Particle aggregation | EPFL Graph Search

Particle agglomeration refers to the formation of assemblages in a suspension and represents a mechanism leading to the functional destabilization of colloidal systems. During this process, particles dispersed in the liquid phase stick to each other, and spontaneously form irregular particle assemblages, flocs, or agglomerates. This phenomenon is also referred to as coagulation or flocculation and such a suspension is also called unstable. Particle agglomeration can be induced by adding salts or other chemicals referred to as coagulant or flocculant. Particle agglomeration can be a reversible or irreversible process. Particle agglomerates defined as "hard agglomerates" are more difficult to redisperse to the initial single particles. In the course of agglomeration, the agglomerates will grow in size, and as a consequence they may settle to the bottom of the container, which is referred to as sedimentation. Alternatively, a colloidal gel may form in concentrated suspensions which cha

Electrophoretic deposition of multi-scale structured TiO2 surfaces

The long term fixation of biomedical implants constitutes an issue in the clinical praxis. Implant fixation can be improved by functionalizing its surface. In fact, the tissue response around an implant is conditioned by its surface morphological and chemical properties. Coatings for implants (orthopedic and dental) function at the bone-implant fixation interface. As proved by research activities in the biomedical field, coatings with topographic features in the nano- and micro-range are promising in terms of enhanced osteointegration, thus improved implant fixation. As for surface chemistry, titanium dioxide (TiO2) is an estabilished material for biomedical implants thanks to its outstanding physical and chemical properties such as high corrosion resistance and good biocompatibility. Electrophoretic deposition (EPD) is a simple and versatile coating technique. According to literature, EPD is an emerging potential coating technique for biomedical implants. In this work, the use of EPD in the preparation of TiO2 coatings characterized by a controlled multi-scale structured surface was addressed. For this aim, EPD was combined with a new procedure of particle functionalization and with the use of a fugitive spacer (polystyrene, PS) for the sintering treatment. A control and better understanding of the EPD process were achieved through a preliminary parametric study on EPD of TiO2 nanoparticles and PS microbeads. Particle concentration was found to play a key role in the EPD deposit formation of TiO2 nanoparticles (cathodic) and PS microbeads (anodic). A threshold value of particle concentration was identified, below which no deposit growth occurred. An interpretation of this finding was provided on the base of a new formulation of the EPD deposition mechanism. The results of the particle concentration study contributed to the preparation of suspensions with TiO2-PS composite particles, which could be used for cathodic EPD. Composite TiO2-PS particles with TiO2 nanoparticles covering PS microbeads were obtained in a newly developed wet colloidal process based on heterocoagulation and the use of polyelectrolytes. The resulting TiO2-PS particles were cathodically deposited on Ti6Al4V substrates. A sintering post-treatment caused the burning out of the PS beads and the densification of the TiO2 nanoparticles. The desired coatings with controlled micro- and nano-topography were achieved. The investigation on the role of particle concentration in EPD and the new interpretation of the deposition mechanism bring a deeper understanding of the EPD process. The achievement of TiO2 coatings with controlled morphology in the micro- and nano-range prepared by cathodic EPD on Ti6Al4V substrates is a contribution to the ongoing research on biomedical implants. Mechanical tests and surface analysis evaluating wettability and in vitro cell behavior with the achieved coatings are relevant topics for further research.

EPFL2009

Novel Chemosensors for Biologically Important Analytes

Ziya Köstereli

In this work, fluorescent-based chemosensors for the detection of important analytes in aqueous solution are described. The sensors are based on different detection concepts, including analyte-induced aggregation/de-aggregation, pattern-based sensing and micelle-based sensing. In chapter 2, we present an analyte-induced aggregation-type chemosensor for the sensing of spermine. A charge-frustrated amphiphile composed of a highly fluorescent pyrene-1,3,6-trisulfonate head group and an eicosane side chain was used as a fluorescence chemosensor. Analyte-induced aggregation of the dye upon addition of spermine results in pronounced fluorescence quenching. The sensor enables the detection of spermine down to the nanomolar concentration range with good selectivity over closely related biogenic amines such as spermidine. In chapter 3, we describe a conceptually new âone-cuvetteâ sensing system for the pattern-based analysis of seven aminoglycosides antibiotics. The antibiotics include amikacin, apramycin, gentamicin, kanamycin A and B, neomycin, and paromomycin. A mixture of two amphiphiles with fluorescent head groups was used as a sensing ensemble. In buffered aqueous solution, the amphiphiles form a dynamic mixture of micellar aggregates. In the presence of aminoglycosides, the relative amount and the composition of the micelles is modified. Accurate differentiation in the low micromolar concentration range is achieved by a principal component analysis of the spectral data. Also, the sensing system allows the differentiation of pure aminoglycosides from their mixtures. In chapter 4, a fluorescent chemosensor based on analyte-induced aggregation/de-aggregation is described for the sensing of Al3+ and citric acid. In buffered aqueous solution, the amphiphilic dye can form aggregates and the aggregation of the dye is associated with a strong quenching of its fluorescence. The Al3+-induced aggregation is used to sense Al3+ in the low micromolar concentration range with high selectivity. Furthermore, we demonstrate that the non-fluorescent dye-Al3+ complex can be used as a sensing ensemble for the detection of citric acid. The assay is able to quantify the citric acid content of commercial beverages such as energy drinks. A simple micelle-based assay for the fluorescence sensing of vitamin K1 is described. In the following chapter 5, the assay enables the detection of vitamin K1 in the low micromolar concentration range. As a sensing ensemble, a mixture of the surfactant triton X-100 and 1 aminopyrene in buffered aqueous solution is employed. Vitamin K1 co-localizes with the fluorescent pyrene dye in the micelle, resulting in fluorescence attenuation by dynamic quenching. The assay displays good selectivity and can be used to determine the concentration of vitamin K1 in a commercial preparation. In chapter 6, a fluorescent-based sensor array for the optical analysis of purine derivatives is described. The array is composed of four polysufonated fluorescent dyes. The complexation of the analytes results in partial quenching of the fluorescence. The Sensor array enables the identification of ten purine derivatives including caffeine, theophylline, theobromine, purine, hypoxanthine, paraxanthine, 8-chlorotheophylline, 6-mercaptopurine, cladribine and penciclovir at low millimolar concentration. Furthermore, it is possible to use the array for obtaining information about the quantity and the purity of samples.

EPFL2015

In-situ observations of aerosol-cloud interactions in Ny-Ålesund, Svalbard, during fall 2019 and spring 2020

Paraskevi Georgakaki, Ghislain Gilles Jean-Michel Motos, Athanasios Nenes, Jörg Wieder

The Arctic region suffers an extreme vulnerability to climate change, with an increase in surface air temperatures that have reached twice the global rate during several decades (McBean et al., 2005). The role of clouds, and in particular low-levels clouds and fog, in this arctic amplification by regulating the energy transport from and to space has recently gained interest among the scientific community. The NASCENT 2019-2020 campaign (Ny-Ålesund AeroSol Cloud ExperimeNT) based in Ny-Ålesund, Svalbard (79º North) aimed at studying the microphysical and chemical properties of low-level clouds using measurements both at the sea level and at the Zeppelin station (475 m a.s.l.). Specifically, the susceptibility of droplet formation, which has recently been shown to be highly dependent on aerosol levels in European alpine valleys (Georgakaki et al., under review), could strongly vary between the fall to winter months, with pristine-like conditions, and the higher particle concentrations generally found in spring, known as the arctic haze. First results using a scanning mobility particle sizer (SMPS) and a cloud condensation nuclei counter (CCNC) confirmed that aerosol concentrations in the range 10 < Dpart [nm] < 500 were approximatively 4-5 times higher during the months of spring 2021 compared to those of fall 2020. In addition, we found relatively low values of the aerosol hygroscopic parameter κ, generally below 0.3, consistently with previous studies in the arctic region (Moore et al., 2011). Georgakaki, P., Bougiatioti, A., Wieder, J., Mignani, C., Kanji, Z. A., Henneberger, J., Hervo, M., Berne, A. and Nenes, A.: On the drivers of droplet variability in Alpine mixed-phase clouds, , 34, under review. McBean, G., Alekseev, G., Chen, D., Førland, E., Fyfe, Groisman, J., P. Y., King, R., Melling, H., Voseand, R., Whitfield, P. H.: Arctic climate: past and present. Arctic Climate Impacts Assessment (ACIA), C. Symon, L. Arris and B. Heal, Eds., Cambridge University Press, Cambridge, 21-60, 2005. Moore, R. H., Bahreini, R., Brock, C. A., Froyd, K. D., Cozic, J., Holloway, J. S., Middlebrook, A. M., Murphy, D. M. and Nenes, A.: Hygroscopicity and composition of Alaskan Arctic CCN during April 2008, Atmospheric Chemistry and Physics, 11(22), 11807–11825, https://doi.org/10.5194/acp-11-11807-2011, 2011.

2021