Claudio Toncelli

Steering surface topographies of electrospun fibers: understanding the mechanisms

A profound understanding of how to tailor surface topographies of electrospun fibers is of great importance for surface sensitive applications including optical sensing, catalysis, drug delivery and tissue engineering. Hereby, a novel approach to comprehend the driving forces for fiber surface topography formation is introduced through inclusion of the dynamic solvent-polymer interaction during fiber formation. Thus, the interplay between polymer solubility as well as computed fiber jet surface temperature changes in function of time during solvent evaporation and the resultant phase separation behavior are studied. The correlation of experimental and theoretical results shows that the temperature difference between the polymer solution jet surface temperature and the dew point of the controlled electrospinning environment are the main influencing factors with respect to water condensation and thus phase separation leading to the final fiber surface topography. As polymer matrices with enhanced surface area are particularly appealing for sensing applications, we further functionalized our nanoporous fibrous membranes with a phosphorescent oxygen-sensitive dye. The hybrid membranes possess high brightness, stability in aqueous medium, linear response to oxygen and hence represent a promising scaffold for cell growth, contactless monitoring of oxygen and live fluorescence imaging in 3-D cell models.

2,2′:6′,2′′-Terpyridine-functionalized redox-responsive hydrogels as a platform for multi responsive amphiphilic polymer membranes

Nanophase-separated amphiphilic polymer co-networks are ideally suited as responsive membranes due to their stable co-continuous structure. Their functionalization with redox-responsive 2,2′:6′,2′′-terpyridine–metal complexes and light-responsive spiropyran derivatives leads to a novel material with tunable optical, redox and permeability properties. The versatility of the system in complexing various metal ions, such as cobalt or iron at different concentrations, results in a perfect monitoring over the degree of crosslinking of the hydrophilic poly(2-hydroxyethyl acrylate) channels. The reversibility of the complexation, the redox state of the metal and the isomerization to the merocyanine form upon UV illumination was evidenced by cyclic voltammetry, UV-Vis and permeability measurements under sequential conditions. Thus, the membrane provides light and redox addressable functionalities due to its adjustable and mechanically stable hydrogel network.

Nanoparticle‐Based Fluoroionophore for Analysis of Potassium Ion Dynamics in 3D Tissue Models and In Vivo

The imaging of real-time fluxes of K+ ions in live cell with high dynamic range (5-150 mM) is of paramount importance for neuroscience and physiology of the gastrointestinal tract, kidney and other tissues. In particular, the research on high-performance deep-red fluorescent nanoparticle-based biosensors is highly anticipated. We found that BODIPY-based FI3 K+-sensitive fluoroionophore encapsulated in cationic polymer RL100 nanoparticles displays unusually strong efficiency in staining of broad spectrum of cell models, such as primary neurons and intestinal organoids. Using comparison of brightness, photostability and fluorescence lifetime imaging microscopy (FLIM) we confirmed that FI3 nanoparticles display distinctively superior intracellular staining compared to the free dye. We evaluated FI3 nanoparticles in real-time live cell imaging and found that it is highly useful for monitoring intra- and extracellular K+ dynamics in cultured neurons. Proof-of-concept in vivo brain imaging confirmed applicability of the biosensor for visualization of epileptic seizures. Collectively, this data makes fluoroionophore FI3 a versatile cross-platform fluorescent biosensor, broadly compatible with diverse experimental models and that crown ether-based polymer nanoparticles can provide a new venue for design of efficient fluorescent probes.