Dual Activation of Molecular Oxygen and Surface Lattice Oxygen in Single Atom Cu1/TiO2 Catalyst for CO Oxidation
The in‐depth mechanism on the simultaneous activation of O2 and surface lattice O2− 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 t...
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Published in | Angewandte Chemie International Edition Vol. 61; no. 48; pp. e202212273 - n/a |
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Main Authors | , , , , , , , , , , , , , , , , |
Format | Journal Article |
Language | English |
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Abstract | The in‐depth mechanism on the simultaneous activation of O2 and surface lattice O2− 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 CuI 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 O2−, achieving the dual activation of O2 and surface lattice O2−. 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 O2− can by modulating the electron properties of SACs can boost the heterogeneous catalytic oxidation activity.
The isolated Cu1+ on Cu1/TiO2 single atom catalysts (SACs) facilitated the simultaneous activation of chemisorbed O2 and 2‐coordinated surface lattice O2−, 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. |
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AbstractList | The in‐depth mechanism on the simultaneous activation of O2 and surface lattice O2− 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 CuI 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 O2−, achieving the dual activation of O2 and surface lattice O2−. 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 O2− can by modulating the electron properties of SACs can boost the heterogeneous catalytic oxidation activity. The in‐depth mechanism on the simultaneous activation of O2 and surface lattice O2− 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 CuI 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 O2−, achieving the dual activation of O2 and surface lattice O2−. 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 O2− can by modulating the electron properties of SACs can boost the heterogeneous catalytic oxidation activity. The isolated Cu1+ on Cu1/TiO2 single atom catalysts (SACs) facilitated the simultaneous activation of chemisorbed O2 and 2‐coordinated surface lattice O2−, 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. |
Author | Zhang, Lizhi Zhang, Qi Bai, Xuedong Guo, Yanbing Li, Xiaomin Wang, Liming Xu, Jue Yang, Ji Zhu, Yuhua Chen, Wei Zhang, Huan Luo, Zhu Shen, Huan Pan, Chuanqi Fang, Yarong Wang, Jinlong Song, Fei |
Author_xml | – sequence: 1 givenname: Yarong surname: Fang fullname: Fang, Yarong organization: Central China Normal University – sequence: 2 givenname: Qi surname: Zhang fullname: Zhang, Qi organization: Central China Normal University – sequence: 3 givenname: Huan surname: Zhang fullname: Zhang, Huan organization: Chinese Academy of Sciences – sequence: 4 givenname: Xiaomin surname: Li fullname: Li, Xiaomin organization: Chinese Academy of Sciences – sequence: 5 givenname: Wei surname: Chen fullname: Chen, Wei organization: Central China Normal University – sequence: 6 givenname: Jue surname: Xu fullname: Xu, Jue organization: Central China Normal University – sequence: 7 givenname: Huan surname: Shen fullname: Shen, Huan organization: Central China Normal University – sequence: 8 givenname: Ji surname: Yang fullname: Yang, Ji organization: Central China Normal University – sequence: 9 givenname: Chuanqi surname: Pan fullname: Pan, Chuanqi organization: Central China Normal University – sequence: 10 givenname: Yuhua surname: Zhu fullname: Zhu, Yuhua organization: Central China Normal University – sequence: 11 givenname: Jinlong surname: Wang fullname: Wang, Jinlong organization: Central China Normal University – sequence: 12 givenname: Zhu surname: Luo fullname: Luo, Zhu organization: Central China Normal University – sequence: 13 givenname: Liming surname: Wang fullname: Wang, Liming organization: Chinese Academy of Sciences – sequence: 14 givenname: Xuedong surname: Bai fullname: Bai, Xuedong organization: Chinese Academy of Sciences – sequence: 15 givenname: Fei surname: Song fullname: Song, Fei organization: Chinese Academy of Sciences – sequence: 16 givenname: Lizhi surname: Zhang fullname: Zhang, Lizhi organization: Central China Normal University – sequence: 17 givenname: Yanbing orcidid: 0000-0002-5399-1739 surname: Guo fullname: Guo, Yanbing email: guoyanbing@mail.ccnu.edu.cn organization: Central China Normal University |
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Snippet | The in‐depth mechanism on the simultaneous activation of O2 and surface lattice O2− on one active metallic site has not been elucidated yet. Herein, we report... |
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SubjectTerms | Activated Surface Lattice Oxygen Carbon monoxide Catalysts Charge transfer Chemisorption Copper Cu/TiO2 Catalyst Dual Activation Hybridization Molecular Oxygen Oxidation Oxygen Single Atom Catalyst Single atom catalysts Switches Titanium Titanium dioxide |
Title | Dual Activation of Molecular Oxygen and Surface Lattice Oxygen in Single Atom Cu1/TiO2 Catalyst for CO Oxidation |
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