Journal
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
Volume 12, Issue 28, Pages 6519-6525Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpclett.1c01584
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Funding
- National Natural Science Foundation of China [22022308, 21773254]
- Youth Innovation Promotion Association CAS [Y202007]
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The study identifies the formation of quadruple bonding interactions in a gas-phase ion IrV+, enabling the oxidation of four CO molecules by IrVO4+. This finding overturns the general impression on the mechanism of CO oxidation by vanadium oxide clusters.
The generation and characterization of multiple metal-metal (M-M) bonds between early and late transition metals is vital to correlate the nature of multiple M-M bonds with the related reactivity in catalysis, while the examples with multiple M-M bonds have been rarely reported. Herein, we identified that the quadruple bonding interactions were formed in a gas-phase ion IrV+ with a dramatically short Ir-V bond. Oxidation of four CO molecules by IrVO4+ is a highly exothermic process driven by the generation of stable products IrV+ and CO2, and then IrV+ can be oxidized by N2O to regenerate IrVO4+. This finding overturns the general impression that vanadium oxide clusters are unwilling to oxidize multiple CO molecules because of the strong V-O bond and that at most two oxygen atoms can be supplied from a single V-containing cluster in CO oxidation. This study emphasizes the potential importance of heterobimetallic multiple M-M bonds in related heterogeneous catalysis.
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