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Articles |
Departamento de Mineralogia e Petrologia, Instituto de Geociências, Universidade de Brasília, Brasília 70910-900, DF, Brasil
E-mail address: mamoura{at}unb.br
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ABSTRACT |
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 Top Abstract IntroductionGeological Setting and...Mineral AnalysesSulfides CompositionsArsenatesDiscussionConclusionsAknowledgementsReferences |
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Keywords: indium, sphalerite, roquesite, arsenate, Mangabeira granite, Brazil.
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INTRODUCTION |
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TopAbstractIntroductionGeological Setting and...Mineral AnalysesSulfides CompositionsArsenatesDiscussionConclusionsAknowledgementsReferences |
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Evolved topaz–albite granite of the Mangabeira Massif and its hydrothermal products generated unique Sn–In mineralization in central Brazil. Besides their petrological significance, the rare topaz granites are known in the literature for their economic importance, as they are commonly related to rare-metal deposits (Pollard 1995). The Mangabeira massif contains roquesite (CuInS2) and dzhalindite [In(OH)3] (Botelho & Roger 1990) and the only known occurrence of yanomamite (InAsO4·2H2O) in the world (Botelho et al. 1994). It is also of special mineralogical importance as it contains other rare minerals, such as arsenates not previously reported in Brazil, as well as unknown arsenates.
We present here the results of a detailed mineralogical investigation of the Sn–In-mineralized area of the Mangabeira granitic massif. In this paper, we focus on the textural and chemical characteristics of rare and unknown arsenates that occur in the study area and discuss the relationship between In-rich sphalerite, roquesite and In-rich stannite-group minerals.
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GEOLOGICAL SETTING AND PARAGENESIS |
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TopAbstractIntroductionGeological Setting and...Mineral AnalysesSulfides CompositionsArsenatesDiscussionConclusionsAknowledgementsReferences |
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8Be6(SiO4)6S2] in this area, which is restricted to greisen composed of quartz, topaz, helvite and either zinnwaldite or Li-bearing phengite.
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The dominant rock in the Main Greisenized Zone is a pink equigranular granite, composed of quartz (30%), microperthitic microcline (30–35%) and pure albite (30–35%). Primary Li-bearing siderophyllite is rarely preserved, and is commonly transformed to Li-bearing phengite. The accessory minerals are zircon, monazite, magnetite and, locally, ilmenite. Where greisenized, the granite becomes richer in phengite (10%) and contains metasomatic anhedral topaz, monazite, fluorite and disseminated cassiterite. The greisen formed by alteration of this granite, a phengite–quartz greisen, contains late Ba, Bi, Cu and Pb arsenates.
The topaz–albite granite has intruded the biotite granite, and is responsible for the development of a metasomatic aureole. The topaz–albite granite is white and contains quartz (30–35%), microperthitic microcline (20%), pure albite (20–25%), magmatic topaz (5–20%) and zinnwaldite (10%). Zircon, monazite and cassiterite are rare. Magmatic topaz occurs as euhedral crystals (20 µm) included in albite (Moura & Botelho 2000). The autometasomatism of this granite developed zinnwaldite greisen, which contains quartz, zinnwaldite, topaz, cassiterite and monazite in different proportions (Moura & Botelho 2000).
The quartz–topaz rock is white, massive, composed mainly of quartz, topaz, zinnwaldite, arsenopyrite and cassiterite. Topaz occurs either as subhedral grains (0.5 mm) partially altered to zinnwaldite or as euhedral crystals (30 µm) included in quartz or in the larger grains of topaz. Accessory minerals are monazite, zircon, fluorite, sphalerite, ferberite, löllingite, chalcopyrite, pyrite, bismuthinite, galena, stannite-group minerals, tennantite, argentite, bismuth, and roquesite. Secondary minerals include native copper, scorodite, malachite, digenite, chalcocite, enargite, bornite, covellite, phenakite [Be2(SiO4)] and Ba, Bi, In, K, Pb, U, Y–Cu and Sn arsenates. Potentially economic concentrations of indium (up to 1 wt%) and minerals (roquesite, dzhalindite and yanomamite) occur predominantly in the quartz–topaz rock, but also in greisen and albitized biotite granite.
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MINERAL ANALYSES |
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TopAbstractIntroductionGeological Setting and...Mineral AnalysesSulfides CompositionsArsenatesDiscussionConclusionsAknowledgementsReferences |
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Because of the interference between indium and tin in the analysis of tin-rich minerals by EPMA (Schwartz-Schampera & Herzig 2002), a systematic increase of 0.05 to 0.1 wt% In2O3 was registered during analysis of the tin standard (In-free cassiterite). As there is interference of the InL
in the SnL line, a window for the detection of the In-peak alone was selected during the calibration procedure and adopted for the determination of indium contents in cassiterite and Sn-rich minerals. Nevertheless, In L X-rays also interfere with SnL
emission, creating a composite peak. As the separation of the SnL and InL peaks is very difficult, an interference correction of 0.1 wt% was applied in In2O3 contents of cassiterite and tin-rich minerals. The same procedure was used by Legendre & Rossi (1994) to analyze In-containing cassiterite. The authors tested the method by comparing results of the EPMA analysis of cassiterite containing variable concentrations of indium with LA–ICP–MS data for the same grains. The results showed an excellent correspondence of indium contents obtained with the two methods.
As most of the secondary arsenates from the Mangabeira massif are hydrated and poorly crystalline, some compositions show a variation as a result in the electron-microprobe data, even using a larger diameter of the beam. Nevertheless, the presence of non-quantified elements was eliminated after detailed investigation of the energy-dispersion spectra of the minerals. The amount of H2O was estimated by subtraction of the total from 100 wt%. For the arsenate analyses, all Fe was reported as trivalent iron, by analogy with similar and identified species, such as scorodite and segnitite, and also because a high-oxidation-state environment is postulated for the formation of these secondary minerals in the Mangabeira massif.
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SULFIDES COMPOSITIONS |
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TopAbstractIntroductionGeological Setting and...Mineral AnalysesSulfides CompositionsArsenatesDiscussionConclusionsAknowledgementsReferences |
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Sphalerite occurs as generally anhedral inclusions in arsenopyrite, but also in quartz, topaz and cassiterite from the greisens and the quartz–topaz rock (Fig. 2). Two types of sphalerite are petrographically distinguished in the Mangabeira massif: a red sphalerite (~20 µm), which occurs only as inclusions in arsenopyrite, quartz, cassiterite and topaz (Fig. 2a), and a yellow one (20 µm – 1.5 mm), which occurs either as inclusions in arsenopyrite or as disseminated grains in the mineralized rocks and exogreisens (Fig. 2b).
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Roquesite (CuInS2) occurs as inclusions in arsenopyrite and as fine lamellae along cleavage planes of sphalerite and also as large irregular bands in a sphalerite crystal (Figs. 2c, d) included in arsenopyrite from the quartz–topaz rock. The association sphalerite–roquesite occurs along with tennantite, chalcopyrite, bismuthinite and galena. This textural relationship suggests that roquesite probably exsolved from sphalerite containing more than 6.7 wt% In.
Minerals of the stannite group, stannite (Cu2FeSnS4) and ferrokësterite [Cu2(Fe,Zn)SnS4], are rare accessory minerals in the Main Greisenized Zone. They occur mainly as inclusions in arsenopyrite and are important carriers of In in the Mangabeira massif, with mean In values of 1.77 wt% (Table 2). Other deposits reported in the literature with In-rich stannite are the Yakutia Sn sulfide deposit, where the mineral contains 0.15 wt% In (Ivanov & Lizunov 1959), Mount Pleasant (Boorman & Abbott 1967, Sinclair et al. 2006), where a hexagonal In-poor stannite (0.04 wt% In) and a tetragonal In-rich stannite (2.1 wt% In) were described, the polymetallic Goka deposit, Japan (9.63 wt% In; Murao & Furuno 1990), and the Toyoha lead – zinc – silver vein-type deposit, from which Ohta (1989) described stannite with 9.85 wt% In.
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ARSENATES |
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TopAbstractIntroductionGeological Setting and...Mineral AnalysesSulfides CompositionsArsenatesDiscussionConclusionsAknowledgementsReferences |
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Scorodite is the most common arsenate found in the Mangabeira massif. It is widespread as a product of arsenopyrite alteration in greisens and in the quartz–topaz rock, but it also fills fractures in quartz, zinnwaldite and topaz, attesting to its late character. Data obtained from more than one hundred analyses of scorodite show that homogeneous scorodite contains up to 7 wt% In2O3.
Yanomamite (InAsO4·2H2O) occurs in the same association as scorodite (Botelho et al. 1994), as euhedral grains commonly intergrown with scorodite and, rarely, with dzhalindite. Although yanomamite contains minor amounts of iron in its structure, the maximum substitution is In0.85Fe0.15.
Other arsenates studied in detail from the Mangabeira massif include Sn, Pb, Bi, Ba, K and Y–Cu arsenates, which will be described below.
Tin arsenate
An unnamed tin arsenate mineral occurs as either discrete grains or filling fractures of pre-existing minerals in strongly altered quartz–topaz rock. Locally, it is associated with probable native tin. The arsenate grains are yellow to brownish yellow, anhedral, rarely euhedral, 0.1 to 1 mm across, zoned, isotropic and with a high index of refraction (Fig. 4a).
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This Y-bearing Cu–Al arsenate is green and occurs as clusters of transparent to translucent microcrystals filling vugs in altered quartz–topaz rock or associated with cassiterite crystals (Fig. 4b). Under the polarizing microscope, the mineral is pale green, anisotropic, with medium to high relief. Its representative mean chemical composition is 42 wt% CuO, 38% As2O5, 4% Al2O3, 4% Y2O3, 9% calculated H2O, and minor amounts of WO3, Fe2O3 and PbO. The composition is similar to goudeyite [Cu6Al(AsO4)3(OH)6·3H2O] described by Wise (1978), which has 47 wt% CuO, 28% As2O5, 4% Al2O3, 3.44% Y2O3, 11% H2O and 1.37% CaO. Goudeyite is considered the Al analog of agardite-(Y), (Y,Ca)Cu6[(AsO4)3(OH)6]·3H2O (Dietrich et al. 1969, Wise 1978).
Lead arsenate
The lead arsenate mineral is pale yellow, has a high index of refraction, and occurs as either fillings of microfractures in quartz and zinnwaldite grains or as discrete grains in altered quartz–topaz rock. It has an anomalous blue interference-color where filling fractures. The mineral also forms zoned grains where it is associated with the tin arsenate, such that its nucleus is rich in lead and its border is rich in tin, or with argentite and scorodite. In the latter case, the nucleus of the grain is argentite and grades to an intermediate zone of scorodite and an outer zone of lead arsenate (Figs. 4c, d).
Quantitative electron-microprobe analyses yielded a mean composition of 28 wt% As2O5, 24% Fe2O3, 31% PbO, 5% Al2O3, 12% calculated H2O, and no SO3 (Table 4). Beudantite [PbFe3(AsO4)(SO4)(OH)6] and segnitite [PbFe3H(AsO4)2(OH)6] have optical characteristics similar to those found in this arsenate. However, taking into account the mineral’s chemical composition and the classification scheme for the alunite–jarosite family proposed by Birch et al.(1992), this arsenate is tentatively classified as segnitite, for which Birch et al.(1992) reported 1 wt% Al2O3 and obtained powder-diffraction data that resemble those for sulfate-free beudantite.
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The bismuth arsenate is rare in the Mangabeira quartz–topaz rock, in which it occurs either as discrete grains 200 µm across included in quartz or filling fractures in altered arsenopyrite. The mineral is dark brown under uncrossed nicols and has a high relief.
Results of electron-microprobe analyses, which vary widely, possibly owing to the loose character of the grains studied, indicate a compositional range of 59 to 74 wt% Bi2O3, 18 to 25% As2O5, 0 to 6% Fe2O3 and 2 to 14% H2O (estimated). The composition is considered to be similar to preisingerite [Bi3O(AsO4)2(OH)] (Anthony et al. 2000), although at Mangabeira, the bismuth arsenate is optically different.
Pharmacosiderite
The mineral identified as pharmacosiderite [KFe3+ 4 (AsO4)3(OH)4·7H2O] is yellowish green, with a medium to high relief; it occurs as individual grains or occupies mica-bearing fractures in hydrothermally altered rocks of the Main Greisenized Zone (Fig. 4e). It is usually isotropic, but some grains are anisotropic, which probably corresponds to the anomalous anisotropy described in pharmacosiderite by Palache et al.(1963).
Electron-microprobe analyses of the mineral indicate a composition with 36–41 wt% As2O5, 33% Fe2O3, 3–5% Al2O3, 3–6% K2O, and less than 1% ZnO, PbO and CuO, similar to pharmacosiderite (39.47 wt% As2O5, 36.57% Fe2O3, 5.39% K2O and 18.56% H2O) (Anthony et al. 2000). The chemical composition of the grains analyzed can be expressed using the ideal formula of pharcamosiderite, but considering a substitution of aluminum for iron.
Barium arsenate
An unnamed barium arsenate was identified in the quartz–topaz rock. The mineral occurs as grains up to 500 µm in size. They are pale to brownish yellow, with medium to high relief, generally massive and rarely with rhombic habit (Fig. 4f). The euhedral grains are isotropic, but some have an anomalous grayish blue interference-color. The massive grains are in some cases associated with masses of scorodite, and also appear to be products of the alteration of arsenopyrite.
Despite some scatter (Table 5), attributed to the massive nature of the grains studied and their hydrated nature, the data point to an unknown barium mineral with a composition that can be considered in some way similar to that of pharmacosiderite and barium-pharmacosiderite [BaFe4(AsO4)3(OH)5·5(H2O)]. Taking into account the scatter in the analytical data obtained and in order to approach neutrality in the mineral formula, the empirical formula (Ba0.7K0.3) Fe3+ 6(AsO4)5(OH)5·H2O is suggested for the mineral (Table 5).
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Chenevixite [Cu2Fe2(AsO4)2(OH)4·H2O] (Palache et al. 1963, Williams 1977) was identified in a greisen sample from the evolved biotite granite in contact with the quartz–topaz rock. The mineral occurs as a product of arsenopyrite alteration. It is brown and massive.
In the Mangabeira massif, the mineral contains 39 wt% As2O5, 25% Fe2O3, 25% CuO, 2% Al2O3, 1% PbO, 0.4% In2O3 and 9% H2O (calculated). This composition is comparable to that of theoretical chenevixite, which has 38.1 wt% As2O5, 26.49% Fe2O3, 26.40% CuO and 8.97% H2O (Williams 1977).
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DISCUSSION |
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TopAbstractIntroductionGeological Setting and...Mineral AnalysesSulfides CompositionsArsenatesDiscussionConclusionsAknowledgementsReferences |
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According to Johan (1988), the only possible mechanism capable of explaining the entry of indium in the structure of Fe-free sphalerite is the substitution Cu+ + In3+ = 2Zn2+, but the author was not able to explain the preferential concentration of In and Cu in 111 planes of sphalerite. In the samples from the Mangabeira massif, In and Cu concentrations along the structural planes of sphalerite were observed to be due to the presence of roquesite in these directions, which favors the hypothesis of Oen et al. (1980). Burke & Kieft (1980) also observed the association of sphalerite and roquesite in Långban, Sweden, where there is intercalation of dark brown In-rich sphalerite (9–10 wt% In) with colorless to pale brown areas, with 0–5.5 wt% In. The presence of these zones, together with the ratio Cu/In = 1 (atom basis) in sphalerite, led the authors to propose a partial solid-solution given by the formula Zn2–2xCuxInxS2. Kieft & Damman (1990) suggested that In-rich sphalerite from Gåsborn, Sweden, is a mixture of sphalerite, chalcopyrite and roquesite.
The observation of roquesite lamellae along cleavage planes in sphalerite without substitution textures in the Brazilian samples studied and the chemical composition of the two different types of sphalerite from the quartz–topaz rock of the Mangabeira massif suggest that the observed sphalerite–roquesite association attests to the existence of a discontinuous solid-solution between roquesite and sphalerite. In this case, the lamellae in the cleavage planes of sphalerite would be the product of exsolution from sphalerite supersaturated in indium.
Kieft & Damman (1990) estimated at 2 wt% the maximum solubility of indium in Fe-rich sphalerite (12 wt% Fe). Nevertheless, in the Mangabeira samples, Fe-poor sphalerite (~ 5 wt% Fe) with up to 6.7 wt% In is still homogeneous, which suggests that the solubility of indium in Fe-poor sphalerite might be three times higher than in Fe-rich sphalerite. The role of iron in the solubility of indium in the sphalerite structure should be better investigated.
A coupled substitution Cu2Sn – 2(Zn,Fe) between sphalerite and stannite-group minerals (y = –1.1778x + 7.8115; R2 = 0.9864) is supported by the EPMA data obtained for the Mangabeira samples (Table 2, Fig. 5). Similar results were reported by Ohta (1989) and Sinclair et al.(2006). On the basis of the observed paragenesis and the chemical data obtained (Table 2), the solid solutions stannite–sphalerite and sphalerite–roquesite, illustrated on a Cu – Fe+Zn(+Cd) – In+Sn diagram (Fig. 5), form a pseudoternary system sphalerite – stannite – roquesite, as proposed by Oen et al. (1980).
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In the Mangabeira massif, indium was initially concentrated in sphalerite, but also in stannite-group minerals and chalcopyrite. Indium-rich sphalerite is in equilibrium with the paragenesis cassiterite, ferberite and löllingite, which crystallized between 490 and 530°C, calculated using the arsenopyrite geothermometer (Botelho 1992). High temperatures for the formation of the quartz–topaz rock, together with a low pressure, have also been obtained from fluid-inclusion and stable-isotope studies (Moura et al. 2004).
During the late hydrothermal and supergene stages, arsenic was released from arsenopyrite and combined with different metals to form secondary arsenates. Indium migrated from the In-rich sulfides to form scorodite and yanomamite.
The data obtained from more than one hundred analyses of scorodite compared to those of yanomamite (Botelho et al. 1994) indicate the absence of a continuous solid-solution between those minerals, although homogeneous scorodite can contain up to 7 wt% In2O3. The presence of a break in the series is presumably due to the great difference in ionic radius between Fe3+ and In3+.
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CONCLUSIONS |
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TopAbstractIntroductionGeological Setting and...Mineral AnalysesSulfides CompositionsArsenatesDiscussionConclusionsAknowledgementsReferences |
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Indium incorporation into the sphalerite structure probably occurred according to the relation Cu + In + Fe = 3Zn, although the coupled substitution 2(Zn,Fe) = CuIn also is present. Textural relationships and detailed chemical data obtained in this study support the existence of the pseudoternary system sphalerite – stannite – roquesite and justify the proposal that In-rich sphalerite containing up to 6 wt% indium can be homogeneous, which implies that indium exsolution from the structure does not occur if indium values are lower than 6 wt% in Fe-poor sphalerite.
The alteration of the high-temperature hydrothermal assemblage in the Mangabeira area, probably by a supergene process, enhanced the formation of dzhalindite and secondary arsenates, such as pharmacosiderite, segnitite, chenevixite, goudeyite, metazeunerite and unknown bismuth, barium and tin hydrated arsenates. A continuous solid-solution between scorodite and yanomamite is not supported by the chemical data presented here.
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AKNOWLEDGEMENTS |
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TopAbstractIntroductionGeological Setting and...Mineral AnalysesSulfides CompositionsArsenatesDiscussionConclusionsAknowledgementsReferences |
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REFERENCES |
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TopAbstractIntroductionGeological Setting and...Mineral AnalysesSulfides CompositionsArsenatesDiscussionConclusionsAknowledgementsReferences |
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Received January 12, 2006 ,revised manuscript accepted October 18, 2006.
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