Raphaël Ihringer’s research while affiliated with Swiss Federal Institute of Technology in Lausanne and other places

Electrical output behaviour obtained on solid oxide fuel cell stacks, based on planar anode supported cells (50 or 100 cm2 active area) and metallic interconnects, is reported. Stacks (1–12 cells) have been operated with cathode air and anode hydrogen flows between 750 and 800 °C operating temperature. At first polarisation, an activation phase (increase in power density) is typically observed, ascribed to the cathode but not clarified. Activation may extend over days or weeks. The materials are fairly resistant to thermal cycling. A 1-cell stack cycled five times in 4 days at heating/cooling rates of 100–300 K h−1, showed no accelerated degradation. In a 5-cell stack, open circuit voltage (OCV) of all cells remained constant after three full cycles (800–25 °C). Power output is little affected by air flow but markedly influenced by small fuel flow variation. Fuel utilisation reached 88% in one 5-cell stack test. Performance homogeneity between cells lay at ±4–8% for three different 5- or 6-cell stacks, but was poor for a 12-cell stack with respect to the border cells. Degradation of a 1-cell stack operated for 5500 h showed clear dependence on operating conditions (cell voltage, fuel conversion), believed to be related to anode reoxidation (Ni). A 6-cell stack (50 cm2 cells) delivering 100 Wel at 790 °C (1 kWel L−1 or 0.34 W cm−2) went through a fuel supply interruption and a thermal cycle, with one out of the six cells slightly underperforming after these events. This cell was eventually responsible (hot spot) for stack failure.

Our SOFC stack development technology is based on the unique SOFConnexTM concept, using flexible gas distribution layers between metal sheet interconnect and thin ASE cells. Flexibility is given both in material and design. This ensures proper electrical contact over the whole cell (50 cm2 active), without necessitating restrictive cell fabrication tolerances, and allows easy adaptation and evolution of the flowfields. With the presently used configuration, several multiple cell stacks were assembled and tested. Reproducible stack power density (H2 fuel, λ = 1.5-2, 800°C maximum local temperature) is 0.5 W/cm2 at 0.7 V average cell voltage (1.5 kWe/L), for 67% fuel utilisation (35% LHV electrical efficiency). Performance with simulated POX-syngas (H2/CO/N2) was close to that with H2. Degradation is the focus of attention now that adequate power density and efficiency using the SOFConnex™ approach have been established and reproduced.

A tape casting co-sintering route is described in which thin dense layers of LaSrFeCoO3 (LSFC) have been formed on planar, porous MgO substrates 100- 200 micron thick. SEM analysis of the sintered structure showed that it was possible to eliminate most of the residual porosity in the LSFC layer, but maintain a porosity between 25 and 45% in the MgO support layer. The LSFC layer dit not reveal many cracks. The overall shrinkage of the co-sintered structure was about 25%. The LSFC layer topography was smooth and uniform with a metallic-like lustre. A good correlation was obtained between the observed microstructure and the gas permeability measurements made at room temperature.

Progress on anode supported cell stacks (SOFCONNEX design, 50 m2 per cell) is presented. A 6-cell stack and a 8 cell-stack were mounted and tested with hydrogen fuel at 800 degre C, yielding 100 W el and 140 W el, corresponding to a power density of 1kW el/L (0.34 W/cm2). Fuel utilisation was 50% and electrical efficiency 25%. A one-cell stack delivered 0.4 W/cm 2 at 70% fuel utilisation and 33 % electrical efficiency, and showed a performance increase over its 450 h test period. Another one-cell stack was monitored and variable conditions (20-50 % fuel utilisation, 0.2-0.5 A/cm 2) for 5500 h including several thermal cycles, with -5%/1000 h degradation

Recent progress in our development of anode supported electrolyte (ASE) SOFcells is reported. The cells are fabricated by cocasting of aqueous slurries of NiO/YSZ and 8YSZ, followed by cofiring. A gradient cathode is deposited by screenprinting successive layers of LSM/YSZ composite and lanthanum cobaltite, followed by a 2nd firing step. Full cells show a final thickness of ? 0.25 mm, high flexibility and reasonable warpage. Proper anode current collection is crucial and obtained by cofiring an additional outer layer together with the substrate. Power density can reach 0.2 W/cm2 at 600°C with active cathodes (LSC, short-lived) and >1 W/cm2 at 810°C with the LSM cathode. Stability was tested during 2900 h, giving an average degradation of 3%/1000 h at 0.5 A/cm2 current density. Degradation can be delayed by short-time polarisation at higher current density: e.g. “reactivation” at 0.85 A/cm2 (30 min.) delayed degradation by 300 h.

To increase power density at reduced temperature operation of SOFC, thin film 8YSZ electrolytes were deposited on Ni–YSZ anode support plates by tape casting and cofiring. Cathode behaviour, limiting cell output at lower temperature, was studied in more detail. Cathodes were deposited by screenprinting and firing. With consecutive layers of doped lanthanum manganite and cobaltite, power density of 0.5 W cm−2 at 750°C was obtained using hydrogen fuel. On cells of 100 cm2, no fuel diffusion limitation above 70% conversion occurred, and electrical efficiency of 35% was achieved. Actual cell temperature increases significantly above a current density of 0.3 A cm−2. This effect causes erroneous electrode and cell characteristics.

Abstract: A short overview of recent work on electroceramic materials relevant to methane-fueled SOFC systems is given. Various fuel feed options are considered, such as pure methane, biogas, and the addition of reforming agents. The principle and implementation into SOFC systems of mixed conducting ceramics for oxygen separation is described, as well as their characterisation by electrochemical methods. Ceramic anodes capable of operating with methane-rich fuel injection are presented. The document concludes with electrochemical results on planar anode supported ceramic fuel cells operating at reduced temperature.

Ni-YSZ anode supports show a fundamentally different microstructure from screenprinted Ni-YSZ anodes on YSZ electrolyte supports. Of high density and composed of fine zirconia and nickel oxide to allow for cofiring with a thin zirconia electrolyte film (5 µm), the anode support shows advantages of adequate strength and increased electrochemical activity probably not only limited to the TPB, unlike screen printed porous anodes. Areas up to 100 cm2 have been fabricated. Electrochemical cell testing produced results of >80% fuel utilisation, 35% electrical efficiency and >20 W at 800°C using hydrogen fuel. Unusually high ohmic loss (*3 x theoretical) on supported cells is consistently observed. The smallest loss is measured when employing thin dense cathodes of a mixed conducting material. Overall cell performance (at *800 °C) is more determined by the cathode than by the anode support.