Simulation of calcium phosphate prenucleation clusters in aqueous solution: association beyond Ion pairing

Natalya A. Garcia, Riccardo Innocenti Malini, Colin L. Freeman, Raffaella Demichelis, Paolo Raiteri (Corresponding author), Nico A.J.M. Sommerdijk, John H. Harding, Julian D. Gale

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Abstract

Classical molecular dynamics simulations and free energy methods have been used to obtain a better understanding of the molecular processes occurring prior to the first nucleation event for calcium phosphate biominerals. The association constants for the formation of negatively charged complexes containing calcium and phosphate ions in aqueous solution have been computed, and these results suggest that the previously proposed calcium phosphate building unit, [Ca(HPO4)3]4-, should only be present in small amounts under normal experimental conditions. However, the presence of an activation barrier for the removal of an HPO4 2- ion from this complex indicates that this species could be kinetically trapped. Aggregation pathways involving CaHPO4, [Ca(HPO4)2]2-, and [Ca(HPO4)3]4- complexes have been explored with the finding that dimerization is favorable up to a Ca/HPO4 ratio of 1:2.

Original languageEnglish
Pages (from-to)6422-6430
Number of pages9
JournalCrystal Growth and Design
Volume19
Issue number11
DOIs
Publication statusPublished - Nov 2019

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    Garcia, N. A., Malini, R. I., Freeman, C. L., Demichelis, R., Raiteri, P., Sommerdijk, N. A. J. M., Harding, J. H., & Gale, J. D. (2019). Simulation of calcium phosphate prenucleation clusters in aqueous solution: association beyond Ion pairing. Crystal Growth and Design, 19(11), 6422-6430. https://doi.org/10.1021/acs.cgd.9b00889