Kinetics and Thermodynamics of Sr Permeation in CeO2-Based Barrier Layers for Solid-Oxide Electrolyzer Cells

Rowberg, Andrew J. E.; Van Winkle, Madeline; Slomski, Heather S.; Chatterjee, Sourav; Kane, Nicholas J.; Yu, Henry; Kim, Namhoon; Ginley, David S.; Gorman, Brian P.; Shulda, Sarah; Heo, Tae Wook; Kweon, Kyoung Eun; Wood, Brandon C.

doi:10.1021/acsami.5c12101

Kinetics and Thermodynamics of Sr Permeation in CeO₂-Based Barrier Layers for Solid-Oxide Electrolyzer Cells

Journal Article · Tue Sep 16 00:00:00 EDT 2025 · ACS Applied Materials & Interfaces

DOI:https://doi.org/10.1021/acsami.5c12101· OSTI ID:2997204

^[1]; Van Winkle, Madeline ^[2]; ^[3]; Chatterjee, Sourav ^[1]; Kane, Nicholas J. ^[4]; Yu, Henry ^[1]; Kim, Namhoon ^[1]; Ginley, David S. ^[2]; Gorman, Brian P. ^[5]; Shulda, Sarah ^[2]; ^[1]; ^[1]; ^[1]

Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)
National Renewable Energy Laboratory (NREL), Golden, CO (United States)
National Renewable Energy Laboratory (NREL), Golden, CO (United States); Colorado School of Mines, Golden, CO (United States)
Idaho National Laboratory (INL), Idaho Falls, ID (United States)
Colorado School of Mines, Golden, CO (United States)

Solid-oxide electrolyzer cells (SOECs) convert steam to hydrogen efficiently at high temperatures. However, during operation, the diffusion of cations or impurities through the cells due to electrode degradation can cause unwanted secondary phases to form, which may degrade device performance. Here, in this study, we use atomistic and mesoscale simulations coupled with experimental analysis to study the diffusion of Sr through the Gd-doped CeO₂ (GDC) barrier layer used to protect the yttria-stabilized zirconia (YSZ) electrolyte in SOECs. From our atomistic calculations, we find Sr diffusion to be negligibly slow in bulk GDC; however, surface diffusion is much more favorable. Subsequent mesoscale simulations show that Sr diffusion is activated when the porosity of GDC exceeds ∼10% and significantly exceeds diffusion in bulk and grain boundary regions. We also find that SrO-based species can accumulate at GDC surfaces; however, SrO aggregation and coarsening will be limited by the large lattice mismatch between GDC and SrO. Energy-dispersive X-ray spectroscopy (EDS) and electron diffraction confirm that Sr can accumulate within GDC pores and form disperse Sr-containing secondary phases. Altogether, Sr diffusion in dense GDC is unlikely to give rise to thick SrO layers, which would severely limit device performance. The formation of Sr-containing secondary phases can largely be avoided by restricting the porosity of the GDC layer as much as possible.

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 Nuclear Energy (NE)

Grant/Contract Number:: AC36-08GO28308; AC52-07NA27344; AC07-05ID14517

OSTI ID:: 2997204

Report Number(s):: LLNL--JRNL-2007077

Journal Information:: ACS Applied Materials & Interfaces, Journal Name: ACS Applied Materials & Interfaces Journal Issue: 39 Vol. 17; ISSN 1944-8244; ISSN 1944-8252

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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