INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
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2022
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IF 8.025
Chang Li,Benzhi Ju,Shufen Zhang
Cellulose-based vitrimers were prepared using a crosslinkable macromolecular plasticizer and acetylated carboxymethyl cellulose via twin-screw extrusion. The cellulose-based material was toughened by the entanglement between the macromolecular plasticizer segments, and the exudation of the plasticizer was avoided by crosslinking. The prepared materials exhibited excellent hydrophobicity and shape memory properties. The plasticizer was evidently effective, and the reprocessing was completed at 130 °C within 15 min. The materials could be reprocessed at a lower temperature over a short period of time without any obvious degradation. After reprocessing three times, the material performance did not decrease significantly, thus showing good potential for regeneration and recycling.
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PubMed
高影响因子
CELLULOSE
·
2021
·Vol. 28
·期 5
·2879-2888
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IF 5.044
Li Chang,Ju Benzhi,Zhang Shufen
The synthesis of the first cellulose-based vitrimer is described. Dynamic ester bonds were responsible for the dynamic properties of carboxymethyl cellulose (CMC)-based vitrimer. The addition of suitable catalyst and glycerol in the vitrimer formulations was crucial for the reprocessability of these materials. Thermogravimetric and dynamic mechanical analyses tensile strength tests were performed to investigate the effect of the catalyst and glycerol on the thermal stability and mechanical properties of the materials. A minimum amount of 5 mol% of 1,5,7-triazabicyclo[4.4.0]dec-5-ene with respect to the carboxyl group content was required to maintain reprocessability by hot press. The CMC vitrimer exhibited good reprocessability and shape memory ability. Our work demonstrates that cellulose, the most abundant bio-resource on the planet, can be a promising raw material for bio-based vitrimer due to its excellent renewability and low cost. Graphic abstract
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高影响因子
POLYMER
·
2020
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IF 4.231
Shuaipeng Wang,Na Teng,Jinyue Dai,Jingkai Liu,Lijun Cao,Weiwei Zhao,Xiaoqing Liu
Fabrication of mechanically robust and catalyst-free vitrimers is of great importance, but often challenging. Herein, a facile strategy to achieve this goal by incorporation of intramolecular hydrogen bonds into the dynamic covalent network is demonstrated. Specifically, glycidyl methacrylate (GMA) is reacted with bio-renewable malic acid (MA) to generate a UV-curable resin containing ester linkages. On account of the proximity between the α -carbonyl and β -hydroxyl groups in MA, six-membered-ring intramolecular hydrogen bonds ( O-H⋯O=C ) are formed in the cross-linked network. This formation of intramolecular hydrogen bonds endows the network with enhanced and outstanding mechanical properties , showing tensile strength and Young's modulus of 117.7 MPa and 3.66 GPa, respectively. Meanwhile, the network is able to efficiently alter its topology without external catalyst through transesterifications reactions at high temperatures. We attributed this phenomenon to the presence of intramolecular hydrogen bonds which make the α -carbonyl carbon more positive and be more reactive towards nucleophilic attack, and thus facilitate the transesterification reaction. This work suggests a promising route to achieve catalyst-free thermosets with superior mechanical performances, good self-healing ability and reprocessability.
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JOURNAL OF POLYMERS AND THE ENVIRONMENT
·
2023
·
IF 5.3
Zhang Yongjie,Lin Zichun,Li Xiaopei,Li Guangdong
Vitrimer uniquely simultaneously combines the opposed thermoset-like properties (mechanical properties, durability, creep/solvent resistance) and thermoplastic-like properties (reshapability, recyclability), thus arousing great enthusiasms in the design, preparation and characterization of vitrimer. From a practical point of view, it is of great value to develop one-step and scalable synthetic procedures for high performance vitrimers. Starting from two highly available and non-expensive commodity materials, namely, ethylene acrylic acid copolymer (EAA) and triglycidyl isocyanurate (TGIC), a series of EAA-TGIC vitrimer materials with varying cross-linking degrees were prepared via a one-step, scalable and practical synthetic approach. Under mild melt compounding conditions, ring-opening of epoxy groups towards carboxyl groups in EAA occurred, resulting in cross-linking of EAA by dynamic β-hydroxyl ester covalent bonds. The formation of covalent cross-linking network in EAA-based vitrimer materials was proved by FTIR and swelling test. The thermo-mechanical, tensile, reprocessing and thermal properties of EAA-TGIC vitrimer were systematically studied. The results showed that EAA-TGIC vitrimer with high gel contents, and thus, excellent solvent resistances, were achieved. Tensile tests revealed that EAA-TGIC vitrimers exhibited premium mechanical properties with well-balanced rigidity and toughness and that the mechanical properties of recovered EAA-TGIC vitrimer remained almost unchanged compared to those of as-prepared EAA-TGIC vitrimer. This study offers a long sought-after solution for the cost-effective recycling of cross-linked polyethylenes and provides new possibilities for keeping difficult-to-recycle cross-linked polyethylenes in the circular loop.
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高影响因子
PROGRESS IN ORGANIC COATINGS
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2023
·
IF 6.6
Chang Cong,Jixiao Wang,Zhan Wang,Guangyu Xing,Zhi Wang
Epoxy vitrimers with thermal-healing ability are widely studied to prolong the service life of materials. But the conventional preparation and healing strategy, involving external catalysts, preheating, hot press or/and heating the entire coating, are not applicable for the large-scale applications. In this work, a room-temperature brushable oxidized carbon black (OCB)/epoxy vitrimer composite based on dynamic transesterification reaction with excellent protective performance and localized photothermal-healing was prepared by solvent method. No external catalysts, preheating and hot press was needed in the preparation process. The experimental results demonstrate that the composite coatings exhibited an excellent metal protective performance. The effective non-contact local photothermal-healing can be achieved in 20 Min., and the scratch width can apparently narrow over 95 % and the impedance moduli of the composite coatings can be recovered from 263 Ω·cm 2 to above 10 8 Ω·cm 2 . The OCB/epoxy vitrimer composite coating, combining ideal metal protective performance with non-contact local photothermal-healing performance, has great promise for many practical applications in large-scale, such as metal protection and solar-energy collector.
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ACS Applied Materials & Interfaces
·
2019
·
IF 8.456
Wei Zhao,Zihao Feng,Zhenhua Liang,Yanfeng Lv,Fukang Xiang,Chuanyin Xiong,Chao Duan,Lei Dai,Yonghao Ni
Vitrimer, the third category of polymer materials, combines the properties of traditional thermosets and thermoplastics and has gained much interest from industry since the first report in 2011. Currently, many researchers focus on the exploration of new chemistry for novel vitrimer synthesis but pay less attention to the fabrication of vitrimer composites based on known vitrimer systems. The latter can not only largely decrease the cost of vitrimers but also provide a facile way to increase the variety of vitrimer-based materials and extend the applications of vitrimers in different fields. In this study, we developed a new class of vitrimer composite using polycarbonate as a matrix and natural cellulose paper as the reinforcing framework for the first time. The resultant materials possess exceptional mechanical properties and great thermal/chemical stability, simultaneously exhibiting a series of smart properties, such as shape-memory, reshaping, self-healing, and reprocessing. Noteworthily, the two main components of the resultant materials, polycarbonate and natural cellulose, can be easily recycled under mild conditions; thus, these new vitrimer composites qualify as novel green and sustainable materials.
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高影响因子
POLYMER DEGRADATION AND STABILITY
·
2025
·
IF 7.4
Xingyu Liu,Xuanyue Hong,Yi Wang,Jun Lin,Jujun Ruan,Shaojian He
Currently, the primary limitation hindering the sustainable application of epoxy (EP) vitrimers lies in the inherent trade-off among high mechanical performance, efficient recovery capability and mild recycling conditions. To address this challenge, we designed an EP polymer that leverages the high rigidity of imine bonds and the rapid bond exchange of boronic ester linkages, simultaneously achieving high mechanical performance, efficient recovery capability, and mild-condition recyclability. The resulting material exhibits a high mechanical strength of 78.6 MPa, excellent recovery efficiency (>90% after two cycles of crushing and then hot-pressing at 130°C), and mild solvent-assisted closed-loop recycling. Furthermore, carbon fiber-reinforced polymers (CFRPs) fabricated with this EP vitrimer demonstrated complete degradation in (solvent) within 30 min at 50°C. The reclaimed carbon fibers (CF) retained pristine surface morphology and preserved 96% of their original mechanical properties, enabling highly efficient and non-destructive recovery. These findings highlight the potential of this EP vitrimer system, offering a promising strategy for the sustainable development of polymer materials.
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高影响因子
INDUSTRIAL CROPS AND PRODUCTS
·
2025
·
IF 6.2
Yanna Zhao,Yingying Zhang,Xiaowei Bai,Yuqi Wang,Yiqing Li,Shuai Yang
Vitrimer has become an emerging application to solve the problem of thermoset pollution and resource wastage due to its reversible cross-linked network structure that enables reuse and recycling of materials. However, it is still challenging and difficult to achieve full bioresourcing and to prepare recycling pathways with excellent mechanical strength and high efficiency. In this study, a bisphenol derivative monomer with imine bonds was first synthesized with tyramine (TA) and terephthalaldehyde (TPA), and then the monomer was used together with 4,4′-diaminodiphenyl disulfide (4-AFD) to co-cure epoxidized soybean oil (ESO) to construct an epoxy vitrimer material (ETA) with a bi-dynamic network structure. ETA-3 exhibits high 5 % thermal stability T d 5 % (319.17 °C) and energy storage modulus E (2085.35 MPa). Notably, due to the fact that it exhibits a short relaxation time (32.24 s) and low activation energy (70.07 KJ/mol), ETA can achieve the repair of scratches within 30 min at 100 °C. This test demonstrates that ETA vitrimer has a better self-repairing performance, which contributes to the continuous development of vegetable oil-based polymeric materials.
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COMPOSITES SCIENCE AND TECHNOLOGY
·
2024
·
IF 8.3
Mei Fang,Xiang Liu,Yuezhan Feng,Ming Huang,Chuntai Liu,Changyu Shen
The emergence of vitrimers breaks through the limitation of traditional carbon fiber reinforced thermoset composites (CFRP) caused by their permanent crosslinking molecular networks. Herein, the dynamic cross-linked network of vitrimer was synthesized from Bisphenol A diglycidyl ether (DGEBA) and glutaric anhydride (GA) under the catalysis of zinc acetylacetonate (Zn(acac) 2 ), and the corresponding carbon fiber reinforced vitrimer composites (CF/V x ) were prepared via an impregnation and hot pressing process. The dynamic covalent adaptable networks (CANs) of vitrimer endow CF/V x with stress relaxation and creep characteristics. By adjusting the catalyst content, the dynamic performance of CF/V 0.05 can be optimized to achieve the highest viscous flow activation energy (60 kJ/mol) and the lowest characteristic relaxation time (1.0 × 10 −3 s). The unique dynamic properties enable CF/V x with reprocessability at high temperature. Typically, the flexural modulus of CF/V 0.05 decreased from 87 ± 1.81 GPa at room temperature to 4.62 ± 0.28 GPa at 220 °C, which confirms the feasibility of thermoplastic forming of CF/V 0.05 at high temperatures. Based on this, a CF/V 0.05 -based cap-shaped component was successfully manufactured through a thermoforming process . Additionally, the CF/V 0.05 composites also exhibit repairability for interlaminar fractures. The optimal CF/V 0.05 can achieve a repair efficiency of 128 % under the hot press conditions of 180 °C, 10 MPa and 1 h. Hence, the reprocessable and repairable CF/V x composites hold enormous potential in the engineering field.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2026
·
IF 8.7
Yuyan Xiao,Ningning Zhang,Aoqian Xi,Li Zhou,Yanning Zeng
Developing high-performance, closed-loop recyclable, and bio-based adhesives remains a significant challenge due to the inherent trade-off between crosslinking density and reprocessability. Herein, we report a bio-based vitrimer adhesive derived from peach gum polysaccharide (PGP) via vinylogous urethane (VU) chemistry. PGP was first modified with tert-butyl acetoacetate, followed by crosslinking with a fatty acid-derived diamine to form dynamic VU networks (PUV-x). The resulting PUV-1.0 network exhibits excellent mechanical properties (tensile strength up to 28.5 MPa, Young's modulus of 427.0 MPa, and elongation at break of 67.0%) and high thermal stability ( T s = 174.5 °C). Benefiting from the associative exchange of VU bonds, the material demonstrates rapid stress relaxation (activation energy of 30.4 KJ·mol −1 ), efficient self-healing (16 min at 100 °C) of surface scratches, and weldability. Moreover, the PUV-1.0 adhesive exhibits strong adhesion to various substrates (wood, steel, and glass), achieving an adhesion strength of up to 18.9 MPa on wood. It also maintains stable bonding performance under extreme temperatures (−22 to 100 °C) and in harsh environments (water, acid, alkali, sweater, and ethanol). The network can be chemically degraded and closed-loop recycled via transamination reactions, and the adhesive can be removed on demand from different substrates. This work provides a high-performance, and recyclable vitrimer adhesive platform, highlighting the potential of PGP in advanced bio-based materials.
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JOURNAL OF APPLIED POLYMER SCIENCE
·
2025
·
IF 2.8
Mingsheng Li,Jiazhu Xu,Shizhe Peng,Shouyang Hu,Shiyang Yi,Yiming Xu,Jingwen Li,Yonghong Cheng,Lei Zhang
An efficient method for introducing dynamic imine bonds into epoxy resins has been developed, resulting in a dynamic network that does not require specialized curing agents. The vanillin-based dynamic epoxy resin demonstrates excellent thermal, mechanical, and electrical properties. Additionally, a dynamic epoxy resin based on 4-hydroxyterephthalaldehyde has been designed, further enhancing these properties through increased imine bond content, which elevates the glass transition temperature ( T g ), dynamic characteristics, and mechanical strength, while preserving insulating capabilities. Both the vanillin-based and high imine-content dynamic epoxy resins exhibit successful mechanical and chemical recyclability. Overall, the dynamic epoxy resins, with their combination of high performance and recyclability, are promising candidates for environmentally sustainable applications and lay a foundation for the development of fully recyclable composite materials.
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高影响因子
INDUSTRIAL CROPS AND PRODUCTS
·
2025
·
IF 6.2
Zhiping Su,Mingrui Pan,Shizhen Qin,Zuli Zheng,Haiyan Xu,Shaobo Zhang,Liping Ning,Shanshan Jia
Traditional wood-plastic composites (WPCs) usually employed fossil-based non-degradable plastics as the polymer matrix, making WPCs poor in sustainability and degradability. Herein, a new kind of sustainable and degradable WPCs, wood-vitrimer composites (WVCs, i.e., WPs/Cel-DIP composite), was developed by integrating wood powders (WPs) into a cellulose-based dynamic imine polymer (Cel-DIP) matrix via heat-pressing formation technique. The resulting WVCs exhibited ultrahigh tensile strength (56.1 MPa), flexural strength (94.9 MPa), Young's modulus (2.5 GPa), and flexural modulus (10.3 GPa). The WVCs possessed extremely high thermostability with the glass-transition temperature ( T g ) of 230–250 °C and thermal degradation temperature ( T d ) of ˃ 300 °C. The WVCs also exhibited low water absorption ratio (as low as 2 wt%) and excellent water resistance. Moreover, such WVCs could be chemically degraded by depolymerized the dynamic imine crosslinking networks of Cel-DIP via acid-catalyzed hydrolysis. Such WVCs represent a kind of novel, sustainable, and environmentally friendly biomass-based composites.
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