Dual-crosslinking side chains with an asymmetric chain structure: a facile pathway to a robust, self-healable, and re-dissolvable polysiloxane elastomer for recyclable flexible devices

Lin, Ziqian; Deng, Haiqin; Hou, Yang; Liu, Xiaoxuan; Xu, Ruijie; Xiang, Hongping; Peng, Zhongquan; Minzhi, Rong; Zhang, Ming Qiu

doi:10.1039/d2ta01535h

Cited by 32 publications

(22 citation statements)

References 72 publications

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“…Elastomers feature viscoelasticity and the ability to respond easily and reversibly to large deformations under stress. − As an indispensable part of our daily life, elastomers are promising for applications in tires, seals, protective coatings, wearable electronics, shape memory materials, and health-care monitoring. − However, elastomers often inevitably encounter the formation and expansion of internal microcracks during their service life, which further results in functional failure and premature discard. Taking into account the serious burden on resources and the environment, tremendous efforts have been devoted to introducing dynamic covalent bonds (such as Diels–Alder bonds, , disulfide bonds, − diselenide bonds, boronic ester bonds, − imine bonds, − and oxime-carbamate bonds − ) or noncovalent interactions (such as hydrogen bonds, − metal–ligand coordination, − host–guest interactions, ionic interactions, , and π–π stacking interactions) into the elastomers to achieve intrinsic self-healability. Remarkably, there is an incongruous contradiction between mechanical performance and healing capacity .…”

Section: Introductionmentioning

confidence: 99%

A Strategy of Thiolactone Chemistry to Construct Strong and Tough Self-Healing Supramolecular Polyurethane Elastomers via Hierarchical Hydrogen Bonds and Coordination Bonds

Cai

et al. 2023

Ind. Eng. Chem. Res.

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Self-healing elastomers with extended service life and enhanced reliability have attracted extensive attention in recent years due to their broad application in fields such as protective coatings, wearable electronics, shape memory materials, and health-care monitoring. However, it is challenging to simultaneously optimize the mechanical properties (strength and toughness) and self-healing capacity of the elastomers. Herein, thiolactone chemistry was delicately used as a bridge to address this conundrum by incorporating 2-ureido-4[1H]-pyrimidinone (UPy) motifs and imidazole ligands into the side chains of linear polyurethane. The synergistic cross-linking of UPy Hbonds and Zn 2+ -imidazole coordination afforded a robust supramolecular network to significantly improve the strength. Meanwhile, these dynamic cross-linking points acted as sacrificial bonds for energy dissipation under external stress, which played a dominant role in toughening. Therefore, the resultant elastomer (PU-Im-UPy-Zn) exhibited a tensile strength of 9.1 MPa, a breaking elongation of 989%, and toughness up to 62.1 MJ m −3 . In addition, the reversible exchange of hierarchical hydrogen bonds (single H-bonds between the carbamate groups and quadruple H-bonds of the UPy dimers) and coordination bonds as well as the high mobility of side chains were conducive to repairing under mild conditions. The superficial scratches completely disappeared at 60 °C, and a satisfactory healing efficiency of 78% was observed after 24 h. This work provides some insights into future design of self-healable supramolecular polyurethane elastomers integrated with conspicuous strength and toughness.

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Section: Introductionmentioning

confidence: 99%

A Strategy of Thiolactone Chemistry to Construct Strong and Tough Self-Healing Supramolecular Polyurethane Elastomers via Hierarchical Hydrogen Bonds and Coordination Bonds

Cai

et al. 2023

Ind. Eng. Chem. Res.

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“…The FTIR spectra of AOI and H-AOI are shown in Figure 2a. The absorption peak of N-H stretching vibration appears at 3368 cm -1 , the absorption peak of N-H bending vibration is 1533 cm -1 [35], and the absorption peak at 1730 cm -1 belongs to the stretching vibration of the carbonyl group (C=O). This is the characteristic peak of the carbamate group, resulting from the reaction of isocyanate groups (-NCO) with hydroxyl groups (-OH).…”

Section: Results and Discussion 41 Structure Analysis Of H-aoimentioning

confidence: 99%

Synthesis and properties of a novel waterborne photosensitive resin for 3D printing

Luo¹,

Zhang²,

Xu³

et al. 2023

Express Polym. Lett.

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A series of novel waterborne photosensitive resins were prepared successfully with poly(propylene oxide) bis(2-aminopropyl ether), tricyclodecane dimethanol diacrylate, 2-isocyanatoethyl acrylate, and hydrochloric acid by Michael addition reaction. The results show that with the increasing double bonds content, the double bonds conversion increases from 78.7, 85.6 to 92.8% in the photopolymerization, respectively, and the gel content of the UV-cured film increases from 48.05, 69.10 to 83.28%. In addition, the glass transition temperature and tensile strength of the UV-cured film follow the same increasing trend. Moreover, the content of hydrochloride has a great influence on the hydrophilicity of the waterborne photosensitive resins. The studies indicated that as the hydrochloride content decreases, the surface water contact angle of the UV-cured film increases from 10.8, 22.9 to 51.5°, and water absorption decreases from 26.55, 16.20 to 11.06%, respectively. Moreover, the waterborne photosensitive resins exhibited a high printing accuracy together with a good effect of washing and are promising for 3D printing.

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“…In recent years, several green cross-linking systems have been reported (azidoalkyl cycloaddition, boron ester, Diels–Alder, etc.). Amino-functionalized polydimethylsiloxanes have attracted considerable interest from researchers due to their strong reactivity , and the availability of polymers of different molecular weights and functionalities for commercial use. − It allows catalyst-free cross-linking with a variety of cross-linkers, such as Aza-Michael reactions, − ureas from reaction with isocyanates, , and imine bonding through reaction with aldehydes . However, even though these reactions are already catalyst-free cross-linking systems, the adhesion properties of the prepared elastomers are relatively poor.…”

Section: Introductionmentioning

confidence: 99%

Bioinspired High-Performance Silicone Elastomers by Catalyst-Free Dopamine Cross-Linking

Liu,

Hu,

Zheng

et al. 2024

Ind. Eng. Chem. Res.

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Silicone elastomers, as good sealants and adhesives, have been widely applied in protective coatings, architectural decoration, electronic packaging, and other fields. However, the traditional cross-linking of silicone elastomers is highly dependent on toxic catalysts or heavy metals, which may inevitably lead to severe environmental pollution. Moreover, most silicone elastomers suffer from a poor adhesive performance. In this study, inspired by the high adhesion properties of mussels, an eco-friendly and catalyst-free silicone elastomer with high adhesion properties was prepared by using dopamine as a cross-linker and amino-functionalized polysiloxane as a base. Under mild conditions (pH = 8.5), dopamine was self-polymerized and underwent Michael addition and Schiff base reactions with amino groups to form robust elastomers. It was found that the cross-linking degree gradually increases with the dopamine content increasing from 2 to 6%, and the solvent resistance and thermal stability exhibit significant improvement. Meanwhile, the tensile strength increased by 245% from 0.22 to 0.77 MPa. Especially, the as-obtained silicone elastomers have excellent adhesion to different materials. The lap shear strength with aluminum substrates (1.09 MPa) is 3.6 times higher than that of conventional silicone elastomers. The development of catalyst-free bioinspired silicone elastomers with high adhesion may shed light on the research of eco-friendly silicone materials and offer innovative insight for mussel-inspired adhesives.

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Dual-crosslinking side chains with an asymmetric chain structure: a facile pathway to a robust, self-healable, and re-dissolvable polysiloxane elastomer for recyclable flexible devices

Abstract: A strategy of dual-crosslinking side chains with an asymmetric chain structure can facilely fulfill robustly self-healable and re-dissolvable polysiloxane elastomer, ensuring the large-scale applications in recyclable flexible devices and adhesives.

Cited by 32 publications

References 72 publications

A Strategy of Thiolactone Chemistry to Construct Strong and Tough Self-Healing Supramolecular Polyurethane Elastomers via Hierarchical Hydrogen Bonds and Coordination Bonds

A Strategy of Thiolactone Chemistry to Construct Strong and Tough Self-Healing Supramolecular Polyurethane Elastomers via Hierarchical Hydrogen Bonds and Coordination Bonds

Synthesis and properties of a novel waterborne photosensitive resin for 3D printing

Bioinspired High-Performance Silicone Elastomers by Catalyst-Free Dopamine Cross-Linking

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