Sensitization of Nanocrystalline Metal Oxides with a Phosphonate-Functionalized Perylene Diimide for Photoelectrochemical Water Oxidation with a CoO x Catalyst

Kirner, Joel T.; Finke, Richard G.

doi:10.1021/acsami.7b05874

Title: Sensitization of Nanocrystalline Metal Oxides with a Phosphonate-Functionalized Perylene Diimide for Photoelectrochemical Water Oxidation with a CoO _x Catalyst

Journal Article · Thu Jul 20 00:00:00 EDT 2017 · ACS Applied Materials and Interfaces

DOI:https://doi.org/10.1021/acsami.7b05874· OSTI ID:1415254

Kirner, Joel T. ^[1];

^[1]

Colorado State Univ., Fort Collins, CO (United States). Dept. of Chemistry

A planar organic thin film composed of a perylene diimide dye (N,N'-bis(phosphonomethyl)-3,4,9,10-perylenediimide, PMPDI) with photoelectrochemically deposited cobalt oxide (CoO_x) catalyst was previously shown to photoelectrochemically oxidize water (DOI: 10.1021/am405598w). Herein, the same PMPDI dye is studied for the sensitization of different nanostructured metal oxide (nano-MO_x) films in a dye-sensitized photoelectrochemical cell architecture. Dye adsorption kinetics and saturation decreases in the order TiO₂ > SnO₂ >> WO₃. Despite highest initial dye loading on TiO₂ films, photocurrent with hydroquinone (H₂Q) sacrificial reductant in pH 7 aqueous solution is much higher on SnO₂ films, likely due to a higher driving force for charge injection into the more positive conduction band energy of SnO₂. Dyeing conditions and SnO₂ film thickness were subsequently optimized to achieve light-harvesting efficiency >99% at the λmax of the dye, and absorbed photon-to-current efficiency of 13% with H₂Q, a 2-fold improvement over the previous thin-film architecture. A CoO_x water-oxidation catalyst was photoelectrochemically deposited, allowing for photoelectrochemical water oxidation with a faradaic efficiency of 31 ± 7%, thus demonstrating the second example of a water-oxidizing, dye-sensitized photoelectrolysis cell composed entirely of earth-abundant materials. However, deposition of CoO_x always results in lower photocurrent due to enhanced recombination between catalyst and photoinjected electrons in SnO₂, as confirmed by open-circuit photovoltage measurements. Possible future studies to enhance photoanode performance are also discussed, including alternative catalyst deposition strategies or structural derivatization of the perylene dye.

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Research Organization:: Colorado State Univ., Fort Collins, CO (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: FG02-04ER15591; CHE-1057723

OSTI ID:: 1415254

Alternate ID(s):: OSTI ID: 1429611

Journal Information:: ACS Applied Materials and Interfaces, Journal Name: ACS Applied Materials and Interfaces Vol. 9 Journal Issue: 33; ISSN 1944-8244

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 35 works

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75 CONDENSED MATTER PHYSICS
SUPERCONDUCTIVITY AND SUPERFLUIDITY
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
77 NANOSCIENCE AND NANOTECHNOLOGY
dye-sensitized photoelectrochemical cell
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Title: Sensitization of Nanocrystalline Metal Oxides with a Phosphonate-Functionalized Perylene Diimide for Photoelectrochemical Water Oxidation with a CoO x Catalyst

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Title: Sensitization of Nanocrystalline Metal Oxides with a Phosphonate-Functionalized Perylene Diimide for Photoelectrochemical Water Oxidation with a CoO _x Catalyst