Integrating catalytic reactions with molecular assembly is a promising means of achieving controllable supramolecular polymerization.We report herein a novel and controllable method for in situ supramolecular polymeri...Integrating catalytic reactions with molecular assembly is a promising means of achieving controllable supramolecular polymerization.We report herein a novel and controllable method for in situ supramolecular polymerization via organometallic-catalyzed macromolecular metamorphosis.To this end,covalent polymers with polypentenamer backbones and pendant supramolecular motifs are designed and synthesized.By depolymerizing the polymers with Grubbs catalysts,the supramolecular motifs can be gradually released from the polymers to the solution.Supramolecular polymerization occurs when a critical concentration is reached.The supramolecular polymerization process was readily controlled by varying the rate of the depolymerization reaction.This work presents a novel approach that uses organometallic catalysis to transform covalent polymers into supramolecular polymers.It offers a new means of constructing complex molecular systems in a controllable manner.展开更多
基金We gratefully acknowledge the financial support from National Key R&D Program of China(grant no.2021YFA1501600)National Natural Science Foundation of China(grant no.21901077)+2 种基金Natural Science Foundation of Guangdong Province(grant no.2016ZT06C322)Open Project of State Key Laboratory for Supramolecular Structure and Materials(grant no.SKLSSM2021012)the Research Fund Program of Guangdong Provincial Key Laboratory of Functional and Intelligent Hybrid Materials and Devices(grant no.2019B121203003).
文摘Integrating catalytic reactions with molecular assembly is a promising means of achieving controllable supramolecular polymerization.We report herein a novel and controllable method for in situ supramolecular polymerization via organometallic-catalyzed macromolecular metamorphosis.To this end,covalent polymers with polypentenamer backbones and pendant supramolecular motifs are designed and synthesized.By depolymerizing the polymers with Grubbs catalysts,the supramolecular motifs can be gradually released from the polymers to the solution.Supramolecular polymerization occurs when a critical concentration is reached.The supramolecular polymerization process was readily controlled by varying the rate of the depolymerization reaction.This work presents a novel approach that uses organometallic catalysis to transform covalent polymers into supramolecular polymers.It offers a new means of constructing complex molecular systems in a controllable manner.