A Self‐Healing System for Polydicyclopentadiene Thermosets

Lee, Young Bum; Suslick, Benjamin A.; de Jong, Derek; Wilson, Gerald O.; Moore, Jeffrey S.; Sottos, Nancy R.; Braun, Paul V.

doi:10.1002/adma.202309662

A Self‐Healing System for Polydicyclopentadiene Thermosets

Journal Article · Tue Dec 19 23:00:00 EST 2023 · Advanced Materials

DOI:https://doi.org/10.1002/adma.202309662· OSTI ID:2246973

Lee, Young Bum ^[1]; Suslick, Benjamin A. ^[2]; de Jong, Derek ^[3]; Wilson, Gerald O. ^[4]; Moore, Jeffrey S. ^[5]; Sottos, Nancy R. ^[1]; ^[5]

Beckman Institute for Advanced Science and Technology University of Illinois Urbana–Champaign Urbana IL 61801 USA, Material Research Laboratory University of Illinois Urbana–Champaign Urbana IL 61801 USA, Department of Materials Science and Engineering University of Illinois Urbana–Champaign Urbana IL 61801 USA
Beckman Institute for Advanced Science and Technology University of Illinois Urbana–Champaign Urbana IL 61801 USA, Department of Chemistry University of Illinois Urbana–Champaign Urbana IL 61801 USA
Beckman Institute for Advanced Science and Technology University of Illinois Urbana–Champaign Urbana IL 61801 USA, Department of Materials Science and Engineering University of Illinois Urbana–Champaign Urbana IL 61801 USA
Autonomic Materials Incorporated Champaign IL 61822 USA
Beckman Institute for Advanced Science and Technology University of Illinois Urbana–Champaign Urbana IL 61801 USA, Material Research Laboratory University of Illinois Urbana–Champaign Urbana IL 61801 USA, Department of Materials Science and Engineering University of Illinois Urbana–Champaign Urbana IL 61801 USA, Department of Chemistry University of Illinois Urbana–Champaign Urbana IL 61801 USA

Abstract

Self‐healing offers promise for addressing structural failures, increasing lifespan, and improving durability in polymeric materials. Implementing self‐healing in thermoset polymers faces significant manufacturing challenges, especially due to the elevated temperature requirements of thermoset processing. To introduce self‐healing into structural thermosets, the self‐healing system must be thermally stable and compatible with the thermoset chemistry. This article demonstrates a self‐healing microcapsule‐based system stable to frontal polymerization (FP), a rapid and energy‐efficient manufacturing process with a self‐propagating exothermic reaction (≈200 °C). A thermally latent Grubbs‐type complex bearing two N ‐heterocyclic carbene ligands addresses limitations in conventional G2‐based self‐healing approaches. Under FP's elevated temperatures, the catalyst remains dormant until activated by a Cu(I) co‐reagent, ensuring efficient polymerization of the dicyclopentadiene (DCPD) upon damage to the polyDCPD matrix. The two‐part microcapsule system consists of one capsule containing the thermally latent Grubbs‐type catalyst dissolved in the solvent, and another capsule containing a Cu(I) coagent blended with liquid DCPD monomer. Using the same chemistry for both matrix fabrication and healing results in strong interfaces as demonstrated by lap‐shear tests. In an optimized system, the self‐healing system restores the mechanical properties of the tough polyDCPD thermoset. Self‐healing efficiencies greater than 90% via tapered double cantilever beam tests are observed.

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Sponsoring Organization:: USDOE

Grant/Contract Number:: NONE; AR0001330

OSTI ID:: 2246973

Alternate ID(s):: OSTI ID: 2246974
OSTI ID: 2575765

Journal Information:: Advanced Materials, Journal Name: Advanced Materials Journal Issue: 11 Vol. 36; ISSN 0935-9648

Publisher:: Wiley Blackwell (John Wiley & Sons)Copyright Statement

Country of Publication:: Germany

Language:: English

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