Interfacial charge transfer dynamics in TiO2-sensitizer-Ru4POM photocatalytic systems for water oxidation

Zhuangqun Huang; Yurii V. Geletii; David Wu; Chantelle L. Anfuso; Djamaladdin G. Musaev; Craig L. Hill; Tianquan Lian

doi:10.1117/12.893079

19 September 2011 Interfacial charge transfer dynamics in TiO₂-sensitizer-Ru₄POM photocatalytic systems for water oxidation

Zhuangqun Huang, Yurii V. Geletii, David Wu, Chantelle L. Anfuso, Djamaladdin G. Musaev, Craig L. Hill, Tianquan Lian

Author Affiliations +

Proceedings Volume 8109, Solar Hydrogen and Nanotechnology VI; 810903 (2011) https://doi.org/10.1117/12.893079
Event: SPIE Solar Energy + Technology, 2011, San Diego, California, United States

Abstract

Efficient solar-driven catalytic water oxidation is one of the main challenges in solar-to-fuel conversion. In this proceeding, we investigate three approaches for constructing electron acceptor -sensitizer - catalysts systems for photocatalytic water oxidation and our current understanding of the relevant fundamental processes involved. We demonstrated that an all-inorganic molecular water oxidation catalyst (WOC), [{Ru₄O₄(OH)₂(H2O)₄}(γ-SiW10O36)2]10- (or Ru₄POM), catalyzed a homogenous O₂ evolution system with 27% quantum efficiency in homogeneous solution in the presence of sensitizer (Ru(bpy)3) and sacrificial electron donor.¹ This suggests the feasibility of a heterogeneous photoelectrochemical system in which the photoanode integrates all three components: electron acceptor, photosensitizer, and WOC. We prepare a photocatalytic electrode based on Ru₄POM and a dye-sensitized nanoporous TiO₂ film for efficient light-harvesting and charge separation. Ultrafast spectroscopic studies of this triadic nanocomposite indicate efficient charge separation from the excited sensitizer to TiO₂ and efficient regeneration of the ground state of the dye. The latter can be attributed to Ru₄POM oxidation by the photogenerated dye cation and has a yield of > 80% within 1 ns.

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Zhuangqun Huang, Yurii V. Geletii, David Wu, Chantelle L. Anfuso, Djamaladdin G. Musaev, Craig L. Hill, and Tianquan Lian "Interfacial charge transfer dynamics in TiO₂-sensitizer-Ru₄POM photocatalytic systems for water oxidation", Proc. SPIE 8109, Solar Hydrogen and Nanotechnology VI, 810903 (19 September 2011); https://doi.org/10.1117/12.893079

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