Others have reported materials that resemble the hierarchical structure and chemical composition of nacre using a β-chitin matrix 14 and layer-by-layer polyelectrolyte-clay dispersions 15. For example, several research groups have investigated ways to mineralize collagen intrafibrillarly, in order to mimic the natural mineralization process of bone tissue 13. Tissues such as bone and nacre have motivated the development of synthetic mineralizing materials 12. For example, negatively charged domains in non-collagenous 10 and non-amelogenin 7 proteins are known to stabilize crystal nucleation, whereas the degree of collagen cross-linking in bone is known to affect its mineral density, microarchitecture, and stiffness 11. The charge 6, conformation 7, supramolecular assembly 8, and posttranslational cross-linking 9 of specific macromolecules of the organic matrix have key multifunctional roles during the biomineralization process. This process is based on a highly dynamic environment regulated by an organic matrix that nucleates and directs the hierarchical growth and morphogenesis of mineralized tissue 5. In particular, the field of biomaterials would greatly benefit from the functionalities that can emerge from well-defined hierarchical organizations 4.īiomineralization, the process by which minerals are formed by living organisms under strict biological control, is responsible for the well-defined structure and subsequent function of mineralized tissues 5. The capacity to create synthetic materials that emulate such ingenious architectures represents a major goal in materials science and an opportunity to tune and profoundly improve functionality 3. Materials such as nacre, bone, and dental enamel possess distinct structural organization at different length scales, which enhance their bulk material properties and functionality 2. Nature is rich with examples of sophisticated materials displaying outstanding properties that emerge from their specific hierarchical structure 1. Our study represents a potential strategy for complex materials design that may open opportunities for hard tissue repair and provide insights into the role of molecular disorder in human physiology and pathology. The structures can be grown over large uneven surfaces and native tissues as acid-resistant membranes or coatings with tuneable hierarchy, stiffness, and hardness. The materials comprise elongated apatite nanocrystals that are aligned and organized into microscopic prisms, which grow together into spherulite-like structures hundreds of micrometers in diameter that come together to fill macroscopic areas. Here we report a protein-mediated mineralization process that takes advantage of disorder–order interplay using elastin-like recombinamers to program organic–inorganic interactions into hierarchically ordered mineralized structures. A major goal in materials science is to develop bioinspired functional materials based on the precise control of molecular building blocks across length scales.
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