- Constitutional Dynamic Selection at Low Reynolds Number in a Triple Dynamic System: Covalent Dynamic Adaptation Driven by Double Supramolecular Self-Assembly
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A triple dynamic complex system has been designed, implementing a dynamic covalent process coupled to two supramolecular self-assembly steps. To this end, two dynamic covalent libraries (DCLs), DCL-1 and DCL-2, have been established on the basis of dynamic covalent C-C/C-N organo-metathesis between two Knoevenagel derivatives and two imines. Each DCL contains a barbituric acid-based Knoevenagel constituent that may undergo a sequential double self-organization process involving first the formation of hydrogen-bonded hexameric supramolecular macrocycles that subsequently undergo stacking to generate a supramolecular polymer SP yielding a viscous gel state. Both DCLs display selective self-organization-driven amplification of the constituent that leads to the SP. Dissociation of the SP on heating causes reversible randomization of the constituent distributions of the DCLs as a function of temperature. Furthermore, diverse distribution patterns of DCL-2 were induced by modulation of temperature and solvent composition. The present dynamic systems display remarkable self-organization-driven constitutional adaption and tunable composition by coupling between dynamic covalent component selection and two-stage supramolecular organization. In more general terms, they reveal dynamic adaptation by component selection in low Reynolds number conditions of living systems where frictional effects dominate inertial behavior.
- Gu, Ruirui,Lehn, Jean-Marie
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p. 14136 - 14146
(2021/09/15)
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- Self-organization of hydrogen-bonding naphthalene chromophores into J-type nanorings and H-type nanorods: Impact of regioisomerism
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Regioisomers of self-assembling molecules resulted in the evolution of distinct 0D and 1D nanostructures, namely nanorings and nanorods (see picture). J- and H-type excitonic coupling of naphthalene chromophores was found in the nanostructures. The bulk l
- Yagai, Shiki,Goto, Yusaku,Lin, Xu,Karatsu, Takashi,Kitamura, Akihide,Kuzuhara, Daiki,Yamada, Hiroko,Kikkawa, Yoshihiro,Saeki, Akinori,Seki, Shu
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supporting information; experimental part
p. 6643 - 6647
(2012/08/13)
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