Tuning Pt-CeO<sub>2</sub> interactions by high-temperature vapor-phase synthesis for improved reducibility of lattice oxygen.

Pereira-Hernández, Xavier Isidro; DeLaRiva, Andrew; Muravev, Valery; Kunwar, Deepak; Xiong, Haifeng; Sudduth, Berlin; Engelhard, Mark; Kovarik, Libor et al. · Nat Commun · 2019

basic_science · Level V

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Abstract

In this work, we compare the CO oxidation performance of Pt single atom catalysts (SACs) prepared via two methods: (1) conventional wet chemical synthesis (strong electrostatic adsorption-SEA) with calcination at 350 °C in air; and (2) high temperature vapor phase synthesis (atom trapping-AT) with calcination in air at 800 °C leading to ionic Pt being trapped on the CeO<sub>2</sub> in a thermally stable form. As-synthesized, both SACs are inactive for low temperature (<150 °C) CO oxidation. After treatment in CO at 275 °C, both catalysts show enhanced reactivity. Despite similar Pt metal particle size, the AT catalyst is significantly more active, with onset of CO oxidation near room temperature. A combination of near-ambient pressure X-ray photoelectron spectroscopy (NAP-XPS) and CO temperature-programmed reduction (CO-TPR) shows that the high reactivity at low temperatures can be related to the improved reducibility of lattice oxygen on the CeO<sub>2</sub> support.