Ion-Specific Interactions Engender Dynamic and Tailorable Properties in Biomimetic Cationic Polyelectrolytes
Filip J. Aubrecht
Department of Chemistry, Brown University, 324 Brook Street, Providence, RI-02912 USA
Contribution: Data curation (lead), Investigation (lead), Methodology (lead), Writing - original draft (supporting), Writing - review & editing (supporting)
Search for more papers by this authorKennalee Orme
Department of Chemistry, Brown University, 324 Brook Street, Providence, RI-02912 USA
Indicates that these authors contributed equally.
Contribution: Investigation (supporting), Writing - original draft (supporting), Writing - review & editing (supporting)
Search for more papers by this authorAiden Saul
Department of Chemistry, Brown University, 324 Brook Street, Providence, RI-02912 USA
Indicates that these authors contributed equally.
Contribution: Data curation (supporting), Methodology (supporting)
Search for more papers by this authorHongyi Cai
Materials Science and Engineering, Cornell University, Ithaca, New York, 14853 USA
Contribution: Formal analysis (supporting), Methodology (supporting), Writing - review & editing (supporting)
Search for more papers by this authorDr. Tharindu A. Ranathunge
Department of Chemistry, Brown University, 324 Brook Street, Providence, RI-02912 USA
Contribution: Investigation (supporting), Writing - review & editing (supporting)
Search for more papers by this authorProf. Meredith N. Silberstein
Sibley School of Mechanical and Aerospace Engineering, Cornell University, Ithaca, New York, 14853 USA
Contribution: Methodology (supporting), Writing - review & editing (supporting)
Search for more papers by this authorCorresponding Author
Prof. Benjamin R. McDonald
Department of Chemistry, Brown University, 324 Brook Street, Providence, RI-02912 USA
Contribution: Conceptualization (lead), Formal analysis (lead), Supervision (lead), Writing - original draft (lead), Writing - review & editing (lead)
Search for more papers by this authorFilip J. Aubrecht
Department of Chemistry, Brown University, 324 Brook Street, Providence, RI-02912 USA
Contribution: Data curation (lead), Investigation (lead), Methodology (lead), Writing - original draft (supporting), Writing - review & editing (supporting)
Search for more papers by this authorKennalee Orme
Department of Chemistry, Brown University, 324 Brook Street, Providence, RI-02912 USA
Indicates that these authors contributed equally.
Contribution: Investigation (supporting), Writing - original draft (supporting), Writing - review & editing (supporting)
Search for more papers by this authorAiden Saul
Department of Chemistry, Brown University, 324 Brook Street, Providence, RI-02912 USA
Indicates that these authors contributed equally.
Contribution: Data curation (supporting), Methodology (supporting)
Search for more papers by this authorHongyi Cai
Materials Science and Engineering, Cornell University, Ithaca, New York, 14853 USA
Contribution: Formal analysis (supporting), Methodology (supporting), Writing - review & editing (supporting)
Search for more papers by this authorDr. Tharindu A. Ranathunge
Department of Chemistry, Brown University, 324 Brook Street, Providence, RI-02912 USA
Contribution: Investigation (supporting), Writing - review & editing (supporting)
Search for more papers by this authorProf. Meredith N. Silberstein
Sibley School of Mechanical and Aerospace Engineering, Cornell University, Ithaca, New York, 14853 USA
Contribution: Methodology (supporting), Writing - review & editing (supporting)
Search for more papers by this authorCorresponding Author
Prof. Benjamin R. McDonald
Department of Chemistry, Brown University, 324 Brook Street, Providence, RI-02912 USA
Contribution: Conceptualization (lead), Formal analysis (lead), Supervision (lead), Writing - original draft (lead), Writing - review & editing (lead)
Search for more papers by this authorAbstract
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.
Conflict of Interests
The authors declare no conflict of interest.
Open Research
Data Availability Statement
The data that support the findings of this study are available in the supplementary material of this article.
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