Traditionally, synthetic chemistry has always focused on yielding a target compoundfrom the linear application of chemical transformations. After each step, a singlecompound is usually required and the presence of mixtures often demands lengthypurification prior to the next synthetic step. The emerging field of systems chemistryaims to study the currently under-exploited science of networks and complex mixtures. Through the chemistry of reversible chemical bonds, dynamic covalent chemistry (DCC), the creation of networks of compounds linked through a plethora of equilibrium processes, termed dynamic combinatorial libraries (DCLs), is possible. In this research, a DCL based on imine/nitrone exchange is designed and presented. The DCL is subsequently coupled to an irreversible chemical reaction based on molecular recognition and the dramatic responses observed within the DCL are discussed.The properties of the dynamic systems developed during the course of this researchare then applied to the competition between emerging self-replicators in an attempt todemonstrate Darwinian Evolution. A thorough discussion of the inherent limitationsplaced upon a system by kinetic selection is presented in the context of self-replicators.Finally, non-linear chemical dynamics are discussed and successfully incorporatedinto a competitive replication scenario. The application of reaction diffusion frontsallows a self-replicating system to break the stranglehold of kinetic selection andexhibit its dominance over weaker competitors.
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Overcoming limited selectivity in recognition-mediated replicating systems
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