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Keywords = dynamic covalent polymer

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34 pages, 19922 KB  
Review
Dynamic Covalent Bonds in 3D-Printed Polymers: Strategies, Principles, and Applications
by Trong Danh Nguyen, My Thi Ngoc Nguyen and Jun Seop Lee
Appl. Sci. 2025, 15(21), 11755; https://doi.org/10.3390/app152111755 - 4 Nov 2025
Viewed by 78
Abstract
Dynamic covalent bonds within polymer materials have been the subject of ongoing research. These bonds impart polymers, particularly thermosets, with capabilities for self-healing and reprocessing. Concurrently, three-dimensional (3D) printing techniques have undergone rapid advancement and widespread adoption. Since polymers are among the primary [...] Read more.
Dynamic covalent bonds within polymer materials have been the subject of ongoing research. These bonds impart polymers, particularly thermosets, with capabilities for self-healing and reprocessing. Concurrently, three-dimensional (3D) printing techniques have undergone rapid advancement and widespread adoption. Since polymers are among the primary materials used in 3D printing, networks featuring dynamic covalent bonds have emerged as a prominent research area. This review outlines approaches for incorporating dynamic covalent bonds into polymers suitable for 3D printing and examines representative studies that leverage these chemistries in material design. Polymers produced using these strategies demonstrate both self-healing and reprocessability, primarily via bond-exchange (metathesis) reactions. In addition, we discuss how the type and amount of dynamic bonds in the network affect the resulting material properties, with particular emphasis on their mechanical, physical, and thermal performance. In particular, the introduction of dynamic covalent bonds seems to significantly improve the degree of anisotropy, which has been the limitation of 3D printing techniques. Finally, we compile recent applications for objects printed from polymers that include dynamic covalent bonds. Full article
(This article belongs to the Section Additive Manufacturing Technologies)
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40 pages, 7197 KB  
Review
Pultrusion and Vitrimer Composites: Emerging Pathways for Sustainable Structural Materials
by Vishal Kumar, Khaled W. Shahwan, Wenbin Kuang, Kevin L. Simmons, Philip Taynton and Emily R. Cieslinski
J. Compos. Sci. 2025, 9(10), 559; https://doi.org/10.3390/jcs9100559 - 13 Oct 2025
Viewed by 1087
Abstract
Pultrusion is a manufacturing process used to produce fiber-reinforced polymer composites with excellent mechanical, thermal, and chemical properties. The resulting materials are lightweight, durable, and corrosion-resistant, making them valuable in aerospace, automotive, construction, and energy sectors. However, conventional thermoset composites remain difficult to [...] Read more.
Pultrusion is a manufacturing process used to produce fiber-reinforced polymer composites with excellent mechanical, thermal, and chemical properties. The resulting materials are lightweight, durable, and corrosion-resistant, making them valuable in aerospace, automotive, construction, and energy sectors. However, conventional thermoset composites remain difficult to recycle due to their infusible and insoluble cross-linked structure. This review explores integrating vitrimer technology a novel class of recyclable thermosets with dynamic covalent adaptive networks into the pultrusion process. As only limited studies have directly reported vitrimer pultrusion to date, this review provides a forward-looking perspective, highlighting fundamental principles, challenges, and opportunities that can guide future development of recyclable high-performance composites. Vitrimers combine the mechanical strength (tensile strength and modulus) of thermosets with the reprocessability and reshaping of thermoplastics through dynamic bond exchange mechanisms. These polymers offer high-temperature reprocessability, self-healing, and closed-loop recyclability, where recycling efficiency can be evaluated by the recovery yield retention of mechanical properties and reuse cycles meeting the demand for sustainable manufacturing. Key aspects discussed include resin formulation, fiber impregnation, curing cycles, and die design for vitrimer systems. The temperature-dependent bond exchange reactions present challenges in achieving optimal curing and strong fiber–matrix adhesion. Recent studies indicate that vitrimer-based composites can maintain structural integrity while enabling recycling and repair, with mechanical performance such as flexural and tensile strength comparable to conventional composites. Incorporating vitrimer materials into pultrusion could enable high-performance, lightweight products for a circular economy. The remaining challenges include optimizing curing kinetics, improving interfacial adhesion, and scaling production for widespread industrial adoption. Full article
(This article belongs to the Section Polymer Composites)
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12 pages, 2200 KB  
Article
Cross-Linked Supramolecular Polyurea Elastomers with Mechanical Robustness and Recyclability
by Yanping Li, Chong Wang and Bo Qin
Molecules 2025, 30(20), 4061; https://doi.org/10.3390/molecules30204061 - 12 Oct 2025
Viewed by 483
Abstract
Cross-linked polymers are indispensable in advanced applications, but suffer from poor recyclability due to permanent covalent networks. Herein, we report recyclable supramolecular polyurea elastomers that integrate ureidopyrimidinone-based quadruple hydrogen-bonding motifs directly into the polymer backbone. The dynamic and reversible nature of these motifs [...] Read more.
Cross-linked polymers are indispensable in advanced applications, but suffer from poor recyclability due to permanent covalent networks. Herein, we report recyclable supramolecular polyurea elastomers that integrate ureidopyrimidinone-based quadruple hydrogen-bonding motifs directly into the polymer backbone. The dynamic and reversible nature of these motifs imparts the SPUEs with remarkable malleability and reprocessability while preserving the robustness of conventional polyureas. The SPUEs display remarkable mechanical robustness, solvent resistance, and facile reprocessability through hot-pressing, producing homogeneous films with minimal performance loss. Impressively, tensile strength, elongation at break, and toughness retained high recovery after reprocessing, demonstrating excellent closed-loop mechanical recyclability. This work showcases supramolecular engineering as a powerful strategy to reconcile mechanical robustness with recyclability in cross-linked polymers, offering new opportunities for sustainable thermosets and elastomers in circular materials design. Full article
(This article belongs to the Special Issue Recyclable Supramolecular Polymer Materials)
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20 pages, 2449 KB  
Article
Suppressed Autoxidation, Enhanced Antioxidant Activity, and Improved Cytocompatibility of Epigallocatechin Gallate via Alginate Site-Specific Conjugation with Tunable Substitution Degree
by Nunnarpas Yongvongsoontorn, Maho Kihara, Masaya Inada, Joo Eun Chung and Motoichi Kurisawa
Int. J. Mol. Sci. 2025, 26(17), 8725; https://doi.org/10.3390/ijms26178725 - 7 Sep 2025
Viewed by 1178
Abstract
Epigallocatechin-3-gallate (EGCG), a major polyphenol in green tea, exhibits strong antioxidant activity but suffers from poor stability due to rapid autoxidation under physiological conditions. In this study, we developed alginate–EGCG conjugates via a site-selective thiol-quinone addition reaction under mild aqueous conditions. The conjugation [...] Read more.
Epigallocatechin-3-gallate (EGCG), a major polyphenol in green tea, exhibits strong antioxidant activity but suffers from poor stability due to rapid autoxidation under physiological conditions. In this study, we developed alginate–EGCG conjugates via a site-selective thiol-quinone addition reaction under mild aqueous conditions. The conjugation preserved EGCG’s flavanic structure while enabling tunable degrees of substitution (DS). We systematically evaluated the oxidative stability, antioxidant activity, and cytocompatibility of alginate–EGCG conjugates in comparison with free EGCG and a mixture of EGCG and alginate. Alginate–EGCG conjugates significantly suppressed EGCG autoxidation, reduced hydrogen peroxide generation, and improved cytocompatibility in human renal epithelial cells, especially at a low DS. Furthermore, alginate–EGCG conjugates retained or even enhanced superoxide anion radical scavenging activity, with higher DS conjugates exhibiting greater antioxidant effects. In addition, dynamic light scattering analysis revealed DS-dependent particle formation via self-assembly. These findings demonstrate that covalent conjugation with natural polymers is an effective strategy to improve oxidative stability and biological functionality of plant-derived polyphenols, offering a promising approach for developing advanced antioxidant materials for food, cosmetic, and biomedical applications. Full article
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17 pages, 2566 KB  
Article
Synergistic Epichlorohydrin-Crosslinked Carboxymethyl Xylan for Enhanced Thermal Stability and Filtration Control in Water-Based Drilling Fluids
by Yutong Li, Fan Zhang, Bo Wang, Jiaming Liu, Yu Wang, Zhengli Shi, Leyao Du, Kaiwen Wang, Wangyuan Zhang, Zonglun Wang and Liangbin Dou
Gels 2025, 11(8), 666; https://doi.org/10.3390/gels11080666 - 20 Aug 2025
Viewed by 564
Abstract
Polymers derived from renewable polysaccharides offer promising avenues for the development of high-temperature, environmentally friendly drilling fluids. However, their industrial application remains limited by inadequate thermal stability and poor colloidal compatibility in complex mud systems. In this study, we report the rational design [...] Read more.
Polymers derived from renewable polysaccharides offer promising avenues for the development of high-temperature, environmentally friendly drilling fluids. However, their industrial application remains limited by inadequate thermal stability and poor colloidal compatibility in complex mud systems. In this study, we report the rational design and synthesis of epichlorohydrin-crosslinked carboxymethyl xylan (ECX), developed through a synergistic strategy combining covalent crosslinking with hydrophilic functionalization. When incorporated into water-based drilling fluid base slurries, ECX facilitates the formation of a robust gel suspension. Comprehensive structural analyses (FT-IR, XRD, TGA/DSC) reveal that dual carboxymethylation and ether crosslinking impart a 10 °C increase in glass transition temperature and a 15% boost in crystallinity, forming a rigid–flexible three-dimensional network. ECX-modified drilling fluids demonstrate excellent colloidal stability, as evidenced by an enhancement in zeta potential from −25 mV to −52 mV, which significantly improves dispersion and interparticle electrostatic repulsion. In practical formulation (1.0 wt%), ECX achieves a 620% rise in yield point and a 71.6% reduction in fluid loss at room temperature, maintaining 70% of rheological performance and 57.5% of filtration control following dynamic aging at 150 °C. Tribological tests show friction reduction up to 68.2%, efficiently retained after thermal treatment. SEM analysis further confirms the formation of dense and uniform polymer–clay composite filter cakes, elucidating the mechanism behind its high-temperature resilience and effective sealing performance. Furthermore, ECX demonstrates high biodegradability (BOD5/COD = 21.3%) and low aquatic toxicity (EC50 = 14 mg/L), aligning with sustainable development goals. This work elucidates the correlation between molecular engineering, gel microstructure, and macroscopic function, underscoring the great potential of eco-friendly polysaccharide-based crosslinked polymers for industrial gel-based fluid design in harsh environments. Full article
(This article belongs to the Section Gel Chemistry and Physics)
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41 pages, 2973 KB  
Review
Self-Healing, Electroconductive Hydrogels for Wound Healing Applications
by Duarte Almeida, Diogo Dias, Frederico Castelo Ferreira and Teresa Esteves
Gels 2025, 11(8), 619; https://doi.org/10.3390/gels11080619 - 8 Aug 2025
Viewed by 2603
Abstract
Electroconductive, self-healing hydrogels have surfaced as a versatile tool for advanced wound care applications, since they combine classic hydrogels’ moist and biomimetic environment with the dynamic electrical responsiveness that can function as an accelerator of tissue repair processes. Recent advances report the automatic [...] Read more.
Electroconductive, self-healing hydrogels have surfaced as a versatile tool for advanced wound care applications, since they combine classic hydrogels’ moist and biomimetic environment with the dynamic electrical responsiveness that can function as an accelerator of tissue repair processes. Recent advances report the automatic restoration of materials after mechanical disruption through various mechanisms, such as ionic or covalent bonds and supramolecular interactions. This property is crucial for biomaterials, as they are often applied in skin regions with high motility and, therefore, a high risk of breakage. By integrating within these networks compounds that are electrically active—polymers such as PEDOT:PSS or polypyrrole, or 2D nanomaterials such as graphene—it is possible to confer responsiveness to these hydrogels, which can lead to increases in fibroblast proliferation, antimicrobial properties, and angiogenesis. Furthermore, these biomaterials must have skin-mimicking mechanical properties and can also be loaded with drugs to improve their healing properties even further. This review synthesizes the chemistry behind the self-healing and electroconductive properties of these materials and expands on the available literature on this field and their biological outcomes, while also providing a look into the future of these promising materials, aiming at their integration in standard wound care strategies. Full article
(This article belongs to the Special Issue Application of Hydrogels in Medicine)
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18 pages, 4008 KB  
Article
Carboxymethyl Chitosan Cinnamaldehyde Coated SilverNanocomposites for Antifungal Seed Priming in Wheat: A Dual-Action Approach Toward Sustainable Crop Protection
by María Mondéjar-López, María Paz García-Simarro, Lourdes Gómez-Gómez, Oussama Ahrazem and Enrique Niza
Polymers 2025, 17(15), 2031; https://doi.org/10.3390/polym17152031 - 25 Jul 2025
Viewed by 650
Abstract
Biogenic silver nanoparticles (AgNPs) were synthesized via a green chemistry strategy using wheat extract and subsequently functionalized with a carboxymethyl chitosan–cinnamaldehyde (CMC=CIN) conjugate through covalent imine bonding. The resulting nanohybrid (AgNP–CMC=CIN) was extensively characterized to confirm successful biofunctionalization: UV–Vis spectroscopy revealed characteristic cinnamaldehyde [...] Read more.
Biogenic silver nanoparticles (AgNPs) were synthesized via a green chemistry strategy using wheat extract and subsequently functionalized with a carboxymethyl chitosan–cinnamaldehyde (CMC=CIN) conjugate through covalent imine bonding. The resulting nanohybrid (AgNP–CMC=CIN) was extensively characterized to confirm successful biofunctionalization: UV–Vis spectroscopy revealed characteristic cinnamaldehyde absorption peaks; ATR-FTIR spectra confirmed polymer–terpene bonding; and TEM analysis evidenced uniform nanoparticle morphology. Dynamic light scattering (DLS) measurements indicated an increase in hydrodynamic size upon coating (from 59.46 ± 12.63 nm to 110.17 ± 4.74 nm), while maintaining low polydispersity (PDI: 0.29 to 0.27) and stable surface charge (zeta potential ~ −30 mV), suggesting colloidal stability and homogeneous polymer encapsulation. Antifungal activity was evaluated against Fusarium oxysporum, Penicillium citrinum, Aspergillus niger, and Aspergillus brasiliensis. The minimum inhibitory concentration (MIC) against F. oxysporum was significantly reduced to 83 μg/mL with AgNP–CMC=CIN, compared to 708 μg/mL for uncoated AgNPs, and was comparable to the reference fungicide tebuconazole (52 μg/mL). Seed priming with AgNP–CMC=CIN led to improved germination (85%) and markedly reduced fungal colonization, while maintaining a favorable phytotoxicity profile. These findings highlight the potential of polysaccharide-terpene-functionalized biogenic AgNPs as a sustainable alternative to conventional fungicides, supporting their application in precision agriculture and integrated crop protection strategies. Full article
(This article belongs to the Special Issue Polymer Materials for Environmental Applications)
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12 pages, 4279 KB  
Article
Dynamic Ester-Linked Vitrimers for Reprocessable and Recyclable Solid Electrolytes
by Xiaojuan Shi, Hui Zhang and Hongjiu Hu
Polymers 2025, 17(14), 1991; https://doi.org/10.3390/polym17141991 - 21 Jul 2025
Viewed by 662
Abstract
Traditional covalently cross-linked solid-state electrolytes exhibit desirable mechanical durability but suffer from limited processability and recyclability due to their permanent network structures. Incorporating dynamic covalent bonds offers a promising solution to these challenges. In this study, we report a reprocessable and recyclable polymer [...] Read more.
Traditional covalently cross-linked solid-state electrolytes exhibit desirable mechanical durability but suffer from limited processability and recyclability due to their permanent network structures. Incorporating dynamic covalent bonds offers a promising solution to these challenges. In this study, we report a reprocessable and recyclable polymer electrolyte based on a dynamic ester bond network, synthesized from commercially available materials. Polyethylene glycol diglycidyl ether (PEGDE) and glutaric anhydride (GA) were cross-linked and cured in the presence of benzyl dimethylamine (BDMA), forming an ester-rich polymer backbone. Subsequently, 1,5,7-triazabicyclo[4.4.0]dec-5-ene (TBD) was introduced as a transesterification catalyst to facilitate network rearrangement. Lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) was incorporated to establish efficient ion transport pathways. By tuning the cross-linking density and catalyst ratio, the electrolyte achieved an ionic conductivity of 1.89 × 10−5 S/cm at room temperature along with excellent reprocessability. Full article
(This article belongs to the Special Issue Recycling and Circularity of Polymeric Materials)
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36 pages, 7153 KB  
Review
Enhancing the Biological Functionality of Hydrogels Using Self-Assembling Peptides
by Woo Hyun Kwon, Kyoung Choi, Sang Jun Park, GeumByeol Park, Cho Young Park, Yoo Han Seo, Chun-Ho Kim and Jun Shik Choi
Biomimetics 2025, 10(7), 442; https://doi.org/10.3390/biomimetics10070442 - 4 Jul 2025
Viewed by 1922
Abstract
Hydrogels are ECM-mimicking three-dimensional (3D) networks that are widely used in biomedical applications; however, conventional natural and synthetic polymer-based hydrogels present limitations such as poor mechanical strength, limited bioactivity, and low reproducibility. Self-assembling peptides (SAPs) offer a promising alternative, as they can form [...] Read more.
Hydrogels are ECM-mimicking three-dimensional (3D) networks that are widely used in biomedical applications; however, conventional natural and synthetic polymer-based hydrogels present limitations such as poor mechanical strength, limited bioactivity, and low reproducibility. Self-assembling peptides (SAPs) offer a promising alternative, as they can form micro- and nanostructured hydrogels through non-covalent interactions and allow precise control over their biofunctionality, mechanical properties, and responsiveness to biological cues. Through rational sequence design, SAPs can be engineered to exhibit tunable mechanical properties, controlled degradation rates, and multifunctionality, and can dynamically regulate assembly and degradation in response to specific stimuli such as pH, ionic strength, enzymatic cleavage, or temperature. Furthermore, SAPs have been successfully incorporated into conventional hydrogels to enhance cell adhesion, promote matrix remodeling, and provide a more physiologically relevant microenvironment. In this review, we summarize recent advances in SAP-based hydrogels, particularly focusing on their novel biofunctional properties such as anti-inflammatory, antimicrobial, and anticancer activities, as well as bioimaging capabilities, and discuss the mechanisms by which SAP hydrogels function in biological systems. Full article
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31 pages, 4977 KB  
Review
Polyimine-Based Self-Healing Composites: A Review on Dynamic Covalent Thermosets for Sustainable and High-Performance Applications
by Xiaoxue Wang, Si Zhang and Yun Chen
Polymers 2025, 17(12), 1607; https://doi.org/10.3390/polym17121607 - 9 Jun 2025
Cited by 3 | Viewed by 2032
Abstract
Polyimine-based composites have emerged as a promising class of dynamic covalent thermosets, combining high mechanical strength, thermal stability, self-healing, recyclability, and reprocessability. This review systematically summarizes recent advances in polyimine synthesis, highlighting dynamic covalent chemistry (DCC) strategies such as imine exchange and reversible [...] Read more.
Polyimine-based composites have emerged as a promising class of dynamic covalent thermosets, combining high mechanical strength, thermal stability, self-healing, recyclability, and reprocessability. This review systematically summarizes recent advances in polyimine synthesis, highlighting dynamic covalent chemistry (DCC) strategies such as imine exchange and reversible Schiff base reactions. Structural customization can be achieved by incorporating reinforcing phases such as carbon nanotubes, graphene, and bio-based fibers. Advanced fabrication methods—including solution casting, hot pressing, and interfacial polymerization—enable precise integration of these components while preserving structural integrity and adaptability. Mechanical performance analysis emphasizes the interplay between dynamic bonds, interfacial engineering, and multiscale design strategies. Polyimine composites exhibit outstanding performance characteristics, including a self-healing efficiency exceeding 90%, a tensile strength reaching 96.2 MPa, and remarkable chemical recyclability. Emerging engineering applications encompass sustainable green materials, flexible electronics, energy storage devices, and flame-retardant systems. Key challenges include balancing multifunctionality, enhancing large-scale processability, and developing low-energy recycling strategies. Future efforts should focus on interfacial optimization and network adaptivity to accelerate the industrial translation of polyimine composites, advancing next-generation sustainable materials. Full article
(This article belongs to the Collection Progress in Polymer Applications)
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16 pages, 19335 KB  
Article
The Silylation Effect of C/SiC Nanofillers on Mechanical Properties of Cellulose Nanocomposite: Insights from Molecular Dynamics Simulations
by Ahmad Y. Al-Maharma, Bernd Markert and Franz Bamer
J. Compos. Sci. 2025, 9(6), 284; https://doi.org/10.3390/jcs9060284 - 31 May 2025
Viewed by 833
Abstract
Silylation treatment improves the hydrophobicity of cellulose by reducing the number of hydroxyl groups in the cellulose chains that are available to react with moisture in the surrounding environment. Additionally, silylation increases stress transfer from cellulose to synthetic nanofillers by forming covalent bonds [...] Read more.
Silylation treatment improves the hydrophobicity of cellulose by reducing the number of hydroxyl groups in the cellulose chains that are available to react with moisture in the surrounding environment. Additionally, silylation increases stress transfer from cellulose to synthetic nanofillers by forming covalent bonds between the hydroxyl groups of cellulose and the oxidized surface of these nanofillers. This study investigates the impact of silane coupling agents on the tensile properties of cellulose nanocomposites. The cellulose nanocomposites are reinforced with four types of C/SiC-based nanofillers: carbon nanotubes, graphene nanoplatelets, silicon carbide nanotubes, and silicon carbide nanoplatelets. Subsequently, the nanofillers are subjected to surface treatment using the silane coupling agent KH550. The mechanical properties of the cellulose nanocomposites are evaluated by molecular dynamics simulations based on the polymer’s consistent forcefield. The results indicate that the reinforcements of silylated silicon carbide nanotubes and carbon nanotubes increase the tensile modulus of cellulose by 18.03% and 24.58%, respectively, compared to their untreated counterparts. Furthermore, the application of silylation treatment on the surface of C/SiC nanofillers increases the yield strength and ultimate tensile strength of cellulose nanocomposites due to enhanced load transfer between cellulose and these reinforcements. Full article
(This article belongs to the Special Issue Characterization and Modelling of Composites, Volume III)
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28 pages, 17687 KB  
Review
Research Status and Potential Direction for Thermoplastic Shape Memory Polymers and Composites: A Review
by Shuai Yang, Yang He, Zijian Song and Yingchun Li
Polymers 2025, 17(10), 1360; https://doi.org/10.3390/polym17101360 - 15 May 2025
Cited by 3 | Viewed by 1362
Abstract
Shape memory polymers (SMPs), due to the programmable deformation and recovery ability, exhibit widespread potential in fields of biomedical devices, smart actuators, and engineering structures. Thermoplastic SMPs, which possess the intrinsic linear molecular chain structures, are able to be processed through diverse methods, [...] Read more.
Shape memory polymers (SMPs), due to the programmable deformation and recovery ability, exhibit widespread potential in fields of biomedical devices, smart actuators, and engineering structures. Thermoplastic SMPs, which possess the intrinsic linear molecular chain structures, are able to be processed through diverse methods, in addition to being re-processed after process-forming, compared with thermoset SMPs. The environmental recycling characteristics for thermoplastic SMPs describe their wide use potential and prospect. In this paper, a comprehensive description of mechanism, matrix polymers, actuations, and applications for thermoplastic SMPs and composites was reviewed. Furthermore, two promising potential developing directions, 4D printing metamaterial and dynamic covalent networks, were proposed. The multifunctionality and enhanced performances of thermoplastic SMPs and composites exhibited excellent application value, which is significant for future advancements. Full article
(This article belongs to the Section Polymer Applications)
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34 pages, 6438 KB  
Review
Advancements in Injectable Hydrogels for Controlled Insulin Delivery: A Comprehensive Review of the Design, Properties and Therapeutic Applications for Diabetes and Its Complications
by Lin Li and Ya Wang
Polymers 2025, 17(6), 780; https://doi.org/10.3390/polym17060780 - 14 Mar 2025
Cited by 2 | Viewed by 4128
Abstract
Glycemic management in diabetes patients remains heavily reliant on multiple daily insulin injections, which often leads to poor patient compliance and an elevated risk of hypoglycemia. To overcome these limitations, injectable hydrogels capable of encapsulating insulin within polymeric networks have emerged as a [...] Read more.
Glycemic management in diabetes patients remains heavily reliant on multiple daily insulin injections, which often leads to poor patient compliance and an elevated risk of hypoglycemia. To overcome these limitations, injectable hydrogels capable of encapsulating insulin within polymeric networks have emerged as a promising alternative. Ideally, a single injection can form an in situ depot that allows prolonged glycemic control and lower injection frequency. This review summarizes recent advances in injectable hydrogels for controlled insulin delivery, focusing on the polymer sources, crosslinking strategies, and stimuli-responsive release mechanisms. Synthetic polymers such as PEG, PNIPAM, and Pluronics dominate the current research due to their highly tunable properties, whereas naturally derived polysaccharides and proteins generally require further modifications for enhanced functionality. The crosslinking types, ranging from relatively weak physical interactions (hydrogen bonds, hydrophobic interactions, etc.) to dynamic covalent bonds with higher binding strength (e.g., Schiff base, phenylboronate ester), significantly influence the shear-thinning behavior and stimuli-responsiveness of hydrogel systems. Hydrogels’ responsiveness to temperature, glucose, pH, and reactive oxygen species has enabled more precise insulin release, offering new options for improved diabetic management. Beyond glycemic regulation, this review also explores insulin-loaded hydrogels for treating complications. Despite the progress, challenges such as burst release, long-term biocompatibility, and scalability remain. Future research should focus on optimizing hydrogel design, supported by robust and comprehensive data. Full article
(This article belongs to the Section Polymer Applications)
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23 pages, 6274 KB  
Review
Dynamic Bonds in Biopolymers: Enhancing Performance and Properties
by Trong Danh Nguyen and Jun Seop Lee
Polymers 2025, 17(4), 457; https://doi.org/10.3390/polym17040457 - 9 Feb 2025
Cited by 6 | Viewed by 3280
Abstract
As the demand for polymer materials increases, conventional petroleum-based synthetic polymers face several significant challenges, including raw material depletion, environmental issues, and the potential for biotoxicity in biological applications. In response, bio-based polymers derived from natural sources, such as cellulose, alginate, chitosan, and [...] Read more.
As the demand for polymer materials increases, conventional petroleum-based synthetic polymers face several significant challenges, including raw material depletion, environmental issues, and the potential for biotoxicity in biological applications. In response, bio-based polymers derived from natural sources, such as cellulose, alginate, chitosan, and gelatin, have garnered attention due to their advantages of biocompatibility and biodegradability. However, these polymers often suffer from poor physical stability due to the high density of hydrogen bonds and the large structure of pyranose rings. This review explores the potential of incorporating dynamic covalent bonds into biopolymers to overcome these limitations. The chemical structures of biopolymers contain numerous functional groups that can serve as anchoring sites for dynamic bonds, thereby enhancing the mechanical properties and overall stability of the polymer network. The review discusses the performance improvements achievable through dynamic covalent bonds and examines the future potential of this technology to enhance the physical properties of biopolymers and expand their applicability in biological fields. Full article
(This article belongs to the Section Biobased and Biodegradable Polymers)
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20 pages, 3507 KB  
Review
Epoxy-Based Vitrimers for Sustainable Infrastructure: Emphasizing Recycling and Self-Healing Properties
by Myung Kue Lee, Min Ook Kim, Taehwi Lee, Sanghwan Cho, Dongchan Kim, Wonghil Chang, Yongseok Kwon, Seongkwan Mark Lee, Ju Kwang Kim and Bong Cheol Son
Polymers 2025, 17(3), 373; https://doi.org/10.3390/polym17030373 - 30 Jan 2025
Cited by 4 | Viewed by 4095
Abstract
Epoxy-based vitrimers represent a paradigm shift in material science, offering an unprecedented combination of mechanical robustness, environmental sustainability, and reconfigurability. These dynamic polymer systems utilize associative dynamic covalent bonds (DCBs) such as transesterification to blend the structural integrity of thermosets with the recyclability [...] Read more.
Epoxy-based vitrimers represent a paradigm shift in material science, offering an unprecedented combination of mechanical robustness, environmental sustainability, and reconfigurability. These dynamic polymer systems utilize associative dynamic covalent bonds (DCBs) such as transesterification to blend the structural integrity of thermosets with the recyclability and self-healing properties of thermoplastics. This unique combination makes vitrimers ideal candidates for high-performance applications in industries such as civil engineering, where material durability, repairability, and environmental compatibility are critical. Epoxy-based vitrimers, in particular, exhibit exceptional self-healing capabilities, allowing them to autonomously repair microcracks and damage, restoring mechanical properties under appropriate stimuli such as heat or light. Their recyclability further aligns with global sustainability goals by reducing material waste and lifecycle costs. Recent advancements have also integrated bio-based feedstocks and scalable manufacturing methods, enhancing the feasibility of these materials for industrial applications. This review explores the underlying self-healing mechanisms, dynamic recycling processes, and the emerging role of epoxy-based vitrimers in civil engineering. Challenges related to scalability, mechanical optimization, and regulatory acceptance are also discussed, with a focus on their potential to drive sustainable innovation in infrastructure materials. Full article
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