International Journal of Hydrogen Energy, Vol.44, No.48, 26577-26588, 2019
Oxygen isotope exchange in proton-conducting oxides based on lanthanum scandates
A method of the oxygen isotope exchange with equilibration of the gas phase was used in order to obtain the temperature dependences of the oxygen surface exchange and diffusion coefficients of the proton-conducting oxides La1-xSrxScO3-delta (x = 0; 0.04; 0.09) in the temperature range of 600-900 degrees C and oxygen pressure of 1.01 kPa. The diffusion and oxygen surface exchange coefficients increase with the strontium content in oxides. The rates of the individual stages of the oxygen exchange process on the surface of the oxides were determined. The oxygen incorporation was revealed to be rate-determining for the undoped LaScO3 oxide. However, for the strontium-doped oxides La1-xSrxScO3-delta (x = 0.04; 0.09), the difference between the rates of oxygen dissociative adsorption and oxygen incorporation decreases with increasing the strontium concentration, in a way that for the La0.91Sr0.09ScO3-delta oxide these stages become competing. The possible reasons for these differences in oxygen surface exchange kinetics were analyzed in this paper. Using the obtained oxygen diffusion coefficients, the oxygen-ionic conductivities in accordance with the Nernst-Einstein equation, and the contributions of the oxygen-ion and proton components of the total conductivity of the La1-xSrxScO3-delta (x = 0.04; 0.09) oxides in the wet reducing atmosphere (pH(2)O = 2.35 kPa, pO(2) = 10(-15) Pa) were calculated. The proton transference numbers were found to be close to unit at the wet reducing atmospheres in the temperature range of 500-600 degrees C. (C) 2019 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved.
Keywords:Lanthanum scandate;Oxygen tracer diffusion;Oxygen surface exchange;Isotope exchange;Segregation;Proton-conducting oxides