Correction for 'Elucidating the role of multivalency, shape, size and functional group density on antibacterial activity of diversified supramolecular nanostructures enabled by templated assembly' by Amrita Sikder , , 2023, , 171-178, https://doi.org/10.1039/D2MH01117D.
View Article and Find Full Text PDFAs agriculture strives to feed an ever-increasing number of people, it must also adapt to increasing exposure to minute plastic particles. To learn about the accumulation of nanoplastics by plants, we prepared well-defined block copolymer nanoparticles by aqueous dispersion polymerisation. A fluorophore was incorporated via hydrazone formation and uptake into roots and protoplasts of Arabidopsis thaliana was investigated using confocal microscopy.
View Article and Find Full Text PDFWith the increased prevalence of antibiotic-resistant infections, there is an urgent need to develop novel antibacterial materials. In addition, gaining a complete understanding of the structural features that impart activity toward target microorganisms is essential to enable materials optimisation. Here we have reported a rational design to fabricate antibacterial supramolecular nanoparticles with variable shape, size and cationic group density, by exploiting noncovalent interactions between a shape determining template amphiphile and a cationic amphiphile to introduce charge on the nanoparticle surface.
View Article and Find Full Text PDFThe design and fabrication of synthetic self-assembled systems that can mimic some biological features require exquisitely sophisticated components that make use of supramolecular interactions to attain enhanced structural and functional complexity. In nature, nucleobase interactions play a key role in biological functions in living organisms, including transcription and translation processes. Inspired by nature, scientists are progressively exploring nucleobase synthons to create a diverse range of functional systems with a plethora of nanostructures by virtue of molecular-recognition-directed assembly and flexible programmability of the base-pairing interactions.
View Article and Find Full Text PDFSelf-assembled supramolecular architectures are ubiquitous in nature. A synchronized combination of dynamic noncovalent interactions is the major driving force in forming unique structures with high-precision control over the self-assembly of supramolecular materials. Herein, we have achieved programmable nanostructures by introducing single/multiple H-bonding units in a supramolecular building block.
View Article and Find Full Text PDFBioinspired self-assembly has been explored with diverse synthetic scaffolds, among which amphiphiles are perhaps the most extensively studied systems. Classical surfactants or amphiphilic block copolymers, depending on the hydrophobic-hydrophilic balance, produce distinct nanostructures, which hold promise for applications ranging from biology to materials sciences. Nevertheless, their immiscibility-driven aggregation does not provide the opportunity to precisely regulate the internal order, morphology, or functional group display, which is highly desirable, especially in the context of biological applications.
View Article and Find Full Text PDFThis article reports the antimicrobial activity of two segmented amphiphilic polyurethanes, PU-1 and PU-2, containing a primary or secondary amine group, respectively. In acidic water, intrachain H-bonding among the urethanes followed by hierarchical assembly resulted in the formation of capsules ( = 120 ± 20 and 100 ± 17 nm for PU-1 and PU-2, respectively) with a highly positive surface charge. They showed selective interactions with bacterial cell mimicking liposomes over mammalian cell mimicking liposomes with favorable enthalpy and entropy contributions, which was attributed to the electrostatic interaction and hydrophobic effect.
View Article and Find Full Text PDFThis article elucidates H-bonding-regulated directional supramolecular assembly of naphthalene diimide (NDI)-derived unsymmetric cationic bola-shaped π-amphiphiles and systematic investigations on the thermodynamics of their interaction with bacteria mimic lipid vesicles and antimicrobial activity with mechanistic insights. Four NDI-amphiphiles (NDI-1, NDI-2, NDI-3, and NDI-2a) have been studied, all of which contain a central NDI chromophore, a nonionic wedge, an amine containing a head group, and a hydrazide group. In NDI-2 and NDI-2a, the hydrophilic wedge and the head group (pyridine) are the same but the location of the hydrazide group is different.
View Article and Find Full Text PDFProgrammable assembly of biomolecules is a fast growing research area that aims to emulate nature's elegance in creating numerous hierarchical self-assembled structures, which are responsible for unimaginably difficult biological functions. Protein assembly is a particularly challenging task, owing to their structural diversity, conformational heterogeneity, and high molecular weight. This article reveals the ability of a supramolecular structure-directing unit (SSDU) to regulate the entropically favourable supramolecular assembly of a covalently conjugated protein (bovine serum albumin (BSA)) to produce well-defined protein-decorated micelles with remarkably high thermal stability, suppression of the thermal denaturation of the protein, and retention of enzymatic activity.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
February 2019
Herein we describe the H-bonding-regulated nanostructure, thermodynamics, and multivalent binding of two bolaamphiphiles NDI-1 and NDI-2 consisting of a hydrophobic naphthalene diimide connected to a hydrophilic wedge by a H-bonding group and a glucose moiety on its two arms. NDI-1 and NDI-2 differ by the single H-bonding group, namely, hydrazide or amide, which triggers the formation of vesicles and cylindrical micelles, respectively. Although the extended H-bonding ensures stacking with head-to-head orientation and the formation of an array of the appended glucose moieties in both systems, the adaptive cylindrical structure exhibited superior multivalent binding with concanavalin A (ConA) to that of the vesicle.
View Article and Find Full Text PDFThis manuscript reports solvent tunable functional nano-assemblies of an unsymmetrical bola-shaped π-amphiphile (NDI-PY) which consists of a hydrophobic naphthalene-diimide (NDI) chromophore connected to a non-ionic hydrophilic wedge and a pyridine group at its two opposite arms. Importantly, it contains a hydrazide group located at the hydrophobic domain between the NDI-chromophore and the hydrophilic-wedge to drive the supramolecular assembly by directional H-bonding. NDI-PY exhibits spontaneous assembly in water as well as in a highly non-polar solvent like tetra-chloroethylene (TCE) by the synergistic effect of H-bonding and π-stacking interaction.
View Article and Find Full Text PDFThe article describes the self-assembly of a series of unsymmetrical bola-shaped π-amphiphiles (NDI-1, NDI-1a, NDI-2, NDI-3, and NDI-4) consisting of a hydrophobic naphthalene-diimide (NDI) chromophore attached to a nonionic hydrophilic wedge and an anionic headgroup in the two opposite arms of the central NDI. By design, only a single hydrazide group is linked either on the ionic or nonionic arm of the NDI. NDI-1 and NDI-1a are regioisomers differing only in the location of the hydrazide group, placed in the nonionic or ionic arm, respectively.
View Article and Find Full Text PDFThe presence of a bulky peripheral wedge destabilizes the homo-assembly of an amide functionalized acceptor (A) monomer and thereby enables the formation of an alternating supramolecular copolymer with an amide appended donor (D) monomer the synergistic effect of H-bonding and the charge-transfer (CT) interaction with a remarkably high of 31 000 M. In sharp contrast, H-bonding driven homo-polymers of A and D are formed by just replacing the bulky chains of the A monomer with linear hydrocarbons. By taking advantage of the clear difference in the critical temperature for the onset of the AA or DD homo-assemblies and DA co-assembly ( ≫ or ), the supramolecular polymerization pathway of the NDI-monomer could be fully diverted from isodesmic to cooperative in the presence of a small amount of DAN which helped the production of nucleating sites involving the D-A CT-complex at a relatively higher temperature and the subsequent chain growth at following the nucleation-elongation model.
View Article and Find Full Text PDFAn adaptable and efficient molecular recognition pair has been established by taking advantage of the complementary nature of donor-acceptor interactions together with the strength of hydrogen bonds. Such distinct molecular recognition propagates in orthogonal directions to effect extended alternating co-assembly of two different appended molecular entities. The dimensions of the assembled structures can be tuned by stoichiometric imbalance between the donor and acceptor building blocks.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
June 2015
A unique supramolecular strategy enables the unidirectional assembly of two bola-shaped unsymmetric π-amphiphiles, NDI-1 and NDI-2, which feature a naphthalene-diimide chromophore connected to nonionic and anionic head groups on opposite arms. The amphiphiles differ only in the location of a hydrazide group, which is placed either on the nonionic or on the anionic arm of NDI-1 and NDI-2, respectively. The formation of hydrogen bonds between the hydrazides, which compensates for electrostatic and steric factors, promotes unidirectional alignment and the formation of monolayer vesicles.
View Article and Find Full Text PDFRoom temperature photolysis of a triply-bridged borylene complex, [(μ(3)-BH)(Cp*RuCO)(2)(μ-CO)Fe(CO)(3)] (1 a; Cp* = C(5)Me(5)), in the presence of a series of alkynes, 1,2-diphenylethyne, 1-phenyl-1-propyne, and 2-butyne led to the isolation of unprecedented vinyl-borylene complexes (Z)-[(Cp*RuCO)(2)(μ-CO)B(CR)(CHR')] (2: R, R' = Ph; 3: R = Me, R' = Ph; 4: R, R' = Me). This reaction permits a hydroboration of alkyne through an anti-Markovnikov addition. In stark contrast, in the presence of phenylacetylene, a metallacarborane, closo-[1,2-(Cp*Ru)(2)(μ-CO)(2){Fe(2)(CO)(5)}-4-Ph-4,5-C(2)BH(2)] (5 a), is formed.
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