Carbodiimide‐Driven Toughening of Interpenetrated Polymer Networks

Rajawasam, Chamoni W. H.; Tran, Corvo; Sparks, Jessica L.; Krueger, William H.; Hartley, C. Scott; Konkolewicz, Dominik

doi:10.1002/anie.202400843

Title: Carbodiimide‐Driven Toughening of Interpenetrated Polymer Networks

Journal Article · 10 April 2024 · Angewandte Chemie (International Edition)

DOI: https://doi.org/10.1002/anie.202400843 · OSTI ID:2336610

Rajawasam, Chamoni W. H. ^[1]; Tran, Corvo ^[1]; Sparks, Jessica L. ^[2]; Krueger, William H. ^[1];

^[1];

^[1]

Department of Chemistry and Biochemistry Miami University Oxford OH 45056 USA
Department of Chemical Paper and Biomedical Engineering Miami University Oxford OH 45056 USA

Abstract Recent work has demonstrated that temporary crosslinks in polymer networks generated by chemical “fuels” afford materials with large, transient changes in their mechanical properties. This can be accomplished in carboxylic‐acid‐functionalized polymer hydrogels using carbodiimides, which generate anhydride crosslinks with lifetimes on the order of minutes to hours. Here, the impact of the polymer network architecture on the mechanical properties of transiently crosslinked materials was explored. Single networks (SNs) were compared to interpenetrated networks (IPNs). Notably, semi‐IPN precursors that give IPNs on treatment with carbodiimide give much higher fracture energies (i.e., resistance to fracture) and superior resistance to compressive strain compared to other network architectures. A precursor semi‐IPN material featuring acrylic acid in only the free polymer chains yields, on treatment with carbodiimide, an IPN with a fracture energy of 2400 J/m ² , a fourfold increase compared to an analogous semi‐IPN precursor that yields a SN. This resistance to fracture enables the formation of macroscopic complex cut patterns, even at high strain, underscoring the pivotal role of polymer architecture in mechanical performance.

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Sponsoring Organization:: USDOE

Grant/Contract Number:: NONE; SC0018645

OSTI ID:: 2336610

Alternate ID(s):: OSTI ID: 2336611

Journal Information:: Angewandte Chemie (International Edition), Journal Name: Angewandte Chemie (International Edition) Journal Issue: 20 Vol. 63; ISSN 1433-7851

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

Country of Publication:: Germany

Language:: English

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