Hydrogen Isotopic Composition of Individual <i>n</i>-Alkanes as an Intrinsic Tracer for Bioremediation and Source Identification of Petroleum Contamination

Pond, Kristy L.; Huang, Yongsong; Wang, Yi; Kulpa, Charles F.

doi:10.1021/es011140r

Cited by 90 publications

(53 citation statements)

References 20 publications

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“…Fractionations associated with aerobic biodegradation of alkanes have been studied at the molecular level by Pond et al (2002). Short n-alkanes (n-C 14 to n-C 18 ) biodegrade quickly with a ∼12‰ to 25‰ D-enrichment in residual alkanes, whereas longer n-alkanes biodegrade more slowly and are fractionated by <5‰ (Pond et al 2002).…”

Section: Biodegradation and Early Diagenesismentioning

confidence: 99%

“…Short n-alkanes (n-C 14 to n-C 18 ) biodegrade quickly with a ∼12‰ to 25‰ D-enrichment in residual alkanes, whereas longer n-alkanes biodegrade more slowly and are fractionated by <5‰ (Pond et al 2002). Biodegradation of petroleum under anaerobic conditions (e.g., within oil reservoirs) has not been reported to cause significant D/H fractionation at the bulk level (e.g., Schoell & Redding 1978, dos Santos Neto & Hayes 1999, although a ∼35‰ Denrichment in n-alkanes was recently reported for severely biodegraded petroleums (Sun et al 2005).…”

Section: Biodegradation and Early Diagenesismentioning

confidence: 99%

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Hydrogen Isotopic (D/H) Composition of Organic Matter During Diagenesis and Thermal Maturation

Schimmelmann

Sessions

Mastalerz

2006

Annu. Rev. Earth Planet. Sci.

264

165

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Changes in the D/H ratio of sedimentary organic matter (SOM) during thermal maturation have been difficult to interpret because the effects of hydrogen exchange and kinetic fractionations are confounded in natural samples. Recent analytical developments have significantly improved our understanding of the responsible mechanisms. In this paper, we review experimental and field data that document a progressive increase in the D/H ratio of most organic hydrogen at the bulk and molecular levels, and suggest that the transfer of hydrogen from water to organic matter is the most important mechanism leading to those changes. SOM and water in natural petroleum systems approach a pseudoequilibrium D/H fractionation of about −80 to −110‰. D/H ratios of organic hydrogen can preserve quantitative information about paleoclimate throughout diagenesis, and some qualitative information through catagenesis.

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Section: Biodegradation and Early Diagenesismentioning

confidence: 99%

Section: Biodegradation and Early Diagenesismentioning

confidence: 99%

Hydrogen Isotopic (D/H) Composition of Organic Matter During Diagenesis and Thermal Maturation

Schimmelmann

Sessions

Mastalerz

2006

Annu. Rev. Earth Planet. Sci.

264

165

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“…T he hydrogen-isotopic composition ( 2 H/ 1 H or D/H ratio, commonly expressed as a ␦D value) of lipids is being explored by scientists with diverse interests, including the origins of natural products (1,2), biogeochemical cycles (3), petroleum systems (4), and paleoclimate (5-7). Because the D/H ratios of lipids are generally conserved over Ϸ10 6 -year time scales (8), they are a potentially useful tracer of biogeochemical pathways and processes in the environment.…”

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confidence: 99%

Large D/H variations in bacterial lipids reflect central metabolic pathways

Zhang¹,

Gillespie

Sessions

2009

Proc. Natl. Acad. Sci. U.S.A.

196

268

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Large hydrogen-isotopic (D/H) fractionations between lipids and growth water have been observed in most organisms studied to date. These fractionations are generally attributed to isotope effects in the biosynthesis of lipids, and are frequently assumed to be approximately constant for the purpose of reconstructing climatic variables. Here, we report D/H fractionations between lipids and water in 4 cultured members of the phylum Proteobacteria, and show that they can vary by up to 500‰ in a single organism. The variation cannot be attributed to lipid biosynthesis as there is no significant change in these pathways between cultures, nor can it be attributed to changing substrate D/H ratios. More importantly, lipid/water D/H fractionations vary systematically with metabolism: chemoautotrophic growth (approximately ؊200 to ؊400‰), photoautotrophic growth (؊150 to ؊250‰), heterotrophic growth on sugars (0 to ؊150‰), and heterotrophic growth on TCA-cycle precursors and intermediates (؊50 to ؉200‰) all yield different fractionations. We hypothesize that the D/H ratios of lipids are controlled largely by those of NADPH used for biosynthesis, rather than by isotope effects within the lipid biosynthetic pathway itself. Our results suggest that different central metabolic pathways yield NADPH-and indirectly lipids-with characteristic isotopic compositions. If so, lipid ␦D values could become an important biogeochemical tool for linking lipids to energy metabolism, and would yield information that is highly complementary to that provided by 13 C about pathways of carbon fixation.fatty acids ͉ fractionation ͉ metabolism ͉ hydrogen isotopes T he hydrogen-isotopic composition ( 2 H/ 1 H or D/H ratio, commonly expressed as a ␦D value) of lipids is being explored by scientists with diverse interests, including the origins of natural products (1, 2), biogeochemical cycles (3), petroleum systems (4), and paleoclimate (5-7). Because the D/H ratios of lipids are generally conserved over Ϸ10 6 -year time scales (8), they are a potentially useful tracer of biogeochemical pathways and processes in the environment. Most research to date has focused on higher plants, in which environmental water is the sole source of external hydrogen and consequently provides primary control over the D/H ratio of biosynthesized lipids (9). Although ␦D values for plant lipids and environmental water are generally well correlated, they are also substantially offset from each other. The biochemical basis for this lipid/water fractionation is not well understood. It is generally assumed to arise from a combination of isotope effects during photosynthesis and the biosynthesis of lipids (9-12), and is often treated as approximately constant to reconstruct isotopic compositions of environmental water as a paleoclimate proxy.There is, however, mounting evidence that the net D/H fractionation between lipids and water can vary by up to 150‰ in plants, even in the same organism (12-16). Modest fractionations associated with fatty acid elongation and desaturation ...

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“…In the context of intrinsic bioremediation, isotopic fractionation of 13 C/ 12 C has been demonstrated repeatedly for toluene Pelz et al, 2001; and first indications concerning an isotopic fractionation of benzene have been presented (Volkering et al, 2001). Also isotopic fractionation of deuterium/hydrogen has been reported Pond et al, 2002). The highest isotope fractionation factors are associated with reducing conditions and the lowest ratios are associated with aerobic and nitratereducing environments.…”

Section: Isotopic Fractionationmentioning

confidence: 94%

Intrinsic Aromatic Hydrocarbon Biodegradation for Groundwater Remediation

Tiehm

Schulze

2003

Oil & Gas Science and Technology - Rev. IFP

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Résumé -Biodégradation intrinsèque des hydrocarbures aromatiques pour la réhabilitation de nappes aquifères -La biodégradation intrinsèque, qui représente le processus clé de l'atténuation naturelle, est de plus en plus couramment envisagée comme une alternative aux procédés plus actifs pour la réhabilitation de sites contaminés. Dans cet article, la biodégradation intrinsèque des BTEX et des HAP est discutée. La première partie passe en revue la compréhension actuelle de la dégradation microbienne des hydrocarbures aromatiques ainsi que les méthodes disponibles pour l'évaluation de la bioréhabilitation intrinsèque. Le concept et les résultats obtenus lors d'une étude de cas sont présentés dans une seconde partie. La biodégradation anaérobie et la biodégradation aérobie contribuent toutes deux à l'élimination des polluants de sites contaminés, comme les anciennes usines à gaz ou les décharges polluées par des huiles de pyrolyse. Les processus de biodégradation intrinsèque engendrent habituellement une suite de zones de redox (méthanogène, sulfatoréductrice, Fe(III)-réductrice, dénitifiante, aérobie) dans le panache des polluants dans l'aquifère en aval de la source de contamination. Les méthodes d'évaluation dans ces différentes zones de redox comprennent l'analyse hydro-et géochimique, la mesure des potentiels redox et la détermination de l'hydrogène. La biodégradation des polluants visés peut être démontrée par la modification des profils de polluant, par le fractionnement isotopique, par des produits spécifiques du métabolisme et par des études en microcosmes sur des échantillons du terrain. Les études en microcosmes constituent un outil particulièrement utile pour identifier les mécanismes de dégradation et pour étudier le rôle d'accepteurs d'électrons spécifiques et des conditions redox. Lors d'une étude de cas, nous avons examiné la biodégradation intrinsèque d'un site pollué par des huiles de pyrolyse. Du fait de la faible capacité de sorption de l'aquifère, la diminution de la concentration en polluant le long du panache d'eau polluée a été majoritairement attribuée à de la biodégradation. La réduction des sulfates et la réduction de Fe(III) étaient les principaux processus redox au coeur du panache d'eau souterraine. Les changements de profil des polluants le long du panache indiquaient l'existence de processus de biodégradation actifs, par exemple, la biodégradation du toluène et du naphtalène dans des zones anaérobies. Dans des microcosmes pollués avec des polluants modèles, la biodégradation du toluène et de l'éthylbenzène a été observée en conditions sulfatoréductrices. La dégradation du toluène, de l'éthylbenzène, du benzène et du naphtalène avait lieu en présence de Fe(III). En conditions aérobies, tous les BTEX et HAP étaient rapidement dégradés.Abstract -Intrinsic Aromatic Hydrocarbon Biodegradation for Groundwater RemediationIntrinsic biodegradation, representing the key process in natural attenuation, is increasingly considered for the remediation of contaminated sites as an alternative to mor...

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Hydrogen Isotopic Composition of Individual n-Alkanes as an Intrinsic Tracer for Bioremediation and Source Identification of Petroleum Contamination

Cited by 90 publications

References 20 publications

Hydrogen Isotopic (D/H) Composition of Organic Matter During Diagenesis and Thermal Maturation

Hydrogen Isotopic (D/H) Composition of Organic Matter During Diagenesis and Thermal Maturation

Large D/H variations in bacterial lipids reflect central metabolic pathways

Intrinsic Aromatic Hydrocarbon Biodegradation for Groundwater Remediation

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