First Principles Modeling Of Oxygen Reduction at Complex Perovskite Surfaces for Fuel Cell and Gas Separation Applications
EMSL Project ID
42498
Abstract
Using DFT first principles method implemented in VASP 5.0 computer code for large scale parallel calculations, we will study the atomic, electronic structure and physico-chemical properties of oxygen adsorbed at the surface of advanced complex perovskites (Ba,Sr)(Co,Fe)O3 [BSCF]. Based on these calculations, we will study surface adsorbate and defect properties and thus thermodynamics and the kinetics of oxygen reduction process. Understanding of the limiting stage of this process is of key importance for solid oxide fuel cell and gas separation membrane applications. This multidisciplinary study (surface science, theoretical physics, defect chemistry, catalysis, large scale computing) will allow us to suggest interpretation to existing state-of-the-art experiments (e.g. impedance and Raman spectroscopy) and to improve efficiency of existing devices. The planned VASP calculations are very time consuming due to the necessity of the electronic and atomic structure optimization for low symmetrical quantum systems containing hundreds of atoms including defects as well as taking into account strongly correlated nature of materials under study. Based on our experience with similar systems, we request 100.000 node hours on CHINOOK Lunix Cluster . The proposal is non-proprietary, general with a remote access. The proposed work is consistent with EMSL 2010 Call 'Science of Interfacial Phenomena', including investigations of dynamical processes at surfaces and coupling to theory and modeling and the EMSL mission in general (to provide innovative solutions to the environmental challenges as well as those related to energy production).
Project Details
Project type
Exploratory Research
Start Date
2011-01-01
End Date
2012-01-08
Status
Closed
Released Data Link
Team
Principal Investigator
Team Members
Related Publications
Evarestov R, E Blokhin, D Gryaznov, EA Kotomin, R Merkle, and J Maier. 2012. "Jahn-Teller Effect in the Phonon Properties of Defective SrTiO3 from First Principles." Physical Review. B, Condensed Matter 85(17):174303. doi:10.1103/PhysRevB.85.174303
Heifets E, EA Kotomin, Y Mastrikov, S Piskunov, and J Maier. 2011. "Thermodynamics of ABO3-Type Perovskite Surfaces." Chapter 19 in Thermodynamics – Interaction Studies – Solids, Liquids and Gases, ed. Juan Carlos Moreno-Pirajan, pp. 491-518. InTech, Manhattan, NY.
Kotomin EA, R Merkle, Y Mastrikov, MM Kukla, and J Maier. 2013. "Energy Conversion: Solid Oxide Fuel Cells." Chapter 6 in Computational Approaches to Energy Materials, ed. A Walsh, A Sokol, R Catlow, pp. 149-186. John Wiley & Sons, Ltd., Hoboken, NJ.
Kukla MM, EA Kotomin, R Merkle, Y Mastrikov, and J Maier. 2013. "Combined Theoretical and Experimental Analysis of Processes Determining Cathode Performance in Solid Oxide Fuel Cells." Physical Chemistry Chemical Physics. PCCP 15:5443-5471. doi:10.1039/C3CP44363A
Merkle R, Y Mastrikov, EA Kotomin, MM Kukla, and J Maier. 2011. "First Principles Calculations of Oxygen Vacancy Formation and Migration in Ba1?xSrxCo1?yFeyO3?? Perovskites." Journal of the Electrochemical Society 159(2):B219-B226. doi:10.1149/2.077202jes