Volume 142, Issue 23 e56981
RESEARCH ARTICLE

Enhanced Multifunction in Polyurethane Elastomers via Regulation of Triple-Crosslinked Network With Dynamic Covalent and Noncovalent Bonds

Rongmei Su

Rongmei Su

Chongqing Key Laboratory of Soft-Matter Material Manufacturing, Department of Chemistry and Chemical Engineering, Southwest University, Chongqing, China

Contribution: Conceptualization (lead), Data curation (lead), Formal analysis (lead), ​Investigation (lead), Methodology (lead), Project administration (lead), Resources (lead), Software (lead), Validation (lead), Visualization (lead), Writing - original draft (lead)

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Pu Huang

Pu Huang

National Key Laboratory of Aerospace Chemical Power, Hubei Institute of Aerospace Chemotechnology, Xiangyang, Hubei, China

Contribution: Conceptualization (supporting), Data curation (supporting), Formal analysis (supporting), Resources (supporting), Validation (supporting), Visualization (supporting)

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Lin Gan

Lin Gan

Chongqing Key Laboratory of Soft-Matter Material Manufacturing, Department of Chemistry and Chemical Engineering, Southwest University, Chongqing, China

Contribution: Conceptualization (supporting), Data curation (supporting), ​Investigation (supporting), Methodology (supporting), Validation (supporting), Visualization (supporting)

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Shuiping Zhou

Shuiping Zhou

National Key Laboratory of Aerospace Chemical Power, Hubei Institute of Aerospace Chemotechnology, Xiangyang, Hubei, China

Contribution: ​Investigation (supporting), Methodology (supporting), Project administration (supporting), Visualization (supporting), Writing - original draft (supporting)

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Xiaoan Li

Xiaoan Li

Chongqing Key Laboratory of Soft-Matter Material Manufacturing, Department of Chemistry and Chemical Engineering, Southwest University, Chongqing, China

Contribution: Software (supporting), Validation (supporting), Visualization (supporting)

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Wei Li

Corresponding Author

Wei Li

National Key Laboratory of Aerospace Chemical Power, Hubei Institute of Aerospace Chemotechnology, Xiangyang, Hubei, China

Correspondence:

Wei Li ([email protected])

Jin Huang ([email protected])

Yi He ([email protected])

Contribution: Funding acquisition (supporting), Writing - review & editing (supporting)

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Jin Huang

Corresponding Author

Jin Huang

Chongqing Key Laboratory of Soft-Matter Material Manufacturing, Department of Chemistry and Chemical Engineering, Southwest University, Chongqing, China

Correspondence:

Wei Li ([email protected])

Jin Huang ([email protected])

Yi He ([email protected])

Contribution: Funding acquisition (lead), Project administration (lead), Resources (lead), Validation (lead), Writing - review & editing (lead)

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Yi He

Corresponding Author

Yi He

School of Materials Science and Engineering, Sichuan University of Science and Engineering, Zigong, China

Correspondence:

Wei Li ([email protected])

Jin Huang ([email protected])

Yi He ([email protected])

Contribution: Supervision (supporting), Validation (supporting), Writing - review & editing (lead)

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First published: 12 March 2025

Funding: This research is financially supported by the funded by Open Research Fund Program of the National Key Laboratory of Aerospace Chemical Power (NKLACP120241B02).

ABSTRACT

Self-healing polyurethane elastomers with dynamic crosslinking networks are promising candidates for intelligent next-generation coatings. However, their constitutive relation shows conflicts between high mechanical performance and room-temperature self-healing, as well as recyclability. Here, a regulation strategy of a dynamic triple-crosslinked network in the hard domain was proposed to achieve multifunction enhancement via covalent borate ester bonds coupling noncovalent. The distribution and ratio of borate ester bonds, boron-nitrogen coordination bonds, and multiple hydrogen bonds were meticulously designed to balance fracture and reconstruction of the molecular network. The introduced borate ester bonds enabled the basic room-temperature self-healing and mechanical performance of polyurethane elastomers through molecule-level topological evolution. The designed boron-nitrogen coordination bonds and abundant hydrogen bonds provided external noncovalent reversible crosslinking networks, thus improving tensile strength and toughness as physical crosslinking points. The obtained polyurethane elastomers exhibited impressive light transmittance of 93%, a tensile strength of 41.07 MPa, elongation at break of 1673.20%, toughness of 166.74 MJ m−3, and almost entirely room-temperature self-healing in 48 h. These polyurethane elastomers even maintained 90% of their original mechanical properties after suffering three recycles. This strategy may promote the practical application of intelligent self-healing polyurethane coatings in the automobile and flexible electronic industry.

Conflicts of Interest

The authors declare no conflicts of interest.

Data Availability Statement

The data that support the findings of this study are available from the corresponding author upon reasonable request.

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