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

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.

SUBMITTER: Jehle F

PROVIDER: S-EPMC7018715 | biostudies-literature | 2020 Feb

REPOSITORIES: biostudies-literature

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

Jehle Franziska F Macías-Sánchez Elena E Sviben Sanja S Fratzl Peter P Bertinetti Luca L Harrington Matthew J MJ

Nature communications 20200213 1

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 ...[more]

PMID: 32054841

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Project description:The aerospace and automotive industries find that relying solely on the intrinsic resistance of alloys is inadequate to safeguard aircraft and automotive structural components from harsh environmental conditions. While it is difficult to attribute accidents exclusively to coating failure due to the involvement of multiple factors, there are instances where defects in the coating initiate a wear or degradation process, leading to premature and unplanned structural failures. Metallic coatings have been introduced to protect the aircraft mainly from wear due to the extreme temperatures and moisture exposure during their service life. Bare metallic coatings have a limited lifespan and need to be replaced frequently. Herein, the strength and wear resistance of zinc (Zn) coating is enhanced using varying concentrations of diamond particles as an additive in the Zn matrix (Zn-D). The dispersion strengthening mechanism is attributed to the high hardness (70 HRC), and reduced friction-of-coefficient (0.21) and dissipation energy (4.6 × 10-4 J) of electrodeposited Zn-D7.5 (7.5 g l-1 of diamond concentration) composite coating. Moreover, enhanced wear resistance with minimum wear volume (1.12 × 10-3 mm3) and wear rate (1.25 × 10-3 mm3 N-1 m-1) of the Zn-D7.5 composite coating resulted in perfect blending of diamond with Zn. The improved hardness and wear resistance for Zn-D7.5 (optimum 7.5 g l-1 diamond concentration) is due to the steadiness between well-dispersed diamonds in Zn and enrichment in load-bearing ability due to the incorporation of diamond particles. Electronic structure calculations on the zinc-diamond composite models (two configurations adopted) have been performed using the density functional theory (DFT) approach, and the in silico studies appeared to facilitate meaningful and evocative outcomes. Zn-doped diamond (C10@Zn) without hydrogen (H) atoms (binding energy: 418 kcal mol-1, i.e. showing an endothermic reaction and thermodynamically not favourable) was detected to be more stable than the Zn-doped diamond (C10H16@Zn) consisting of hydrogen (H) atoms (binding energy: -33.3 kcal mol-1, i.e. showing an exothermic reaction and thermodynamically preferable). Thus, a composite coating of zinc and diamond can be a suitable candidate for the aerospace and automotive industries.

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

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

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