Improvement of transport properties and hydrogen permeation of chemically-stable proton conducting oxides bases on the system BaZr1-x-yYxMyO3-δ

[EN] The structural and transport properties as well as the chemical stability of a series of proton-conducting oxides based on yttrium-doped barium zirconate were investigated. Specifically, Pr-, Fe- and Mn-doped BaZr1-x-yYxMyO3-delta compounds were prepared by solid state reaction. The compound exhibiting the highest total and protonic conductivity at elevated temperatures under reducing atmospheres was BaZr0.8Y0.15Mn0.05O3-delta. Temperature-programmed reduction experiments revealed a particular redox behavior related to the Mn-species under selected conditions. The hydrogen permeation was thoroughly studied as a function of the temperature, hydrogen concentration and the humidification degree in the sweep gas. Moreover, the transient processes induced by alternate step changes in the humidification degree of the sweep gas were analysed. The highest steady hydrogen evolution flow exceeded 0.03 ml min(-1) cm(-2) (0.9 mm-thick membrane) at 1000 degrees C for the humidified sweep gas. The stability of BaZr0.8Y0.15M0.05O3-delta under operation-relevant atmospheres (CO2-rich reducing atmosphere at high temperature) was tested using different techniques ( X-ray diffraction (XRD), Raman, SEM, TEM and TG) and the results showed that this material is stable even when exposed to 115 ppm H2S.Financial support by the Spanish Ministry for Economics and Competitiveness (JAE-Pre 08-0058, ENE2008-06302 and ENE2011-24761 grants) and the Helmholtz Association of German Research Centers through the Helmholtz Alliance MEM-BRAIN (Initiative and Networking Fund) is kindly acknowledged. Dr M. Ivanova thanks the Northern European Innovative Energy Research Program N-INNER (grant no. 09- 064274) and the German Federal Ministry of Education and Research (BMBF) for supporting the N-INNER Project ‘‘Novel High Temperature Proton and Mixed-Proton Electron Conductors for Fuel Cells and H2-separation membranes’’ (Contract 03SF0330).Escolástico Rozalén, S.; Ivanova, M.; Solis Díaz, C.; Roitsch, S.; Meulenberg, WA.; Serra Alfaro, JM. (2012). Improvement of transport properties and hydrogen permeation of chemically-stable proton conducting oxides bases on the system BaZr1-x-yYxMyO3-δ. RSC Advances. 2(11):4932-4943. doi:10.1039/C2RA20214JS4932494321