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Cited by 517Polymer Surface Interaction StudiesMarine Biology and Environmental ChemistryCalcium Carbonate Crystallization and Inhibition

Strong reversible Fe 3+ -mediated bridging between dopa-containing protein films in water

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Zeng, Hongbo, Hwang, Dong Soo, Israelachvili, Jacob N., Waite, J. Herbert·2010·Proceedings of the National Academy of Sciences
DOI 10.1073/pnas.1007416107PMC PMC2919964
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Abstract

Metal-containing polymer networks are widespread in biology, particularly for load-bearing exoskeletal biomaterials. Mytilus byssal cuticle is an especially interesting case containing moderate levels of Fe 3+ and cuticle protein—mussel foot protein-1 (mfp-1), which has a peculiar combination of high hardness and high extensibility. Mfp-1, containing 13 mol % of dopa (3, 4-dihydroxyphenylalanine) side-chains, is highly positively charged polyelectrolyte (pI ∼ 10) and didn’t show any cohesive tendencies in previous surface forces apparatus (SFA) studies. Here, we show that Fe 3+ ions can mediate unusually strong interactions between the positively charged proteins. Using an SFA, Fe 3+ was observed to impart robust bridging ( W ad ≈ 4.3 mJ/m 2 ) between two noninteracting mfp-1 films in aqueous buffer approaching the ionic strength of seawater. The Fe 3+ bridging between the mfp-1-coated surfaces is fully reversible in water, increasing with contact time and iron concentration up to 10 μM; at 100 μM, Fe 3+ bridging adhesion is abolished. Bridging is apparently due to the formation of multivalent dopa-iron complexes. Similar Fe-mediated bridging ( W ad ≈ 5.7 mJ/m 2 ) by a smaller recombinant dopa-containing analogue indicates that bridging is largely independent of molecular weight and posttranslational modifications other than dopa. The results suggest that dopa-metal interactions may provide an energetic new paradigm for engineering strong, self-healing interactions between polymers under water.

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  • When the ratio of catechol to Fe3+ is high (the amount of Fe3+ is low), catechol and Fe3+ are prone to forming more tri-complexes.

    “When the ratio of catechol to Fe3+ is high (the amount of Fe3+ is low), catechol and Fe3+ are prone to forming more tri-complexes [63,64].”

    From Mussel-Inspired Injectable Adhesive Hydrogels for Biomedical Applications (2024) · cites this paper as [63]

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Cited by

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Authors
Zeng, H., Hwang, D. S., Israelachvili, J. N., & Waite, J. H.
Affiliations
  • University of Alberta (CA)
  • Materials Research Laboratory, and
  • Department of Chemical Engineering,
  • University of California, Santa Barbara (US)
ORCID
Venue
Proceedings of the National Academy of Sciences
Publisher
National Academy of Sciences
Published
2010-07-06
Volume
107
Issue
29
Pages
12850-12853
ISSN
  • 0027-8424 (ISSN-L)
  • 1091-6490
DOI
10.1073/pnas.1007416107
PMC
PMC2919964
OpenAlex
W2024486172
Cited by
517
References
1
Citations by year
2026: 18 · 2025: 30 · 2024: 25 · 2023: 31 · 2022: 36 · 2021: 55 · 2020: 39 · 2019: 43 · 2018: 40 · 2017: 27 · 2016: 35 · 2015: 34 · 2014: 34 · 2013: 21 · 2012: 30
FWCI
11.31
Type
journal article
Language
en
Open access
Locations
  • Proceedings of the National Academy of Sciences (publishedVersion)
  • PubMed Central (publishedVersion)
  • PubMed (publishedVersion)
  • Open Access System for Information Sharing (Pohang University of Science and Technology) (submittedVersion, cc-by-nc-nd)
Funders
  • National Science Foundation (DMR05- 20415)
  • National Institutes of Health
  • National Institute of Dental and Craniofacial Research (R01DE018468, R01DE015415)
  • Division of Materials Research (DMR-0520415)
Topics
  • Physical Sciences › Materials Science › Surfaces, Coatings and Films › Polymer Surface Interaction Studies
  • Physical Sciences › Engineering › Ocean Engineering › Marine Biology and Environmental Chemistry
  • Physical Sciences › Materials Science › Biomaterials › Calcium Carbonate Crystallization and Inhibition
Keywords
DOPA, polyelectrolyte films, reversible adhesion, biomimetic biomaterials, surface force apparatus
MeSH terms
Adhesiveness, Aluminum Silicates, Animals, Biomechanical Phenomena, Dihydroxyphenylalanine, Iron, Proteins, Recombinant Proteins, Water, Microscopy, Atomic Force, Mytilus

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