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Activated Self-Resolution and Error-Correction in Catalytic Reaction Networks

preprint
submitted on 18.01.2021, 18:56 and posted on 19.01.2021, 13:28 by Fredrik Schaufelberger, Olof Ramstrom

To understand the emergence of function in complex reaction networks is a primary goal of systems chemistry and origin-of-life studies. Especially challenging is the establishment of systems that simultaneously exhibit several functionality parameters 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, displaying rate accelerations of retro-MBH reactions up to 104 times. This study demonstrates how efficient self-sorting of catalytic systems can be achieved through an interplay of several complex emergent functionalities.

History

Email Address of Submitting Author

olof_ramstrom@uml.edu

Institution

University of Massachusetts Lowell

Country

United States

ORCID For Submitting Author

0000-0002-1533-6514

Declaration of Conflict of Interest

No conflicts of interest

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