Zhaofu Meng

Humic acid coated Fe3O4 magnetic nanoparticles as highly efficient Fenton-like catalyst for complete mineralization of sulfathiazole

Humic acid coated Fe(3)O(4) magnetic nanoparticles (Fe(3)O(4)/HA) were prepared for the removal of sulfathiazole from aqueous media. Fe(3)O(4)/HA exhibited high activity to produce hydroxyl (OH) radicals through catalytic decomposition of H(2)O(2). The degradation of sulfathiazole was strongly temperature-dependent and favored in acidic solution. The catalytic rate was increased with Fe(3)O(4)/HA dosage and H(2)O(2) concentration. When 3 g L(-1) of Fe(3)O(4)/HA and 0.39 M of H(2)O(2) were introduced to the aqueous solution, most sulfathiazole was degraded within 1h, and >90% of total organic carbon (TOC) were removed in the reaction period (6h). The major final products were identified as environmentally friendly ions or inorganic molecules (SO(4)(2-), CO(2), and N(2)). The corresponding degradation rate (k) of sulfathiazole and TOC was 0.034 and 0.0048 min(-1), respectively. However, when 3 g L(-1) of bare Fe(3)O(4) were used as catalyst, only 54% of TOC was eliminated, and SO(4)(2-) was not detected within 6h. The corresponding degradation rate for sulfathiazole and TOC was 0.01 and 0.0016 min(-1), respectively. The high catalytic ability of Fe(3)O(4)/HA may be caused by the electron transfer among the complexed Fe(II)-HA or Fe(III)-HA, leading to rapid regeneration of Fe(II) species and production of OH radicals.

Preparation of polydopamine coated Fe3O4 nanoparticles and their application for enrichment of polycyclic aromatic hydrocarbons from environmental water samples

Core/shell structured magnetic Fe3O4/polydopamine (Fe3O4/PDA) nanoparticles have been successfully synthesized and developed as a magnetic solid-phase extraction (SPE) adsorbent in dispersion mode for the determination of trace polycyclic aromatic hydrocarbons (PAHs) in environmental samples. The Fe3O4/PDA synthetic procedure is simple and involves no organic solvents. Only 20mg of Fe3O4/PDA adsorbents are required to extract PAHs from 500mL water samples. The adsorption attains equilibrium rapidly and analysts are eluted with acetonitrile readily. The extraction efficiency is not influenced by salt concentrations up to 300mM and pH values over the range 4-11. Under optimized conditions, the detection limits of PAHs are in the range of 0.5-1.9ngL(-1). The accuracy of the method is evaluated by the recoveries of PAHs from environmental samples. Good recoveries (76.4-107%) with low relative standard deviations from 1.0% to 9.7% are achieved. Comparison study shows that the recoveries of target PAHs are low when they are extracted using traditional SPE method even with the addition of methanol or tetrabutylammonium bromide surfactants in water samples, suggesting great application potential of magnetic SPE method to preconcentrate highly hydrophobic contaminants (such as PAHs) from large volume of water samples. This new SPE method provides several advantages, such as simplicity, low environmental impact, high extraction efficiency, high breakthrough volumes, convenient extraction procedure, and short analysis time.

Easy Synthesis of Surface-Tunable Carbon-Encapsulated Magnetic Nanoparticles: Adsorbents for Selective Isolation and Preconcentration of Organic Pollutants

We have prepared core/shell structured carbon-encapsulated magnetic nanoparticles (CMNPs) with a simple method by using inorganic iron salt and glucose solution as precursor substance. The synthetic procedure does not require the use of organic solvents. We have utilized X-ray photoelectron spectroscopy, infrared spectroscopy, X-ray diffraction, and Raman analysis to examine the surface properties of CMNPs prepared at different temperature. The specific surface areas, magnetization and contents of graphitized carbon on carbon shell of CMNPs increase with heat treatment temperature. The obtained CMNPs are used to adsorb or preconcentrate bisphenol A (BPA), 4-n-nonylphenol (4-NP), 4-tert-octylphenol (4-OP), diethyl phthalate (DEP), dipropyl phthalate (DPP), dibutyl phthalate (DBP) dicyclohexyl phthalate (DCHP), dioctyl phthalate (DOP), sulfonamide, tetracyclines, and quinolones antibiotics organic compounds from water samples. The adsorption of analytes is mainly based on π-π stacking interaction, hydrophobic interaction and hydrogen bonds between analytes and graphitic carbon. As a result, the adsorption or extraction behaviors of CMNPs to analytes are controlled by the content of oxygen-containing species and graphitized carbon on carbon shell of CMNPs. CMNPs prepared at 200 °C have ample oxygen-containing species (80%) on surface and favor the adsorption and extraction of quinolones antibiotics. CMNPs heated at 300-500 °C with the graphitization efficiency of carbon shell lower than 50% exhibit great preconcentration performance to BPA, 4-NP, 4-OP, DBP, DCHP, DOP, tetracyclines, and quinolones antibiotics. CMNPs prepared at 850 °C are highly graphitized (80%) and have strong adsorption affinity to all model analytes; however, they can quantitatively extract only highly polar sulfonamide antibiotics and moderately polar DEP, DPP because of hard desorption of other model analytes. We suggest that the appropriate adsorbent to certain organic contaminants can be obtained with this technique just by tuning the heat temperature without any post-treatment.

Strong adsorption of chlorotetracycline on magnetite nanoparticles.

In this work, environmentally friendly magnetite nanoparticles (Fe(3)O(4) MNPs) were used to adsorb chlorotetracycline (CTC) from aqueous media. Fe(3)O(4) MNPs exhibit ultrahigh adsorption ability to this widely used antibiotic. The adsorption behavior of CTC on Fe(3)O(4) MNPs fitted the pseudo-second-order kinetics model, and the adsorption equilibrium was achieved within 10h. The maximum Langmuir adsorption capacity of CTC on Fe(3)O(4) (476 mg g(-1)) was obtained at pH 6.5. Thermodynamic parameters calculated from the adsorption data at different temperature showed that the adsorption reaction was endothermic and spontaneous. Low concentration of NaCl and foreign divalent cations hardly affected the adsorption. Negative effect of coexisting humic acid (HA) on CTC adsorption was also observed when the concentration of HA was lower than 20 mg L(-1). But high concentration of HA (>20 mg L(-1)) increased the CTC adsorption on Fe(3)O(4) MNPs. The matrix effect of several environmental water samples on CTC adsorption was not evident. Fe(3)O(4) MNPs were regenerated by treatment with H(2)O(2) or calcination at 400°C in N(2) atmosphere after separation from water solution by an external magnet. This research provided a high efficient and reusable adsorbent to remove CTC selectively from aqueous media.

Fast defluorination and removal of norfloxacin by alginate/Fe@Fe3O4 core/shell structured nanoparticles.

Alginate-Fe(2+)/Fe(3+) polymer coated Fe(3)O(4) magnetic nanoparticles (Fe(3)O(4)@ALG/Fe MNPs) with core/shell structure are prepared and used as heterogeneous Fenton nanocatalyst to degrade norfloxacin (NOF). The Fenton-like process based on Fe(3)O(4)@ALG/Fe shows much higher efficiency on NOF degradation. Compared with Fe(3)O(4) nanoparticle-H(2)O(2) system, NOF degradation in Fe(3)O(4)@AlG/Fe-H(2)O(2) system can be conducted in a wide pH range (pH 3.5-6.5) and independent on temperature. With 0.98 mM H(2)O(2) and 0.4 g L(-1) Fe(3)O(4)@ALG/Fe, 100% of NOF and 90% of TOC is removed within 60 min, and the fluorine element in NOF molecule changes into F(-) ions within 1 min, indicating that NOF degradation in this Fenton-like reaction is performed through direct defluorination pathway. XPS analysis shows that TOC removal in reaction solution mainly results from the adsorption of NOF degradation intermediates on catalyst. Due to the paramagneticity and high saturation magnetization of Fe(3)O(4)@ALG/Fe, the used catalyst with adsorbed NOF intermediate is collected from aqueous solution by applying an external magnetic field, leading to complete removal of NOF from water samples. As being composed of inorganic materials and biopolymer, Fe(3)O(4)@ALG/Fe MNPs are robust, thermo-stable, nontoxic and environmentally friendly. These attractive features endow Fe(3)O(4)@ALG/Fe as a potent Fenton-like catalyst for fluoroquinolones degradation.