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Progress in Chemistry 2023, Vol. 35 Issue (1): 135-156 Previous Articles   Next Articles

• Review •

Fabrication Strategies to Self-Healing Silicone Materials

Juan Ye1, Ziqian Lin1, Weijian Li1, Hongping Xiang1(), Minzhi Rong2, Mingqiu Zhang2   

  1. 1 Guangdong Provincial Key Laboratory of Functional Soft Condensed Matter, School of Materials and Energy, Guangdong University of Technology,Guangzhou 510006, China
    2 Key Laboratory for Polymeric Composite and Functional Materials of Ministry of Education, Key Laboratory of High Performance Polymer Based Composites of Guangdong Province, School of Chemistry, Sun Yat-sen University,Guangzhou 510275, China
  • Received: Revised: Online: Published:
  • Contact: *e-mail: xianghongping@gdut.edu.cn
  • Supported by:
    National Natural Science Foundation of China(52033011); National Natural Science Foundation of China(52273104); Guangdong Basic and Applied Basic Research Foundation(2022A1515011972)
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In recent years, inspired by the natural phenomenon that the living organism can automatically repair its damaged skin and bone via itself metabolism, researchers have successfully developed self-healing materials that can self-heal their microcracks. The self-healing of materials can effectively extend the service life of materials, improve working stability and thus reduce the waste of resources. Recently, the self-healable silicone materials originated from the synergistic combination of self-healing function and good properties of silicone materials, have become a research focus in functional materials. Furthermore, since the external stimuli such as UV irradiation, temperature and solvent are the external driving force for materials to fulfill self-healability, and affect largely the self-healing efficiency. More importantly, different stimuli have different advantages and disadvantages, and application fields. Therefore, this study aims to summarize and analyze the research progress of extrinsic and intrinsic self-healing silicone materials especially in the past five years according to their external stimuli. The intrinsic self-healing silicone materials that contain different dynamic polysiloxane crosslinking networks activated by different external stimuli, are emphatically discussed. Additionally, a brief prospect for the future development of self-healing silicone materials is also provided.

Contents

1 Introduction

2 Extrinsic self-healing silicone materials

2.1 Hydrolytic condensation crosslinking

2.2 Hydrosilylation crosslinking

2.3 Photo-crosslinking

3 Intrinsic self-healing silicone materials

3.1 Thermal-activated self-healing silicone materials

3.2 Photo-activated self-healing silicone materials

3.3 Medium-driven self-healing silicone materials

4 Conclusion and outlook

Key words: silicone materials, extrinsic self-healing, intrinsic self-healing, stimulus-response factor
Fig. 1 (a) Mechanism of microcapsule self-healing materials: crack formation, the microcapsule breaking and releasing the healing agent, and the healing agent reacting with catalyst to realize healing[19]; (b) schematic diagram of different dynamic reversible structures used in intrinsic self-healing materials[25]
Fig. 2 (a) Schematic illustration of the melamine-urea-formaldehyde shell-forming reaction and condensation polymerization of PDMS in the presence of the DBTL catalyst; (b) self-healing of the dual-microcapsule-integrated silicone composite at room temperature for 24 h after cracking[27]
Fig. 3 (a) The self-healing procedures with dual capsule systems; (b) the crosslinking reaction between Sylgard 184 Part A and hydrogen silicone oil by hydrosilylation[29]
Fig. 4 Mechanism of self-healing silicone resin with CS-RGO microcapsules[31]
Fig. 5 Intrinsic self-healing silicone materials based on different stimulus-response factors
Fig. 6 (a) Synthesis of PDMS-PUa; (b) self-repairing process of PDMS-PUa with 5.0 wt% DCOIT at room temperature; (c) images of the tested panels coated with PDMS-PUa/DCOIT after immersion in seawater for 90 and 180 d[43]
Fig. 7 (a) The chemical structure of PDPU elastomer; (b) the microscope images of self-healing PDPU; (c) output voltages of gaS-Solid interacted triboelectric nanogenerators based on the PDPU before damage and after healing; (d) the sensing performance of self-powered electronic skin based on PDPU[44]
Fig. 8 Self-healing mechanism of PDMS elastomer based on reversible dissociation/association of multivalent hydrogen bonds[46]
Fig. 9 (a) Preparation of polysiloxane elastomer PMFS containing DA bonds; (b) schematic illustration of self-healing process[48]
Fig. 10 (a) Synthesis of silicone oligomer with reactive motifs; (b) illustration of self-healing within the graphene-reinforced polysiloxane nanocomposite[50]
Fig. 11 (a) Schematic structure of the PDMS-COO-Zn polymer network at different temperatures;(b) microscopic images of a film before (left) and after (right) healing at 80 ℃ for 4 h;(c) objects printed by PDMS-COO-Zn polymer and their applications[57]
Fig. 12 (a) The structure of polymer complex Zn(Hbimcp)2-PDMS; (b) energy dissipation process for [Zn(Hbimcp)2]2+; (c) photographs of a film before and after stretching; (d) optical image of a film sustaining a 1000 g load[58]
Fig. 13 (a) The dynamic crosslinked PDMS elastomer; (b) mechanisms of recycling and water-driven malleability[63]
Fig. 14 (a) Preparation of ionically crosslinked elastomers from PDMS-g-COOH and ZnO; (b) Self-healing images of the original (left), cut (middle) and re-hot-pressed (right) samples; (c) Stretching images of healed PDMS elastomer[65].
Fig. 15 (a) Schematic illustration of UV/thermal dual crosslinked silicone elastomers; (b) photographs for the self-healing and reprocessing of the silicone elastomers[66]
Fig. 16 (a) Synthesis process of PDMS-PU elastomer; (b) schematic illustration of the self-healing process within the PDMS-PU elastomer based on radical-mediated disulfide bonds exchange reaction under heating[74]
Fig. 17 (a) Synthetic route of PIH;(b)schematic diagram of self-healing process of PIH elastomer based on disulfide metathesis reaction. The dyed PIH-12.5 was cut in half, and self-healed for 3 h at 25 ℃. The healed film can load a mass of 50 g. (c) PIH composites with rapid room temperature self-healing function under the ablation of butane flame[76]
Fig. 18 (a) Schematic representation of the self-healing process of PDMS elastomer; (b) self-healing illustration of square sample cut into several pieces and healed sample being stretched[79]
Fig. 19 (a) Reversibility of Si—O—Si bonds in poly(silsesquioxane) containing TEA; (b) LSCM images showing the self-healing process of a scratch (50 μm in average width)[80]
Fig. 20 (a) Schematic representation of the self-healing mechanism for the blend based on π-π stacking; (b) SEM images of the fractured film under increasing temperature[81]
Fig. 21 (a) The proposed ideal structure of the supramolecular polymer network based on strong crosslinking H-bonds, weak crosslinking H-bonds, and disulfide metathesis; (b) photographs of film after self-healing and enabling high stretchability (left) and (right) self-healing of film in a 30% NaCl solution at -10 ℃[91]
Fig. 22 Mechanism of self-healing PDMS-SS-DOPA-Fe material and the performance of the flexible PDMS-SS-DOPA1-Fe2-based strain sensor[92]
Fig. 23 (a) Preparation of self-healing silicone elastomers (PDETAS-FBA) based on dual asymmetric dynamic cross-linked chain structure; (b) the self-healing and reprocessing of PDETAS-FBA[24]
Fig. 24 (a) Synthesis process of the crosslinked silicone elastomer containing disulfide bonds; (b) silicone elastomer recycled in solid state under sunlight[99]
Fig. 25 (a) Synthesis of disulfide-linked SEs; (b) self-repairing experiments of SE-3 under UV light (365 nm) for 30 min (ⅰ) or heating at 150 ℃ for 2 h (ⅱ); (c) bonding performance test[100]
Fig. 26 The schematic diagram of light-healing process of Zn(abpy)2 -PDMS[101]
Fig. 27 Mechanism of the water-enabled healing process[104]
Fig. 28 (a) Plasticization of ionic aggregate by CO2 gas activiated network rearrangement; (b) photograph of self-healing behavior of cherry blossom-shaped PDMS-75Na film at 26 ℃[105]
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