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Tuning Pt-CeO2 interactions by high-temperature vapor-phase synthesis for improved reducibility of lattice oxygen

2019; Nature Portfolio; Volume: 10; Issue: 1 Linguagem: Inglês

10.1038/s41467-019-09308-5

2041-1723

Xavier Isidro Pereira Hernández, Andrew DeLaRiva, Valery Muravev, Deepak Kunwar, Haifeng Xiong, Berlin Sudduth, Mark Engelhard, Libor Kovařík, Emiel J. M. Hensen, Yong Wang, Abhaya K. Datye,

Catalysis and Hydrodesulfurization Studies

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 CeO2 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 CeO2 support.