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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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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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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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New sustainable polymers with on-demand depolymerization property

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Science China Chemistry 2024年第9期67卷 2803-2841页

作者： Yangyang Sun Zesheng An Yanshan Gao Rongrong Hu Ye Liu Hua Lu Xiao-Bing Lu Xuan Pang Anjun Qin Yong Shen Youhua Tao Yu-Zhong Wang Junpeng Wang Gang Wu Guang-Peng Wu Tie-Qi Xu Xing-Hong Zhang Yuetao Zhang Zhenbiao Zhang Jian-Bo Zhu Miao Hong Zhibo Li State Key Laboratory of Organometallic Chemistry Shanghai Institute of Organic Chemistry Chinese Academy of Sciences State Key Laboratory of Supramolecular Structure and materials College of Chemistry Jilin University State Key Laboratory of Luminescent materials and Devices Guangdong Provincial Key Laboratory of Luminescence from Molecular Aggregates South China University of Technology State Key Laboratory of Fine Chemicals Frontiers Science Center for Smart Materials Dalian University of Technology Beijing National Laboratory for molecular Sciences Center for Soft Matter Science and Engineering Key Laboratory of Polymer Chemistry and Physics of Ministry of Education College of Chemistry and Molecular Engineering Peking University Key Laboratory of Polymer ecomaterials Changchun Institute of Applied Chemistry Chinese Academy of Sciences State Key Laboratory Base of eco-Chemical Engineering College of Chemical Engineering Qingdao University of Science and Technology The collaborative innovation center for eco-friendly and fire-safety polymeric materials (mo 5 National Engineering Laboratory of Eco-Friendly Polymeric Materials (Sichuan) College of Chemistry State Key Laboratory of Polymer Materials Engineering Sichuan University School of Polymer Science and Polymer Engineering the University of Akron moE Key Laboratory of Macromolecular Synthesis and Functionalization Department of Polymer Science and Engineering Zhejiang University State and Local Joint Engineering Laboratory for Novel Functional polymeric materials Jiangsu Key Laboratory of Advanced Functional Polymer Design and Application Suzhou Key Laboratory of Macromolecular Design and Precision Synthesis College of ChemistryChemical Engineering and Materials Science Soochow University

To combat the crisis of today's synthetic polymers arising from unsustainable production and disposal, it is essential for the synthetic polymer community to reshape the current polymer industry with sustainable polymers. As an emerging class of sustainable polymers, the development of chemically depolymerizable polymers(CDPs), which can undergo closed-loop depolymerization/repolymerization cycles to reproduce virgin polymers without the loss of properties from recovered monomers, offers an ideal solution to preserve finite natural resources, provides a feasible solution to the end-of-life issue of polymer waste, and thereby establishes a circular materials economy. However, two grand key challenges have been encountered in the establishment of practically useful CDPs: how to balance polymerization and depolymerization ability and how to unify conflicted depolymerizability and physical properties. Accordingly, this critical review article presents our vision for summarizing feasible strategies to overcome the above two significant challenges and the design principles for constructing an ideal CDP by highlighting selected major progress made in this rapidly expanding field.

关键词： chemically depolymerizable polymers sustainable polymers depolymerization monomer recovery degradation plastics

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Multifunctional protective aerogel with superelasticity over−196 to 500℃

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Nano Research 2022年第9期15卷 7797-7805页

作者： Bo-Wen Liu Min Cao Yi-Ying Zhang Yu-Zhong Wang Hai-Bo Zhao 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

Protective materials that possess superelasticity and multifunctionality over a broad temperature range are urgently needed in various advanced ***,under harsh work conditions,the performance of current materials may largely deteriorate to lose protective ***,we report a bidirectionally oriented multi-walled carbon nanotubes(MWCNTs)-reinforced chitosan carbon aerogel(CS-MWCNT)that possesses superelasticity,high electromagnetic interference shielding,thermal insulation,and infrared stealth at both low temperatures(such as liquid nitrogen)and high temperatures(such as alcohol flames).Highly oriented lamellar arch structures combined with an MWCNTs-reinforced carbon skeleton act as elastic segments to disperse the stress during compression and endow CS-MWCNT with the ability to recover to almost the original size after being compressed at−196-500℃.The lamellar structures make CS-MWCNT thermally insulating and infrared stealth with a low thermal conductivity of~0.03 W/(m·K).Furthermore,a high electromagnetic interference(EMI)shielding effect of 64 dB is realized via an absorption-dominant EMI shielding mechanism derived from the successive inherently conductive carbon lamella,and the EMI shielding performance is largely maintained after treatment under extreme conditions like low temperature,high temperature,as well as cyclic *** work provides a new strategy for the development of temperature-invariant multifunctional aerogels for harsh environment applications.

关键词： superelasticity electromagnetic interference shielding heat insulation infrared stealth extreme environment

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Thermotolerant and fireproof gel polymer electrolyte toward high-performance and safe lithium-ion battery

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Journal of Energy Chemistry 2022年第2期31卷 9-18页

作者： Man-Cheng Long Ting Wang Ping-Hui Duan You Gao Xiu-Li Wang Gang Wu 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

Poly(ethylene oxide)(PEO)and its derivatives based gel polymer electrolytes(GPEs)are severely limited in advanced and safe lithium-ion batteries(LIBs)owing to the intrinsically high flammability of liquid electrolytes and *** adding flame retardants to the GPEs can suppress their flammability and thus improve the safety of LIBs,but results in deteriorative electrochemical ***,a novel GPE with chemically bonded flame retardant(*** vinylphosphonate)in cross-linked polyethylene glycol diacrylate matrix,featuring both high-safety and high-performance,is *** as-prepared GPE storing the commercial 1 mol L^(-1) LiPF6 electrolyte resists high temperature of 200℃and cannot be ignited as well as possesses a high ionic conductivity(0.60 m S cm^(-1))and good compatibility with ***,the LiFePO_(4)/Li battery with this GPE delivers a satisfactory capacity of 142.2 m A h g^(-1) and a superior cycling performance with a capacity retention of 96.3%and a coulombic efficiency of close to 100%for 350 cycles at 0.2 C under ambient ***,the battery can achieve steady charge–discharge for 100 cycles with a coulombic efficiency of 99.5%at 1 C under 80℃and run normally even at a high temperature of 150℃or under the exposure to butane *** scanning calorimetry manifests significantly improved battery safety compared to commercial battery *** work provides a new pathway for developing next-generation advanced LIBs with enhanced performance and high safety.

关键词： Gel polymer electrolyte Poly(ethylene oxide) Flame retardant Vinylphosphonate Lithium-ion batteries

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Chemically recyclable copolyesters from bio-renewable monomers:controlled synthesis and composition-dependent applicable properties

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Science China Chemistry 2023年第7期66卷 2062-2069页

作者： 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 UniversityChengdu 610064China

The development of chemically recyclable polymers is a promising solution to address the dual challenges of the environment and resources caused by petroleum-based *** recent advancements,it is highly desirable for developing recyclable polymers to meet the requirements of both practical uses and well-performed ***-renewable monomers have been paid great attention recently as promising potential candidates for establishing a sustainable circular polymer ***,a sequential copolymerization of various bio-renewable n-alkyl substituted δ-valerolactone((R)VLs)and p-dioxanone(PDO)is conducted to synthesize novel chemically recyclable diblock copolymers poly(p-dioxanone)-block-poly(n-alkyl-valerolactones)(PPDO-b-P(R)VLs)with well-defined and controlled *** properties of copolymers including thermal property,crystallization,mechanical property,hydrophilicity and transport property can be tuned effectively to meet the requirements of practical uses by alternating the alkyl substituents(R)and the P(R)VLs *** addition,the high-efficiency and facile chemical recycling of copolymers to PDO and(R)VL comonomers is realized with a high yield of>96.5%and a high purity of 99%.

关键词： bio-renewable monomers ring-opening polymerization block copolyester tunable properties chemical recyclability

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Electrode-compatible fluorine-free multifunctional additive regulating solid electrolyte interphase and solvation structure for high-performance lithium-ion batteries

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能源化学:英文版 2023年第8期83卷 239-246,I0008页

作者： Qing-Song Liu Yi-Zhou Quan Mei-Chen Liu Guo-Rui Zhu Xiu-Li Wang Gang Wu 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 610064SichuanChina

The rapid development and widespread application of lithium-ion batteries(LIBs) have increased demand for high-safety and high-performance LIBs. Accordingly, various additives have been used in commercial liquid electrolytes to severally adjust the solvation structure of lithium ions, control the components of solid electrolyte interphase, or reduce flammability. While it is highly desirable to develop low-cost multifunctional electrolyte additives integrally that address both safety and performance on LIBs, significant challenges remain. Herein, a novel phosphorus-containing organic small molecule, bis(2-methoxyethyl) methylphosphonate(BmoP), was rationally designed to serve as a fluorine-free and multifunctional additive in commercial electrolytes. This novel electrolyte additive is low-toxicity,high-efficiency, low-cost, and electrode-compatible, which shows the significant improvement to both electrochemical performance and fire safety for LIBs through regulating the electrolyte solvation structure, constructing the stable electrode-electrolyte interphase, and suppressing the electrolyte combustion. This work provides a new avenue for developing safer and high-performance LIBs.

关键词： Multifunctional additives Electrode compatibility Solid electrolyte interface Solvation structure Lithium-ion batteries

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Flame-retardant oligomeric electrolyte additive for self-extinguishing and highly-stable lithium-ion batteries:Beyond small molecules

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Journal of Energy Chemistry 2023年第9期84卷 374-384页

作者： Yi-Zhou Quan Qing-Song Liu Mei-Chen Liu Guo-Rui Zhu 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 610064SichuanChina

Preparing both safe and high-performance lithium-ion batteries(LIBs) based on commonly used commercial electrolytes is highly desirable,yet *** overcome the poor compatibility of conventional small-molecular flame-retardants as electrolyte additives for safe LIBs with graphite anodes,in this study,we propose and design a novel low-cost flame-retardant oligomer that achieves an accurate and complete reconciliation of fire safety and electrochemical performance in *** to the integration of phosphonate units and polyethylene glycol(PEG) chains,this oligomer,which is a phosphonatecontaining PEG-based oligomer(PPO),not only endows commercial electrolytes with excellent flame retardancy but also helps stabilize the electrodes and Li-ion ***,adding 15 wt% of PPO can reduce 70% of the self-extinguishing time and 54% of total heat release for commercial ***,LiFePO_(4)/lithium and graphite/lithium cells as well as LiFePO_(4)/graphite pouch full cells exhibit good long-term cycling stability.

关键词： Flame-retardant oligomer safety Compatibility Graphite anodes Lithium-ion batteries

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Controlled synthesis and closed-loop chemical recycling of biodegradable copolymers with composition-dependent properties

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Science China Chemistry 2022年第5期65卷 943-953页

作者： Yi-Teng Yan Gang Wu Si-Chong Chen Yu-Zhong Wang The collaborative innovation center for eco-friendly and fire-safety polymeric materials(moE) National Engineering Laboratory ofEco-Friendly Polymeric Materials(Sichuan)State Key Laboratory of Polymer Materials EngineeringCollege of ChemistrySichuan UniversityChengdu 610064China

The closed-loop recycling concept of the polymer wastes into building-block chemicals is attractive,but the closed-loop recycling of copolymers enabled by energy-efficient chemical recycling and cost-effective separations is still facing great ***,for the first time,a one-pot sequential copolymerization of γ-butyrolactone(γ-BL) and p-dioxanone(PDO)using an economical ureas/alkoxides catalytic system is conducted to synthesize biodegradable and chemically recyclable poly-(γ-butyrolactone)-block-poly(p-dioxanone)(PγBL-b-PPDO) diblock copolymers with well-defined and controlled *** composition-dependent properties of PγBL-b-PPDO copolymers,including thermal properties and crystallization behavior,are *** results show that the thermal stability and crystalline ability of PγBL are enhanced observably by introducing the PPDO ***,the PγBL-b-PPDO copolymers can be depolymerized efficiently into the corresponding co-monomers with a yield of over 95% by simply low-temperature pyrolysis under ***,γ-BL and PDO monomers are selectively separated with an isolated purity of about 99% based on the difference in their physicochemical ***,their repolymerization is realized to obtain the copolymers with nearly identical structures and thermostability,demonstrating the closed-loop recycling of copolymers,i.e.,*** research provides important guidance for the design of novel sustainable polymers towards more efficient chemical recycling,separation and regeneration.

关键词： biodegradable copolyester poly(p-dioxanone) tunable properties closed-loop chemical recycling

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