BIOMACROMOLECULES
·
2017
·
IF 5.246
Xin Zhang,Jiayun Xu,Chao Lang,Shanpeng Qiao,Guo An,Xiaotong Fan,Linlu Zhao,Chunxi Hou,Junqiu Liu
Self-healing, one of the exciting properties of materials, is frequently used to repair the damage of biological and artificial systems. Here we have used enzymatic catalysis approaches to develop a fast self-healing hydrogel, which has been constructed by dynamic aldimine cross-linking of pillar[5]arene-derivant and dialdehyde-functionalized PEG followed by encapsulation of glucose oxidase (GOx) and catalase (CAT). In specific, the two hydroxyl groups at terminal of PEG4000 are functionalized with benzaldehydes that can interact with amino-containing pillar[5]arene-derivant through dynamic aldimine cross-links, resulting in reversible dynamic hydrogels. Modulus analysis indicated that storage modulus (G′) and loss modulus (G″) of the hydrogel increased obviously as the concentration of dialdehyde-functionalized PEG4000 (DF-PEG4000) increased or the pH values decreased. Once glucose oxidase (GOx) and catalase (CAT) are located, the hydrogel could be fast repaired, with self-healing efficiency up to 100%. Notably tensile test showed that the repair process of pillararene-based hydrogel can finish in several minutes upon enzyme catalysis, while it needed more than 24 h to achieve this recovery without enzymes. This enzyme-regulated self-healing hydrogel would hold promise for delivering drugs and for soft tissue regeneration in the future.
研究领域:
材料科学
·
生物医学工程
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产品关联
DOI
PubMed
高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2015
·
IF 2.752
Jiao Wang,Xiao Chen,Wanling Cui,Sijing Yi
pH-responsive vesicles have been prepared from the mixture of 1-(10-(4-formyl-phenoxy) decyl)-pyridinium (FDP) or 1-methyl-3-(10-(4-formyl-phenoxy) decyl) imidazolium (FDI) with 1-octyl amine at a molar ratio of 1:1 in alkaline aqueous solutions. Their structures and morphologies were characterized by transmission electron microscopy with sample preparations by negative staining or freeze-fracture. Basically, the spherical unilamellar vesicles were formed with the mean diameters respectively of about 71 and 107 nm for two supra-amphiphile systems, which were based on the formation of dynamic imine bonds between amine and FDP (i-FDP) or FDI (i-FDI). The loading and release studies of a fluorophore, Nile red (NR), demonstrated the capabilities of these vesicles to encapsulate NR and a rapid release at low pH environment. The vesicles from i-FDP behaved relatively more sensitive to acidic environment than those from i-FDI. The dynamic transitions of supra-amphiphiles were characterized by nuclear magnetic resonance or fluorescence emission spectroscopy measurements. A lower critical micelle concentration and a higher aldehyde conversion efficiency of i-FDI than those of i-FDP were observed. The characteristics of facile formation, fast dissociation, and switchable morphologies of studied systems should be referable for designing novel smart supra-amphiphile systems with potential applications as controlled drug delivery systems.
研究领域:
生物化学
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材料科学
·
药物递送
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产品关联
DOI
高影响因子
ACS Applied Polymer Materials
·
2025
·
IF 4.7
Yanhan Tao,Hui Yang,Zhijun Liu,Guoming Yuan,Kunxin Wang,Kun Wu,Jun Shi
One kind of liquid crystal monomer (LM) based on a biphenyl mesomorphic unit was synthesized from 4,4′-biphenyldicarboxaldehyde and 4-amino-3-methylphenol. Then two films (LM/TPTMP and LM/PETMP) were prepared by reacting the two thiols (TPTMP and PETMP) with the liquid crystal monomer (LM), respectively. These two films simultaneously exhibit intrinsically high thermal conductivity and intrinsic self-healing properties. Due to the presence of biphenyl liquid crystal units in LM and its highly symmetrical structure, a distinct nematic liquid crystal phase can be observed through a polarized optical microscope when heated to the liquid crystal phase transition temperature. The crystallite size of LM was calculated as 37 nm by an X-ray diffractometer (XRD). The films exhibit outstanding thermal conductivity, with LM/TPTMP achieving a thermal conductivity in the horizontal direction (λ∥) of 0.700 W/(m·K), which is significantly higher than that of epoxy resin-based intrinsic thermal conductivity materials in the range of 0.2–0.4 W/(m·K). The introduction of thiol flexible segments endowed the materials with good mechanical strength, with LM/PETMP demonstrating a tensile strength of 4.74 MPa and an elongation at break of 42.57%. Furthermore, the incorporation of dynamic imine bonds imparted excellent self-healing properties to the films. Specifically, LM/PETMP could retain 73% and 65.2% of its original tensile strength after one and three cycles of self-healing behavior, respectively. This type of high intrinsic thermal conductivity (λ) and excellent intrinsic self-healing performance film is expected to solve the problems of safety and service life of high-precision smart devices.
研究领域:
材料科学
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高分子化学
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产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2020
·
IF 8.758
Zhen Shi,Jing Kang,Ling Zhang
The synthesis of polymeric materials that simultaneously possess multiple excellent mechanical properties and high-efficient self-healability at room temperature is always a huge challenge. Here, we report the synthesis of a transparent polyurea material that can self-heal at room temperature with the aid of water and, meanwhile, has multiple remarkable mechanical performances, including super-high strength, excellent toughness, and large stretchability. Thanks to the synergistic enhancement of both dynamic imine bonds and hierarchical hydrogen bonds within the networks, the resulting polyureas have a world-record tensile strength of 41.2 MPa when compared with other polyurethanes that can self-heal at room temperature and, at the same time, a large breaking strain of 823.0% and a superior toughness of 127.2 MJ/m3. Besides the influence of imine bonds, the mechanical properties of the polyureas are also strongly related to the density and strength of the hierarchical hydrogen bonds within the polyurea networks, and these two factors could be finely controlled by adjusting the mass ratio of the soft segments with different chain lengths and the types of diisocyanates used for polyurea synthesis, respectively. More importantly, the highly dynamic characteristic of both imine bonds and hierarchical hydrogen bonds within the polyureas endows the materials with repeated water-enabled room-temperature self-healing capacity with a high healing efficiency of 92.2%. Moreover, the polyureas can also be recycled or remolded under mild conditions by the hot-pressing or dissolution/casting process. The synthesized polyureas also show great potential in damping applications with a loss factor larger than 0.3 over the temperature range from 12 to 75 °C. It is believed that polyureas with super-high and well-tunable mechanical properties and high-efficient room-temperature self-healing ability have great potential to substitute traditional irreparable polymers in diverse practical applications.
研究领域:
材料科学
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化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
EUROPEAN POLYMER JOURNAL
·
2025
·
IF 6.3
Long-Yang Zhan,Ping Li,Yi-Dong Li,Yin Ran,Jian-Bing Zeng
Biobased epoxy vitrimers (BEVs) offer a promising solution to the recyclability and resource challenges associated with traditional epoxy thermosets. However, numerous existing BEVs suffer from inadequate properties or complex fabrication processes. Herein, we present a fully biobased, high-performance epoxy vitrimer synthesized from renewable and commercially available feedstocks: resorcinol diglyceryl ether (DGER), vanillin (VAN), and 1,10-diaminodecane (DDA). A dynamic imine crosslinker (DIC) was synthesized from VAN and DDA, which then underwent solvent-free and catalyst-free melt curing with DGER to form the BEV. Detailed studies of the curing kinetics of DGER-DIC and the properties of the resulting BEV were conducted, with comparisons to a control fossil-based epoxy vitrimer made from bisphenol A diglycidyl ether (DGEBA) and DIC. The DGER-DIC system showed a curing activation energy of 62.43 ± 3.73 kJ·mol –1 , slightly lower than DGEBA-DIC’s 67.71 ± 2.38 kJ·mol –1 . The BEV exhibited excellent mechanical properties, featuring a tensile strength amounting to 69.23 MPa and a Young’s modulus at 1.91 GPa, along with high thermal stability. The imine bonds provided fast stress relaxation, self-healing performance, and excellent reprocessability, with tensile strength recovering over 90 % after multiple processing cycles. These properties rival those of the DGEBA derived epoxy vitrimers, highlighting the potential of DGER as a sustainable alternative for creating recyclable epoxy thermosets.
研究领域:
材料科学
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可持续化学
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产品关联
DOI
高影响因子
Polymers
·
2025
·Vol. 17
·期 5
·571
·
IF 4.9
Lei Chen,Na Ning,Gang Zhou,Yan Li,Shicheng Feng,Zhengyan Guo,Yi Wei
Conventional epoxy thermosets, with irreversible crosslinking networks, cannot be reprocessed and recycled. Furthermore, the utilization of petroleum-based materials accelerates the depletion of non-renewable resources. The introduction of dynamic covalent bonds and the use of bio-based materials for thermosets can effectively address the above issues. Herein, a series of bio-based epoxy vitrimers with dynamic covalent imine bonds were synthesized via a simple solvent-free, one-pot method using vanillin-derived aldehyde monomers, 4,4-diaminodiphenylsulfone (DDS) and bisphenol F diglycidyl ether (BFDGE) as raw materials. The effect of crosslinking density, crosslinking structure and imine bond content on the resulting bio-based vitrimers was studied, demonstrating their excellent thermal properties, UV shielding and solvent resistance, as well as outstanding mechanical properties compared to those of the previously reported vitrimers. In particular, the cured neat resin of vitrimer had a maximum tensile strength of 109 MPa and Young’s modulus of 6257 MPa, which are higher than those of previously reported imine-based vitrimers. The dynamic imine bonds endow these vitrimers with good reprocessability upon heating (over 70% recovery) and degradation under acidic conditions, enabling recycling by physical routes and gentle degradation by chemical routes. This study demonstrates a simple and effective process to prepare high-performance bio-based and recycled epoxy thermosets.
研究领域:
材料科学
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化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Polymers
·
2024
·Vol. 16
·期 9
·1262
·
IF 4.7
Peng Wang,Zhuochao Wang,Wenxin Cao,Jiaqi Zhu
Transparent polysiloxane elastomers with good self-healing and reprocessing abilities have attracted significant attention in the field of artificial skin and flexible displays. Herein, we propose a simple one-pot method to fabricate a room temperature self-healable polysiloxane elastomer (HPDMS) by introducing dynamic and reversible imine bonds and boroxine into polydimethylsiloxane (PDMS) networks. The presence of imine bonds and boroxine is proved by FT−IR and NMR spectra. The obtained HPDMS elastomer is highly transparent with a transmittance of up to 80%. The TGA results demonstrated that the HPDMS elastomer has good heat resistance and can be used in a wide temperature range. A lower glass transition temperature (Tg, −127.4 °C) was obtained and revealed that the elastomer is highly flexible at room temperature. Because of the reformation of dynamic reversible imine bonds and boroxine, the HPDMS elastomers exhibited excellent autonomous self-healing properties. After healing for 3 h, the self-healing efficiency of HPDMS reached 96.3% at room temperature. Moreover, the elastomers can be repeatedly reprocessed multiple times under milder conditions. This work provides a simple but effective method to prepare transparent self-healable and reprocessable polysiloxane elastomers.
研究领域:
材料科学
·
高分子化学
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF MATERIALS SCIENCE
·
2021
·Vol. 56
·期 28
·15733-15751
·
IF 4.22
Liu Xiaohong,Zhang Ending,Feng Zhiqiang,Liu Jiaming,Chen Bifang,Liang Liyan
Traditional epoxy resin materials are widely used in coatings, composite materials, electronic packaging materials, etc. They are usually made of unsustainable fossil resources and cannot be recycled under mild conditions. Degradable thermosetting resins with dynamic covalent structure provide a potential solution to this conflict. In this paper, using biomass energy vanillin, m-xylylenediamine and 1, 6-hexanediamine as raw materials, two dynamic imine bond curing agents were synthesized, and then cured with DGEBA to prepare two bio-based imine epoxy vitrimers. The thermal and mechanical properties of two imine epoxy vitrimers were studied and compared in detail. Results showed that the two types of polymers exhibit excellent thermal stability and solvent resistance. At the same time, the tensile strength, modulus and elongation at break were comparable to or even better than those of conventional bisphenol A epoxy resin. In addition, due to the hydrolysis of the dynamic imine bonds, vitrimers had degradable characteristic, and its degradation also exhibited temperature, solvent and acidity dependence. More importantly, the recyclable carbon fiber reinforced polymer composites made of these two vitrimers could be completely degraded under weak acid conditions, and the nondestructive recycling of carbon fiber composites could be realized. We envision that this vitrimers with simple process, excellent comprehensive properties and degradability will make it a potential candidate for applications in sustainable structural materials.
研究领域:
材料科学
·
化学工程
✓ 已验证
DOI
高影响因子
ChemSusChem
·
2024
·Vol. 17
·期 14
·e202301708
·
IF 7.5
Sujuan Zhang,Jianjun Yi,Jiming Chen,Yong Li,Baoliang Liu,Zaijun Lu
Graphical In this study, imine-containing polybenzoxazine vitrimer (C-ABZ) was synthesized through a condensation reaction between an aldehyde-containing benzoxazine oligomer (O-ABZ) and 1,12-dodecanediamine. The dynamic exchangeable characteristics of imine bonds impart C-ABZ with weldabilities and reprocessabilities. At the same time, the hydrophobic polybenzoxazine backbone significantly improve the water resistance of imine bonds. Traditional polybenzoxazine thermosets cannot be reprocessed or recycled due to the permanent crosslinked networks. The dynamic exchangeable characteristics of imine bonds can impart the networks with reprocessabilities and recyclabilities. This study reported a weldable, reprocessable, and water-resistant polybenzoxazine vitrimer (C-ABZ) crosslinked by dynamic imine bonds. It was synthesized through a condensation reaction between an aldehyde-containing benzoxazine oligomer (O-ABZ) and 1,12-dodecanediamine. The resulting C-ABZ was able to be welded and reprocessed due to the dynamic exchange of imine bonds. The tensile strengths of the welded C-ABZ and the reprocessed C-ABZ after three cycles of hot-pressing were 76.7, 81.3, 70.8, and 58.1 Mpa, with corresponding tensile strength recovery ratios of 74.1 %, 78.6 %, 68.4 %, and 56.1 %, respectively. Furthermore, the polybenzoxazine backbone significantly improved the water resistance of the imine bonds. After immersing in water for 30 days at room temperature, the weight gain of C-ABZ was less than 1 % with corresponding tensile strength and tensile strength retention ratio of 59.5 Mpa and 57.5 %, respectively. Although the heat resistance of C-ABZ decreased slightly with increased hot-pressing cycles, a glass transition temperature ( T g, tanδ ) of 150 °C was retained after the third hot-pressing. Overall, these findings demonstrate that the C-ABZ possesses excellent comprehensive performances.
研究领域:
材料科学
·
化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Applied Polymer Materials
·
2023
·
IF 5
Bing Chen,Geng Lai,Zhangyou Liu,Wenhui Luo,Shufeng Lin,Huagui Zhang,Mingfeng Chen
The development of multifunctional epoxy resins that can be degradable and reprocessed is of great significance for the conservation of non-renewable resources and environmental protection. Herein, curing agents based on nitrogen–silicone Schiff base (BOB) and silica-bridged epoxy resin (ETOD) were designed and successfully synthesized. Then, ETOD was cured using BOB to fabricate a multi-silicon-bridge epoxy vitrimer containing dynamic imine bonds (BOB/ETOD). Notably, because of the presence of a large number of siloxane chain segments, BOB/ETOD exhibited excellent flame retardancy (the peak heat release rate (pHRR) was 57.7% lower than that of conventional epoxy resin (DDM/EP) and a carbon residual rate (RC700) of 27.7%, which is 1.6 times higher than that of DDM/EP). Furthermore, the networks of BOB/ETOD could topologically rearrange due to the reversible exchange reaction of imine bonds, making them degradable and reprocessable. Surprisingly, BOB/ETOD also had excellent antimicrobial (the antimicrobial rate was up to 93%) and UV-blocking properties. This work provides a simple and effective solution for the development of multifunctional epoxy-based vitrimers, which is conducive to further expanding the application field of epoxy resins.
研究领域:
材料科学
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环境科学
·
高分子化学
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Polymer Materials
·
2025
·
IF 4.7
Shang Ke Yang,Yan Xiao Mu,De Li,Tong Li,Hai Lan Lin,Ai Ping Zhang,Jun Bian,Dai Qiang Chen,Ke Cheng Yang
Developing biobased thermoplastic polyurethane (TPU) from renewable biomass resources is becoming urgent due to resource scarcity and environmental protection requirements. Herein, a chain extender diol (VAN–OH) containing dynamic imine bonds was synthesized using renewable biomass resource vanillin (VAN), then combined with 1,4-butanediol (BDO) in various proportions, and reacted with poly(caprolactone diol) and 4,4′-diphenylmethane diisocyanate to synthesize degradable biobased TPU (BTPUs) with excellent performance. Fourier transform infrared, 1H NMR, X-ray diffraction, DMA, thermogravimetric analysis, molecular weight, chemical degradation, and mechanical tests systematically investigated the relationships between the polymer chain structure and the performance of BTPUs. The experimental results demonstrated that the high regularity and strong polar bonds (imine and ether) of VAN–OH enhanced the interactions between macromolecular chains and improved the hydrogen bonding combination, crystallinity, and phase separation of BTPUs, thereby exerting significant contributions to their thermomechanical and degradable properties. BVTPU1 with a mole ratio of BDO/VAN–OH = 7.5:2.5 exhibited the best mechanical performance, degradation time was 37.5% shorter, and initial pyrolysis temperature increased by 13.8% compared to BTPU0 without VAN–OH. In addition, BTPUs have shown some biodegradability and environmental friendliness in soil burial experiments under natural conditions.
研究领域:
材料科学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
MACROMOLECULAR RAPID COMMUNICATIONS
·
2022
·Vol. 43
·期 23
·2200562
·
IF 5.006
Jie Mao,Tong Wu,Zhenbin Tang,Long Xia,Liu He,Birong Zeng,Yiting Xu,Conghui Yuan,Lizong Dai
The underlying trend of colloidal synthesis has focused on extending the structure and composition complexity of colloidal particles. Hollow and yolk–shell particles are successful examples that have potential applications in frontier fields. In this paper, a facile and controllable etching method based on the molecular exchange of the dynamic imine bond to generate cavities in polymer particles is developed. Starting from boronate ester polymer particles and inorganic@boronate core–shell particles with the imine bonds incorporated in the polymer networks, the etching method easily affords hollow and yolk–shell particles with tunable shell thicknesses. The molecular exchange dynamics analysis indicates that guest amine molecules cause the reconstruction of imine bonds and the leakage of molecular and oligomer fragments, resulting in the formation of the hollow structure. This molecular exchange-based etching method may be of interest in the construction of polymer architectures with increased composition and structure complexities.
研究领域:
材料科学
·
化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）