Ion‐Specific Interactions Engender Dynamic and Tailorable Properties in Biomimetic Cationic Polyelectrolytes

Aubrecht, Filip J.; Orme, Kennalee; Saul, Aiden; Cai, Hongyi; Ranathunge, Tharindu A.; Silberstein, Meredith N.; McDonald, Benjamin R.

doi:10.1002/ange.202408673

Title: Ion‐Specific Interactions Engender Dynamic and Tailorable Properties in Biomimetic Cationic Polyelectrolytes

Journal Article · 04 September 2024 · Angewandte Chemie

DOI: https://doi.org/10.1002/ange.202408673 · OSTI ID:2530470

Aubrecht, Filip J. ^[1]; Orme, Kennalee ^[1]; Saul, Aiden ^[1]; Cai, Hongyi ^[2]; Ranathunge, Tharindu A. ^[1]; Silberstein, Meredith N. ^[3];

^[1]

Department of Chemistry Brown University 324 Brook Street Providence RI-02912 USA
Materials Science and Engineering Cornell University Ithaca New York 14853 USA
Sibley School of Mechanical and Aerospace Engineering Cornell University Ithaca New York 14853 USA

Abstract Biomaterials such as spider silk and mussel byssi are fabricated by the dynamic manipulation of intra‐ and intermolecular biopolymer interactions. Organisms modulate solution parameters, such as pH and ion co‐solute concentration, to effect these processes. These biofabrication schemes provide a conceptual framework to develop new dynamic and responsive abiotic soft material systems. Towards these ends, the chemical diversity of readily available ionic compounds offers a broad palette to manipulate the physicochemical properties of polyelectrolytes via ion‐specific interactions. In this study, we show for the first time that the ion‐specific interactions of biomimetic polyelectrolytes engenders a variety of phase separation behaviors, creating dynamic thermal‐ and ion‐responsive soft matter that exhibits a spectrum of physical properties, spanning viscous fluids to viscoelastic and viscoplastic solids. These ion‐dependent characteristics are further rendered general by the merger of lysine and phenylalanine into a single, amphiphilic vinyl monomer. The unprecedented breadth, precision, and dynamicity in the reported ion‐dependent phase behaviors thus introduce a broad array of opportunities for the future development of responsive soft matter; properties that are poised to drive developments in critical areas such as chemical sensing, soft robotics, and additive manufacturing.

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Sponsoring Organization:: USDOE

Grant/Contract Number:: SC0019141

OSTI ID:: 2530470

Journal Information:: Angewandte Chemie, Journal Name: Angewandte Chemie Journal Issue: 41 Vol. 136; ISSN 0044-8249

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

Country of Publication:: Germany

Language:: English

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