Proceedings of September Meeting 2016 (NFM16)
Publication date: 14th June 2016
Fabrication of photocatalytic semiconductor particle-based photoelectrodes (PE) using simple dipping procedures – scaled in commercial battery production – can be a route to overcome the efficiency-cost trade-off of solar hydrogen(1).The ability to vary the morphology and arrangement of the particles allows for designing high-performing particle-based PE. In addition, inter-particle necking procedure, surface passivation and co-catalyst deposition can further improve the PE’s performance. The impact of morphology, arrangement, and material combinations on multi-physical transport phenomena and, consequently, solar to hydrogen efficiency must be understood to provide design guidelines for high-performing particle-based PE.
A combined experimental-numerical approach was used to study particulate LaTiO2N PE. Photocurrent measurements of LaTiO2N were performed using front and back illumination with amorphous TiO2 inter-particle necking(2), NiOx/CoOx/Co(OH)2 catalysts and Ta2O5 passivation layer. These measurements were compared with a 2D numerical model combining electromagnetic wave propagation, charge transport and conservation in the particles, semiconductor-electrolyte charge transfer(3) and approximating the morphology by equivalent pillars. Experimental results showed higher photocurrent under back illumination compared to front illumination. The 2D numerical model confirmed this behaviour, i.e. hole transport was not limiting but rather the electron transport towards the collector leading to improved photocurrents for back illumination. The numerical model was then used to explore the impact of co-catalyst deposition, surface passivation, necking procedure, and modification of bulk material properties on the performance of particle-based PE.
The combined experimental-numerical approach allowed for the identification and quantification of material challenges and design considerations in particle-based PE. Future investigation using a more complex geometry in the computational model will be undertaken to provide potential performance improvement resulting from the particle morphology.
References
(1) M. Dumortier, S. Tembhurne and S. Haussener, Energy Environ. Sci., 2015, 3614–3628.
(2) S. Landsmann, A. E. Maegli, M. Trottmann, C. Battaglia, A. Weidenkaff and S. Pokrant, ChemSusChem, 2015, 8, 3451–3458.
(3) Y. K. Gaudy and S. Haussener, J. Mater. Chem. A, 2016, 4, 3100–3114.
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