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• W2331565348 abstract "The present study explored photoinduced radical processes caused by interaction of CH4 and NH3 with a photoexcited surface of a complex metal oxide: magnesium–aluminum spinel (MgAl2O4; MAS). UV irradiation of MAS in vacuo yielded V-type color centers as evidenced by the 360 nm band in difference diffuse reflectance spectra. Interaction of these H-bearing molecules with photogenerated surface-active hole states (OS–•) yielded radical species which on recombination produced more complex molecules (including heteroatomic species) relative to the initial molecules. For the MAS/CH4 system, photoinduced dissociative adsorption of CH4 on surface-active hole centers produced •CH3 radicals that recombined to yield CH3CH3. For MAS/NH3, a similar dissociative adsorption process led to formation of •NH2 radicals with formation of NH2NH2 as an intermediate product; continued UV irradiation ultimately yielded N2. For the mixed MAS/CH4/NH3 system, however, interaction of adsorbed NH3 and CH4 on the UV-activated surface of MAS yielded •NH2 and •CH3 radicals, respectively, which produced CH3–NH2 followed by loss of the remaining hydrogens to form a surface-adsorbed cyanide, CNS, species. Recombination of photochemically produced radicals released sufficient energy to re-excite the solid spinel, generating new surface-active sites and a flash luminescence (emission decay time at 520 nm, τ ∼ 6 s for the MAS/NH3 case) referred to as the PhICL effect." @default.
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• W2331565348 date "2012-05-02" @default.
• W2331565348 modified "2023-09-26" @default.
• W2331565348 title "Photoinduced Radical Processes on the Spinel (MgAl₂O₄) Surface Involving Methane, Ammonia, and Methane/Ammonia" @default.
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• W2331565348 doi "https://doi.org/10.1021/la300370q" @default.
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