Proceedings of September Meeting 2016 (NFM16)
Publication date: 14th June 2016
Semiconductor passivation and protection films are crucial especially under anodic conditions upon evolution of oxygen. Additional requirements for these films comprise sufficient transparency and conductivity in order to support optimized light-incoupling and charge carrier transport. Usually, protective films are realized by depositing metal oxide or metallic overlayers onto the semiconductor. In this work, the facile fabrication of an ultrathin organic protection/passivation coating functionalized with RuO2 water oxidation catalysts on silicon is demonstrated [1]. Silicon photoanodes coated with the polymeric protection layer showed stable photocurrents in excess of 15 mA/cm2 and a photovoltage of 500 mV. Key to the fabrication method is the exploitation of the twofold catalytic activity of RuO2 towards alcohol polymerization and water oxidation. Comparative analyses by photoelectron spectroscopy, X-ray diffraction and photoelectrochemical assessment prove the in-situ formation of a polymeric interface layer concomitantly deposited during electrophoretic transport of RuO2 towards the silicon substrate. The presence of carbon sp2-bonds in this film suggests a reaction route via iodine-mediated electro-reductive polymerization of alcohols which could be confirmed by extensive analysis in dependence of the organic solvents used for the electrophoretic deposition process. Based on these findings, a detailed reaction scheme is developed to elucidate the individual steps of coupling of hydrocarbons to the silicon surface and the subsequent transformation of sp3 to sp2 bonds by E2-elimination. Surface terminal groups, encompassing C-OH and C=O, finally realize stability against electrophilic attack and account for the observed degradation-free operation of the photoanode in acidic electrolytes. This is one of the first demonstrations of a highly stable inorganic-organic hybrid system for light-induced oxygen evolution.
[1] Anahita Azarpira, Thomas Schedel-Niedrig, H.-J. Lewerenz, Michael Lublow, Adv. Energy Mater. 1502314 (2016). DOI: 10.1002/aenm.201502314
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