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Bouchard, Daniel

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Bouchard, Daniel
Affiliation principale
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https://libra.unine.ch/handle/123456789/30594

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  • Publication
    Accès libre
    Documentation of time-scales for onset of natural attenuation in an aquifer treated by a crude-oil recovery system
    (2015-4)
    Ponsin, Violaine
    ;
    Maier, Joachim
    ;
    Guelorget, Yves
    ;
    Hunkeler, Daniel 
    ;
    Bouchard, Daniel 
    ;
    Villavicencio, Hakeline
    ;
    Höhener, Patrick
    A pipeline transporting crude-oil broke in a nature reserve in 2009 and spilled 5100 m3 of oil that partly reached the aquifer and formed progressively a floating oil lens. Groundwater monitoring started immediately after the spill and crude-oil recovery by dual pump-and-skim technology was operated after oil lens formation. This study aimed at documenting the implementation of redox-specific natural attenuation processes in the saturated zone and at assessing whether dissolved compounds were degraded. Seven targeted water sampling campaigns were done during four years in addition to a routine monitoring of hydrocarbon concentrations. Liquid oil reached the aquifer within 2.5 months, and anaerobic processes, from denitrification to reduction of sulfate, were observable after 8 months. Methanogenesis appeared on site after 28 months. Stable carbon isotope analyses after 16 months showed maximum shifts in δ13C of + 4.9 ± 0.22‰ for toluene, + 2.4 ± 0.19‰ for benzene and + 0.9 ± 0.51‰ for ethylbenzene, suggesting anaerobic degradation of these compounds in the source zone. Estimations of fluxes of inorganic carbon produced by biodegradation revealed that, in average, 60% of inorganic carbon production was attributable to sulfate reduction. This percentage tended to decrease with time while the production of carbon attributable to methanogenesis was increasing. Within the investigation time frame, mass balance estimations showed that biodegradation is a more efficient process for control of dissolved concentrations compared to pumping and filtration on an activated charcoal filter.
  • Publication
    Accès libre
    Carbon Isotope Fractionation during Diffusion and Biodegradation of Petroleum Hydrocarbons in the Unsaturated Zone: Field Experiment at Værløse Airbase, Denmark, and Modeling
    (2008)
    Bouchard, Daniel 
    ;
    Hunkeler, Daniel 
    ;
    Gaganis, Petros
    ;
    Aravena, Ramon
    ;
    Höhener, Patrick
    ;
    Broholm, Mette M.
    A field experiment was conducted in Denmark in order to evaluate the fate of 13 volatile organic compounds (VOCs) that were buried as an artificial fuel source in the unsaturated zone. Compound-specific isotope analysis showed distinct phases in the 13C/12C ratio evolution in VOC vapors within 3 m from the source over 114 days. At day 3 and to a lesser extent at day 6, the compounds were depleted in 13C by up to −5.7‰ with increasing distance from the source compared to the initial source values. This trend can be explained by faster outward diffusion of the molecules with 12C only compared to molecules with a 13C. Then, the isotope profile leveled out, and several compounds started to become enriched in 13C by up to 9.5‰ with increasing distance from the source, due to preferential removal of the molecules with 12C only, through biodegradation. Finally, as the amount of a compound diminished in the source, a 13C enrichment was also observed close to the source. The magnitude of isotope fractionation tended to be larger the smaller the mass of the molecule was. This study demonstrates that, in the unsaturated zone, carbon isotope ratios of hydrocarbons are affected by gas-phase diffusion in addition to biodegradation, which was confirmed using a numerical model. Gas-phase diffusion led to shifts in δ13C >1‰ during the initial days after the spill, and again during the final stages of source volatilization after >75% of a compound had been removed. In between, diffusion has less of an effect, and thus isotope data can be used as an indicator for hydrocarbon biodegradation.
  • Publication
    Accès libre
    Carbon Isotope Fractionation During Volatilization of Petroleum Hydrocarbons and Diffusion Across a Porous Medium: A Column Experiment
    (2008)
    Bouchard, Daniel 
    ;
    Höhener, Patrick
    ;
    Hunkeler, Daniel 
    The study focuses on the effect of volatilization, diffusion, and biodegradation on the isotope evolution of volatile organic compounds (VOCs) in a 1.06 m long column filled with alluvial sand. A liquid mixture of 10 VOCs was placed at one end of the column, and measurements of VOC vapor concentrations and compound-specific isotope ratios (δ13C) were performed at the source and along the column. Initially, the compounds became depleted in 13C by up to −4.8‰ along the column axis, until at 26 h, uniform isotope profiles were observed for most compounds, which is expected for steady-state diffusion. Subsequently, several compounds (n-pentane, benzene, n-hexane) became enriched in 13C throughout the column. For the same compounds, a significant decrease in the source vapor concentration and a gradual enrichment of 13C by up to 5.3‰ at the source over a period of 336 h was observed. This trend can be explained by a larger diffusive mass flux for molecules with light isotopes compared to those with a heavy isotope, which leads to a depletion of light isotopes in the source. The isotope evolution of the source followed closely a Rayleigh trend and the obtained isotope enrichment factor corresponded well to the ratio between the diffusion coefficients for heavy and light molecules as expected based on theory. In contrast to diffusion, biodegradation had generally only a small effect on the isotope profiles, which is expected because in a diffusion-controlled system the isotope shift per decrease of mass flux is smaller than in an advection-controlled system. These findings open interesting perspectives for monitoring source depletion with isotope and have implications for assessing biodegradation and source variability in the unsaturated zone based on isotopes.