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Title: Active site localization of methane oxidation on Pt nanocrystals

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 in this paper, 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.

Authors:
 [1];  [1]; ORCiD logo [1];  [1];  [1];  [1]; ORCiD logo [2];  [3];  [3];  [3];  [4];  [4];  [5];  [5]; ORCiD logo [6]; ORCiD logo [1]
  1. Sogang Univ., Seoul (Korea). Dept. of Physics
  2. Argonne National Lab. (ANL), Argonne, IL (United States). Materials Science Division; Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
  3. Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
  4. Argonne National Lab. (ANL), Argonne, IL (United States). Center for Nanoscale Materials, Nanoscale Science and Technology Division
  5. Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany). PETRA III
  6. Seoul National Univ. (Korea, Republic of). Dept. of Materials Science and Engineering
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
National Research Foundation of Korea (NRF); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1468753
Grant/Contract Number:  
AC02-06CH11357; AC02-05CH11231
Resource Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 9; Journal Issue: 1; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Kim, Dongjin, Chung, Myungwoo, Carnis, Jerome, Kim, Sungwon, Yun, Kyuseok, Kang, Jinback, Cha, Wonsuk, Cherukara, Mathew J., Maxey, Evan, Harder, Ross, Sasikumar, Kiran, K. R. S. Sankaranarayanan, Subramanian, Zozulya, Alexey, Sprung, Michael, Riu, Dohhyung, and Kim, Hyunjung. Active site localization of methane oxidation on Pt nanocrystals. United States: N. p., 2018. Web. doi:10.1038/s41467-018-05464-2.
Kim, Dongjin, Chung, Myungwoo, Carnis, Jerome, Kim, Sungwon, Yun, Kyuseok, Kang, Jinback, Cha, Wonsuk, Cherukara, Mathew J., Maxey, Evan, Harder, Ross, Sasikumar, Kiran, K. R. S. Sankaranarayanan, Subramanian, Zozulya, Alexey, Sprung, Michael, Riu, Dohhyung, & Kim, Hyunjung. Active site localization of methane oxidation on Pt nanocrystals. United States. doi:10.1038/s41467-018-05464-2.
Kim, Dongjin, Chung, Myungwoo, Carnis, Jerome, Kim, Sungwon, Yun, Kyuseok, Kang, Jinback, Cha, Wonsuk, Cherukara, Mathew J., Maxey, Evan, Harder, Ross, Sasikumar, Kiran, K. R. S. Sankaranarayanan, Subramanian, Zozulya, Alexey, Sprung, Michael, Riu, Dohhyung, and Kim, Hyunjung. Fri . "Active site localization of methane oxidation on Pt nanocrystals". United States. doi:10.1038/s41467-018-05464-2. https://www.osti.gov/servlets/purl/1468753.
@article{osti_1468753,
title = {Active site localization of methane oxidation on Pt nanocrystals},
author = {Kim, Dongjin and Chung, Myungwoo and Carnis, Jerome and Kim, Sungwon and Yun, Kyuseok and Kang, Jinback and Cha, Wonsuk and Cherukara, Mathew J. and Maxey, Evan and Harder, Ross and Sasikumar, Kiran and K. R. S. Sankaranarayanan, Subramanian and Zozulya, Alexey and Sprung, Michael and Riu, Dohhyung and Kim, Hyunjung},
abstractNote = {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 in this paper, 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.},
doi = {10.1038/s41467-018-05464-2},
journal = {Nature Communications},
number = 1,
volume = 9,
place = {United States},
year = {2018},
month = {8}
}

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    Works referencing / citing this record:

    Active site localization of methane oxidation on Pt nanocrystals
    text, January 2018

    • Chung, Myunwoo; Carnis, Jerome; Kim, Sungwon
    • Deutsches Elektronen-Synchrotron, DESY, Hamburg
    • DOI: 10.3204/pubdb-2018-03330

    Formation and Functioning of Bimetallic Nanocatalysts: The Power of X‐ray Probes
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    • Filez, Matthias; Redekop, Evgeniy A.; Dendooven, Jolien
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