Abstract
Bone is one of Nature's most remarkable materials, not only for its mechanical properties but also for its ability to repair fractures and remodel its microstructure in response to stress. At the nanoscale bone is a supramolecular matrix of collagen fibers reinforced by hydroxyapatite crystals with a high degree of order. Emulating elements of the biological synthesis of this composite could help develop strategies for advanced materials. Previous work has demonstrated the use of functionalized peptide amphiphile nanofibers in a two-dimensional system to emulate hydroxyapatite mineralization in natural bone. We describe here an artificial, in vitro biomineralization process that allows a similar process to occur in three dimensions. The system employs the natural enzyme alkaline phosphatase and a phosphorylated, anionic nanofiber gel matrix to template hydroxyapatite nanocrystals with size, shape, and crystallographic orientation resembling natural bone mineral. The formation of this biomimetic mineral in three dimensions results from the synergy of fiber-induced nucleation and the temporal control of phosphate ion harvesting by the enzyme. Gradual enzymatic harvesting of ions for crystal growth and the strong nucleating ability of the phosphorylated fibers suppresses uncontrolled precipitation of mineral. The strategy could lead to biomimetic materials to promote bone regeneration or the synthesis of hybrid materials with crystallographically defined structures.