Abstract. Mineral aerosol particles nucleate ice, and many insights have been obtained
on water freezing as a function of mineral surface properties such as charge
or morphology. Previous studies have mainly focused on pristine samples
despite the fact that aerosol particles age under natural atmospheric
conditions. For example, an aerosol-containing cloud droplet can go through
freeze–melt or evaporation–condensation cycles that change the surface
structure, the ionic strength, and pH. Variations in the surface properties
of ice-nucleating particles in the atmosphere have been largely overlooked.
Here, we use an environmental cell in conjunction with nonlinear
spectroscopy (second-harmonic generation) to study the effect of freeze–melt
processes on the aqueous chemistry at silica surfaces at low pH. We found
that successive freeze–melt cycles disrupt the dissolution equilibrium,
substantially changing the surface properties and giving rise to marked
variations in the interfacial water structure and the ice nucleation ability
of the surface. The degree of order of water molecules, next to the surface,
at any temperature during cooling decreases and then increases again with
sample aging. Along the aging process, the water ordering–cooling
dependence and ice nucleation ability improve continuously.
Abstract. This research specifi cally focused on the development of a novel methodology to reduce excess nitrate in drinking water utilizing zerovalent iron nanoparticles (nZVI)-stabilized radiation-grafted copolymer matrix. nZVI was synthesized by borohydrate reduction of FeCl 3 and stabilized on acrylic acid (AAc)-grafted non-woven polyethylene/polypropylene (NWPE/PP-g-AAc) copolymer matrix, which was grafted using gamma radiation. The use of nZVI for environmental applications is challenging because of the formation of an oxide layer rapidly in the presence of oxygen. Therefore, radiation-grafted NWPE/PP synthetic fabric was used as the functional carrier to anchor nZVI and enhance its spreading and stability. The chemical reduction of nitrate by nZVI-adsorbed NWPE/PP-g-AAc (nZVI-Ads-NWP) fabric was examined in batch experiments at different pH values. At low pH values, the protective layers on nZVI particles can be readily dissolved, exposing the pure iron particles for effi cient chemical reduction of nitrate. After about 24 h, at pH 3, almost 96% of nitrate was degraded, suggesting that this reduction process is an acid-driven, surface-mediated process. The nZVI-water interface has been characterized by the 1-pK Basic Stern Model (BSM). An Eley-Rideal like mechanism well described the nitrate reduction kinetics. In accordance with green technology, the newly synthesized nZVI-Ads--NWP has great potential for improving nitrate reduction processes required for the drinking water industry.
Mobility and bioavailability of radionuclides in the environment strongly depend on their aqueous speciation, adsorption behavior and the solubility of relevant solid phases. In the present context, we focus on naturally occurring Th-232 at a location in central Sri Lanka presenting high background radiation levels. Four different soil samples were characterized using X-ray Absorption Spectroscopy (XAS) at the Th L3-edge (16.3 keV), Scanning Electron Microscopy (SEM) and Energy Dispersive X-ray (EDX) spectroscopy. X-ray Absorption Near Edge Structure (XANES) spectra are applied as a fingerprint indication for Th existing in different chemical environments. Linear combination fitting (LCF) of the Extended X-ray Absorption Fine Structure (EXAFS) data involving reference Th-monazite (phosphate) and thorianite (oxide) compounds suggested that Th is mostly present as Th-phosphate (76 ± 2%) and Th-oxide (24 ± 2%), even though minor amounts of thorite (silicate) were also detected by SEM–EDX. Further studies on selected individual particles using micro-focus X-ray Fluorescence (μ-XRF) and micro-X-ray Absorption Spectroscopy (μ-XAS) along with SEM–EDX elemental mapping provided information about the nature of Th-bearing mineral particles regarding mixed phases. This is the first study providing quantitative and XAS based speciation information on Th-mineral phases in soil samples from Sri Lanka.
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