Interaction of SrO-terminated SrTiO3 surface with oxygen, carbon dioxide, and water

Aleksandar Tsekov Staykov, Shun Fukumori, Kazunari Yoshizawa, Kenta Sato, Tatsumi Ishihara, John Kilner

研究成果: ジャーナルへの寄稿記事

2 引用 (Scopus)

抄録

The interaction of SrO terminated SrTiO3 surface with molecular carbon dioxide and water has been investigated using first-principle theoretical methods and surface analysis techniques. We have studied the formation of a surface SrCO3 layer and various possible products of H2O interaction with the SrO surface, such as, surface chemisorbed water and the formation of a surface hydroxide layer. The co-adsorption of CO2 and H2O was explained both theoretically and experimentally showing that its products follow a complex temperature dependence and as a result, the surface composition may vary between carbonate and surface chemisorbed water. Our theoretical simulations have shown that the presence of water molecules in the gas phase might assist the molecular oxygen/lattice oxygen exchange reaction by stabilization of the surface oxo species in the transition state with a hydrogen bond mechanism. As a result, the activation barrier for molecular oxygen dissociation is decreased leading to an increase in the surface exchange rate constant. Our study demonstrates that the SrO terminated SrTiO3 surface is not static but instead, dynamically responds to external factors such as gas composition, humidity, and temperature. As a result, the surface phases can show different trends for the surface exchange reaction with molecular oxygen by either an increase or decrease in the exchange rate.

元の言語英語
ページ(範囲)22662-22672
ページ数11
ジャーナルJournal of Materials Chemistry A
6
発行部数45
DOI
出版物ステータス出版済み - 1 1 2018

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Carbon Dioxide
Carbon dioxide
Oxygen
Water
Molecular oxygen
Surface waters
Gases
strontium titanium oxide
Carbonates
Surface analysis
Surface structure
Rate constants
Atmospheric humidity
Hydrogen bonds
Stabilization
Chemical activation
Adsorption
Temperature
Molecules
Chemical analysis

All Science Journal Classification (ASJC) codes

  • Chemistry(all)
  • Renewable Energy, Sustainability and the Environment
  • Materials Science(all)

これを引用

Interaction of SrO-terminated SrTiO3 surface with oxygen, carbon dioxide, and water. / Staykov, Aleksandar Tsekov; Fukumori, Shun; Yoshizawa, Kazunari; Sato, Kenta; Ishihara, Tatsumi; Kilner, John.

:: Journal of Materials Chemistry A, 巻 6, 番号 45, 01.01.2018, p. 22662-22672.

研究成果: ジャーナルへの寄稿記事

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AU - Sato, Kenta

AU - Ishihara, Tatsumi

AU - Kilner, John

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AB - The interaction of SrO terminated SrTiO3 surface with molecular carbon dioxide and water has been investigated using first-principle theoretical methods and surface analysis techniques. We have studied the formation of a surface SrCO3 layer and various possible products of H2O interaction with the SrO surface, such as, surface chemisorbed water and the formation of a surface hydroxide layer. The co-adsorption of CO2 and H2O was explained both theoretically and experimentally showing that its products follow a complex temperature dependence and as a result, the surface composition may vary between carbonate and surface chemisorbed water. Our theoretical simulations have shown that the presence of water molecules in the gas phase might assist the molecular oxygen/lattice oxygen exchange reaction by stabilization of the surface oxo species in the transition state with a hydrogen bond mechanism. As a result, the activation barrier for molecular oxygen dissociation is decreased leading to an increase in the surface exchange rate constant. Our study demonstrates that the SrO terminated SrTiO3 surface is not static but instead, dynamically responds to external factors such as gas composition, humidity, and temperature. As a result, the surface phases can show different trends for the surface exchange reaction with molecular oxygen by either an increase or decrease in the exchange rate.

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