Self-sorting of equilibrating metallosupramolecular DCLs via constitutional crystallization

摘要

Zn~(2+) and Pb~(2+) and ligands 1 and 2 self-assemble in solution to generate DCLs of interexchanging metallosupramolecular subcomponents, which convert into robust species of unique stoichiometry via constitutional crystallization.rnDynamic combinatorial chemistry (DCC) has been used as a powerful tool to discover new receptors, drugs, catalysts and materials. The reversible interactions of molecular systems serve to bring into play the constitutional evolution of dynamic systems toward the selection of exchanging architectures. This can be related to "chemical collectivism"~(2a) as described some years ago by Menger, giving rise nowadays to the emerging discipline of "systems chemistry".~(2b-d) In the past few years, new different approaches to DCC have been reported for the resolution of dynamic combinatorial libraries (DCL), notably by freezing the reversible equilibria of DCL. Investigations on DCC by Ramstroem et al. have highlighted the wide potentialities of dynamic combinatorial resolution processes (DCR) of molecular DCLs, kinetically controlled in the second step by irreversible enzymatic and tandem reactions or by crystallization.