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Shape-assisted self-assembly.

ABSTRACT: Self-assembly and molecular recognition are critical processes both in life and material sciences. They usually depend on strong, directional non-covalent interactions to gain specificity and to make long-range organization possible. Most supramolecular constructs are also at least partially governed by topography, whose role is hard to disentangle. This makes it nearly impossible to discern the potential of shape and motion in the creation of complexity. Here, we demonstrate that long-range order in supramolecular constructs can be assisted by the topography of the individual units even in the absence of highly directional interactions. Molecular units of remarkable simplicity self-assemble in solution to give single-molecule thin two-dimensional supramolecular polymers of defined boundaries. This dramatic example spotlights the critical function that topography can have in molecular assembly and paves the path to rationally designed systems of increasing sophistication.

SUBMITTER: Woods JF

PROVIDER: S-EPMC9237116 | biostudies-literature | 2022 Jun

REPOSITORIES: biostudies-literature

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Shape-assisted self-assembly.

Woods Joseph F JF Gallego Lucía L Pfister Pauline P Maaloum Mounir M Vargas Jentzsch Andreas A Rickhaus Michel M

Nature communications 20220627 1

Self-assembly and molecular recognition are critical processes both in life and material sciences. They usually depend on strong, directional non-covalent interactions to gain specificity and to make long-range organization possible. Most supramolecular constructs are also at least partially governed by topography, whose role is hard to disentangle. This makes it nearly impossible to discern the potential of shape and motion in the creation of complexity. Here, we demonstrate that long-range ord ...[more]

PMID: 35760814

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Project description: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 β-cyclodextrin (βCD) and adamantane (Ad) residues (βCD(x)-SAP and Ad(y)-SAP microparticles, where x and y are the mol% contents of βCD 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 (AdNH3Cl) assisted the formation of assemblies from βCD(x)-SAP and Ad(y)-SAP microparticles, indicating that AdNH3Cl acts as a chemical stimulus for macroscopic assemblies of βCD(x)-SAP and Ad(y)-SAP microparticles. In this study, we have thus studied the assembling behavior of βCD(x)-SAP microparticles with Ad(y)-SAP microparticles and unmodified SAP microparticles assisted by AdNH3Cl, as well as the shape of the resulting macroscopic assemblies. AdNH3Cl assisted the formation of assemblies from βCD(16.2)-SAP and Ad(15.1)-SAP microparticles, in which AdNH3Cl crosslinked the SAP microparticles through the formation of inclusion complexes of βCD residues with the Ad residue and the electrostatic interaction of ammonium and carboxylate residues. Assemblies of βCD(26.7)-SAP and unmodified SAP microparticles were formed at the concentrations of AdNH3Cl ([AdNH3Cl]0) higher than a certain level (ca. 0.05 mM). The aspect ratio (a/b) of assemblies showed a maximum at [AdNH3Cl]0 ~ 0.10 mM, indicating that the chemical stimulus, i.e., addition of AdNH3Cl, controls the shape of assemblies formed from βCD(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.

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Shape-assisted self-assembly.

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Shape-assisted self-assembly.

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