Single alloy nanoparticle x-ray imaging during a catalytic reaction

Young Yong Kim; Thomas F. Keller; Tiago J. Goncalves; Manuel Abuin; Henning Runge; Luca Gelisio; Jerome Carnis; Vedran Vonk; Philipp N. Plessow; Ivan A. Vartaniants; Andreas Stierle

doi:10.1126/sciadv.abh0757

Single alloy nanoparticle x-ray imaging during a catalytic reaction

Young Yong Kim, Thomas F. Keller, Tiago J. Goncalves, Manuel Abuin, Henning Runge, Luca Gelisio, Jerome Carnis, Vedran Vonk, Philipp N. Plessow, Ivan A. Vartaniants, Andreas Stierle

Department of Electrical and Electronic Engineering

Research output: Contribution to journal › Article › peer-review

Abstract

The imaging of active nanoparticles represents a milestone in decoding heterogeneous catalysts’ dynamics. We report the facet-resolved, surface strain state of a single PtRh alloy nanoparticle on SrTiO₃ determined by coherent x-ray diffraction imaging under catalytic reaction conditions. Density functional theory calculations allow us to correlate the facet surface strain state to its reaction environment–dependent chemical composition. We find that the initially Pt-terminated nanoparticle surface gets Rh-enriched under CO oxidation reaction conditions. The local composition is facet orientation dependent, and the Rh enrichment is nonreversible under subsequent CO reduction. Tracking facet-resolved strain and composition under operando conditions is crucial for a rational design of more efficient heterogeneous catalysts with tailored activity, selectivity, and lifetime.

Original language	English
Article number	eabh0757
Journal	Science Advances
Volume	7
Issue number	40
DOIs	https://doi.org/10.1126/sciadv.abh0757
Publication status	Published - 2021 Oct

Bibliographical note

Funding Information:
Funding from the European Union H2020 project “Nanoscience Foundries and Fine Analysis” (NFFA), grant no. 654360, from BMBF grant 5K13WC3 (PT-DESY), and from DFG SFB 1441 prefunding is acknowledged. This work was supported by the Helmholtz Association Initiative and Networking Fund (grant no. HRSF-0002), the Russian Science Foundation (grant no. 18-41-06001), and the state of Baden-Württemberg through bwHPC (bwUniCluster and JUSTUS, RV bw17D011).

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Copyright © 2021 The Authors, some rights reserved.

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title = "Single alloy nanoparticle x-ray imaging during a catalytic reaction",

abstract = "The imaging of active nanoparticles represents a milestone in decoding heterogeneous catalysts{\textquoteright} dynamics. We report the facet-resolved, surface strain state of a single PtRh alloy nanoparticle on SrTiO3 determined by coherent x-ray diffraction imaging under catalytic reaction conditions. Density functional theory calculations allow us to correlate the facet surface strain state to its reaction environment–dependent chemical composition. We find that the initially Pt-terminated nanoparticle surface gets Rh-enriched under CO oxidation reaction conditions. The local composition is facet orientation dependent, and the Rh enrichment is nonreversible under subsequent CO reduction. Tracking facet-resolved strain and composition under operando conditions is crucial for a rational design of more efficient heterogeneous catalysts with tailored activity, selectivity, and lifetime.",

author = "Kim, {Young Yong} and Keller, {Thomas F.} and Goncalves, {Tiago J.} and Manuel Abuin and Henning Runge and Luca Gelisio and Jerome Carnis and Vedran Vonk and Plessow, {Philipp N.} and Vartaniants, {Ivan A.} and Andreas Stierle",

note = "Funding Information: Funding from the European Union H2020 project “Nanoscience Foundries and Fine Analysis” (NFFA), grant no. 654360, from BMBF grant 5K13WC3 (PT-DESY), and from DFG SFB 1441 prefunding is acknowledged. This work was supported by the Helmholtz Association Initiative and Networking Fund (grant no. HRSF-0002), the Russian Science Foundation (grant no. 18-41-06001), and the state of Baden-W{\"u}rttemberg through bwHPC (bwUniCluster and JUSTUS, RV bw17D011). Publisher Copyright: Copyright {\textcopyright} 2021 The Authors, some rights reserved.",

year = "2021",

month = oct,

doi = "10.1126/sciadv.abh0757",

language = "English",

volume = "7",

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AU - Kim, Young Yong

AU - Keller, Thomas F.

AU - Goncalves, Tiago J.

AU - Abuin, Manuel

AU - Runge, Henning

AU - Gelisio, Luca

AU - Carnis, Jerome

AU - Vonk, Vedran

AU - Plessow, Philipp N.

AU - Vartaniants, Ivan A.

AU - Stierle, Andreas

N1 - Funding Information: Funding from the European Union H2020 project “Nanoscience Foundries and Fine Analysis” (NFFA), grant no. 654360, from BMBF grant 5K13WC3 (PT-DESY), and from DFG SFB 1441 prefunding is acknowledged. This work was supported by the Helmholtz Association Initiative and Networking Fund (grant no. HRSF-0002), the Russian Science Foundation (grant no. 18-41-06001), and the state of Baden-Württemberg through bwHPC (bwUniCluster and JUSTUS, RV bw17D011). Publisher Copyright: Copyright © 2021 The Authors, some rights reserved.

PY - 2021/10

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N2 - The imaging of active nanoparticles represents a milestone in decoding heterogeneous catalysts’ dynamics. We report the facet-resolved, surface strain state of a single PtRh alloy nanoparticle on SrTiO3 determined by coherent x-ray diffraction imaging under catalytic reaction conditions. Density functional theory calculations allow us to correlate the facet surface strain state to its reaction environment–dependent chemical composition. We find that the initially Pt-terminated nanoparticle surface gets Rh-enriched under CO oxidation reaction conditions. The local composition is facet orientation dependent, and the Rh enrichment is nonreversible under subsequent CO reduction. Tracking facet-resolved strain and composition under operando conditions is crucial for a rational design of more efficient heterogeneous catalysts with tailored activity, selectivity, and lifetime.

AB - The imaging of active nanoparticles represents a milestone in decoding heterogeneous catalysts’ dynamics. We report the facet-resolved, surface strain state of a single PtRh alloy nanoparticle on SrTiO3 determined by coherent x-ray diffraction imaging under catalytic reaction conditions. Density functional theory calculations allow us to correlate the facet surface strain state to its reaction environment–dependent chemical composition. We find that the initially Pt-terminated nanoparticle surface gets Rh-enriched under CO oxidation reaction conditions. The local composition is facet orientation dependent, and the Rh enrichment is nonreversible under subsequent CO reduction. Tracking facet-resolved strain and composition under operando conditions is crucial for a rational design of more efficient heterogeneous catalysts with tailored activity, selectivity, and lifetime.

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Single alloy nanoparticle x-ray imaging during a catalytic reaction

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