Skip to main content

Lund University Publications

LUND UNIVERSITY LIBRARIES

Dissipative Cyclic Reaction Networks : Mechanistic Insights into a Minor Enantiomer Recycling Process

Margarita, Cristiana ; Nash, Anna Laurell ; Ahlstrand, David A. ; Ahlquist, Mårten S.G. ; Wendt, Ola F. LU ; Fransson, Linda and Moberg, Christina (2024) In ChemSystemsChem 6(2).
Abstract

An analysis of an out-of-equilibrium cyclic reaction network which continuously converts a minor undesired product enantiomer to the desired major enantiomer by irreversible addition of chemical fuel and irreversible elimination of spent fuel is presented. The reaction network is maintained as long as fuel is added; interrupted fuel addition drives the system towards equilibrium, but the cyclic process restarts upon resumed fuel addition, as demonstrated by three consecutive fuel cycles. The process is powered by the hydrolysis of methyl cyanoformate to HCN and monomethyl carbonic acid, which decomposes to CO2 and MeOH. The time it takes to reach steady state depends on the rate of conversion of the fuel and decreases with... (More)

An analysis of an out-of-equilibrium cyclic reaction network which continuously converts a minor undesired product enantiomer to the desired major enantiomer by irreversible addition of chemical fuel and irreversible elimination of spent fuel is presented. The reaction network is maintained as long as fuel is added; interrupted fuel addition drives the system towards equilibrium, but the cyclic process restarts upon resumed fuel addition, as demonstrated by three consecutive fuel cycles. The process is powered by the hydrolysis of methyl cyanoformate to HCN and monomethyl carbonic acid, which decomposes to CO2 and MeOH. The time it takes to reach steady state depends on the rate of conversion of the fuel and decreases with increased conversion rate. Three catalysts, one metal catalyst and two enzymes, together constitute an efficient regulation system allowing control of the forward, backward and waste-forming steps, thereby assuring the production of high yields of products with high enantiopurity.

(Less)
Please use this url to cite or link to this publication:
author
; ; ; ; ; and
organization
publishing date
type
Contribution to journal
publication status
published
subject
keywords
catalysts, enantioselective, kinetic modeling, out-of-equilibrium systems, regulation
in
ChemSystemsChem
volume
6
issue
2
article number
e202300045
publisher
Wiley
external identifiers
  • scopus:85187624737
ISSN
2570-4206
DOI
10.1002/syst.202300045
language
English
LU publication?
yes
id
faad1713-d01c-444c-b615-0da35ba9901f
date added to LUP
2024-04-10 11:49:39
date last changed
2024-04-10 13:14:18
@article{faad1713-d01c-444c-b615-0da35ba9901f,
  abstract     = {{<p>An analysis of an out-of-equilibrium cyclic reaction network which continuously converts a minor undesired product enantiomer to the desired major enantiomer by irreversible addition of chemical fuel and irreversible elimination of spent fuel is presented. The reaction network is maintained as long as fuel is added; interrupted fuel addition drives the system towards equilibrium, but the cyclic process restarts upon resumed fuel addition, as demonstrated by three consecutive fuel cycles. The process is powered by the hydrolysis of methyl cyanoformate to HCN and monomethyl carbonic acid, which decomposes to CO<sub>2</sub> and MeOH. The time it takes to reach steady state depends on the rate of conversion of the fuel and decreases with increased conversion rate. Three catalysts, one metal catalyst and two enzymes, together constitute an efficient regulation system allowing control of the forward, backward and waste-forming steps, thereby assuring the production of high yields of products with high enantiopurity.</p>}},
  author       = {{Margarita, Cristiana and Nash, Anna Laurell and Ahlstrand, David A. and Ahlquist, Mårten S.G. and Wendt, Ola F. and Fransson, Linda and Moberg, Christina}},
  issn         = {{2570-4206}},
  keywords     = {{catalysts; enantioselective; kinetic modeling; out-of-equilibrium systems; regulation}},
  language     = {{eng}},
  number       = {{2}},
  publisher    = {{Wiley}},
  series       = {{ChemSystemsChem}},
  title        = {{Dissipative Cyclic Reaction Networks : Mechanistic Insights into a Minor Enantiomer Recycling Process}},
  url          = {{http://dx.doi.org/10.1002/syst.202300045}},
  doi          = {{10.1002/syst.202300045}},
  volume       = {{6}},
  year         = {{2024}},
}