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Title: In Situ Industrial Bimetallic Catalyst Characterization using Scanning Transmission Electron Microscopy and X-ray Absorption Spectroscopy at One Atmosphere and Elevated Temperature

Abstract

We have developed a new experimental platform for in situ scanning transmission electron microscope (STEM) energy dispersive X-ray spectroscopy (EDS) which allows real time, nanoscale, elemental and structural changes to be studied at elevated temperature (up to 1000 °C) and pressure (up to 1 atm). Here we demonstrate the first application of this approach to understand complex structural changes occurring during reduction of a bimetallic catalyst, PdCu supported on TiO2, synthesized by wet impregnation. We reveal a heterogeneous evolution of nanoparticle size, distribution, and composition with large differences in reduction behavior for the two metals. We show that the data obtained is complementary to in situ STEM electron energy loss spectroscopy (EELS) and when combined with in situ X-ray absorption spectroscopy (XAS) allows correlation of bulk chemical state with nanoscale changes in elemental distribution during reduction, facilitating new understanding of the catalytic behavior for this important class of materials.

Authors:
 [1];  [2];  [2];  [1];  [1];  [1]; ORCiD logo [1];  [3]
+ Show Author Affiliations
  1. School of Materials, University of Manchester, Manchester M13 9PL United Kingdom
  2. BP Research Center, Naperville IL 60563 USA
  3. School of Materials, University of Manchester, Manchester M13 9PL United Kingdom, Argonne National Laboratory, Photon Sciences Division, Argonne IL 60439 USA
Publication Date:
Research Org.:
Argonne National Laboratory (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1374919
Alternate Identifier(s):
OSTI ID: 1374920; OSTI ID: 1623517
Grant/Contract Number:  
AC02-06CH11357
Resource Type:
Published Article
Journal Name:
ChemPhysChem
Additional Journal Information:
Journal Name: ChemPhysChem; Journal ID: ISSN 1439-4235
Publisher:
ChemPubSoc Europe
Country of Publication:
Germany
Language:
English
Subject:
Chemistry; Physics

Citation Formats

Prestat, Eric, Kulzick, Matthew A., Dietrich, Paul J., Smith, Matthew, Tien, Mr. Eu-Pin, Burke, M. Grace, Haigh, Sarah J., and Zaluzec, Nestor J. In Situ Industrial Bimetallic Catalyst Characterization using Scanning Transmission Electron Microscopy and X-ray Absorption Spectroscopy at One Atmosphere and Elevated Temperature. Germany: N. p., 2017. Web. doi:10.1002/cphc.201700425.
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Prestat, Eric, Kulzick, Matthew A., Dietrich, Paul J., Smith, Matthew, Tien, Mr. Eu-Pin, Burke, M. Grace, Haigh, Sarah J., & Zaluzec, Nestor J. In Situ Industrial Bimetallic Catalyst Characterization using Scanning Transmission Electron Microscopy and X-ray Absorption Spectroscopy at One Atmosphere and Elevated Temperature. Germany. https://doi.org/10.1002/cphc.201700425
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Prestat, Eric, Kulzick, Matthew A., Dietrich, Paul J., Smith, Matthew, Tien, Mr. Eu-Pin, Burke, M. Grace, Haigh, Sarah J., and Zaluzec, Nestor J. Mon . "In Situ Industrial Bimetallic Catalyst Characterization using Scanning Transmission Electron Microscopy and X-ray Absorption Spectroscopy at One Atmosphere and Elevated Temperature". Germany. https://doi.org/10.1002/cphc.201700425.
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@article{osti_1374919,
title = {In Situ Industrial Bimetallic Catalyst Characterization using Scanning Transmission Electron Microscopy and X-ray Absorption Spectroscopy at One Atmosphere and Elevated Temperature},
author = {Prestat, Eric and Kulzick, Matthew A. and Dietrich, Paul J. and Smith, Matthew and Tien, Mr. Eu-Pin and Burke, M. Grace and Haigh, Sarah J. and Zaluzec, Nestor J.},
abstractNote = {We have developed a new experimental platform for in situ scanning transmission electron microscope (STEM) energy dispersive X-ray spectroscopy (EDS) which allows real time, nanoscale, elemental and structural changes to be studied at elevated temperature (up to 1000 °C) and pressure (up to 1 atm). Here we demonstrate the first application of this approach to understand complex structural changes occurring during reduction of a bimetallic catalyst, PdCu supported on TiO2, synthesized by wet impregnation. We reveal a heterogeneous evolution of nanoparticle size, distribution, and composition with large differences in reduction behavior for the two metals. We show that the data obtained is complementary to in situ STEM electron energy loss spectroscopy (EELS) and when combined with in situ X-ray absorption spectroscopy (XAS) allows correlation of bulk chemical state with nanoscale changes in elemental distribution during reduction, facilitating new understanding of the catalytic behavior for this important class of materials.},
doi = {10.1002/cphc.201700425},
journal = {ChemPhysChem},
number = ,
volume = ,
place = {Germany},
year = {Mon Jun 12 00:00:00 EDT 2017},
month = {Mon Jun 12 00:00:00 EDT 2017}
}
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Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
https://doi.org/10.1002/cphc.201700425
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Cited by: 11 works
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Figures / Tables:

Figure 1 Figure 1: Characterization of calcined PdCu titania supported catalyst in vacuum. a) HAADF image where intensity differentiates the denser Pd particles from the titania support. b) STEM-EDS elemental mapping which demonstrates that the visible nanoparticles are principally Pd (red) while Cu (green) is more uniformly distributed on the titania support.more » A comparison of the simultaneously acquired spectral signatures (from the red and blue square regions on (a)) is shown for c) EDS and d) EELS respectively. The EELS signature for Cu is below the signal to noise demonstrating the difficulty of using EELS for mapping of transition metal catalysts at low loadings on a relatively thick support.« less
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