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

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.


Email Address of Submitting Author


University of Massachusetts Lowell


United States

ORCID For Submitting Author


Declaration of Conflict of Interest

No conflicts of interest