Complex structural dynamics of nanocatalysts revealed in Operando conditions by correlated imaging and spectroscopy probes

Li, Y.; Zakharov, D.; Zhao, S.; Tappero, R.; Jung, U.; Elsen, A.; Baumann, Ph.; Nuzzo, R. G.; Stach, E. A.; Frenkel, A. I.

doi:10.1038/ncomms8583

Title: Complex structural dynamics of nanocatalysts revealed in Operando conditions by correlated imaging and spectroscopy probes

Journal Article · Mon Jun 29 04:00:00 UTC 2015 · Nature Communications

DOI: https://doi.org/10.1038/ncomms8583 · OSTI ID:1228968

Li, Y. ^[1]; Zakharov, D. ^[2]; Zhao, S. ^[3]; Tappero, R. ^[4]; Jung, U. ^[5]; Elsen, A. ^[5]; Baumann, Ph. ^[1]; Nuzzo, R. G. ^[6]; Stach, E. A. ^[2]; Frenkel, A. I. ^[1]

Yeshiva Univ., New York, NY (United States)
Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN)
Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN); Univ. of Illinois at Urbana-Champaign, Urbana, IL (United States)
Brookhaven National Lab. (BNL), Upton, NY (United States). Photon Sciences Division
Univ. of Illinois at Urbana-Champaign, Urbana, IL (United States)
Univ. of Illinois at Urbana-Champaign, Urbana, IL (United States); KTH Royal Inst. of Technology, Stockholm (Sweden)

Understanding how heterogeneous catalysts change size, shape and structure during chemical reactions is limited by the paucity of methods for studying catalytic ensembles in working state, that is, in operando conditions. Here by a correlated use of synchrotron X-ray absorption spectroscopy and scanning transmission electron microscopy in operando conditions, we quantitatively describe the complex structural dynamics of supported Pt catalysts exhibited during an exemplary catalytic reaction—ethylene hydrogenation. This work exploits a microfabricated catalytic reactor compatible with both probes. The results demonstrate dynamic transformations of the ensemble of Pt clusters that spans a broad size range throughout changing reaction conditions. Lastly, this method is generalizable to quantitative operando studies of complex systems using a wide variety of X-ray and electron-based experimental probes.

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Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: SC0012704; FG02-03ER15476; FG02-05ER15688

OSTI ID:: 1228968

Report Number(s):: BNL--111043-2015-JA

Journal Information:: Nature Communications, Journal Name: Nature Communications Vol. 6; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

References (39)

Methanol oxidation over model cobalt catalysts: Influence of the cobalt oxidation state on the reactivity Zafeiratos, S.; Dintzer, T.; Teschner, D. Journal of Catalysis, Vol. 269, Issue 2 https://doi.org/10.1016/j.jcat.2009.11.013	journal	February 2010
Environmental electron microscopy (ETEM) for catalysts with a closed E-cell with carbon windows Giorgio, S.; Sao Joao, S.; Nitsche, S. Ultramicroscopy, Vol. 106, Issue 6 https://doi.org/10.1016/j.ultramic.2006.01.006	journal	April 2006
Noncrystalline-to-Crystalline Transformations in Pt Nanoparticles Li, Long; Wang, Lin-Lin; Johnson, Duane D. Journal of the American Chemical Society, Vol. 135, Issue 35 https://doi.org/10.1021/ja405497p	journal	August 2013
Characterization of Palladium Nanoparticles by Using X-ray Reflectivity, EXAFS, and Electron Microscopy Sun, Yuan; Frenkel, Anatoly I.; Isseroff, Rebecca Langmuir, Vol. 22, Issue 2 https://doi.org/10.1021/la052686k	journal	January 2006
Revealing the Atomic Restructuring of Pt–Co Nanoparticles Xin, Huolin L.; Alayoglu, Selim; Tao, Runzhe Nano Letters, Vol. 14, Issue 6 https://doi.org/10.1021/nl500553a	journal	May 2014
Towards the computational design of solid catalysts Nørskov, J.; Bligaard, T.; Rossmeisl, J. Nature Chemistry, Vol. 1, Issue 1, p. 37-46 https://doi.org/10.1038/nchem.121	journal	April 2009
Heterogeneities of individual catalyst particles in space and time as monitored by spectroscopy Buurmans, Inge L. C.; Weckhuysen, Bert M. Nature Chemistry, Vol. 4, Issue 11 https://doi.org/10.1038/nchem.1478	journal	October 2012
Picometre-precision analysis of scanning transmission electron microscopy images of platinum nanocatalysts Yankovich, Andrew B.; Berkels, Benjamin; Dahmen, W. Nature Communications, Vol. 5, Issue 1 https://doi.org/10.1038/ncomms5155	journal	June 2014
BoxPlotR: a web tool for generation of box plots Spitzer, Michaela; Wildenhain, Jan; Rappsilber, Juri Nature Methods, Vol. 11, Issue 2 https://doi.org/10.1038/nmeth.2811	journal	January 2014
The Impact of Nanoscience on Heterogeneous Catalysis Bell, A. T. Science, Vol. 299, Issue 5613 https://doi.org/10.1126/science.1083671	journal	March 2003
Reaction-Driven Restructuring of Rh-Pd and Pt-Pd Core-Shell Nanoparticles Tao, F.; Grass, M. E.; Zhang, Y. Science, Vol. 322, Issue 5903 https://doi.org/10.1126/science.1164170	journal	November 2008
In Situ Studies of Chemistry and Structure of Materials in Reactive Environments Tao, F.; Salmeron, M. Science, Vol. 331, Issue 6014 https://doi.org/10.1126/science.1197461	journal	January 2011
Transition States Between Pyramids and Domes During Ge/Si Island Growth Ross, F. M. Science, Vol. 286, Issue 5446 https://doi.org/10.1126/science.286.5446.1931	journal	December 1999
Operando Spectroscopy: the Knowledge Bridge to Assessing Structure-Performance Relationships in Catalyst Nanoparticles Bañares, Miguel A. Advanced Materials, Vol. 23, Issue 44 https://doi.org/10.1002/adma.201101803	journal	September 2011
Real-Time Characterization of Formation and Breakup of Iridium Clusters in Highly Dealuminated Zeolite Y Uzun, Alper; Gates, Bruce C. Angewandte Chemie, Vol. 120, Issue 48 https://doi.org/10.1002/ange.200802140	journal	August 2008
Real-Time Characterization of Formation and Breakup of Iridium Clusters in Highly Dealuminated Zeolite Y Uzun, Alper; Gates, Bruce C. Angewandte Chemie International Edition, Vol. 47, Issue 48 https://doi.org/10.1002/anie.200802140	journal	August 2008
Methanol oxidation over model cobalt catalysts: Influence of the cobalt oxidation state on the reactivity Zafeiratos, S.; Dintzer, T.; Teschner, D. Journal of Catalysis, Vol. 269, Issue 2 https://doi.org/10.1016/j.jcat.2009.11.013	journal	February 2010
Environmental electron microscopy (ETEM) for catalysts with a closed E-cell with carbon windows Giorgio, S.; Sao Joao, S.; Nitsche, S. Ultramicroscopy, Vol. 106, Issue 6 https://doi.org/10.1016/j.ultramic.2006.01.006	journal	April 2006
In Situ TEM Study of Catalytic Nanoparticle Reactions in Atmospheric Pressure Gas Environment Xin, Huolin L.; Niu, Kaiyang; Alsem, Daan Hein Microscopy and Microanalysis, Vol. 19, Issue 6 https://doi.org/10.1017/S1431927613013433	journal	September 2013
Supported Metal Clusters: Synthesis, Structure, and Catalysis Gates, B. C. Chemical Reviews, Vol. 95, Issue 3 https://doi.org/10.1021/cr00035a003	journal	May 1995
Comparative in Operando Studies in Heterogeneous Catalysis: Atomic and Electronic Structural Features in the Hydrogenation of Ethylene over Supported Pd and Pt Catalysts Jung, Ulrich; Elsen, Annika; Li, Yuanyuan ACS Catalysis, Vol. 5, Issue 3 https://doi.org/10.1021/cs501846g	journal	February 2015
Noncrystalline-to-Crystalline Transformations in Pt Nanoparticles Li, Long; Wang, Lin-Lin; Johnson, Duane D. Journal of the American Chemical Society, Vol. 135, Issue 35 https://doi.org/10.1021/ja405497p	journal	August 2013
Characterization of Palladium Nanoparticles by Using X-ray Reflectivity, EXAFS, and Electron Microscopy Sun, Yuan; Frenkel, Anatoly I.; Isseroff, Rebecca Langmuir, Vol. 22, Issue 2 https://doi.org/10.1021/la052686k	journal	January 2006
Shape-Dependent Catalytic Activity of Platinum Nanoparticles in Colloidal Solution Narayanan, Radha; El-Sayed, Mostafa A. Nano Letters, Vol. 4, Issue 7 https://doi.org/10.1021/nl0495256	journal	July 2004
Revealing the Atomic Restructuring of Pt–Co Nanoparticles Xin, Huolin L.; Alayoglu, Selim; Tao, Runzhe Nano Letters, Vol. 14, Issue 6 https://doi.org/10.1021/nl500553a	journal	May 2014
Nanoscale chemical imaging of a working catalyst by scanning transmission X-ray microscopy de Smit, Emiel; Swart, Ingmar; Creemer, J. Fredrik Nature, Vol. 456, Issue 7219 https://doi.org/10.1038/nature07516	journal	November 2008
Towards the computational design of solid catalysts Nørskov, J.; Bligaard, T.; Rossmeisl, J. Nature Chemistry, Vol. 1, Issue 1, p. 37-46 https://doi.org/10.1038/nchem.121	journal	April 2009
Heterogeneities of individual catalyst particles in space and time as monitored by spectroscopy Buurmans, Inge L. C.; Weckhuysen, Bert M. Nature Chemistry, Vol. 4, Issue 11 https://doi.org/10.1038/nchem.1478	journal	October 2012
Picometre-precision analysis of scanning transmission electron microscopy images of platinum nanocatalysts Yankovich, Andrew B.; Berkels, Benjamin; Dahmen, W. Nature Communications, Vol. 5, Issue 1 https://doi.org/10.1038/ncomms5155	journal	June 2014
Visualization of oscillatory behaviour of Pt nanoparticles catalysing CO oxidation Vendelbo, S. B.; Elkjær, C. F.; Falsig, H. Nature Materials, Vol. 13, Issue 9 https://doi.org/10.1038/nmat4033	journal	July 2014
BoxPlotR: a web tool for generation of box plots Spitzer, Michaela; Wildenhain, Jan; Rappsilber, Juri Nature Methods, Vol. 11, Issue 2 https://doi.org/10.1038/nmeth.2811	journal	January 2014
Entamoeba histolytica exploits the autophagy pathway in macrophages to trigger inflammation in disease pathogenesis Begum, Sharmin; Moreau, France; Dufour, Antoine Mucosal Immunology, Vol. 14, Issue 5 https://doi.org/10.1038/s41385-021-00408-4	journal	May 2021
Applications of extended X-ray absorption fine-structure spectroscopy to studies of bimetallic nanoparticle catalysts Frenkel, Anatoly I. Chemical Society Reviews, Vol. 41, Issue 24 https://doi.org/10.1039/c2cs35174a	journal	January 2012
The Impact of Nanoscience on Heterogeneous Catalysis Bell, A. T. Science, Vol. 299, Issue 5613 https://doi.org/10.1126/science.1083671	journal	March 2003
The Problem with Determining Atomic Structure at the Nanoscale Billinge, S. J. L.; Levin, I. Science, Vol. 316, Issue 5824 https://doi.org/10.1126/science.1135080	journal	April 2007
Reaction-Driven Restructuring of Rh-Pd and Pt-Pd Core-Shell Nanoparticles Tao, F.; Grass, M. E.; Zhang, Y. Science, Vol. 322, Issue 5903 https://doi.org/10.1126/science.1164170	journal	November 2008
In Situ Studies of Chemistry and Structure of Materials in Reactive Environments Tao, F.; Salmeron, M. Science, Vol. 331, Issue 6014 https://doi.org/10.1126/science.1197461	journal	January 2011
Influence of the support on surface rearrangements of bimetallic nanoparticles in real catalysts Divins, N. J.; Angurell, I.; Escudero, C. Science, Vol. 346, Issue 6209 https://doi.org/10.1126/science.1258106	journal	October 2014
Transition States Between Pyramids and Domes During Ge/Si Island Growth Ross, F. M. Science, Vol. 286, Issue 5446 https://doi.org/10.1126/science.286.5446.1931	journal	December 1999

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Identification of carbon-encapsulated iron nanoparticles as active species in non-precious metal oxygen reduction catalysts Varnell, Jason A.; Tse, Edmund C. M.; Schulz, Charles E. Nature Communications, Vol. 7, Issue 1 https://doi.org/10.1038/ncomms12582	journal	August 2016
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