Recently, Jiang Ling, researcher Jiang Ling, associate researcher Xie Hua of the State Key Laboratory of Molecular Reaction Dynamics (Group 1112), Dalian Institute of Chemical Physics, Chinese Academy of Sciences, and associate professor Liu Zhiling, School of Chemistry and Materials Science, Shanxi Normal University, New progress has been made in the study of the oxidation mechanism of carbon monoxide, and related research results are published in The Journal of Physical Chemistry Letters in the form of Supplementary Journal Cover.
As one of the important prototype reactions, the carbon monoxide (CO) oxidation reaction has attracted great attention in heterogeneous catalysis. Recent studies have shown that transition metal oxides have good catalytic properties for CO oxidation, and the reactivity of peripheral oxygen is more competitive than bridge oxygen. However, the microscopic mechanism of CO oxidation by co-adsorbed CO molecules has yet to be further studied. Using cluster spectroscopy experimental methods, key reaction intermediates can be detected in situ from the microscopic atomic and molecular scale, and their size, geometry and electronic structure, metal oxidation valence state, etc. on the reaction activity and mechanism can be studied to reveal the catalysis The reaction mechanism is of great significance.
In this work, researchers took the carbonyl complex ion of niobium nickel monooxygen as the research object and found that co-adsorbed CO ligands played an important role in CO oxidation. Using an independently developed cluster mass spectrometry and photoelectron imaging spectroscopy combined experimental device, NbNiO (CO) n-key reaction intermediates were successfully detected. The results show that during the continuous carbonylation of NbNiO, when n≤6, the CO ligand is coordinated to the metal core, and the oxygen atom on the metal monooxygen remains in the form of bridge oxygen; while when n≥7 The bridge oxygen migrates to the CO ligand to form CO2 ligand, which realizes CO oxidation. Theoretical calculations show that the continuously adsorbed CO ligands compete with bridge oxygen on the one hand for chemical bonding with the metal core, which promotes oxygen migration and on the other hand promotes the charge accumulation of metal atoms. This study deepened the understanding of the carbon monoxide oxidation reaction mechanism.
The above research work was supported by the National Natural Science Foundation of China Science Center project, general project, Chinese Academy of Sciences Class B strategic leading science and technology special projects.
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