AbstractArsenic (As) contamination of groundwater and surface water is a worldwide problem. Exposure to arsenic in drinking water is an important current public health issue. Arsenic is well known for its carcinogenic and teratogenic effects. The U.S. Environmental Protection Agency (USEPA) has recently enacted a stricter drinking water standard for arsenic that lowers the maximum contaminant level (MCL) from 50 to 10 ug l-1.Localized elevated As concentrations in groundwater or surface water have been attributed to the natural release of As from the weathering of As bearing minerals. Microbial reduction of arsenate (As(V)) to arsenite (As(III)) and ferric (hydr)oxides to Fe(II) is hypothesized to be the dominant mechanisms of As mobilization in subsurface environments. If oxidizing conditions can be restored, As can be immobilized by the formation of As(V) and ferric (hydr)oxides. As(V) is more strongly adsorbed than As(III) at circumneutral conditions by common non-iron metal oxides in sediments such as those of aluminum. Ferric (hydr)oxides have strong affinity for both As(III) and As(V) in circumneutral environments. Oxygen can be introduced into the anaerobic zone by injection of gaseous O2 to promote oxidation reactions of As(III) and Fe(II), but O2 is poorly soluble and chemically reactive and thus difficult to distribute in the subsurface. Nitrate or chlorate can be considered as alternative oxidants with advantages over elemental oxygen due to their high aqueous solubility and lower chemical reactivity which together enable them to be better dispersed in the saturated subsurface.The objective of this study is to evaluate the importance of anoxic oxidation of As(III) to As(V) by anaerobic microorganisms such as chemolithotrophic denitrifying bacteria and chlorate respiring bacteria in the biogeochemical cycle of arsenic. This study also investigated a arsenic potential bioremediation strategy based on injecting nitrate or chlorate into contaminated groundwater and surface water under anaerobic conditions.In this study, denitrification or chlorate reduction linked to the oxidation of As(III) to As(V) was shown to be a widespread microbial activity in anaerobic sludge and sediment samples that were not previously exposed to arsenic contamination. The biological oxidation of As(III) utilizing nitrate or chlorate as sole electron acceptor was feasible and stable over prolonged periods of operation in continuous-flow anaerobic bioreactors. Evidence for the complete denitrification was demonstrated by direct measurement of N2 formation dependent on As(III) addition. Also complete chlorate reduction to chloride was attributable to the oxidation of As(III). A 16S rRNA gene clone library characterization of enrichment cultures indicated that the predominant phylotypes responsible for As(III) oxidation linked to denitrification were from the genus Azoarcus and the family Comamonadaceae. A bioremediation strategy was explored that is based on injecting nitrate to support the microbial oxidation of Fe(II) and As(III) in the subsurface as a means to immobilize arsenic. Two models were utilized to illustrate the mechanisms of As removal.1) Sediment columns packed with activated alumina were utilized to demonstrate the role of nitrate in supporting microbial As(III) oxidation and arsenic mobility in anoxic sediments containing mostly non-iron oxides;2) Sand-packed columns were used to simulate natural anaerobic groundwater and sediment systems with co-occurring As(III) and Fe(II) in the presence or absence of nitrate. Microbial oxidation by denitrifying microorganisms lead to the formation of ferric (hydroxides) which adsorbed As(V) formed from As(III)-oxidation.The studies presented here demonstrate that anoxic microbial oxidation of As(III) and Fe(II) linked to denitrification significantly enhance the immobilization of As in the anaerobic subsurface environments.
| Identifer | oai:union.ndltd.org:arizona.edu/oai:arizona.openrepository.com:10150/194899 |
| Date | January 2008 |
| Creators | Sun, Wenjie |
| Contributors | Sierra-Alvarez, Maria Reyes, Field, James A., Sierra-Alvarez, Maria Reyes, Field, James A., Ela, Wendell P., Maier, Raina M. |
| Publisher | The University of Arizona. |
| Source Sets | University of Arizona |
| Language | English |
| Detected Language | English |
| Type | text, Electronic Dissertation |
| Rights | Copyright © is held by the author. Digital access to this material is made possible by the University Libraries, University of Arizona. Further transmission, reproduction or presentation (such as public display or performance) of protected items is prohibited except with permission of the author. |
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