Influence of surface restructuring on the activity of SrTiO3 photoelectrodes for photocatalytic hydrogen reduction

Yihuang Xiong, Ismaila Dabo

Research output: Contribution to journalArticle

Abstract

Perovskite photoelectrodes are being extensively studied in search for photocatalytic materials that can produce hydrogen through water splitting. The solar-to-hydrogen efficiency of these materials is critically dependent on the electrochemical state of their surface. Here, we develop an embedded quantum-mechanical approach using the self-consistent continuum solvation model to predict the relation between band alignment, electrochemical stability, and photocatalytic activity taking into account the long-range polarization of the semiconductor electrode under electrical bias. Using this comprehensive model, we calculate the charge-voltage response of various reconstructions of a solvated SrTiO3 surface, revealing that interfacial charge trapping exerts primary control on the electrical response and surface stability of the photoelectrode. Our results provide a detailed molecular-level interpretation of the enhanced photocatalytic activity of SrTiO3 upon voltage-induced restructuring of the semiconductor-solution interface.

Original languageEnglish (US)
Article number065801
JournalPhysical Review Materials
Volume3
Issue number6
DOIs
StatePublished - Jun 17 2019

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Hydrogen
surface stability
water splitting
electric potential
hydrogen
Semiconductor materials
solvation
Charge trapping
trapping
alignment
Solvation
Electric potential
continuums
Perovskite
electrodes
polarization
Polarization
Electrodes
Water
strontium titanium oxide

All Science Journal Classification (ASJC) codes

  • Materials Science(all)
  • Physics and Astronomy (miscellaneous)

Cite this

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title = "Influence of surface restructuring on the activity of SrTiO3 photoelectrodes for photocatalytic hydrogen reduction",
abstract = "Perovskite photoelectrodes are being extensively studied in search for photocatalytic materials that can produce hydrogen through water splitting. The solar-to-hydrogen efficiency of these materials is critically dependent on the electrochemical state of their surface. Here, we develop an embedded quantum-mechanical approach using the self-consistent continuum solvation model to predict the relation between band alignment, electrochemical stability, and photocatalytic activity taking into account the long-range polarization of the semiconductor electrode under electrical bias. Using this comprehensive model, we calculate the charge-voltage response of various reconstructions of a solvated SrTiO3 surface, revealing that interfacial charge trapping exerts primary control on the electrical response and surface stability of the photoelectrode. Our results provide a detailed molecular-level interpretation of the enhanced photocatalytic activity of SrTiO3 upon voltage-induced restructuring of the semiconductor-solution interface.",
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Influence of surface restructuring on the activity of SrTiO3 photoelectrodes for photocatalytic hydrogen reduction. / Xiong, Yihuang; Dabo, Ismaila.

In: Physical Review Materials, Vol. 3, No. 6, 065801, 17.06.2019.

Research output: Contribution to journalArticle

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AU - Xiong, Yihuang

AU - Dabo, Ismaila

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AB - Perovskite photoelectrodes are being extensively studied in search for photocatalytic materials that can produce hydrogen through water splitting. The solar-to-hydrogen efficiency of these materials is critically dependent on the electrochemical state of their surface. Here, we develop an embedded quantum-mechanical approach using the self-consistent continuum solvation model to predict the relation between band alignment, electrochemical stability, and photocatalytic activity taking into account the long-range polarization of the semiconductor electrode under electrical bias. Using this comprehensive model, we calculate the charge-voltage response of various reconstructions of a solvated SrTiO3 surface, revealing that interfacial charge trapping exerts primary control on the electrical response and surface stability of the photoelectrode. Our results provide a detailed molecular-level interpretation of the enhanced photocatalytic activity of SrTiO3 upon voltage-induced restructuring of the semiconductor-solution interface.

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