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Este trabalho teve como objetivo avaliar a tolerância e a capacidade de fitorremediação de crotalária (Crotalaria spectabilis), sorgo (Sorghum bicolor), nabo forrageiro (Raphanus sativus), amendoim (Arachis hypogaea) e alfafa (Mendicago sativa) a solos contaminados por tebuthiuron. Para determinar a tolerância das plantas ao herbicida estas foram submetidas a 5 diferentes doses (300, 600, 1200, 2400 e 4800 gramas de ingrediente ativo por hectare gi.a. ha-1) e comparadas com uma testemunha que não recebeu aplicação do herbicida. Crotalária, Nabo forrageiro e alfafa se mostraram sensíveis ao herbicida, mesmo na menor dose de aplicação, enquanto sorgo se mostrou tolerante ao herbicida até a dose de 600 gi.a. ha-1 tendo apresentado fitointoxicação de 80% na dose de 1200 gi.a. ha-1 e amendoim foi tolerante até a dose de 4800 gi.a. ha-1 para a qual apresentou apenas 40% de fitointoxicação. Plantas de amendoim e sorgo foram submetidas a dose de contaminação de 600 gi.a. ha-1 aplicada por meio de uma solução de trabalho contendo 17,47kBq (Quilobecquerels) de 14C-tebuthiuron. As duas plantas foram capazes de remediar o solo, no entanto amendoim se mostrou mais eficiente reduzindo a contaminação em 75,8% enquanto sorgo retirou do solo 44,49% do herbicida contaminante / This study aimed to evaluate the tolerance and phytoremediation capacity of sunn hemp (Crotalaria spectabilis), sorghum (Sorghum bicolor), turnip (Raphanus sativus), peanuts (Arachis hypogaea) and alfalfa (Mendicago sativa) in tebuthiuron contaminated soil. To determine the tolerance to the herbicide, plants were subjected to five different doses (300, 600, 1200, 2400 and 4800 grams of active ingredient per hectare gi.a. ha-1) and compared with a control that had no herbicide application. Sunn hemp, turnip forage and alfalfa were sensitive to the herbicide, even at the lowest application dose, while sorghum showed tolerance to the herbicide at 600 gi.a. ha-1 dose, having 80% phytointoxication presented at dose 1200 gi.a. ha-1 and peanut was tolerant at dose 4800 gi.a. ha-1 for which it showed only 40% of phytointoxication. Peanut and sorghum plants were subjected to a contamination dose 600 gi.a. ha-1 applied in a work solution containing 17.47kBq (Kilobecquerels) of 14C-tebuthiuron. The two plants were able to remediate the soil, however peanut was more efficient reducing contamination by 75.8% while sorghum removed 44.49% of the soil contaminant herbicide

Este trabalho teve como objetivo avaliar a tolerância e a capacidade de fitorremediação de crotalária (Crotalaria spectabilis), sorgo (Sorghum bicolor), nabo forrageiro (Raphanus sativus), amendoim (Arachis hypogaea) e alfafa (Mendicago sativa) a solos contaminados por tebuthiuron. Para determinar a tolerância das plantas ao herbicida estas foram submetidas a 5 diferentes doses (300, 600, 1200, 2400 e 4800 gramas de ingrediente ativo por hectare gi.a. ha-1) e comparadas com uma testemunha que não recebeu aplicação do herbicida. Crotalária, Nabo forrageiro e alfafa se mostraram sensíveis ao herbicida, mesmo na menor dose de aplicação, enquanto sorgo se mostrou tolerante ao herbicida até a dose de 600 gi.a. ha-1 tendo apresentado fitointoxicação de 80% na dose de 1200 gi.a. ha-1 e amendoim foi tolerante até a dose de 4800 gi.a. ha-1 para a qual apresentou apenas 40% de fitointoxicação. Plantas de amendoim e sorgo foram submetidas a dose de contaminação de 600 gi.a. ha-1 aplicada por meio de uma solução de trabalho contendo 17,47kBq (Quilobecquerels) de 14C-tebuthiuron. As duas plantas foram capazes de remediar o solo, no entanto amendoim se mostrou mais eficiente reduzindo a contaminação em 75,8% enquanto sorgo retirou do solo 44,49% do herbicida contaminante / This study aimed to evaluate the tolerance and phytoremediation capacity of sunn hemp (Crotalaria spectabilis), sorghum (Sorghum bicolor), turnip (Raphanus sativus), peanuts (Arachis hypogaea) and alfalfa (Mendicago sativa) in tebuthiuron contaminated soil. To determine the tolerance to the herbicide, plants were subjected to five different doses (300, 600, 1200, 2400 and 4800 grams of active ingredient per hectare gi.a. ha-1) and compared with a control that had no herbicide application. Sunn hemp, turnip forage and alfalfa were sensitive to the herbicide, even at the lowest application dose, while sorghum showed tolerance to the herbicide at 600 gi.a. ha-1 dose, having 80% phytointoxication presented at dose 1200 gi.a. ha-1 and peanut was tolerant at dose 4800 gi.a. ha-1 for which it showed only 40% of phytointoxication. Peanut and sorghum plants were subjected to a contamination dose 600 gi.a. ha-1 applied in a work solution containing 17.47kBq (Kilobecquerels) of 14C-tebuthiuron. The two plants were able to remediate the soil, however peanut was more efficient reducing contamination by 75.8% while sorghum removed 44.49% of the soil contaminant herbicide

Ingestion exposure estimates typically use a default bioavailability of 100%, thereby assuming that the entirety of an ingested dose is absorbed into systemic circulation. However, the actual bioavailability of ingested contaminants is oftentimes lower than 100%. The research described herein investigates the use of the Simulator of the Human Intestinal Microbial Ecosystem (SHIME) for the calculation of <i>in vitro</i> bioaccessibility (IVBA), a conservative predictor of bioavailability, of mercury (Hg) from traditional northern foods and arsenic (As) from soils. The primary objective of the research described herein is to address data-gaps which have hindered attempts to incorporate IVBA into risk assessment on more than a case-by-case basis. The hypotheses of this thesis are that (1) the bioaccessibility of contaminants is dependent upon concentration due to kinetic limitations on dissolution, (2) gastrointestinal (GI) microbes in the ileum and colon alter contaminant bioaccessibility and/or speciation, (3) the GI microbial effect on bioaccessibility is toxicologically relevant, and (4) metal bioaccessibility is predictable according to dissolution kinetics.<p> Mercury bioaccessibility from country food samples was independent of total Hg concentration (F=0.5726, P=0.578) whereas As bioaccessibility was inversely related to total As concentration for Nova Scotia mine tailings, synthesized ferrihydrite with adsorbed AsV, and synthesized amorphous scorodite (P=2 x 10-10). Isotherm analysis indicated that, at high soil As concentrations, saturation of simulated GI fluids limited As bioaccessibility under gastric conditions whereas kinetic limitations constrained As bioaccessibility under intestinal conditions. Additionally, we demonstrated that GI microbes may affect Hg bioaccessibility, either increasing or decreasing bioaccessibility depending upon the type of food. For example, the bioaccessibility of HgT decreased in the presence of GI microbial activity for caribou kidney, caribou tongue, seal blood, seal brain, seal liver, and walrus flesh. In contrast, HgT bioaccessibility from Arctic char and seal intestine increased in the presence of GI microbial activity. Similarly, colon microbial activity increased (Fishers Protected LSD, P<0.05) As bioaccessibility from synthesized amorphous scorodite (56 110%), Nova Scotia mine tailings (140 300%), an agricultural soil (53%) and an ironstone soil (350%) containing elevated arsenic concentrations. However, under small intestinal conditions, this microbial effect was transient and demonstrated a small effect size. The toxicological relevance of microbial effects upon As bioaccessibility was assessed using a juvenile swine model with co-administration of oral antibiotics (neomycin and metronidazole). This study research indicated that microbial effects on As bioaccessibility are not reflected in the juvenile swine model. For example, the microbial communities present in the pigs proximal colon clustered according to antibiotic treatment (e.g. microbial communities of antibiotic treated pigs differed from non-treated pigs). Despite this, the urinary arsenic excretion (and hence arsenic bioavailability) of antibiotic-treated juvenile swine orally exposed to soil-borne arsenic was equivalent (Holm-Sidak, P=0.930) to the urinary arsenic excretion of juvenile swine not treated with antibiotics. Therefore, in vitro GI models may not need to include a microbially active intestinal stage when measuring As IVBA.<p> Metal bioaccessibility from soils appears predictable according to fundamental chemical properties of the metal-of-concern. Specifically, metal bioaccessibility of 7 of the 13 metals (V, Ni, Zn, Cu, U, Cd, & Ba but not Tl, Pb, As, Se, Cr, and Hg) regulated according to Canadian Council of Ministers of the Environment Soil Quality Guidelines (CCME SQG) were strongly dependent (R2 = 0.7) on water exchange rate constants of metal cations (kH20) indicating that desorption kinetics may serve as the foundation of a predictive model of metal bioaccessibility.

Ingestion exposure estimates typically use a default bioavailability of 100%, thereby assuming that the entirety of an ingested dose is absorbed into systemic circulation. However, the actual bioavailability of ingested contaminants is oftentimes lower than 100%. The research described herein investigates the use of the Simulator of the Human Intestinal Microbial Ecosystem (SHIME) for the calculation of <i>in vitro</i> bioaccessibility (IVBA), a conservative predictor of bioavailability, of mercury (Hg) from traditional northern foods and arsenic (As) from soils. The primary objective of the research described herein is to address data-gaps which have hindered attempts to incorporate IVBA into risk assessment on more than a case-by-case basis. The hypotheses of this thesis are that (1) the bioaccessibility of contaminants is dependent upon concentration due to kinetic limitations on dissolution, (2) gastrointestinal (GI) microbes in the ileum and colon alter contaminant bioaccessibility and/or speciation, (3) the GI microbial effect on bioaccessibility is toxicologically relevant, and (4) metal bioaccessibility is predictable according to dissolution kinetics.<p> Mercury bioaccessibility from country food samples was independent of total Hg concentration (F=0.5726, P=0.578) whereas As bioaccessibility was inversely related to total As concentration for Nova Scotia mine tailings, synthesized ferrihydrite with adsorbed AsV, and synthesized amorphous scorodite (P=2 x 10-10). Isotherm analysis indicated that, at high soil As concentrations, saturation of simulated GI fluids limited As bioaccessibility under gastric conditions whereas kinetic limitations constrained As bioaccessibility under intestinal conditions. Additionally, we demonstrated that GI microbes may affect Hg bioaccessibility, either increasing or decreasing bioaccessibility depending upon the type of food. For example, the bioaccessibility of HgT decreased in the presence of GI microbial activity for caribou kidney, caribou tongue, seal blood, seal brain, seal liver, and walrus flesh. In contrast, HgT bioaccessibility from Arctic char and seal intestine increased in the presence of GI microbial activity. Similarly, colon microbial activity increased (Fishers Protected LSD, P<0.05) As bioaccessibility from synthesized amorphous scorodite (56 110%), Nova Scotia mine tailings (140 300%), an agricultural soil (53%) and an ironstone soil (350%) containing elevated arsenic concentrations. However, under small intestinal conditions, this microbial effect was transient and demonstrated a small effect size. The toxicological relevance of microbial effects upon As bioaccessibility was assessed using a juvenile swine model with co-administration of oral antibiotics (neomycin and metronidazole). This study research indicated that microbial effects on As bioaccessibility are not reflected in the juvenile swine model. For example, the microbial communities present in the pigs proximal colon clustered according to antibiotic treatment (e.g. microbial communities of antibiotic treated pigs differed from non-treated pigs). Despite this, the urinary arsenic excretion (and hence arsenic bioavailability) of antibiotic-treated juvenile swine orally exposed to soil-borne arsenic was equivalent (Holm-Sidak, P=0.930) to the urinary arsenic excretion of juvenile swine not treated with antibiotics. Therefore, in vitro GI models may not need to include a microbially active intestinal stage when measuring As IVBA.<p> Metal bioaccessibility from soils appears predictable according to fundamental chemical properties of the metal-of-concern. Specifically, metal bioaccessibility of 7 of the 13 metals (V, Ni, Zn, Cu, U, Cd, & Ba but not Tl, Pb, As, Se, Cr, and Hg) regulated according to Canadian Council of Ministers of the Environment Soil Quality Guidelines (CCME SQG) were strongly dependent (R2 = 0.7) on water exchange rate constants of metal cations (kH20) indicating that desorption kinetics may serve as the foundation of a predictive model of metal bioaccessibility.

The objective of this research was to evaluate the treatment efficiency of a trichloroethylene (TCE) contaminated soil by combined technologies of the suspension of palladized nanoiron and electrokinetic remediation process. First, nanoiron and palladized nanoiron were prepared using the chemical reduction method. Then they were characterized by various methods. Micrographs of scanning electron microscopy have shown that a majority of these nanoparticles were in the range of 50-80 nm. Specific surface areas were determined to be 76.88 m2/g and 100.61 m2/g for the former and latter, respectively. Results of X-ray diffractometry have shown that both types of nanoiron were poor in crystallinity. Three anionic dispersants were employed for evaluating their performance in stabilizing various nanoiron. Results have demonstrated that an addition of 1 wt% of Dispersant E during nanoiron preparation would result in a good stabilization of nanoiron. If the system pH was adjusted to 2.99, nanoparticles would settle rapidly. Batch tests were carried out to investigate the effects of various operating parameters on degradation of TCE in aqueous solutions. Experimental results have indicated that palladized nanoiron outperformed nanoiron in treatment of TCE in this study. The employment of Dispersant E would enhance the treatment efficiency further. Test results also showed that a linear increase of reaction rate constant was found with an increasing dose of palladium from 0.05 wt% to 1 wt% based on the mass of nanoiron. Further, an exponential increase of reaction rate constant would be obtained with an increasing pH. As for mixing intensity, it was found to be insignificant to the treatment efficiency of TCE in aqueous solutions. The final stage of this study was to evaluate the treatment efficiency of combined technologies of the suspension of palladized nanoiron and electrokinetic remediation process in treating a TCE-contaminated soil. Test conditions used were given as follows: (1) initial TCE concentration: 160-181 mg/kg; (2) electric potential gradient: 1 V/cm; (3) daily addition of 20 mL of suspension of palladized nanoiron (2.5 g/L) to the electrode reservoir; and (4) reaction time: 6 days. Test results have shown that addition of palladized iron suspension to the cathode reservoir yielded the lowest residual TCE concentration in soil. Namely, about 92.5% removal of TCE from soil. On the other hand, addition of palladized iron suspension to the anode reservoir would enhance the degradation of TCE therein. Based on the above findings, the treatment method employed in this work was proven to be a novel and efficient one in treating TCE-contaminated soil.

Abstract This research was to evaluate the treatment efficiency for in-situ treatment of pentachlorophenol (PCP) contaminated soil by electrokinetics-Fenton process combined with biodegradation. An electric gradient of 1V/cm, and graphite electrodes were employed in all experiments. Soil types, catalyst types and dosage, hydrogen peroxide concentration, cathode reservoir liquid species and reaction time were employed as the experimental factors in this study. In this study, no matter electrokinetics-Fenton process or the electrokinetics-biodegradation in the latter, prolong the reaction time can promote the removal and destruction efficiency (DRE) of target pollutant from soil. By using 0.0196 M FeSO4 with 3.5% H2O2, the DRE was only lower 2% than 0.098 M FeSO4 with 3.5% H2O2.It showed that using 0.0196 M FeSO4 can provide enough Fe2+ to react with H2O2. By increasing H2O2 concentration from 0.35% to 3.5%, a DRE rised from 68.34% to 79.77%. When iron powder was used as catalyst, the residual pentachloroplenol concentration near to anode reservoir lower than 0.0196 M FeSO4 was used. But the DRE was 56.58% lower than the 68.34% of using 0.0196 M FeSO4.As the influences of soil types to electrokinetics-Fenton process, the residual concentration of pollutant for Soil No. 2 was higher than Soil No. 1. A DRE of only 59.22% was obtained. It is postulated that a much higher content of organic matter with Soil No. 2 whereas lower the treatment efficiency because of consumption of hydroxyl radicals by the organic matter of soil. For the influence of different reservoir liquid species, in this study 0.1M acetic buffer solution was used as cathode reservoir liquid, expected to promote the removal efficiency. From the result of experiment that could not reach the expected treatment efficiency of increasing the removal efficiency from soil. From the experiment of electrokinetics process combined with cometabolism, a treatment efficiency of only 25.67% was obtained. The content of pollutant within every section of soil column were still higher than predict. But by using electrokinetics-Fenton process to pretreat the pollutant within soil first, the increasing efficiency of biodegradation was found. Even when reaction time was prolonged, the pollutant could be completely eliminated from soil. If only used iron minerals to proceed electrokinetics-Fenton process naturally exited in the soil, a DRE of only 20