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• W4200242521 abstract "Undercoordinated, bridging O-atoms (Obr) are highly active as H-acceptors in alkane dehydrogenation on IrO2(110) surfaces but transform to HObrgroups that are inactive toward hydrocarbons. The low C-H activity and high stability of the HObrgroups cause the kinetics and product selectivity during CH4oxidation on IrO2(110) to depend sensitively on the availability of Obratoms prior to the onset of product desorption. From temperature programmed reaction spectroscopy (TPRS) and kinetic simulations, we identified two Obr-coverage regimes that distinguish the kinetics and product formation during CH4oxidation on IrO2(110). Under excess Obrconditions, when the initial Obrcoverage is greater than that needed to oxidize all the CH4to CO2and HObrgroups, complete CH4oxidation is dominant and produces CO2in a single TPRS peak between 450 and 500 K. However, under Obr-limited conditions, nearly all the initial Obratoms are deactivated by conversion to HObror abstracted after only a fraction of the initially adsorbed CH4oxidizes to CO2and CO below 500 K. Thereafter, some of the excess CHxgroups abstract H and desorb as CH4above ∼500 K while the remainder oxidize to CO2and CO at a rate that is controlled by the rate at which Obratoms are regenerated from HObrduring the formation of CH4and H2O products. We also show that chemisorbed O-atoms ('on-top O') on IrO2(110) enhance CO2production below 500 K by efficiently abstracting H from Obratoms and thereby increasing the coverage of Obratoms available to completely oxidize CHxgroups at low temperature. Our results provide new insights for understanding factors which govern the kinetics and selectivity during CH4oxidation on IrO2(110) surfaces." @default.
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• W4200242521 date "2022-05-13" @default.
• W4200242521 modified "2023-10-14" @default.
• W4200242521 title "Kinetics and selectivity of methane oxidation on an IrO₂(110) film" @default.
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• W4200242521 doi "https://doi.org/10.1088/1361-648x/ac449f" @default.
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