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Title: Operando characterization of catalysts through use of a portable microreactor

Abstract

To provide new understandings of the mechanisms of catalytic reactions, improved methods are needed than can monitor changes in the electronic, structural and chemical properties of catalysts, doing so in the operando conditions in which catalysts work. We describe here a microreactor-based approach that integrates the capabilities of advanced x-ray, electron, optical and gas-phase compositional analysis techniques in operando conditions. For several exemplary catalytic systems, we demonstrate how this approach enables characterization of three major factors contributing to structure-property correlations evidenced in heterogeneously catalyzed reactions, namely: the atomic structure and elemental compositions of nanocatalysts; the physiochemical properties of the support and catalyst-support interfaces; and the gas and surface-phase chemistry occurring under operando conditions. We highlight the generality of the approach as well as outline opportunities for future developments.

Authors:
 [1];  [2];  [3];  [3];  [4];  [4];  [3];  [5];  [6];  [6]
  1. Univ. of Illinois, Urbana, IL (United States); Brookhaven National Lab., Upton, NY (United States)
  2. Yeshiva Univ., New York, NY (United States)
  3. Brookhaven National Lab. (BNL), Upton, NY (United States)
  4. City College of New York, New York, NY (United States)
  5. Univ. of Illinois, Urbana, IL (United States)
  6. Yeshiva Univ., New York, NY (United States); Brookhaven National Lab. (BNL), Upton, NY (United States)
Publication Date:
Research Org.:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1224779
Alternate Identifier(s):
OSTI ID: 1239774
Report Number(s):
BNL-108512-2015-JA; BNL-108433-2015-JA
Journal ID: ISSN 1867-3880; KC0403020
Grant/Contract Number:  
SC0012704; SC0012335; FG02-03ER15476
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
ChemCatChem
Additional Journal Information:
Journal Name: ChemCatChem; Journal ID: ISSN 1867-3880
Publisher:
ChemPubSoc Europe
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Center for Functional Nanomaterials; heterogeneous catalysis; microcell; operando characterization; 36 MATERIALS SCIENCE; operando characterization

Citation Formats

Zhao, Shen, Li, Yuanyuan, Stavitski, Eli, Tappero, Ryan, Crowley, Stephen, Castaldi, Marco J., Zakharov, Dmitri N., Nuzzo, Ralph G., Frenkel, Anatoly I., and Stach, Eric A. Operando characterization of catalysts through use of a portable microreactor. United States: N. p., 2015. Web. doi:10.1002/cctc.201500688.
Zhao, Shen, Li, Yuanyuan, Stavitski, Eli, Tappero, Ryan, Crowley, Stephen, Castaldi, Marco J., Zakharov, Dmitri N., Nuzzo, Ralph G., Frenkel, Anatoly I., & Stach, Eric A. Operando characterization of catalysts through use of a portable microreactor. United States. https://doi.org/10.1002/cctc.201500688
Zhao, Shen, Li, Yuanyuan, Stavitski, Eli, Tappero, Ryan, Crowley, Stephen, Castaldi, Marco J., Zakharov, Dmitri N., Nuzzo, Ralph G., Frenkel, Anatoly I., and Stach, Eric A. 2015. "Operando characterization of catalysts through use of a portable microreactor". United States. https://doi.org/10.1002/cctc.201500688. https://www.osti.gov/servlets/purl/1224779.
@article{osti_1224779,
title = {Operando characterization of catalysts through use of a portable microreactor},
author = {Zhao, Shen and Li, Yuanyuan and Stavitski, Eli and Tappero, Ryan and Crowley, Stephen and Castaldi, Marco J. and Zakharov, Dmitri N. and Nuzzo, Ralph G. and Frenkel, Anatoly I. and Stach, Eric A.},
abstractNote = {To provide new understandings of the mechanisms of catalytic reactions, improved methods are needed than can monitor changes in the electronic, structural and chemical properties of catalysts, doing so in the operando conditions in which catalysts work. We describe here a microreactor-based approach that integrates the capabilities of advanced x-ray, electron, optical and gas-phase compositional analysis techniques in operando conditions. For several exemplary catalytic systems, we demonstrate how this approach enables characterization of three major factors contributing to structure-property correlations evidenced in heterogeneously catalyzed reactions, namely: the atomic structure and elemental compositions of nanocatalysts; the physiochemical properties of the support and catalyst-support interfaces; and the gas and surface-phase chemistry occurring under operando conditions. We highlight the generality of the approach as well as outline opportunities for future developments.},
doi = {10.1002/cctc.201500688},
url = {https://www.osti.gov/biblio/1224779}, journal = {ChemCatChem},
issn = {1867-3880},
number = ,
volume = ,
place = {United States},
year = {Fri Oct 09 00:00:00 EDT 2015},
month = {Fri Oct 09 00:00:00 EDT 2015}
}

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Works referencing / citing this record:

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