Catalytic resonance theory: parallel reaction pathway control
Abstract
Catalytic enhancement of chemical reactions via heterogeneous materials occurs through stabilization of transition states at designed active sites, but dramatically greater rate acceleration on that same active site can be achieved when the surface intermediates oscillate in binding energy. The applied oscillation amplitude and frequency can accelerate reactions orders of magnitude above the catalytic rates of static systems, provided the active site dynamics are tuned to the natural frequencies of the surface chemistry. In this work, differences in the characteristics of parallel reactions are exploited via selective application of active site dynamics (0 < ΔU < 1.0 eV amplitude, 10-6 < f < 104 Hz frequency) to control the extent of competing reactions occurring on the shared catalytic surface. Simulation of multiple parallel reaction systems with broad range of variation in chemical parameters revealed that parallel chemistries are highly tunable in selectivity between either pure product, even when specific products are not selectively produced under static conditions. Two mechanisms leading to dynamic selectivity control were identified: (i) surface thermodynamic control of one product species under strong binding conditions, or (ii) catalytic resonance of the kinetics of one reaction over the other. These dynamic parallel pathway control strategies applied to amore »
- Authors:
-
[1];
[2];
[2];
[2];
[3];
[4];
[3];
[1]
- Department of Chemical Engineering and Materials Science, University of Minnesota, Minneapolis, USA, Catalysis Center for Energy Innovation
- Department of Chemical Engineering and Materials Science, University of Minnesota, Minneapolis, USA
- Catalysis Center for Energy Innovation, University of Delaware, Newark, USA, Department of Chemical Engineering
- Catalysis Center for Energy Innovation, University of Delaware, Newark, USA, Department of Chemical and Biomolecular Engineering
- Publication Date:
- Research Org.:
- Univ. of Delaware, Newark, DE (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1604103
- Alternate Identifier(s):
- OSTI ID: 1801383
- Grant/Contract Number:
- SC0001004
- Resource Type:
- Published Article
- Journal Name:
- Chemical Science
- Additional Journal Information:
- Journal Name: Chemical Science Journal Volume: 11 Journal Issue: 13; Journal ID: ISSN 2041-6520
- Publisher:
- Royal Society of Chemistry (RSC)
- Country of Publication:
- United Kingdom
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Citation Formats
Ardagh, M. Alexander, Shetty, Manish, Kuznetsov, Anatoliy, Zhang, Qi, Christopher, Phillip, Vlachos, Dionisios G., Abdelrahman, Omar A., and Dauenhauer, Paul J. Catalytic resonance theory: parallel reaction pathway control. United Kingdom: N. p., 2020.
Web. doi:10.1039/C9SC06140A.
Ardagh, M. Alexander, Shetty, Manish, Kuznetsov, Anatoliy, Zhang, Qi, Christopher, Phillip, Vlachos, Dionisios G., Abdelrahman, Omar A., & Dauenhauer, Paul J. Catalytic resonance theory: parallel reaction pathway control. United Kingdom. https://doi.org/10.1039/C9SC06140A
Ardagh, M. Alexander, Shetty, Manish, Kuznetsov, Anatoliy, Zhang, Qi, Christopher, Phillip, Vlachos, Dionisios G., Abdelrahman, Omar A., and Dauenhauer, Paul J. Wed .
"Catalytic resonance theory: parallel reaction pathway control". United Kingdom. https://doi.org/10.1039/C9SC06140A.
@article{osti_1604103,
title = {Catalytic resonance theory: parallel reaction pathway control},
author = {Ardagh, M. Alexander and Shetty, Manish and Kuznetsov, Anatoliy and Zhang, Qi and Christopher, Phillip and Vlachos, Dionisios G. and Abdelrahman, Omar A. and Dauenhauer, Paul J.},
abstractNote = {Catalytic enhancement of chemical reactions via heterogeneous materials occurs through stabilization of transition states at designed active sites, but dramatically greater rate acceleration on that same active site can be achieved when the surface intermediates oscillate in binding energy. The applied oscillation amplitude and frequency can accelerate reactions orders of magnitude above the catalytic rates of static systems, provided the active site dynamics are tuned to the natural frequencies of the surface chemistry. In this work, differences in the characteristics of parallel reactions are exploited via selective application of active site dynamics (0 < ΔU < 1.0 eV amplitude, 10-6 < f < 104 Hz frequency) to control the extent of competing reactions occurring on the shared catalytic surface. Simulation of multiple parallel reaction systems with broad range of variation in chemical parameters revealed that parallel chemistries are highly tunable in selectivity between either pure product, even when specific products are not selectively produced under static conditions. Two mechanisms leading to dynamic selectivity control were identified: (i) surface thermodynamic control of one product species under strong binding conditions, or (ii) catalytic resonance of the kinetics of one reaction over the other. These dynamic parallel pathway control strategies applied to a host of simulated chemical conditions indicate significant potential for improving the catalytic performance of many important industrial chemical reactions beyond their existing static performance.},
doi = {10.1039/C9SC06140A},
journal = {Chemical Science},
number = 13,
volume = 11,
place = {United Kingdom},
year = {2020},
month = {4}
}
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