Polymer最新文献

{"title":"Drawing-Induced Structure and Conductivity Relationship in Polyimide-Based Graphite Fiber","authors":"Yan He, Zhaokun Ma, Zihan Chen, Ruiyang Li","doi":"10.1016/j.polymer.2026.130757","DOIUrl":"https://doi.org/10.1016/j.polymer.2026.130757","url":null,"abstract":"Owing to its designable molecular structure and simple carbonization, Polyimide (PI) is considered as a promising precursor for high thermal conductivity carbon materials. In this study, PI fibers with planar molecular chains were synthesized via a partial chemical imidization method. Subsequently, PI-based graphite fibers (PI-GFs) were prepared via multi-step thermal imidization, carbonization, and graphitization. Most importantly, different drawing levels of stress (ranging from 0 to the ultimate tensile stress) were applied separately during thermal imidization and carbonization, aiming to investigate their effects on the structure and conductive properties of the resulting PI-GFs. Drawing during thermal imidization functions through orientation induction and crystallite growth facilitation, creating an ordered precursor template that promotes the formation of larger graphite crystallites. Drawing during carbonization operates via suppressed disordering and oriented templating, guiding carbon network reorganization along the fiber axis.","PeriodicalId":405,"journal":{"name":"Polymer","volume":"49 1","pages":""},"PeriodicalIF":4.6,"publicationDate":"2026-09-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148884652","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Oxidized Hyaluronic Acid/Gelatin/Carboxymethyl Chitosan/Layered Double Hydroxide-Based Injectable Hydrogel for Localized Drug Delivery in Cartilage Degeneration","authors":"Vinh-Han Dac Le, Hai Sang Duong, Que-Phuong Le Huynh, Kim-Hang T. Le, Lan Le, Trung Duc Pham, Han Ngoc Cai, Thao Uyen Le, Cuong Hung Luu, Chau T.T. Ngo, Giang V.H. Phan","doi":"10.1016/j.polymer.2026.130752","DOIUrl":"https://doi.org/10.1016/j.polymer.2026.130752","url":null,"abstract":"Articular cartilage defects present a persistent clinical challenge owing to the tissue’s avascular nature and inherently limited regenerative capacity, and they frequently progress to osteoarthritis and irreversible joint dysfunction. Existing therapeutic strategies provide only temporary symptomatic relief and fail to restore native cartilage architecture. In this study, we developed an injectable dual-drug-loaded hydrogel as a proof-of-concept platform for localized therapeutic delivery and structural support for cartilage repair. The hydrogel was fabricated through Schiff-base crosslinking among oxidized hyaluronic acid (OHA), gelatin (GEL), and carboxymethyl chitosan (CMCs), with optimized final concentrations of 0.6%, 0.67%, and 3.2% (w/v), respectively. Layered double hydroxide nanoparticles (LDHs) were incorporated at concentration of 0.5 % to reinforce the hydrogel network and enable sustained release of salvianolic acid B (SalB) and dexamethasone (DEX). The degree of oxidation of OHA was determined to be 35%, and dynamic imine bond formation within the crosslinked network was confirmed by FT-IR spectroscopy. The resulting hydrogel exhibited an interconnected porous microstructure, favorable injectability, self-healing capability, and broad tissue adhesion. LDH incorporation significantly prolonged SalB release, from nearly 95% within 5 days in the LDH-free hydrogel to about 71% over 14 days in the LDH-containing formulation, and also moderated DEX release relative to LDH-free controls. Good biocompatibility of the nanocomposite hydrogel was demonstrated by MSC viability and chorioallantoic membrane assays, while short-term subcutaneous administration in mice confirmed <ce:italic>in vivo</ce:italic> injectability and local gel formation. Collectively, this OHA/GEL/CMCs/LDH (OGCL) hydrogel integrates <ce:italic>in situ</ce:italic> gelation, tunable physicochemical properties, and sustained dual-drug release, representing a promising minimally invasive platform for potential cartilage repair applications that warrants further biological validation.","PeriodicalId":405,"journal":{"name":"Polymer","volume":"177 1","pages":""},"PeriodicalIF":4.6,"publicationDate":"2026-08-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148884706","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"A Synthetically-Simplified Polymer Donor Based on Trifluorophenyl and Non-fluorinated Benzodithiophene Units for Low-Cost Organic Solar Cells","authors":"Wenzhuo Qi, Changbiao Ma, Hui Luo, Jianfeng Li, Qiaoqiao Zhao, Zicheng Ding, Shengzhong Frank Liu, Xiaochen Wang, Yongfang Li","doi":"10.1016/j.polymer.2026.130759","DOIUrl":"https://doi.org/10.1016/j.polymer.2026.130759","url":null,"abstract":"The development of low-cost, high-efficiency photovoltaic materials is crucial for the commercialization of organic solar cells (OSCs). However, conventional polymer donors often suffer from elaborate synthetic procedure, leading to high production cost. Herein, we report a low-cost polymer donor, PF06B, featuring a non-fluorinated benzodithiophene (BDT) donor unit and a trifluorophenyl acceptor unit, designed via a bidirectional simplification strategy. Utilizing inexpensive, commercially available 1,4-dibromo-2,3,5,6-tetrafluorobenzene ($3/g) as the precursor, the complete synthesis of PF06B is streamlined to eight steps, yielding a synthetic complexity index of 27.2 and an estimated production cost of 30-45 $/g, significantly lower than those of benchmark polymers PM6 and D18. In addition, PF06B exhibits complementary absorption spectrum and good energy-level alignment with non-fullerene acceptors, such as L8-BO and L8-Ph. The favorable interchain aggregation enables an optimal active layer morphology. The OSCs based on PF06B:L8-Ph achieves a power conversion efficiency 15.45%. This work provides a viable pathway toward low-cost and high-performance organic photovoltaics.","PeriodicalId":405,"journal":{"name":"Polymer","volume":"14 1","pages":""},"PeriodicalIF":4.6,"publicationDate":"2026-08-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148884704","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"One-Step Dual-Curing Encapsulant Based on Thermodynamic Matching via Photoinduced Thermal Activation: Synergistic Mechanism and Performance","authors":"Haibin Liu, Yan Li, YiYang Lou, Chenyang Shen, Mingming Yu, Ying Sun","doi":"10.1016/j.polymer.2026.130745","DOIUrl":"https://doi.org/10.1016/j.polymer.2026.130745","url":null,"abstract":"To overcome the deformation and cracking of photocurable encapsulants in large-scale optical device potting—originating from volumetric shrinkage and internal stress—this study develops a photoinduced thermally activated one-step dual-curing encapsulant composed of a modified IPDA/epoxy system (TCS) and an optimized acrylate photocurable system (UCS), based on thermodynamic matching between the exothermic enthalpy of acrylate free-radical photopolymerization and the activation energy of epoxy ring-opening. Theoretical calculations and experimental results show that the UCS photopolymerization exotherm (181.5 J/g) is energetically sufficient, when compared with the epoxy ring-opening activation energy expressed per unit mass (∼153 J/g), to provide the thermal impetus for initiating the thermal curing of TCS, establishing a thermodynamic foundation for achieving synergistic curing without a secondary thermal curing step. At UCS-to-TCS mass ratios ranging from 10:1 to 10:5, concurrent free-radical and ring-opening polymerizations induce in situ formation of a fibrous interpenetrating polymer network (IPN), with the thermal component conversion exceeding 90%. Relative to the single photocuring system, the optimal formulation (10:3) yields 41% and 13.2% increases in tensile and impact strengths, respectively, along with 35.7 °C and 29.2 °C elevations in initial and maximum thermal decomposition temperatures. At a ratio of 10:5, the IPN-mediated suppression of light scattering and stress concentration reduces volumetric shrinkage by 77% and decreases the yellowness index by 61.7%, achieving an integrated balance of rapid curing and dimensional stability. This work offers an efficient, secondary-heating-free alternative for optical encapsulation applications.","PeriodicalId":405,"journal":{"name":"Polymer","volume":"351 1","pages":""},"PeriodicalIF":4.6,"publicationDate":"2026-08-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148884707","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Reactive poly(styrene-co-maleic anhydride) microspheres for simultaneous toughening and strengthening of epoxy resin","authors":"Canzhang Wang, Liang Xu, Junfeng Qian, Qun Chen, Jing Zhang","doi":"10.1016/j.polymer.2026.130751","DOIUrl":"https://doi.org/10.1016/j.polymer.2026.130751","url":null,"abstract":"High-performance epoxy resins (EPs) are indispensable matrices for advanced load-bearing composites, such as wind turbine blades and automotive lightweight structures. Achieving concurrent improvements in the mechanical and thermal performance of EP remains challenging for conventional toughening approaches. In this study, divinylbenzene (DVB)-crosslinked poly(styrene-co-maleic anhydride) (SMA) microspheres were synthesized via self-stabilized precipitation polymerization (2SP) and subsequently incorporated into the EP matrix. The microspheres combine reactive surface anhydride groups with a rigid aromatic backbone. The anhydride groups can participate in the epoxy–anhydride curing reaction, thereby improving the interfacial compatibility between the microspheres and the EP matrix. Meanwhile, the rigid benzene rings restrict segmental mobility and increase the rigidity of the crosslinked network. Curing kinetic analysis revealed that the incorporation of SMA microspheres reduced the apparent activation energy of the SMA/EP system, suggesting that the curing reaction was facilitated. This reduction may be attributed to the participation of surface anhydride groups in the cross-linking reaction and hydroxyl-mediated autocatalytic effects. Mechanical evaluations showed that, at an SMA loading of 2 wt%, the tensile strength of the SMA/EP composite reached 72.0 MPa, corresponding to a 48.8% increase compared with neat EP. At a loading of 3 wt%, the impact strength reached a maximum value of 19.2 kJ/m<ce:sup loc=\"post\">2</ce:sup>, indicating a substantial improvement in toughness. In addition, dynamic mechanical analysis (DMA) indicated that SMA microspheres increased the crosslinking density, while differential scanning calorimetry (DSC) showed that the glass transition temperature (T<ce:inf loc=\"post\">g</ce:inf>) increased by approximately 9 °C compared with neat EP. These results highlight reactive SMA microspheres as promising modifiers for epoxy composites requiring balanced strength, toughness, and thermal performance.","PeriodicalId":405,"journal":{"name":"Polymer","volume":"25 1","pages":""},"PeriodicalIF":4.6,"publicationDate":"2026-08-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148884709","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Chain-growth Copolymerization of (R)-Glycidyl Butyrate and CO2 with Controlled Molecular Weight Enabled by a POSS-Supported Multiborane/Phosphazene/Alcohol System: Degradable Glycerol-Derived Polycarbonates","authors":"Bingxin Tang, Yunlong Chen, Huaan Wang, Xianhao Xin, Yue Chen, Wu Gao, Xinhui Kou, Xiaowu Wang","doi":"10.1016/j.polymer.2026.130753","DOIUrl":"https://doi.org/10.1016/j.polymer.2026.130753","url":null,"abstract":"The copolymerization of CO<ce:inf loc=\"post\">2</ce:inf> with functional epoxides offers an attractive and sustainable route to degradable polycarbonates, yet the chain-growth copolymerization of glycidyl ester derivatives with controlled molecular weights remains underdeveloped. Herein, we report a metal-free catalytic system composed of a nanoscopic polyhedral oligomeric silsesquioxanes derived multiborane (POSS-B8), 1-tert-butyl-2,2,4,4,4-pentakis(dimethylamino)-2λ<ce:sup loc=\"post\">5</ce:sup>,4λ<ce:sup loc=\"post\">5</ce:sup>-catenadi(phosphazene) (<ce:sup loc=\"post\"><ce:italic>t</ce:italic></ce:sup>BuP<ce:inf loc=\"post\">2</ce:inf>), and benzyl alcohol for the selective copolymerization of (<ce:italic>R</ce:italic>)-glycidyl butyrate (RGB) and CO<ce:inf loc=\"post\">2</ce:inf>. This ternary system enables chain-growth copolymerization process with controlled molecular weight under mild conditions, affording polycarbonates with high monomer conversion (99%), high polymer selectivity (99%), and high carbonate linkage content (90%) while suppressing cyclic carbonate formation at 10–25 °C. Systematic variation of temperature, CO<ce:inf loc=\"post\">2</ce:inf> pressure, catalyst loading, and initiator loading shows that the process remains efficient at reduced catalyst loading (0.05 mol%) and that molecular weight can be tuned by the amount of benzyl alcohol. Kinetic analysis reveals the copolymerization is quasi-first-order dependence on both RGB and catalyst concentration, quasi-zero-order dependence on CO<ce:inf loc=\"post\">2</ce:inf> pressure, and linear molecular weight growth with RGB conversion. The resulting protected polycarbonate undergoes <ce:italic>p</ce:italic>H-dependent hydrolytic degradation to glycerol, butyric acid, and cyclic carbonate products, demonstrating a sustainable route from CO<ce:inf loc=\"post\">2</ce:inf> and a functional glycidyl ester to degradable polycarbonates.","PeriodicalId":405,"journal":{"name":"Polymer","volume":"43 1","pages":""},"PeriodicalIF":4.6,"publicationDate":"2026-08-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148884705","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Efficient synthesis of highly optically pure l-lactide via cyclodepolymerization of poly(l-lactic acid)","authors":"Xiaodong Fang, Xiaodie Zhu, Sheng Wang, Xiaohong Li, Yingfeng Tu","doi":"10.1016/j.polymer.2026.130754","DOIUrl":"https://doi.org/10.1016/j.polymer.2026.130754","url":null,"abstract":"<ce:small-caps><ce:italic>l</ce:italic></ce:small-caps>-Lactide (<ce:italic>L</ce:italic>-LA) is an important intermediate for the industrial production of poly(<ce:small-caps><ce:italic>l</ce:italic></ce:small-caps>-lactic acid) (PLLA). However, it remains a challenge to afford <ce:italic>L</ce:italic>-LA in high yield, high efficiency, and high optical purity. Here, we report an efficient catalytic cyclodepolymerization (CDP) of PLLA under relatively mild temperatures (≤180 °C) and high vacuum to afford <ce:italic>L</ce:italic>-LA with high optical purity. Sixteen commercial metal and organic base catalysts are employed for CDP. For most metal catalysts, efficient PLLA CDP for <ce:italic>L</ce:italic>-LA with a high yield exceeding 90% can be achieved within 4 h. The crude <ce:italic>L</ce:italic>-LA is composed of &gt;95% <ce:italic>L</ce:italic>-LA, which displays a high optical purity with a high <ce:italic>ee</ce:italic>% value over 99% after recrystallization. Various influencing factors on CDP are carefully investigated. Our results reveal that increasing the depolymerization temperature, time and catalyst loading can significantly boost the yield of crude <ce:italic>L</ce:italic>-LA, but excessive temperature and high catalyst loading tend to deteriorate the purity of <ce:italic>L</ce:italic>-LA. Notably, the recycled catalyst can be reused repeatedly for CDP with no evident loss of catalytic efficiency and stereoselectivity. The CDP of PLLA for <ce:italic>L</ce:italic>-LA follows an intramolecular backbiting mechanism, which accompanies with the occurrence of intermolecular transesterification. Moreover, the obtained high-purity <ce:italic>L</ce:italic>-LA can be further used to fabricate PLLA with high molecular weight and good crystallinity.","PeriodicalId":405,"journal":{"name":"Polymer","volume":"41 1","pages":""},"PeriodicalIF":4.6,"publicationDate":"2026-08-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148884708","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"A Bio-Derived Hydrogel Electrolyte with a Hydrogen-Bond-Regulated Water Microenvironment for Coupled Electrode Stabilization in High-Temperature Zn||MnO2 Batteries","authors":"Kaiqi Jin, Xingyun Zhu, Yingbo Zhao, Zuoyi Xiao, Qingda An, Dan Li","doi":"10.1016/j.polymer.2026.130750","DOIUrl":"https://doi.org/10.1016/j.polymer.2026.130750","url":null,"abstract":"Zn||MnO<ce:inf loc=\"post\">2</ce:inf> batteries operated at elevated temperatures often undergo changes in the local water microenvironment of electrolytes, accompanied by intensified parasitic reactions and reduced stability of the Zn anode and MnO<ce:inf loc=\"post\">2</ce:inf> cathode. Herein, a bio-derived hydrogel electrolyte is prepared from locust bean gum and acrylamide through hydrogen-bond regulation. During polymerization, hydroxyl-rich locust bean gum interacts with the resulting polyacrylamide network through hydrogen bonding and chain entanglement, contributing to water retention and continuous pathways for hydrated Zn<ce:sup loc=\"post\">2+</ce:sup> transport. FTIR and Raman analyses reveal a redistribution of the hydrogen-bonding environment, indicating reorganization of polymer–water interactions within the LAG network. This regulated water microenvironment reduces thermally induced water loss while maintaining sufficient molecular mobility for hydrated Zn<ce:sup loc=\"post\">2+</ce:sup> transport. The LAG hydrogel electrolyte exhibits an apparent Zn<ce:sup loc=\"post\">2+</ce:sup> transference number of 0.73, an ion-transport activation energy of 7.4 kJ mol<ce:sup loc=\"post\">-1</ce:sup>, and improved mass retention at 60 °C. These characteristics are associated with moderated interfacial pH variation, reduced Zn corrosion and by-product accumulation, and lower Mn dissolution and cathode deterioration during cycling. At 60 °C, Zn||Ti cells deliver an average Coulombic efficiency of 98% over 130 cycles, Zn||Zn symmetric cells operate for more than 300 h, and Zn||MnO<ce:inf loc=\"post\">2</ce:inf> full cells retain 90.1% of their initial capacity after 1000 cycles at 2 A g<ce:sup loc=\"post\">-1</ce:sup>. This work presents a hydrogen-bond-regulation approach for coupled electrode stabilization in Zn||MnO<ce:inf loc=\"post\">2</ce:inf> batteries under elevated-temperature conditions.","PeriodicalId":405,"journal":{"name":"Polymer","volume":"2 1","pages":""},"PeriodicalIF":4.6,"publicationDate":"2026-08-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148884710","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Recyclable coumarin-based dynamic covalent porous hydrogels using high internal phase emulsion templating","authors":"D.G.N. Vindya Dikella, Neil Ayres","doi":"10.1016/j.polymer.2026.130747","DOIUrl":"https://doi.org/10.1016/j.polymer.2026.130747","url":null,"abstract":"Traditional cross-linked polymers are not recyclable due to their permanent covalent crosslinks, which contribute to environmental problems. Porous polymeric networks made using polymerized high internal phase emulsion (polyHIPE) templating offer control over porosity, porous structure, and material properties; however, there are very few studies on creating recyclable polyHIPEs. Coumarin is a fast, effective, and reversible photoresponsive functional group that can undergo dimerization via cycloaddition and subsequent photocleavage under different wavelengths of UV light. Here, for the first time, recyclable, highly porous hydrogels have been synthesized using polyHIPE templating by incorporating photoresponsive coumarin groups. Water-soluble linear copolymers were prepared using free-radical polymerization of coumarin-acrylate monomers with <ce:italic>N</ce:italic>,<ce:italic>N</ce:italic>-dimethylacrylamide and subsequently crosslinked with 365 nm UV light in an oil-in-water HIPE template to produce polyHIPE hydrogels. Coumarin-based polyHIPE hydrogels (CPHH) derived from templates with a dispersed phase content of over 75% exhibited an interconnected, open-cell pore morphology. The swelling ratio and mechanical properties of the CPHHs could be tuned by varying the dispersed phase content in the template or the coumarin content in the copolymers. Importantly, these polyHIPE hydrogels were able to recycle back to copolymer using 254 nm UV light and reused to prepare new nonporous and porous hydrogels. Recycled polyHIPE hydrogels exhibited interconnected pore morphology, and their mechanical properties were retained after recycling.","PeriodicalId":405,"journal":{"name":"Polymer","volume":"43 1","pages":""},"PeriodicalIF":4.6,"publicationDate":"2026-08-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148884712","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Thermomechanical properties and self-healing behavior of vitrimers with dual dynamic disulfide and ester networks: Insights from molecular dynamics simulations","authors":"Bin Xu, Wei Jian, Lu Ren, Shu Mao, Feiping Tang, Lusheng Li, Wei Hu","doi":"10.1016/j.polymer.2026.130749","DOIUrl":"https://doi.org/10.1016/j.polymer.2026.130749","url":null,"abstract":"Vitrimers, a novel class of dynamic covalent polymers that undergo topological network rearrangement, exhibit mechanical properties and self-healing behaviors that are closely related to their network structure. However, for vitrimer systems containing dual-dynamic bonds, it remains unclear how the relative content of dynamic bonds affects mechanical properties as well as self-healing efficiency at the microscopic level, and whether a synergistic effect exists between different bond types. In this study, all-atom molecular dynamics simulations were employed to construct crosslinked network models containing dynamic disulfide and ester bonds. A bond exchange algorithm based on a cutoff-distance criterion was implemented to simulate uniaxial tensile deformation, stress relaxation, and self-healing processes. The simulation results show that the ratio of crosslinker significantly influences the thermomechanical behavior. Changing the crosslinker ratio simultaneously alters network connectivity, crosslinking state, residual molecular chains, and the availability of dynamic exchange sites, resulting in coupled effects on thermomechanical behavior and stress relaxation. An optimal crosslinker ratio enables the network to maintain structural integrity while providing a sufficient density of dynamic bonds, thereby optimizing the overall mechanical performance. Furthermore, the introduction of ester bonds into the disulfide-containing system significantly improves self-healing efficiency, revealing a clear synergistic effect between the two types of dynamic bonds. This study aims to investigate the thermomechanical properties and self-healing performance of vitrimers with different crosslinker ratios through molecular dynamics simulations, providing a theoretical basis for experimental optimization of vitrimer formulations and the development of highly efficient self-healing materials.","PeriodicalId":405,"journal":{"name":"Polymer","volume":"17 1","pages":""},"PeriodicalIF":4.6,"publicationDate":"2026-08-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148884711","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}