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Electro-Chemical-Mechanical Coupled Modeling of Oxygen Electrodes in Solid Oxide Electrolyzer Cells

Solid oxide electrolyzer cell (SOECs), which is an electrochemical device to split water with electricity to generate hydrogen, have received widespread attention for multi-day or seasonal energy storage to integrate variable renewable energy (VRE) into the grid [1]. Even though there have been tremendous material development and performance improvement of the technology in the past decade [2], challenges remain in understanding its degradation mechanism, especially the delamination of oxygen electrode/electrolyte interface [3-5]. Developing new oxygen electrodes which could decelerate the degradation and extend the stack lifetime beyond 60,000 hours at 1.5A/cm2 would significantly drive the stack price down to $100/kW and hydrogen cost down to $2/kg [6].
 In the state-of-the-art SOECs, pure ionic conductor 8 mol% Y2O3 doped ZrO2 (YSZ) and Gadolinium-doped Ceria (GDC) are usually used as the dense electrolyte and the buffer layer; mixed electronic and ionic conductor (MIEC) La1-xSrxCo1-yFeyO3-d (LSCF) is widely used as the oxygen electrode [7]. Such cells still suffer from short lifetimes with current densities over 1A/cm2. To overcome the challenge, a bilayer oxygen electrode structure, consisting of a commercial LSCF-GDC porous backbone coated by a thin SrCo0.9Ta0.1O3-
 d (SCT10) film (denoted as LSCF-SCT bilayer design), has been proposed and demonstrated with much higher performance compared to traditional LSCF electrode (single layer design) [8]. The new oxygen electrode has an inherently fast oxygen evolution reaction (OER) electrokinetics (or high oxygen evolution rate) and can mitigate the delamination problem by minimizing the accumulation of oxygen in oxygen evoluation reaction (OER) electrode lattice and thus chemical stresses.
 In this study, based upon an Electro-Chemical-Mechanical coupled model, we will correlate the crack length at the oxygen electrode/electrolyte interface with the electrochemical performance of the cell, specifically the voltage-current curve (Fig.1a). We will use J-integral (Fig.1b) as the fracture criteria to evaluate the crack growth rate under different current densities and with different oxygen electrode designs. LSCF single layer design is the baseline of the study. The long-term performance improvement of LSCF-SCT bilayer design will be compared against the baseline and its degradation mechanism will be investigated. The model will also be validated by long-term overpotential testing data as a function of time under 1A/cm2. It will be used as an optimization tool to mitigate delamination and extend the cell lifetime under higher current densities.
 
 
 Key Words: Electrolysis, Oxygen Electrode (OE), Delamination, Chemical Expansion, J integral, Crack Growth Rate
 
 
 
 
 
 Figure 1
