Publication date: 15th December 2014
Direct solar water splitting has gained a lot of attention by the scientific community during the past years. It became apparent that the anode material where the Oxygen evolution reaction (OER) occurs plays a key role for the design of efficient water splitting devices. Tantalum-based oxide nitrides and nitrides are considered as promising candidates for photoanode materials, due to their appropriate band gaps and band levels. The band gaps and band levels in these materials can be tuned by their composition (doping, O/N ratio) as well as by their crystal structure. In addition, nanostructuring can lead to beneficial effects including light scattering and reduced diffusion pathways for improved charge carrier collection.
In this contribution we investigate the influence of the crystal structure of tantalum oxide nitrides and nitrides as well as the effect of nanostructuring on their performance as photoanodes for water oxidation. Starting from presynthesized model powders with different crystal structures and compositions, model electrodes could be prepared via electrophoretic deposition (EPD). On the other hand the combination of sol-gel chemistry, templating techniques and ammonolysis, yielded mesoporous tantalum oxide nitride and nitride thin film electrodes. In both cases, functionalization with suitable water oxidation catalysts (CoPi, NiOx, MnOx etc.) was eventually performed to improve the water oxidation kinetics as well as inhibit photocorrosion.
Photoelectrochemical investigations show a clear influence of the crystal structure as well as of the morphology on the photocatalytic performance. Our results highlight the importance of structural and morphological design as key factors for the synthesis of efficient photoanodes.
Financial support from DFG (SPP 1613, FI 1885/1–1, LE 781/13–1) is gratefully acknowledged.
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