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

MPS-Authors
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Jehle,  Franziska
Damien Faivre, Biomaterialien, Max Planck Institute of Colloids and Interfaces, Max Planck Society;

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Macías-Sánchez,  Elena
Luca Bertinetti (Indep. Res.), Biomaterialien, Max Planck Institute of Colloids and Interfaces, Max Planck Society;

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Sviben,  Sanja
Yael Politi, Biomaterialien, Max Planck Institute of Colloids and Interfaces, Max Planck Society;

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Fratzl,  Peter
Peter Fratzl, Biomaterialien, Max Planck Institute of Colloids and Interfaces, Max Planck Society;

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Bertinetti,  Luca
Luca Bertinetti (Indep. Res.), Biomaterialien, Max Planck Institute of Colloids and Interfaces, Max Planck Society;

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Harrington,  Matthew J.
Matthew Harrington, Biomaterialien, Max Planck Institute of Colloids and Interfaces, Max Planck Society;

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Citation

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.


Cite as: http://hdl.handle.net/21.11116/0000-0005-A730-8
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.