Abstract
With the aim of mimicking biological machines, in which the delicate arrangement of nanomechanical units lead to the output of specific functions upon the external stimulus, the construction of dual stimuli-responsive rotaxane-branched dendrimers was realized in this study. Starting from a switchable organometallic [2]rotaxane precursor, the employment of a controllable divergent approach allowed for the successful synthesis of a family of rotaxane-branched dendrimers up to the third generation with 21 switchable rotaxane moieties located on each branch. More importantly, upon the addition and removal of dimethylsulfoxide (DMSO) molecule or acetate anion as the external stimulus, the amplified responsiveness of the switchable rotaxane units endowed the resultant rotaxane-branched dendrimers the solvent- or anion-controlled molecular motions, thus leading to the dimension modulation. Therefore, we successfully constructed a family of rotaxane-branched dendrimers with dual stimuli-responsiveness that will be a privileged platform for the construction of dynamic supramolecular materials.
Highlights
With the aim of mimicking biological machines, in which the delicate arrangement of nanomechanical units lead to the output of specific functions upon the external stimulus, the construction of dual stimuli-responsive rotaxane-branched dendrimers was realized in this study
The inspiration of the construction of Mechanically interlocked molecules (MIMs)-based artificial molecular machines comes from the living systems, in which well self-organization of functional nanomechanical moieties enables the intriguing amplification of collective molecular motions to perform vital biological functions9–11
The introduction of switchable rotaxane units into the dendritic scaffold imparted the switchable feature to the resultant rotaxane-branched dendrimers when the external stimulus was added
Summary
With the aim of mimicking biological machines, in which the delicate arrangement of nanomechanical units lead to the output of specific functions upon the external stimulus, the construction of dual stimuli-responsive rotaxane-branched dendrimers was realized in this study. Upon the addition and removal of dimethylsulfoxide (DMSO) molecule or acetate anion as the external stimulus, the amplified responsiveness of the switchable rotaxane units endowed the resultant rotaxane-branched dendrimers the solvent- or anion-controlled molecular motions, leading to the dimension modulation. With the addition of dimethylsulfoxide (DMSO) molecule or acetate anion as the competitive hydrogen bonding acceptor, the directional and switchable mechanical motion of rotaxane on each branch was realized, leading to the dynamics and dimension modulation of the integrated rotaxane-branched dendrimers (Fig. 1). The controllable mechanical motions of rotaxane moieties could influence the dynamics and dimensions of rotaxane-branched dendrimers, which might be applied in the reversible uptake and release applications, or even switchable organocatalysis in the future
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