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- W2069937019 abstract "The mechanism of the H2-assisted selective catalytic reduction of NO with propane (H2−C3H8 SCR) over Ag+-exchanged MFI zeolite (Ag−MFI) was investigated by spectroscopic studies. Transient IR experiments at 573 K indicate that H2 addition increases the rates of C3H8 oxidation to acetate on Ag−MFI and NO oxidation to the weakly adsorbed NO2. IR spectra obtained during steady-state C3H8 SCR indicate that H2 addition increases the coverage of acetate, Ag+−NCO, and Al3+−NCO. The reaction of acetate with NO2 yields, via CH3NO2, NCO species, and their hydrolysis yields NH3 as a final precursor of N2. In situ UV−vis and EXAFS measurements at 573 K shows that, during the H2 + O2 and H2−C3H8 SCR reactions, Ag+ ions and partially reduced Ag42+ clusters coexist. ESR spectra obtained after exposing a H2 + O2 gas mixture show the formation of superoxide ions. Combined with the results in our previous studies, the following mechanism is proposed: The Ag42+ cluster and protons formed by H2 reduction of Ag+ ions are involved in the reductive activation of molecular oxygen into superoxide ion, which should act as an effective oxidant for C3H8 oxidation to oxygenates such as acetate and NO oxidation to NO2. Thus, H2 addition increases the coverage of surface intermediates (NCO species) and the gas-phase concentration of NO2 and consequently increases the rate of N2 formation." @default.
- W2069937019 created "2016-06-24" @default.
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- W2069937019 date "2007-04-05" @default.
- W2069937019 modified "2023-09-26" @default.
- W2069937019 title "Reaction Mechanism of H<sub>2</sub>-Promoted Selective Catalytic Reduction of NO with C<sub>3</sub>H<sub>8</sub> over Ag−MFI Zeolite" @default.
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- W2069937019 doi "https://doi.org/10.1021/jp070322q" @default.
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