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Activated Self‐Resolution and Error‐Correction in Catalytic Reaction Networks **
Author(s) -
Schaufelberger Fredrik,
Ramström Olof
Publication year - 2021
Publication title -
chemistry – a european journal
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 1.687
H-Index - 242
eISSN - 1521-3765
pISSN - 0947-6539
DOI - 10.1002/chem.202100208
Subject(s) - nucleophile , catalysis , adduct , set (abstract data type) , function (biology) , sorting , chemistry , molecule , resolution (logic) , computer science , combinatorial chemistry , organic chemistry , algorithm , artificial intelligence , evolutionary biology , biology , programming language
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.