Unravelling the interfacial water structure at the photocatalyst strontium titanate by sum frequency generation spectroscopy

The direct conversion of solar energy to hydrogen is considered as a possible method to produce carbon neutral hydrogen fuel. The mechanism of photocatalytic water splitting involves the chemical breakdown of water and re-assembly into hydrogen and oxygen at the interface of a photocatalyst. The sel...

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Veröffentlicht in:Physical chemistry chemical physics : PCCP 2023-11, Vol.25 (45), p.31471-3148
Hauptverfasser: Buessler, Martin, Maruyama, Shingo, Zelenka, Moritz, Onishi, Hiroshi, Backus, Ellen H.G
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Sprache:eng
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Zusammenfassung:The direct conversion of solar energy to hydrogen is considered as a possible method to produce carbon neutral hydrogen fuel. The mechanism of photocatalytic water splitting involves the chemical breakdown of water and re-assembly into hydrogen and oxygen at the interface of a photocatalyst. The selection rules of a suitable material are well established, but the fundamental understanding of the mechanisms, occurring at the interface between the catalyst and the water, remains missing. Using surface specific sum frequency generation spectroscopy, we present here characterisation of the interface between water and the photocatalyst strontium titanate (SrTiO 3 ). We monitor the OH-stretching vibrations present at the interface. Their variations of intensities and frequencies as functions of isotopic dilution, pH and salt concentration provide information about the nature of the hydrogen bonding environment. We observe the presence of water molecules that flip their orientation at pH 5 indicating the point of zero charge of the SrTiO 3 layer. These water molecules are oriented with their hydrogen away from the surface when the pH of the solutions is below 5 and pointing towards the surface when the pH is higher than 5. Besides, water molecules donating a H-bond to probably surface TiOH groups are observed at all pH. Unravelling the water structure at the interface between the photocatalyst strontium titanate and water by sum frequency generation spectroscopy.
ISSN:1463-9076
1463-9084
DOI:10.1039/d3cp03829g