The stability of transition-metal catalysts in aqueous solutions is a central concern for the durability of many electrocatalytic systems, such as fuel cells, redox flow batteries, and metal-air batteries. In this talk, I will present an accurate and practical computational method to predict and compare the thermodynamic stability of transition-metal electrodes and transition-metal ions under realistic conditions. The computational method relies mainly on a recently developed self-interaction correction (the Koopmans-compliant method) [1,2] that overcomes the limitations of current density-functional theory approximations in describing the ionization and solvation of atomic species in water.  The model also incorportates the response of the solvent by combining an atomistic explicit description of the first shell of water molecules and a continuum implicit representation of the surrounding liquid environment.  The proposed approach opens up new opportunities to understand and improve the durability of electrochemical cells from first principles.
1. I. Dabo, A. Ferretti, N. Poilvert, Y. Li., N. Marzari, M. Cococcioni, Phys. Rev. B 82, 115121 (2010).
2. N. L. Nguyen, G. Borghi, A. Ferretti, I. Dabo, and N. Marzari, Phys. Rev. Lett. 114, 166405 (2015).
3. A. J. Cohen, P. Mori-Sánchez, W. Yang, Science 321, 792 (2008).
4. O. Andreussi, I. Dabo, N. Marzari, J. Chem. Phys. 136, 064102 (2012).