Item talk:Q253016
From geokb
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"name": "Experimental investigation on thermochemical sulfate reduction by H2S initiation",
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"value": "10.1016/j.gca.2008.04.036",
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"name": "Geochimica et Cosmochimica Acta",
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"abstract": "Hydrogen sulfide (H2S) is known to catalyze thermochemical sulfate reduction (TSR) by hydrocarbons (HC), but the reaction mechanism remains unclear. To understand the mechanism of this catalytic reaction, a series of isothermal gold-tube hydrous pyrolysis experiments were conducted at 330\u00a0\u00b0C for 24\u00a0h under a constant confining pressure of 24.1\u00a0MPa. The reactants used were saturated HC (sulfur-free) and CaSO4\u00a0in the presence of variable H2S partial pressures at three different pH conditions. The experimental results showed that the\u00a0in-situ\u00a0pH of the aqueous solution (herein,\u00a0in-situ\u00a0pH refers to the calculated pH of aqueous solution under the experimental conditions) can significantly affect the rate of the TSR reaction. A substantial increase in the TSR reaction rate was recorded with a decrease in the\u00a0in-situ\u00a0pH value of the aqueous solution involved. A positive correlation between the rate of TSR and the initial partial pressure of H2S occurred under acidic conditions (at\u00a0pH\u00a0\u223c3\u20133.5). However, sulfate reduction at pH \u223c5.0 was undetectable even at high initial H2S concentrations. To investigate whether the reaction of H2S(aq)\u00a0and\u00a0HSO4-\u00a0occurs at pH \u223c3, an additional series of isothermal hydrous pyrolysis experiments was conducted with CaSO4\u00a0and variable H2S partial pressures in the absence of HC at the same experimental temperature and pressure conditions. CaSO4\u00a0reduction was not measurable in the absence of paraffin even with high H2S pressure and acidic conditions. These experimental observations indicate that the formation of organosulfur intermediates from H2S reacting with hydrocarbons may play a significant role in sulfate reduction under our experimental conditions rather than the formation of elemental sulfur from H2S reacting with sulfate as has been suggested previously (Toland W. G. (1960) Oxidation of organic compounds with aqueous sulphate.\u00a0J. Am. Chem. Soc.\u00a082, 1911\u20131916).Quantification of labile organosulfur compounds (LSC), such as thiols and sulfides, was performed on the products of the reaction of H2S and HC from a series of gold-tube non-isothermal hydrous pyrolysis experiments conducted at about pH 3 from 300 to 370\u00a0\u00b0C and a 0.1-\u00b0C/h heating rate. Incorporation of sulfur into HC resulted in an appreciable amount of thiol and sulfide formation. The rate of LSC formation positively correlated with the initial H2S pressure. Thus, we propose that the LSC produced from H2S reaction with HC are most likely the reactive intermediates for H2S initiation of sulfate reduction. We further propose a three-step reaction scheme of sulfate reduction by HC under reservoir conditions, and discuss the geological implications of our experimental findings with regard to the effect of formation water and oil chemistry, in particular LSC content.",
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