ISSN 1819-7140, Russian Journal of Pacific Geology, 2017, Vol. 11, No. 1, pp. 73–80. © Pleiades Publishing, Ltd., 2017. Original Russian Text © V.V. Ershov, 2017, published in Tikhookeanskaya Geologiya, 2017, Vol. 36, No. 1, pp. 78–86.
On the Problem of Variability in the Chemical Composition of Mud–Volcanic Waters: Evidence from the Yuzhno-Sakhalinsk Mud Volcano V. V. Ershov Institute of Marine Geology and Geophysics, Far East Branch, Russian Academy of Sciences, ul. Nauki 1B, Yuzhno-Sakhalinsk, 693022 Russia e-mail:
[email protected] Received April 4, 2015
Abstract⎯The results of hydrogeochemical observations on the Yuzhno-Sakhalinsk mud volcano in 2010– 2014 are considered. The chemical analysis of samples of mud–volcanic waters was carried out at various analytical centers, which is similar to the common situation where hydrochemical data for a volcano are obtained by different researchers. It is shown that the chemical composition of the mud–volcanic waters is relatively stable in time and space (for different gryphons of the volcano). This allows us to determine the characteristic range of hydrogeochemical indicators. For each year of observations, the coefficients of variation for the concentrations of Na, Mg, Ca, K, and HCO3 mostly range from 10 to 30%. However, the concentrations analyzed in individual samples may differ significantly from each other. These natural variations are a likely source of errors in the interpretation of hydrochemical data. In addition, it is necessary to account for the specifics of mud–volcanic waters as an object of analytical chemical investigations. Keywords: mud volcano, mud–volcanic waters, chemical composition, variability, monitoring, gryphon– salse activity, Sakhalin DOI: 10.1134/S1819714017010031
Therefore, it is important to know the chemical composition of underground waters more exactly. Hydrochemical investigations of mud volcanoes in various regions of the world are carried out for the solution of similar tasks, namely for study of the sources of mud–volcanic material and conditions of its migration to the surface. Such investigations include single sampling, the collection of only a small portion of a sample from an individual mud volcano during the whole period of study. In the case of repeated sampling, the period between the samples often reaches several decades. At the same time, the application of genetic coefficients requires that samples be representative, which will be the case only if the composition of the mud–volcanic waters is homogeneous and constant. It is evident from the data available that gryphons/salses of the same mud volcano may deliver waters of various classes and types [20, 21, 25–28]. The Khamamdag mud volcano (Prikurinskaya oblast, Azerbaijan), with four genetic types of waters classified by V.A. Sulin as sodic hydrocarbonate, sodic sulfate, calcium chloride, and magnesium chloride, is considered as an example in [1]. These peculiarities are traditionally explained by the occurrence of gryphon roots at various stratigraphic horizons, i.e., by
INTRODUCTION Mud volcanoes are natural fluid–dynamic systems in which energy and matter are intensely transported from the Earth’s interior to the surface along the fault zones in the Earth’s crust. Many aspects of mud volcanism, such as the genesis, mechanism of activity, and relationships to other natural processes and phenomena are still poorly explained and remain at the level of hypothesis. Mud–volcanic waters, as one of the components of mud–volcanic activity, are a variety of underground waters, and in this context, mud volcanism is considered in our paper. Study of the chemical composition of underground waters is an integral part of hydrogeological prospecting and provides solution of some important problems. For example, the concentrations of alkali metals (Li, Rb, and Cs) and their proportions indicate the contribution of mantle fluid to feeding of hot springs [2]. It has been suggested to use the B/Br ratio for analysis of the endogenic component in underground waters [7]. An attempt was made to distinguish geochemical associations indicating active faults in [3]. Other relationships between the components of underground waters traditionally applied in hydrogeological practice (Na/Cl, Cl/Br, etc.) are genetically important as well. 73
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the presence of several isolated feeding channels at several feeding reservoirs at different depths within the individual volcano. It is logical to assume that the chemical composition of mud–volcanic waters may vary in time as well, at least due to the clearly reflected cyclic recurrence/periodicity of the mud–volcanic activity. For example, it is shown in [19] that mineralization of waters reaches 3.6 g/L during eruptions of the Pugachev mud volcano, whereas water released from gryphons in the rest period has mineralization within 340–840 mg/L. As is evident from [1, 20], the influence of mud–volcanic chambers decreases in the period of quietness, and waters come mostly from the horizons of the upper structural stage. Deeper horizons are involved during the mud–volcanic activity. It is shown in [9–11] that the chemical composition of mud–volcanic waters is different not only for volcanoes with different activity, but for gryphons with different activity within the same volcano. In fact, the latter is an alternative explanation for the heterogeneous composition of mud–volcanic waters from various gryphons of the same volcano. Active mud volcanoes, or the most active periods of volcanic activity, or the most active gryphons are characterized by high concentrations of hydrocarbonate ion and many other minor elements (B, Li, Sr, Cs, Rb, and others) and by increase in the rNa/rCl coefficient from 1–1.3 to 3– 4.6. Note that there are other ideas on the considered problem. For example, it is shown in [24] that analyses of the waters of the Shugo and Gora Gnilaya mud volcanoes (Taman Peninsula) in 1913 and 1933 match perfectly with each other, which indicates only slight changes.
errors during hydrogeological interpretation of the data. Thus, the problem of constancy in the chemical composition of mud–volcanic waters is still not solved. The degree of possible instability of the chemical composition is also little-studied. In general, the discussed variability may occur in time, as well as in space (in different gryphons of the same volcano). Time variations may result from natural cycles in mud–volcanic activity or from external factors, such as endogenic events (e.g., earthquakes) or weather conditions. Errors in chemical analysis may be considered as an additional reason for variability. To avoid errors in the genetic interpretation of geochemical data or, in particular, to discover the hydrogeoseismic variations, we should not neglect the factors controlling variability in the chemical composition of mud–volcanic waters. The current study is aimed at review and analysis of the results of hydrochemical observations on the Yuzhno-Sakhalinsk mud volcano for obtaining reliable estimates of the measured indicators and understanding of the character of variability in the chemical composition of mud–volcanic waters. OBJECT OF THE STUDY
In addition, it is shown in [9] that the mud–volcanic activity may depend on the seismic regime of the region, which indicates the relationship of the volcanoes of the Kerch–Taman mud–volcanic province with increasing seismic activity in the region in 1965– 1967. In this case, we come to the widely discussed but poorly researched idea on the usage of mud volcanoes as indicators of regional geodynamic processes.
The Yuzhno-Sakhalinsk mud volcano is located in the southern part of the Sakhalin Peninsula, ~18 km to the northwest of Yuzhno-Sakhalinsk. The geological and hydrogeological conditions of this region are considered in detail in [13, 23]. Therefore, here we discuss some general information only. The volcano is controlled by the Central Sakhalin submeridional reversed fault–thrust, along which the Cretaceous rocks were moved on the Paleogene–Neogene deposits in the eastern direction. Strong eruptions of the Yuzhno-Sakhalinsk mud volcano were registered in 1959, 1979, and 2001. One relatively weak eruption occurred between 1994 and 1996; another one, at the beginning of 2011 [14, 18].
It is necessary to mention study [22], mainly aimed at investigation of heterogeneities in the chemical and isotope compositions of underground waters. Hydrogeochemical observations on the Shugo, Gladkovskii, and Shapsuginskii mud volcanoes (Taman Peninsula) were carried out in this study. The samples were collected hourly over three days. Such three-day measurements were performed in 1999–2001 once per season (except for the winter months). Finally, hourly, daily, and seasonal variations in the chemical composition were registered. There is a correlation between variations in the chemical composition of mud–volcanic waters and volcanic activity and the seismic environment in the region. In this relation, the results of episodic measurements of the chemical composition may differ quite significantly, which may result in
Judging from the spatial position and morphology of the gryphons, several relatively independent groups of gryphons are distinguished on the volcano [12, 13]. Groups III and IV are characterized by the highest number of gryphons (Fig. 1). Most of the active gryphons are located there as well. We define the activity of gryphons as the portion of water–mud mixture and free gases released from the gryphon per unit time. Some gryphons of the same group stop functioning and gradually die, but new gryphons appear nearby. The total number of gryphons remains almost constant in the same group. The total number of gryphons on the volcano is 50–70. According to their position, most of the gryphons on the volcano form a belt with a length of ~300 m and a width of ~60 m oriented along the Central Sakhalin fault. This fact provides
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evidence for genetic relationships between the Yuzhno-Sakhalinsk mud volcano and this fault. Sampling of the water–mud mixture released from the gryphons for further chemical analysis of the mud–volcanic waters was carried out from different groups of gryphons, but most of the sampled gryphons corresponded to groups II, III, IV, and VIII. Active gryphons were preferable. The concentration of solid phase in the samples of water–mud mixture mostly ranged from 40 to 80% of the total sample volume.
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142.0° 142.5° 143.0° 143.5°
1
48.0°
2 3
47.5°
4 Yuzhno-Sakhalinsk mud volcano
II 5
47.0° Yuzhno-Sakhalinsk
N
46.5°
METHODS OF THE STUDY Single sampling of the volcano does not provide reliable (averaged from the large data set) estimates of hydrochemical indicators, range of variations for the measured parameters, and explanations for the variability of these indicators. Because of this, the samples of the water–mud mixture were collected systematically from several gryphons of the Yuzhno-Sakhalinsk mud volcano (Table 1). In some cases, parallel samples were collected. Note that the Yuzhno-Sakhalinsk mud volcano is considered as a convenient and accessible polygon allowing us to carry out various natural experiments. Regularities in the mud–volcanic activity observed for this volcano most likely may be applied to mud volcanism in general. Before the chemical analysis, the samples were cleaned of mud suspension using paper and membrane (0.45 μm) filters. The chemical analytical studies in different years were carried out at the Far East Federal University (FEFU); Far East Geological Institute, Far East Branch, Russian Academy of Sciences (FEGI FEB RAS); Institute of Microelectronics Technology and High Purity Materials, Russian Academy of Sciences (IMTHPM RAS); and Institute of Marine Geology and Geophysics, Far East Branch, Russian Academy of Sciences (IMGG FEB RAS). The concentration of the major anions (except for HCO3) and cations was analyzed by the methods of capillary electrophoresis (CE) and ionic chromatography (IC). The concentration of hydrocarbonate ion
S 46.0° VIII VII
VI
V IV
0 I
50 m
III II
Fig. 1. Schematic map of the Yuzhno-Sakhalinsk mud volcano. (1) Groups of gryphons; (2) lines contouring the zone of gryphons on the volcano; (3) mud field from volcanic eruption in 2001; (4) mud field from volcanic eruption in 2011; (5) no. of gryphon group.
was determined by the titration method. Analysis of the element composition was carried out by the method of atomic emission spectrometry (ICP-AES). Diversity in the applied chemical analytic methods and laboratories entails some loss of accuracy of the
General information on sampling of mud–volcanic waters on the Yuzhno-Sakhalinsk mud volcano and on further chemical–analytical studies Date
Number of sampled gryphons
Number of samples
2010—23.09
6
6
2011—02.06
16
24
2012—11.10
7
7
2013—27.06, 24.07, 23.08, 13.09, 04.10, 25.10
5 8
2014—22.08, 04.09, 09.10
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Analytical laboratory
Method of analysis
FEFU
ICP-AES, CE
FEFU, FEGI FEB RAS
ICP-AES, CE
FEGI FEB RAS
ICP-AES, IC
16
IMGG FEB RAS, FEGI FEB RAS
ICP-AES, IC
26
IMGG FEB RAS, FEGI ICP-AES, IC FEB RAS, IMTHPM RAS
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8
10 1
2
3 Na, g/L
pH
8
5
6 14 13 12 11 10 9 8 7 6 5 5.0
3 350 300 250 200 150 100 50 0 240 200 160 120 80 40 0 200
Ca, mg/L
HCO3, g/L
Mg, mg/L
4
Cl, g/L
4.5 4.0 3.5
SO4, mg/L
K, mg/L
469 mg/L 93 mg/L
150 100 50 0
2010
2011
2012
2
6
7
3.0 60 50 40 30 20 10 0
1
7
9
2013
2010
2011
2012
2013
2014
2014
Fig. 2. pH values and concentrations of major anions in mud–volcanic waters from the Yuzhno-Sakhalinsk mud volcano in 2010–2014. (1) Maximum, minimum, and median values for each year of observations; (2) average value and its confidence interval, maximum and minimum values for each year of observations; (3) values of hydrochemical indicators from [23].
performed hydrochemical measurements, but perfectly simulates the situation where the hydrochemical data for the same mud volcano are obtained by different researchers in different years. RESULTS AND DISCUSSION The concentrations of various components in the composition of mud–volcanic waters obtained in each year of observations are considered as random values. The average value and confidence interval for the average value were calculated for each of them (Figs. 2 and 3). The interval estimate was made for a confi-
Fig. 3. Concentrations of major cations in mud–volcanic waters from the Yuzhno-Sakhalinsk mud volcano in 2010– 2014. (1) Average value and its confidence interval, maximum and minimum values for each year of observations; (2) values of hydrochemical indicators from [23].
dence probability of 0.9 assuming the asymptotic character of the set applied for calculation of the average value. Since the volume of the data sets was quite small (from 6 to 26 samples), the Student’s distribution was used instead of the normal distribution, which expands the confidence interval and, therefore, increases reliability. Analyzing the hydrochemical data obtained, we can provide the averaged characteristics of the mud– volcanic waters of the Yuzhno-Sakhalinsk mud volcano. Mud–volcanic waters are highly mineralized (mostly from 18 to 23 g/L), poor-alkaline (pH from 7.5 to 8.5), and belong to the sodic hydrocarbonate– chloride type. The concentrations of major ions have the following ranges: HCO3, from 10 to 12 g/L; Cl, from 3.8 to 4.2 g/L; Na, from 5.5 to 6.5 g/L. These
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characteristics are common for all samples collected in different years and from different gryphons of the volcano. It is evident that the average hydrochemical indicators slightly change from year to year. Some indicators are characterized by quite wide variations for the same field season. This is discussed below. The water–mud mixture from the gryphons of the volcano is a dispersion with a high content of solid particles of various sizes (from submicronic to millimeter). Because of this, it is impossible to carry out hydrochemical measurements in situ. The dispersion phase and dispersion medium are separated by settling and filtering. There may be a quite long period (several days or more, with account for transportation to the place of analysis) between sampling and chemical analysis. It is evident that in this time, the aqueous solution undergoes some changes, but it is not clear how strong these changes are. Special experiments show that the pH of the filtered samples of mud–volcanic waters which are kept at room temperature under the laboratory conditions increases by more than 1 over one–two weeks. In our opinion, this is explained by the fact that the mud–volcanic waters contain dissolved CO2, the concentration of which is significantly higher than the equilibrium one under normal conditions. Removal of excessive CO2 from the solution results in alkalization of the mud–volcanic waters. With increasing pH, the concentration of Ca gradually decreases in the samples. The walls of the containers of the samples were covered with white bloom (most likely CaCO3). This assumption is supported by thermodynamic calculations providing evidence for significant oversaturation of the mud–volcanic waters in calcite. Similar processes probably proceed during preparation of the samples for further chemical analysis. Therefore, we assume that the pH values for the samples collected in 2010 (and for some samples collected in 2014) are slightly overestimated. The low concentrations of HCO3 in the samples collected in 2010 (and for some samples collected in 2014) are explained by the high pH, at which a portion of the hydrocarbonate ion transforms to carbonate ion due to dissociation. Most likely, the concentrations of Ca in the mud–volcanic waters are slightly underestimated for all of the studied samples. In 2010 and 2012, relatively small numbers of samples were collected once per year. Because of this, we cannot ignore the slight dissolution of these samples by atmospheric precipitates. This may explain the relatively low concentrations of chloride ion in the mud– volcanic waters in 2010 and 2012. Interestingly, the eruption of the Yuzhno-Sakhalinsk mud volcano at the beginning of 2011 did not entail obvious changes to the hydrochemical regime of the volcano. It is clearly evident that all of the indicators obtained in all years of observations are characterized by quite narrow confidence intervals for average values. Consequently, the mud–volcanic waters in all RUSSIAN JOURNAL OF PACIFIC GEOLOGY
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gryphons of the volcano have similar chemical compositions. This allows us to suggest a single water source for the Yuzhno-Sakhalinsk mud volcano. The concentration of SO4 in the mud–volcanic waters, which varies significantly in each year of observation, is an exception. The coefficient of variation (percent ratio of mid-square deviation to average value) for sulfate ion ranges from 45 to 100%. Chloride ion has the lowest coefficient of variation: from 2.4 to 6.7%. In spite of a certain space–time stability of hydrochemical indicators, samples with hydrochemical indicators significantly different from the average values (both higher and lower) are abundant. We should consider the errors of the chemical analysis in the further discussion of the data obtained. The presence of accreditation in the RusAccreditation is often applied as a criterion of reliability of the results of a chemical–analytical laboratory. In fact, this is an important factor providing evidence for competence of a laboratory for any kinds of tests. Obtaining of accreditation confirms the laboratory’s compliance with legal requirements. However, this should not be taken as an absolute rule. Intralaboratory comparative tests (ICT) are one of the most important methods to check the qualification of a laboratory upon accreditation. For example, such tests for accreditation in the sphere of chemical analysis of various types of water (drinking, natural, mineral, technical, etc.) are carried out by the analytical center of water quality control ZAO ROSA [6]. Several criteria for evaluating ICT results are applied. One of them is the consistency of the errors declared by the laboratory. This criterion demonstrates the ability of a laboratory to provide an error, which figures in the applied methodology of chemical analysis. Another criterion is consistency with a particular value for measurement error established by the relevant normative document [4]. The third criterion is consistency with the Z index, which is related to the standard deviation from the licensed value of the controlled indicator calculated by the results of all laboratories participating in the ICT. In other words, this criterion shows the place of the considered laboratory among all other participants of a particular stage in the ICT. Analysis of the appropriate publications and normative documents [4, 5, 15– 17] shows that the relative error of the chemical analysis of underground waters is 10–25%. The results of analysis obtained in individual laboratories of the ICT and following the mentioned criteria may differ by a factor of 1.2–1.45. At the same time, a well-managed (from the position of quality) laboratory with experienced staff may sometimes provide unsatisfactory results of testing [6]. Thus, even in the case of a consistent composition of mud–volcanic waters, individual measurements may differ by a factor of 1.5. Therefore, to obtain reliable data on the studied natural object, a certain minimum number of samples must be collected. No. 1
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Concentration of bromide-ion, mg/L
18 2
16 y = 0.00164x + 1.27 R2 = 0.9970
14 12
1
10 8 y = 0.00137x + 0.026 R2 = 0.9994
6 4 2 0
1000 2000 3000 4000 5000 6000 7000 8000 9000 10000 Peak area
Fig. 4. Calibration line for bromide ion during analysis of aqueous solutions by the method of ionic chromatography. (1) Line for the samples prepared using deionized water; (2) line for the samples prepared using the model solution simulating the matrix of mud–volcanic waters from the South-Sakhalinsk mud volcano.
It is logical to check our considerations on the results of independent studies. We can use study [23], where the data on the chemical composition of two samples of mud–volcanic waters from the YuzhnoSakhalinsk mud volcano are reported. It is evident that the concentrations of HCO3, Cl, SO4, Na, and K cannot be considered as typical for the Yuzhno-Sakhalinsk mud volcano (Figs. 2 and 3). This may result in errors during interpretation of the hydrochemical data. For example, the genetic coefficient rNa/rCl for waters from the Yuzhno-Sakhalinsk mud volcano has a typical range from 2.1 to 2.4, whereas, according to [23], this coefficient is 2.04 for one sample and 2.64 for the other. Application of the data from this study results in underestimation of the temperature of the formation of waters by several tens of °C during calculations by the Na–K and K–Mg hydrochemical geothermometers [29]. However, these deviations may be considered as insignificant in comparison with the situation with calculation of the B/Br ratio. As is evident from [23], the concentration of Br is 0.2 mg/L in one sample and 0.05 mg/L in the other sample; the B/Br ratios are 1290 and 6900, respectively. It is suggested to use the B/Br ratio for distinguishing the endogenic component in underground waters. It is much higher in the hydrotherms of areas of modern volcanism (from 9.4 to 45.4) [7]. It is shown that the underground waters of the Urengoi deposit (West Siberia) have a positive correlation between B/Br and temperature calculated by the Na–K geothermometer [8]. The values of B/Br >1.2 correspond to temperatures of the solution formation of >150°C. It is evident that such high values of B/Br for the Yuzhno-Sakhalinsk mud volcano (higher by two orders of magnitude in com-
parison with those of the hydrotherms) are difficult to explain. Analysis of our data (>40 samples in 2012–2014) shows that the concentration of Br in the mud–volcanic waters of the Yuzhno-Sakhalinsk mud volcano mostly ranges from 3.5 to 6.5 mg/L. With account for the typical concentrations of B in the mud–volcanic waters (30 samples in 2011–2014), the B/Br ratio will vary from 30 to 85. It is also necessary to take into account during the chemical analysis that mud–volcanic water is the specific object of the study. Proportions of the concentrations of some components reach 1/1000, which results in the specific matrix effect: the presence of one component with a high concentration in the sample interferes with the measurement of the other component with a much lower concentration. Special laboratory experiments were carried out for estimation of this influence. Calibration on the model solution was done in addition to common calibration for the chemical analysis of aqueous solutions by the method of ionic chromatography. The model solution simulated the sodic hydrocarbonate–chloride matrix of the mud–volcanic waters from the Yuzhno-Sakhalinsk mud volcano and had the following chemical composition: HCO3, 10 g/L; Cl, 4 g/L; Na, 3.77 g/L. It is evident that the presence of the model solution results in underestimation of the Br content (Fig. 4). The relative error is especially high for the lower concentrations. Therefore, the real values of the B/Br ratio will be lower and comparable with the same indicator for thermal waters in the regions of modern volcanism. Thus, the standard methodologies of chemical analysis do not fully account for the specific character of some samples of underground waters. Because
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of this, the results obtained by different researchers during single sampling may be significantly different. CONCLUSIONS Our hydrogeochemical observations have allowed us to characterize the variability in the chemical composition of the mud–volcanic waters from the Yuzhno-Sakhalinsk mud volcano, to obtain reliable estimates (averaged by the huge data set) of the hydrochemical indicators, and to determine the limits of variability for the measured indicators. The chemical composition of the mud–volcanic waters is relatively stable in time and space (in various gryphons of the volcano). The most significant variations are observed for the concentration of SO4, but the reasons for this are still not clear. The relatively weak eruption of the volcano at the beginning of 2011 did not have any significant impact on the hydrochemical indicators. Thus, the hydrochemical regime of the volcano for the five years of our observations was characterized by a single source of the liquid phase of the mud–volcanic material and its invariability. In this relation, we can reasonably expect that observations properly organized on other volcanoes will allow us to confirm the quite high invariability in the chemical composition of mud–volcanic waters. In addition, such invariability allows us to suggest that the hydrochemical regime of mud volcanoes reacts only to intense external influence (e.g., close and strong earthquakes). In this case, mud volcanoes may be used as an indicator of the state of the geological environment. In spite of the absence of significant variations in the average hydrochemical indicators, there is a quite wide value of scatter within each year of observations. This scattering is rather sufficient for probable errors in interpretation of hydrochemical data in the case of single sampling. To minimize these errors, it is also necessary to account for the specifics of mud–volcanic waters as an object of chemical–analytical studies. The range of observed variations cannot be fully explained by error in the chemical analysis. We can postulate the probable presence of a fine structure of the hydrochemical regime of the mud volcano. For this reason, detailed hydrogeochemical monitoring of the Yuzhno-Sakhalinsk mud volcano would be advisable. ACKNOWLEDGMENTS The author is grateful to A.V. Kopanina, I.F. Osennyaya, and I.I. Vlasova for help in field works. This study was partly supported by the Russian Foundation for Basic Research (project no. 15-05-01768). RUSSIAN JOURNAL OF PACIFIC GEOLOGY
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Recommended for publishing by B.W. Levin Translated by A. Bobrov
RUSSIAN JOURNAL OF PACIFIC GEOLOGY
Vol. 11
No. 1
2017
