Publication date: 10th April 2024
Acceptor-doped barium zirconates are of major interest as proton conducting electrolyte materials for electrochemical applications at intermediate operating temperatures. The conduction of protons through polycrystalline yttrium doped barium cerium zirconates (BZCY) is hindered by the formation of space charge regions at grain boundaries caused by a positive core charge. During high temperature sintering, the positive core charge additionally acts as a driving force for acceptor dopant segregation. Yttrium segregation to grain boundaries has been observed in sintered ceramics but the fundamental relationships between the degree of segregation and protonic conductivity are not explored. Here, we present a comprehensive study of the influence of yttrium segregation on the chemical composition and structure at grain boundaries in BZCY and its impact on electrochemical properties. We designed an out-of-equilibrium model material, that displays no observable segregation and used it as a starting point to observe the kinetics of segregation and the induced changes in grain boundary conductivity after varied thermal histories. Furthermore, we coupled the electrochemical results derived from impedance spectroscopy to atomic resolution transmission electron microscopy. We discovered that atomically sharp acceptor segregation drastically increases the grain boundary conductivity both in the model system and reference samples processed by the industrially applied solid state reactive sintering (SSRS) route.
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