Baroque dolomites and others geode-like sparry carbonates occur. The principal mineralogical association of these syn- and late-diagenetic mineralizations ...
Mineral. Deposita 31, 84-92 (1996)
MINERALIUM DEPOSITA 9 Springer-Vedag 1996
Lead isotope study of Zn-Pb ore deposits associated with the Basque-Cantabrian basin and Paleozoic basement, Northern Spain F. Velasco, A. Pesquera, J.M. Herrero Departamento de Mineralogia y Petrologia. Universidad del Pals Vasco, Apdo. 644, E-48080 Bilbao, Spain Received: 1 November 1993/Accepted: 3 February 1995
Abstract. A total of forty-three galena samples from syngenetic and epigenetic Pb-Zn mineralizations emplaced in the Lower Cretaceous Basque-Cantabrian basin and Paleozoic basement of the Cinco Villas massif in the western Pyrenees, have been analyzed for Pb-isotopic composition. Galena from sedex mineralizations hosted in Carboniferous clastic rocks in the Cinco Villas massif display an homogeneous lead isotopic signature (2~176 ~ 18.43, 2~176 ,,~ 15.66, 2~ 2~ ~ 38.69) suggesting a single lead reservoir. These values are slightly more radiogenic than lead from other European Hercynian deposits, possibly reflecting the influence of a more evolved upper crustal source. Underlying Paleozoic sediments are proposed as lead source for the Cinco Villas massif ores. Analyses from twenty-six galena samples from the four strata-bound ore districts hosted in Mesozoic rocks reveal the existence of two populations regarding their lead isotopic composition. Galena from the western Santander districts (e.g., Reocin) is characterized by more radiogenic isotope values (z~176 ~ 18.74, 2~176 ~ 15.67, 2~ 2~ ~ 38.73) than those from the central and eastern districts (Troya-Legorreta, Central and Western Vizcaya, 2~176 ~ 18.59, 2~176 ~ 15.66, 2~ 2~ ~ 38.73). In all districts, the most likely source for these mineralizations was the thick sequence of Lower Cretaceous clastic sediments. The existence of two separate lead isotopic populations could be the result of regional difference in the composition of the basement rocks and the clastic sediments derived of it or different evolution histories. In both sub-basins, isotopic ratios indicate an increase in crustal influence as the age of the ores decreases.
In the western Pyrenees and in the Basque-Cantabrian basin, northern Spain, sediment-hosted Zn-Pb deposits are found in two geological settings: (1) Carboniferous clastic metasediments in the Cinco Villas massif, and (2) carbonate rocks of Lower Cretaceous age deposited at platform margins. Pb-Zn mineralizations also are known
in a third geological area setting, the Paleozoic Sierra de la Demanda massif, located south of the Lower Cretaceous Basque-Cantabrian basin (Fig. 1). The first setting includes sedex ore deposits affected by Hercynian regional deformation and metamorphism with subsequent remobilization processes (Pesquera 1985; Pesquera and Velasco 1989, 1993). In the second geological area, i.e. in the Lower Cretaceous carbonate rocks, Mississippi Valley-type and sedex ore deposits occur (Herrero and Velasco 1988; Herrero 1989; Velasco et al. 1993). The purpose of this contribution is to present lead isotope data for forty-three galena samples from both groups of sediment-hosted Zn-Pb deposits in the western Pyrenees and Basque-Cantabrian basin in order to investigate possible lead sources and genetic models. In addition, five galena samples from occurrences in Cambrian rocks of the Sierra de la Demanda were also studied with the aim of obtaining the first data about the lead isotopic composition of this Paleozoic massif, which is a possible lead source. A relatively broad comparison exists for the deposits hosted in Paleozoic rocks with similar studies in ore deposits in France, the Alps and the Central Europe (see references late). In contrast, lead isotope data from European ore deposits hosted in Cretaceous sedimentary rocks are scarce.
Ore deposits and geological setting The Paleozoic Cinco Villas massif The Paleozoic Cinco Villas massif, and the Labourd and Alduides massifs, represent the Hercynian basement at the western part of the Alpine belt of the Pyrenees (Fig. 1). The NNE-trending Pamplona fault separates the Cinco Villas and the Alduides massifs. The important Marble Slip Sheet or Leiza Fault, a possible continuation of the north Pyrenean Fault (Ducasse et al. 1986; Rat 1988) borders the Cinco Villas massif on the south. Two main Carboniferous sedimentary formations occur in the Cinco Villas massif: a lower one, Aranaz Limestone Formation of possible Namurian age (Heddebaut 1973) which crop out in the central area of the massif, and an upper one, Cinco Villas Formation
85
Fig. 1. Geological sketch map of the Basque-Cantabrian region (northern Spain) showing the location of Santander (1), Western Vizcaya (2), Bilbao (3), Central (4), Troya (5), Arditurri (6), and Demanda (7) districts and other Zn-Pb mineralizations(Velasco et al. 1993). Numbers of the districts and ore deposits correspond to Pb-isotope data listed in Table 1
dated as Westphalian (Requadt et al. 1977) consisting of clastic sedimentary rocks, including mainly shales and sandstones, with minor conglomerates and interlayered limestones. During the Hercynian deformation of these rocks isoclinal folding, schistosity and low grade regional metamorphism developed, locally reaching maximum temperatures close to 450~ (Pesquera and Velasco 1988). A syntectonic calco-alkaline granitoid (Pesquera 1985; Pesquera and Pons 1989), the Aya pluton, has intruded in the northern area. Subordinate mafic dikes and sills are present. In the Cinco Villas massif the most important mining districts were Arditurri and Vera de Bidasoa-Modesta; extractive activity stopped in 1984. They are Sedex-type deposits (Pesquera et al. 1985; Pesquera and Velasco 1989, 1993) hosted by clastic metasediments of the Cinco Villas Formation. The ore is dominantly banded and consists of sphalerite, galena, fluorite, barite, siderite, pyrite, chalcopyrite, calcite and quartz. Some depositional textures are preserved but the regional low grade metamorphism and ductile deformations have lead to widespread recrystallization and local remobilization. Some of the deposits are located in the vicinity of Aya pluton and previous studies (Pesquera and Velasco 1979; Herrero et al. 1981) postulated a genetic association with fluids derived from the granite. However, new observations and studies support an exhalatire-sedimentary character and preintrusive origin for these ore deposits (Pesquera et al. 1985; Pesquera and Velasco 1989, 1993). These deposits present some analogies with Zn-Pb ores in Ordovieian and Devonian rocks of the central Pyrenees (Pouit 1978;
Pouit and Bois 1986) and with ores in Cambrian rocks in the Sierra de la Demanda.
Sierra de la Demanda The Paleozoic stratigraphic sequence of the Sierra de la Demanda includes Cambrian, Ordovician and Carboniferous metasediments, mainly sandstones and shales with occasional dolostone beds in the lower part. These Paleozoic rocks have been affected by three Hercynian deformation phases accompanied by a low to very low grade regional metamorphism (Colchen 1974). Zn-Pb mineralizations can be largely divided into three groups (Ibifiez et al. 1993) comprising deformed and metamorphosed deposits, probably of sedex character (e.g. Carmina mine), Fe-Ni-Cu-bearing vein-type deposits, and late cross-cutting galena-rich mineralizations (e.g. Najerilla, St. Cristdbal).
The Lower Cretaceous Basque-Cantabrian basin In the Basque-Cantabrian region important thicknesses of Mesozoic sedimentation resulted from the opening of an intra-plaque basin beginning at 250 Ma (Rat 1988), i.e. before the opening of the
86 central Atlantic. Lying over Paleozoic rocks similar to those described at the Cinco Villas massif, the Mesozoic sequence starts with Triassic clastic and carbonate rocks with significant evaporite intercalation that developed diapiric domes. Some mafic volcanic rocks are also found. Jurassic platform carbonates follow. The Upper Jurassic-Lower Cretaceous represents a period with thick deposits of sediments, in the central part of the basin, arranged in three main complexes (Rat 1959): the continental clastic "Wealden" (shale and sandstones of Upper Jurassic-Barremian age), the extremely variable and well-developed sedimentation of carbonate ramp called "Urgonian" facies (constituted by platform limestones and basin marls and mudstones with siliciclastics intercalations, aged Aptian-Albian), and another terrigenous episode ranging from fluvial to deep turbiditic sedimentation ("Supra-Urgonian", Upper Albian-Lower Cenomanian). Upper Albian to Cenomanian alkaline flows of submarine volcanic and volcanoclastic rocks (Azambre and Rossy 1976) locally occur interlayered with flysch turbidites and platform carbonates. Upper Cretaceous platforms are well represented in the southern area of Basque-Cantabrian basin. The stratigraphy and sedimentology of the Lower Cretaceous rocks, host of the ore deposits under discussion, have been studied mainly by Rat (1959,1983), Pujalte (1977), Garcia-Mondejar, (1979,1990a, 1990b), Pascal (1985) and Fernfindez-Mendiola (1986). According to these authors, the carbonate platform and clastic sedimentation were mostly governed by synsedimentary tectonics and two main sub-basins developed: the peri-Asturian area (Cantabrian graben) and the Bilbao graben (Rat, 1988). Thickness and sedimentary facies variations indicate that these sub-basins behaved independently. The majority of ore deposits and occurrences are strata-bound and hosted in carbonate formations of two ages: BedoulianGargasian limestones (e.g. Reocin mine, Troya mine), and Lower Albian carbonate rocks (e.g. Legorreta mine, Western Vizcaya district). Several metallogenic studies have been carried out in this region (Vadala et al. 1981; Herrero et al. 1987; Herrero and Velasco 1988, 1989; Herrero 1989; Gil 1991; Velasco et al. 1993; FernandezMartinez 1994). Geographically, Zn-Pb deposits are grouped in four populations: Santander district, Western Vizcaya district, Central area, and Troya-Legorreta district (Fig. 1). These are classified into three types, mainly based on the morphology, features, mineralogy and age of the host stratigraphic rocks: strata-bound, vein, and diapir related mineralizations (Velasco et al. 1993). Iron carbonates are the only ore minerals in some deposits located mainly in the central part of the basin (Bilbao district, Gil 1991). The strata-bound ores show replacement, overgrowth, collomorphic grapelike, breccia zones and cross-cutting, disseminations, collapse breccia, diagenetic recrystallization and banded and brecciated textures. Baroque dolomites and others geode-like sparry carbonates occur. The principal mineralogical association of these syn- and late-diagenetic mineralizations includes sphalerite, galena, pyrite, Fe-rieh carbonates, quartz and minor chalcopyrite, fluorite and barite. Silicification,dolomitization and iron-bearing carbonate alterations of the country rocks are frequent. Their features are very similar to Mississippi Valley-type ore mineralizations (Herrero et al. 1988; Velasco et al. 1993). Associated with strata-bound deposits or located in "Supraurgonian" sediments, fracture filling ores (vein type), which are locally F-bearing or Cu-bearing, are commonly present (e.g. Matienzo). A subordinate type of Zn-Pb sulfide mineralizations showing disseminated or vein-type morphologies, appears to be related to Triassic rocks in the border of exposed Upper Cretaceous diapirs (e.g. Jugo). According to Herrero (1989) and Velasco et al. (1993) the proposed ore genesis model involves migration of basinal brines, in part resulting from dewatering, having been channelled by synsedimentary fractures associated with the graben structures. This interpretation is consistent with the diagenetic evolution of the terrigenous lithologies of the early Cretaceous sequence at different depths and presumably relatively high temperature (Arostegui et al. 1991) since anchimetamorphism was reached at least in the central sectors of the basin.
Sampling and analytical procedures Most of the analyzed galenas come from stratiform and vein deposits in Carboniferous and from strata-bound Zn( + Pb) deposits hosted in Lower Cretaceous host rocks (ore deposit numbers in Fig. 1 and Table 1). The samples were collected from individual galena grains and hand-picked under the microscope with a steel needle, obtaining, in most cases, pure separates. The exceptions are deformed galena grains from Paleozoic deposits which contain a few mineral impurities (mainly fluorite, barite and sphalerite). A small amount of galena powder was placed in a teflon vessel and dissolved in concentrated nitric acid. Lead was purified by micro-electrodeposition techniques, converted into a nitrate and dissolved in water for loading on the mass spectrometer. For each sample, about 200-500 nanograms of lead was loaded onto outgassed single rhenium filaments in a mixture of silica-gel and phosphoric acid. Ratios were determined on a VG ISOMASS 54E thermal ionization mass spectrometer run in a fully automated mode (Gulson et al. 1984) at the CSIRO Division of Exploration Geoscience (New South Wales, Australia). All ratios were normalized to the accepted values of NBS 981 by applying a correction factor of + 0.08% per atomic mass unit. Estimated precision is about + 0.1% for 2~176 and 2~176 and + 0.05% for z~176 (at the 95% confidence limit, based on ~ 1200 analyses). The Pb blanks for the total procedure were ,~ 2 nanograms.
Isotope resuits T h e following p r e s e n t a t i o n of the i s o t o p i c d a t a follows a r e g i o n a l subdivision of the P a l e o z o i c a n d M e s o z o i c ore deposits. T h e d a t a are listed in T a b l e 1 a n d are d i s p l a y e d in Fig. 2. The m o s t striking feature of these d i a g r a m s is that lead c o m p o s i t i o n of bulk g a l e n a in this region outlines a g r o w t h curve very close to t h a t d e s c r i b e d b y C u m m i n g a n d R i c h a r d s (1975) for a l e a d e v o l u t i o n related to the u p p e r crust. A noticeable c h a r a c t e r i s t i c of this plot is t h a t analyses from each ore district are r e m a r k a b l y uniform.
Pb isotope composition of galenas in Carboniferous Cinco Villas rocks T h e results for 12 g a l e n a samples from the d e f o r m e d a n d m e t a m o r p h o s e d Z n - P b d e p o s i t s h o s t e d in the schistose succession of the C i n c o Villas massif, i n c l u d i n g galenab e a r i n g veins (Table 1 a n d Fig. 2) have i n d i s t i n g u i s h a b l e lead i s o t o p i c ratios. This single a n d h o m o g e n e o u s p o p u l a tion d i s p l a y s a linear a r r a y a n d small degree of i s o t o p i c dispersion, a n d this is so even a m o n g different o r e b o d i e s (e.g. A r d i t u r r i a n d M o d e s t a mines) as m u c h as 30 k m apart. T h e m a j o r i t y of the galenas c o n t a i n lead whose 2~176 2~176 and 2~176 ratios v a r y little (18.41-18.46, 15.65-15.68, a n d 38.62-38.75, respectively).
Pb isotope compositions from strata-bound deposits in Lower Cretaceous carbonates W e r e p o r t 21 lead i s o t o p e analyses from s t r a t a - b o u n d sedex a n d syndiagenetic deposits b e l o n g i n g to A p t i a n A l b i a n host r o c k s a n d 5 analyses from galenas from
87 Table 1. Lead isotope composition of galena samples in the Basque-Cantabrian ore deposits Host rocksb
2~176
z~176
2~176
Model ager (Ma)
Dol Dol Dol Dol Dol
18,723 18,745 18,728 18,733 18,761
15,663 15,686 15,673 15,662 15,693
38,702 38,772 38,723 38,695 38,789
88 116 103 79 118
Lim Lira Lira Lira Lirn Lim Lira
18,586 18,564 18,581 18,606 18,584 18,587 18,598
15,663 15,657 15,665 15,679 15,657 15,657 15,668
38,745 38,710 38,743 38,797 38,738 38,739 38,767
177 181 184 193 167 165 178
Vein (diapiric) Vein (diapiric) Strata-bound Strata-bound Strata-bound Strata-bound
Lira Lira Lim Lim Lim Lim
18,580 18,608 18,598 18,546 18,567 18,581
15,650 15,653 15,669 15,632 15,658 15,678
38,628 38,702 38,730 38,584 38,665 38,700
157 144 180 146 180 197
Strata-bound Strata-bound Strata-bound Strata-bound Strata-bound Strata-bound Strata-bound Strata-bound
Lim Lim Lim Lim Lim Lira Lim Lim
18,591 18,608 18,591 18,593 18,621 18,595 18,618 18,553
15,668 15,665 15,665 15,664 15,660 15,657 15,652 15,648
38,660 38,746 38,689 38,771 38,759 38,712 38,782 38,664
184 166 159 174 149 160 136 171
Paleozoic basement: Cinco Villas massif (Carboniferous host rocks) 6 Arditurri district 9 Otxamentegi Vein-type shl 9 Otxamentegi Stratiform shl 9 Otxamentegi Stratiform shl 10 Oportuna Stratiform shl 10 Oportuna Stratiform shl 10 Sta. Barbara Stratiform shl 10 Sta. B~trbara Stratiform shl 10 Sta. B~trbara Vein-type shl 10 Sta. Barbara Stratiform shl 10 Oportuna Stratiform shl 11 Modesta Stratiform shl 11 Modesta Stratiform shl
18,442 18,421 18,410 18,457 18,437 18,444 18,420 18,451 18,425 18,460 18,423 18,443
15,667 15,651 15,649 15,674 15,661 15,667 15,655 15,699 15,655 15,682 15,656 15,662
38,702 38,660 38,620 38,735 38,625 38,687 38,680 38,709 38,690 38,756 38,657 38,695
280 264 268 282 272 278 272 277 269 295 272 270
Paleozoic basement: Sierra de la Demanda massif (Cambrian host rocks) 7 Sierra de la Demanda 12 Carmina Stratiform? shl 13 Najerilla Vein-type shl 13 Najerilla Vein-type shl 14 S. Cristobal Vein-type shl 14 S. Cristobal Vein-type shl
17,816 18,424 18,411 18,240 18,223
15,610 15,663 15,651 15,640 15,626
37,939 38,717 38,686 38,412 38,376
607 284 271 366 352
Map Numbera
Sample
Morphology
Lower Cretaceous: Basque-Cantabrian basin 1 Santander district 1 Reocin Strata-bound 1 Reocin Strata-bound 1 Reocin Strata-bound 1 Udias Strata-bound 1 Udias Strata-bound 2 Western Vizcaya district 3 Matienzo Vein-type 3 Txomin Strata-bound 3 Anselma Strata-bound 4 Siete Puertas Strata-bound 4 La Rasa Corta Strata-bound 4 E1 Somo Strata-bound 4 La Rasa Vein-type 4 Central district 5 Jugo 5 Jugo 6 Katabera 6 Katabera 6 Aitzgorri 6 Aitzgorri 5 Troya-Legorreta district 7 Troya 7 Troya 7 Troya 7 Troya 7 Troya 7 Troya 8 Legorreta 8 Legorreta
"Numbers in first column are ore deposit locations in Fig. 1 bHost rocks: Dol, dolostones; Lim, limestones; Shl, shales eModel ages (Million years) according to Stacey and Kramers (1975)
remobilized veins. T w o separate populations indicating i m p o r t a n t differences in P b composition according the geographic position are observed (Figs. 2, 3): (1) the first relates to the central and eastern ore deposits whose
isotopic compositions show a limited spread, with individual deposits (e.g. T r o y a mine, Western Vizcaya district) appearing very h o m o g e n e o u s ; (2) a second cluster belonging to the western area of the Cretaceous basin (e.g.
88
coinciding with the growth curve of Cumming and Richards (1975), which is nearly parallel to the upper crust trend according to the Plumbotectonics model (Doe and Zartman 1979), and indicating that the studied deposits from Sierra de la Demanda have a similar lead source.
Lower Cretaceous 15,70
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Discussion
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Fig. 2. Leadisotope ratios of galenas of the Basque-Cantabrianore deposits reported in a 2~176 versus 2~176 diagram. C&R and S&K are the Cummingand Richards (1975) and Stacey and Kramers (1975)growth curves; Upper Crust is the evolutionary curve of Zartman and Doe (1981). Dashed fields encloselead isotope compositions of the Paleozoic,Central-Eastern,and Santander districts of the region Reocin and Udias mines, Santander district) exhibits the most radiogenic linear trend known in the region. These results provide evidence for two well-defined lead isotope provinces within the Cretaceous Basque-Cantabrian basin. One is characterized by high 2~176 values and coincides with ore deposits located in the graben of the peri-Asturian area. The other province corresponds to the central and eastern part of the Bilbao graben, situated to the north of the Sierra de la Demanda and to the west of the Cinco Villas Paleozoic massif. Both are characterized by radiogenic values of an upper crustal lead source. Furthermore, these isotopic compositions could reflect increasingly differentiated continental rocks. Plots also reveal a striking uniformity for the ore deposits of each province.
Pb &otope composition f r o m ore deposits in Cambrian -rocks
A preliminary sampling has been carried out in old mine dumps from Sierra de la Demanda massif (Carmina, St. Crist6bal and Najerilla mines), hosted in Cambrian sedimentary rocks and considered to be the main source area of the Mesozoic detritic sediments of the basin. Although the number of samples analyzed is limited (5 galena concentrates), we can distinguish three separate populations (Fig. 3): (1) the less radiogenic sample (2~176 about 17.82) belonging to the sedex Carmina deposit; (2) a second population represented by samples from the St. Crist6bal mine (saddle-shape veins), whose isotopic compositions correspond to 2~176 between 18.22 and 18.24; (3) and a third from the Najerilla mine (vein systems) that overlaps the Carboniferous population of the Basque-Paleozoic massif. In the 2 0 7 Pb/ 2 0 # Pb and the 2 0 8 Pb/ 2 0 4 Pb versus 2 0 6 Pb/ 2 0 4 Pb diagrams the three populations altogether describe a line of evolution
Isotopic data from different kinds of mineral deposits in western and central Europe, summarized in Fig. 3 (I and II fields), provide a comparison basis for the lead isotope ratios from northern Spanish deposits. Ore deposits in field I comprise syngenetic and epigenetic strata-bound sulfides hosted in Cambrian-Precambrian rocks and other remobilized mineralizations from previous ore deposits. Data from the following Pb-Zn ore deposits were considered: mineralizations from Montaigne Noire and Cbvennes, southern Massif Central, France (Brevart et al. 1982; Marcoux and Moelo 1991), syngenetic and syndiagenetic ores from the Iglesiente-Sulcis area, SW Sardinia, Italy (Boni and Koeppel 1985; Ludwig et al. 1989), strata-bound mineralizations from the Armorican massif, France (Oh et al. 1989), stratiform base metal deposits from Central Europe (Bielicki and Tischendorf 1991), and strata-bound deposits from northwestern Spain (Tornos and Arias 1993). This field I also include basalt-hosted massive sulfide deposits related to a source with mantle affinity reported by Fox et al. (1988), Hallberg (1989) and Billstr6m (1990). In Fig. 3, field II, characterized by more radiogenic isotopic ratios, encloses data of strata-bound ores, vein deposits related to granites and late fracturation in Hercynian terrains ("Hercynian" signature) and some sulfide massive mineralizations. Within this field are included the following base metal mineralizations: stratiform, stratabound and vein deposits from Montagne Noire and Cevennes (Brevart et al. 1982; Marcoux and Calvez 1985; Le Guen et al. 1991; Marcoux and Moelo 1991; Sinclair et al. 1993), strata-bound deposits from the Eastern and Southern Alps (Kdppel and Schroll 1988; Lattanzi et al. 1992), veins and strata-bound deposits from the Moldanubian and Saxothuringian zones, Central Europe (Bielicki and Tischendorf 1991), massive sulfide deposits from the Iberian Pyrite Belt (Marcoux et al. 1992), massive volcanogenic mineralization at Parys Mountain, north Wales (Fletcher et al. 1993), and veins and strata-bound deposits hosted by Paleozoic to Triassic clastic and carbonate rocks from Betic Cordillera (Arribas and Tosdal 1994). We also define a third field (Ill) which encloses data for strata-bound, sedex and vein deposits hosted in Lower Cretaceous rocks from northern Spain. The isotopic data from the Carmina mine (Sierra de la Demanda) plot in the centre of"Cambrian" I field (Fig. 3) and presumably its lead is derived from crustal rocks characterized by relatively low U/Pb ratios and thus reasonably depleted the uranium derived isotopes 2~ and 2~ Within the "Hercynian" II field plot the metamorphosed and deformed Paleozoic Zn-Pb shale-hosted ore deposits of the Arditurri ore field and Modesta mine (Fig. 1, 2, and Table 1) located in the Cinco Villas massif, and the uneconomic deposits of St. Cristdbal and
89 o_ g
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