Non-equilibrium crystallization pathways of manganese oxides in aqueous solution

Wenhao Sun (), Daniil A. Kitchaev, Denis Kramer and Gerbrand Ceder ()
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Wenhao Sun: Lawrence Berkeley National Laboratory
Daniil A. Kitchaev: Massachusetts Institute of Technology
Denis Kramer: University of Southampton
Gerbrand Ceder: Lawrence Berkeley National Laboratory

Nature Communications, 2019, vol. 10, issue 1, 1-9

Abstract: Abstract Aqueous precipitation of transition metal oxides often proceeds through non-equilibrium phases, whose appearance cannot be anticipated from traditional phase diagrams. Without a precise understanding of which metastable phases form, or their lifetimes, targeted synthesis of specific metal oxides can become a trial-and-error process. Here, we construct a theoretical framework to reveal the nanoscale and metastable energy landscapes of Pourbaix (E-pH) diagrams, providing quantitative insights into the size–dependent thermodynamics of metastable oxide nucleation and growth in water. By combining this framework with classical nucleation theory, we interrogate how solution conditions influence the multistage oxidation pathways of manganese oxides. We calculate that even within the same stability region of a Pourbaix diagram, subtle variations in pH and redox potential can redirect a non-equilibrium crystallization pathway through different metastable intermediates. Our theoretical framework offers a predictive platform to navigate through the thermodynamic and kinetic energy landscape towards the rational synthesis of target materials.

Date: 2019
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DOI: 10.1038/s41467-019-08494-6

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