Proceedings of nanoGe Fall Meeting 2018 (NFM18)
DOI: https://doi.org/10.29363/nanoge.nfm.2018.024
Publication date: 6th July 2018
Recently, Ham et al. reported that aluminum incorporation into SrTiO3 microparticles followed by modification with Rh2-yCryO3 produces a superior overall water splitting catalyst with 30% apparent quantum efficiency at 350 nm. Based on transient IR spectroscopy, the improved activity was attributed to the removal of Ti3+ recombination sites. Here we use results from photoelectron spectroscopy (XPS) and density functional theory to show that Al3+ incorporation into the perovskite lattice not only reduces the number of Ti3+ deep recombination sites and but also promotes the formation of oxygen vacancies in the material. The oxygen vacancies form a mini-band 0.2 eV above the valence band whose energy position strongly depends on the spatial separation between Al3+ sites and oxygen vacancies. The vacancy band is believed to aid photochemical charge separation in this metal oxide. Particle suspensions of the material inside of a baggie reactor promote overall water splitting under direct sunlight illumination with 0.1% solar to hydrogen efficiency.
References
Ham, Y., T. Hisatomi, Y. Goto, Y. Moriya, Y. Sakata, A. Yamakata, J. Kubota, and K. Domen, Flux-Mediated Doping of SrTiO3 Photocatalysts for Efficient Overall Water Splitting. Journal of Materials Chemistry A, 2016. 4(8): p. 3027-3033. http://dx.doi.org/10.1039/C5TA04843E