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Barren and Li–Sn–Ta Mineralized Pegmatites from NW Spain (Central Galicia): a Comparative Study of Their Mineralogy, Geochemistry, and Wallrock Metasomatism

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Barren and Li–Sn–Ta Mineralized Pegmatites from NW Spain (Central Galicia): a Comparative Study of Their Mineralogy, Geochemistry, and Wallrock Metasomatism minerals Article Barren and Li–Sn–Ta Mineralized Pegmatites from NW Spain (Central Galicia): A Comparative Study of Their Mineralogy, Geochemistry, and Wallrock Metasomatism Ana Roza Llera, Mercedes Fuertes-Fuente * , Antonia Cepedal and Agustín Martin-Izard Department of geology, University of Oviedo, Arias de Velasco s/n, 33005 Oviedo, Spain; [email protected] (A.R.L.); [email protected] (A.C.); [email protected] (A.M.-I.) * Correspondence: [email protected] Received: 31 October 2019; Accepted: 27 November 2019; Published: 29 November 2019 Abstract: In Central Galicia, there are occurrences of barren and Li–Sn–Ta-bearing pegmatites hosted by metasedimentary rocks. A number of common and contrasting features between Panceiros pegmatites (barren) and Li–Sn–Ta mineralized Presqueira pegmatite are established in this study. K-feldspar and muscovite have the same trace elements (Rb, Cs, P, Zn, and Ba), but the mineralized one has the highest Rb and Cs and the lowest P contents. The barren bodies show fluorapatite and eosphorite–childrenite replacing early silicates. The mineralized body has primary phosphates (fluorapatite and montebrasite), a metasomatic paragenesis (fluorapatite and goyazite) replacing early silicates, and a late hydrothermal assemblage (vivianite and messelite). Ta–Nb oxides from the Presqueira body show a trend from columbite-(Fe) to tantalite-(Fe) and tapiolite-(Fe). In this body, the Li-aluminosilicate textures support primary crystallization of petalite that was partially transformed into Spodumene + Quartz (SQI) during cooling, and into myrmekite during a Na-metasomatism stage. As a result of both processes, spodumene formed. The geochemical study supports magmatic differentiation increasing from the neighboring granites to the Li–Sn–Ta mineralized pegmatite. In both barren and mineralized bodies, the pegmatite-derived fluids that migrated into the wallrock were enriched in B, F, Li, Rb, and Cs and, moreover, in Sn, Zn, and As. Keywords: wallrock signature; Li–Sn–Ta pegmatite; spodumene; petalite; myrmekite; columbite–tantalite; tantaliferous cassiterite; NW Spain 1. Introduction Some rare elements, mainly those that support high-technology industry, have an increasing demand due to their variety of uses in new technologies. Among these elements, also known as high-technology metals, Ta, Li, and Sn are in high demand owing to their use in capacitors for wireless technology, in battery applications, and in liquid crystal displays (LCD) and touch-screen displays. These metals can occur in high concentrations in pegmatites and occasionally form ore deposits. Consequently, data to improve the prospecting criteria for rare metal ores in pegmatites are critical for the localization of undiscovered resources ([1] and references therein). The presence of Li–Sn–Ta mineralization associated with pegmatites is known in Galicia, northwestern Spain (e.g., [2–4]), and, moreover, there are several occurrences of barren pegmatites. This work focuses on a Li–Sn–Ta mineralized body, the Presqueira pegmatite, which is a non-outcropping body that has been recently explored by a mining company, and a swarm of pegmatites that are barren in Li–Sn–Ta bearing minerals, the Panceiros pegmatites. In this research, we have carried out a comparative study of the whole-rock and mineral geochemistry of the barren and the mineralized bodies and their host-rock together with Minerals 2019, 9, 739; doi:10.3390/min9120739 www.mdpi.com/journal/minerals Minerals 2019, 9, 739 2 of 37 theMinerals possible 2019 parental, 9, 739 granites. The main aim of this research is to evaluate tools for the exploration2 of 37 of Li–Sn–Ta enriched pegmatites such as trace-elements in major pegmatite-forming minerals and geochemicalexploration signatures of Li–Sn–Ta of metasedimentaryenriched pegmatites wall such rock. as trace-elements in major pegmatite-forming minerals and geochemical signatures of metasedimentary wall rock. 2. Geological Setting 2. Geological Setting The studied pegmatites are located in the vicinity of the village of Cerdedo (Pontevedra, Galicia), in NW SpainThe studied (Figure pegmatites1). Geologically, are located this areain the is vicinity in the Iberian of the village Massif, of which Cerded presentso (Pontevedra, the westernmost Galicia), exposuresin NW ofSpain the European(Figure 1). Variscides Geologically, in the this southwestern area is in the limb Iberian of the arcMassif, described which by presents this chain the in Westernwesternmost Europe. exposures The Iberian of the Massif European has been Variscides divided in into the several southwestern zones [5 limb], one of of the the arc innermost described zones by beingthis thechain “Galicia in Western Trás-Os-Montes Europe. The Zone” Iberian (GTMZ), Massif wherehas been these divided pegmatites into several are located. zones [5], The one GTMZ of the [6 ] representsinnermost a stackzones of being allochthonous the “Galicia and Trás-Os-Mont parautochthonouses Zone” units (GTMZ), thrust over where the autochthonousthese pegmatites Central are Iberianlocated. Zone The (Figure GTMZ1). [6] Two represents domains a havestack beenof allo distinguishedchthonous and within parautochthonous the GTMZ ([ 6units,7] and thrust references over therein):the autochthonous The Schistose Central Domain, Iberian also Zone known (Figure as the 1). Parautochthonous Two domains have Domain, been distinguished and the Allochthonous within the GTMZ ([6,7] and references therein): The Schistose Domain, also known as the Parautochthonous Complexes, emplaced over the parautochthonous pile and composed of ophiolitic and catazonal Domain, and the Allochthonous Complexes, emplaced over the parautochthonous pile and units of more exotic origin [8–10]. The studied pegmatites are in the Schistose Domain, which is an composed of ophiolitic and catazonal units of more exotic origin [8–10]. The studied pegmatites are allochthonous sequence emplaced on the lower Paleozoic and Precambrian rocks of the Central Iberian in the Schistose Domain, which is an allochthonous sequence emplaced on the lower Paleozoic and Zone. This Domain is constituted by a lower Paleozoic metasedimentary sequence, more than 4000 m Precambrian rocks of the Central Iberian Zone. This Domain is constituted by a lower Paleozoic thick, interpreted as the most external sediments of the continental margin of Gondwana [6,7,10–14]. metasedimentary sequence, more than 4000 m thick, interpreted as the most external sediments of Twothe stratigraphic continental margin units, the of lowerGondwana one known [6,7,10–14]. as the Two Nogueira stratigraphic group andunits, the the upper lower one one as known the Paraño as group,the Nogueira have been group established and the inupper the Schistose one as the Domain. Paraño group, The Paraño have been group established (Figure2), in which the Schistose hosts the PresqueiraDomain. pegmatite,The Paraño constitutesgroup (Figure a more 2), which than hosts 3000 mthe thick Presqueira succession pegmatite, of siliciclastic constitutes rocks, a more Cambrian than to3000 lower m Silurianin thick succession age [7 ].of Insiliciclastic the studied rocks, area, Cambrian this group to lower is mainly Silurianin formed age by[7]. schist, In the studied some of area, them graphite-rich,this group is and mainly subordinate formed quartzite.by schist, Insome addition, of them some graphite-rich, authors [6, 15and] define subordinate another quartzite. stratigraphic In unitaddition, underlying some theauthors Paraño [6,15] Group, define referredanother strati to asgraphic the Santa unit Baia underlying group (Figurethe Paraño2). Group, Several referred authors (e.g.,to as [13 the,16 ,Santa17]) point Baia group out that (Figure the Santa 2). Several Baia Groupauthors belongs (e.g., [13,16,17]) to the Central point out Iberian that the footwall Santa ofBaia the SchistoseGroup belongs Domain. to Thisthe Central stratigraphic Iberian group footwall hosts of the the Schistose Panceiros Domain pegmatites. This stratigraphic and is mainly group made hosts up of schistthe Panceiros and paragneisses pegmatites in theand area is mainly of study. made up of schist and paragneisses in the area of study. Figure 1. Geological map of the NW Iberian Massif showing the location of the studied area in the Figure 1. Geological map of the NW Iberian Massif showing the location of the studied area in the Galicia-TrGalicia-Trás-Os-Montesás-Os-Montes Zone Zone (modified (modified from from [ 9[9]).]). Minerals 2019, 9, 739 3 of 37 The tectonic style of the GTMZ is dominated by the thrust regime related to nappe emplacement during the Variscan Orogeny. There are two Variscan deformation events associated with nappe emplacement [7]: D1, recumbent folds with axial plane cleavage (S1), which are visible only when affecting the quartzite beds; and D2, also consisting of recumbent folds with axial plane crenulation cleavage or schistosity (S2) and having phyllonite fabrics developed in association with the Galicia- Trás-os-Montes basal thrust. After the nappe emplacement, the tectonic evolution becomes predominantly a wrench regime during the last deformation event (D3), which is characterized by folds with subvertical axial planes and shear zones (right folds) at all scales that include crenulation. At the same time, large volumes of synkinematic and late synkinematic granitoids are emplaced [11]. As regards the metamorphism, the Allochthonous Complexes have undergone an early high pressure (HP) metamorphism, which characterizes them
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