Nano- and Mesoscale Structures of Amorphous Calcium Carbonate Indicate Nanoscale Assembly Processes
2021
Here, we approach the issue
of ACC ultrastructure by applying a method for determining atomically resolved structures of
amorphous materials using Monte Carlo simulations constrained by both X-ray and
neutron scattering data. This structural analysis approach allows us to develop
a detailed model for ACC at the atomic level. Our findings reveal that synthetic
ACC, rapidly precipitated at high pH, consists of two-nanometer sized units
containing a high degree of near range order similar to partially disordered
nano-crystals. Small-angle scattering analyses show a multi-scale hierarchical
organisation of the structure, supportive of a multi-step colloid self-assembly
process. Computer simulations and high-resolution transmission electron
microscopy show that the mesostructure of ACC resembles that of a glassy gel
with crystalline material in domains. Our findings support the formation of ACC
by a nanoparticle aggregation process that likely starts from prenucleation
clusters in solution.
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