RESUMEN

Water contamination resulting from coal spills is one of the largest environmental problems affecting communities in the Appalachia Region of the United States. This coal slurry contains potentially toxic substances, such as hydrocarbons, heavy metals, and coal cleaning chemicals, and its leakage into water bodies (lakes, rivers, and aquifers) can lead to adverse health effects not only for freshwater bodies and plant life but also for humans. This study focused on two major experiments. The first experiment involved the use of biochar to create a biochar-polysulfone (BC-PSf) flat-sheet multifunctional membrane to remove organic contaminants, and the other major experiment compared eco-friendly (gamma-valerolactone-GVL; Rhodiasolv® PolarClean-PC) and petroleum-derived solvents (i.e., N-methyl-pyrrolidone-NMP) in the fabrication of the biochar-polysulfone membranes. The resulting membranes were tested for their efficiency in removing both positively and negatively charged organic contaminants from the collected water at varying pH values. A comparative life cycle assessment (LCA) with accompanying uncertainty and sensitivity analyses was carried out to understand the global environmental impacts of incorporating biochar, NMP, GVL, and PC in the synthesis of PSf/NMP, BC-PSf/NMP, PSf/GVL, BC-PSf/GVL, PSf/PC, and BC-PSf/PC membranes at a set surface area of 1000 m2. The results showed that the addition of biochar to the membrane matrix increased the surface area of the membranes and improved both their adsorptive and mechanical properties. The membranes with biochar incorporated in their matrix showed a higher potential for contaminant removal than those without biochar. The environmental impacts normalized to the BC-PSf/GVL membrane showed that the addition of biochar increased global warming impacts, eutrophication, and respiratory impacts by over 100% in all the membrane configurations with biochar. The environmental impacts were highly sensitive to biochar addition (Spearman's coefficient > 0.8). The BC/PSf membrane with Rhodiasolv® PolarClean had the lowest associated global environmental impacts among all the membranes with biochar. Ultimately, this study highlighted potential tradeoffs between functional performance and global environmental impacts regarding choices for membrane fabrication.

RESUMEN

The global water crisis growth has led to a tremendous increase in membrane technology research. Membranes are favored over many other technologies for water treatment because, in principle, they require no chemical additives and can be used isothermally at low temperatures. Membranes that can reject contaminants and salts, produce adequate permeate flux values, and require minimal cleaning are highly demanded. However, most synthesized membranes on the market have associated problems, such as membrane fouling; inverse relationships between flux and solute rejection; and the high cost of synthesis, operation, and maintenance. Therefore, there is a continuied need to produce membranes with properties that make them able to sustain flux and selectivity over time. This research study focused on increasing the surface charge and hydrophilicity of polysulfone (PSf) membranes by incorporating sulfonate-functionalized poly-ether-ether-ketone (SPEEK) into PSf/N-Methyl-2-pyrrolidone (PSf/NMP) membranes. The sulfonation of the PEEK provided a net increase in negative charge on the surface of the membranes that enabled charge repulsion to take place, thus increasing the rejection of ions. In this project, the effect of the applied potential on the performance of SPEEK: PSf/NMP membranes was evaluated. The characterization of the as-synthesized membranes was carried out using the surface's structure and morphology, contact angle, and zeta potential. Furthermore, a voltage of 1.5 V was applied to the membranes in the presence of various salts (sodium chloride, calcium chloride, and potassium chloride salts) to evaluate the effects of the applied potential on solute rejection. It was found that both the permeability and the selectivity of the membranes increased when the voltage was applied. The obtained results indicate that incorporating SPEEK into PSf/NMP membranes increased the hydrophilicity of the membranes, and under the applied voltage, the incorporation allowed it to function as an electrodialysis process that is capable of removing ions from water bodies by utilizing the charge repulsion of ions.

RESUMEN

Microcystin-LR (MC-LR) is a toxin produced by cyanobacteria that can bloom in freshwater supplies. This study describes a new strategy for remediation of MC-LR that combines linearization of the toxin using microcystinase A, MlrA, enzyme with rejection of linearized byproducts using membrane filtration. The MlrA enzyme was expressed in Escherichia coli (E. coli) and purified via a His-tag with 95% purity. Additionally, composite membranes made of 95% polysulfone and 5% sulfonated polyether ether ketone (SPEEK) were fabricated and used to filter a solution containing cyclic and linearized MC-LR. Tests were also performed to measure the adsorption and desorption of MC-LR on polysulfone/SPEEK membranes. Liquid chromatography-mass spectrometry (LC-MS) was used to characterize the progress of linearization and removal of MC-LR. Results indicate that the MlrA was successful at linearizing MC-LR. Membrane filtration tests showed rejection of 97% of cyclic MC-LR and virtually all linearized MC-LR, with adsorption to the membranes being the main rejection mechanism. Adsorption/desorption tests indicated that methanol could be used to strip residual MC-LR from membranes to regenerate them. This study demonstrates a novel strategy of remediation of microcystin-tainted water, combining linearization of MC-LR to a low-toxicity byproduct along with removal by membrane filtration.

Asunto(s)

Ultrafiltración , Agua , Escherichia coli , Toxinas Marinas , Microcistinas/química

RESUMEN

Naled, an organophosphate pesticide, received considerable attention during 2016 as it was applied aerially to control the first mosquito-borne Zika virus outbreak in the continental United States. Stakeholders living in affected areas raised concerns about its environmental impacts. One factor influencing environmental impacts is the persistence of the chemical applied. The objective of this study was to evaluate the persistence of naled - and its degradation bi-product, dichlorvos - in natural waters. Initial naled concentrations were measured at ground level after full-scale aerial spray activities. Laboratory experiments were designed to evaluate factors (fresh versus marine water chemistry, temperature, and sunlight) that may promote the degradation of naled and dichlorvos in the environment. Results show that natural fresh and marine water chemistry promoted naled degradation as experiments with de-ionized water resulted in half-lives greater than 6 days. The half-life in natural waters without light ranged from 5 to 20 h with lower half lives at higher temperatures. Under light exposure, degradation was accelerated and yielded more dichlorvos. Detectable levels (0.05 µM for naled and 0.10 µM for dichlorvos) were measured in water samples collected from the field during aerial spray events. Results can be used in risk assessments that consider both naled and dichlorvos to better understand ecological impacts and to develop improved public health recommendations.