Evaluation and Upscaling of Impregnated La0.20Sr0.25Ca0.45TiO3 Fuel Electrodes for Solid Oxide Electrolysis Cells Under H2O, CO2 and Co-Electrolysis Conditions

Abstract

As a result of a successful collaboration between the University of St Andrews and HEXIS AG over the past >10 years, an alternative solid oxide fuel cell (SOFC) fuel electrode material (to the state-of-the-art Ni/CGO fuel electrode) has been intensively researched and developed 1 at a button cell scale (1 cm2 active area), 2 tested under harsh operating conditions and upscaled to short stack scale (5 cells each of 100 cm2 active area), 1,3 in addition to being integrated into full combined heat and power units (60 cells each of 100 cm2 active area) with nominal 1-1.5 kW power outputs. 3,4 This highly robust fuel electrode comprises a La0.20Sr0.25Ca0.45TiO3 (LSCTA-) ‘backbone’ with cerium gadolinium oxide (CGO) and Rh impregnates, offering stability toward redox/thermoredox/thermal cycling, overload or stress testing, degradation comparable to the state-of-the-art SOFCs and exposure to sulphurised natural gas. 1 This material, therefore, addresses many of the challenges presented by the Ni/CGO fuel electrodes.Given the success of this material as a SOFC fuel electrode and the growing demand for production of ‘green’ hydrogen and synthesis gas through high-temperature electrolysis, 5 it is also desirable to assess its performance in solid oxide electrolysis cells (SOECs). In this paper, the authors present a comprehensive study of the performance of SOECs containing the aforementioned titanate-based fuel electrodes.Firstly, testing of button cell scale SOECs (1 cm2 active area) in pure CO2 and H2O/H2 mixtures, carried out at the University of St Andrews and HEXIS AG, will be outlined, including promising initial test data from VI curves and AC impedance spectroscopic analysis. Subsequently, information on durability testing of the aforementioned SOECs will be provided. This data indicates that high degradation is observed during testing in H2O/H2/N2 mixtures when employing a LSM-YSZ/LSM air electrode, most likely due to delamination caused by oxygen evolution at the triple phase boundary between LSM and YSZ particles and at the air electrode-electrolyte interface, which is significantly minimised by replacement with a LSCF-CGO air electrode. Finally, upscaling of this technology to a 5 x 5 cm footprint SOEC (16 cm2 active area) containing the aforementioned fuel electrode, a stabilised zirconia electrolyte and a LSCF-CGO air electrode will be outlined. Encouraging results from a ~600 hour test at 850 °C will be presented, including operation in 54 % H2O:46 % CO2 and pure CO2 at 1.47 V, as well as in 51 % H2O:49 % N2 at 1.29 V (without the use of a reducing gas). References 1 R. Price, M. Cassidy, J. G. Grolig, G. Longo, U. Weissen, A. Mai and J. T. S. Irvine, Advanced Energy Materials, 2021, 11, 2003951.2 R. Price, M. Cassidy, J. G. Grolig, A. Mai and J. T. S. Irvine, J. Electrochem. Soc., 2019, 166, F343–F349.3 M. C. Verbraeken, B. Iwanschitz, E. Stefan, M. Cassidy, U. Weissen, A. Mai and J. T. S. Irvine, Fuel Cells, 2015, 5, 682–688.4 R. Price, H. Bausinger, G. Longo, U. Weissen, M. Cassidy, J. G. Grolig, A. Mai and J. T. S. Irvine, In Preparation, 2022.5 J. B. Hansen, Faraday Discuss., 2015, 182, 9 – 48.