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Dual Activation of Molecular Oxygen and Surface Lattice Oxygen in Single Atom Cu 1 /TiO 2 Catalyst for CO Oxidation.

Yarong FangQi ZhangHuan ZhangXiaomin LiWei ChenJue XuHuan ShenJi YangChuanqi PanYuhua ZhuJinlong WangZhu LuoLiming WangXuedong BaiFei SongLizhi ZhangYanbing Guo
Published in: Angewandte Chemie (International ed. in English) (2022)
The in-depth mechanism on the simultaneous activation of O 2 and surface lattice O 2- on one active metallic site has not been elucidated yet. Herein, we report a strategy for the construction of abundant oxygen activation sites by rational design of Cu 1 /TiO 2 single atom catalysts (SACs). The charge transfer between isolated Cu and TiO 2 support generates abundant Cu I and 2-coordinated O lat sites in Cu 1 -O-Ti hybridization structure, which facilitates the chemisorption and activation of O 2 molecules. Simultaneously, the Cu 1 -O-Ti induced TiO 2 lattice distortion activate the adjacent surface lattice O 2- , achieving the dual activation of O 2 and surface lattice O 2- . The Cu 1 -O-Ti active site switches the CO oxidation mechanism from Eley-Rideal (80 °C) to Mars-van Krevelen route (200 °C) with the increase of reaction temperature. The dual activation of O 2 and surface lattice O 2- can by modulating the electron properties of SACs can boost the heterogeneous catalytic oxidation activity.
Keyphrases
  • metal organic framework
  • visible light
  • aqueous solution
  • quantum dots
  • hydrogen peroxide
  • molecular dynamics
  • single molecule
  • nitric oxide
  • highly efficient
  • room temperature
  • high density