine bonds are isolated within hydrophobic microenvironments generated by the rigid and hydrophobic polyimide chains and the benzene ring of *** a result,the PI-CP plastics are highly stable in highly acidic and basic aqueous solutions and other commonly used organic *** PI-CP plastic shows outstanding flame retardancy with a limiting oxygen index value of 48.8%.More importantly,the PI-CP plastic can be depolymerized to generate the original PI-NH_(2)and CPCHO monomers in high yields(∼97%)and *** recovered monomers can be used to refabricate the original plastics,establishing highly efficient polymer-monomer-polymer circulation and a sustainable plastics economy.

关键词： closed-loop recyclable plastics recyclable polymers reversibly cross-linked polymers flame retardancy supramolecular polymers

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Thienothiophene-centered ladder-type π-systems that feature distinct quinoidal π-extension

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Chinese Chemical Letters 2024年第5期35卷 249-253页

作者： Jiaxiang Guo Zeyi Li Tianyu Zhang Xinyu Tian Yue Wang Chuandong Dou State Key laboratory of Supramolecular Structure and materials College of ChemistryJilin UniversityChangchun 130012China Jiangsu Engineering laboratory of Novel Functional polymeric materials Soochow UniversitySuzhou 215123China

Quinoidalπ-conjugated structures,a kind of fundamental subunits for organicπ-systems,may produce some intriguing optical,electronic and magnetic properties of polycyclic hydrocarbons(PHs).Herein,we report two thienothiophene-centered ladder-type polycyclic molecules(1 and 2),which possess one quinoidal thienothiophene moiety and two para-quinodimethane(p-QDM)subunits,*** theoretically and experimentally studied,while 1 is a fully closed-shell molecule,2 owns an open-shell structure along with partial contribution of tetraradical state that is induced by the resonance of ***,although 2 has a largerπ-conjugated skeleton and open-shell electronic state,it exhibits larger bandgap and blue-shifted *** the other hand,the reversible oxidation activity of 1 enables the preparation of its dication 1^(2+),and the studies on its single-crystal and aromatic structures demonstrate that its two positive charges are delocalized onto the oxygen atoms,thus achieving fullyπ-extended structure and near-infrared *** study not only gains insight into quinoidalπ-subunits,but also provides an important basis for the development of antiaromatic and open-shellπ-electron materials.

关键词： Thienothiophene Quinoidal conjugation Open-shell structure Aromaticity Photophysical properties

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Polymer Mechanochemistry on Reactive Species Generated from Mechanochemical Reactions

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Chinese Journal of Chemistry 2024年第12期42卷 1418-1432页

作者： Xiaolong Chen Hang Shen Zhengbiao Zhang State and Local Joint Engineering laboratory for Novel Functional polymeric materials Suzhou Key Laboratory of Macromolecular Design and Precision SynthesisCollege of ChemistryChemical Engineering and Materials ScienceSoochow UniversitySuzhouJiangsu 215123China

Comprehensive Summary Polymer mechanochemistry on reactive species has attracted more and more attentions over the past 20 years,as the mechanochemical generation of reactive species has a great potential in developing different polymeric materials for various purposes,such as stress detection,self-healing,self-strengthening,controllable degradation and release of small *** this review,we first discuss the recent progress on polymer mechanochemistry of the reactive species that are generated from the mechanochemical reactions of *** types of reactive species,including radical,zwitterion,ionic,carbene and neutral intermediates,and their applications were reviewed in *** mechanochemical reactions are sensitive to the mechanophore structure and polymer framework,we then discuss how mechanophore isomerism,polymer structure,polymer attachment point,and polymer architecture influence the mechanophore *** last,we provide our perspectives on the polymer mechanochemistry of reactivespecies.

关键词： Stimuli-responsive polymers Polymer mechanochemistry Mechanophore Mechanochemical reaction Reactive species

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Persistent radical anion of perylene dianhydride:an emerging metal-free photocatalyst for near-infrared photocontrolled RAFT polymerization

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Science China Chemistry 2024年第2期67卷 677-686页

作者： Haitao Zhao Guoqing Bian Xiang Xu Weiwei He Lifen Zhang Zhenping Cheng State and Local Joint Engineering laboratory for Novel Functional polymeric materials Jiangsu Key Laboratory of Advanced Functional Polymer Design and ApplicationSuzhou Key Laboratory of Macromolecular Design and Precision SynthesisCollege of ChemistryChemical Engineering and Materials ScienceSoochow UniversitySuzhou215123China

Developing a new type of photocatalyst(PC) and catalytic mechanism for near-infrared(NIR) photocontrolled reversibledeactivation radical polymerization(RDRP) system is charming but ***,a novel PC of the persistent radical anion(PRA)(possessing the properties of both radical and anion) was developed for NIR photocontrolled reversible additionfragmentation chain transfer(RAFT) polymerization,enabling successful polymerization while gaining a deep insight into the mechanism of photo-induced electron transfer RAFT(PET-RAFT) *** from the conventional and wellaccepted reductive quenching(RQ) pathway,in which the radical anion intermediates of PCs(PCs^(·-)) must be generated in an excited state(ES),here,the PRA(3,4,9,10-perylenetetracarboxylic dianhydride radical anion(PTCDA^(·-))) could generate conveniently in situ in the ground state(GS) and subsequently serve as highly efficient PC in the NIR region(740–850 nm).The successful implementation of this strategy elucidates the peculiar role played by light and the real way of electron transfer *** fact,the transfer of a single electron from PRA to chain transfer agent(CTA) and cleavage of the C–S bonds is a process from ES to GS,rather than always from GS(PCs^(·-)) to GS(CTA) in the RQ pathway as is well known to *** addition,the excellent spatial-temporal control and powerful penetration ability of the NIR light were also confirmed by this PRAcatalyzed polymerization system.

关键词： photocatalyst persistent radical anion(PRA) near-infrared(NIR)light reversible-deactivation radical polymerization(RDRP) photo-induced electron transfer RAFT(PET-RAFT)polymerization

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