Publication date: 10th April 2024
Triple ionic-electronic conducting oxides, in which electron holes, oxygen ions, and protons are simultaneously mobile, are garnering massive attention as potential oxygen electrodes in protonic ceramic cells. While their high electrocatalytic activities and proton transport abilities generally provide opportunities for enhanced performance of the electrochemical cells, the lack of fundamental knowledge on the proton uptake mechanism hinders the rational modification and design of the materials. Herein, we investigate the proton uptake mechanism in double-perovskite PrBa0.5Sr0.5Co1.5Fe0.5O5+δ (PBSCF), a candidate material exhibiting the triple ionic-electronic conducting property. The proton solubility of PBSCF is examined by direct observation of proton using secondary ion mass spectrometry. We then comprehensively discuss the correlations between previously hypothesized proton uptake mechanisms (hydration vs hydrogenation) and experimentally measured properties such as mass and conductivity changes. This work provides a guideline for establishing the design principles of triple ionic-electronic conducting oxides based on mechanistic understanding.
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