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Title: Pulse response analysis using the Y-procedure: A data science approach

Abstract

We report that pulse response experiments can provide a wealth of data for transient kinetic studies of gas phase heterogeneous reactions, with the ability to paint a detailed picture of intrinsic reaction kinetics pertaining to complex catalytic mechanisms. A novel framework called the Y-Procedure was developed by Yablonsky et al. to extract information from non-steady-state kinetic data (Yablonsky et al., 2007). The Y-Procedure reconstructs the chemical transformation rate and gas composition in the catalytic zone with no a priori assumptions on the kinetic model and is used to relate changes in catalytic reaction rates and kinetic parameters to changes in a catalyst’s surface composition. This paper provides a detailed description of the data science work flow implemented in the Y-procedure through an experimental example of oxygen adsorption on platinum. Lastly, this powerful method, along with a robust list of pre-processing methodology, will enable deeper understanding of kinetic processes and mechanism to be derived from the TAP pulse response technique.

Authors:
ORCiD logo [1]; ORCiD logo [2];  [3];  [4]; ORCiD logo [5]; ORCiD logo [2]; ORCiD logo [1]
  1. Idaho National Lab. (INL), Idaho Falls, ID (United States). Energy & Environment Science and Technology; Center for Advanced Energy Studies, Idaho Falls, ID (United States)
  2. Idaho National Lab. (INL), Idaho Falls, ID (United States). Energy & Environment Science and Technology
  3. Univ. of Oslo (Norway). Centre for Materials Science and Nanotechnology (SMN), Department of Chemistry
  4. Washington Univ., St. Louis, MO (United States). Department of Chemical Engineering
  5. Ghent University (Belgium). Department of Mathematical Analysis
Publication Date:
Research Org.:
Idaho National Laboratory (INL), Idaho Falls, ID (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Energy Efficiency Office. Advanced Manufacturing Office
OSTI Identifier:
1478468
Alternate Identifier(s):
OSTI ID: 1495270
Report Number(s):
INL/JOU-18-44371-Rev001
Journal ID: ISSN 0009-2509
Grant/Contract Number:  
AC07-05ID14517
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Chemical Engineering Science
Additional Journal Information:
Journal Volume: 192; Journal Issue: C; Journal ID: ISSN 0009-2509
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 03 NATURAL GAS; TAP Reactor

Citation Formats

Kunz, M. Ross, Borders, Tammie, Redekop, Evgeniy, Yablonsky, Gregory S., Constales, Denis, Wang, Lucun, and Fushimi, Rebecca. Pulse response analysis using the Y-procedure: A data science approach. United States: N. p., 2018. Web. doi:10.1016/j.ces.2018.06.078.
Kunz, M. Ross, Borders, Tammie, Redekop, Evgeniy, Yablonsky, Gregory S., Constales, Denis, Wang, Lucun, & Fushimi, Rebecca. Pulse response analysis using the Y-procedure: A data science approach. United States. https://doi.org/10.1016/j.ces.2018.06.078
Kunz, M. Ross, Borders, Tammie, Redekop, Evgeniy, Yablonsky, Gregory S., Constales, Denis, Wang, Lucun, and Fushimi, Rebecca. 2018. "Pulse response analysis using the Y-procedure: A data science approach". United States. https://doi.org/10.1016/j.ces.2018.06.078. https://www.osti.gov/servlets/purl/1478468.
@article{osti_1478468,
title = {Pulse response analysis using the Y-procedure: A data science approach},
author = {Kunz, M. Ross and Borders, Tammie and Redekop, Evgeniy and Yablonsky, Gregory S. and Constales, Denis and Wang, Lucun and Fushimi, Rebecca},
abstractNote = {We report that pulse response experiments can provide a wealth of data for transient kinetic studies of gas phase heterogeneous reactions, with the ability to paint a detailed picture of intrinsic reaction kinetics pertaining to complex catalytic mechanisms. A novel framework called the Y-Procedure was developed by Yablonsky et al. to extract information from non-steady-state kinetic data (Yablonsky et al., 2007). The Y-Procedure reconstructs the chemical transformation rate and gas composition in the catalytic zone with no a priori assumptions on the kinetic model and is used to relate changes in catalytic reaction rates and kinetic parameters to changes in a catalyst’s surface composition. This paper provides a detailed description of the data science work flow implemented in the Y-procedure through an experimental example of oxygen adsorption on platinum. Lastly, this powerful method, along with a robust list of pre-processing methodology, will enable deeper understanding of kinetic processes and mechanism to be derived from the TAP pulse response technique.},
doi = {10.1016/j.ces.2018.06.078},
url = {https://www.osti.gov/biblio/1478468}, journal = {Chemical Engineering Science},
issn = {0009-2509},
number = C,
volume = 192,
place = {United States},
year = {Sat Jun 30 00:00:00 EDT 2018},
month = {Sat Jun 30 00:00:00 EDT 2018}
}

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Cited by: 8 works
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