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 › Article › Scientific › peer-review

8 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
Journal	Advanced Materials Interfaces
DOIs	https://doi.org/10.1002/admi.202201491
Publication status	Published - Oct 2022
Externally published	Yes
MoE publication type	A1 Journal article-refereed

Funding

T.‐P.H. and Y.C. contributed equally to this work. The authors thank Malene Laugesen for assistance with optical microscopy, Carsten Pedersen for assistance with technical issues, Kaja Borup Løvschall for assistance with polymerization technique queries, and Amanda Birkedal for the sketch of biological organisms in Figure 1A . This research was supported by the Danish Council for Independent Research Technology and Production Sciences (Grant No. 0602‐02426B) and the Carlsberg Foundation through a Carlsberg Foundation's Distinguished Postdoctoral Fellowship to TPH (Grant No. 21903) as well as the China Scholarship Council.

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.",

keywords = "adhesion, coacervates, DOPA, mussel-inspired adhesives, phase separation",

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",

note = "Funding Information: T.‐P.H. and Y.C. contributed equally to this work. The authors thank Malene Laugesen for assistance with optical microscopy, Carsten Pedersen for assistance with technical issues, Kaja Borup L{\o}vschall for assistance with polymerization technique queries, and Amanda Birkedal for the sketch of biological organisms in Figure 1A . This research was supported by the Danish Council for Independent Research Technology and Production Sciences (Grant No. 0602‐02426B) and the Carlsberg Foundation through a Carlsberg Foundation's Distinguished Postdoctoral Fellowship to TPH (Grant No. 21903) as well as the China Scholarship Council. Publisher Copyright: {\textcopyright} 2022 The Authors. Advanced Materials Interfaces published by Wiley-VCH GmbH.",

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AU - Huynh, Tan Phat

AU - Chen, Yaqing

AU - Bach-Gansmo, Fiona L.

AU - Dehli, Jeppe

AU - Ibsen, Vicki N.

AU - Foss, Morten

AU - Tvilum, Anne S.

AU - Zelikin, Alexander N.

AU - Birkedal, Henrik

N1 - Funding Information: T.‐P.H. and Y.C. contributed equally to this work. The authors thank Malene Laugesen for assistance with optical microscopy, Carsten Pedersen for assistance with technical issues, Kaja Borup Løvschall for assistance with polymerization technique queries, and Amanda Birkedal for the sketch of biological organisms in Figure 1A . This research was supported by the Danish Council for Independent Research Technology and Production Sciences (Grant No. 0602‐02426B) and the Carlsberg Foundation through a Carlsberg Foundation's Distinguished Postdoctoral Fellowship to TPH (Grant No. 21903) as well as the China Scholarship Council. Publisher Copyright: © 2022 The Authors. Advanced Materials Interfaces published by Wiley-VCH GmbH.

PY - 2022/10

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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.

KW - adhesion

KW - coacervates

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DO - 10.1002/admi.202201491

M3 - Article

AN - SCOPUS:85139614683

SN - 2196-7350

JO - Advanced Materials Interfaces

JF - Advanced Materials Interfaces

ER -

Efficient Wet Adhesion through Mussel-Inspired Proto-Coacervates

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Keywords

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