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The structure of a catalyst often changes in reactive environments, and following the structural evolution is crucial for the identification of the catalyst's active phase and reaction mechanism. Here we present an atomic-scale study of CO oxidation on a model Rh/Fe 3 O 4 (001) "single-atom" catalyst, which has a very different evolution depending on which of the two reactants, O 2 or CO, is adsorbed first. Using temperature-programmed desorption (TPD) combined with scanning tunneling microscopy (STM) and X-ray photoelectron spectroscopy (XPS), we show that O 2 destabilizes Rh atoms, leading to the formation of Rh x O y clusters; these catalyze CO oxidation via a Langmuir-Hinshelwood mechanism at temperatures as low as 200 K. If CO adsorbs first, the system is poisoned for direct interaction with O 2 , and CO oxidation is dominated by a Mars-van-Krevelen pathway at 480 K.

Adsorbate-induced structural evolution changes the mechanism of CO oxidation on a Rh/Fe3O4(001) model catalyst

Adsorbate-induced structural evolution changes the mechanism of CO oxidation on a Rh/Fe₃O₄(001) model catalyst