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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

Analytical method for optimal source reduction with monitored natural attenuation in contaminated aquifers

A method is developed for optimizing monitored natural attenuation (MNA) and the reduction in the aqueous source zone concentration (??C) required to meet a site-specific regulatory target concentration. The mathematical model consists of two one-dimensional equations of mass balance for the aqueous phase contaminant, to coincide with up to two distinct zones of transformation, and appropriate boundary and intermediate conditions. The solution is written in terms of zone-dependent Peclet and Damko??hler numbers. The model is illustrated at a chlorinated solvent site where MNA was implemented following source treatment using in-situ chemical oxidation. The results demonstrate that by not taking into account a variable natural attenuation capacity (NAC), a lower target ??C is predicted, resulting in unnecessary source concentration reduction and cost with little benefit to achieving site-specific remediation goals.

Conference Paper↗

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↗

A hydrogen-based subsurface microbial community dominated by methanogens

The search for extraterrestrial life may be facilitated if ecosystems can be found on Earth that exist under conditions analogous to those present on other planets or moons. It has been proposed, on the basis of geochemical and thermodynamic considerations, that geologically derived hydrogen might support subsurface microbial communities on Mars and Europa in which methanogens form the base of the ecosystem1-5. Here we describe a unique subsurface microbial community in which hydrogen-consuming, methane-producing Archaea far outnumber the Bacteria. More than 90% of the 16s ribosomal DNA sequences recovered from hydrothermal waters circulating through deeply buried igneous rocks in Idaho are related to hydrogen-using methanogenic microorganisms. Geochemical characterization indicates that geothermal hydrogen, not organic carbon, is the primary energy source for this methanogen-dominated microbial community. These results demonstrate that hydrogen-based methanogenic communities do occur in Earth's subsurface, providing an analogue for possible subsurface microbial ecosystems on other planets.

Nature↗

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↗

Methyl t-Butyl Ether Mineralization in Surface-Water Sediment Microcosms under Denitrifying Conditions

Mineralization of [U-14C] methyl t-butyl ether (MTBE) to 14CO2 without accumulation of t-butyl alcohol (TBA) was observed in surface-water sediment microcosms under denitrifying conditions. Methanogenic activity and limited transformation of MTBE to TBA were observed in the absence of denitrification. Results indicate that bed sediment microorganisms can effectively degrade MTBE to nontoxic products under denitrifying conditions.

Applied and Environmental Microbiology↗

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

To evaluate the potential contribution of in situ biodegradation as a mechanism for natural attenuation of MTBE in surface water, surface water sediments were collected from streams and lakes at 11 sites throughout the US and the ability of the indigenous microorganisms to mineralize [U-14C] MTBE to 14CO2 under aerobic conditions was examined. 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. The microorganisms, which inhabit the bed sediments of streams and lakes could degrade MTBE efficiently and this capability is widespread in the environment. 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. 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.

Conference Paper↗

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↗

Acetogenic microbial degradation of vinyl chloride

Under methanogenic conditions, microbial degradation of [1,2- 14 C]vinyl chloride (VC) resulted in significant (14 ± 3% maximum recovery) but transient recovery of radioactivity as 14 C-acetate. Subsequently, 14 C-acetate was degraded to 14 CH 4 and 14 CO 2 (18 ± 2% and 54 ± 3% final recoveries, respectively). In contrast, under 2-bromoethanesulfonic acid (BES) amended conditions, 14 C-acetate recovery remained high (27 ± 1% maximum recovery) throughout the study, no 14 CH 4 was produced, and the final recovery of 14 CO 2 was only 35 ± 4%. These results demonstrate that oxidative acetogenesis may be an important mechanism for anaerobic VC biodegradation. Moreover, these results (1) demonstrate that microbial degradation of VC to CH 4 and CO 2 may involve oxidative acetogenesis followed by acetotrophic methanogenesis and (2) suggest that oxidative acetogenesis may be the initial step in the net oxidation of VC to CO 2 reported previously under Fe(III)-reducing, SO 4 -reducing, and humic acids-reducing conditions.

Environmental Science & Technology↗

The significance of microbial processes in hydrogeology and geochemistry

Microbial processes affect the chemical composition of groundwater and the hydraulic properties of aquifers in both contaminated and pristine groundwater systems. The patterns of water-chemistry changes that occur depend upon the relative abundance of electron donors and electron acceptors. In many pristine aquifers, where microbial metabolism is limited by the availability of electron donors (usually organic matter), dissolved inorganic carbon (DIC) accumulates slowly along aquifer flow paths and available electron acceptors are consumed sequentially in the order dissolved oxygen > nitrate > Fe(III) > sulfate > CO2 (methanogenesis). In aquifers contaminated by anthropogenic contaminants, an excess of available organic carbon often exists, and microbial metabolism is limited by the availability of electron acceptors. In addition to changes in groundwater chemistry, the solid matrix of the aquifer is affected by microbial processes. The production of carbon dioxide and organic acids can lead to increased mineral solubility, which can lead to the development of secondary porosity and permeability. Conversely, microbial production of carbonate, ferrous iron, and sulfide can result in the precipitation of secondary calcite or pyrite cements that reduce primary porosity and permeability in groundwater systems.

Hydrogeology Journal↗

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↗