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F. H. Chapelle

Publications and source records attributed to F. H. Chapelle.

At least 37 records · Page 2Linked to original sources

TBA biodegradation in surface-water sediments under aerobic and anaerobic conditions

The potential for [U-14C] TBA biodegradation was examined in laboratory microcosms under a range of terminal electron accepting conditions. TBA mineralization to CO2 was substantial in surface-water sediments under oxic, denitrifying, or Mn(IV)-reducing conditions and statistically significant but low under SO4-reducing conditions. Thus, anaerobic TBA biodegradation may be a significant natural attenuation mechanism for TBA in the environment, and stimulation of in situ TBA bioremediation by addition of suitable terminal electron acceptors may be feasible. No degradation of [U-14C] TBA was observed under methanogenic or Fe(III)-reducing conditions.

Environmental Science & Technology

Natural attenuation of chlorinated solvents at Area 6, Dover Air Force Base: Groundwater biogeochemistry

Monitored natural attenuation (MNA) has recently emerged as a viable groundwater remediation technology in the United States. Area 6 at Dover Air Force Base (Dover, DE) was chosen as a test site to examine the potential for MNA of tetrachloroethene (PCE) and trichloroethene (TCE) in groundwater and aquifer sediments. A "lines of evidence" approach was used to document the occurrence of natural attenuation. Chlorinated hydrocarbon and biogeochemical data were used to develop a site-specific conceptual model where both anaerobic and aerobic biological processes are responsible for the destruction of PCE, TCE, and daughter metabolites. An examination of groundwater biogeochemical data showed a region of depleted dissolved oxygen with elevated dissolved methane and hydrogen concentrations. Reductive dechlorination likely dominated in the anaerobic portion of the aquifer where PCE and TCE levels were observed to decrease with a simultaneous increase in cis-1,2-dichloroethene (cis-DCE), vinyl chloride (VC), ethene, and dissolved chloride. Near the anaerobic/aerobic interface, concentrations of cis-DCE and VC decreased to below detection limits, presumably due to aerobic biotransformation processes. Therefore, the contaminant and daughter product plumes present at the site appear to have been naturally attenuated by a combination of active anaerobic and aerobic biotransformation processes. ?? 2002 Elsevier Science B.V. All rights reserved.

Journal of Contaminant Hydrology

Microbial mineralization of ethene under sulfate-reducing conditions

Previous investigations demonstrated that respiratoly reductive dechlorination of vinyl chloride (VC) can be efficient even at H 2 concentrations (≤2 n M ) that are characteristic of SO 4 -reducing conditions. In the study reported here, microorganisms indigenous to a lake-bed sediment completely mineralized [1,2- 14 C] ethene to 14 14CO 2 when incubated under SO 4 -reducing conditions. Together, these observations argue for a novel mechanism for the net anaerobic oxidation of VC to CO 2 : reductive dechlorination of VC to ethene followed by anaerobic oxidation of ethene to CO 2 . Moreover, the results of this study suggest that reliance on ethene and/or ethane accumulation as a quantitative indicator of complete reductive dechlorination of chioroethene contaminants may not be warranted.

Bioremediation Journal

Effect of redox conditions on MTBE biodegradation in surface water Sediments

Microbial degradation of methyl tert-butyl ether (MTBE) was observed in surface water-sediment microcosms under anaerobic conditions. The efficiency and products of anaerobic MTBE biodegradation were dependent on the predominant terminal electron-accepting conditions. In the presence of substantial methanogenic activity, MTBE biodegradation was nominal and involved reduction of MTBE to the toxic product, tert-butyl alcohol (TBA). In the absence of significant methanogenic activity, accumulation of [14C]TBA generally decreased, and mineralization of [U-14C]MTBE to 14CO2 generally increased as the oxidative potential of the predominant terminal electron acceptor increased in the order of SO4, Fe(III), Mn(IV) < NO3 < O2. Microbial mineralization of MTBE to CO2 under Mn(IV)or SO4-reducing conditions has not been reported previously. The results of this study indicate that microorganisms inhabiting the sediments of streams and lakes can degrade MTBE effectively under a range of anaerobic terminal electron-accepting conditions. Thus, anaerobic bed sediment microbial processes may provide a significant environmental sink for MTBE in surface water systems throughout the United States.

Environmental Science & Technology

Methyl tert-butyl ether biodegradation by indigenous aquifer microorganisms under natural and artificial oxic conditions

Microbial communities indigenous to a shallow groundwater system near Beaufort, SC, degraded milligram per liter concentrations of methyl tert -butyl ether (MTBE) under natural and artificial oxic conditions. Significant MTBE biodegradation was observed where anoxic, MTBE-contaminated groundwater discharged to a concrete-lined ditch. In the anoxic groundwater adjacent to the ditch, concentrations of MTBE were >1 mg/L. Where groundwater discharge occurs, dissolved oxygen (DO) concentrations beneath the ditch exceeded 1.0 mg/L to a depth of 1.5 m, and MTBE concentrations decreased to <1 μg/L prior to discharge. MTBE mass flux calculations indicate that 96% of MTBE mass loss occurs in the relatively small oxic zone prior to discharge. Samples of a natural microbial biofilm present in the oxic zone beneath the ditch completely degraded [U- 14 C]MTBE to [ 14 C]CO 2 in laboratory liquid culture studies, with no accumulation of intermediate compounds. Upgradient of the ditch in the anoxic, MTBE- and BTEX-contaminated aquifer, addition of a soluble oxygen release compound resulted in oxic conditions and rapid MTBE biodegradation by indigenous microorganisms. In an observation well located closest to the oxygen addition area, DO concentrations increased from 0.4 to 12 mg/L in <60 days and MTBE concentrations decreased from 20 to 3 mg/L. In the same time period at a downgradient observation well, DO increased from <0.2 to 2 mg/L and MTBE concentrations decreased from 30 to <5 mg/L. These results indicate that microorganisms indigenous to the groundwater system at this site can degrade milligram per liter concentrations of MTBE under natural and artificial oxic conditions.

Environmental Science & Technology

Widespread potential for microbial MTBE degradation in surface-water sediments

Microorganisms indigenous to stream and lake bed sediments, collected from 11 sites throughout the United States, demonstrated significant mineralization of the fuel oxygenate, methyl-tert-butyl ether (MTBE). Mineralization of [U-14C]MTBE to 14CO2 ranged from 15 to 66% over 50 days and did not differ significantly between sediments collected from MTBE contaminated sites and from sites with no history of MTBE exposure. This result suggests that even the microbial communities indigenous to newly contaminated surface water systems will exhibit some innate ability to attenuate MTBE under aerobic conditions. The magnitude of MTBE mineralization was related to the sediment grain size distribution. A pronounced, inverse correlation (p < 0.001; r2 = 0.73) was observed between the final recovery of 14CO2 and the percentage content of silt and clay sized grains (grain diameter < 0.125 mm). The results of this study indicate that the microorganisms that inhabit the bed sediments of streams and lakes can degrade MTBE efficiently and that this capability is widespread in the environment. Thus aerobic bed sediment microbial processes may provide a significant environmental sink for MTBE in surface water systems throughout the United States and may contribute to the reported transience of MTBE in some surface waters.

Environmental Science & Technology

Potential contribution of microbial degradation to natural attenuation of MTBE in surface water systems

The potential contribution of in situ biodegradation as a mechanism for natural attenuation of MTBE in surface water was studied. Surface water sediments from streams and lakes at 11 sites throughout the US. Microbial degradation of [U-14C] MTBE was observed in surface-water-sediment microcosms under anaerobic conditions, but the efficiency and products of anaerobic MTBE biodegradation were strongly dependent on the predominant terminal electron accepting conditions. In the presence of substantial methanogenic activity, MTBE biodegradation was nominal and involved reduction of MTBE to t-butanol (TBA). Under more oxidizing conditions, minimal accumulation of 14C-TBA and significant mineralization of [U-14C] MTBE to 14CO2 were observed. Microorganisms inhabiting the bed sediments of streams and lakes could degrade MTBE effectively under a range of anaerobic terminal electron accepting conditions. Thus, anaerobic bed sediment microbial processes also might contribute to natural attenuation of MTBE in surface water systems throughout the US. This is an abstract of a paper presented at the 222nd ACS National Meting (Chicago, IL 8/26-30/2001).

ACS Division of Environmental Chemistry, Preprints

Redox conditions and the efficiency of chlorinated ethene biodegradation: Laboratory studies

The potential for biodegradation of highly reduced groundwater contaminants is greatest under aerobic conditions and least under CO2-reducing (methanogenic) conditions. Laboratory studies conducted using [1,2-14C] vinyl chloride (VC) indicate the same pattern applies to the anaerobic oxidation of relatively reduced chloroethylenes. Recent studies, showing that CH4 can be a significant product of microbial degradation of VC under methanogenic conditions, clarified mechanisms underlying anaerobic VC mineralization and emphasized the redox dependence of this process. A microcosm study conducted with stream bed sediments demonstrated rapid degradation of [1,2-14C] VC and simultaneous production of 14CO2 and 14CH4. The results of acetate mineralization studies indicated that these sediments contained active acetotrophic methanogens. VC degradation involved an initial transformation to acetate via oxidative acetogenesis followed by acetotrophic methanogenesis to yield CO2 and CH4 as final products. Based on these recent results, a conceptual model for anaerobic microbial degradation of VC to non-chlorinated products can be proposed.

Conference Paper

Redox conditions and the efficiency of chlorinated ethene biodegradation: Field studies

The effect of redox conditions on the efficiency of chlorinated ethene biodegradation was investigated at two field sites. One site (NAS Cecil Field, FL) is characterized by predominantly Fe(III)-reducing conditions in the contaminant source area, grading to predominantly sulfate- reducing conditions downgradient. This sequence of redox conditions led to relatively inefficient biodegradation of chlorinated ethenes, with high concentrations of trichloroethene extending more than 400 meters downgradient of the source area. In contrast, a second site (NBS Kings Bay, GA) characterized by predominantly sulfate-reducing conditions in the source area followed by Fe(III)-reducing conditions downgradient. In this system perchloroethene (PCE) and TCE were rapidly biodegraded and extended less than 100 meters downgradient. Rates of ground- water transport are similar at the two sites (???0.2 m/d) indicating that the succession of redox processes, rather than other hydrologic factors, is the principal control on biodegradation. In particular, redox conditions that favor the initial reduction of highly chlorinated ethenes (methanogenic or sulfate-reducing conditions) followed by more oxidizing conditions (Fe(III)- reducing or oxic conditions) favors efficient biodegradation. Thus, documenting the succession of redox processes is an important step in understanding the efficiency of chlorinated ethene biodegradation in ground-water systems.

Conference Paper

Aerobic mineralization of MTBE and tert-butyl alcohol by stream-bed sediment microorganisms

Microorganisms indigenous to the stream-bed sediments at two gasoline- contaminated groundwater sites demonstrated significant mineralization of the fuel oxygenates, methyl tert-butyl ether (MTBE) and tert-butyl alcohol (TBA). Up to 73% of [U-14C]-MTBE and 84% of [U-14C]-TBA were degraded to 14CO2 under mixed aerobic/anaerobic conditions. No significant mineralization was observed under strictly anaerobic conditions. The results indicate that, under the mixed aerobic/anaerobic conditions characteristic of stream-bed sediments, microbial processes may provide a significant environmental sink for MTBE and TBA delivered to surface water bodies by contaminated groundwater or by other sources.Microorganisms indigenous to the stream-bed sediments at two gasoline-contaminated groundwater sites demonstrated significant mineralization of the fuel oxygenates, methyl tert-butyl ether (MTBE) and tert-butyl alcohol (TBA). Up to 73% of [U-14C]-MTBE and 84% of [U-14C]-TBA were degraded to 14CO2 under mixed aerobic/anaerobic conditions. No significant mineralization was observed under strictly anaerobic conditions. The results indicate that, under the mixed aerobic/anaerobic conditions characteristic of stream-bed sediments, microbial processes may provide a significant environmental sink for MTBE and TBA delivered to surface water bodies by contaminated groundwater or by other sources.

Environmental Science & Technology

Microbial mineralization of VC and DCE under different terminal electron accepting conditions

Production of 14CO2 from [1,2-14C] dichloroethene (DCE) or [1,2-14C] vinyl chloride (VC) was quantified in aquifer and stream-bed sediment microcosms to evaluate the potential for microbial mineralization as a pathway for DCE and VC biodegradation under aerobic, Fe(III)-reducing, SO4-reducing, and methanogenic conditions. Mineralization of [1,2-14C] DCE and [1,2-14C] VC to 14CO2 decreased under increasingly reducing conditions, but significant mineralization was observed for both sediments even under anaerobic conditions. VC mineralization decreased in the order of aerobic > Fe(III)-reducing > SO4-reducing > methanogenic conditions. For both sediments, VC mineralization was greater than DCE mineralization under all electron-accepting conditions examined. For both sediments, DCE mineralization was at least two times greater under aerobic conditions than under anaerobic conditions. Although significant microbial mineralization of DCE was observed under anaerobic conditions, recovery of 14CO2 did not differ substantially between anaerobic treatments.

Anaerobe

Field and laboratory evidence for intrinsic biodegradation of vinyl chloride contamination in a Fe(III)-reducing aquifer

Intrinsic bioremediation of chlorinated ethenes in anaerobic aquifers previously has not been considered feasible, due, in large part, to 1) the production of vinyl chloride during microbial reductive dechlorination of higher chlorinated contaminants and 2) the apparent poor biodegradability of vinyl chloride under anaerobic conditions. In this study, a combination of field geochemical analyses and laboratory radiotracer ([1,2-14C] vinyl chloride) experiments was utilized to assess the potential for intrinsic biodegradation of vinyl chloride contamination in an Fe(III)-reducing, anaerobic aquifer. Microcosm experiments conducted under Fe(III)-reducing conditions with material from the Fe(III)-reducing, chlorinated-ethene contaminated aquifer demonstrated significant oxidation of [1,2-14C] vinyl chloride to 14CO2 with no detectable production of ethene or other reductive dehalogenation products. Rates of degradation derived from the microcosm experiments (0.9-1.3% d-1) were consistent with field-estimated rates (0.03-0.2% d-1) of apparent vinyl chloride degradation. Field estimates of apparent vinyl chloride biodegradation were calculated using two distinct approaches; 1) a solute dispersion model and 2) a mass balance assessment. These findings demonstrate that degradation under Fe(III) reducing conditions can be an environmentally significant mechanism for intrinsic bioremediation of vinyl chloride in anaerobic ground-water systems.

Journal of Contaminant Hydrology

Geochemistry of the northern Atlantic Coastal Plain aquifer system

Sediments of the northern Atlantic Coastal Plain comprise a complex multiaquifer flow system. On a large scale (greater than 500 square miles) ground water in this system evolves from predominantly calcium magnesium bicarbonate water with a low dissolved-solids content and low pH, near outcrop-recharge areas, to predominantly sodium bicarbonate water with a high-dissolved solids content and high pH, downgradient. This sodium bicarbonate water then grades into a sodium chloride water. This large-scale predictable progression of hydrochemical facies results from the summation of many smaller scale geochemical processes that chiefly depend on the sedimentary depositional environments of the aquifers.

Northern Atlantic coastal plain

Lack of correlation between organic acid concentrations and predominant electron-accepting processes in a contaminated aquifer

Long-term (1992-1995) monitoring data from a petroleum hydrocarbon- contaminated aquifer were used to examine the hypothesis that concentrations of low molecular weight (LMW) aliphatic organic acids reflect terminal electron-accepting processes. During the period of study, concentrations of dissolved hydrogen (H2) indicated that methanogenic, sulfate-reducing, and iron(III)-reducing conditions predominated at the site. However, there was no correlation between LMW organic acid concentrations and concentrations of dissolved H2. These results indicate that organic acid concentrations are not a reliable indicator of local redox conditions at this site.

Environmental Science & Technology