Abstract
The study of nucleation and growth from supersaturated ion solutions is a key area of interest in biomineralization research and beyond with high-resolution in situ imaging techniques such as liquid cell transmission electron microscopy (LCTEM) attracting substantial attention. However, there is increasing experimental evidence that experiments performed with this technique differ from those performed in bulk solutions due to the spatial restriction, which is a prerequisite for LCTEM to provide electron transparent samples. We have performed 2D Finite Elements (FE) simulations to study the impact of confinement on the steady state concentration profiles around a nanoparticle in a supersaturated solution of the constituent ions. We find that confinement below a critical value significantly reduces the concentration of available ions in solutions and hence the stability of the precipitates. These findings could explain the necessity to substantially increase ion activities of Ca2+ and CO32− to induce precipitation in LCTEM.
Highlights
Precipitation in confinement is a phenomenon of significant interest in a number of areas such as geology [1], environmental research [2] as well as biomineralization and biomorphism [3,4]
It has been studied with a variety of techniques such as electron microscopy and X-ray spectroscopy to reveal the details of the transformation process from ion solutions to solid, often crystalline, precipitates
The recent advent of liquid cell transmission electron microscopy techniques raises the prospect of investigating crystal growth in situ at the nanometer level [5,6] and the question of how the confinement, which is a prerequisite for the application of this technique, affects the dynamics of crystallization
Summary
Precipitation in confinement is a phenomenon of significant interest in a number of areas such as geology (e.g., the impact of salt crystallization in rocks) [1], environmental research (e.g., for the remediation of contaminants) [2] as well as biomineralization and biomorphism [3,4] It has been studied with a variety of techniques such as electron microscopy and X-ray spectroscopy to reveal the details of the transformation process from ion solutions to solid, often crystalline, precipitates. The application of LCTEM for the investigation of particle precipitation and dissolution dynamics in polar solvents such as water, where the precipitates are either of amorphous or crystalline nature and a key problem is the mechanism of ion transport and its impact on the stability of precipitates This is important when taking into account the spatial boundary conditions defining the problem, namely the confinement of the liquid by thin membranes to create an electron transparent sample.
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