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

Abstract

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.

Authors:
 [1];  [2];  [3];  [4];  [5];  [5];  [1];  [6];  [2];  [1]
  1. Yeshiva Univ., New York, NY (United States)
  2. Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN)
  3. Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN); Univ. of Illinois at Urbana-Champaign, Urbana, IL (United States)
  4. Brookhaven National Lab. (BNL), Upton, NY (United States). Photon Sciences Division
  5. Univ. of Illinois at Urbana-Champaign, Urbana, IL (United States)
  6. Univ. of Illinois at Urbana-Champaign, Urbana, IL (United States); KTH Royal Inst. of Technology, Stockholm (Sweden)
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1228968
Report Number(s):
BNL-111043-2015-JA
Journal ID: ISSN 2041-1723
Grant/Contract Number:  
SC0012704; FG02-03ER15476; FG02-05ER15688
Resource Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 6; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 77 NANOSCIENCE AND NANOTECHNOLOGY

Citation Formats

Li, Y., Zakharov, D., Zhao, S., Tappero, R., Jung, U., Elsen, A., Baumann, Ph., Nuzzo, R. G., Stach, E. A., and Frenkel, A. I. Complex structural dynamics of nanocatalysts revealed in Operando conditions by correlated imaging and spectroscopy probes. United States: N. p., 2015. Web. doi:10.1038/ncomms8583.
Li, Y., Zakharov, D., Zhao, S., Tappero, R., Jung, U., Elsen, A., Baumann, Ph., Nuzzo, R. G., Stach, E. A., & Frenkel, A. I. Complex structural dynamics of nanocatalysts revealed in Operando conditions by correlated imaging and spectroscopy probes. United States. doi:10.1038/ncomms8583.
Li, Y., Zakharov, D., Zhao, S., Tappero, R., Jung, U., Elsen, A., Baumann, Ph., Nuzzo, R. G., Stach, E. A., and Frenkel, A. I. Mon . "Complex structural dynamics of nanocatalysts revealed in Operando conditions by correlated imaging and spectroscopy probes". United States. doi:10.1038/ncomms8583. https://www.osti.gov/servlets/purl/1228968.
@article{osti_1228968,
title = {Complex structural dynamics of nanocatalysts revealed in Operando conditions by correlated imaging and spectroscopy probes},
author = {Li, Y. and Zakharov, D. and Zhao, S. and Tappero, R. and Jung, U. and Elsen, A. and Baumann, Ph. and Nuzzo, R. G. and Stach, E. A. and Frenkel, A. I.},
abstractNote = {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.},
doi = {10.1038/ncomms8583},
journal = {Nature Communications},
number = ,
volume = 6,
place = {United States},
year = {2015},
month = {6}
}

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    journal, May 2016

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