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Rapid dissolution of cinnabar in crude oils at reservoir temperatures facilitated by reduced Sulfur Ligands
Umeå University, Faculty of Science and Technology, Department of Chemistry.
Umeå University, Faculty of Science and Technology, Department of Chemistry.
Umeå University, Faculty of Science and Technology, Department of Chemistry.ORCID iD: 0000-0001-9570-8738
2018 (English)In: ACS Earth and Space Chemistry, ISSN 2472-3452, Vol. 2, no 10, p. 1022-1028Article in journal (Refereed) Published
Abstract [en]

Mercury (Hg) is present in petrochemical samples, including crude oils, and the processing and use of petroleum products contribute to global Hg emissions. We present a refined theory on geochemical processes controlling Hg concentrations in crude oil by studying dissolution kinetics and solubility thermodynamics of cinnabar (α-HgS(s)) in different crude oils held at reservoir temperatures. In a black light crude oil, α-HgS(s) dissolved in an apparent zero-order reaction with a rate of 0.14−0.58 μmoles m−2 s −1 at 170−230 °C and an estimated activation energy of 43 kJ mol−1 . For crude oil samples with a total sulfur concentration spanning 0.15− 2.38% (w/w), the measured dissolution rate varied between 0.05 and 0.24 μmoles m−2 s−1 at 200 °C. Separate tests showed that thiols and, to a lesser extent, organic sulfides increased the solubility of α-HgS(s) in isooctane at room temperature compared to thiophenes, disulfides, and elemental sulfur. Long-term (14 days) α-HgS(s) solubility tests in a crude oil at 200 °C generated dissolved Hg concentrations in the 0.3% (w/w) range. The high α-HgS(s) dissolving capacity of the crude oils was more than 2 orders of magnitude greater than the highest reported Hg concentration in crude oils globally. On the basis of the kinetic and solubility data, it was further concluded that α-HgS(s) is not stable under typical petroleum reservoir conditions and would decompose to elemental mercury (Hg0 ). Our results suggest that source/reservoir temperature, abundance of reduced sulfur compounds in the crude oil, and dissolved Hg0 evasion processes are principal factors controlling the ultimate Hg concentration in a specific crude oil deposit.

Place, publisher, year, edition, pages
American Chemical Society (ACS), 2018. Vol. 2, no 10, p. 1022-1028
Keywords [en]
mercury, crude oil, cinnabar, dissolution kinetics, thiol compounds
National Category
Environmental Sciences
Identifiers
URN: urn:nbn:se:umu:diva-153709DOI: 10.1021/acsearthspacechem.8b00096ISI: 000448087400006OAI: oai:DiVA.org:umu-153709DiVA, id: diva2:1268174
Available from: 2018-12-05 Created: 2018-12-05 Last updated: 2018-12-05Bibliographically approved

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Lambertsson, LarsFrech, WolfgangBjörn, Erik

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