Publication date: 31st March 2013
Photoelectrochemical (PEC) water splitting requires an ideal semiconductor material with a high stability and a good absorption of the solar spectrum. Oxides are generally stable in aqueous solutions, but their bandgap is usually too large to efficiently absorb sunlight. Nitrides, on the other hand, have ideal bandgaps but they are prone to corrosion. Oxynitrides are therefore potential candidates to obtain the best of both worlds: the oxide’s stability and the nitride’s strong light absorption. One of the most promising oxynitrides for solar water splitting is tantalum oxynitride (β-TaON). Due to its favorable band positions, it is thermodynamically able to split water without any external bias. However, its synthesis is very challenging. In this study, we propose ‘oxynitrogenography’ as an approach towards the controlled and reproducible synthesis of any Ta-O-N phase, including the desired β-TaON phase. Tantalum oxide thin films were nitridated in a tube furnace under controlled flows of ammonia, water and hydrogen, while following the optical transmission of the film in-situ. The optical absorption changes in the film can be directly correlated to the presence of different phases (Ta2O5, TaOxNy, Ta3N5), due to their different absorption edges. As a result, the thermodynamic equilibrium conditions to obtain these various phases were determined, and a phase diagram was constructed. Finally, the physical characteristics, electronic properties, and PEC performance of these phases will be presented.
In situ optical transmission following the nitridation of tantalum oxide thin films under controlled flows of ammonia, water and hydrogen. The optical absorption of the film changes over time and can be directly correlated to the presence of different phases (Ta2O5, TaOxNy, Ta3N5), due to their different absorption edges.
Dabirian, A.; et al. Energy Procedia 2012, 22, 15-22.
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