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

Franziska Jehle, Elena Macías-Sánchez, Sanja Sviben, Peter Fratzl, Luca Bertinetti () and Matthew J. Harrington ()
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Franziska Jehle: Max Planck Institute of Colloids and Interfaces
Elena Macías-Sánchez: Max Planck Institute of Colloids and Interfaces
Sanja Sviben: Max Planck Institute of Colloids and Interfaces
Peter Fratzl: Max Planck Institute of Colloids and Interfaces
Luca Bertinetti: Max Planck Institute of Colloids and Interfaces
Matthew J. Harrington: Max Planck Institute of Colloids and Interfaces

Nature Communications, 2020, vol. 11, issue 1, 1-9

Abstract: 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.

Date: 2020
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DOI: 10.1038/s41467-020-14709-y

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