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Can microbially-generated hydrogen sulfide account for the rates of U(VI) reduction by a sulfate-reducing bacterium?

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Abstract

In situ remediation of uranium contaminated soil and groundwater is attractive because a diverse range of microbial and abiotic processes reduce soluble and mobile U(VI) to sparingly soluble and immobile U(IV). Often these processes are linked. Sulfate-reducing bacteria (SRB), for example, enzymatically reduce U(VI) to U(IV), but they also produce hydrogen sulfide that can itself reduce U(VI). This study evaluated the relative importance of these processes for Desulfovibrio aerotolerans, a SRB isolated from a U(VI)-contaminated site. For the conditions evaluated, the observed rate of SRB-mediated U(VI) reduction can be explained by the abiotic reaction of U(VI) with the microbially-generated H2S. The presence of trace ferrous iron appeared to enhance the extent of hydrogen sulfide-mediated U(VI) reduction at 5 mM bicarbonate, but had no clear effect at 15 mM. During the hydrogen sulfide-mediated reduction of U(VI), a floc formed containing uranium and sulfur. U(VI) sequestered in the floc was not available for further reduction.

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Abbreviations

A predicted :

Acetate concentration predicted from the stoichiometric ratio of acetate production to ethanol consumption (mM)

A 0 :

Acetate concentration at the initial time (mM)

C :

Covariance matrix

f aq :

Fraction of mole of hydrogen sulfide in the aqueous phase

f aq,i−1 :

Fraction of mole of hydrogen sulfide in the aqueous phase on day i − 1

f g :

Fraction of mole of hydrogen sulfide in the gas phase

\( f_{{{\text{H}}_{ 2} {\text{S,aq}}}} \) :

Fraction of mole of H2S in the total mole of hydrogen sulfide in the aqueous phase = \( \frac{{{\text{H}}_{ 2} {\text{S}}_{{(\rm{aq})}} }}{{\text{H}}_{2} {\text{S}}_{(\rm{aq})} + {\text{HS}}^{-}_{(\rm{aq})}}\)

J :

Jacobian matrix

k :

Pseudo second-order rate constant for ethanol utilization (l/mg protein/day)

k H :

Henry’s law constant (atm/mol fraction)

M T :

Total mole of hydrogen sulfide in a serum bottle (mmol)

n :

Number of data points for uranium measurements

p :

Number of fitting parameters for uranium reduction kinetics

R :

Gas constant = 0.08206 \( \left({\frac{{{\text{l}} \cdot {\text{atm}}}}{{\text{mol}} \cdot {\text{K}}}} \right)\)

r A :

Stoichiometric ratio of acetate production to ethanol consumption

r sulfide :

Stoichiometric ratio of hydrogen sulfide production to ethanol consumption

S :

Ethanol concentration (mM)

S measured :

Measured ethanol concentration (mM)

S 0 :

Ethanol concentration at the initial time (mM)

S predicted :

Ethanol concentration predicted from a kinetic model (mM)

S p,mol,i−1 :

Mol of ethanol in a serum bottle on day i − 1 predicted from a kinetic model and accounted for the ethanol loss due to sampling effect (mmol)

S p,mol,i :

Mol of ethanol in a serum bottle on day i predicted from a kinetic model (mmol)

SSreg :

Sum of the squared errors of the measured values from the values predicted by a model

SStot :

Sum of the squared errors of the measured values from the mean of all measured values

Sulfide p,i :

Mole of hydrogen sulfide in a serum bottle predicted from the stoichiometric ratio of hydrogen sulfide production to ethanol consumption on day i (mmol)

Sulfide p,i−1 :

Mole of hydrogen sulfide in a serum bottle predicted from the stoichiometric ratio of hydrogen sulfide production to ethanol consumption on day i−1 (mmol)

t :

Time (d)

T :

Absolute temperature (K)

U(VI)in :

Initial concentration of U(VI) (μM)

X :

Protein concentration as proxy of biomass concentration (mg protein/l)

X −1 :

Inverse of matrix X

X T :

Transpose of matrix X

Y :

Biomass yield on ethanol (g protein/mol ethanol)

σs 2 :

Mean square fitting error for improved estimate of measured ethanol data ((mM)2)

\( \rho_{\text{w}} \) :

Density of water (kg/m3)

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Acknowledgments

This work was funded by the Environmental Remediation Science Program (ERSP), U.S. Department of Energy, under grant number DOEAC05-00OR22725. We thank two anonymous reviewers for thoughtful reviews and recommendations that significantly improved the manuscript.

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Correspondence to Craig S. Criddle.

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Boonchayaanant, B., Gu, B., Wang, W. et al. Can microbially-generated hydrogen sulfide account for the rates of U(VI) reduction by a sulfate-reducing bacterium?. Biodegradation 21, 81–95 (2010). https://doi.org/10.1007/s10532-009-9283-x

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  • DOI: https://doi.org/10.1007/s10532-009-9283-x

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