Electrochemical Stability of Metastable Materials

By Arunima K. Singh, Lan Zhou, A. Shinde, S. Suram, Joseph H. Montoya, Donny Winston, J. Gregoire, Kristin A. Persson. 2017

268 citations recorded by the source corpus.

We present a first-principles-based formalism to provide a quantitative measure of the thermodynamic instability and propensity for electrochemical stabilization, passivation, or corrosion of metastable materials in aqueous media. We demonstrate that this formalism can assess the relative Gibbs free energy of candidate materials in aqueous media as well as their decomposition products, combining solid and aqueous phases, as a function of pH and potential. On the basis of benchmarking against 20 stable as well as metastable materials reported in the literature and also our experimental characterization of metastable triclinic-FeVO4, we present quantitative estimates for the relative Gibbs free energy and corresponding aqueous regimes where these materials are most likely to be stable, form inert passivating films, or steadily corrode to aqueous species. Furthermore, we show that the structure and composition of the passivating films formed on triclinic-FeVO4 are also in excellent agreement with the Point D...

Subfields: Materials Chemistry, Renewable Energy, Sustainability and the Environment

View Paper: https://www.semanticscholar.org/paper/2173c1a5b470733e9d47257a04e8d8e020e95451

Citations in the corpus

• A foundation model for atomistic materials chemistry. (2023, unknown): “The Pourbaix diagrams are constructed via the formalism described in ( 75, 76 ), where only the energies of the relevant solids are calculated while corrected experimentally-derived energies are used for the aqueous ions.”