Understanding the processes governing performance and durability of solid oxide electrolysis cells.

Operation of a Ni-YSZ electrode supported Solid Oxide Cell (SOC) was studied in both fuel cell mode (FC-mode) and electrolysis cell mode (EC-mode) in mixtures of H2O/H2, CO2/CO, H2O/H2O/CO2/CO at 750 °C, 800 °C and 850 °C. Although the SOCs are reversible, the polarisation characterisation shows that the kinetics for the reduction of H2O and CO2 is slower compared to oxidation of H2 and CO, and that oxidation/reduction in CO2/CO mixtures is slower than in H2O/H2 mixtures. The kinetic differences are partly related to the polarisation heating and the entropy change.

Eliminating degradation in solid oxide electrochemical cells by reversible operation.

One promising energy storage technology is the solid oxide electrochemical cell (SOC), which can both store electricity as chemical fuels (electrolysis mode) and convert fuels to electricity (fuel-cell mode). The widespread use of SOCs has been hindered by insufficient long-term stability, in particular at high current densities. Here we demonstrate that severe electrolysis-induced degradation, which was previously believed to be irreversible, can be completely eliminated by reversibly cycling between electrolysis and fuel-cell modes, similar to a rechargeable battery.

TOF-SIMS characterization of impurity enrichment and redistribution in solid oxide electrolysis cells during operation.

TOF-SIMS analyses of state-of-the-art high temperature solid oxide electrolysis cells before and after testing under different operating conditions were performed. The investigated cells consist of an yttria stabilized zirconia (YSZ) electrolyte, a La1-xSrxMnO3-δ composite anode and a Ni-YSZ cermet cathode. The surfaces and cross-sections of the cells were analyzed, and several elemental impurities like Si, Ca and Na were identified and spatially mapped and their enrichment and migration during operation is reported.

Origin of electrolyte-dopant dependent sulfur poisoning of SOFC anodes.

The mechanisms governing the sulfur poisoning of the triple phase boundary (TPB) of Ni-XSZ (X2O3 stabilized zirconia) anodes have been investigated using density functional theory. The calculated sulfur adsorption energies reveal a clear correlation between the size of the cation dopant X(3+) and the sulfur tolerance of the Ni-XSZ anode; the smaller the ionic radius, the higher the sulfur tolerance. The mechanistic study shows that the size of X(3+) strongly influences XSZ's surface energy, which in turn determines the adhesion of Ni to XSZ.

Light at the interface: the potential of attenuated total reflection infrared spectroscopy for understanding heterogeneous catalysis in water.

IR spectroscopy has been an important tool for studying detailed interactions of reactants and reaction-intermediates with catalyst surfaces. Studying reactions in water is, however, far from trivial, due to the excessive absorption of infrared light by water. One way to deal with this is the use of Attenuated Total Reflection spectroscopy (ATR-IR) minimizing the path length of infrared light through the water.

The influence of water and pH on adsorption and oxidation of CO on Pd/Al2O3--an investigation by attenuated total reflection infrared spectroscopy.

Adsorption and oxidation of carbon monoxide over a Pd/Al2O3 catalyst layer was investigated both in gas phase and water. Both adsorption and oxidation of CO are significantly affected by the presence of liquid water. Water influences the potential of the metal particles as well as the dipole moment of the adsorbed CO molecule directly, which is reflected both in large red shifts and a higher infrared intensity when experiments are carried out in water.

In situ attenuated total reflection infrared (ATR-IR) study of the adsorption of NO2-, NH2OH, and NH4+ on Pd/Al2O3 and Pt/Al2O3.

In relation to the heterogeneous hydrogenation of nitrite, adsorption of NO2-, NH4+, and NH2OH from the aqueous phase was examined on Pt/Al2O3, Pd/Al2O3, and Al2O3. None of the investigated inorganic nitrogen compounds adsorb on alumina at conditions presented in this study. NO2-(aq) and NH4+(aq) on the other hand show similar adsorption characteristics on both Pd/Al2O3 and Pt/Al2O3.

CO adsorption and oxidation at the catalyst-water interface: an investigation by attenuated total reflection infrared spectroscopy.

Adsorption of carbon monoxide and oxidation of preadsorbed carbon monoxide from gas and aqueous phases were studied on a platinum catalyst deposited on a ZnSe internal reflection element (IRE) using attenuated total reflection infrared (ATR-IR) spectroscopy. The results of this study convincingly show that it is possible to prepare platinum metal layers strongly attached to an IRE, which are stable for over 3 days in aqueous-phase experiments. It is shown that ATR-IR spectroscopy is a suitable technique to study adsorption and catalytic reactions occurring at the interface of a solid catalyst in an aqueous reaction mixture, even with an extreme low-surface-area catalyst.