Figure
1.
Location of the borate districts and Neogene basins in western Turkey (modified from Helvacı and Orti, 1998).
| Citation: | Şükrü Koç, Özge Kavrazlı, İsmail Koçak. Geochemistry of Kestelek Colemanite Deposit, Bursa, Turkey. Journal of Earth Science, 2017, 28(1): 63-77. doi: 10.1007/s12583-015-0616-x
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Turkey has about 72% of total global borate reserves. These reserves are located in Kestelek (Bursa), Bigadiç (Balıkesir), Kırka (Eskişehir) and Emet (Kütahya) in the western Anatolia (Fig. 1).
According to previous studies, all borate deposits in Turkey including the Kestelek deposit, were formed in Miocene lakes associated with volcanic activity which started in Paleogene and lasted to the beginning of Quaternary (Erkül et al., 2005; Helvacı, 2004, 2003; Helvacı and Alonso, 2000; Floyd et al., 1998; Helvacı and Orti, 1998; Helvacı, 1995; Kistler and Helvacı, 1994; Helvacı and Alaca 1991; Akyol and Akgün, 1990; Helvacı and Dora, 1985; Helvacı, 1983; Yılmaz et al., 1982; Özpeker and İnan, 1978; İnan, 1975; Özpeker, 1969; Meixner, 1956; Helke, 1955). Helvacı (2001) stated that colemanite is the dominant mineral in the Kestelek deposit which is followed in decreasing abundances by ulexite, probertite and hydroboracite which are accompanied by quartz, zeolite and montmorillonite group minerals. As outlined above, only geologic and mineralogic studies have been conducted at the Kestelek deposit. There are a few geochemical studies which include B, Sr, Li and As analysis on a trachyandesite sample from the Kestelek deposit (Helvacı and Alonso, 2000) and major element geochemistry of tuff and tuffaceous rocks in borate deposits in the western Anatolia (Helvacı et al., 1993). In addition, Koçak (1989) suggested that Li is particularly enriched in montmorillonite within the borate deposits and new studies are needed to extract Li from this mineral. In another study by Helvacı et al. (2004) Li2O content of clay minerals in the Kestelek deposit was found as 0.15%-0.17% while that of waste rock and tailings was determined to be 0.22%. In summary, there has been no comprehensive study on major and trace element geochemistry of colemanite samples from the Kestelek deposit in the western Anatolia.
The authors conducted a series of projects on borate deposits in western Anatolia. For example, in a study on geochemical characteristics of Bigadiç borate deposit, Koçak and Koç (2012, 2011, 2009) examined major and trace element geochemistry of borate minerals and their enrichment levels. Moreover, Se, Sr, Li, Sb and Mo were found to be significantly enriched with respect to average values of earth crust and andesite. Results of a previous study on Kestelek deposit are discussed in Koç et al. (2008a, b, c) and Koçak and Koç (2011) and presented in the present study.
In this study, major and trace element geochemistry of Kestelek borates are examined. In this concept, principally, recharge and depositional conditions of borate formation are evaluated on the basis of geochemical data. First of all, major and trace element (including REE) contents and enrichments of borate minerals are investigated. Using cross correlations, the origin of elements is discussed and physicochemical conditions of depositional environment are explained based on REE abundances and anomalies. The depth-dependent variations in element concentrations are also determined with the use of core data from boreholes.
A total of 6 surface samples and 16 samples from boreholes SK1 (Ö.S.-7), SK78 (Ö.S.-1), SK57 (Ö.S.-2), SK66 (Ö.S.-4), SK76 (Ö.S.-6) and SK18 (Ö.S.-5) provided by the Kestelek Bor Exploitation Management comprise the material of this study. Data from these boreholes were correlated and samplings from different depths were considered to be a single borehole data (Fig. 4). All collected samples are only crystal masses from boron-bearing levels. Before the analysis, samples were cleaned by pressured air and then washed to remove clay particles. Geochemical analysis was conducted at Automaticity in Cognition Motivation & Evaluation (ACME) laboratory and laboratory of Development of Technology Department of Eti Maden General Directorate. Analysis at ACME laboratory was conducted with inductively coupled plasma-mass spectrometry (ICP-MS) method which comprises of 53 elements. The analyses conducted with inductively coupled plasma-emission spectrometry (ICP-ES) and ICP-MS methods cover major oxides, trace elements and REE elements. In this study, major and trace element terms are used with respect to terminology for silicate rocks and, in fact, regarding concentration level, Ca and Si are considered as the major elements while others are minor or trace elements. Results of major elements in the elemental form are given in Table S1.
B2O3analysis was carried out at the Laboratory of Development of Technology Department of Eti Maden General Directorate. After powdering, 0.5 g sample was dissolved by heating. It was titrated with 0.5 N NaOH phenolphthalein indicator and B2O3% was found from the following formula
| %B2O3=0.017405×FNaOH×VNaOHT×100 |
where FNaOH=NaOH factor, VNaOH=0.5 N NaOH consumption, T=amount of sample, 0.017 405=amount of B2O3 for 1 mol NaOH.
In the mineralogic examinations petrographic microscope, X-ray diffractometer and confocal Raman method were used. XRD studies were conducted with Rigaku D brand max 2200 Ultima/PC device at the laboratory of Turkish Petroleum Corporation (TPAO). The Raman studies were conducted on unclosed thin sections with the use of Olympus BX41 confocal Raman spectrometer at the Petrography Research and Application Laboratory of the Geology Department of Ankara University. In order to determine clay assemblage associated with Kestelek colemanites X-ray diffractometer (XRD) method was used. For this, samples were sieved through 0.062 mm sieve at TPAO Laboratory. Powder mounts were prepared from the grinded mass. Oriented clays obtained by mechanical and chemical methods were packed on channeled glass. Whole rock and clay mounts were analyzed for both ethylene-glycolation and heating conditions. X-ray diffractograms were evaluated together. Diffractograms were obtained with the use of Rigaku D/max 2200 Ultima+/PC brand XRD device and Cu target at conditions of 40 KV, 20 mA, 1.540 59 Å (CuKα1) wave length and 2º/min scan speed. Results were evaluated using the Jade-7.0 program with respect to ICCD (International Centre for Diffraction Data) and ICSD (Inorganic Crystal Structure Database).
The Kestelek borate deposit is located 28 km southeast of Mustafa Kemalpaşa Town of the city of Bursa. In previous studies on Kestelek colemanite deposit and its surrounding areas (Helvacı, 1992; Koçak, 1989; Özpeker, 1969), stratigraphic sequence was described as pre-Miocene basement rocks and overlying unconformable Neogene units (Figs. 2-3). In this study, geological description of the Kestelek borate deposit is taken from Koçak (1989) who described Neogene units in detail.
In stratigraphic section of Koçak (1989) (Fig. 4), Paleozoic schists are the oldest rocks of pre-Miocene basement units. Schists are unconformably overlain by Triassic greywacke and metasandstones which are also unconformably covered with Jurassic limestones. Upper Cretaceous serpentinite and radiolarites set above these units with a tectonic contact. The Neogene units that unconformably rest on all these rocks are divided into 6 different lithologic units as Neogene lower units (Neogene Lower-1 and Neogene Lower-2) and Neogene upper units (Neogene Upper-1, Neogene Upper-2, Neogene Upper-3 and Neogene Upper-4). The Plio-Quaternary and Quaternary formations unconformably lie on the upper most part of sequence. In the stratigraphic sequence, volcanites are observed in Upper Neogene borate level and as lavas of andesite and rhyolite composition and tuff and agglomerate to the top. As shown in Fig. 1b, Neogene lower and upper units are divided into several subgroups. The sequence starts with conglomerate and sandstone at the base and continues with clay with lignite levels, marl, limestone, tuff and agglomerate. Marl, limestone, tuff and borate deposition took place when the tectonic stability was established. During that period, increasing of volcanic activity resulted in formation of andesite and rhyolite and tuff and agglomerates were deposited together with sediments. The sequence is completed with loosely cemented conglomerate, sandstone and limestone alternation. These units are unconformably overlain by Plio-Quaternary reddish, loose, coarse pebble, clay and debris deposits. The upper most part is characterized by various Quaternary deposits. The borate levels under investigation are generally composed of clay-tuff-marl alternation which is accompanied by detritics, carbonates and volcanites.
Previous studies (Helvacı, 2001, 1992, 1983; Helvacı and Alonso, 2000; Koçak, 1989; İTÜ, 1985, 1982; Atan, 1981; Yalçınkaya and Afşar, 1980; Özpeker, 1969) explained the occurrence of borate deposit in a similar manner. As pointed out by Koçak (1989), Helvacı (1992), Helvacı and Alonso (2000) and Helvacı (2001), Kestelek borate deposit was formed during the Miocene in playa lakes developed in inter-mountainous closed basins associated with extensional regime and growth faults in volcanically and seismically active regions in western Turkey.
Due to extensional tectonism that was prevailed in the region during the Miocene, lakes were formed in depressional areas by block faulting and/or graben activity. In Kestelek, basal conglomerates were deposited in a narrow lacustrine environment. This was followed by a swamp regime that gave rise to formation of coal (lignite) deposits. Marl-clayey limestones above the coal layers indicate that the lake became deeper. By the starting of volcanic activity and humid regime in the Upper Miocene the lake was enlarged and coarse detritic materials from fluvial and shallow lacustrine environments were deposited in large areas. This facilitated reinstallation of swamp conditions and coal layers in some parts. The volcanism increased its activity and lake was deepened again and water covered wide areas where marl-clayey limestones with minute detritic material were deposited. Volcanic units such as andesite and rhyolite together with clay-marl-tuff-sandstone are predominated at the upper parts of the sequence. As a result of increase in the volcanic activity tuff, agglomerate and lavas were formed (Koçak, 1989).
By the ceasing of volcanic activity in the late Upper Miocene, the lake became shallow and stagnant where laminated clays, marls and tuffs were intercalated (Koçak, 1989). Boron-bearing hydrothermal solutions gave rise to formation of borate levels within the clay-tuff-marl alternations. Borate and clay-tuff-marl alternations of varying thickness indicate a depositional regime that repeatedly changes with respect to varying climatic conditions. Thinning tuff bands may also indicate that volcanism was continued as sporadic eruptions.
The climate was hot and dry during the course of borate formation and therefore the recharge/evaporation ratio was very low, the lake gradually shrunk. This is supported by wedging, laterally transitional and partly lacking lithologies.
In Pliocene, a thick sequence was formed due to rain-wash process consisting of conglomerate, sandstone, clay, volcanic interbeddings and carbonate rocks and the borate deposition was ceased. The lake attained its broadest extent and it shrunk and then became extinct at the end of Pliocene. In the meantime, the basin was uplifted and clay, sand, conglomerate and molasse were deposited and folding and faulting were formed (Koçak, 1989). Finally, travertine, terrace, mollase and alluvium materials were accumulated in the Quaternary and the basin gained its recent morphologic appearance (Koçak, 1989).
In previous studies (Koçak, 1989; İTÜ, 1985; Helvacı, 1983; Özpeker, 1969), ore levels, considering their different morphologic appearance, were examined in three levels (lower, middle and upper). In these levels, the main mineral is colemanite which is followed in decreasing abundances by ulexite, probertite and hydroboracite (Helvacı, 2001, 1983; Helvacı and Orti, 1998; Koçak, 1989; Özpeker, 1969).
In the present study, descriptions were made in accordance with classification of ore levels. Colemanite is the sole borate mineral. Macroscopically colemanite is colorless but is mostly white, yellow and gray colored and contains radial and nodular textures. In thin section, colemanite shows granular texture. Grains are euhedral, subhedral and generally anhedral.
Some colemanite thin sections contain calcite, aragonite, quartz and clay minerals. Most of samples are composed of pure colemanite crystals.
XRD determinations yield that the mineralization paragenesis is composed of colemanite, calcite, quartz, aragonite, smectite, illite, chlorite and corrensite (Figs. 5-6). In the Raman analysis, heulandite was also recorded. Based on XRD data, proportions of clay minerals are 80% smectite, 15% illite and about 5% chlorite. Corrensite is regular mixed layer form of smectite and illite and crystallizes in the lake water (Weaver and Pollard, 1973). We have no sufficient data to show that colemanite has a primary or secondary origin.
In this study, a detailed geochemical survey was conducted. The first step of this investigation is to determine depth-dependent variations of the environment based on the results of major, trace and REE element contents of samples collected from lower, middle and upper zones of the Kestelek deposit. Thus, element abundances in colemanite samples and their meanings are discussed. In addition, all major and trace elements were correlated with each other and element groups with similar patterns were determined. Moreover, depth-dependent variations in element contents were also examined. Rare earth element contents were also evaluated to determine physiochemical properties of colemanite depositional environment.
Abundances of major elements of Kestelek boron ore (colemanite) samples in ppm and wt.% are given in Table S1. In this table, concentration ranges for elements and the average concentrations of studied samples and those of earth crust, andesite and freshwaters are also presented. In the colemanite samples, major elements in the order of abundance are Ca (18.84 wt.%), Si (1.36 wt.%), Mg (5 923 ppm), Al (3 549 ppm), Fe (2 604 ppm), K (1 985 ppm), Na (686 ppm), Ti (295 ppm) and P (105 ppm) (Table S1). Comparison of these values with average concentrations of earth crust and andesite yields that, except for Ca, concentrations of all other elements decrease. Considering earth crust abundance, Ca increase 4.6 folds and other elements decrease at various rates (about 1 to 44 folds). Freshwater values of all major elements are much lower than those of lake water from which colemanite was deposited indicating that the environment received a considerable terrestrial or volcanic input. In volcanosedimentary ore deposits, high Al and Ti contents are indicative of sedimentary contribution (Choi and Hariya, 1992; Nicholson, 1990; Roy et al., 1990; Crerar et al., 1982; Bonatti et al., 1972). Concentrations of Al (3 549 ppm) and Ti (295 ppm) of Kestelek borate deposits are even lower than those of earth crust. That is why, there is no doubt that some amount of elements in the basin are of terrestrial origin but volcanic processes are the main agent to supply material to the lacustrine environment.
In borate deposition environments, the presence of some cations is important to define crystallization of certain minerals. In addition to some physicochemical conditions of the environment such as pH, temperature and concentration, the availability and abundance of Na, Ca and Mg are determinant. For example, Na2O/CaO ratios reveal the type of mineral to be crystallized. Based on fundamental studies on this matter (Christ et al., 1967; Bowser, 1964), some geochemical studies were conducted on Eskişehir (Turkey) borate deposits (Sunder, 1980; Baysal and Ataman, 1975; İnan, 1975). Results of these studies suggest that Ca-borates are formed with Na2O/CaO ratios less than 5%, Na-Ca borates with Na2O/CaO ratios of 5%-95% and Na borates with ratios above 95%. Ca content of Kestelek boron samples, except for sample Ö.-1 (18.67%), is around 19% and average Na concentration is 0.069% (Table S1). These data show that Na2O/CaO ratio is significantly less than 5% limit value and only Ca-borates can be formed in the basin. If Na content is quite high colemanite might be accompanied by Ca-Na and Ca-Mg borates. However, this is not the case at Kestelek. The absence of inyoite (Ca2B6O11·13H2O) and ulexite (Na2CaB5O9·8H2O) in the ore paragenesis shows that colemanite formation is associated with Na2O/CaO < 5%. Previously formed Ca-borates can be stable only if they are covered with clays or clastic material (İnan, 1975).
Depth-dependent variation of major elements is shown in Fig. 7 where borate ores are classified as lower, middle and upper ores and ranked in the diagram with respect to their depths. It is noticeable that curves of Na and Mg which are key cations for the borate formation are very similar and that of Ca is entirely different. Al, Si, Fe, Ti and K curves are very similar to those of Na and Mg. On the other hand, like Ca, P shows a different behavior with respect to entire group. The difference in P curves is particularly noticeable in the middle ore zone and phosphorus curves are somewhat consistent with those of entire group at lower and upper zones. The average Ca concentration in the Kestelek colemanite samples is 18.8%. Calcium is the dominant element for colemanite formation and with the exception of two samples its concentrations does not change with increasing depth. Although sample Ö.S.6-1 has the highest concentrations for all elements, Ca coserpantint of this sample is less than the average.
B2O3 concentrations were measured on 16 borehole samples (4 samples from the upper, 5 from the middle zone and 7 from the lower) (Table 1). The average B2O3content of deposit is 28.43%. Depth-dependent variation of B2O3concentration in the Kestelek borate deposit is illustrated in Fig. 8. As shown from this figure, borate content of deposit changes in time and the lowest concentrations are recorded in the middle ore zone. B2O3 content in the lower is slightly increased.
| Samples | B2O3 |
| Ö.S.4-1 | 32.36 |
| Ö.S.7-1 | 40.02 |
| Ö.S.2-1 | 30.45 |
| Ö.S.6-1 | 8.96 |
| Ö.S.1-1 | 18.79 |
| Ö.S.1-2 | 18.79 |
| Ö.S.7-2 | 34.12 |
| Ö.S.2-2 | 20.00 |
| Ö.S.6-2 | 15.31 |
| Ö.S.5-1 | 35.84 |
| Ö.S.5-2 | 35.84 |
| Ö.S.4-2 | 34.97 |
| Ö.S.1-3 | 16.01 |
| Ö.S.7-3 | 40.54 |
| Ö.S.2-3 | 44.81 |
| Ö.S.6-3 | 28.01 |
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In analysis of colemanite samples from the Kestelek borate deposit concentrations of 28 different trace elements were first reported in the present study. Results of trace element contents given in Table 3 are compared with their average abundances in earth crust, andesite and freshwater. These 28 elements are more enriched in colemanite samples than freshwater. On the other hand, except for Li, Cs, Sb, As, Sr and Se, element concentrations are much lower than average values of earth crust and andesite. The rate of decrease with respect to earth crust and andesite averages is 1-38 folds. The most decreased elements are Zr (24-38), Cu (27-19), Y (19-14), Ag (12-12), Ba (10-14), Co (8-4), Pb (8-10), Rb (6-5), U (4-3), Cr (4-2), Ni (3-4) in ppm, and Au (1-*) in ppb. Considering freshwaters averages, significant increases were recorded for all trace elements which are ranked with respect to coefficient of increase as Se (397 545), Sr (92 011), Li (54 900), Co (52 556), Ni (59 762), Cr (48 750), U (12 600), Sb (11 900), As (9 118), Pb (7 440), Cs (7 028), Zn (6 218), Ba (4 962), Hg (2 400), Mo (1 535), Cu (1 022) in ppm, and Au (306) and Ag (20) in ppb.
With respect to earth crust and andesite averages, Li (3-3), Cs (4-6), Sb (6-6), As (10-10), Sr (12-6), and Se (795-795) in ppm were considerably enriched in Kestelek colemanite samples.
Se, a chalcophile element, shows the highest enrichment. The concentration range of Se in the samples is 0.30 ppm-51.5 ppm with average of 39.75 ppm (Table S2). Considering that the average Se content in the earth crust and andesite is 0.05 ppm, Se concentration of Kestelek colemanite samples has increased about 795-folds. The main source of Se is volcanic activity, and therefore, it is mostly found in volcanic rocks, sulfur depositions, hydrothermal formations particularly epithermal Sb, Ag, Au and Hg (Halilova, 2004; Elkin and Margrave, 1968).
Because geochemical characteristics of Sr are similar to those of Ba, Ca and sometimes K, it is the second mostabundant element in the studied samples. The concentration range of Sr is2 074 ppm-8 626 ppm with average of 4 601 ppm. The average concentrations of Sr in earth crust, freshwater and andesite are 375 ppm, 50×10-3 ppm and 800 ppm (Table S2). In this respect, Sr has enriched 12-folds with respect to earth crust average, 92 011-folds with respect to freshwaters average and 6-folds with respect to andesite average. Sr might be incorporated into Kestelek colemanite deposit by dissolution of both magmatic and volcanic rocks. In the stage following the solidification of magma, Sr might be enriched in volatile-rich solutions (e.g., Cl, F, and B) and post-magmatic formations (Bürküt, 1977).
Although Kestelek borate ores (colemanite samples) contain significant amount of Sr, tunellite (SrB6O10·4H2O) is absent in the deposit. Sunder (1980) mentioned about primary tunellite formation in Sarıkaya area (Eskişehir, Turkey) which is crystallized at initial temperatures (25ºC) in lower and upper ulexite zones where Sr is supplied by exsolution. The fact that colemanite occurs at temperatures close to 40 ºC explains the absence of any other borate mineral or Sr-borate rather than colemanite at Kestelek.
The concentration range of As in Kestelek samples is 0.2 ppm-128 ppm with average of 18.24 ppm. In the Kestelek samples As is about 10-fold enriched with respect to earth curst and andesite averages (1.8-1.9). Considering the freshwater average (2×10-3) it is 9 118-fold enriched. Arsenic is a chalcophile element and derived from volcanic activity and hydrothermal solutions (Akçay, 2002).
The concentration range of Sb in Kestelek samples is 0.02 ppm-6.77 ppm with average of 1.14 ppm. Sb is about 6-fold enriched with respect to earth curst and andesite averages (0.2 ppm) and 11 900-fold enriched with respect to freshwater average (0.1×10-3ppm). Sb is a chalcophile element and very common at low-temperature hydrothermal (epithermal) stage. It is associated with As, Hg, Pb, Ag, Au, and Se. It is known that Sb is closely associated with volcanic activity (Petrascheck and Pohl, 1982).
The average concentrations of Cs in the earth crust and andesites are 3 ppm and 2.3 ppm, respectively. Cs content of Kestelek colemanites are in the range of 0.10 ppm-67.10 ppm with average of 11.5 ppm (Table S2). Based on this, Cs concentration has increased 4-6 folds. Cs is particularly found in K-bearing minerals and Li-bearing micas (Bürküt, 1977). The ionic radius of Cs, one of the largest alkali cations, is larger than that of major elements and however it can replace K. During the course of magmatic crystallization, Cs is in volatile phase and since it is more volatile than Rb and K, Cs is mostly found in K-rich volcanic rocks.
Li which was studied in Kestelek colemanites (Helvacı et al., 2004, 1993; Helvacı and Alonso, 2000; Koçak, 1989) has an average earth crust concentration of 20 ppm. As shown in Table S2, Li content of studied colemanite samples is 0.7 ppm-178 ppm. Considering the average concentration of 55 ppm, Li concentration of Kestelek samples has increased about 3-folds. In previous unpublished studies (Etibank), Li content of colemanites is reported to be in the range of 31 ppm-170 ppm.
Si, Mg, Al, Fe, K, Ti and P show strong-very strong positive correlations. Most of trace elements in Table S3 are also strongly positively correlated with these major elements and between each other. These trace elements are Cr, Cu, Zn, As, Rb, Zr, Mo, Sb, Cs, Hg, Pb, U, Co, Li, Y, Ni and REE. In addition, TOT/C and TOT/S show strong-very strong positive correlations with major and trace elements. Some major elements such as Si, Al and Ti and trace elements such as Cr, Zr and REE are resistant to alteration and indicate detrital origin (Fu et al., 2011; Boggs, 2009). Elements of this group were transported to the lake together with detrital clays.
Although the medium is oxygenated, there is a very strong positive correlation between Fe and TOT/S indicating an iron sulfur source. Phosphorus, which behaves like clay group, is negatively correlated with Ca (-0.60). This relation might indicate that P is not derived from apatite but transported to the basin via clay minerals.
B and Ca, which are the major components of colemanite samples, show weak positive correlation (0.43) (Table S3). The relation of these two elements with other elements is similar. For example, B does not correlate with Se, Sr and Te and Ca does not correlate with Sr, Au and Te. In addition, B and Ca are negatively correlated with all other elements which are a part of large group together with clays. Boron is weakly-very weakly negatively correlated while Ca is strongly-very strongly negatively correlated with members of this group. These relations imply the difference between B-Ca and elements of the large group. Particularly, strong negative correlation of Ca definitely shows genetic difference from the clay group. Weak to very weak correlation of B might indicate that this element is not derived from a single source. There is a weak positive correlation between Ca and Sr (0.50). However, B and Se are not correlated, indicating a genetic relation between Ca and Se.
Ca is weakly correlated with TOT/C (-0.48) and strongly correlated with TOT/S (-0.72). These relations imply that part of C in TOT/C is of organic origin and the origins of Ca and S are different and not derived from Ca-sulfate minerals.
Sr, Au and Te are not significantly correlated with other major and trace elements given in Table S3. Strontium is weakly positively correlated (0.20-0.43) with major and trace elements which are associated with clay minerals. Au and Te are correlated with none of the elements. Au only shows very weak-weak correlation with B (-0.45). All these indicate that Sr, Au and Te are not significantly related with other elements.
Evaluations on correlation coefficients (Table S3) and cluster analysis (Fig. 9) show that major and trace elements of Kestelek colemanite samples comprise three different groups. The first group is represented by major elements (Si, Mg, Al, Fe, K, Ti, and P) which are found in clays and associated trace elements (Cr, Cu, Zn, As, Rb, Zr, Mo, Sb, Cs, Hg, Pb, U, Co, Li, Y, Ni, and REE) and TOT/C and TOT/S. The second group is composed of B, Ca and Se which are negatively correlated with the first group elements. The third one consists of Sr, Au and Te triplet which are not correlated with previous groups.
Overall assessment of element correlations and geochemical behaviors explained in previous sections reveals some results regarding the genesis. Most of elements within the colemanite samples are of sulfidic character which indicates a contribution from exsolutions and hydrothermal solutions revealed by volcanic activity. However, it was determined in correlation analysis that most elements are associated with clays which is indicative of a detrital source. In this respect, both volcanism and terrestrial input must have influenced the formation of depositional environment. Among the elements most enriched in colemanite samples, As, Cs, Sb and Li are of detrital origin whilst Se together with B and Ca are of non-detrital origin. However, some part of B which shows weak positive correlation with Ca should have been transported with clays. Likewise, Sr has a detrital origin and is also associated with volcanic rocks.
REE’s with average abundances (in ppm) of La (2.29), Ce (4.36), Pr (0.41), Nd (2.13), Sm (0.48), Eu (0.12), Gd (0.37), Tb (0.06), Dy (0.34), Ho (0.11), Er (0.24), Yb (0.21), and Lu (0.04) show very low concentration trends (Table S4).
In order to examine physicochemical conditions of the deposition environment of Kestelek borates and genetic relations of elements, REE abundances were normalized with respect to PAAS (Post-Archean Australian Shales) average values. As shown from these diagrams constructed for upper, middle and lower zones (Fig. 10), samples show at least two distinct behaviors.
Regarding samples from the upper zone (Fig. 10a), there is no significant anomaly for three curves at the top and curves follow a flat pattern. Heavy rare earth elements (HREE) are slightly enriched in comparison to light rare earth elements (LREE). Some anomalies are clearly shown in REE contents of samples at the lower zone. In these curves Ce displays negative but Eu and Ho display positive anomalies. Ce anomaly reflects the redox character of the environment. The negative Ce anomaly shows that the environment has a high oxygen fugacity value (fO2) and Eu anomaly reflects a hydrothermal source (Canet et al., 2005; Constantopoulos, 1988). Nance and Taylor (1977), Bhatia (1985) and Sant’Anna et al. (2006) stated that positive Eu anomaly is an indicator of magmatic source. The positive Eu anomaly also indicates the presence of CO2 (Gale et al., 1997; Graf, 1977) which can be associated with CO2 produced by volcanic exsolutions. Due to similarity in ionic radius of Ho and Ca, these elements are expected to show positive correlation in colemanite samples.
Curves of middle and lower zones are mostly similar (Figs. 10b-10c). Samples in upper part of both ore zones are represented by a flat pattern. However, some anomalies are noticeable in lower curves. For example, although not significant as for the samples from the upper zone, there is a negative Ce anomaly. As in the samples from the upper zone, positive Eu and Ho anomalies are conspicuous. Unlike the upper zone, one of the samples from the middle and lower zones displays negative Pranomaly.
In general, samples are enriched in LREE and MREE. LREE’s are more stable than HREE’s (Cantrell and Bryne, 1987). Enrichment of LREE’s might indicate redeposition of REE’s by washing out in any part of hydrothermal system. Enrichment of MREE’s is characteristic to natural fluids and acidic washing out (Johannesson et al., 1996; Fee et al., 1992). REE compositions from the intermediate acidic rocks are represented by positive Eu anomaly and MREE enrichment (Johannesson et al., 1996).
Based on the results of REE contents of upper, middle and lower ore zones (Table S3), La/Lu ratios > 1 (71.6, 90.6 and 82.7 for upper, middle and lower zones, respectively) and positive Eu anomaly is apparent which is indicative of intermediate acidic and high-temperature conditions (Bau, 1991).
The fact that REE’s show at least two groups of trends imply at least two different depositional regimes. For depositional conditions represented by flat lines REE’s are mostly unchanged. These lines belong to pure crystal and carbonate-bearing ore samples. The second group of curves which displays significant anomalies belongs to clay-bearing and nodular ore samples and is characterized by depositional conditions with high oxygen fugacity and negative Ce and positive Eu anomalies indicating hydrothermal contribution.
The Kestelek borate deposit was formed during the Miocene in playa lakes of an intermountain basin which was developed at the beginning of Paleogene in volcanically and seismically active basins associated with growth faults and grabens affected the western Anatolia (Helvacı and Alonso, 2000; Helvacı, 1992; Koçak, 1989). In response to climatic changes, this lacustrine basin deepened, broadened, became shallow and shrank from time to time. The effect of volcanism which was very active at the beginning of Miocene diminished in the Upper Miocene. Borate deposits of varying thickness alternated with volcanosedimentary units and clay-tuff-marl deposits are indicative of frequently changing climate regime. Thinning tuff band shows that volcanism continued in small pulses.
Colemanite is the sole borate mineral in the paragenesis of deposit. It is accompanied by lesser amount of calcite, aragonite, smectite, illite, chlorite, corrensite, heulandite and quartz. Inyoite and ulexite which are observed in other borate deposits are absent at Kestelek. These minerals are preserved since Ca-borate is covered with clay, tuff and marl.
XRD analysis of colemanite samples shows that accompanying clay minerals are composed of 80% smectite, 15% illite and about 5% chlorite. In addition, diffractograms of clay samples reveal trace amount of corrensite.
The average values of major elements recorded in the Kestelek boron ore (colemanite), in the order of abundance, are Ca (18.84 wt.%), Si (1.36 wt.%), Mg (5 923 ppm), Al (3 549 ppm), Fe (2 604 ppm), K (1 985 ppm), Na (686 ppm), Ti (295 ppm) and P (105 ppm). Except for Ca, concentrations of all major elements decrease with respect to average concentrations of earth crust and andesite.
In this study, concentrations of 28 trace elements were examined in colemanite samples (Table S2). Based on the average concentrations of earth crust and andesite, with the exception of Li, Cs, Sb, As, Sr, and Se, significant decreases were observed in concentrations of all other trace elements. Although Kestelek borate deposit was formed in a lacustrine environment, major and trace element concentrations of colemanite samples are found to be considerably enriched with respect to freshwater averages. Among the trace elements Li, Cs, Sb, As, Sr and particularly Se are significantly enriched in the samples.
Correlation analysis indicates two different sources for the elements: (a) detrital origin for Al, Ti, Si, Mg, K, Fe, P, Cr, Cu, Zn, As, Rb, Zr, Mo, Sb, Cs, Hg, Pb, U, Co, Li, Ni, and REE. TOT/C and TOT/S are also included in this group, (b) non-detrital group for B, Ca and Se which are negatively correlated with the elements of previous group. However, negative correlation of B is at weak-very weak level which might indicate that boron is mostly derived from volcanism (e.g., hydrothermal solutions, exsolutions) and partly from a detrital source (surrounding volcanic rocks). The strong correlation of Ca with TOT/S shows that sulfur is of volcanic origin rather than derivation from Ca-sulfate minerals. Weak correlation of TOT/C indicates the presence of some amount of organic C in the total carbon.
Element groups determined in depth-dependent variations are greatly similar to those observed in correlation analysis.
Distribution diagrams of rare earth elements imply that there are at least two different depositional regimes which are also clearly supported by two different grouping of curves. Flat curves represent depositional conditions where REE’s mostly remain unchanged. These curves belong to pure crystal or carbonate-bearing ore samples. The second group of curves which is characterized by several significant anomalies is from clay-bearing samples and nodular ore samples. They are indicative of a depositional regime with high oxygen fugacity and characterized by negative Ce and positive Eu anomalies showing a hydrothermal contribution.
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Figures(10) / Tables(1)
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Şükrü Koç, Özge Kavrazlı, İsmail Koçak. Geochemistry of Kestelek Colemanite Deposit, Bursa, Turkey. Journal of Earth Science, 2017, 28(1): 63-77. doi: 10.1007/s12583-015-0616-x
| Samples | B2O3 |
| Ö.S.4-1 | 32.36 |
| Ö.S.7-1 | 40.02 |
| Ö.S.2-1 | 30.45 |
| Ö.S.6-1 | 8.96 |
| Ö.S.1-1 | 18.79 |
| Ö.S.1-2 | 18.79 |
| Ö.S.7-2 | 34.12 |
| Ö.S.2-2 | 20.00 |
| Ö.S.6-2 | 15.31 |
| Ö.S.5-1 | 35.84 |
| Ö.S.5-2 | 35.84 |
| Ö.S.4-2 | 34.97 |
| Ö.S.1-3 | 16.01 |
| Ö.S.7-3 | 40.54 |
| Ö.S.2-3 | 44.81 |
| Ö.S.6-3 | 28.01 |
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