Jump to ContentJump to Main Navigation
Show Summary Details
More options …

Open Geosciences

formerly Central European Journal of Geosciences

Editor-in-Chief: Jankowski, Piotr

1 Issue per year


IMPACT FACTOR 2016 (Open Geosciences): 0.475

CiteScore 2016: 0.87

SCImago Journal Rank (SJR) 2016: 0.346
Source Normalized Impact per Paper (SNIP) 2016: 0.690

Open Access
Online
ISSN
2391-5447
See all formats and pricing
More options …

Organic-inorganic interactions in the system of pyrrole-hematite-water at elevated temperatures and pressures

Kangle Ding
  • Key Laboratory of Exploration Technologies for Oil and Gas Resources of Ministry of Education, Yangtze University, Jingzhou 434023, Hubei, China; School of Chemistry and Environmental Engineering, Yangtze University, Jingzhou 434023, Hubei, China
  • Other articles by this author:
  • De Gruyter OnlineGoogle Scholar
Published Online: 2015-11-03 | DOI: https://doi.org/10.1515/geo-2015-0050

Abstract

The distribution and abundance of pyrrolic compounds in sediments and crude oils are most likely influenced by inorganic sedimentary components. In this paper, thermal simulation experiments on the system pyrrole-hematite-water were carried out at elevated temperatures and pressures in order to investigate the effect of organic-inorganic interactions on the preservation of pyrrolic compounds. Compositions of the reaction products were analyzed with GC-MS and GC-FID methods. In the closed system pyrrole-hematite-water, the nitrogen-oxygen exchange obviously occurred at temperatures above 350ºC in accordance with the thermochemical calculation. Large amounts of furan and ammonia were generated after simulation experiments, indicating that the conversion of pyrrole into furan was the dominant reaction. Thermochemical exchange effect between organic nitrogen and inorganic oxygen was obviously facilitated by elevated temperatures and found to be catalyzed by hematite, but inhibited by the increasing volume of water. Thermodynamically water spontaneously reacts with pyrrole above 300ºC. The reaction of pyrrole-hematite-water is an exothermic process in which the reaction heat positively correlates with temperature. The heat released was estimated as 9.0 KJ/(mol) pyrrole - 15.0 KJ/(mol) pyrrole in typical oil reservoirs (100ºC–150ºC) and 15.0–23.0 KJ/(mol) pyrrole in typical gas reservoirs (150ºC–200ºC). The calculated activation energy of the nitrogen-oxygen atom exchange is about 129.59 kJ/mol. According to the experimental results, a small amount of water may effectively initiate the nitrogen-oxygen exchange. The study would improve our evaluating of the preservation and fate of pyrrolic compounds in deeply buried geologic settings and further understanding of thermochemical processes behind the degradation of petroleum.

Keywords: pyrrolic compounds; simulation experiments; pyrrole-hematite-water; organic-inorganic interaction; exothermic process

References

  • [1] Bakr M.M.Y.,Wilkes H., The influence of facies and depositional environment on the occurrence and distribution of carbazoles and benzocarbazoles in crude oils: a case study from the Gulf of Suez, Egypt, Org. Geochem. 2002, 33, 561–580 CrossrefGoogle Scholar

  • [2] Bennett B., Lager A., Russell C.A., Love G.D., Larter S.R., Hydropyrolysis of algae, bacteria, archaea and lake sediments; insights into the origin of nitrogen compounds in petroleum, Org. Geochem. 2004, 35, 1427–1439 CrossrefGoogle Scholar

  • [3] Zhang C.M., Zhang Y.Q., Zhang M., Zhao H.J., Cai C.F., Carbazole distributions in rocks from non-marine depositional environments, Org. Geochem. 2008, 39, 868–878 Web of ScienceCrossrefGoogle Scholar

  • [4] Clegg H., Wilkes H., Horsfield B., Carbazole distributions in carbonate and clastic source rocks, Geochim. Cosmochim. Acta. 1997, 61, 5335–5345 CrossrefGoogle Scholar

  • [5] Clegg H., Wilkes H., Oldenburg T., Santamaría-Orozco D., Horsfield B., Influence of maturity on carbazole and benzocarbazole distributions in crude oils and source rocks from the Sonda de Campeche, Gulf of Mexico, Org. Geochem. 1998, 29, 183–194 CrossrefGoogle Scholar

  • [6] Harrison E., Telnaes N., Wilhelms A., Horsfield B., Van Duin A., Bennett B., Larter S.R., Maturity controls on carbazole distributions in coals and source rocks. In: Poster Sessions from the 18th International Meeting on Organic Geochemistry, Maastricht 1997, 22–26 Google Scholar

  • [7] Horsfield B., Clegg H.,Wilkes H., Santamara-Orozco D.,Maturity control of carbazole distribution in petroleum systems, Naturwissenschaften 1998, 85, 233–237 CrossrefGoogle Scholar

  • [8] Li M.W., Yao H.X., Stasiuk L.D., Effect of maturity and petroleum expulsion on pyrrolic nitrogen compound yields and distributions in Duvernay Formation petroleum source rocks in central Alberta, Canada, Org. Geochem. 1997, 26, 731–744 CrossrefGoogle Scholar

  • [9] Li M.W., Fowler M.G., Obermajer M., Stasiuk L.D., Snowdon L.R., Geochemical characterisation of Middle Devonian oils in NW Alberta, Canada: possible source and maturity effect on pyrrolic nitrogen compounds, Org. Geochem. 1999, 30, 1039–1057 CrossrefGoogle Scholar

  • [10] Bakel A.J., Philp R.P., The distribution and quantitation of organonitrogen compounds in crude oils and rock pyrolysates, Org. Geochem. 1990, 16, 353–367 CrossrefGoogle Scholar

  • [11] Li M.W, Larter S.R., Stoddart D., Bjoroy M., Fractionation of pyrrolic nitrogen compounds in petroleum during migration: derivation of migration-related geochemical parameters. In: Cubitt J., EnglandW.A. (Eds.), The Geochemistry of Reservoirs, Geological Society, London, 1995, 103–123 Google Scholar

  • [12] Li M.W, Osadetz K.G.M., Fowler M.G., Snowdon L.R., Stasiuk L.D., Yao H.X., Hwang R.J., Jenden P.D., Grant B.D., Idiz E., Case studies of secondary oil migration in the Williston Basin. In: Christopher J.E., Bend S. (Eds.), Proceedings of the 9th International Williston Basin Symposium (Saskatchewan Geological Society, Regina, Canada. Special publication No. 13), 1998, 247–253 Google Scholar

  • [13] Larter S.R., Bowler B.F.J., Li M.W., Chen M., Brincat D., Bennett B., Noke K., Donohoe P., Simmons D., Kohnen M., Allan J., Telnaes N., Horstad I., Molecular Indicators of Secondary Oil Migration Distances, Nature 1996, 383, 593–597 Google Scholar

  • [14] Terken J.M.J., Frewin N.L., The Dhahaban petroleum system of Oman, Am. Assoc. Pet. Geol. Bull. 2000, 84, 523–544 Google Scholar

  • [15] Wang T.G., Li S.M., Zhang S.C., Oil migration in the Lunnan region, Tarim Basin, Chian based on the pyrrolic nitrogen compound distribution, J. Petro. Sci. Eng. 2004, 41, 123–134 Google Scholar

  • [16] Zhang C.M., Li S.T., Yang, J.M., Yang, S.K.,Wang, J.R., Petroleum migration and mixing in the Pearl River Mouth Basin, South China Sea, Mar. Pet. Geol. 2004, 21, 215–224 CrossrefGoogle Scholar

  • [17] Siskin M., Katritzky A.R., Reactivity of organic compounds in hot water: Geochemical and technological implications, Science 1991, 254, 231–237 CrossrefGoogle Scholar

  • [18] Helgeson H.C., Knox A.M., Owens C.E., Shock E.L., Petroleum, oil field waters, and antigenic mineral assemblages: Are they in metastable equilibrium in hydrocarbon reservoirs? Geochim. Cosmochim. Acta. 1993, 57, 3295–3339 CrossrefGoogle Scholar

  • [19] Stalker L., Farrimond P., Larter S.R., Water as an oxygen source for the production of oxygenated compounds (including CO2 precursors) during kerogen maturation, Adv. Org. Geochem. 1994, 22, 477–486 Google Scholar

  • [20] Lewan M.D., Experiments on the role of water in petroleum formation, Geochim. Cosmochim. Acta. 1997, 61, 3691–3723 CrossrefGoogle Scholar

  • [21] Lu S.T., Ruth E., Kaplan I.R., Pyrolysis of kerogen in the absence and presence of montmorillonite-I, the generation, degradation and isomerization of steranes and triterpanes at 200 and 300∘, Org. Geochem. 1989, 14, 491–499 Google Scholar

  • [22] Mango F.D., Hightower J.W., James A.T., Role of transition-metal catalysis in the formation of natural gas, Nature 1994, 368, 536– 538 CrossrefGoogle Scholar

  • [23] Mango F.D., Transition metal catalysis in the generation of natural gas, Org. Geochem. 1996, 24, 977–984 CrossrefGoogle Scholar

  • [24] Mango F.D., Hightower J.W., The catalytic decomposition of petroleum into natural gas, Geochim. Cosmochim. Acta. 1997, 61, 5347–5350 CrossrefGoogle Scholar

  • [25] Seewald J.S., Aqueous geochemistry of low molecular weight hydrocarbons at elevated temperatures and pressures: Constraints from mineral buffered laboratory experiments, Geochim. Cosmochim. Acta. 2001, 65, 1641–1644 CrossrefGoogle Scholar

  • [26] Seewald J.S., Organic-inorganic interaction in petroleumproducing sedimentary basins, Nature 2003, 426, 327–333 Google Scholar

  • [27] Dean J.A., Lange’s handbook of chemistry, McGraw-Hill Professional, New York, 1998 Google Scholar

  • [28] BurnhamA.K., Sweeney J.J., A chemical kinetic model of vitrinite maturation and reflectance, Geochim. Cosmochim. Acta. 1989, 53, 2649–2657 CrossrefGoogle Scholar

  • [29] Huang W.L., Experimental study of vitrinite maturation: effects of temperature, time, pressure, water and hydrogen index, Org. Geochem. 1996, 24, 233–241 CrossrefGoogle Scholar

  • [30] Schenk H.J., Dieckmann V., Prediction of petroleum formation: the influence of laboratory heating rates on kinetic parameters and geological extrapolations, Mar. Pet. Geol. 2004, 21, 79–95 CrossrefGoogle Scholar

  • [31] Yaws C.L., Yaws’ Handbook of Thermodynamic and Physical Properties of Chemical Compounds, Knovel, New York, 2003 Google Scholar

  • [32] Tanabe K., Solid acids and bases, Kodansha, Tokyo and academic press, New York, 1970 Google Scholar

About the article

Received: 2014-01-05

Accepted: 2014-11-27

Published Online: 2015-11-03


Citation Information: Open Geosciences, Volume 7, Issue 1, ISSN (Online) 2391-5447, DOI: https://doi.org/10.1515/geo-2015-0050.

Export Citation

©2015 Kangle Ding. This work is licensed under the Creative Commons Attribution-NonCommercial-NoDerivatives 3.0 License. BY-NC-ND 3.0

Comments (0)

Please log in or register to comment.
Log in