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TITLE: Chromium Poisoning of Cathode in Solid Oxide Fuel Cells: Mechanisms and Mitigation Strategies

ABSTRACT: Solid oxide fuel cells (SOFCs) have gained renewed interest due to their high energy-conversion efficiency, new discovery of fossil fuel sources, and low greenhouse gas emission. However, performance degradation during long-term operation is one of the greatest challenges to overcome for commercialization of SOFCs. At intermediate temperatures, chromium (Cr) vapor species that form over chromia-forming alloy interconnect, can transport and deposit in the cathode, and poison the cathode performance. Although extensive studies have been conducted on the Cr-poisoning phenomena, the mechanism of cathode performance degradation still needs to be clarified. Therefore, there is an urgent need to understand the degradation mechanisms and develop corresponding mitigation strategies.

In this research, anode-supported cells with (La,Sr)MnO3-based cathode were fabricated. The cells were electrochemically tested with and without the presence of chromia-forming alloy interconnect, and operating conditions including cathode atmosphere, current condition, and interconnect contact were varied independently. It was found that both humidity and cathodic current promote chromium poisoning. Microstructural characterizations also confirmed that larger amounts of chromium-containing deposits are present at the cathode/electrolyte interfaces of the cell tested with cathodic current and/or humidity.

With the help of free energy minimization calculations, the equilibrium cell potentials for Cr vapor species reductions are estimated and found to be very close to the open-circuit potential of the cell. Combining the experimental and computational results, the roles of humidity and cathodic current in Cr-poisoning are evaluated, and a mechanism associated to Cr vapor species dissociation at the triple-phase-boundaries is proposed.

To evaluate the Cr-poisoning effects on cell performance, an analytical polarization model is used for quantitatively separating the contribution of various cell polarizations. By curve-fitting the current-voltage traces to this model, the changes of cathode polarizations due to Cr-poisoning are quantified. Under normal operating conditions, the cathodic activation polarization is determined to be most negatively impacted by Cr-poisoning.

Mitigation of the Cr-poisoning effects using a dense lab-developed CuMn1.8O4 spinel interconnect coating was demonstrated. Employing the spinel coated interconnect mesh in on-cell tests, it was found that both the degradation in cell performance and Cr deposition in the cathode are significantly mitigated.

COMMITTEE: Advisor: Uday B. Pal, MSE/ME; Srikanth Gopalan, MSE/ME; Soumendra N. Basu, MSE/ME; Vinod Sarin, MSE/ME; Chair: Keith Brown, MSE/ME