Molecular dynamics interpretation of hydrogen bonds for colorless, water-resistant, tough, and self-healable elastomers

Seon Mi Kim, Minkyung Lee, Sanggil Park, Seul A. Park, Hyeonyeol Jeon, Jun Mo Koo, Sung Bae Park, Hyo Jeong Kim, Youngho Eom, Eun Seong Lee, Hyungjun Kim, Dongyeop X. Oh, Jeyoung Park

Research output: Contribution to journalArticlepeer-review

16 Scopus citations

Abstract

Transparent, self-healing elastomers play a vital role as protective coatings, particularly in display applications. However, mechanical toughness and efficient self-restoration are often mutually exclusive. A performance equilibrium can be achieved through the molecular design of reversible bonds. However, aromatic disulfide-based dynamic covalent bonds produce an unattractive coloration owing to electron chromophores. In addition, H-bond moieties induce unintended adhesion to the substrates and are limited by hydration-induced weakening. In this study, the molecular design of aliphatic disulfides is presented for colorless, non-tacky, and water-resistant elastomers that rapidly self-heal at ambient temperatures. By employing molecular dynamics simulations, we demonstrate that an excess of H-bond acceptors promotes shorter bond exchange durations while maintaining a higher quantity of cohesive H-bonds, surpassing the performance of equivalent donor/acceptor systems at identical donor concentrations. In addition, dynamic H-bond exchange enables effective healing, whereas the increased H-bond cross-linking density ensures both waterproofness and an impressive tensile strength of 45 MPa. Furthermore, the absence of aromatic groups grants the elastomers a remarkable transmittance of 99%. The optimized properties achieved in this study using the proposed strategic molecular designs will further the commercialization of self-healing thermoplastic polyurethanes as intelligent protective coatings.

Original languageEnglish
Pages (from-to)22737-22748
Number of pages12
JournalJournal of Materials Chemistry A
Volume11
Issue number42
DOIs
StatePublished - 27 Sep 2023

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Publisher Copyright:
© 2023 The Royal Society of Chemistry.

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