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Materials nanoarchitecturing via cation-mediated protein assembly : making limpet teeth without mineral

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Ukmar-Godec,  Tina
Damien Faivre, 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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Dunlop,  John W. C.
John Dunlop, Biomaterialien, Max Planck Institute of Colloids and Interfaces, Max Planck Society;

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Grabiger,  Michal A.
Damien Faivre, Biomaterialien, Max Planck Institute of Colloids and Interfaces, Max Planck Society;

Nguyen,  Huynh
John Dunlop, Biomaterialien, Max Planck Institute of Colloids and Interfaces, Max Planck Society;

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Faivre,  Damien
Damien Faivre, Biomaterialien, Max Planck Institute of Colloids and Interfaces, Max Planck Society;

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Citation

Ukmar-Godec, T., Bertinetti, L., Dunlop, J. W. C., Godec, A., Grabiger, M. A., Masic, A., et al. (2017). Materials nanoarchitecturing via cation-mediated protein assembly: making limpet teeth without mineral. Advanced Materials, 29(27): 1701171. doi:10.1002/adma.201701171.


Cite as: http://hdl.handle.net/11858/00-001M-0000-002D-4798-8
Abstract
Teeth are designed to deliver high forces while withstanding the generated stresses. Aside from isolated mineral-free exception (e.g., marine polychaetes and squids), minerals are thought to be indispensable for tooth-hardening and durability. Here, the unmineralized teeth of the giant keyhole limpet (Megathura crenulata) are shown to attain a stiffness, which is twofold higher than any known organic biogenic structures. In these teeth, protein and chitin fibers establish a stiff compact outer shell enclosing a less compact core. The stiffness and its gradients emerge from a concerted interaction across multiple length-scales: packing of hydrophobic proteins and folding into secondary structures mediated by Ca2+ and Mg2+ together with a strong spatial control in the local fiber orientation. These results integrating nanoindentation, acoustic microscopy, and finite-element modeling for probing the tooth's mechanical properties, spatially resolved small- and wide-angle X-ray scattering for probing the material ordering on the micrometer scale, and energy-dispersive X-ray scattering combined with confocal Raman microscopy to study structural features on the molecular scale, reveal a nanocomposite structure hierarchically assembled to form a versatile damage-tolerant protein-based tooth, with a stiffness similar to mineralized mammalian bone, but without any mineral.