Catalytic CO Oxidation by Noble-Metal-Free Ni2 VO4,5- Clusters: A CO Self-Promoted Mechanism

The Journal of Physical Chemistry Letters
Li-Na WangSheng-Gui He

Abstract

Catalytic CO oxidation is an important model reaction in gas-phase studies to provide a clear structure-reactivity understanding in related heterogeneous catalysis, whereas CO oxidation catalyzed by noble-metal (NM) free species has been scarcely reported, and the fundamental aspects are elusive. Herein a CO self-promoted mechanism of catalytic CO oxidation by O2 mediated with the Ni2VO4,5- clusters was experimentally identified and theoretically rationalized. The catalysis was characterized by mass spectrometry and quantum chemistry calculations. Ni2VO5- can oxidize CO to generate an oxygen-deficient product Ni2VO4-, which can only adsorb CO to give rise to Ni2VO4CO-, and the oxidative reactivity of Ni2VO4- can be boosted by the adsorbed  CO. This finding reinforces the significance that the attached CO can modify the electronic structure of the Ni2 unit in Ni2VO4CO- and make the Ni2 unit behave like NM atoms to store the released electrons in an oxygen atom transfer process.

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Citations

Oct 22, 2020·Dalton Transactions : an International Journal of Inorganic Chemistry·Zhiling LiuZichao Tang
Apr 27, 2021·The Journal of Physical Chemistry. a·Yun-Zhu LiuSheng-Gui He
Jul 10, 2021·The Journal of Physical Chemistry Letters·Le-Shi ChenSheng-Gui He
Jan 14, 2020·The Journal of Physical Chemistry. a·Zhiling LiuZichao Tang
Mar 4, 2020·Journal of the American Chemical Society·Nikita LevinUeli Heiz
Jul 18, 2019·The Journal of Physical Chemistry. a·Xiao-Na LiSheng-Gui He

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