Proceedings of nanoGe Fall Meeting 2018 (NFM18)
Publication date: 6th July 2018
The coupling of light absorbers to cocatalysts is of crucial importance for efficient solar-driven photoelectrocatalytic water splitting.[1,2] Recently we achieved effective loading of visible light-active porous hybrid TiO2-CNx (CNx –poly(aminoimino)heptazine, melon, “graphitic carbon nitride”) photoanodes for water photooxidation with ultrasmall (~1-2 nm), highly disordered CoO(OH)x nanoparticles using a two-step impregnation method.[3] Under visible light (l > 420 nm) irradiation, the resulting photoanodes significantly outperformed photoanodes loaded with conventional cobalt-based cocatalyst (Co-Pi) comprising larger nanoparticles (~5 nm) both in terms of Faradaic efficiency of oxygen evolution (by the factor of 2) and performance stability under long-term irradiation.
The contribution will focus on elucidating the advantages of using ultrasmall CoO(OH)x nanoparticles as cocatalysts. A combination of STEM, XAS, cyclic voltammetry, and photoelectrochemical techniques was used to elucidate the advantages of using ultrasmall CoO(OH)x nanoparticles as cocatalysts. Specifically, due to their high transparency in visible range, higher loading of porous photoanodes with cobalt catalytic sites could be achieved, while the photocurrent losses due to parasitic light absorption by the cocatalyst are minimized. Importantly, EXAFS data recorded before and after photoelectrocatalysis indicated that the significant enhancement in stability of ultrasmall CoO(OH)x nanoparticles in borate as compared to phosphate electrolytes can be explained by the difference in structural ordering dictated by interaction of the electrolyte anions with cobalt ions.
The carbon nitrate soft matter matrix is further examined for capability of accumulation of charges (electron or holes) when coupled with Pt or MoSx nanoparticles. In particular photopotential decay measurements under open-circuit conditions will be discussed to assess the charging-discharging properties. Correlation between photocatalytic hydrogen evolution and dynamics of light-induced charge carries will be addressed.
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