Dynamics and Photochemical H2 Evolution of Dye-NiO Photocathodes with a Biomimetic FeFe-Catalyst

Liisa J. Antila, Pedram Ghamgosar, Somnath Maji, Haining Tian, Sascha Ott, Leif Hammarström

Research output: Contribution to journalArticle

33 Citations (Scopus)

Abstract

Mesoporous NiO films were cosensitized with a coumarin 343 dye and a proton reduction catalyst of the [Fe2(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 (t50% ∼ 6 ps) reduction of the catalyst on the surface with a ∼70% yield. The reduced catalyst was long-lived (2 μs to 20 ms), which may allow protonation and a second reduction step of the catalyst to occur. A photoelectrochemical device based on this photocathode produced H2 with a Faradaic efficiency of ∼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.

Original languageEnglish
Pages (from-to)1106-1111
Number of pages6
JournalACS Energy Letters
Volume1
Issue number6
DOIs
Publication statusPublished - Dec 9 2016

Fingerprint

Photocathodes
Biomimetics
Coloring Agents
Dyes
Catalysts
Protonation
Carbon Monoxide
Benzene
Gas chromatography
Fourier transform infrared spectroscopy
Deterioration
Protons
Desorption
Experiments
Degradation

ASJC Scopus subject areas

  • Chemistry (miscellaneous)
  • Energy Engineering and Power Technology
  • Fuel Technology
  • Renewable Energy, Sustainability and the Environment
  • Materials Chemistry

Cite this

Dynamics and Photochemical H2 Evolution of Dye-NiO Photocathodes with a Biomimetic FeFe-Catalyst. / Antila, Liisa J.; Ghamgosar, Pedram; Maji, Somnath; Tian, Haining; Ott, Sascha; Hammarström, Leif.

In: ACS Energy Letters, Vol. 1, No. 6, 09.12.2016, p. 1106-1111.

Research output: Contribution to journalArticle

Antila, Liisa J. ; Ghamgosar, Pedram ; Maji, Somnath ; Tian, Haining ; Ott, Sascha ; Hammarström, Leif. / Dynamics and Photochemical H2 Evolution of Dye-NiO Photocathodes with a Biomimetic FeFe-Catalyst. In: ACS Energy Letters. 2016 ; Vol. 1, No. 6. pp. 1106-1111.
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