Interfacial assembly of dendritic microcapsules with host–guest chemistry
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This chapter introduces microfluidic strategies to controllably prepare monodisperse hollow microcapsules with microfluidic-generated double emulsions as templates. Using microfluidic devices, monodisperse water-in-oil-in-water (W/O/W) double emulsions are obtained and used as templates to fabricate monodisperse EC microcapsules. Most of the attempts to prepare alginate microcapsules using single emulsions as templates usually result in solid microspheres. The chapter shows the preparation of micron-sized monodisperse calcium alginate microcapsules by combining the microfluidic emulsification with internal gelation. Microfluidic technology with precise manipulation of emulsion droplets and high encapsulation efficiency has already shown great potential in the fabrication of monodisperse microcapsules for encapsulation and delivery. Based on microfluidics, the chapter then shows a simple emulsion-template approach for fabricating monodisperse hydrogel-based microcapsules with repeated glucose response under physiological temperature and glucose concentration conditions. It also introduces the microfluidic fabrication of multi-stimuli-responsive microcapsules with adjustable controlled-release by embedding temperature-responsive submicrospheres as "microvalves" into the magnetic- and pH-responsive microcapsule membrane.
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Abstract Amphiphilicity is one of the molecular bases for self‐assembly. By tuning the amphiphilicity of building blocks, controllable self‐assembly can be realized. This article reviews different routes for tuning amphiphilicity and discusses different possibilities for self‐assembly and disassembly in a controlled manner. In general, this includes irreversible and reversible routes. The irreversible routes concern irreversible reactions taking place on the building blocks and changing their molecular amphiphilicity. The building blocks are then able to self‐assemble to form different supramolecular structures, but cannot remain stable upon loss of amphiphilicity. Compared to the irreversible routes, the reversible routes are more attractive due to the good control over the assembly and disassembly of the supramolecular structure formed via tuning of the amphiphilicity. These routes involve reversible chemical reactions and supramolecular approaches, and different external stimuli can be used to trigger reversible changes of amphiphilicity, including light, redox, pH, and enzymes. It is anticipated that this line of research can lead to the fabrication of new functional supramolecular assemblies and materials.
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This chapter contains sections titled: Self-Assembly. Self-Organization Programmed Supramolecular Systems Self-Assembly of Inorganic Architectures Self-Assembly of Double-Helical and Triple-Helical Metal Complexes: The Helicates Multicomponent Self-Assembly Supramolecular Arrays of Metal Ions. Racks, Ladders, Grids Self-Assembly of Organic Supramolecular Structures Self-Assembly by Hydrogen-Bonding. Janus Molecules Molecular Recognition-Directed Assembly of Organized Phases Supramolecular Polymer Chemistry Molecular Recognition-Directed Self-Assembly of Ordered Solid-State Structures Physico-Chemical Methods of Investigation Self-Recognition. Instructed System Paradigm Supramolecular Synthesis, Assistance and Replication Supramolecular Synthesis Supramolecular Assistance to Synthesis Replication. Self-Replication Supramolecular Chirality and Self-Assembly Supramolecular Materials. Nanochemistry Chemionics
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The supramolecular oligomers play an important role because their preorganized precise structures lead to a well-defined structure–property relationship. Here, we employed an α-hemolysin nanopore as a single molecule tool to investigate the self-assembly supramolecular oligomers of bis(p-sulfonatocalix[4]arene) (bisSC4) and bis(methylviologen) (bisMV4+). The self-assembly of supramolecular oligomers could be dynamic monitored at single molecule level. The association constant between bisSC4 and bisMV4+ was calculated based on current blockage frequencies at the single molecule level. This work provides a complementary method to characterize the self-assembly oligomers with low molecular weight in solution.
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This manuscript reports the synthesis and the self-assembly of (4-3,4,5-3,5)nG2-CH2-Boc-l-Tyr-l-Ala-OMe dendritic dipeptides (n = 12, 16). These dendritic dipeptides self-assemble both in solution and in solid states into helical porous supramolecular columns that mimic porous transmembrane proteins. These supramolecular assemblies provide also a new class of tubular supramolecular polymers.
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In the past few years, a new family of supramolecular metallodendrimers, which possess cavities with well-defined shape and size, have attracted widespread attention. Coordination-driven self-assembly has proven to be a simple and highly efficient approach for the preparation of cavity-cored supramolecular metallodendrimers. This feature article focuses on the recent progress in the construction of a variety of cavity-cored supramolecular metallodendrimers via coordination-driven self-assembly. The characterization and hierarchical self-assembly behaviour of such metallodendrimers are also discussed.
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Metallo-supramolecular self-assembly tends to be performed with single metal ions and single, highly symmetrical, ligands. This simplifies the self-assembly process as without sufficient bias within the system a mixture of products may be formed. However, with various applications of metallo-supramolecular species having been demonstrated, the ability to generate more intricate architectures is keenly sought after. The use of reduced symmetry ligands is one route to this goal, and allows access to lower-symmetry assemblies. Multiple coordination pockets can also be introduced in this manner, giving rise to assemblies with metal ions in different coordination environments, which can be exploited for the controlled synthesis of mixed-metal species. Herein we discuss the different approaches that have been used to control self-assembly with low symmetry ligands, including the use of mixed-denticity ligands, the incorporation of geometric constraints, charge separation strategies and the use of repulsive or attractive non-covalent interactions between ligands.
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Abstract The control over supramolecular interactions and obtaining information beyond the molecular scale is an extended challenge. The intriguing self‐assembly of a perylene‐3,4,9,10‐tetracarboxylic acid diimide (PDI)‐based novel bolaamphiphilic probe is experienced within an artificial environment that is restrained by using supramolecular crystallization and molecular recognition. The bolaamphiphile with a hydrophilic [18]‐azacrown ether ring produced nanoaggregates due to differing solubilities in organic and aqueous media. A structural evolution was observed in the presence of alkali metal ions as guests. The metal complexes form a pseudo‐cationic structure, which is further involved in an ionic self‐assembly with biomolecules, thus resulting new spectroscopic information on the dye self‐assembly. The overarching aim of this study is to emphasize the importance of the concept of supramolecular adaptability, which has been used to establish an environment‐friendly behavior based on noncovalent forces, thus leading to the evolution of new assembly structures and photophysical properties.
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