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Engineering triple O-Ti-O vacancy associates for efficient water-activation catalysis.

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Researchers precisely fabricated and identified triple oxygen-titanium-oxygen vacancy associates (VOVTiVO) in Ni-doped TiO2 catalysts. This defect engineering enhances water dissociation and catalytic activity for key reactions.

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Area of Science:

  • Materials Science
  • Catalysis
  • Surface Chemistry

Background:

  • Defect engineering in catalysts tunes electronic and geometric structures.
  • Precise control and identification of catalyst defects, especially clustered vacancies, remain challenging.
  • The origin of vacancy configurations is largely unknown.

Purpose of the Study:

  • To achieve controllable fabrication and quantitative identification of triple O-Ti-O vacancy associates (VOVTiVO) in nanosized Ni-doped TiO2.
  • To elucidate the role of these specific vacancy associates in catalytic reactions.
  • To understand the mechanism of defect formation and its impact on active sites.

Main Methods:

  • Controllable fabrication of nanosized Ni-doped TiO2.
  • Quantitative identification of vacancy configurations using experimental and theoretical analyses.
  • In situ studies of hydroxyl adsorption and its role in defect formation.

Main Results:

  • Successfully fabricated and identified triple O-Ti-O vacancy associates (VOVTiVO).
  • Terminal hydroxyls adsorbed at unsaturated cationic sites are crucial for VOVTiVO formation.
  • VOVTiVO enhances H2O dissociation and OH* deprotonation, improving catalytic site regeneration.
  • Single VO sites are prone to saturation by hydroxyls, reducing active site availability.
  • Ni-doped TiO2 with VOVTiVO showed comparable performance in hydrogen evolution and hydrodechlorination reactions.

Conclusions:

  • Terminal hydroxyls play a key role in forming beneficial VOVTiVO defects.
  • VOVTiVO defects are crucial for efficient H2O dissociation and catalyst regeneration.
  • Engineering vacancy-associated active sites is vital for designing high-performance catalysts for H2O-involved reactions.