Impact of Sr-Containing Secondary Phases on Oxide Conductivity in Solid-Oxide Electrolyzer Cells

Rowberg, Andrew J. E.; Slomski, Heather S.; Kim, Namhoon; Strange, Nicholas A.; Gorman, Brian P.; Shulda, Sarah; Ginley, David S.; Kweon, Kyoung E.; Wood, Brandon C.

doi:10.1021/acs.chemmater.4c00511

Impact of Sr-Containing Secondary Phases on Oxide Conductivity in Solid-Oxide Electrolyzer Cells

Journal Article · Sat Jun 15 00:00:00 EDT 2024 · Chemistry of Materials

DOI:https://doi.org/10.1021/acs.chemmater.4c00511· OSTI ID:2397031

^[1]; Slomski, Heather S. ^[2]; Kim, Namhoon ^[1]; ^[3]; Gorman, Brian P. ^[4]; Shulda, Sarah ^[5]; Ginley, David S. ^[5]; ^[1]; ^[1]

Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)
National Renewable Energy Laboratory (NREL), Golden, CO (United States); Colorado School of Mines, Golden, CO (United States)
SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)
Colorado School of Mines, Golden, CO (United States)
National Renewable Energy Laboratory (NREL), Golden, CO (United States)

Solid-oxide electrolyzer cells (SOECs) based on a yttria-stabilized zirconia (YSZ) oxide electrolyte produce hydrogen from water with the assistance of excess thermal energy; however, Sr diffusion within the Gd-doped CeO₂ (GDC) barrier layer during processing or operation can lead to the formation of unwanted secondary phases such as SrO and SrZrO₃. Here, to establish and compare the degree of impact of these phases on SOEC performance, we conduct first-principles calculations to study their bulk oxide conductivities and compare them to that of the YSZ electrolyte. We find that SrO has a low conductivity arising from the poor mobility and low concentration of mobile oxygen vacancies, and its presence in SOECs should therefore be avoided. SrZrO₃ also has a lower oxide conductivity than YSZ; however, this discrepancy is primarily due to lower vacancy concentrations rather than low mobility. We find that sufficient levels of Y-doping on the Zr site can increase oxygen vacancy concentrations in SrZrO₃ to achieve an oxide ionic conductivity on par with that of YSZ, thereby mitigating any potential deleterious effect on transport performance. Energy-dispersive X-ray spectroscopy confirms that Y is the most common minority element present in SrZrO₃ forming near the GDC–YSZ interface, alleviating concerns regarding the impact of SrZrO₃ on device performance. These results from our combined computational–experimental analysis can inform future engineering strategies designed to limit the detrimental effects of Sr-induced secondary phase formation on SOEC performance.

View Accepted Manuscript (DOE)

Research Organization:: Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)

Sponsoring Organization:: USDOE National Nuclear Security Administration (NNSA); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Hydrogen Fuel Cell Technologies Office (HFTO); USDOE Office of Science (SC)

Grant/Contract Number:: AC52-07NA27344; AC36-08GO28308

OSTI ID:: 2397031

Alternate ID(s):: OSTI ID: 2396648
OSTI ID: 2440284

Report Number(s):: LLNL--JRNL-860613; 1091726

Journal Information:: Chemistry of Materials, Journal Name: Chemistry of Materials Journal Issue: 13 Vol. 36; ISSN 0897-4756

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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