Active site localization of methane oxidation on Pt nanocrystals

Nature Communications
Dongjin KimHyunjung Kim

Abstract

High catalytic efficiency in metal nanocatalysts is attributed to large surface area to volume ratios and an abundance of under-coordinated atoms that can decrease kinetic barriers. Although overall shape or size changes of nanocatalysts have been observed as a result of catalytic processes, structural changes at low-coordination sites such as edges, remain poorly understood. Here, we report high-lattice distortion at edges of Pt nanocrystals during heterogeneous catalytic methane oxidation based on in situ 3D Bragg coherent X-ray diffraction imaging. We directly observe contraction at edges owing to adsorption of oxygen. This strain increases during methane oxidation and it returns to the original state after completing the reaction process. The results are in good agreement with finite element models that incorporate forces, as determined by reactive molecular dynamics simulations. Reaction mechanisms obtained from in situ strain imaging thus provide important insights for improving catalysts and designing future nanostructured catalytic materials.

References

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Citations

Apr 2, 2019·Angewandte Chemie·Matthias FilezGuy B Marin
Sep 7, 2019·Journal of Synchrotron Radiation·Alexander BjörlingJosé Solla-Gullón
Feb 16, 2019·Proceedings of the National Academy of Sciences of the United States of America·Yuan GaoLinda Young
Jul 31, 2020·Scientific Reports·Ni LiMarie-Ingrid Richard
Jan 8, 2021·Physical Review Letters·Alexander BjörlingFilipe R N C Maia
Apr 2, 2021·ACS Nano·Rafael A VicentePablo S Fernández
May 1, 2021·Journal of Physics. Condensed Matter : an Institute of Physics Journal·Florian MeneauAline Ribeiro Passos
Jun 30, 2019·Nano Letters·Dongjin KimHyunjung Kim
Apr 17, 2020·ACS Applied Materials & Interfaces·Ying-Juan HaoFa-Tang Li
Oct 2, 2021·Science Advances·Young Yong KimAndreas Stierle

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Methods Mentioned

BETA
X-ray

Software Mentioned

LAMMPS
COMSOL

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