Title: Non-equilibrium crystallization pathways of manganese oxides in aqueous solution
Authors: Sun, Wenhao
Kitchaev, Daniil A.
Kramer, Denis 
Ceder, Gerbrand
Language: en
Subject (DDC): DDC::500 Naturwissenschaften und Mathematik::540 Chemie::541 Physikalische Chemie
Issue Date: 2019
Publisher: Nature Publishing Group
Document Type: Article
Journal / Series / Working Paper (HSU): Nature Communications 
Volume: 10
Page Start: 1
Page End: 9
Publisher Place: [London]
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.
Organization Units (connected with the publication): Engineering Sciences, University of Southampton, Southampton, SO17 1BJ, UK
ISSN: 2041-1723
DOI: 10.1038/s41467-019-08494-6
Appears in Collections:Publications of the HSU Researchers (before HSU)

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