Understanding carbon contamination in the proton-conducting zirconates and cerates

Rowberg, Andrew J. E.; Swift, Michael W.; Van de Walle, Chris G.

doi:10.1039/D1CP01902C

Title: Understanding carbon contamination in the proton-conducting zirconates and cerates

Journal Article · Wed Jul 07 00:00:00 EDT 2021 · Physical Chemistry Chemical Physics. PCCP

DOI:https://doi.org/10.1039/D1CP01902C· OSTI ID:1806230

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Materials Department, University of California, Santa Barbara, USA
Center for Computational Materials Science, US Naval Research Laboratory, Washington, USA

Carbon contamination is a significant concern for proton-conducting oxides in the cerate and zirconate family, particularly for BaCeO₃. Here, we use first-principles calculations to evaluate carbon stability in SrCeO₃, BaCeO₃, SrZrO₃, and BaZrO₃. The cerates require more carbon-poor environments to prevent carbonate formation, though this requirement can be loosened through the use of more oxygen-poor growth conditions. Carbonate formation is not the only concern, however. We find that interstitial carbon has lower formation energies in the cerates relative to the zirconates, leading to higher carbon concentrations that compete with the desired oxygen vacancy formation. We also examine the mobility of carbon interstitials, finding that both migration barriers and binding energies to acceptors are lower in the cerates. As a result, the cerates are likely to degrade when exposed to carbon at operating temperatures. Furthermore, our results show definitively why the cerates are less stable than the zirconates with respect to carbon and elucidate the mechanisms contributing to their instability, thereby helping to explain why alloying with zirconium will enhance their operational efficiency.

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Research Organization:: Univ. of California, Santa Barbara, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities Division; National Science Foundation (NSF) Graduate Research Fellowship Program

Grant/Contract Number:: AC02-05CH11231; FG02-07ER46434; 1650114

OSTI ID:: 1806230

Alternate ID(s):: OSTI ID: 1798211; OSTI ID: 1798227

Journal Information:: Physical Chemistry Chemical Physics. PCCP, Journal Name: Physical Chemistry Chemical Physics. PCCP Vol. 23 Journal Issue: 26; ISSN 1463-9076

Publisher:: Royal Society of Chemistry (RSC)Copyright Statement

Country of Publication:: United Kingdom

Language:: English

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