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unknown
Hydrogen isotope exchange between n-alkanes and water under hydrothermal conditions
Authors
Abrajano
Abrajano
+98 more
Allen
Allen
Aubourg
Barker
Bell
Berndt
Boreham
Burruss
Capaccioni
Capaccioni
Charlou
Coplen
Cruse
Eglinton
Eoghan P. Reeves
Fisher
Foustoukos
Foustoukos
Fu
Hagemann
Harbert
Hartshorn
Ho
Hoering
Holm
Horibe
Horita
Hunt
Jeffrey S. Seewald
Johnson
Kadko
Kadko
Knyazev
Konn
Leif
Leif
Lewan
Lewan
Lin
Lippmann
Liu
Liu
McCollom
McCollom
McCollom
McCollom
McCollom
Ni
Nurmi
Onstott
Oremland
Palmer
Proskurowski
Proskurowski
Reynolds
Sachse
Sackett
Schefuss
Schimmelmann
Schimmelmann
Schimmelmann
Schimmelmann
Schmidt
Schoell
Sean P. Sylva
Seewald
Seewald
Seewald
Seewald
Seewald
Seewald
Sessions
Sessions
Sessions
Seyfried
Seyfried
Sherwood
Sherwood Lollar
Sherwood Lollar
Sherwood Lollar
Sherwood Lollar
Sherwood Lollar
Sherwood Lollar
Shock
Shock
Siskin
Surdam
Tang
Tissot
Toulmin
Wang
Wang
Wang
Wang
Ward
Weres
Whiticar
Zhang
Publication date
10 March 2011
Publisher
'Elsevier BV'
Doi
Cite
Abstract
Author Posting. © The Author(s), 2011. This is the author's version of the work. It is posted here by permission of Elsevier B.V. for personal use, not for redistribution. The definitive version was published in Geochimica et Cosmochimica Acta 77 (2012): 582–599, doi:10.1016/j.gca.2011.10.008.To investigate the extent of hydrogen isotope (2H and 1H) exchange between hydrocarbons and water under hydrothermal conditions, we performed experiments heating C1–C5 n-alkanes in aqueous solutions of varying initial 2H/1H ratios in the presence of a pyrite-pyrrhotite-magnetite redox buffer at 323ºC and 35–36MPa. Extensive and reversible incorporation of water-derived hydrogen into C2–C5 n-alkanes was observed on timescales of months. In contrast, comparatively minor exchange was observed for CH4. Isotopic exchange is facilitated by reversible equilibration of n-alkanes and their corresponding n-alkenes with H2 derived from the disproportionation of water. Rates of δ2H variation in C3+ n-alkanes decreased with time, a trend that is consistent with an asymptotic approach to steady-state isotopic compositions regulated by alkane-water isotopic equilibrium. Substantially slower δ2H variation was observed for ethane relative to C3–C5 n-alkanes, suggesting that the greater stability of C3+ alkenes and isomerization reactions may dramatically enhance rates of 2H/1H exchange in C3+ n-alkanes. Thus, in reducing aqueous environments, reversible reaction of alkenes and their corresponding alkanes facilitates rapid 2H/1H exchange between alkyl- and water-bound hydrogen on relatively short geological timescales at elevated temperatures and pressures. The proximity of some thermogenic and purported abiogenic alkane δ2H values to those predicted for equilibrium 2H/1H fractionation with ambient water suggests that this process may regulate the δ2H signatures of some naturally occurring hydrocarbons.This research received financial support from the Department of Energy (grant DE-FG02-97ER14746), the National Science Foundation (grant OCE-0549829) and the WHOI Deep Ocean Exploration Institute Graduate Fellowship (to E.P. Reeves)
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