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Hydrocarbon Gases (C1–C5) and Organic Matter in Bottom Sediments of the Ivankovo Reservoir on the Volga River N

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Hydrocarbon Gases (C1–C5) and Organic Matter in Bottom Sediments of the Ivankovo Reservoir on the Volga River N ISSN 00978078, Water Resources, 2013, Vol. 40, No. 3, pp. 285–296. © Pleiades Publishing, Ltd., 2013. Original Russian Text © N.S. Safronova, E.S. Grishantseva, G.S. Korobeinik, 2013, published in Vodnye Resursy, 2013, Vol. 40, No. 3, pp. 274–286. WATER QUALITY AND PROTECTION: ENVIRONMENTAL ASPECTS Hydrocarbon Gases (C1–C5) and Organic Matter in Bottom Sediments of the Ivankovo Reservoir on the Volga River N. S. Safronovaa, E. S. Grishantsevaa, and G. S. Korobeinikb a Moscow State University, Moscow, 119991 Russia Email: [email protected] b Vernadsky Institute of Geochemistry and Analytical Chemistry, Russian Academy of Sciences, ul. Kosygina 19, GSP1, Moscow, 119991 Russia Received June 21, 2011 Abstract—The results of studying the composition of hydrocarbon gases (C1–C5) and organic matter in bot tom sediments of the Ivankovo Reservoir in 1995, 2004, and 2005 are given. The methods used in the study include vaporphase gas chromatography, instrumental pyrolysis gas chromatography, and massspectrom 13 etry for determining organic carbon δ Corg. The gas field of bottom sediments in different regions of the res ervoir varies widely in terms of gas saturation and the spectrum of hydrocarbon gases. This suggests the het erogeneous composition of organic matter in the sediments and different conditions of its input and transfor mation processes. The gases were found to contain saturated hydrocarbons from methane to pentane C1–C5, including isomers iC4 and iC5 and unsaturated compounds C2–C4. A correlation was found to exist between methane distribution and the distribution of its more highmolecular homologues, which confirms their genetic relationship in bottom sediments. The obtained results show an increase in the rate of microbi ological processes and organic matter transformation for most regions in the Ivankovo Reservoir. The only exceptions are the zones of Moshkovichskii Bay and the sections at Gorodnya and Konakovo, where tech nogenic organic matter is being accumulated. The high information value of hydrocarbon gases as bio geochemical markers of the sources of organic matter and the rates of its transformation is demonstrated. The isotopic composition of organicmatter carbon in the bottom sediments of the Ivankovo Reservoir δ 13C var ies from –26.1 to –30.86‰. Keywords: bottom sediments, organic matter, gas hydrocarbons, vaporphase gas chromatography, pyrolysis gas chromatography, mass spectrometry DOI: 10.1134/S0097807813020085 INTRODUCTION the end hydrocarbon product of OM mineralization, and can serve as an indicator of those processes. How The role of bottom sediments (BS) in the life of a ever, the concentration of methane, especially in top water body is extremely high. The composition and sampling horizons, can demonstrate the effect of both properties of BS reflect the totality of biological, methanogenesis processes and the properties of meth chemical, and physical processes taking place in the ane as a very mobile gas with low sorption capacity and water body. The rates of biochemical processes of comparatively low water solubility. Because of this, the organic matter (OM) transformation are evaluated by geochemical data on methane distribution in BS a wide range of characteristics. The reduction of low should be studied along with other gas characteristics. molecular OM in BS of freshwater bodies is accompa nied by the production of the majority of methane and Studies show that the distribution of gaseous other lowmolecular hydrocarbons, whose concentra hydrocarbons (HC) in natural features is a function of tions can be used to evaluate the ecological state of the original OM and its transformation processes. The water body [4, 5, 8–10, 13, 14]. The accumulation of specific features of the distribution of gaseous HC can gases in BS depends on OM composition and concen be used as typical organic–geochemical characteris tration. Informative biogeochemical markers of OM tics [7, 12]. sources and its transformation processes are gaseous To collect information about the sources of matter hydrocarbons. Gasometry methods are in wide use in containing compounds of natural and anthropogenic geochemical studies [2, 3, 11, 18]. The total rate of OM, the following tasks were formulated: OM biodegradation processes is mostly assessed by the measured methane content, because methane forms to determine the concentrations of hydrocarbon and occurs in the biosphere almost ubiquitously; it is gases (С1–С5) and to consider the regularities in their 285 286 SAFRONOVA et al. N Ivan’kovskii Pool Peretrusovskii Bay Soz R. 8 Omuntinskii Bay Tver 10 Volzskii Babninskii Bay Peremerki Cr. Pool 9 Moshkovicheskii Dubna Bay 12 7 ГРЭС 13 Vidogoshchi 6 Konakovo 1 2 3 Donkhovka R. Melkovo Ploski Redkino 4 14 11 5 Gorodishche Shoshinskii Pool Novozavidovskii Fig. 1. BS sampling scheme in the Ivankovo Reservoir. Sections: (1) Gorodnya, (2) Melkovo, (3) NizovkaVolga, (4) Nizovka Shosha, (5) Gorodishche, (6) Ploski, (7) Konakovo, (8) Korcheva, (9) Klintsy, (10) Dubna. Bays: (11) Vesna, (12) Fedorovskii, (13) Korovinskii; (14) Redkinskii Canal. distribution in the top BS layers of the Ivankovo Res generalized characteristics of OM have recently ervoir; gained in popularity in geochemical studies [6, 16, 19]. to determine the concentration of total OM com Vaporphase gas chromatography and instrumental ponents; pyrolysis gas chromatography is used for comprehen to study the isotopic composition of organic carbon sive study of the composition of OM in BS. Mass spec 13 Corg for BS. trometry was used to study the distribution of isotopes 13 of organic carbon δ Corg. METHODS OF STUDIES Gas Chromatography The object of study was the BS of the Ivankovo Res ervoir, for which very few data are available in the lit Gases in BS were studied by vaporphase chroma erature about the concentration and distribution of tography. The analytical procedure included the lowmolecular HC [11, 15]. Field studies were carried extraction of gases from BS by equilibrium vapor out in 1995, 2004, and 2005. The sampling was carried method under static conditions and the subsequent out at 13 sections and in 7 bays from Tver City to determination of the composition and concentration Dubna Town (Fig. 1). of components on gas chromatography [18]. The multicomponent analysis of the composition To extract gases from BS, 1 g of sample material of gaseous and solid phases of BS was carried out for was placed in 15ml glass flasks, distilled water was sediment samples taken in summer by GOIN tube added to 2/3 of flask volume, and the flasks were sealed from the upper horizon of BS (top 10–15 cm) in by selfsealing rubber plugs. After shaking, the flasks points in areas subject to different level of technogenic were placed in a thermostat and exposed at 70°С for impact. 30 min. Next, 1 ml of gas was taken and placed in the OM composition is very diverse. Because of this, flow of carrier gas in “Tsvet500" gas chromatograph the analytical methods for the separation and determi with a flameionization detector (Russia). Analysis of nation of individual compounds and OM classes are methane and other light HC was carried out on "Tsvet very complicated and, sometimes, practically unreal 500" gas chromatograph with a flameionization izable. The most widespread modern method for detector. HC were separated in a packed column with effective separation and analysis of complex multi modified aluminum oxide under isothermal regime of component organic mixture is chromatography [1, 2, column thermostat operation. The optimal conditions 17, 18]. Rapid instrumental methods for determining for the separation and quantitative determination of WATER RESOURCES Vol. 40 No. 3 2013 HYDROCARBON GASES (C1–C5) AND ORGANIC MATTER 287 hydrocarbon components in gas phase were found The mass of the sample under study was 5–100 mg. [18]. Under optimal operation conditions of RE 2 analyzer Analysis procedure enable determining hydrocar in the specified pyrolysis cycle, the relative standard bons of the series С1–С5 with saturated, unsaturated, deviation for the characteristics to be evaluated varies and isomeric structure: СН4, С2Н6, С2Н4, С3Н8, from 1 to 8%. The lower concentration detection lim С3Н6, iС4Н10, С4Н10, С4Н8, ∑С5Н12 (the sum of its are 0.01–0.03 mg/g. pentanes and isopentanes). The quantitative analysis was made by absolute calibration method. The lower boundaries of the concentrations determined by the Method for Determining the Isotopic Composition of Corg method were 0.001–0.01 μL/kg, depending on the δ13 compound being analyzed. The relative standard devi The isotopic analysis of Corg was carried out on ation varies from 2 to 6% depending on the concentra mass spectrometers Delta S and Delta Plus. The sedi tion and mass of HC. ment samples were first crushed in a ball mill Reatsch HM 200. Carbonates were removed by 10% HCl solu tion. The samples were washed and dried at 60°С. A Pyrolysis Method of OM Studying weighed portion of the sample was used to determine The method of pyrolysis gas chromatography is in the isotopic composition with the use of a CHNsys wide use for obtaining rapid and adequate information tem of mass spectrometer. The instrumental accuracy about the qualitative composition and the amount of was ±0.1%. The reproducibility of the entire cycle, OM in ecological–geochemical objects. including sample preparation, is not higher than ±0.3‰ PDB [2, 3]. The method is highly sensitive and rapid; it enables one to treat small samples by standard equipment. Of wide use now are pyrolysis methods developed for DISCUSSION OF RESULTS automatic analyzers of ROCKEVAL type and operat ing in fully automated regime—from loading the sam The major sources of anthropogenic impact onto ples to the output of data on the concentration of com the reservoir are the industrial plants of the towns of ponents and the evaluated characteristics in the form Tver and Konakovo and the settlements of Redkino of tables and plots [6, 16, 19].
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