The synthesis of carbohydrate-functionalized thermosensitive poly(Nisopropylacrylamide) microgels and their ability to bind carbohydrate-binding pathogens upon temperature switch are reported. It is found that the microgels' binding affinity is increased above their lower critical solution temperature (LCST), enabling thermotriggerable capture of pathogens. Here, a series of microgels with comparatively low mannose functionalization degrees below 1 mol % is achieved by a single polymerization step. Upon increase in mannose density, the microgel size increases, and the LCST decreases to 26 °C. Clustering with concanavalin A indicated that binding affinity is enhanced by a higher mannose content and by raising the temperature above the LCST. Binding studies with Escherichia coli confirm stronger specific interactions above the LCST and formation of mechanically stable aggregates enabling efficient separation of E. coli by filtration. For small incubation times above the LCST, the microgels' potential to release pathogens again below the LCST is confirmed also. Compared to existing switchable scaffolds, microgels nearly entirely composed of a thermosensitive material undergo a large change in volume, which allows them to drastically vary the density of ligands to switch between capture and release. This straightforward yet novel approach is likely compatible with a broad range of bioactive ligands. Therefore, thermosensitive microgels represent a promising platform for the specific capture or release of cells or pathogens.
Thermoresponsive microgels undergo a volume phase transition from a swollen state under good solvent conditions to a collapsed state under poor solvent conditions. The most prominent examples of such responsive...
Probing the rotational and translational diffusion and colloidal stability of nanorods is of significant fundamental interest with implications for many different applications. Recently R. Nixon-Luke and G. Bryant presented a...
Over
the last decade,
the interest in carbon dots, graphene dots,
or similar carbon-based nanoparticles has increased considerably.
This interest is based on potentially high fluorescent quantum yields,
controllable excitation-dependent emission, low toxicity, and convenient
reaction conditions. Carbon dots are often seen as a promising alternative
to classical semiconductor quantum dots that are typically made from
toxic semiconductor materials. Surprisingly, aspects like the atomic
structure, composition, mechanism of formation, and precise understanding
of the photophysical properties of carbon dots are still mostly unknown.
The large number of different precursor systems and the variety in
synthesis routes make a direct comparison of different systems difficult.
To advance this, we went for a systematic approach and compared the
results of four synthesis routes using two different precursor systems.
We used different spectroscopy and microscopy methods including fluorescence
correlation spectroscopy to characterize the different reaction products.
We found that for syntheses solely based on citric acid as the precursor,
we obtain particles where the emission wavelength is strongly dependent
on the excitation wavelength despite relatively low quantum yields.
In comparison, when urea is added as a nitrogen doping reactant, we
observe vastly increased quantum yields. By making use of a combination
of dialysis and column chromatography, we were able to isolate various
luminescent species with high quantum yields and verify the existence
of different molecular fluorophores. A detailed and consistent characterization
of the reaction products during the course of purification revealed
strong interactions between molecular fluorophores and larger reaction
products.
To explore dense packings of soft colloids, scattering experiments are ideal to access the structure factor. However, for soft microgels determination of the structure factor is difficult because of the low contrast of the polymer network and potential microgel interpenetration and deformation that change the form factor contribution. Here, we employ small-angle X-ray scattering (SAXS) to study soft, thermoresponsive microgels with poly-N-isopropylacrylamide (PNIPAM) shells and gold nanoparticle cores. The scattering of the gold cores dominates the scattering patterns and allows precise determination of the microgel volume fraction over a broad range of concentrations. At high volume fractions we find distinct patterns with sharp Bragg peaks allowing extraction of the structure factor and characterization of the phases combined with UV-Vis spectroscopy. The unique scattering contrast of our core-shell microgels combined with SAXS opens up new ways to investigate dense packings of soft microgels including in situ studies of phase transitions.
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