Electrolysis of water at SrTiO3 photoelectrodes

Distinguishing between the statistical and stochastic formalisms for electron-transfer processes in fuel-forming photoelectrochemical systems

Amit Kumar, Patrick G. Santangelo, Nathan S Lewis

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Abstract

Conventional photoelectrochemical and photovoltaic theory predicts a light intensity threshold for sustaining the net electrolysis of water using semiconductor electrodes, but a stochastic charge-transfer formalism for photoelectrolysis reactions does not predict such threshold behavior. This work examines the theoretical and experimental aspects of light-assisted water electrolysis using n-type SrTiO3/H2O interfaces. A theoretical framework, based upon simple chemical kinetic considerations, has been formulated to describe the behavior of such photoelectrosynthetic cells. Experiments conducted on the n-SrTiO3/5.0 M NaOH(aq)/Pt photoelectrosynthetic cell have revealed a threshold in the short-circuit electrolysis current at 5 × 10-5 W/cm2 of 325-nm illumination. Additional theory and experiments have provided insight into relationships between two-electrode regenerative photoelectrochemical cells, two-electrode photoelectrosynthetic cells, and three-electrode potentiostatic cells. These experiments and theory indicate that a conventional chemical kinetic treatment of interfacial electron-transfer rates appears to be sufficient to describe the photoelectrochemical behavior of SrTiO3 and TiO2/aqueous junctions.

Original languageEnglish
Pages (from-to)834-842
Number of pages9
JournalJournal of Physical Chemistry
Volume96
Issue number2
Publication statusPublished - 1992

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electrolysis
Electrolysis
electron transfer
Electrodes
Electrons
Water
cells
Reaction kinetics
electrodes
water
thresholds
Photoelectrochemical cells
reaction kinetics
Experiments
Short circuit currents
sustaining
short circuits
Charge transfer
Lighting
luminous intensity

ASJC Scopus subject areas

  • Physical and Theoretical Chemistry

Cite this

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title = "Electrolysis of water at SrTiO3 photoelectrodes: Distinguishing between the statistical and stochastic formalisms for electron-transfer processes in fuel-forming photoelectrochemical systems",
abstract = "Conventional photoelectrochemical and photovoltaic theory predicts a light intensity threshold for sustaining the net electrolysis of water using semiconductor electrodes, but a stochastic charge-transfer formalism for photoelectrolysis reactions does not predict such threshold behavior. This work examines the theoretical and experimental aspects of light-assisted water electrolysis using n-type SrTiO3/H2O interfaces. A theoretical framework, based upon simple chemical kinetic considerations, has been formulated to describe the behavior of such photoelectrosynthetic cells. Experiments conducted on the n-SrTiO3/5.0 M NaOH(aq)/Pt photoelectrosynthetic cell have revealed a threshold in the short-circuit electrolysis current at 5 × 10-5 W/cm2 of 325-nm illumination. Additional theory and experiments have provided insight into relationships between two-electrode regenerative photoelectrochemical cells, two-electrode photoelectrosynthetic cells, and three-electrode potentiostatic cells. These experiments and theory indicate that a conventional chemical kinetic treatment of interfacial electron-transfer rates appears to be sufficient to describe the photoelectrochemical behavior of SrTiO3 and TiO2/aqueous junctions.",
author = "Amit Kumar and Santangelo, {Patrick G.} and Lewis, {Nathan S}",
year = "1992",
language = "English",
volume = "96",
pages = "834--842",
journal = "Journal of Physical Chemistry",
issn = "0022-3654",
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TY - JOUR

T1 - Electrolysis of water at SrTiO3 photoelectrodes

T2 - Distinguishing between the statistical and stochastic formalisms for electron-transfer processes in fuel-forming photoelectrochemical systems

AU - Kumar, Amit

AU - Santangelo, Patrick G.

AU - Lewis, Nathan S

PY - 1992

Y1 - 1992

N2 - Conventional photoelectrochemical and photovoltaic theory predicts a light intensity threshold for sustaining the net electrolysis of water using semiconductor electrodes, but a stochastic charge-transfer formalism for photoelectrolysis reactions does not predict such threshold behavior. This work examines the theoretical and experimental aspects of light-assisted water electrolysis using n-type SrTiO3/H2O interfaces. A theoretical framework, based upon simple chemical kinetic considerations, has been formulated to describe the behavior of such photoelectrosynthetic cells. Experiments conducted on the n-SrTiO3/5.0 M NaOH(aq)/Pt photoelectrosynthetic cell have revealed a threshold in the short-circuit electrolysis current at 5 × 10-5 W/cm2 of 325-nm illumination. Additional theory and experiments have provided insight into relationships between two-electrode regenerative photoelectrochemical cells, two-electrode photoelectrosynthetic cells, and three-electrode potentiostatic cells. These experiments and theory indicate that a conventional chemical kinetic treatment of interfacial electron-transfer rates appears to be sufficient to describe the photoelectrochemical behavior of SrTiO3 and TiO2/aqueous junctions.

AB - Conventional photoelectrochemical and photovoltaic theory predicts a light intensity threshold for sustaining the net electrolysis of water using semiconductor electrodes, but a stochastic charge-transfer formalism for photoelectrolysis reactions does not predict such threshold behavior. This work examines the theoretical and experimental aspects of light-assisted water electrolysis using n-type SrTiO3/H2O interfaces. A theoretical framework, based upon simple chemical kinetic considerations, has been formulated to describe the behavior of such photoelectrosynthetic cells. Experiments conducted on the n-SrTiO3/5.0 M NaOH(aq)/Pt photoelectrosynthetic cell have revealed a threshold in the short-circuit electrolysis current at 5 × 10-5 W/cm2 of 325-nm illumination. Additional theory and experiments have provided insight into relationships between two-electrode regenerative photoelectrochemical cells, two-electrode photoelectrosynthetic cells, and three-electrode potentiostatic cells. These experiments and theory indicate that a conventional chemical kinetic treatment of interfacial electron-transfer rates appears to be sufficient to describe the photoelectrochemical behavior of SrTiO3 and TiO2/aqueous junctions.

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