TY - JOUR
T1 - Ab Initio Thermodynamic Modeling of Electrified Metal-Oxide Interfaces
T2 - Consistent Treatment of Electronic and Ionic Chemical Potentials
AU - Zeng, Zhenhua
AU - Hansen, Martin Hangaard
AU - Greeley, Jeff
AU - Rossmeisl, Jan
AU - Björketun, Mårten
PY - 2015
Y1 - 2015
N2 - Solid oxide fuel cells are attractive devices in a sustainable energy context because of their fuel flexibility and potentially highly efficient conversion of chemical to electrical energy. The performance of the device is to a large extent determined by the atomic structure of the electrode-electrolyte interface. Lack of atomic-level information about the interface has limited the fundamental understanding, which further limits the opportunity for optimization. The atomic structure of the interface is affected by electrode potential, chemical potential of oxygen ions, temperature and gas pressures. Here we present a scheme to determine the metal-oxide interface structure at a given set of these environmental parameters based on quantum chemical calculations. As an illustration we determine the structure of a Ni-YSZ anode as a function of electrode potential at 0 and 1000 K. We further describe how the structural information can be used as a starting point for accurate calculations of the kinetics of fuel oxidation reactions, in particular the hydrogen oxidation reaction. More generally, we anticipate that the scheme will be a valuable theoretical tool to describe solid-solid interfaces. [Figure]
AB - Solid oxide fuel cells are attractive devices in a sustainable energy context because of their fuel flexibility and potentially highly efficient conversion of chemical to electrical energy. The performance of the device is to a large extent determined by the atomic structure of the electrode-electrolyte interface. Lack of atomic-level information about the interface has limited the fundamental understanding, which further limits the opportunity for optimization. The atomic structure of the interface is affected by electrode potential, chemical potential of oxygen ions, temperature and gas pressures. Here we present a scheme to determine the metal-oxide interface structure at a given set of these environmental parameters based on quantum chemical calculations. As an illustration we determine the structure of a Ni-YSZ anode as a function of electrode potential at 0 and 1000 K. We further describe how the structural information can be used as a starting point for accurate calculations of the kinetics of fuel oxidation reactions, in particular the hydrogen oxidation reaction. More generally, we anticipate that the scheme will be a valuable theoretical tool to describe solid-solid interfaces. [Figure]
KW - L03 Poster Session - May 26 2015 6:00PM
U2 - 10.1149/MA2015-01/31/1786
DO - 10.1149/MA2015-01/31/1786
M3 - Journal article
SN - 2151-2043
VL - MA2015-01
JO - W S S A Meeting Abstracts (Online)
JF - W S S A Meeting Abstracts (Online)
IS - 31
M1 - 201786
ER -