Efficient Wet Adhesion through Mussel-Inspired Proto-Coacervates

Tan Phat Huynh; Yaqing Chen; Fiona L. Bach-Gansmo; Jeppe Dehli; Vicki N. Ibsen; Morten Foss; Anne S. Tvilum; Alexander N. Zelikin; Henrik Birkedal

doi:10.1002/admi.202201491

Efficient Wet Adhesion through Mussel-Inspired Proto-Coacervates

Tan Phat Huynh^*, Yaqing Chen, Fiona L. Bach-Gansmo, Jeppe Dehli, Vicki N. Ibsen, Morten Foss, Anne S. Tvilum, Alexander N. Zelikin, Henrik Birkedal

^*Corresponding author for this work

Research output: Contribution to journal/Conference contribution in journal/Contribution to newspaper › Journal article › Research › peer-review

6 Citations (Scopus)

Abstract

Adhesion underwater is a major challenge. Mussel-inspired complex coacervates functionalized with L-3,4-dihydroxyphenylalanine (L-DOPA) are proposed for underwater adhesives through versatile chemistry of DOPA, however, simple, efficient, controllable, and nontoxic procedures to harness them are still under investigation. In this study, inspired from the mussel byssus formation process, coacervate adhesives are formed underwater by simple injection of an acidic proto-coacervate of DOPA functionalized polyelectrolytes on underwater surfaces. The proto-coacervate is initially an acidic liquid, it increased in pH due to water diffusion, resulting in coacervation driven by electrostatic interaction, without the requirement for pH adjustment or organic solvents. Additionally, the pH of liquid–liquid phase separation is tuned by substituting polyelectrolytes with different pK_a, which satisfied different pH requirement in real life. The coacervate-based adhesives on glass substrates exhibit strengths comparable to commercial glues when dry and to mussel glue when wet, showing high biocompatibility in human epidermis in vitro.

Original language	English
Article number	2201491
Journal	Advanced Materials Interfaces
Volume	10
Issue	1
Number of pages	12
ISSN	2196-7350
DOIs	https://doi.org/10.1002/admi.202201491
Publication status	Published - Jan 2023

Keywords

adhesion
coacervates
DOPA
mussel-inspired adhesives
phase separation

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10.1002/admi.202201491Licence: CC BY

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title = "Efficient Wet Adhesion through Mussel-Inspired Proto-Coacervates",

abstract = "Adhesion underwater is a major challenge. Mussel-inspired complex coacervates functionalized with L-3,4-dihydroxyphenylalanine (L-DOPA) are proposed for underwater adhesives through versatile chemistry of DOPA, however, simple, efficient, controllable, and nontoxic procedures to harness them are still under investigation. In this study, inspired from the mussel byssus formation process, coacervate adhesives are formed underwater by simple injection of an acidic proto-coacervate of DOPA functionalized polyelectrolytes on underwater surfaces. The proto-coacervate is initially an acidic liquid, it increased in pH due to water diffusion, resulting in coacervation driven by electrostatic interaction, without the requirement for pH adjustment or organic solvents. Additionally, the pH of liquid–liquid phase separation is tuned by substituting polyelectrolytes with different pKa, which satisfied different pH requirement in real life. The coacervate-based adhesives on glass substrates exhibit strengths comparable to commercial glues when dry and to mussel glue when wet, showing high biocompatibility in human epidermis in vitro.",

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author = "Huynh, {Tan Phat} and Yaqing Chen and Bach-Gansmo, {Fiona L.} and Jeppe Dehli and Ibsen, {Vicki N.} and Morten Foss and Tvilum, {Anne S.} and Zelikin, {Alexander N.} and Henrik Birkedal",

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AU - Dehli, Jeppe

AU - Ibsen, Vicki N.

AU - Foss, Morten

AU - Tvilum, Anne S.

AU - Zelikin, Alexander N.

AU - Birkedal, Henrik

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N2 - Adhesion underwater is a major challenge. Mussel-inspired complex coacervates functionalized with L-3,4-dihydroxyphenylalanine (L-DOPA) are proposed for underwater adhesives through versatile chemistry of DOPA, however, simple, efficient, controllable, and nontoxic procedures to harness them are still under investigation. In this study, inspired from the mussel byssus formation process, coacervate adhesives are formed underwater by simple injection of an acidic proto-coacervate of DOPA functionalized polyelectrolytes on underwater surfaces. The proto-coacervate is initially an acidic liquid, it increased in pH due to water diffusion, resulting in coacervation driven by electrostatic interaction, without the requirement for pH adjustment or organic solvents. Additionally, the pH of liquid–liquid phase separation is tuned by substituting polyelectrolytes with different pKa, which satisfied different pH requirement in real life. The coacervate-based adhesives on glass substrates exhibit strengths comparable to commercial glues when dry and to mussel glue when wet, showing high biocompatibility in human epidermis in vitro.

AB - Adhesion underwater is a major challenge. Mussel-inspired complex coacervates functionalized with L-3,4-dihydroxyphenylalanine (L-DOPA) are proposed for underwater adhesives through versatile chemistry of DOPA, however, simple, efficient, controllable, and nontoxic procedures to harness them are still under investigation. In this study, inspired from the mussel byssus formation process, coacervate adhesives are formed underwater by simple injection of an acidic proto-coacervate of DOPA functionalized polyelectrolytes on underwater surfaces. The proto-coacervate is initially an acidic liquid, it increased in pH due to water diffusion, resulting in coacervation driven by electrostatic interaction, without the requirement for pH adjustment or organic solvents. Additionally, the pH of liquid–liquid phase separation is tuned by substituting polyelectrolytes with different pKa, which satisfied different pH requirement in real life. The coacervate-based adhesives on glass substrates exhibit strengths comparable to commercial glues when dry and to mussel glue when wet, showing high biocompatibility in human epidermis in vitro.

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Efficient Wet Adhesion through Mussel-Inspired Proto-Coacervates

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