Vaterite is a crystalline polymorph of calcium carbonate that exhibits low stability in comparison with the other crystalline polymorphs of calcium carbonate. It often assumes a spherical shape. The physical properties of vaterite are utilized in advanced biomaterials such as drug delivery systems (DDSs). The potential application of vaterite in DDSs demands a comprehensive understanding of its dissolution rate as a function of PO
4 concentration. Using in situ optical studies, we analyzed the dissolution behavior of vaterite in a simulated PO
4-containing biogenic environment. The varying physicality (i.e., the pseudo-physiological conditions) of vaterite were investigated using high-resolution cryogenic transmission electron microscopy and small-angle X-ray scattering. In addition, we measured the PO
4/Ca ratio in each part of vaterite spherulites using field-emission scanning electron microscopy in conjunction with energy-dispersive X-ray spectroscopy and inductively coupled plasma atomic emission spectrometry.
We categorized the vaterite spherulites into three parts—the shell, mantle, and core parts—on the basis of their dissolution behavior and PO
4 response. The PO
4 response to the dissolution dynamics increases toward the outer part, although the adsorption rate decreases in the presence of PO
4 and PO
4 fluorescence materials. The composition of the shell part was nearly identical to that of ideal vaterite, whereas the inner part exhibited a high C/Ca ratio and a poorly crystalline phase referred to as vaterite-like material. The dissolution rate of each part was 0.23–1.58 nm/s (shell), 0.63–3.19 nm/s (mantle), and 1.38–5.71 nm/s (core). The vaterite and vaterite-like materials were further identified according to their composition and particle size distribution.
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