Mechanism of the bacterial reduction of sulphate from isotope fractionation studies

Harrison, A. G.; Thode, H. G.

doi:10.1039/tf9585400084

Cited by 430 publications

(299 citation statements)

References 3 publications

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confidence: 72%

“…These values indicate that the abstraction of H from methane by methane monooxygenase is associated with little to no reversibility (see discussion in § 4.4.1.2). This interpretation is consistent with the strong energetic favorability of methane oxidation to methanol and downstream products in the presence of abundant O 2 , a strong electron acceptor (Cicerone and Oremland, 1988;Hanson and Hanson, 1996).The new experimental constraints on clumped isotopologue fractionation during aerobic methane oxidation also afford an opportunity to briefly evaluate whether aerobic methane oxidation has influenced methane clumped isotopologue data available in the literature from various environments. In particular, because methane oxidation demonstrably produces nonequilibrium clumped isotopologue signatures in 89 Chapter 4.…”

supporting

confidence: 72%

“…This organism uses the enzymes soluble methane monooxygenase (sMMO) and particulate methane monooxygenase (pMMO) to oxidize methane to methanol, which is further oxidized to CO 2 as an end product (Hanson and Hanson, 1996). Carbon derived from methane can also be assimilated into cellular biomass.…”

Section: Introductionmentioning

confidence: 99%

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The geochemistry of methane isotopologues

Wang¹

2017

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This thesis documents the origin, distribution, and fate of methane and several of its isotopic forms on Earth. Using observational, experimental, and theoretical approaches, I illustrate how the relative abundances of 12 CH 4 , 13 CH 4 , 12 CH 3 D, and 13 CH 3 D record the formation, transport, and breakdown of methane in selected settings.Chapter 2 reports precise determinations of 13 CH 3 D, a "clumped" isotopologue of methane, in samples collected from various settings representing many of the major sources and reservoirs of methane on Earth. The results show that the information encoded by the abundance of 13 CH 3 D enables differentiation of methane generated by microbial, thermogenic, and abiogenic processes. A strong correlation between clumped-and hydrogen-isotope signatures in microbial methane is identified and quantitatively linked to the availability of H 2 and the reversibility of microbially-mediated methanogenesis in the environment. Determination of 13 CH 3 D in combination with hydrogen-isotope ratios of methane and water provides a sensitive indicator of the extent of C-H bond equilibration, enables fingerprinting of methane-generating mechanisms, and in some cases, supplies direct constraints for locating the waters from which migrated gases were sourced. Chapter 3 applies this concept to constrain the origin of methane in hydrothermal fluids from sediment-poor vent fields hosted in mafic and ultramafic rocks on slow-and ultraslow-spreading mid-ocean ridges. The data support a hypogene model whereby methane forms abiotically within plutonic rocks of the oceanic crust at temperatures above ca. 300• C during respeciation of magmatic volatiles, and is subsequently extracted during active, convective hydrothermal circulation. Chapter 4 presents the results of culture experiments in which methane is oxidized in the presence of O 2 by the bacterium Methylococcus capsulatus strain Bath. The results show that the clumped isotopologue abundances of partially-oxidized methane can be predicted from knowledge of 13 C/ 12 C and D/H isotope fractionation factors alone.: Shuhei Ono, Ph.D. Acknowledgments I fear that this section will not do justice to the people I have not the space to thank individually. Alas, here goes. To those whose names are not specifically listed here, thank you too. I wish first to thank Shuhei Ono. The work this thesis represents could not have happened without his bold vision and the license to explore and question that working in his lab afforded. His unbridled optimism, breadth of scientific curiosity, personal integrity, and accessibility to his personnel are traits I one day hope to emulate. I thank him for his nonjudgmental yet appropriately measured support of many of my ideas-even those that led nowhere-, for believing in me even when I found it difficult to do so myself, and for teaching me to change pump oil, build vacuum lines, and drink Icelandic vodka.I also wish to thank my thesis committee members Jeff Seewald, Roger Summons, and John Pohlman, for their in...

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supporting

confidence: 72%

supporting

confidence: 72%

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The geochemistry of methane isotopologues

Wang¹

2017

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“…This assumption may not always apply because a decrease in sulfate concentration likely minimizes the isotopic fractionation of microbial sulfate reduction and may therefore alter the a SR value. On the basis of the previous experiments, almost no fractionation was observed when the sulfate concentration was below 200 mmol L 21 (Harrison and Thode 1958;Habicht et al 2005). For the natural population of sulfate reducers, the average fractionation is not more than 0.7% 6 5.2% at sulfate concentrations lower than 50 mmol L 21 (Habicht et al 2002).…”

Section: Discussionmentioning

confidence: 97%

Seasonal change in microbial sulfur cycling in monomictic Lake Fukami‐ike, Japan

Nakagawa

Ueno

Hattori

et al. 2012

Limnology & Oceanography

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Sulfur budgets and seasonal progression of sulfur cycling processes were investigated in Lake Fukami-ike, a small monomictic lake in Japan. The sulfur isotopic mass balance shows that the main sulfur source is groundwater inflow (d 34 S 5 215.0%). The sulfate influx is approximately 20% reduced by microbial sulfate reduction and deposited as sulfide (d 34 S 5 222.2%; 34 kmol yr 21 ); the remaining exits from the outflow channel (d 34 S 5 212.6%). In the water column, microbiological analyses reveal that green sulfur bacteria dominate more than 90% of the population in the anoxic layer. A monthly decrease in sulfate concentration at each depth indicates that sulfate reduction proceeds within the water column as a first-order reaction because of low sulfate concentration (, 600 mmol L 21 ). The isotopic fractionation factor of sulfate reduction is estimated to be 0.980 by the isotopic and concentration data of sulfate and sulfide from April to August. Numerical simulation indicates that the relative contribution of phototrophic sulfide oxidation is over 50 times slower than sulfate reduction from April to August but over two times higher from October to November because of lower sulfate conditions (, 300 mmol L 21 ). Sulfate concentration is the factor for controlling the relative contribution of sulfate reduction and phototrophic sulfide oxidation in monomictic lakes, which contrasts with that observed in permanently stratified lakes.

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“…When they reduce sulfate, the bacteria prefer 32S1604 rather than 32S160 3 1802 (LLOYD, 1968;MIZUTANI and RAFTER, 1969b) and 34504 (HARRISON and THODE, 1958), resulting in the significant enrichment of the heavy isotopes of sulfur and oxygen in the remaining sulfate in solution. If the residual sulfates (remaining in solution) after considerable bacterial reduction were involved in the diagenesis of the gypsum ores, the gypsum would exhibit variably heavy sulfur and oxygen isotopic values.…”

Section: Resultsmentioning

confidence: 99%

Sulfur and oxygen isotopic geochemistry of sulfate in the black ore deposits of Japan

1970

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Abstract-The sulfur isotopic values of barite, gypsum and anhydrite from the typical strata-bound submarine ore deposits (black ore deposits) of Miocene age in Japan have a narrow range of +21 to 24%o with respect to the meteoritic sulfur. However, the oxygen isotopic values (in SMOW) vary from +5 to +19%o and have a general tendency to increase in the order : barite < anhydrite -alabaster < secondary gypsum (satin spar and selenite). The sulfate minerals from the late Paleozoic cupriferrous iron sulfide ore deposits of the Yanahara and Besshi mines are similar in the sulfur isotopic values (+11 to +15%o) to inferred Permian sea water sulfate, whereas the oxygen isotopic values have a wide range of variation.The observed sulfur isotopic pattern is most likely due to a submarine hydrothermal system in which sulfate of marine origin (connate or actual sea water) predominated over other sources of sulfur. The variable oxygen isotopic data of sulfate are explained by the oxygen isotopic exchange between sulfate and water during depositional and post-depo sitional processes. The sulfur and oxygen isotopic ratios of "hot sulfate" in the Wairakei and the Red Sea geothermal brines are consistent with this idea.The sulfates in secor dary gypsum ores in the Noto mine are enriched in both 34Sand 180, suggesting that the alteration of the primary ores in this mine may have taken place under the influence of sulfate-reducing bacteria.

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Mechanism of the bacterial reduction of sulphate from isotope fractionation studies

Cited by 430 publications

References 3 publications

The geochemistry of methane isotopologues

The geochemistry of methane isotopologues

Seasonal change in microbial sulfur cycling in monomictic Lake Fukami‐ike, Japan

Sulfur and oxygen isotopic geochemistry of sulfate in the black ore deposits of Japan

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