Highly ordered superstructures composed of inorganic nanoparticles appear in natural and synthetic systems, however the mechanisms of non-equilibrium self-organization that may be involved are still poorly understood. Herein, we performed a kinetic investigation of the precipitation of calcium phosphate using a process widely found in microorganisms: the hydrolysis of urea by enzyme urease. With high initial ratio of calcium ion to phosphate, periodic precipitation was obtained accompanied by pH oscillations in a well-stirred, closed reactor. We propose that an internal pH-regulated change in the concentration of phosphate ion is the driving force for periodicity. A simple model involving the biocatalytic reaction network coupled with burst nucleation of nanoparticles above a critical supersaturation reproduced key features of the experiments. These findings may provide insight to the self-organization of nanoparticles in biomineralization and improve design strategies of biomaterials for medical applications.
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http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7027757 | PMC |
http://dx.doi.org/10.1002/anie.201911213 | DOI Listing |
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