Non-equilibrium crystallization pathways of manganese oxides in aqueous solution
Abstract
Aqueous precipitation of transition metal oxides normally 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. In this work, 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.
- Authors:
-
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
- Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
- Univ. of Southampton (United Kingdom)
- Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
- Publication Date:
- Research Org.:
- Energy Frontier Research Centers (EFRC) (United States). Center for Next Generation of Materials by Design: Incorporating Metastability (CNGMD); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities Division
- OSTI Identifier:
- 1542369
- Grant/Contract Number:
- AC02-05CH11231; AC02-06CH11357
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Nature Communications
- Additional Journal Information:
- Journal Volume: 10; Journal Issue: 1; Journal ID: ISSN 2041-1723
- Publisher:
- Nature Publishing Group
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Citation Formats
Sun, Wenhao, Kitchaev, Daniil A., Kramer, Denis, and Ceder, Gerbrand. Non-equilibrium crystallization pathways of manganese oxides in aqueous solution. United States: N. p., 2019.
Web. doi:10.1038/s41467-019-08494-6.
Sun, Wenhao, Kitchaev, Daniil A., Kramer, Denis, & Ceder, Gerbrand. Non-equilibrium crystallization pathways of manganese oxides in aqueous solution. United States. https://doi.org/10.1038/s41467-019-08494-6
Sun, Wenhao, Kitchaev, Daniil A., Kramer, Denis, and Ceder, Gerbrand. Mon .
"Non-equilibrium crystallization pathways of manganese oxides in aqueous solution". United States. https://doi.org/10.1038/s41467-019-08494-6. https://www.osti.gov/servlets/purl/1542369.
@article{osti_1542369,
title = {Non-equilibrium crystallization pathways of manganese oxides in aqueous solution},
author = {Sun, Wenhao and Kitchaev, Daniil A. and Kramer, Denis and Ceder, Gerbrand},
abstractNote = {Aqueous precipitation of transition metal oxides normally 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. In this work, 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.},
doi = {10.1038/s41467-019-08494-6},
journal = {Nature Communications},
number = 1,
volume = 10,
place = {United States},
year = {Mon Feb 04 00:00:00 EST 2019},
month = {Mon Feb 04 00:00:00 EST 2019}
}
Web of Science
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