Geochemical heterogeneity of a gasoline-contaminated aquifer

Cozzarelli, Isabelle M.; Herman, Janet S.; Baedecker, Mary Jo; Fischer, Jeffrey M.

doi:10.1016/s0169-7722(99)00050-9

Cited by 65 publications

(28 citation statements)

References 35 publications

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“…In contrast, both synthetic and natural crystalline Fe(III) oxides, which are poorly dissolved in NH 2 OH-HCl or dilute HCl, were found to undergo much lower degrees of reduction, and to be preserved in highly reducing (methanogenic) sediments Phillips et al, 1993). Subsequent studies of microbial Fe(III) oxide reduction in a variety of surface and subsurface sediments have verified the potential for near complete reduction of amorphous Fe(III) oxides, and for the preservation of substantial quantities of crystalline Fe(III) oxides (Albrechtsen et al, 1995;Amirbahman et al, 1998;Cozzarelli et al, 1999Cozzarelli et al, , 2000Roden and Wetzel, 1996;Roden and Edmonds, 1997;Tuccillo et al, 1999;Wallmann et al, 1993).…”

Section: Fe(iii) Oxide Mineralogy and Microbial Reducibilitymentioning

confidence: 96%

Microbiological Controls on Geochemical Kinetics 1: Fundamentals and Case Study on Microbial Fe(III) Oxide Reduction

Roden¹

2008

Kinetics of Water-Rock Interaction

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Section: Fe(iii) Oxide Mineralogy and Microbial Reducibilitymentioning

confidence: 96%

Microbiological Controls on Geochemical Kinetics 1: Fundamentals and Case Study on Microbial Fe(III) Oxide Reduction

Roden¹

2008

Kinetics of Water-Rock Interaction

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“…Indeed, substantial concentrations of solid-phase Fe(II) are commonly present in circumneutral anaerobic aquifer sediments contaminated with hydrocarbons or land-ll leachate Baedecker et al 1992;Heron et al 1994b;Albrechtsen et al 1995;Heron and Christensen 1995;Amirbahman et al 1998;Anderson et al 1998;Ludvigsen et al 1998;Cozzarelli et al 1999;Tuccillo et al 1999;Cozzarelli et al 2000) as well as naturally reducing subsurface sediments (McKinley et al 1997;Jakobsen and Postma 1999). These considerations suggest that, from a mechanistic point of view, it is not appropriate to model competitive interactions between Fe(III) oxide reduction and other TEAPs based on the thermodynamic properties of the oxide minerals.…”

Section: Summary and Environmental Implicationsmentioning

confidence: 99%

Influence of Biogenic Fe(II) on Bacterial Crystalline Fe(III) Oxide Reduction

Roden¹,

Urrutia²

2002

Geomicrobiology Journal

224

166

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Bacterial crystalline Fe(III) oxide reduction has the potential to signi cantly in uence the biogeochemistry of anaerobic sedimentary environments where crystalline Fe(III) oxides are abundan t relative to poorly crystalline (amorphous ) phases. A review of published data on solid-phase Fe(III) abundanc e and speciation indicates that crystalline Fe(III) oxides are frequently 2-to¸10-fold more abundan t than amorphous Fe(III) oxides in shallow subsurface sediments not yet subjected to microbial Fe(III) oxide reduction activity. Incubation experiments with coastal plain aquifer sediments demonstrated that crystalline Fe(III) oxide reduction can contribute substantially to Fe(II) production in the presence of added electron donors and nutrients. Controls on crystalline Fe(III) oxide reduction are therefore an important consideration in relation to the biogeochemical impacts of bacterial Fe(III) oxide reduction in subsurface environments. In this paper, the in uence of biogenic Fe(II) on bacterial reduction of crystalline Fe(III) oxides is reviewed and analyzed in light of new experiments conducted with the acetate-oxidizing, Fe(III)-reducing bacterium (FeRB) Geobacter metallireducens. Previous experiments with Shewanella algae strain BrY indicated that adsorption and/or surface precipitation of Fe(II) on Fe(III) oxide and FeRB cell surfaces is primarily responsible for cessation of goethite (®-FeOOH) reduction activity after only a relatively small fraction (generally <10%) of the oxide is reduced. Similar conclusions are drawn from analogous studies with G: metallireducens. Although accumulation of aqueous Fe(II) has the potential to impose thermodynamic constraints on the extent of crystalline Fe(III) oxide reduction, our data on bacterial goethite reduction suggest that this phenomenon cannot universally explain the low microbial reducibility of this mineral. Experiments examining the in uence of exogenous Fe(II) (20 mM FeCl 2 ) on soluble Fe(III)-citrate reduction by G: metallireducens and S: algae showed that high concentrations of Fe(II) did not inhibit Fe(III)-citrate reduction by freshly grown cells, which indicates that surface-bound Fe(II) does not inhibit Fe(III) reduction through a classical end-product enzyme inhibition mechanism. However, prolonged exposure of G: metallireducens and S: algae cells to high concentrations of soluble Fe(II) did cause inhibition of soluble Fe(III) reduction. These ndings, together with recent documentation of the formation of Fe(II) surface precipitates on FeRB in Fe(III)-citrate medium, provide further evidence for the impact of Fe(II) sorption by FeRB on enzymatic Fe(III) reduction. Two different, but not mutually exclusive, mechanisms whereby accumulation of Fe(II) coatings on Fe(III) oxide and FeRB surfaces may lead to inhibition of enzymatic Fe(III) oxide reduction activity (in the absence of soluble electron shuttles and/or Fe(III) chelators) are identi ed and discussed in relation to recent experimental work and theoretical considerations.

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“…However, although there may clearly be a relation between attenuation and permeability, it is highly uncertain how and how strongly attenuation rates are correlated with K. Not even the sign of correlation can be determined a priori. The scientific literature contains empirical evidence and theoretical arguments for both negative and positive correlation (Cvetkovic and Shapiro, 1990;Destouni and Cvetkovic, 1991;Cozzarelli et al, 1999;Cunningham and Fadel, 2007;Jardine, 2008). An objective of the present study, along with the development of the scenario analysis approach, is therefore to investigate how, and how much hydrological solute mass transport through and from a catchment is affected by the complexity and uncertainty associated with the variability and possible cross-correlation of physical mass transport and biogeochemical mass attenuation.…”

Section: Introductionmentioning

confidence: 99%

Diffuse hydrological mass transport through catchments: scenario analysis of coupled physical and biogeochemical uncertainty effects

Persson

Jarsjö

2011

Hydrol. Earth Syst. Sci.

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Abstract. This paper quantifies and maps the effects of coupled physical and biogeochemical variability on diffuse hydrological mass transport through and from catchments. It further develops a scenario analysis approach and investigates its applicability for handling uncertainties about both physical and biogeochemical variability and their different possible cross-correlation. The approach enables identification of conservative assumptions, uncertainty ranges, as well as pollutant/nutrient release locations and situations for which further investigations are most needed in order to reduce the most important uncertainty effects. The present scenario results provide different statistical and geographic distributions of advective travel times for diffuse hydrological mass transport. The geographic mapping can be used to identify potential hotspot areas with large mass loading to downstream surface and coastal waters, as well as their opposite, potential lowest-impact areas within the catchment. Results for alternative travel time distributions show that neglect or underestimation of the physical advection variability, and in particular of those transport pathways with much shorter than average advective solute travel times, can lead to substantial underestimation of pollutant and nutrient loads to downstream surface and coastal waters. This is particularly true for relatively high catchment-characteristic product of average attenuation rate and average advective travel time, for which mass delivery would be near zero under assumed transport homogeneity but can be orders of magnitude higher for variable transport conditions. A scenario of high advection variability, with a significant fraction of relatively short travel times, combined with a relevant average Correspondence to: K. Persson (klas.persson@natgeo.su.se) biogeochemical mass attenuation rate, emerges consistently from the present results as a generally reasonable, conservative assumption for estimating maximum diffuse mass loading, when the prevailing physical and biogeochemical variability and cross-correlation are uncertain.

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Geochemical heterogeneity of a gasoline-contaminated aquifer

Cited by 65 publications

References 35 publications

Microbiological Controls on Geochemical Kinetics 1: Fundamentals and Case Study on Microbial Fe(III) Oxide Reduction

Microbiological Controls on Geochemical Kinetics 1: Fundamentals and Case Study on Microbial Fe(III) Oxide Reduction

Influence of Biogenic Fe(II) on Bacterial Crystalline Fe(III) Oxide Reduction

Diffuse hydrological mass transport through catchments: scenario analysis of coupled physical and biogeochemical uncertainty effects

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