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Activated Self-Resolution and Error-Correction in Catalytic Reaction Networks*.
- Source :
-
Chemistry (Weinheim an der Bergstrasse, Germany) [Chemistry] 2021 Jul 16; Vol. 27 (40), pp. 10335-10340. Date of Electronic Publication: 2021 Apr 30. - Publication Year :
- 2021
-
Abstract
- Understanding the emergence of function in complex reaction networks is a primary goal of systems chemistry and origin-of-life studies. Especially challenging is to create systems that simultaneously exhibit several emergent functions that can be independently tuned. In this work, a multifunctional complex reaction network of nucleophilic small molecule catalysts for the Morita-Baylis-Hillman (MBH) reaction is demonstrated. The dynamic system exhibited triggered self-resolution, preferentially amplifying a specific catalyst/product set out of a many potential alternatives. By utilizing selective reversibility of the products of the reaction set, systemic thermodynamically driven error-correction could also be introduced. To achieve this, a dynamic covalent MBH reaction based on adducts with internal H-transfer capabilities was developed. By careful tuning of the substituents, rate accelerations of retro-MBH reactions of up to four orders of magnitude could be obtained. This study thus demonstrates how efficient self-sorting of catalytic systems can be achieved through an interplay of several complex emergent functionalities.<br /> (© 2021 Wiley-VCH GmbH.)
- Subjects :
- Catalysis
Stereoisomerism
Subjects
Details
- Language :
- English
- ISSN :
- 1521-3765
- Volume :
- 27
- Issue :
- 40
- Database :
- MEDLINE
- Journal :
- Chemistry (Weinheim an der Bergstrasse, Germany)
- Publication Type :
- Academic Journal
- Accession number :
- 33780566
- Full Text :
- https://doi.org/10.1002/chem.202100208