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David Mebane
Associate Professor, Mechanical and Aerospace Engineering

Uncertainty Quantification in SOFC Modeling

The cathode reaction in solid oxide fuel cells is complex and still not completely understood. The most popular SOFC cathode is strontium-doped lanthanum manganate (LSM), which is a conductor of both electrons and oxygen ions. The oxygen conductivity in LSM is very poor, however, its performance as a cathode material is much better than metals like platinum, where oxygen incorporation reactions are limited to the triple phase boundary (TPB) between the air, the electrode and the electrolyte. This suggests that there is some transport of oxygen in LSM, which extends the incorporation reaction to the surface of the electrode. Patterned electrode experiments have been used to quantify the extent of electrode surface that is active, but these are not produced in the same manner as the porous materials that typically serve as SOFC electrodes.

In collaboration with the National Energy Technology Laboratory’s Solid Oxide Fuel Cell program, Bayesian calibration was used to quantify an impedance model for a porous LSM SOFC cathode, generating an estimate of the effective width of the active region (in other words, the extent to which the reduction reaction takes place on the LSM surface away from the TPB) and quantifying model parameters. Microstructural data gathered using X-ray Computed Tomography (Carnegie Mellon) was used to specify critical geometric parameters such as the length of the TPB and the total LSM surface area per unit area of the electrolyte, thus replicating the kind of detailed geometric information available in patterned electrodes. Preliminary results show that a majority of the current moves through the TPB, but a significant minority takes a route through the bulk of LSM within nanometers of the electrolyte.
Bivariate ‘scatter plot’ distribution for the activation enthalpy and pre-exponential factor for the triple-phase boundary reaction. The scale highlights regions of high and low probability. 
Impedance data, along with the model predictions resulting from a draw from the posterior distribution of the model parameters. Red is 700 deg-C, green is 750 and blue is 800 deg-C. Nyquist impedance plots with experiment (x) and model predictions (solid lines). What seems to be a single line in the left-figure is actually a family of curves generated by drawing different parameter sets from the posterior distribution, as illustrated on the right.
Probability distributions for the fraction of current moving through the TPB, or surface pathway (as opposed to the 2PB, or bulk pathway), for 700 (red), 750 (green) and 800 (blue) deg.-C.


Papers