Challenges and breakthroughs in recent research on self-assembly

Ariga, Katsuhiko; Hill, Jonathan P.; Lee, Michael V.; Vinu, Ajayan; Charvet, Richard; Acharya, Somobrata

doi:10.1088/1468-6996/9/1/014109

Cited by 729 publications

(407 citation statements)

References 1,021 publications

(781 reference statements)

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“…Although numerous excellent articles and reviews on the template synthesis have been published [35,36], the comprehensive reviews of LLC-directed synthesis are relatively few [37,38]. In 2007, Hegmann et al gave a short overview of current research in LC nanoscience [39].…”

Section: Liquid Crystals (Lcs)mentioning

confidence: 99%

Lyotropic liquid crystal directed synthesis of nanostructured materials

Wang

Chen

Jiao

2009

Science and Technology of Advanced Materials

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This review introduces and summarizes lyotropic liquid crystal (LLC) directed syntheses of nanostructured materials consisting of porous nanostructures and zero-dimensional (0-D), one-dimensional (1-D) and two-dimensional (2-D) nanostructures. After a brief introduction to the liquid crystals, the LLCs used to prepare mesoporous materials are discussed; in particular, recent advances in controlling mesostructures are summarized. The LLC templates directing the syntheses of nanoparticles, nanorods, nanowires and nanoplates are also presented. Finally, future development in this field is discussed.

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Section: Liquid Crystals (Lcs)mentioning

confidence: 99%

Lyotropic liquid crystal directed synthesis of nanostructured materials

Wang

Chen

Jiao

2009

Science and Technology of Advanced Materials

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“…In a growing effort to emulate the efficacy of biological receptors and enzymes, studies of the preparative, guest-binding, and catalytic properties of synthetic assemblies have been pursued (14)(15)(16)(17)(18)(19)(20)(21). Whereas guest encapsulation has been reported in a variety of media, association processes of organic guests are generally more thermodynamically favorable in water (22,23).…”

mentioning

confidence: 99%

Protein-like proton exchange in a synthetic host cavity

Hart‐Cooper

Sgarlata

Perrin

et al. 2015

Proc. Natl. Acad. Sci. U.S.A.

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The mechanism of proton exchange in a metal-ligand enzyme active site mimic (compound 1) is described through amide hydrogendeuterium exchange kinetics. The type and ratio of cationic guest to host in solution affect the rate of isotope exchange, suggesting that the rate of exchange is driven by a host whose cavity is occupied by water. Rate constants for acid-, base-, and watermediated proton exchange vary by orders of magnitude depending on the guest, and differ by up to 200 million-fold relative to an alanine polypeptide. These results suggest that the unusual microenvironment of the cavity of 1 can dramatically alter the reactivity of associated water by magnitudes comparable to that of enzymes.W ater-mediated proton transfer in molecular cavities plays an essential role in the function of nature's remarkable metabolic machinery (1, 2). Of the broad diversity of enzymecatalyzed reactions, those involving transfer of hydrogen are ubiquitous and of high fundamental importance (3). For instance, ATP synthase employs an internal chain of water molecules to mediate proton transfer across an electrochemical gradient (4, 5). This process drives ATP synthesis, which allows organisms to broadly meet their basic energy needs. Recent studies of tunneling in enzymatic hydron transfer reactions have other far-reaching and broad implications, namely the importance of the dynamic enzyme motions in driving catalysis (6, 7).Of the methods used to study hydron transfer, kinetic studies of the mechanisms of amide hydrogen-deuterium exchange (HDX) have helped to elucidate the dynamic interactions between water and protein surfaces that are central to the unique capabilities of enzymes (8-13). Noncovalent interactions, such as electrostatic effects and hydrogen bonding, have also been shown to exert a significant influence on amide HDX rates. These properties are manifest in amide HDX rate constants that can vary by a factor of a billion for residues on the same protein (8). How these variations arise, and how such a property could be harnessed to drive enzyme-like reactivity, remain challenging questions.In a growing effort to emulate the efficacy of biological receptors and enzymes, studies of the preparative, guest-binding, and catalytic properties of synthetic assemblies have been pursued (14-21). Whereas guest encapsulation has been reported in a variety of media, association processes of organic guests are generally more thermodynamically favorable in water (22, 23). Central to these studies is the notion that the displacement of a high-energy water cluster from a receptor drives guest association, and in some cases, subsequent catalysis. However, despite the abundance of structural data documenting diverse water clusters encapsulated in various host cavities, mechanistic descriptions of the dynamic processes between water and host are rare (24-32).As part of the broader field of synthetic hosts previously mentioned, our group has developed a class of biologically inspired, anionic K 12 Ga 4 L 6 assemblies that exhibit cat...

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“…Traditionally, the structures and properties of amphiphilic molecular self-assembling systems have been tuned by designing the constituent molecules. 16,17 Yet, cohesive interactions between the constituent amphiphilic molecules, their dispersibility (stabilization of the interface between amphiphilic self-assemblies and solvents) and the interactions among solvent molecules all contribute to self-assembly. For example, bilayer membranes are formed not only in water but also in organic solvents including protic and aprotic organic solvents.…”

Section: Introductionmentioning

confidence: 99%

Controlled self-assembly of amphiphiles in ionic liquids and the formation of ionogels by molecular tuning of cohesive energies

Nakashima

Kimizuka

2012

Polym J

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In this paper, the self-assembling characteristics of a series of L-glutamate-based ammonium amphiphiles are studied in ionic liquids (ILs). These cationic amphiphiles are dispersible in imidazolium ILs with bis((trifluoromethyl)sulfonyl)amide (TFSA) anion. Amphiphiles-containing didodecyl ester or short dioctyl amide groups were molecularly dispersed in conventional 1-butyl-3-methylimidazolium TFSA, whereas they formed bilayer membranes when they were dispersed in polar, ether linkageintroduced IL. Thus, the modification of ILs exerts a crucial influence on amphiphilic self-assembly. Enhancement of the intermolecular interactions of L-glutamate amphiphiles is achieved by introducing multiple amide bonds and longer alkyl chains, which leads to better self-assembling properties. These amide-enriched amphiphiles form fibrous bilayer assemblies even in conventional ILs with low cohesive energy densities. These observations confirm that the formation of bilayer membranes in ILs is a general phenomenon when the solute molecules have the appropriate 'ionophilic/ionophobic' nature.

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Challenges and breakthroughs in recent research on self-assembly

Cited by 729 publications

References 1,021 publications

Lyotropic liquid crystal directed synthesis of nanostructured materials

Lyotropic liquid crystal directed synthesis of nanostructured materials

Protein-like proton exchange in a synthetic host cavity

Controlled self-assembly of amphiphiles in ionic liquids and the formation of ionogels by molecular tuning of cohesive energies

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