Supramolecular β-sheet suckerin–based underwater adhesives

Nature has evolved several molecular strategies to ensure adhesion in aqueous environments, where artificial adhesives typically fail. One recently unveiled molecular design for wet-resistant adhesion is the cohesive cross-beta structure characteristic of amyloids, complementing the well-established...

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Main Authors: Deepankumar, Kanagavel, Lim, Chanoong, Polte, Ingmar, Zappone, Bruno, Labate, Cristina, De Santo, Maria P., Mohanram, Harini, Palaniappan, Alagappan, Hwang, Dong Soo, Miserez, Ali
Other Authors: School of Materials Science and Engineering
Format: Article
Language:English
Published: 2020
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Online Access:https://hdl.handle.net/10356/142969
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Institution: Nanyang Technological University
Language: English
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spelling sg-ntu-dr.10356-1429692023-07-14T16:00:15Z Supramolecular β-sheet suckerin–based underwater adhesives Deepankumar, Kanagavel Lim, Chanoong Polte, Ingmar Zappone, Bruno Labate, Cristina De Santo, Maria P. Mohanram, Harini Palaniappan, Alagappan Hwang, Dong Soo Miserez, Ali School of Materials Science and Engineering DRNTU::Engineering::Materials Dopa Residue Specific Incorporation Nature has evolved several molecular strategies to ensure adhesion in aqueous environments, where artificial adhesives typically fail. One recently unveiled molecular design for wet-resistant adhesion is the cohesive cross-beta structure characteristic of amyloids, complementing the well-established surface-binding strategy of mussel adhesive proteins based on 3,4-L-Dihydroxyphenylalanine (Dopa). A family of structural proteins that self-assemble into cross beta-sheet networks are the suckerins discovered in the sucker ring teeth of squids. Here, we shed light on the wet adhesion of cross-beta motifs by producing recombinant suckerin-12, naturally lacking Dopa, and investigating its wet adhesion properties. Surprisingly, the adhesion forces measured on mica are as high as ca. 70 mN m-1, exceeding those measured for all mussel adhesive proteins to date. The pressure-sensitive adhesion of artificial suckerins is largely governed by their cross-beta motif, as evidenced using control experiments with disrupted cross-beta domains that result in almost complete loss of adhesion. We also incorporate Dopa in suckerin-12 using a residue-specific incorporation strategy that replaces Tyrosine with Dopa during expression in Escherichia coli. Although the replacement does not increase the long-term adhesion, it contributes to the initial rapid contact and enhances the adsorption onto model oxide substrates. Our findings suggest that suckerins with supramolecular cross-beta motifs are promising biopolymers for wet-resistant adhesion NRF (Natl Research Foundation, S’pore) MOE (Min. of Education, S’pore) Accepted version 2020-07-16T05:03:41Z 2020-07-16T05:03:41Z 2020 Journal Article Deepankumar, K., Lim, C., Polte, I., Zappone, B., Labate, C., De Santo, M. P., ... Miserez, A. (2020). Supramolecular β‐sheet suckerin–based underwater adhesives. Advanced Functional Materials, 30(16), 1907534-. doi:10.1002/adfm.201907534 1616-301X https://hdl.handle.net/10356/142969 10.1002/adfm.201907534 16 30 en Advanced Functional Materials © 2020 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim. All rights reserved. This paper was published in Advanced Functional Materials and is made available with permission of WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim. application/pdf
institution Nanyang Technological University
building NTU Library
continent Asia
country Singapore
Singapore
content_provider NTU Library
collection DR-NTU
language English
topic DRNTU::Engineering::Materials
Dopa
Residue Specific Incorporation
spellingShingle DRNTU::Engineering::Materials
Dopa
Residue Specific Incorporation
Deepankumar, Kanagavel
Lim, Chanoong
Polte, Ingmar
Zappone, Bruno
Labate, Cristina
De Santo, Maria P.
Mohanram, Harini
Palaniappan, Alagappan
Hwang, Dong Soo
Miserez, Ali
Supramolecular β-sheet suckerin–based underwater adhesives
description Nature has evolved several molecular strategies to ensure adhesion in aqueous environments, where artificial adhesives typically fail. One recently unveiled molecular design for wet-resistant adhesion is the cohesive cross-beta structure characteristic of amyloids, complementing the well-established surface-binding strategy of mussel adhesive proteins based on 3,4-L-Dihydroxyphenylalanine (Dopa). A family of structural proteins that self-assemble into cross beta-sheet networks are the suckerins discovered in the sucker ring teeth of squids. Here, we shed light on the wet adhesion of cross-beta motifs by producing recombinant suckerin-12, naturally lacking Dopa, and investigating its wet adhesion properties. Surprisingly, the adhesion forces measured on mica are as high as ca. 70 mN m-1, exceeding those measured for all mussel adhesive proteins to date. The pressure-sensitive adhesion of artificial suckerins is largely governed by their cross-beta motif, as evidenced using control experiments with disrupted cross-beta domains that result in almost complete loss of adhesion. We also incorporate Dopa in suckerin-12 using a residue-specific incorporation strategy that replaces Tyrosine with Dopa during expression in Escherichia coli. Although the replacement does not increase the long-term adhesion, it contributes to the initial rapid contact and enhances the adsorption onto model oxide substrates. Our findings suggest that suckerins with supramolecular cross-beta motifs are promising biopolymers for wet-resistant adhesion
author2 School of Materials Science and Engineering
author_facet School of Materials Science and Engineering
Deepankumar, Kanagavel
Lim, Chanoong
Polte, Ingmar
Zappone, Bruno
Labate, Cristina
De Santo, Maria P.
Mohanram, Harini
Palaniappan, Alagappan
Hwang, Dong Soo
Miserez, Ali
format Article
author Deepankumar, Kanagavel
Lim, Chanoong
Polte, Ingmar
Zappone, Bruno
Labate, Cristina
De Santo, Maria P.
Mohanram, Harini
Palaniappan, Alagappan
Hwang, Dong Soo
Miserez, Ali
author_sort Deepankumar, Kanagavel
title Supramolecular β-sheet suckerin–based underwater adhesives
title_short Supramolecular β-sheet suckerin–based underwater adhesives
title_full Supramolecular β-sheet suckerin–based underwater adhesives
title_fullStr Supramolecular β-sheet suckerin–based underwater adhesives
title_full_unstemmed Supramolecular β-sheet suckerin–based underwater adhesives
title_sort supramolecular β-sheet suckerin–based underwater adhesives
publishDate 2020
url https://hdl.handle.net/10356/142969
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