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Additive-assisted macroscopic self-assembly and control of the shape of assemblies based on host-guest interaction
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DOI：10.1038/s41598-024-71649-z.png)
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Abstract
En 中文
In these decades, considerable attention has focused on supramolecular polymers due to their unique structures and properties. More recently, macroscopic supramolecular polymers have attracted increasing interest from not only biologists but also materials scientists inspired by the sophisticated structures and functions of living organisms. Since the functions of supramolecular polymers are strongly dependent on their shape, control of the shape is an important issue in controlling the functions of supramolecular polymers. However, the control of shape in macroscopic supramolecular assemblies has not yet been sufficiently investigated. Previously, we studied the macroscopic self-assembly behavior of super absorbent polymer (SAP) microparticles modified with beta-cyclodextrin (beta CD) and adamantane (Ad) residues (beta CD(x)-SAP and Ad(y)-SAP microparticles, where x and y are the mol% contents of beta CD and Ad residues, respectively). More elongated assemblies were formed at higher y, indicating that the shape of assemblies can be controlled by varying the interaction strength. The noteworthy is that 1-adamantanamine hydrochloride (AdNH(3)Cl) assisted the formation of assemblies from beta CD(x)-SAP and Ad(y)-SAP microparticles, indicating that AdNH(3)Cl acts as a chemical stimulus for macroscopic assemblies of beta CD(x)-SAP and Ad(y)-SAP microparticles. In this study, we have thus studied the assembling behavior of beta CD(x)-SAP microparticles with Ad(y)-SAP microparticles and unmodified SAP microparticles assisted by AdNH(3)Cl, as well as the shape of the resulting macroscopic assemblies. AdNH(3)Cl assisted the formation of assemblies from beta CD(16.2)-SAP and Ad(15.1)-SAP microparticles, in which AdNH(3)Cl crosslinked the SAP microparticles through the formation of inclusion complexes of beta CD residues with the Ad residue and the electrostatic interaction of ammonium and carboxylate residues. Assemblies of beta CD(26.7)-SAP and unmodified SAP microparticles were formed at the concentrations of AdNH(3)Cl ([AdNH(3)Cl](0)) higher than a certain level (ca. 0.05 mM). The aspect ratio (a/b) of assemblies showed a maximum at [AdNH(3)Cl](0)similar to 0.10 mM, indicating that the chemical stimulus, i.e., addition of AdNH(3)Cl, controls the shape of assemblies formed from beta CD(26.7)-SAP and unmodified SAP microparticles. This study suggests that other stimuli, e.g., heat, pH, light, redox, and force, can be utilized to control the shape of macroscopic assemblies based on supramolecular interactions.
Keywords:
Macroscopic self-assembly
Host-guest interaction
Super absorbent polymer microparticles
Cyclodextrin
Amines
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