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    Kinetic and spectroscopic responses of pH-sensitive nanoparticles: Influence of the silica matrix
    (London : Royal Society of Chemistry, 2019) Clasen, A.; Wenderoth, S.; Tavernaro, I.; Fleddermann, J.; Kraegeloh, A.; Jung, G.
    Intracellular pH sensing with fluorescent nanoparticles is an emerging topic as pH plays several roles in physiology and pathologic processes. Here, nanoparticle-sized pH sensors (diameter far below 50 nm) for fluorescence imaging have been described. Consequently, a fluorescent derivative of pH-sensitive hydroxypyrene with pKa = 6.1 was synthesized and subsequently embedded in core and core-shell silica nanoparticles via a modified Stöber process. The detailed fluorescence spectroscopic characterization of the produced nanoparticles was carried out for retrieving information about the environment within the nanoparticle core. Several steady-state and time-resolved fluorescence spectroscopic methods hint to the screening of the probe molecule from the solvent, but it sustained interactions with hydrogen bonds similar to that of water. The incorporation of the indicator dye in the water-rich silica matrix neither changes the acidity constant nor dramatically slows down the protonation kinetics. However, cladding by another SiO2 shell leads to the partial substitution of water and decelerating the response of the probe molecule toward pH. The sensor is capable of monitoring pH changes in a physiological range by using ratiometric fluorescence excitation with λex = 405 nm and λex = 488 nm, as confirmed by the confocal fluorescence imaging of intracellular nanoparticle uptake.
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    Stabilizing silica nanoparticles in hydrogels: impact on storage and polydispersity
    (London : RSC Publishing, 2017) Giovannini, Giorgia; Kunc, Filip; Piras, Carmen C.; Stranik, Ondrej; Edwards, Alison A.; Hall, Andrew J.; Gubala, Vladimir
    For successful nanomedicine, it is important that the unique, size-dependent physico-chemical properties of the nanomaterial remain predictably constant during both the storage and the manipulation of the material. Here a novel approach to preserve the colloidal stability and degradation of NPs is described. The concept is simple: (a) a solution of monodisperse particles is formulated into a responsive water- or PBS-based hydrogel; (b) the gel can be reversibly turned into a solution after long term storage by shaking it by hand; (c) the NP can be diluted and used in any desired application without the need for excessive manipulation. The differences between the physico-chemical properties of NPs stored in solution and in gel are compared. Two types of NPs were involved in this study: silica NPs of ∼100 nm and Au-NPs of 30 and 80 nm in diameter. The key findings are: the fibrous matrix of the hydrogel limits the NP mobility, significantly reduces NP aggregation and conserves the NP morphology; both the hydrogelator and the NPs show negligible toxicity towards the model U937 human hematopoietic cell line; undesired leaching of cargo material loaded inside the particles is reduced, which could be an important feature for drug delivery systems.