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Dynamics and Photochemical H-2 Evolution of Dye-NiO Photocathodes with a Biomimetic FeFe-Catalyst
Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry.
Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Molecular Biomimetics.
Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry.
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2016 (English)In: ACS ENERGY LETTERS, ISSN 2380-8195, Vol. 1, no 6, 1106-1111 p.Article in journal, Letter (Refereed) Published
Abstract [en]

Mesoporous NiO films were cosensitized with a coumarin 343 dye and a proton reduction catalyst of the [Fe-2(CO)(6)(bdt)] (bdt = benzene-1,2-dithiolate) family. Femtosecond ultraviolet visible transient absorption experiments directly demonstrated subpicosecond hole injection into NiO from excited dyes followed by rapid (t(50%) similar to 6 ps) reduction of the catalyst on the surface with similar to 70% yield. The reduced catalyst was long-lived (2 mu s to 20 ms), which may allow protonation and a second reduction step of the catalyst to occur. A photo electrochemical device based on this photocathode produced H-2 with a Faradaic efficiency of similar to 50%. Fourier transform infrared spectroscopy and gas chromatography experiments demonstrated that the observed device deterioration with time was mainly due to catalyst degradation and desorption from the NiO surface. The insights gained from these mechanistic studies, regarding development of dye-catalyst cosensitized photocathodes, are discussed.

Place, publisher, year, edition, pages
2016. Vol. 1, no 6, 1106-1111 p.
National Category
Physical Chemistry Nano Technology
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URN: urn:nbn:se:uu:diva-313538DOI: 10.1021/acsenergylett.6b00506ISI: 000390086400005OAI: oai:DiVA.org:uu-313538DiVA: diva2:1070390
Funder
Swedish Research CouncilKnut and Alice Wallenberg FoundationSwedish Energy Agency
Available from: 2017-02-01 Created: 2017-01-20 Last updated: 2017-02-15Bibliographically approved

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