Dataset Information

Highly Stable and Reactive Platinum Single Atoms on Oxygen Plasma-Functionalized CeO₂ Surfaces: Nanostructuring and Peroxo Effects.

ABSTRACT: Atomically dispersed precious metals on oxide supports have recently become increasingly interesting catalytic materials. Nonetheless, their non-trivial preparation and limited thermal and environmental stability constitutes an issue for their potential applications. Here we demonstrate that an oxygen plasma pre-treatment of the ceria (CeO₂ ) surface serves to anchor Pt single atoms, making them active and resistant towards sintering in the CO oxidation reaction. Through a combination of experimental results obtained on well-defined CeO₂ films and theory, we show that the O₂ plasma causes surface nanostructuring and the formation of surface peroxo (O₂ ^2- ) species, favoring the uniform and dense distribution of isolated strongly bonded Pt²⁺ atoms. The promotional effect of the plasma treatment was further demonstrated on powder Pt/CeO₂ catalysts. We believe that plasma functionalization can be applied to other metal/oxide systems to achieve tunable and stable catalysts with a high density of active sites.

SUBMITTER: Wan W

PROVIDER: S-EPMC9315031 | biostudies-literature | 2022 May

REPOSITORIES: biostudies-literature

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Publications

Highly Stable and Reactive Platinum Single Atoms on Oxygen Plasma-Functionalized CeO<sub>2</sub> Surfaces: Nanostructuring and Peroxo Effects.

Wan Weiming W Geiger Julian J Berdunov Nikolay N Lopez Luna Mauricio M Chee See Wee SW Daelman Nathan N López Núria N Shaikhutdinov Shamil S Roldan Cuenya Beatriz B

Angewandte Chemie (International ed. in English) 20220316 20

Atomically dispersed precious metals on oxide supports have recently become increasingly interesting catalytic materials. Nonetheless, their non-trivial preparation and limited thermal and environmental stability constitutes an issue for their potential applications. Here we demonstrate that an oxygen plasma pre-treatment of the ceria (CeO<sub>2</sub> ) surface serves to anchor Pt single atoms, making them active and resistant towards sintering in the CO oxidation reaction. Through a combination ...[more]

PMID: 35243735

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Project description:Propane dehydrogenation (PDH) is an on-purpose catalytic technology to produce propylene from propane that operates at high temperatures, 773-973 K. Several key industry players have been active in developing new catalysts and processes with improved carbon footprint and economics, where Pt-based catalysts have played a central role. The optimization of these catalytic systems through computational and atomistic simulations requires large-scale models that account for their reactivity and dynamic properties. To address this challenge, we developed a new reactive ReaxFF force field (2023-Pt/C/H) that enables large-scale simulations of PDH reactions catalyzed on Pt surfaces. The optimization of force-field parameters relies on a large training set of density functional theory (DFT) calculations of Pt-catalyzed PDH mechanism, including geometries, adsorption and relative energies of reaction intermediates, and key C-H and C-C bond-breaking/forming reaction steps on the Pt(111) surface. The internal validation supports the accuracy of the developed 2023-Pt/C/H force-field parameters, resulting in mean absolute errors (MAE) against DFT data of 14 and 12 kJ mol-1 for relative energies of intermediates and energy barriers, respectively. We demonstrated the applicability of the 2023-Pt/C/H force field with reactive molecular dynamics simulations of propane on different Pt surface topologies and temperatures. The simulations successfully model the formation of propene in the gas phase as well as competitive, unproductive reactions such as deep dehydrogenation and C-C bond cleavage that produce H, C1 and C2 adsorbed species responsible of catalytic deactivation of Pt surface. Results show the following reactivity order: Pt(111) < Pt(100) < Pt(211), and that for the stepped Pt(211) surface, propane activation occurs on low-coordinated Pt atoms at the steps. The measured selectivity as a function of surface topology follows the same trend as activity, the Pt(211) facet being the most selective. The 2023-Pt/C/H reactive force field can also describe the increase of reactivity with the temperature. From these simulations, we were able to estimate the Arrhenius activation energy, 73 kJ mol-1, whose value is close to those reported experimentally for PDH catalyzed by large, supported Pt nanoparticles . The newly developed 2023-Pt/C/H reactive force field can be used in subsequent investigations of different Pt topologies and of collective effects such as temperature, propane pressure, or H surface coverage.

Dataset Information

Highly Stable and Reactive Platinum Single Atoms on Oxygen Plasma-Functionalized CeO₂ Surfaces: Nanostructuring and Peroxo Effects.

Publications

Highly Stable and Reactive Platinum Single Atoms on Oxygen Plasma-Functionalized CeO<sub>2</sub> Surfaces: Nanostructuring and Peroxo Effects.

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Dataset Information

Highly Stable and Reactive Platinum Single Atoms on Oxygen Plasma-Functionalized CeO2 Surfaces: Nanostructuring and Peroxo Effects.

Publications

Highly Stable and Reactive Platinum Single Atoms on Oxygen Plasma-Functionalized CeO<sub>2</sub> Surfaces: Nanostructuring and Peroxo Effects.

Similar Datasets

OmicsDI is part of the ELIXIR infrastructure

Tweets

Highly Stable and Reactive Platinum Single Atoms on Oxygen Plasma-Functionalized CeO₂ Surfaces: Nanostructuring and Peroxo Effects.