Geofluids Assessment of the Ayub and Shafa Hot Springs in Kopet-Dagh Zone (NE Iran): An Isotopic Geochemistry Approach.
Characteristics of springs (especially hot springs) in orogenic regions are due to the interaction between water, the lithosphere, and environmental conditions like lithology, pathways, residence time underground, and many other factors. The origin of elevated temperatures in hydrothermal reservoirs (hot/warm springs) can be due to the geothermal gradient with deep circulation of groundwater through faults, chemical reactions (e.g., in evaporates and oil field brines), heat produced through radioactive decay of long-lived radioactive material (isotopes), and mixing of meteoric water with magmatic water or volcanic vapour in volcanic area [1-11]. The hydrothermal phenomenon most often occurs where the released water and vapour are related to regional volcanic activities. The geothermal heat transfer to the ground surface occurs through aqueous and magmatic/volcanic systems. In an aqueous system, cold surface water can penetrate to depth through deep faults/fractures, where convective currents cause the boiling of water. Subsequently the high temperature groundwater flows upward creating a hydrothermal system on or near the ground surface as hot springs or thermal groundwater discharge within an aquifer . In a geothermal field, an aqueous system can be seen as hot spring, geyser, and mudpot subsystems. Understanding the origin of hydrothermal fluids and the reason for the elevation of temperature is a very important step in revealing the temperature and pressure conditions of the underground reservoirs . To determine the reason and origin of the temperature/heat in a geothermal field, several methods such as remote sensing, geological investigation, geophysical survey, thermal anomalies measurements, and hydrochemical and isotopic method can be applied . Today oxygen and hydrogen isotopes are widely used in geothermal studies to determine the origin and history of geothermal fluids and often serve as natural tracers for the provenance of geothermal water. Most geothermal systems are recharged by meteoric waters and if recharging from shallower groundwater these systems have isotope compositions consistent with local meteoric precipitation . The main objective of this paper is to determine the geothermal reservoir characteristics (type, origin, temperature, and depth of circulation) of Ayub-Peighambar and Shafa (AP and SH) hot springs, in the NE of Iran, using geothermometers and environmental [sup.2]H and [sup.18]O isotopes along with geological and thermal anomalies data of the study area.
2. Sampling Locations and Geology of the Study Area
The AP and SH hot springs, with a temperature range of 36 to 40[degrees]C, are located in the NE of Iran (Figure 1). Field parameter measurement locations and sampling points are illustrated in Figure 2(a). The geological map of the study area was generated using field observations, satellite images, and remote sensing techniques (Figure 2(a)). As illustrated on the geological map, various sedimentary lithological units including massive limestone (Tirgan Formation), marl as pencil marl (Sarcheshmeh Formation), marl-shale (Sanganeh Formation), and sandstone-shale with glauconite (Aitamir Formation) have outcropped in the study area. These formations make the Asiazow anticline with a 15-degree plunge to the west, thrusting and faulting (Figure 2(b)). By oxidation of pyrite, as clearly indicated in thin sections of both Sarcheshmeh and Aitamir Formations, dissolved sulfate was produced , which in turn can be reduced through microbial and thermal reduction process (Hill, 1987; ), which finally results in [H.sub.2]S[O.sub.4] production in the groundwater [18,19].
Travertine around AP hot spring is evidence of a long discharge history at this spring (Figure 3). This indicates that the water of AP hot spring has previously moved upward through faults where the surface temperature and pressure conditions led to oversaturation of the water with respect to carbonate minerals ([C.sub.a]C[O.sub.3]) which in turn caused travertine precipitation. This is confirmed by the presence of calcite and aragonite (usually aragonite forming in deep conditions rather than calcite) structures in thin sections and in Scanning Electron Microscope (SEM) images (Figure 3). The X-Ray Fluorescence (XRF) analysis of travertine indicates that CaO contains 55% of travertine and Atomic Absorption Spectrophotometry (AAS) and Energy Dispersive Spectrometer (EDX) results show that calcium (with 27%) is the major cation in AP travertine (Figure 3). The existence of a large amount of voids in the travertine can be seen clearly in both hand specimens and thin sections (Figure 3), indicating that CO2 was escaping during formation of this thermogenic travertine. There is no evidence for volcanic activities or existence of intrusive igneous rocks, as confirmed by the field observations and reported by previously report .
3. Material and Methods
Water samples were collected in polyethylene 25 mL bottles, from AP and SH hot springs during 2013-2014. All samples were filtered using 0.45 [micro]m membrane and the cation samples were acidified using concentrated HN[O.sub.3] acid. Field parameters, T, pH, Eh, EC, and TDS, were measured during sampling. The geochemical analyses of main cations and anions and the isotopic analyses of [sup.18]O and [sup.2]H in water were performed at the geochemistry and G. G. Hatch Stable Isotope laboratories at the University of Ottawa. Geological formations of the study area were investigated using available maps, remote sensing with satellite images, and field observation. The sediment samples were collected from the AP hot spring frontal pool and their mineral contents were determined from thin sections and binocular microscope. All AAS, XRF, SEM, and EDX analyses on travertine samples were done at the Ferdowsi University of Mashhad. The geothermometry of water samples was determined using Aq.QA hydrochemical software  and cation geothermometers (Na-K) coupled with isotopic ([sup.18]O and [sup.2]H) geochemistry.
4. Results and Discussion
The measured field parameters and major ion concentrations of groundwater samples are listed in Table 1. The origin and type of water and geothermal reservoir characteristics (temperature and depth) of AP and SH hot spring were investigated using geochemistry and geological studies, geothermometers, and environmental [sup.2]H and [sup.18]O isotopes.
4.1. The Origin and Type of Water in the AP and SH Hot Spring. Based on piper diagram AP and SH hot springs fall into the CaS[O.sub.4] facies (Figure 4) and according to Cl-HC[O.sub.3]S[O.sub.4] diagram (Figure 5) we have distinguished mature waters (high content of Cl and is saline), peripheral and shallow waters (HC[O.sub.3] is more than 50%), steam heated waters (S[O.sub.4] is more than 50% and HC[O.sub.3] > Cl), and magmatic and volcanic waters (HC[O.sub.3] [approximately equal to] 0, high S[O.sub.4] and sulfate and chloride type) . Chemically, the AP and SH hot springs samples have the same chemical composition as a chemically homogeneous source and are of the steam heated water type. These samples have considerable concentrations of HC[O.sub.3], Ca, and Mg with Ca-S[O.sub.4] type, indicating deep circulation of meteoric water through the carbonate formation and available deep faults in study area. The increasing of water temperature is probably due to deep circulation and exothermic chemical reactions (probably within the Shourijeh Formation with anhydrite and gypsum). However, a partial melting zone, which emerged through convection currents and faults in the axis of Asiazow anticline, cannot be ruled out.
4.2. Deep Water Circulation Evidence in Quartz of AP Sediment, Thermal Anomalies, and C[O.sub.2] Gas. Since there is no volcanic activity in the area , the possibility of a volcanic source for the AP spring's hydrothermal reservoir has been rejected. The existence of travertine around AP spring provides insight into the circulation of water through faults in the past and present. Cold meteoric waters penetrated and dissolved deep Tirgan limestone formations and then became highly enriched in bicarbonate (HC[O.sub.3]) and sulfate (S[O.sub.4]) (due to reduction of mineral sulfates by bacteria with carbonate mineral dissolution at depth) and precipitated/or not precipitated CaC[O.sub.3] on the ground surface, depending on the pH and Eh of the spring water. This porous thermogenic travertine has had very high amount of C[O.sub.2] which resulted from deep circulation, exothermic chemical reactions, and dissolution of limestone by sulfuric acid. The thermal anomaly map of the study area, prepared based on temperature of local springs' water (Table 1), indicates that the AP and SH hot springs in the study area have the most thermal anomalies (Figure 6). These thermal anomalies are caused by tectonically tensional conditions, which can be confirmed by the presence of travertine as well as joints and faults in the area (e.g., ; Liu et al., 2003). The sedimentary petrography of AP hot spring indicates quartz and rim-burned biotite has been altered to chlorite, via chloritization, which is characteristic of igneous biotite. Although assembled minerals of green chlorite, opaque mineral (pyrite), amphibole, and glauconite can be seen in thin sections (Figure 7), igneous biotite is reported for the first time in this research and needs further investigation. Large amounts of quartz in pool sediments and also in thin section of this sediment confirmed deep circulation of water. The amount of C[O.sub.2] that dissolved in AP hot spring is 9.25 mg/L with a little [H.sub.2]S, exempt of bubbles that escaped , indicating deep circulation of water through the deep faults  that were generated by sulfuric acid in phreatic zone.
4.3. Temperature and Depth Measurements of the Hydrothermal Reservoirs Using Geothermometers. The temperature of hydrothermal reservoirs can be determined using geothermometry . Since geothermometers equilibrate with their surrounding environments under certain temperature and pressure, their equilibrium concentrations in water (from hot springs, soil, and rock) are applied to determine the thermodynamic equilibrium temperature and pressure conditions [26, 27]. This method is very useful in areas without drilled boreholes/wells and it is applicable for initial studies in exploration geothermal fields. To estimate the ranges of temperature in a geothermal reservoir, a large suite of geothermometry tools (minerals, elements, and chemical composition such as silica (Si[O.sub.2]), cations (Na, K, and Li), and gases ([H.sub.2]S, C[O.sub.2], [H.sub.2], C[O.sub.2]/[H.sub.2], and [H.sub.2]S/[H.sub.2])) can be used [15, 26, 28]. The equilibrium concentrations of Na and K in aqueous and solid feldspar phases (1) strongly depend on temperature. Therefore, the Na-K geothermometer can be applied for both [29-31] hot water (250 < T < 300[degrees] C) and very hot water (T > 300 [degrees]C) [15, 29].
Based on chemical composition of the water, the temperature of AP hot springs reservoirs were estimated using the Na-K geothermometer and (2). Also the temperatures were estimated using Aq.QA software by defining Na-K and Si[O.sub.2] as geothermometers. The depth of geothermal reservoir of these springs was calculated using (3)  and all estimated temperature and depth are listed in Table 2.
[K.sup.+] + Na-feldspar = K-feldspar + [Na.sup.+] (1)
T[degrees]C(Na-K) = [933/0.933 + log(Na/K)] - 273.15 (2)
D = (Tg - Ts)/[DELTA]G. (3)
Here, D is the depth of reservoir (km), Tg is the calculated temperature by geothermometers, and Ts refer to the average annual temperature (10.4[degrees]C which is calculated by Domarton and Amberege methods ). Also [DELTA]G is the geothermal gradient (0.03[degrees]C per 1 meter).
4.4. Heat Source Determination Using [sup.18]O and [sup.2]H Isotopes. Based on [delta][sup.18]O and [delta][sup.2]H values of a geothermal water, the heat source of the water may be determined . The [delta][sup.18]O and [delta][sup.2]H values of AP and SH hot springs are plotted within the range of geothermal and meteoric waters (Figure 8). The average [delta][sup.18]O values of the AP and SH hot springs (-10[per thousand], Figure 8) indicate that the heat source cannot be related to volcanic activities (with [delta][sup.18]O value of about 5%) and therefore the geothermal gradient is the primary heat source. Meteoric water, by penetrating to depth through faults/fractures, is heated and altered to a geothermal water, subsequently rising and discharge at the land surface. The deuterium content of these springs (average of -73%, n = 21) is within the range of granitic and metamorphic rocks (-40% to -90%, Figure 8(b)), which is probably due to partial melting and alteration in Kopet-Dagh bedrock that resulted in increasing temperature in spring water (reference for partial melting and alteration). Although this can be confirmed with the existence of biotite in AP hot spring sediment, it needs more investigation.
4.5. Calculating the Depth of Water Circulation Using [sup.18]O and [sup.2]H Isotopes. The depth of water circulation in the AP hot spring reservoir was determined using [delta][sup.18]O and [delta][sup.2]H isotopic compositions and (4) . The maximum depth of water circulation in AP spring is approximately 5 kilometres (Table 2).
[mathematical expression not reproducible] (4)
where d is the depth of water circulation (in km) and [DELTA] is [delta][sup.18]O or [delta][sup.2]H isotopes difference (in [per thousand]) between hot water and cold water spring in the study area.
The DIC and DOC concentrations in AP hot spring are 91 and 3 mg[L.sup.-1], respectively. The high amount of DIC and its enriched [delta][sup.13]C value (-1.3% VDPB) indicate carbonate dissolution in the geothermally heated water flow path. As illustrated in Figure 9, the [sup.13]C-DIC isotope in AP spring is analogous to the range of [sup.13]C derived from carbonate dissolution . Therefore, the Tirgan marine carbonate formation (with [delta][sup.13]C content about 0%) is probably the main recharge source of the AP spring. Meteoric waters percolated through the Tirgan limestone via faults and discharged from the AP spring after passing through underground karst systems. The very low amount of DOC in the AP spring (3 mg[L.sup.-1]) with [delta][sup.13]C-DOC value of -21.4[per thousand] VDPB probably originated from organics in the Sanganeh Formation.
According to geological, hydrogeochemical, and stable isotope studies the AP spring can be classified as a steam heated waters type. The main heat source for the high water temperature (38[degrees]C) in this spring is the geothermal gradient. Using [sup.18]O and [sup.2]H the origin of the water is meteoric which has penetrated via deep faults/dissolution conduits in the study area. Meteoric waters percolated through the Tirgan marine carbonate formation (with [delta][sup.13]C content about 0%) via faults and discharged from the AP spring after passing through underground karst systems. This can be confirmed by high amount of DIC and its enriched [delta][sup.13]C value (-1.3% VDPB). The deep circulation of water in this area can be inferred via high concentration of HC[O.sub.3], Ca, Mg; CaS[O.sub.4] water type; thermogenic travertine and high amount of C[O.sub.2] gas; and thermal anomaly as well. The region is tectonized and has many folds, such as Asiazow anticline which is the main recharge zone of the AP springs. According to Na-K geothermometry, modelling, and stable isotope analyses, the depth of the AP hot spring geothermal reservoir is estimated to be 4-5 kilometres with a temperature of about 150[degrees]C. This great depth combined with the water type suggests a hypogenic karst system signature that needs more investigation.
The authors declare that there is no conflict of interests regarding the publication of this paper.
The authors would like to thank Northern Khorasan Regional Water Company (NKRWC), Groundwater Research Center (GRC) of Ferdowsi University of Mashhad and Ottawa University geochemistry, and G. G. Hatch Stable Isotope laboratories for their help on sampling and sample analysis. They also thank Dr. Matt Herod for reviewing the manuscript and appreciate Mr. Asghari and Mr. Alizadeh's assistance during field work. Financial support was partially provided by NKRWC (CN: KNW89098).
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Hossein Mohammadzadeh and Majid Kazemi
Groundwater Research Center (GRC), Department of Geology, Faculty of Science, Ferdowsi University of Mashhad, P.O. Box 91775-1436, Mashhad, Iran
Correspondence should be addressed to Hossein Mohammadzadeh; email@example.com
Received 8 September 2016; Accepted 29 January 2017; Published 12 March 2017
Academic Editor: Marco Petitta
Caption: FIGURE 1: The study area and the locations of the Ayub-Peighambar and Shafa (AP and SH) hot springs.
Caption: FIGURE 2: (a) Sampling locations and the geological map of the study area and (b) the simulated photographs of (A) Kuh-e-Asiazow anticline; the fold axis with E-W trend has ~15[degrees] plunge to the west. The thrust plane is shown as pink sheets; the view is to the southeast, and (B) a fold-thrust fault in Sanganeh shale and marl, view is to the east .
Caption: FIGURE 3: Travertines hand samples, thin sections, SEM images, and EDX result.
Caption: FIGURE 4: Situation of water samples in the study area on a piper diagram (red circles detect AP and SH hot spring).
Caption: FIGURE 5: Triangular Cl-HC[O.sub.3]-S[O.sub.4] diagram that detects source waters of AP and SH hot springs (a) and other water resources (b) in study area.
Caption: FIGURE 6: The thermal anomalies map of the study area.
Caption: FIGURE 7: Biotite in matrix of quartz in AP spring's sediment.
Caption: FIGURE 8: The range of [delta][sup.18]O (a) and [delta][sup.2]H (b) compositions in various crustal rock and water types  and the range of [delta][sup.18]O and [delta][sup.2]H in the AP hot spring and cold water springs in the study area.
Caption: FIGURE 9: [The [delta].sup.13]C-DIC and [[delta].sub.13]C-DOC in AP hot spring.
TABLE 1: Field parameters, major anion and cation compositions, and isotopic compositions of AP and SH hot spring and adjacent springs. Sample Field ID parameter TDS EC PH T DO Eh (mg[L.sup.-1]) (ms/cm) ([degrees] (% sat) (mv) C) Sp. 1 247 499 8.0 25.0 -- 82 Sp. 2 443 953 8.1 18.0 -- 112 Sp. 3 307 626 7.6 16.9 146 141 Sp. 4 372 782 7.1 14.0 -- 173 Sp. 5 146 334 7.7 16.9 -- 195 Sp. 6 218 444 7.7 12.1 204 184 Sp. 7 296 604 7.5 17.2 137 173 Sp. 8 550 1120 7.5 38.0 65 -22 Sp. 9 770 1559 7.1 21.0 55 104 Sp. 10 469 957 7.3 36.0 19 -72 Sp. 11 454 930 8.3 16.0 -- 58 Sp. 12 404 825 8.1 25.0 -- 131 Sp. 13 780 1591 7.6 22.3 89 196 Sp. 14 615 1256 7.3 16.4 45 112 R. 1 285 581 8.4 22.7 134 150 R. 2 251 511 8.3 26.4 129 134 R. 3 966 1971 8.1 27.0 97 166 R. 4 1280 2612 8.0 29.9 107 135 R. 5 840 1714 8.3 25.5 159 129 W. 1 349 713 7.4 16.4 -- 101 W. 2 462 978 7.1 18.6 92 101 Sample Cations ID (mg[L.sup.-1]) [Ca.sup.+2] [Mg.sup.+] [Na.sup.+] [K.sup.+] Sp. 1 104 33 67 3.1 Sp. 2 147 49 109 3.7 Sp. 3 110 28 84 3.6 Sp. 4 70 250 3 0.0 Sp. 5 89 41 94 3.4 Sp. 6 60 48 34 1.8 Sp. 7 71 52 59 3.4 Sp. 8 87 42 96 3.2 Sp. 9 188 84 170 29.6 Sp. 10 67 40 75 2.1 Sp. 11 280 346 9 17.4 Sp. 12 81 52 99 2.7 Sp. 13 312 552 228 4.0 Sp. 14 230 440 224 0.0 R. 1 53 43 52 1.4 R. 2 172 130 128 64.0 R. 3 318 542 164 16.0 R. 4 30 750 202 26.1 R. 5 360 360 184 21.7 W. 1 190 330 244 8.7 W. 2 200 190 240 13.0 Sample Cations Anions ID (mg[L.sup.-1]) (mg[L.sup.-1]) C[O.sub.3.sup.-2] HC[O.sub.3.sup.-] S[O.sub.4.sup.-2] Sp. 1 16.0 184 130 Sp. 2 0.0 284 336 Sp. 3 24.0 150 234 Sp. 4 28.0 176 36 Sp. 5 64.0 110 343 Sp. 6 80.0 160 85 Sp. 7 60.0 170 172 Sp. 8 16.0 184 349 Sp. 9 8.0 286 707 Sp. 10 4.0 190 263 Sp. 11 56.0 256 423 Sp. 12 24.0 196 392 Sp. 13 21.7 10 695 Sp. 14 21.7 10 366 R. 1 72.0 110 142 R. 2 26.1 5 145 R. 3 4.3 11 880 R. 4 26.1 13 980 R. 5 4.3 11 640 W. 1 26.1 6 280 W. 2 21.7 8 445 Sample Anions Isotope ID (mg[L.sup.-1]) ([per thousand] VSMOW) [Cl.sup.2] [delta] [delta] [sup.2]H [sup.18]O Sp. 1 8 -62.6 -9.0 Sp. 2 35 -61.8 -8.5 Sp. 3 46 -58.8 -8.3 Sp. 4 6 -66.2 -9.4 Sp. 5 49 -70.5 -9.9 Sp. 6 9 -65.6 -9.3 Sp. 7 21 -66.4 -9.1 Sp. 8 43 -73.0 -9.9 Sp. 9 166 -71.8 -9.9 Sp. 10 37 -73.1 -10.2 Sp. 11 52 -- -- Sp. 12 38 -65.3 -8.8 Sp. 13 127 -- -- Sp. 14 32 -- -- R. 1 31 -72.1 -10.1 R. 2 42 -- -- R. 3 75 -- -- R. 4 131 -- -- R. 5 99 -- -- W. 1 44 -- -- W. 2 48 -- -- TABLE 2: Temperatures and depths of hydrothermal reservoirs for AP and SH hot springs, calculated based on Na-K geothermometers [28,31], Aq.QA hydrochemical software , and isotopic method. Ayub Peighambar hot spring Sp8.1 Sp8.2 Sp8.3 Sp8.4 Sp8.5 Using Aq.QA hydrogeochemistry software Temperature (Na-K) <150 <150 <150 <150 <150 Depth (km) * <5 <5 <5 <5 <5 Depth (km) ** 4.65 4.65 4.65 4.65 4.65 Using Mohammadi's  method Temperature (Na-K) 113 114 114 110 111 Depth (km) * 3.76 3.80 3.82 3.66 3.70 Depth (km) ** 3.42 3.45 3.47 3.31 3.35 Isotopic method (all isotope data in % VSMOW) In cold In hot Difference spring spring ([DELTA]) [delta][sup.18]O -9.29 -9.97 -0.68 [delta][sup.2]H -66.47 -73.0 -6.53 Shafa hot spring Sp10.1 Sp10.2 Using Aq.QA hydrogeochemistry software Temperature (Na-K) <150 <150 Depth (km) * <5 <5 Depth (km) ** 4.65 4.65 Using Mohammadi's  method Temperature (Na-K) 101 101 Depth (km) * 3.36 3.36 Depth (km) ** 3.02 3.02 Isotopic method (all isotope data in % VSMOW) Max depth (km) of water circulation [delta][sup.18]O 4.16 [delta][sup.2]H 3.66 * Based on general law of geothermal gradient (30[degrees]C/km). ** Using Marques et al.  approach.
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|Author:||Mohammadzadeh, Hossein; Kazemi, Majid|
|Date:||Jan 1, 2017|
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