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  Hierarchically-structured metalloprotein composite coatings biofabricated from co-existing condensed liquid phases

Jehle, F., Macías-Sánchez, E., Sviben, S., Fratzl, P., Bertinetti, L., & Harrington, M. J. (2020). Hierarchically-structured metalloprotein composite coatings biofabricated from co-existing condensed liquid phases. Nature Communications, 11: 862. doi:10.1038/s41467-020-14709-y.

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Jehle, Franziska1, Author           
Macías-Sánchez, Elena2, Author           
Sviben, Sanja3, Author           
Fratzl, Peter4, Author           
Bertinetti, Luca2, Author           
Harrington, Matthew J.5, Author           
Affiliations:
1Damien Faivre, Biomaterialien, Max Planck Institute of Colloids and Interfaces, Max Planck Society, ou_1863290              
2Luca Bertinetti (Indep. Res.), Biomaterialien, Max Planck Institute of Colloids and Interfaces, Max Planck Society, ou_2231637              
3Yael Politi, Biomaterialien, Max Planck Institute of Colloids and Interfaces, Max Planck Society, ou_1863297              
4Peter Fratzl, Biomaterialien, Max Planck Institute of Colloids and Interfaces, Max Planck Society, ou_1863294              
5Matthew Harrington, Biomaterialien, Max Planck Institute of Colloids and Interfaces, Max Planck Society, ou_1863292              

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 Abstract: Complex hierarchical structure governs emergent properties in biopolymeric materials; yet, the material processing involved remains poorly understood. Here, we investigated the multi-scale structure and composition of the mussel byssus cuticle before, during and after formation to gain insight into the processing of this hard, yet extensible metal cross-linked protein composite. Our findings reveal that the granular substructure crucial to the cuticle’s function as a wear-resistant coating of an extensible polymer fiber is pre-organized in condensed liquid phase secretory vesicles. These are phase-separated into DOPA-rich proto-granules enveloped in a sulfur-rich proto-matrix which fuses during secretion, forming the sub-structure of the cuticle. Metal ions are added subsequently in a site-specific way, with iron contained in the sulfur-rich matrix and vanadium coordinated by DOPA-catechol in the granule. We posit that this hierarchical structure self-organizes via phase separation of specific amphiphilic proteins within secretory vesicles, resulting in a meso-scale structuring that governs cuticle function.

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Language(s): eng - English
 Dates: 2020-02-132020
 Publication Status: Issued
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 Identifiers: DOI: 10.1038/s41467-020-14709-y
DOI: 10.1038/s41467-020-15462-y
PMID: 0584
Other: M:\BM-Publications\2020\JehleNatCom_Hierarchically
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Title: Nature Communications
  Abbreviation : Nat. Commun.
Source Genre: Journal
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Publ. Info: London : Nature Publishing Group
Pages: - Volume / Issue: 11 Sequence Number: 862 Start / End Page: - Identifier: ISSN: 2041-1723