This study reports pH dependent stability of protein dispersions of five common proteins, bovine serum albumin (BSA), human serum albumin (HSA), immunoglobulin (IgG), β-lactoglobulin (β-Lg), and gelatin-B (Gel-B), all having isoelectric pH, pI ≈ 5, in room temperature ionic liquid solutions of 1-methyl-3-alkyl (hexyl/octyl) imidazolium chloride (concentration 0-0.2% w/v). Molecular hydrophobicity index, (H-index = hydrophobicity/hydrophilicity) of these molecules spanned the range 0.43-0.87. Electrophoretic characteristics, surface tension data and hydrodynamic size information revealed that IL solutions provide dispersion stability owing to specific protein-IL binding which did not alter their pI values though their surface charge was considerably screened. Change in maximum (ζ(max)) and minimum (ζ(min)) zeta potential values observed at pH ~3 (maximum protonated state) and pH ~8 (maximum deprotonated state) could be described universally as function of IL concentration, c as Δζ(x) = [1 - exp(-ac)] where Δζ(x) is either |(ζ(max) - ζ(w))|/ζ(w) or |(ζ(min) - ζ(w))|/ζ(w), and ζ(w) is the corresponding value in water. Tensiometry data showed two major stages of protein-IL interactions: (i) for c < cmc of IL, the IL molecules selectively bind with imidazolium cation through electrostatic forces forming protein-IL (complex) and (ii) for c> cmc free IL-aggregates begin to form. Similarly, we can define Δγ(x) as either |(γ(max) - γ(w))|/γ(w) at pH 3 or |(γ(min) - γ(w))|/γ(w) at pH 8. Both Δζ(x) and Δγ(x) showed linear dependence with c, Δγ(min, max) (or Δζ(min, max)) = (1 - K(γ) (or K(ζ)) H-index), where the slopes K(ζ) and K(γ) defined intermolecular interactions. Hydrodynamic radii data revealed protein stabilization, circular dichroism spectra implied retention of secondary structures, and Raman spectra confirmed a marginal increase in water structure. Results concluded that selective binding of IL molecules to protein surface in the form of bilayer screen protein surface charge, thereby, contributing to its dispersion stability.
Herein, we report a facile microwave-assisted synthesis of cadmium-free water-soluble silver indium sulfide (AgInS2 or AIS) and AgInS@ZnS (or AIS@ZnS) core-shell quantum dots (QDs) using glutathione (GSH) as stabilizer. The core and core-shell nanocrystals exhibit tunable bandgap ranging of 2.3–3.1 and 2.4–3.5 eV, mean particle size of 2.5 and 3.25 nm, quantum yield of 26% and 49%, and fluorescence lifetimes of 326 and 438 ns, respectively. The core-shell QDs exhibit color-tunable emission in the visible region (500 to 600 nm), where the tunability was achieved by varying the molar ratio of Ag:In in the precursors. In vitro evaluation of antifungal activity of these water/ buffer stable QDs against the fungal pathogen, Candida albicans demonstrated that these were not toxic to the fungal cells upto a concentration of 100 µg/ml for 16 hours of incubation. Confocal imaging and spectrofluorometric studies showed enhanced fluorescence inside the microbial cells suggesting that AIS@ZnS particles had the capability to easily penetrate the cells. The increased generation of reactive oxygen species was evaluated for the core-shell QDs (photosensitizers) by using 9, 10-anthracenediyl-bis(methylene)dimalonic acid (ABMDMA) as singlet oxygen (1O2) scavenger molecule. These QDs have the potential for use as high contrast cell imaging, photodynamic and antifungal agents.
Study of kinetics of complex coacervation occurring in aqueous 1-octyl-3-methylimidazolium chloride ionic liquid solution of low charge density polypeptide (gelatin A) and 200 base pair DNA, and thermally activated coacervate into anisotropic gel transition, is reported here. Associative interaction between DNA and gelatin A (GA) having charge ratio (DNA:GA = 16:1) and persistence length ratio (5:1) was studied at fixed DNA (0.005% (w/v)) and varying GA concentration (C(GA) = 0-0.25% (w/v)). The interaction profile was found to be strongly hierarchical and revealed three distinct binding regions: (i) Region I showed DNA-condensation (primary binding) for C(GA) < 0.10% (w/v), the DNA ζ potential decrease from -80 to -5 mV (95%) (partial charge neutralization), and a size decrease by ≈60%. (ii) Region II (0.10 < C(GA) < 0.15% (w/v)) indicated secondary binding, a 4-fold turbidity increase, a ζ potential decrease from -5 to 0 mV (complete charge neutralization), which resulted in the appearance of soluble complexes and initiation of coacervation. (iii) Region III (0.15 < C(GA) < 0.25% (w/v)) revealed growth of insoluble complexes followed by precipitation. The hydration of coacervate was found to be protein concentration specific in Raman studies. The binding profile of DNA-GA complex with IL concentration revealed optimum IL concentration (=0.05% (w/v)) was required to maximize the interactions. Small angle neutron scattering (SANS) data of coacervates gave static structure factor profiles, I(q) versus wave vector q, that were remarkably similar and invariant of protein concentration. This data could be split into two distinct regions: (i) for 0.0173 < q < 0.0353 Å(-1), I(q) ~ q(-α) with α = 1.35-1.67, and (ii) for 0.0353 < q < 0.35 Å(-1), I(q) = I(0)/(1 + q(2)ξ(2)). The correlation length found was ξ = 2 ± 0.1 nm independent of protein concentration. The viscoelastic length (≈8 nm) was found to have value close to the persistence length of the protein (≈10 nm). Rheology data indicated that the coacervate phase resided close to the gelation state of the protein. Thus, on a heating-cooling cycle (heating to 50 °C followed by cooling to 20 °C), the heterogeneous coacervate exhibited an irreversible first-order phase transition to an anisotropic ion gel. This established a coacervate-ion gel phase diagram having a well-defined UCST.
In this report, we present a novel application of gold–carbon dot nanoconjugates (Au@CDs) of an average size of around 12.6 nm as a sensor for the detection of cholesterol.
Here, we describe the synthesis of 2–3 nm, hydrophilic, blue fluorescence-emitting carbon dots (C-Dots, made using a DNA precursor) by the hydrothermal route from the gelling concentration of 2% (w/v) DNA.
Herein, we describe synthesis of copper indium gallium selenide (CIGS) nanocrystals by sol-gel method at room temperature, and the optimization of In/Ga ratio revealed best results pertained to Cu 0.19 In 0.24 Ga 0.76 Se 2.7 composition. The morphology and crystal structure of these nanocrystals were ascertained from scanning electron microscopy (SEM) and X-ray diffraction (XRD) studies. These nanocrystals were dispersed in D 2 O-H 2 O binary mixture and these samples were probed for the presence of H 2 O at ppm level (between 9 to 117 ppm) using fluorescence spectroscopy. The fluorescence intensity at the emission wavelength of 485 nm was found to increase with water content, and hence it operated as an excellent water sensor with a fast response time. It was also noted that observable color change of CIGS dispersion made in ethanol occurred, when trace amount of water was added confirming the water sensing ability of this nanomaterial in different environment. Our reproducible experimental results show that CIGS nanocrystals are promising candidate for water detection in D 2 O at ppm level at room temperature operations. Considering the importance of purity of D 2 O in nuclear reactors, these results are of remarkable importance.
Herein we report the first applications of TCNQ as a rapid and highly sensitive off-the-shelf cyanide detector. As a proof-of-concept, we have applied a kinetically selective single-electron transfer (SET) from cyanide to deep-lying LUMO orbitals of TCNQ to generate a persistently stable radical anion (TCNQ(•-)), under ambient condition. In contrast to the known cyanide sensors that operate with limited signal outputs, TCNQ(•-) offers a unique multiple signaling platform. The signal readability is facilitated through multichannel absorption in the UV-vis-NIR region and scattering-based spectroscopic methods like Raman spectroscopy and hyper Rayleigh scattering techniques. Particularly notable is the application of the intense 840 nm NIR absorption band to detect cyanide. This can be useful for avoiding background interference in the UV-vis region predominant in biological samples. We also demonstrate the fabrication of a practical electronic device with TCNQ as a detector. The device generates multiorder enhancement in current with cyanide because of the formation of the conductive TCNQ(•-).
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