10.1021/ja4067805.s001
Morteza Malakoutikhah
Morteza
Malakoutikhah
Jérôme J.-P. Peyralans
Jérôme J.-P.
Peyralans
Mathieu Colomb-Delsuc
Mathieu
Colomb-Delsuc
Hugo Fanlo-Virgós
Hugo
Fanlo-Virgós
Marc C. A. Stuart
Marc
C. A. Stuart
Sijbren Otto
Sijbren
Otto
Uncovering
the Selection Criteria for the Emergence
of Multi-Building-Block Replicators from Dynamic Combinatorial Libraries
American Chemical Society
2013
material
selection criteria
replication pathway
replicators need
library members
MW
Selection Criteria
molecule
combinatorial chemistry
5.6 kDa
emergence
future discovery
combinatorial libraries
fibril fragmentation
Dynamic Combinatorial LibrariesA family
macrocycle size
tunable ring size
2013-12-11 00:00:00
Journal contribution
https://acs.figshare.com/articles/journal_contribution/Uncovering_the_Selection_Criteria_for_the_Emergence_of_Multi_Building_Block_Replicators_from_Dynamic_Combinatorial_Libraries/2343721
A family of self-replicating macrocycles
was developed using dynamic
combinatorial chemistry. Replication is driven by self-assembly of
the replicators into fibrils and relies critically on mechanically
induced fibril fragmentation. Analysis of separate dynamic combinatorial
libraries made from one of six peptide-functionalized building blocks
of different hydrophobicity revealed two selection criteria that govern
the emergence of replicators from these systems. First, the replicators
need to have a critical macrocycle size that endows them with sufficient
multivalency to enable their self-assembly into fibrils. Second, efficient
replication occurs only for library members that are of low abundance
in the absence of a replication pathway. This work has led to spontaneous
emergence of replicators with unrivalled structural complexity, being
built from up to eight identical subunits and reaching a MW of up
to 5.6 kDa. The insights obtained in this work provide valuable guidance
that should facilitate future discovery of new complex self-replicating
molecules. They may also assist in the development of new self-synthesizing
materials, where self-assembly drives the synthesis of the very molecules
that self-assemble. To illustrate the potential of this concept, the
present system enables access to self-assembling materials made from
self-synthesizing macrocycles with tunable ring size ranging from
trimers to octamers.