Dual Activation of Molecular Oxygen and Surface Lattice Oxygen in Single Atom Cu1/TiO2 Catalyst for CO Oxidation. Issue 48 (25th October 2022)

• Record Type: Journal Article
• Authors: Fang, Yarong; Zhang, Qi; Zhang, Huan; Li, Xiaomin; Chen, Wei; Xu, Jue; Shen, Huan; Yang, Ji; Pan, Chuanqi; Zhu, Yuhua; Wang, Jinlong; Luo, Zhu; Wang, Liming; Bai, Xuedong; Song, Fei; Zhang, Lizhi; Guo, Yanbing
• Is Part Of: Angewandte Chemie international edition. Volume 61:Issue 48(2022)
• Page Start: n/a
• Page End: n/a
• Publication Date: 2022-10-25
• Subjects: Activated Surface Lattice Oxygen -- Cu/TiO2 Catalyst -- Dual Activation -- Molecular Oxygen -- Single Atom Catalyst; Chemistry -- Periodicals; 540
• DOI: 10.1002/anie.202212273
• Languages: English
• ISSNs: 1433-7851

Abstract

Abstract: The in‐depth mechanism on the simultaneous activation of O2 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 Cu1 /TiO2 single atom catalysts (SACs). The charge transfer between isolated Cu and TiO2 support generates abundant Cu I and 2‐coordinated Olat sites in Cu1 −O−Ti hybridization structure, which facilitates the chemisorption and activation of O2 molecules. Simultaneously, the Cu1 −O−Ti induced TiO2 lattice distortion activate the adjacent surface lattice O 2−, achieving the dual activation of O2 and surface lattice O 2− . The Cu1 −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 O2 and surface lattice O 2− can by modulating the electron properties of SACs can boost the heterogeneous catalytic oxidation activity. Abstract : The isolated Cu 1+ on Cu1 /TiO2 single atom catalysts (SACs) facilitated the simultaneous activation of chemisorbed O2 and 2‐coordinated surface lattice O 2−, which triggered the CO oxidation through E‐R (80 °C) and MvK (200 °C) routes synergistically with elevated temperature. This finding provides insights and strategy for the rational design of efficient oxidation catalysts with sufficient reactive oxygen species for practical application.