Light-driven water oxidation by a dye-sensitized photoanode with a chromophore/catalyst assembly on a mesoporous double-shell electrode

Liu, Qing; Wang, Degao; Shan, Bing; Sherman, Benjamin D.; Marquard, Seth L.; Eberhart, Michael S.; Liu, Meichuan; Li, Chunhui; Meyer, Thomas J.

doi:10.1063/1.5048780

Title: Light-driven water oxidation by a dye-sensitized photoanode with a chromophore/catalyst assembly on a mesoporous double-shell electrode

Journal Article · Fri Jan 04 00:00:00 EST 2019 · Journal of Chemical Physics

DOI:https://doi.org/10.1063/1.5048780· OSTI ID:1566651

Liu, Qing ^[1]; Wang, Degao ^[1]; Shan, Bing ^[1]; Sherman, Benjamin D. ^[2]; Marquard, Seth L. ^[1];

^[1]; Liu, Meichuan ^[3]; Li, Chunhui ^[4];

^[1]

Univ. of North Carolina, Chapel Hill, NC (United States). Dept. of Chemistry
Texas Christian Univ., Fort Worth, TX (United States). Dept. of Chemistry
Univ. of North Carolina, Chapel Hill, NC (United States). Dept. of Chemistry; Tongji Univ., Shanghai (China)
Univ. of North Carolina, Chapel Hill, NC (United States). Dept. of Chemistry; Zhengzou Univ., Henan (China). Dept. of Chemistry

A mesoporous atomic layer deposition (ALD) double-shell electrode, Al₂O₃ (insulating core)//ALD ZnO|ALD TiO₂, on a fluorine-doped tin oxide (FTO) conducting substrate was explored for a photoanode assembly, FTO//Al₂O₃ (insulating core)//ALD ZnO|ALD TiO₂|–chromophore–catalyst, for light-driven water oxidation. Photocurrent densities at photoanodes based on mesoporous ALD double-shell (ALD ZnO|ALD TiO₂|) and ALD single-shell (ALD ZnO|, ALD TiO₂|) electrodes were investigated for O₂ evaluation by a generator–collector dual working electrode configuration. The high photocurrent densities obtained based on the mesoporous ALD ZnO|ALD TiO₂ photoanode for O₂ evolution arise from a significant barrier to back electron transfer (BET) by the optimized tunneling barrier in the structure with the built-in electric field at the ALD ZnO|ALD TiO₂ interface. The charge recombination is thus largely decreased. Finally, in the films, BET following injection has been investigated through kinetic nanosecond transient absorption spectra, and the results of energy band analysis are used to derive insight into the internal electronic structure of the electrodes.

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Research Organization:: Energy Frontier Research Centers (EFRC) (United States). Alliance for Molecular PhotoElectrode Design for Solar Fuels (AMPED); University of North Carolina, Chapel Hill, NC (United States)

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

Grant/Contract Number:: SC0001011

OSTI ID:: 1566651

Journal Information:: Journal of Chemical Physics, Vol. 150, Issue 4; ISSN 0021-9606

Publisher:: American Institute of Physics (AIP)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 5 works

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
catalysis (homogeneous)
catalysis (heterogeneous)
electrocatalysis
solar (fuels)
photosynthesis (natural and artificial)
defects
charge transport
materials and chemistry by design
mesostructured materials
synthesis (novel materials)
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Title: Light-driven water oxidation by a dye-sensitized photoanode with a chromophore/catalyst assembly on a mesoporous double-shell electrode

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