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Issue 13, 2020
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Catalytic resonance theory: parallel reaction pathway control

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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 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.

Graphical abstract: Catalytic resonance theory: parallel reaction pathway control

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Supplementary files

Article information


Submitted
04 Dec 2019
Accepted
02 Mar 2020
First published
03 Mar 2020

This article is Open Access
All publication charges for this article have been paid for by the Royal Society of Chemistry

Chem. Sci., 2020,11, 3501-3510
Article type
Edge Article

Catalytic resonance theory: parallel reaction pathway control

M. A. Ardagh, M. Shetty, A. Kuznetsov, Q. Zhang, P. Christopher, D. G. Vlachos, O. A. Abdelrahman and P. J. Dauenhauer, Chem. Sci., 2020, 11, 3501
DOI: 10.1039/C9SC06140A

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