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

Author(s):  
Fredrik Schaufelberger ◽  
Olof Ramström
2021 ◽  
Author(s):  
Fredrik Schaufelberger ◽  
Olof Ramstrom

<p>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.</p>


2021 ◽  
Author(s):  
Fredrik Schaufelberger ◽  
Olof Ramstrom

<p>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.</p>


2001 ◽  
Vol 25 (9-10) ◽  
pp. 1185-1198 ◽  
Author(s):  
Sergio P. Bressa ◽  
Néstor J. Mariani ◽  
Néstor O. Ardiaca ◽  
Germán D. Mazza ◽  
Osvaldo M. Martı́nez ◽  
...  

Author(s):  
Alessandro Filisetti ◽  
◽  
Alex Graudenzi ◽  
Chiara Damiani ◽  
Marco Villani ◽  
...  

Life ◽  
2019 ◽  
Vol 9 (2) ◽  
pp. 53
Author(s):  
Atsushi Kamimura ◽  
Kunihiko Kaneko

A great variety of molecular components is encapsulated in cells. Each of these components is replicated for cell reproduction. To address the essential role of the huge diversity of cellular components, we studied a model of protocells that convert resources into catalysts with the aid of a catalytic reaction network. As the resources were limited, the diversity in the intracellular components was found to be increased to allow the use of diverse resources for cellular growth. A scaling relation was demonstrated between resource abundances and molecular diversity. In the present study, we examined how the molecular species diversify and how complex catalytic reaction networks develop through an evolutionary course. At some generations, molecular species first appear as parasites that do not contribute to the replication of other molecules. Later, the species turn into host species that contribute to the replication of other species, with further diversification of molecular species. Thus, a complex joint network evolves with this successive increase in species. The present study sheds new light on the origin of molecular diversity and complex reaction networks at the primitive stage of a cell.


1993 ◽  
Vol 63 (3-4) ◽  
pp. 378-392 ◽  
Author(s):  
Peter F. Stadler ◽  
Walter Fontana ◽  
John H. Miller

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