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Operando ME-DRIFTS study of reaction intermediates during toluene oxidation on CeO 2 nanoparticles supported on MgO hexagonal plates

Catalysis Today, ISSN: 0920-5861, Vol: 426, Page: 114395
2024
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Operando DRIFT spectroscopy was employed to investigate the intermediates involved in the oxidation of toluene on highly dispersed ceria nanoparticles supported on magnesium oxide hexagonal nanoplates. Small CeO 2 nanoparticles dispersed on magnesium oxide hexagonal nanoplates showed enhanced catalytic performance to total toluene combustion compared to a high surface area polycrystalline CeO 2. Selective identification of active surface species was carried out by combining concentration-modulation excitation spectroscopy (c-MES) experiments with phase-sensitive detection (PSD) spectral analysis and a chemometric multivariate curve resolution alternating least squares (MCR-ALS) method. The results revealed a stepwise reaction pathway for toluene oxidation on the catalyst surface. Initially, toluene is molecularly adsorbed and reacts with surface oxygen species to produce intermediate benzyl (C 6 H 5 CH 2 - ). Next, benzyl is stepwise oxidized to benzyloxy/benzyl alcohol, benzaldehyde, and benzoate. Further oxidation of benzoate and the aromatic ring produces formate and carbonate species. On pure CeO 2, formates accumulate on the ceria surface, and only a minor part of them reacts to produce CO 2 (and CO). Instead, formates species are rapidly oxidized to CO 2 on the CeO 2 /MgO catalyst and do not accumulate on the surface, due to the enhanced redox capacity and higher presence of oxygen vacancies of the supported nanoparticles.

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