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By: Sandeep Rai and Shuchi Tiwari.
1Doctoral Progress Committee (DPC) Member, Department of Polymer & Rubber Technology, UPL University of Sustainable Technology, Block No.402, Ankleshwar-Valia Road, Taluka- Valia, Distt- Bharuch, Pin code- 393135, Gujarat, India.
2Assistant Professor, Department of Chemistry, VNR Vignana Jyothi Institute of Engineering & Technology, Hyderabad, Pin code-500118, Telangana, India.
Self-healing polymeric materials are one of the most rapidly growing and technologically transformative classes of smart polymeric materials. Such materials offer the ability to autonomously repair damage and retain & restore functional performance. This capability is very important for polymers, which undergo mechanical failure, micro- cracking, delamination, photo-oxidation, or thermal degradation during service environments. The last decade has been remarkable for developments in self-healing polymers, ranging from extrinsic capsule-based approaches to fully intrinsic dynamic polymer networks which are capable of repeated & stimulus-free healing . This review delves into recent advances in the design, mechanisms, fabrication, and applications of self-healing polymers with focus on dynamic covalent chemistry, supramolecular interactions, reversible crosslinking, microvascular networks, and emerging bio-based architectures.
Key healing mechanisms are Diels–Alder reactions, disulfide exchange, transesterification, dynamic imine bonding, hydrogen-bonding, ionic interactions, π–π stacking, host–guest complexation, & metal–ligand coordination are discussed. The review also highlights how molecular re-configurability, network topology, segmental mobility, and relaxation dynamics govern healing efficiency, and how healing can be activated through heat, light, pH, moisture, electricity, magnetic fields, or completely autonomously.
Applications of self-healing polymers are rapidly growing into various applications like structural composites, coatings, biomedical implants, soft robotics, wearable electronics, 3D printing, energy storage devices, sealants, adhesives, and aerospace materials etc. Incorporation of conductive fillers, nano additives, catalytic species, and stimuli- responsive nanostructures are capable of providing excellent multi-functionality i.e. self- healing conductivity, barrier recovery, and mechanical reinforcement. However, technological challenges still remain regarding scaling up, long-term stability, healing at low temperatures, commercialization, and fundamental understanding of cause of damage evolution.
This review briefly presents an overview of state-of-the-art self-healing polymer technologies and future directions toward development and scaling up sustainable, durable, and intelligent material systems for numerous industrial applications. Focus is on emerging trends like autonomous healing, recyclable dynamic networks, vitrimer- based materials, and bio-mimetic healing strategies similar to natural systems such as skin, bone, and plant resins.
Citation:
Refrences:
1.
Choi K, Noh A, Kim J, Hong PH, Ko MJ, Hong SW. Properties and applications of self-healing polymeric materials: A review. Polymers (Basel). 2023;15(22):4408. doi:10.3390/polym15224408
2.
Srivastav RS, More AP. A comprehensive review of self-healing polymers: Mechanisms, types, and industry implications. Polym Adv Technol. 2025;36:e70092. doi:10.1002/pat.70092
3.
White SR, et al. Advances in microencapsulated self-healing systems. Nature.
2020.
4.
He X, Yu K. Additive manufacturing of self-healing polymers and composites. In: Li G, Feng X, editors. Recent Advances in Smart Self-Healing Polymers and Composites. 2nd ed. Woodhead Publishing; 2022. p. 433–456. doi:10.1016/B978-0-12-823472-3.00010-2
5.
Terryn S, Langenbach J, Roels E, Brancart J, Bakkali-Hassani C, Poutrel QA, et al. A review on self-healing polymers for soft robotics. Mater Today. 2021;47:187–205. doi:10.1016/j.mattod.2021.01.009
6.
Wang X, Ding T. A review on the current state of microcapsule-based self-healing dental composites. J Funct Biomater. 2024;15:165. doi:10.3390/jfb15060165
7.
White SR. Microvascular self-healing materials. University of Illinois. Available from: http://whitegroup.beckman.illinois.edu/research/self-healing-materials/microvascular-healing/
8.
Liao CY, Zhang L, Hu SY, Xia SJ, Li DM. Recent advances of self-healing materials for civil engineering: Models and simulations. Buildings. 2024;14:961. doi:10.3390/buildings14040961
9.
Jin S, Oh DX, Park J. ChemSusChem. 2025;19:e202501023. doi:10.1002/cssc.202501023
10.
Buaksuntear K, Limarun P, Suethao S, Smitthipong W. Non-covalent interaction on the self-healing of mechanical properties in supramolecular polymers. Int J Mol Sci. 2022;23:6902. doi:10.3390/ijms23136902
11.
Reddy KR, El-Zein A, Airey DW, Alonso-Marroquin F, Schubel P, Manalo A. Self-healing polymers: Synthesis methods and applications. Nano Struct Nano Objects. 2020;23:100500. doi:10.1016/j.nanoso.2020.100500
12.
Kontiza A, Kartsonakis IA. Smart composite materials with self-healing properties: A review on design and applications. Polymers (Basel). 2024;16(15):2115. doi:10.3390/polym16152115
13.
Chen J, Wang L, Xu X, Liu G, Liu H, Qiao Y, et al. Self-healing materials-based electronic skin: Mechanism, development and applications. Gels. 2022;8(6):356. doi:10.3390/gels8060356
14.
Choi K, Noh A, Kim J, Hong PH, Ko MJ, Hong SW. Properties and applications of self-healing polymeric materials: A review. Polymers (Basel). 2023;15(22):4408. doi:10.3390/polym15224408
15.
Adil MM, Rabbi MS, Tasnim T. Development of microcapsule-based self-healing composite: A critical review. Alex Eng J. 2025;122:1–17. doi:10.1016/j.aej.2025.02.092
16.
Pries AR, Secomb TW. Making microvascular networks work: Angiogenesis, remodeling, and pruning. Physiology (Bethesda). 2014;29(6):446–455. doi:10.1152/physiol.00012.2014
17.
Han S, Zhang XL, Guo YD, Wang YY, Su JF. Research progress of self-healing materials using hollow fibers. New Chem Mater. 2017.
18.
Ratwani CR, Novoselov KS, Abdelkader AM. Applications and mechanistic insights into intrinsically self-healing polymers with multifunctional 2D materials. SusMat. 2025;5(4):e70028. doi:10.1002/sus2.70028
19.
Ribeiro MM, Simões M, Vitorino C, Mascarenhas-Melo F. Physical crosslinking of hydrogels: The potential of dynamic and reversible bonds in burn care. Coord Chem Rev. 2025;542:216868. doi:10.1016/j.ccr.2025.216868
20.
Strandman S, Zhu XX. Self-healing supramolecular hydrogels based on reversible physical interactions. Gels. 2016;2:16. doi:10.3390/gels2020016
21.
Park JS, Darlington T, Starr AF, Takahashi K, Riendeau J, Hahn HT. Multiple healing effect of thermally activated self-healing composites based on Diels–Alder
reaction. Compos Sci Technol. 2010;70(15):2154–2159. doi:10.1016/j.compscitech.2010.08.017
22.
Ehrhardt D, Mangialetto J, Bertouille J, Van Durme K, Van Mele B, Van den Brande N. Self-healing in mobility-restricted conditions using Diels–Alder cycloadditions. Polymers. 2020;12:2543. doi:10.3390/polym12112543
23.
Jin S, Oh DX, Park J. ChemSusChem. 2025;19:e202501023. doi:10.1002/cssc.202501023
24.
Condò I, Giannitelli SM, Lo Presti D, Cortese B, Ursini O. Overview of dynamic bond based hydrogels for reversible adhesion processes. Gels. 2024;10:442. doi:10.3390/gels10070442
25.
Zeng L, Song M, Gu J, Xu Z, Xue B, Li Y, et al. A highly stretchable self-healing hydrogel based on peptide–metal ion coordination. Biomimetics. 2019;4:36. doi:10.3390/biomimetics4020036
26.
Davletbaeva MI, Sazonov OO. Macromolecular and supramolecular organization of ionomers. Polymers. 2025;17:3188. doi:10.3390/polym17233188
27.
Gao R, Ge Q, Cong H, Zhang Y, Zhao J. Preparation and biomedical applications of cucurbit[n]uril-based supramolecular hydrogels. Molecules. 2023;28:3566. doi:10.3390/molecules28083566
28.
Guo F, Li X, Wang Z, Chen Y, Yue J. Factors affecting self-healing performance of graphene-modified asphalt. Polymers. 2024;16:2482. doi:10.3390/polym16172482
29.
Jiang Y, Ng ELL, Han DX, Yan Y, Chan SY, Wang J, et al. Self-healing polymeric materials for additive manufacturing. Polymers. 2023;15:4206. doi:10.3390/polym15214206
30.
Kothari J, Iroh JO. Self-healing poly(urea formaldehyde) microcapsules: Synthesis and characterization. Polymers. 2023;15:1668. doi:10.3390/polym15071668
31.
Vintila IS, Ghitman J, Iovu H, Paraschiv A, Cucuruz A, Mihai D, et al. Microvascular self-healing approach in polymeric composites. Polymers. 2022;14:2798. doi:10.3390/polym14142798
32.
Choi K, Noh A, Kim J, Hong PH, Ko MJ, Hong SW. Properties and applications of self-healing polymeric materials: A review. Polymers. 2023;15:4408. doi:10.3390/polym15224408
33.
Dallaev R. Advances in materials with self-healing properties: A brief review. Materials. 2024;17:2464. doi:10.3390/ma17102464
34.
Liao CY, Zhang L, Hu SY, Xia SJ, Li DM. Recent advances of self-healing materials for civil engineering: Models and simulations. Buildings. 2024;14:961. doi:10.3390/buildings14040961