This study aims to determine the distribution of particulates carrying heavy metals at selected sites on a college campus using dandelion leaves as collectors. As a comparison, sites far away from the campus surrounding Bristol Motor Speedway Car Racing Stadium were also monitored. To reduce the probability of memory effects from the long-term atmospheric deposition or absorption of metals from soil a seasonal plant, dandelion, was used to monitor the metal contents. The metals monitored are cadmium, calcium, copper, chromium, iron, lead, and zinc. Fourteen sites were monitored and samples were collected once a week initially (growing time of the plant), and later at 4-week interval from 28th March to 31st August of 2007. The metal contents of the nitric acid digested and appropriately diluted samples were determined by flame atomic absorption spectrometry using the regular standard calibration curve and also the standard addition method. From the results obtained, and the careful log of the weather and human activities at the different sites, it is concluded that human activities played a major role in the distribution of metal-laden particulates. Also dandelion leaves were proven to be viable collectors of these particulates without memory effects and as indicators of current particulates generated rather than a long-term cumulative one.

Heavy metal contamination of soils, sediments and groundwater presents an ongoing source of hazardous and persistent environmental pollution. How best to remediate these contaminants is the impetus of continuing research efforts. Methods include containment, ex situ and in situ techniques. A successful in situ method utilizing a combination of emulsified liquid membranes, ELM, and zero-valent metal, ZVM, and bimetals has demonstrated impressive heavy metal reduction in 100 ppm solutions of Cd, Cu, Ni, Pb, Cr and U. This promising in situ method has been employed by the Industrial Chemistry Laboratory at the University of Central Florida and it has demonstrated considerable success in treating several environmental threats. Contaminated soils, surfaces, sediments and groundwater with offending agents such as trichloroethene, polychorobiphenyls and heavy metals have been treated utilizing emulsified liquid membrane systems containing zero-valent iron or bimetal particles. In vial studies, lead spiked sediments have shown repeatable 60% removal of lead after seven days of treatment. A persistent pattern emerged at ten days whereupon remediation levels began to drop. The current study was established to determine the reason for the decline at ten days and beyond. Questions addressed: Does the formation of an impeding oxide layer diminish the remediation capacity of the iron/magnesium system? Does the emulsion reach a maximum capacity to withdraw the contaminant? Do the soil components or the soil structure interfere with the access to the contaminant? This study has yielded insight into the reasons emulsified liquid membrane systems containing zero-valent metals achieved maximum lead removal at day seven, and thereafter begin to lose their effectiveness. A three part study was implemented to address and to answer the three questions pertaining to the consistent pattern of diminishing remediation levels exhibited at day ten and beyond. Initially, from Study I results it appeared that the formation of an impeding oxide layer on the bi-metal which was inside the emulsion droplet and which plated or precipitated with the lead was not occurring at day ten. Results indicated that the iron/magnesium was still capable of removing lead. Furthermore, from Study II results the emulsion dose injected appeared adequate to remove the lead, meaning that the emulsion had not reached its maximum capacity for remediation. The emulsion dose was not a limiting factor. Lastly, Study III results seemed to indicate that the drop in remediation after day seven pertained to the soil structure. There appeared to be some merit to the idea that with aging of the sediment, the lead was diffusing and migrating to some inaccessible interior sites within the sediment particles. Additionally, indications from day ten and day fourteen delineated that a second emulsion dose injection might restore lead removal levels to approach those first observed at day seven and consequently be a useful field application. In order to explore the effectiveness of injecting a second dose of emulsion, another vial study was implemented. The typical pattern of observing sixty percent maximum lead removal at day seven was observed. In separate groups, a second injection of emulsion was added at day five, and then for another vial series, a second dose was added at day seven. The second emulsion dose treatment for either day five or day seven did not yield any increases in percent lead removal. Another theory emerged after viewing micrographs of recovered iron/magnesium compared with fresh ball-milled bimetal. In addition, scanning electron microscopy appeared to confirm the explanation that the emulsified zero-valent metal system might be compromised after day seven. This would lead to exposure of the iron/magnesium to the air and the elements. Corrosion of the bimetal might be occurring. With time, release of the plated or precipitated lead back into the sediment mixture could follow. The results of Study I had led to the conclusion that an impeding oxide layer had not formed; however, this conclusion may have been premature because the recovered iron/magnesium was exposed to lead solution in the vial study. Perhaps if the recovered iron/magnesium was inserted back into an emulsion and injected into lead spiked sediments the percent lead removed might give a more accurate picture of the iron/magnesium's capability to continue performing remediation. Remediation of sediments contaminated with lead is a complicated task because of the complex nature of sediment components. Emulsified liquid membranes utilizing zero-valent bimetals has repeatedly demonstrated impressive results at day seven; however, this treatment method is not without its limitations. Optimal results appear to be gained at day seven after emulsion injection. The bimetal and plated or precipitated lead must be removed at that point; otherwise the effective remediation of the contaminant is progressively reversed.

High concentrations of heavy metals in the soils have potential long-term environmental and health concerns because of their persistence and accumulation tendency in the environment and along the food chain. This study was aimed at studying the feasibility of heavy metals removal from the soil using plants naturally growing in the surroundings of selected polluted sites in Tanzania and soil application of the sorbent materials zeolite and autoclaved aerated concrete (AAC). The results showed that Sporobolus sp. is a hyperaccumulator of Cu. Four other species, Launea cornuta (Oliv &amp; Hiern) O. Jeffrey, Tagetes minuta (L.), Sporobolus sp. and Blotiella glabra (Bory) Tryon showed high potential for phytoextraction of Cu. No hyperaccumulators of Pb and Zn were identified in the area, but Tephrosia candida and Tagetes minuta (L.) were identified as potential plants for phytoextraction of Pb, while Conyza bonariensis (L.) Cronquist, Launea cornuta (Oliv &amp; Hiern) O. Jeffrey, Tagetes minuta (L.), Blotiella glabra (Bory) Tryon, Pteridium aquilinum (L.) Kulm and Polygonum setogulum A. Rich were identified as potential plants for phytoextraction of Zn. The result from sorbent experiments showed that both materials had a potential for remediating metal polluted soils. The AAC had a higher removal capacity for both Zn and Pb than zeolite. The removal capacity of zeolite and AAC in a mixed metal experiment (Pb and Zn) showed a little difference in the sorption capacity of AAC and Zeolite for Pb and Zn respectively. Speciation of the metal in soil shows that the major part of the metal was associated with firmly attached component of the metal in the soil. Compared with the total metal concentration analysed, the available component accounted for 13-39% for Zn and 31-39% for Pb. It can be suggested to co-remediate polluted soils using reactive sorbent nodules and hyper-accumulating plant species. Identification of the best combinations and designs remains the subject of future research. / <p>QC 20121130</p>

Heavy metal contamination in water is a serious environmental and human health issue. Lead (Pb2+) and cadmium (Cd2+) are strictly regulated in wastewater effluent due to their high toxicity at low concentrations. Heavy metals are difficult to remove in conventional biological wastewater treatment because they are water soluble and non-biodegradable. Advanced treatment, such as tight membrane filtration and ion exchange, can be applied but they often require a high electrical energy input and a large amount of chemicals for pre- or post-treatment. Microbial electrolysis cells (MECs) can be used to treat wastewater while simultaneously recovering energy in the form of hydrogen gas. Additionally, MECs were proven to be effective for heavy metal removal. The commonly investigated removal mechanism for heavy metals in MECs is reduction at the cathode where heavy metal ions are reduced to metallic solids. The research presented in this thesis examined the effectiveness of cathodic reduction and other heavy metal removal mechanisms in MECs over a wide range of metal concentrations (10 μg/L-12 mg/L). Lab-scale MEC operation demonstrated successful removal of both Pb2+ and Cd2+ under different electric conditions, operation times, and initial metal concentrations. In addition to cathodic reduction, heavy metal removal in MECs was demonstrated through chemical precipitation at the cathode and electrochemical reduction and biosorption at the bioanode. The results of this research also confirmed the importance of microbial activity at the bioanode to efficiently drive the removal mechanisms in MECs. / Thesis / Master of Applied Science (MASc)

In an electrochemical sensor, the sensing performance is mainly dependent on the mass transport of the analyte towards the working electrode-electrolyte interface and working electrode properties. Carbon nanomaterials like carbon nanotubes are widely employed to modify the working electrode properties for sensitive detection. A simulation model is formulated to investigate the effects of modifying a planar bare electrode with carbon nanotubes on electrochemical detection of fenitrothion (FT, an organophosphate). The model revealed that porous electrodes caused the change in mass transport regime and influenced FT’s electrochemical response. The results aided in understanding the influence of the porous electrode on analyte detection and thus assisted in the fabrication of an ultrasensitive electrochemical sensor. Simulation supported synthesis of a highly sensitive ink to produce highly porous and electrocatalytic electrodes. Activated carbon (AC) possesses high porosity and surface area, but they suffer from lower electrical conductivity. To enhance their conductivity, AC was co-doped with nitrogen and sulfur. Multiwalled carbon nanotubes were incorporated to further improve their porosity and electrocatalytic properties. The synthesized nitrogen-sulfur co-doped activated carbon coated multiwalled carbon nanotube (NS-AC-MWCNT) ink produced highly porous electrocatalytic electrodes. The sensor revealed a 4.9 nM limit of detection (LOD) under optimized conditions. However, it failed to overcome the enzymatic sensors’ performances. The ultrasensitive performance was achieved by incorporating a detecting agent in the ink that instilled analyte capture ability. Metal oxides like ZrO2, MnO2, and MgO possessed affinity towards organophosphate (fenitrothion), heavy-metal ion (lead), and nutrient (nitrite). Metal oxides were modified with 3,4-dihydroxylbenzaldehyde (DHBA) – Chitosan (CHIT) to produce well dispersed and uniformly coated stable electrodes. The ZrO2-DHBA-CHIT/NS-AC-MWCNT sensor achieved a remarkable limit of detection of 1.69 nM for FT. The sensor's performance exceeded the enzymatic-based sensors. The commonly found chemical interferents had negligible interference. The sensor produced reliable and satisfactory performance in lake and tap water. The MnO2-DHBA-CHIT/NS-AC-MWCNT/GCE and MgO-DHBA-CHIT/NS-AC-MWCNT/GCE sensors produced an enormous improvement in the sensor performance compared to unmodified electrodes for lead and nitrite detection. The preliminary results on detecting other pollutants like lead and nitrite showed the importance of the methodology in providing a platform for a new class of metal oxide-based sensors. / Thesis / Doctor of Philosophy (PhD) / The growing population and rapid industrial development are affecting the water quality worldwide. The major water pollutants are organophosphates, heavy metal ions, and nutrients. These water pollutants are harmful, and their bioaccumulation poses a major health concern. In the USA alone, water quality issues are predicted to cost $210 billion annually. Therefore, sensors to detect water pollutants are developed to monitor their environmental footprints. Electrochemical sensors are popularly used to detect water pollutants owing to their low-cost and high sensitivity. The objective of this dissertation was to fabricate highly sensitive and specific electrochemical sensors to detect organophosphate (e.g., fenitrothion, FT), heavy metal ion (e.g., lead), and nutrient (e.g., nitrite). The sensors were fabricated with ink based on nanomaterials like carbon nanotubes and detecting agents like metal oxides. The fabricated sensors achieved very high sensitivity and specificity and can detect water pollutants in lake and tap water.

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