Active site localization of methane oxidation on Pt nanocrystals

Dongjin Kim, Myungwoo Chung, Jerome Carnis, Sungwon Kim, Kyuseok Yun, Jinback Kang, Wonsuk Cha, Mathew J. Cherukara, Evan Maxey, Ross Harder, Kiran Sasikumar, Subramanian Sankaranarayanan, Alexey Zozulya, Michael Sprung, Dohhyung Riu and Hyunjung Kim ()
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Dongjin Kim: Sogang University
Myungwoo Chung: Sogang University
Jerome Carnis: Sogang University
Sungwon Kim: Sogang University
Kyuseok Yun: Sogang University
Jinback Kang: Sogang University
Wonsuk Cha: Argonne National Laboratory
Mathew J. Cherukara: Argonne National Laboratory
Evan Maxey: Argonne National Laboratory
Ross Harder: Argonne National Laboratory
Kiran Sasikumar: Nanoscale Science and Technology Division, Argonne National Laboratory
Subramanian Sankaranarayanan: Nanoscale Science and Technology Division, Argonne National Laboratory
Alexey Zozulya: Deutsches Elektronen-Synchrotron (DESY)
Michael Sprung: Deutsches Elektronen-Synchrotron (DESY)
Dohhyung Riu: Seoul National University of Science and Technology
Hyunjung Kim: Sogang University

Nature Communications, 2018, vol. 9, issue 1, 1-7

Abstract: 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.

Date: 2018
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Persistent link: https://EconPapers.repec.org/RePEc:nat:natcom:v:9:y:2018:i:1:d:10.1038_s41467-018-05464-2

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DOI: 10.1038/s41467-018-05464-2

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