Shining light into the reaction mechanisms of non-ideal metal oxides.

James Durrant^a, Stephanie Pendlebury^a, Camilo Mesa^a, Ernest Pastor^a, Laia Francàs Forcada^a, Yimeng Ma^a^,^b, Andreas Kafizas^a^,^c, Florian Le Formal^a^,^d

^aImperial College London, United Kingdom, South Kensington, Londres, Reino Unido, United Kingdom

^bHelmholtz-Zentrum Berlin für Materialien und Energie GmbH, Germany, Berlin, Germany

^cUniversity College London UCL, Torrington Place, United Kingdom

^dEcole Polytechnique Federale de Lausanne (EPFL), Lausanne, Switzerland

Materials for Sustainable Development Conference (MATSUS)
Proceedings of September Meeting 2016 (NFM16)

Berlin, Germany, 2016 September 5th - 13th

Organizers: Marin Alexe, Enrique Cánovas, Celso de Mello Donega, Ivan Infante, Thomas Kirchartz, Maksym Kovalenko, Federico Rosei, Lukas Schmidt-Mende, Laurens Siebbeles, Peter Strasser, Teodor K Todorov, Roel van de Krol and Ulrike Woggon

Oral, Laia Francàs Forcada, presentation 046
Publication date: 14th June 2016

Hydrogen and other solar fuels have been appointed as one of the future energy vectors. Having natural photosynthesis as inspiration, we can develop a device capable to split water using sunlight, obtaining oxygen and hydrogen. [1], [2] Although rapid progress is being made in the field, the efficiency of artificial systems still remains modest. Several metal oxides semiconductors have been shown to be good candidates to carry out the reactions of Water oxidation (α-Fe₂O₃, BiVO₄, TiO₂) and Proton reduction (Cu₂O structures). Understanding of the limiting factors of these materials has allowed remarkable improvements in their performance. However, compared to molecular systems, whose reaction mechanisms are better understood, there is still a lack of knowledge in metal oxides mechanism of action. In this talk is I will focus on the use of the combined electrochemical and optical technique (PIAS) to probe the catalytic function of semiconductors for solar-to-fuel synthesis [3]. This technique opens a new possibility of studying multielectron reaction mechanisms on non-ideal semiconductors. I will show how using PIAS we can elucidate the rate law of current flow in these systems and how our analysis can shed light in to the reaction mechanism of photoelectrochemical water oxidation and proton reduction reactions. Particularly I will discuss some of the results on α-Fe₂O₃, BiVO₄, TiO₂ as photoanode and Cu₂O structures for proton reduction. All this acquired knowledge will help to depict the mechanism of action of non-ideal semicondutors and so to systematically improve the next generation of photoelectrodes for water splitting.

References:[1] S. Berardi, S. Drouet, L. Francàs, C. Gimbert-Suriñach, M. Guttentag, C. Richmond, T. Stoll, A. Llobet, Chem. Soc. Rev.43 (2014), 7501. [2] Y. Tachibana, L. Vayssieres, James R. DurrantNature photonics 5 (2012), 511.[3] F. Le Formal, E. Pastor, S. D. Tilley, C. A. Mesa, S. R. Pendlebury, M. Grätzel and J. R. Durrant, J. Am. Chem. Soc. 137 (2015), 6629.

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