Single-Electron-Trapped Oxygen Vacancy on Ultrathin WO3·0.33H2O {100} Facets Suppressing Backward Reaction for Promoted H2 Evolution in Pure Water Splitting

Songmei Sun, Ji Wu, Motonori Watanabe, Taner Akbay, Tatsumi Ishihara

Research output: Contribution to journalArticle

Abstract

Solar water splitting to produce hydrogen is a promising solution for global energy issues. One of the main bottlenecks in this technology is the spontaneous fast backward reaction (2H2 + O2 → H2O, ΔG < 0), limiting the solar energy conversion efficiency. How to suppress backward reaction is vitally important but rarely reported. Here we found that single-electron-trapped oxygen vacancy (Vo·) can suppress spontaneous backward reaction in pure water splitting. Taking WO3·0.33H2O catalyst as an example, ultrathin WO3·0.33H2O {100} facets with large amount of surface Vo· realized a continuous H2 evolution from pure water splitting with a productivity of 9.9 μmol/g·h without the assistance of any sacrifice agent and noble metal cocatalyst. Quantum chemical calculations revealed that the backward-reaction suppression ability of Vo· is attributed to the high concentration of localized electrons around Vo·, stimulating unidirectional simultaneous water dissociation into H and OH under light irradiation.

Original languageEnglish
Pages (from-to)2998-3005
Number of pages8
JournalJournal of Physical Chemistry Letters
Volume10
Issue number11
DOIs
Publication statusPublished - Jun 6 2019

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water splitting
Oxygen vacancies
flat surfaces
Electrons
Water
oxygen
electrons
solar energy conversion
Hydrogen
energy conversion efficiency
Precious metals
noble metals
productivity
Energy conversion
Solar energy
Conversion efficiency
Productivity
retarding
Irradiation
dissociation

All Science Journal Classification (ASJC) codes

  • Materials Science(all)
  • Physical and Theoretical Chemistry

Cite this

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title = "Single-Electron-Trapped Oxygen Vacancy on Ultrathin WO3·0.33H2O {100} Facets Suppressing Backward Reaction for Promoted H2 Evolution in Pure Water Splitting",
abstract = "Solar water splitting to produce hydrogen is a promising solution for global energy issues. One of the main bottlenecks in this technology is the spontaneous fast backward reaction (2H2 + O2 → H2O, ΔG < 0), limiting the solar energy conversion efficiency. How to suppress backward reaction is vitally important but rarely reported. Here we found that single-electron-trapped oxygen vacancy (Vo·) can suppress spontaneous backward reaction in pure water splitting. Taking WO3·0.33H2O catalyst as an example, ultrathin WO3·0.33H2O {100} facets with large amount of surface Vo· realized a continuous H2 evolution from pure water splitting with a productivity of 9.9 μmol/g·h without the assistance of any sacrifice agent and noble metal cocatalyst. Quantum chemical calculations revealed that the backward-reaction suppression ability of Vo· is attributed to the high concentration of localized electrons around Vo·, stimulating unidirectional simultaneous water dissociation into H and OH under light irradiation.",
author = "Songmei Sun and Ji Wu and Motonori Watanabe and Taner Akbay and Tatsumi Ishihara",
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T1 - Single-Electron-Trapped Oxygen Vacancy on Ultrathin WO3·0.33H2O {100} Facets Suppressing Backward Reaction for Promoted H2 Evolution in Pure Water Splitting

AU - Sun, Songmei

AU - Wu, Ji

AU - Watanabe, Motonori

AU - Akbay, Taner

AU - Ishihara, Tatsumi

PY - 2019/6/6

Y1 - 2019/6/6

N2 - Solar water splitting to produce hydrogen is a promising solution for global energy issues. One of the main bottlenecks in this technology is the spontaneous fast backward reaction (2H2 + O2 → H2O, ΔG < 0), limiting the solar energy conversion efficiency. How to suppress backward reaction is vitally important but rarely reported. Here we found that single-electron-trapped oxygen vacancy (Vo·) can suppress spontaneous backward reaction in pure water splitting. Taking WO3·0.33H2O catalyst as an example, ultrathin WO3·0.33H2O {100} facets with large amount of surface Vo· realized a continuous H2 evolution from pure water splitting with a productivity of 9.9 μmol/g·h without the assistance of any sacrifice agent and noble metal cocatalyst. Quantum chemical calculations revealed that the backward-reaction suppression ability of Vo· is attributed to the high concentration of localized electrons around Vo·, stimulating unidirectional simultaneous water dissociation into H and OH under light irradiation.

AB - Solar water splitting to produce hydrogen is a promising solution for global energy issues. One of the main bottlenecks in this technology is the spontaneous fast backward reaction (2H2 + O2 → H2O, ΔG < 0), limiting the solar energy conversion efficiency. How to suppress backward reaction is vitally important but rarely reported. Here we found that single-electron-trapped oxygen vacancy (Vo·) can suppress spontaneous backward reaction in pure water splitting. Taking WO3·0.33H2O catalyst as an example, ultrathin WO3·0.33H2O {100} facets with large amount of surface Vo· realized a continuous H2 evolution from pure water splitting with a productivity of 9.9 μmol/g·h without the assistance of any sacrifice agent and noble metal cocatalyst. Quantum chemical calculations revealed that the backward-reaction suppression ability of Vo· is attributed to the high concentration of localized electrons around Vo·, stimulating unidirectional simultaneous water dissociation into H and OH under light irradiation.

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