Correlation Between Microstructure and Performance of GDC-Based Electrodes

Abstract

Gadolinium doped ceria (GDC) gains increasing attention as a promising material for both solid oxide fuel cells (SOFCs) and solid oxide electrolysis cells (SOECs). The GDC-based electrodes demonstrate positive features, e.g. enhanced electrochemical performance in low operation temperatures, resistivity to sulfur poisoning and carbon deposition, etc. As GDC is a mixed electronic-ionic conductor in reducing atmosphere, electrochemical reactions can be supported by the double phase boundary (DPB) at the GDC surface. Several studies demonstrated that the DPB reaction may dominate the electrochemical performance over triple phase boundary (TPB) reaction in Ni-GDC electrodes, where it can account for as much as 95 % of the total reaction depending on the cermet microstructure [1]. Recent studies even show that pure ceria electrodes can achieve substantial power density [2,3]. In this context, the microstructure design principle for GDC-based electrodes should focus on maximizing GDC surface area. Particularly, GDC electrodes with infiltrated GDC nanoparticles or electro-catalytic nanoparticles may achieve competitive performance compared with the conventional Ni-YSZ electrodes. Although many strategies have been proposed to improve performance of GDC-based electrodes, it is difficult to quantitatively compare all the reported results. Furthermore, the correlation between microstructure and performance of pure GDC electrode are still scarce.Several different types of GDC-based electrodes are fabricated and tested in the unified characterization procedure in this study. Four basic designs are considered, i.e. Ni-GDC, GDC-perovskite composites, GDC electrodes with deposited Ni nanoparticles and pure GDC electrodes. Several strategies to modify the GDC surface area are discussed. In addition, the substantial enhancements in the DPB density and electrochemical performance were achieved by precipitating Ni-nanoparticles directly on sub-micron GDC powders at 2wt.% loading. The performance of electrodes was evaluated by electrochemical impedance spectra measurements with various humidity and temperature conditions. The results showed clear dependance between GDC surface area and electrode performance. At the same time, it should be noted that the electrode active thickness depends on the electrode microstructure. In particular, it is in the range of 5 µm for the pure nano-GDC electrode. When the GDC electrode is thicker than the active thickness, it results in large Ohmic resistance due to the electronic conduction in the porous electrode.[1] A. Nenning, M. Holzmann, J. Fleig, A.K. Opitz, Mater. Adv. 2 (2021) 5422–5431.[2] M. Ouyang, A. Bertei, S.J. Cooper, Y. Wu, P. Boldrin, X. Liu, M. Kishimoto, H. Wang, M. Naylor Marlow, J. Chen, X. Chen, Y. Xia, B. Wu, N.P. Brandon, J. Energy Chemistry. 56 (2021) 98–112.[3] W. Jung, K.L. Gu, Y. Choi, S.M. Haile, Energy Env. Sci. 7 (2014) 1685–1692.