Kinetic Self-Sorting of Dynamic Covalent Catalysts with Systemic Feedback Regulation.
Constructing small molecule systems that mimic the functionality exhibited in biological reaction networks is a key objective of systems chemistry. Herein, we report the development of a dynamic catalytic system where the catalyst activity is modulated through a dynamic covalent bond. By connecting a thermodynamically controlled rearrangement process to resolution under kinetic control, the catalyst system underwent kinetic self-sorting, resulting in amplification of a more reactive catalyst while establishing a catalytic feedback mechanism. The dynamic catalyst system furthermore responded to catalytic events by self-perturbation to regulate its own activity, which in the case of upregulation gave rise to systemic autocatalytic behavior.
Department of Chemistry, KTH-Royal Institute of Technology , Teknikringen 30, S-10044 Stockholm, Sweden.
Fredrik
F
Schaufelberger
Department of Chemistry, KTH-Royal Institute of Technology , Teknikringen 30, S-10044 Stockholm, Sweden.
Olof
O
Ramström