Publication date: 10th April 2024
Ruthenium oxide pyrochlores (A2Ru2O7−δ) exhibit high OER activity in aqueous acidic conditions, but the relationship of performance to underlying defect chemistry is not well understood. We study the defect chemistry and transport behavior of these rare acid-stable pyrochlore electrocatalysts to provide insight into OER activity, considering, e.g., the proposed lattice oxygen mechanism. We apply thermogravimetric analysis and impedance spectroscopy on nanopowders using a custom spring-loaded cell as a function of temperature and oxygen partial pressure. We determine 1) as-synthesized oxygen non-stoichiometry (δ) as a function of Y substitution level in Y2+xRu2-xO7-δ (x = 0, 0.1, 0.2, 0.3) through decomposition studies, correlating δ to the observed catalytic activity trend, and 2) isothermal oxygen non-stoichiometry and electrical conductivity of Y2Ru2O7 across a wide pO2 range at temperatures up to 700 °C for insight into the dominant defect chemical and transport processes. Use of nanopowders enables fast equilibration kinetics and access to mass and transport changes at relatively low temperatures.
This work was supported by the NSF (NSF CBET 20-55734 AH170)
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