Supramolecular host–guest systems are generally at thermodynamic equilibrium states or in kinetically trapped states.Herein,we demonstrate the concept of a chemical fuel-driven competitive host–guest assembly featur...Supramolecular host–guest systems are generally at thermodynamic equilibrium states or in kinetically trapped states.Herein,we demonstrate the concept of a chemical fuel-driven competitive host–guest assembly featuring autonomous dynamics.The enabling key principle is to design a chemical fuel that possesses a high binding affinity to defeat the guest transiently,undergoes conversion to a waste product,and exhibit weak binding affinity in order to recover the original host–guest pair.By following this principle,adenosine triphosphate(ATP;chemical fuel and competitive guest),biguanidine-functionalizedβ-cyclodextrin(βCD;host),and an adamantine species(ADA;guest)have been engineered to construct dynamic adaptive macrogels or chemo-mechanochromic microgels with programmed time domains.Our reported methodology provides temporal control over the host–guest process,representing a conceptually new tool for the design of living supramolecular materials.展开更多
基金funded by the Beijing Natural Science Foundation(grant no.6214041)Fundamental Research Funds for the Central Universities(grant no.BLX201918)+1 种基金China Postdoctoral Science Foundation(grant no.2020M670176)the Project of State Key Laboratory of Molecular Engineering of Polymers of Fudan University(grant no.K2021-21).
文摘Supramolecular host–guest systems are generally at thermodynamic equilibrium states or in kinetically trapped states.Herein,we demonstrate the concept of a chemical fuel-driven competitive host–guest assembly featuring autonomous dynamics.The enabling key principle is to design a chemical fuel that possesses a high binding affinity to defeat the guest transiently,undergoes conversion to a waste product,and exhibit weak binding affinity in order to recover the original host–guest pair.By following this principle,adenosine triphosphate(ATP;chemical fuel and competitive guest),biguanidine-functionalizedβ-cyclodextrin(βCD;host),and an adamantine species(ADA;guest)have been engineered to construct dynamic adaptive macrogels or chemo-mechanochromic microgels with programmed time domains.Our reported methodology provides temporal control over the host–guest process,representing a conceptually new tool for the design of living supramolecular materials.
