Defect Dynamics at a Single Pt Nanoparticle during Catalytic Oxidation

Kim, Dongjin; Chung, Myungwoo; Kim, Sungwon; Yun, Kyuseok; Cha, Wonsuk; Harder, Ross; Kim, Hyunjung

doi:10.1021/acs.nanolett.9b01332

Title: Defect Dynamics at a Single Pt Nanoparticle during Catalytic Oxidation

Abstract

Defects can affect all aspects of a material by altering its electronic properties and controlling its chemical reactivity. At defect sites, preferential adsorption of reactants and/or formation of chemical species at active sites are observed in heterogeneous catalysis. Understanding the structural response at defect sites during catalytic reactions provides a unique opportunity to exploit defect control of nanoparticle-based catalysts. However, it remains difficult to characterize the strain and defect evolution for a single nanocrystal catalyst in situ. Here, we report Bragg coherent X-ray diffraction imaging of defect dynamics in an individual Pt nanoparticle during catalytic methane oxidation. We observed that the initially tensile strained regions of the crystal became seed points for the development of further strain and subsequent disappearance of diffraction density during oxidation reactions. Our team's detailed understanding of the catalytically induced deformation at the defect sites and observed reversibility during the relevant steps of the catalytic oxidation process provide important insights of defect control and engineering of heterogeneous catalysts.

Authors:

Kim, Dongjin ^[1]; Chung, Myungwoo ^[1]; Kim, Sungwon ^[1]; Yun, Kyuseok ^[1]; Cha, Wonsuk ^[2]; Harder, Ross ^[2];

^[1]

Sogang Univ., Seoul (Korea)
Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)

Publication Date:: Fri Jun 28 00:00:00 EDT 2019

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)

OSTI Identifier:: 1599887

Grant/Contract Number:: AC02-06CH11357

Resource Type:: Accepted Manuscript

Journal Name:: Nano Letters

Additional Journal Information:: Journal Volume: 19; Journal Issue: 8; Journal ID: ISSN 1530-6984

Publisher:: American Chemical Society

Country of Publication:: United States

Language:: English

Subject:: 36 MATERIALS SCIENCE; 3D strain imaging; Bragg coherent diffraction imaging; Catalyst; Platinum nanoparticle; Strain dynamics

Citation Formats


                    Kim, Dongjin, Chung, Myungwoo, Kim, Sungwon, Yun, Kyuseok, Cha, Wonsuk, Harder, Ross, and Kim, Hyunjung. Defect Dynamics at a Single Pt Nanoparticle during Catalytic Oxidation.  United States: N. p., 2019. 
Web.  doi:10.1021/acs.nanolett.9b01332.

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                    Kim, Dongjin, Chung, Myungwoo, Kim, Sungwon, Yun, Kyuseok, Cha, Wonsuk, Harder, Ross, & Kim, Hyunjung. Defect Dynamics at a Single Pt Nanoparticle during Catalytic Oxidation.  United States.  https://doi.org/10.1021/acs.nanolett.9b01332

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                    Kim, Dongjin, Chung, Myungwoo, Kim, Sungwon, Yun, Kyuseok, Cha, Wonsuk, Harder, Ross, and Kim, Hyunjung. Fri .  
"Defect Dynamics at a Single Pt Nanoparticle during Catalytic Oxidation".  United States.  https://doi.org/10.1021/acs.nanolett.9b01332.  https://www.osti.gov/servlets/purl/1599887.

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@article{osti_1599887,

  title        = {Defect Dynamics at a Single Pt Nanoparticle during Catalytic Oxidation},

  author       = {Kim, Dongjin and Chung, Myungwoo and Kim, Sungwon and Yun, Kyuseok and Cha, Wonsuk and Harder, Ross and Kim, Hyunjung},

  abstractNote = {Defects can affect all aspects of a material by altering its electronic properties and controlling its chemical reactivity. At defect sites, preferential adsorption of reactants and/or formation of chemical species at active sites are observed in heterogeneous catalysis. Understanding the structural response at defect sites during catalytic reactions provides a unique opportunity to exploit defect control of nanoparticle-based catalysts. However, it remains difficult to characterize the strain and defect evolution for a single nanocrystal catalyst in situ. Here, we report Bragg coherent X-ray diffraction imaging of defect dynamics in an individual Pt nanoparticle during catalytic methane oxidation. We observed that the initially tensile strained regions of the crystal became seed points for the development of further strain and subsequent disappearance of diffraction density during oxidation reactions. Our team's detailed understanding of the catalytically induced deformation at the defect sites and observed reversibility during the relevant steps of the catalytic oxidation process provide important insights of defect control and engineering of heterogeneous catalysts.},

  doi          = {10.1021/acs.nanolett.9b01332},

  journal      = {Nano Letters},

  number       = 8,

  volume       = 19,

  place        = {United States},

  year         = {Fri Jun 28 00:00:00 EDT 2019},

  month        = {Fri Jun 28 00:00:00 EDT 2019}

}

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Cited by: 17 works

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Table 1: Gas Environmental Conditions for BCDI Measurements during the Catalytic Reactions

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