Corresponding authorsM. Szekeres (szekeres@chem.u-szeged.hu) and E. Tombácz (tombacz@chem.u-szeged.hu)
Graphical abstract AbstractMagnetite nanoparticles (MNPs) with biocompatible coatings are good candidates for MRI (magnetic resonance imaging) contrasting, magnetic hyperthermia treatments and drug delivery systems. The spontaneous surface induced polymerization of dissolved organic matter on environmental mineral particles inspired us to prepare carboxylated core-shell MNPs by using a ubiquitous polyphenolic precursor. Through the adsorption and in-situ surface polymerization of gallic acid (GA), a polygallate (PGA) coating is formed on the nanoparticles (PGA@MNP) with possible antioxidant capacity. The
Polygallate on magnetite nanoparticles Humic matter on clays 2This is a PDF file of an unedited manuscript that has been accepted for publication. Final edited form is published in Langmuir, 2014, 30:15451−15461. http://dx.doi.org/10.1021/la5038102 present work explores the mechanism of polymerization with the help of potentiometric acid-base titration, dynamic light scattering (for particle size and zeta potential determination), UV-Vis (UVvisible light spectroscopy), FTIR-ATR (Fourier-transformed infrared spectroscopy by attenuated total reflection) and XPS (X-ray photoelectron spectroscopy) techniques. We observed the formation of ester and ether linkages between gallate monomers both in solution and in the adsorbed state. Higher polymers were formed in the course of several weeks both on the surface of nanoparticles and in the dispersion medium. The ratio of the absorbances of PGA supernatants at 400 and 600 nm (i.e., the E4/E6 ratio commonly used to characterize the degree of polymerization of humic materials) was determined to be 4.3, similar to that of humic acids. Combined XPS, dynamic light scattering and FTIR-ATR results revealed that prior to polymerization, the GA monomers became oxidized to polycarboxylic acids due to ring opening while Fe 3+ ions reduced to Fe 2+ . Our published results on the colloidal and chemical stability of PGA@MNPs are referenced thoroughly in the present work. Detailed studies on biocompatibility, antioxidant property and biomedical applicability of the particles will be published.
Titanium oxide particles of various morphologies have been prepared for applications of scientific or industrial interest in recent decades. Besides development of novel synthetic routes and solid-state characterization of the obtained particles, colloidal stability of titanium oxide dispersions was the focus of numerous research groups due to the high importance of this topic in applications in heterogeneous systems. The influence of dissolved ionic compounds, including monovalent salts, multivalent ions and polyelectrolytes, on the charging and aggregation behaviour of titanium oxide materials of spherical and elongated structures will be discussed in the present review.
Charging and aggregation processes of titania nanosheets (TNS) were extensively studied in the presence of oppositely charged or like-charged polyelectrolytes in aqueous dispersions. The surface charge of the TNS was systematically varied by the pH; therefore, positive nanosheets were obtained at pH 4 and negative ones at pH 10. Strong adsorption of poly(styrene sulfonate) (PSS) of high negative line charge density on the TNS was observed at pH 4, leading to charge neutralization and reversal of the original sign of charge of the nanosheets. The adsorption of like-charged poly(diallyldimethylammonium chloride) (PDADMAC) was also feasible through a hydrophobic interaction. The predominating interparticle forces were mainly of the DLVO-type, but additional patch−charge attraction also took place in the case of PSS at low surface coverage. The TNS was found to be hydrophilic at pH 10 and no adsorption of like-charged PSS was possible because of strong electrostatic repulsion between the polyelectrolyte and the surface. The PDADMAC showed high affinity to the oppositely charged TNS surface in alkaline dispersions, giving rise to neutral and positively charged nanosheets at appropriate polyelectrolyte doses. Formation of a saturated PDADMAC layer on the TNS led to high resistance against salt-induced aggregation through the electrosteric stabilization mechanism. These results shed light on the importance of polyelectrolyte concentration, ionic strength, and charge balance on the colloidal stability of TNS, which is especially important in applications, where the nanosheets are dispersed in complex solution containing polymeric compounds and electrolytes.
Nanocomposites of titania nanosheets (TNS), h o r s e r a d i s h p e r o x i d a s e ( H R P ) , a n d p o l y -(diallyldimethylammonium chloride) (PDADMAC) were prepared, and their colloidal and functional stabilities were assessed. HRP quantitatively adsorbed on bare TNS, and the adsorption process did not affect the charging and aggregation behavior of the colloidal system. The obtained TNS−HRP composite was functionalized by PDADMAC to stabilize the enzyme on the surface and to maintain good colloidal stability. Depending on the PDADMAC dose applied, its adsorption on TNS−HRP led to charge reversal of the particles from negative to positive. The formation of a saturated polyelectrolyte layer on the TNS−HRP (TNS−HRP−PDADMAC) gave rise to highly stable colloids, and especially the resistance against saltinduced aggregation was excellent. The enzymatic activity of different systems was investigated as a function of the pH of the medium and over time. The results indicated that HRP remained enzymatically active upon immobilization, and in addition, the pH range of application broadened compared to its native form. The developed TNS−HRP−PDADMAC system can thus be used in a wider pH range and possesses the advantages of a heterogeneous catalyst compared to the bare enzyme.
Critical coagulation concentration (CCC) is a key parameter of particle dispersions, since it provides the threshold limit of electrolyte concentrations, above which the dispersions are destabilized due to rapid particle aggregation. A computational method is proposed to predict CCC values using solely electrophoretic mobility data without the need to measure aggregation rates of the particles. The model relies on the DLVO theory; contributions from repulsive double-layer forces and attractive van der Waals forces are included. Comparison between the calculated and previously reported experimental CCC data for the same particles shows that the method performs well in the presence of mono and multivalent electrolytes provided DLVO interparticle forces are dominant. The method is validated for particles of various compositions, shapes, and sizes.
The preparation of an antioxidant hybrid material by controlled heteroaggregation of manganese oxide nanoparticles (MnO2 NPs) and sulfate-functionalized polystyrene latex (SL) beads was accomplished. Negatively charged MnO2 NPs were prepared...
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