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The key role of mica during igneous concentration of tantalum

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Contrib Mineral Petrol (2014) 167:1009
DOI 10.1007/s00410-014-1009-3
ORIGINAL PAPER
The key role of mica during igneous concentration of tantalum
Aleksandr Stepanov • John A. Mavrogenes •
Sebastien Meffre • Paul Davidson
Received: 12 January 2014 / Accepted: 17 April 2014 / Published online: 27 May 2014
 Springer-Verlag Berlin Heidelberg 2014
Abstract Igneous rocks with high Ta concentrations share
a number of similarities such as high Ta/Nb, low Ti, LREE
and Zr concentrations and granitic compositions. These
features can be traced through fractionated granitic series.
Formation of Ta-rich melts begins with anatexis in the pre-
sence of residual biotite, followed by magmatic crystalliza-
tion of biotite and muscovite. Crystallization of biotite and
muscovite increases Ta/Nb and reduces the Ti content of the
melt. Titanium-bearing oxides such as rutile and titanite are
enriched in Ta and have the potential to deplete Ta at early
stages of fractionation. However, mica crystallization sup-
presses their saturation and allows Ta to increase in the melt.
Saturation with respect to Ta and Nb minerals occurs at the
latest stages of magmatic crystallization, and columbite can
originate from recrystallization of mica. We propose a model
for prediction of intrusion fertility for Ta.
Keywords Rare metal
Deposit
Biotite
Muscovite

Granite fractionation
Anatexis
Granite classification
Introduction
Tantalum and niobium are commonly referred to as
‘‘geochemical twins’’ owing to their strong chemically
Communicated by J. Hoefs.
A. Stepanov (&)
S. Meffre
P. Davidson
ARC Centre of Excellence in Ore Deposits (CODES),
School of Physical Sciences, University of Tasmania,
Private Bag 79, Hobart, Tasmania 7001, Australia
e-mail: sashas@utas.edu.au
J. A. Mavrogenes
Research School of Earth Sciences, The Australian National
University, Mills Road, Bld. 61, Canberra, ACT 0200, Australia
similarity. However, economic concentrations of each
element are found in very different geochemical environ-
ments: tantalum deposits are associated with granitic peg-
matites, whereas niobium is mainly mined from
carbonatites (Kuzmenko 1961; Linnen et al. 2014). Tan-
talum is a strategic metal in limited supply, and thus, Ta
deposits are the target of intense exploration (Galeschuk
and Vanstone 2007; Papp 2011; Linnen et al. 2014).
Society’s ever increasing need for Ta requires a better
understanding of its geochemistry to increase new deposit
discovery rates and reduce exploration risk.
Tantalum and niobium are incompatible lithophile ele-
ments during mantle melting and hence are highly enriched
in the continental crust (Fig. 1). The upper continental
crust has higher Ta/Nb than the bulk Earth, and the
apparent absence of a complementary reservoir with su-
perchondritic Nb/Ta comprises the ‘‘missing Nb paradox’’
(Rudnick et al. 2000; Stepanov and Hermann 2013). Tan-
talum and niobium deposits demonstrate fractionation of
Nb from Ta orders of magnitude larger than observed
globally (Fig. 1). Magmatic fractionation is thought to be
responsible for the formation of Ta-rich melts (Raimbault
et al. 1995; London 2008; Linnen et al. 2012), yet the
specific mineral(s) responsible for fractionating Nb from
Ta are unknown (London 2008). In a recent review of rare
metal pegmatites, Černý et al. (2012) stated that ‘‘the
factors that fractionate Ta from Nb in granites are not yet
fully known’’. It has been proposed that Nb–Ta in granites
could be fractionated hydrothermally (Dostal and Chatter-
jee 2000) or by ‘‘magmatic fluid exsolution’’ (Tartèse and
Boulvais 2010). In pegmatites, Nb–Ta fractionation is
often attributed to the crystallization of columbite–tantalite
[(Mn2?, Fe2?) (Ta, Nb)2O6] (Linnen and Keppler 1997;
Linnen 1998; Chevychelov et al. 2010; Černý et al. 2012).
Muscovite also has been implicated as a mineral able to
123
1009 Page 2 of 8 Contrib Mineral Petrol (2014) 167:1009

fractionate Ta from Nb (Kovalenko et al. 1996; Raimbault
and Burnol 1998). London (2008) proposed that melt su-
percooling could be responsible for early saturation of
columbite–tantalite in pegmatites. The purpose of this
paper is to demonstrate the important role of biotite and
muscovite in fractionation of tantalum from niobium in
granitic melts, and to model tantalum enrichment from
Fig. 1 Tantalum grades and Ta/Nb ratios of the main Ta and Nb
deposits differ widely from the principal reservoirs of the Earth:
chondrite (Jochum et al. 2000), representing primordial Earth and the
average composition of the upper continental crust (Barth et al. 2000),
which is the source of granitic melts. Note that due to the logarithmic
scale on the vertical axis, continental crust and chondrite appear
similar even though they differ by a factor 1.5, and this difference
represents the ‘‘missing Nb paradox’’ (Stepanov and Hermann 2013).
References for Ta deposits are in Table 1, and data for Nb deposits
are from Guimarães and Weiss (2001), Issa Filho et al. (2001),
Cordeiro et al. (2011) and Lynas (2011)
crustal abundances of around 1 up to 1000 ppm in Ta
deposits.
Background
Tantalum deposits are found in Archaean to Proterozoic
granitic pegmatites [the LCT (Li–Cs–Ta) type often asso-
ciated with S-type granites (London 2008); Table 1] or in
late Proterozoic and Phanerozoic leucoapogranites [Yic-
hun, Orlovka, Abu Dabbab, etc. (Severov et al. 1977; Yin
et al. 1995; Fetherston 2004); Table 1]. Ta-bearing peg-
matites and Ta-rich granites share the following charac-
teristics (Table 1 and references therein):
• Major element compositions close to the granite
eutectic, with extremely low mafic components (Mg,
Fe and Ca).
• Enrichment in Li, Cs, Rb, and to a lesser extent Sn and
Be.
• Low concentrations of Ti, Zr and LREE, with LREE
depleted relative to HREE.
• High Nb and Ta contents and high Ta/Nb.
The behaviour of trace elements during melting and
fractional crystallization is controlled primarily by the
partition coefficients of minerals with melt (expressed as
DTa = Tain mineral/Tain melt). Feldspars and quartz have
negligible Nb and Ta contents (Nash and Crecraft 1985;
Acosta-Vigil et al. 2010) and thus do not fractionate these
elements. Niobium and Ta have affinity to Ti, and major
hosts for Nb and Ta in granitoids are the Ti-bearing oxides:
ilmenite, titanite, rutile or magnetite, or silicates: micas and
amphiboles (Nash and Crecraft 1985; Acosta-Vigil et al.

Table 1 Characteristics of some major Ta deposits

Deposit Type Age, Ma Resources, Nb, Ta, Ta/ Ti, By- References
ore, Mt ppm ppm Nb ppm products

Mt Cassiterite (Wodgina), pegmatite 2890–2,830 35 50 250 5 \60 Sn (Sweetapple and Collins 2002)
Australia
Greenbushes, Australia pegmatite 2,527 192 150 500 Li, Sn (Partington 1990; Partington et al.
1995; Klementová and
Rieder 2004)
Tanco, Canada pegmatite 2,576 25 56 300 5.4 100 Cs, Li (Stilling et al. 2006)
Central Africa (Congo, pegmatite 950–990 nk nk nk nk nk Sn (Pohl 2011)
Rwanda, Mozambique)
Volta Grande, Brazil pegmatite 1,930 6.32 64 307 4.8 nk Sn, Li, Fsp (Heinrich 1964; Lagache and
Quemeneur 1997; Schwela 2010)
Abu Dabbab, Egypt Ta-granite 560 44.5 80 205 2.5 nk Sn (Gippsland 2013; Papp 2011)
Nuweibi, Egypt Ta-granite 560 98 66 117 1.8 nk Sn (Gippsland 2013; Papp 2011)
Yichun, China Ta-granite 181 nk nk 150 nk 250 Sn (Yin et al. 1995)
Orlovka, Russia Ta-granite 140 nk 150 200 1.3 100 (Zaraisky et al. 2009)
Ma—millions years; Mt—million tonnes; nk—not known; Fsp—feldspar mined for ceramics

123
Contrib Mineral Petrol (2014) 167:1009
2010; Stepanov and Hermann 2013). Fractional crystalli-
zation is modelled by the Rayleigh formula Cl = C0FD-1
where C0 is original concentration and Cl is concentration
in melt when F fraction of initial melt left after crystalli-
zation of solids with bulk partitioning coefficient D.
Magmatic fractionation of Ti–Nb–Ta in granites
Modelling of fractional crystallization in Ti–Nb–Ta space
demonstrates that each mineral that hosts Ti, Nb and Ta
changes the melt composition in a specific direction
(Fig. 2a, b). Crystallization of Ti-bearing oxides (rutile,
titanite and ilmenite) decreases Ti content and Ta/Nb of the
melts; magnetite reduces the Ti content without fraction-
ating Nb and Ta; amphibole produces mild Ta/Nb
(a)
(c)
Fig. 2 a and b vectors of compositional evolution of granites with
fractionation of the principal minerals: Bt—biotite; Ms—muscovite;
Mgt—magnetite; Ilm—ilmenite; Rt—rutile; Ttn—titanite; Amph—
amphibole. The fractionation vectors are calculated for 50 %
crystallization; diamonds on vectors show 10 % fractionation incre-
ments. Partitioning coefficients and mineral fractions used for
modelling are given in Table 2. The parental liquid composition is
1 wt% TiO2, 5 ppm Nb and 1 ppm Ta. Ta/Nb ratios in granites
Page 3 of 8 1009
fractionation, but leaves Ti in the melt (Tiepolo et al. 2000;
Stepanov and Hermann 2013); and finally, biotite and
muscovite fractionation significantly increases Ta/Nb and
decreases the Ti content of the melt. The decrease in Ta
and Nb contents and Ta/Nb produced by fractionation of
rutile, ilmenite and titanite is the opposite of the trends
observed in granites where Ta/Nb increases with decreas-
ing Ti (Fig. 2c, d).
The increase in Ta/Nb and Ta content together with
decrease in Ti content observed in many granites can be
modelled by fractionation of biotite and muscovite (Fig. 2).
Biotite is a major host for Nb and Ta during crustal melting
(Stepanov and Hermann 2013). The role of muscovite as a
host for Nb and Ta is less well known; however, experimental
data (Stepanov and Hermann 2013) demonstrate that high
pressure muscovite (phengite) has DNb [ DTa similar to
(b)
(d)
relative to c TiO2 and d Ta concentrations in a fractionated series of
granites from various areas. The grey arrows represent schematic
trends of melt evolution, see text for discussion. Granite composi-
tions: Novas Scotia—Dostal and Chatterjee (2000); Kalguty—
Sokolova et al. (2011); Beauvoir—Raimbault et al. (1995); Armor-
ican—Tartèse and Boulvais (2010); Tanco—Stilling et al. (2006) and
Erzgebirge—Förster et al. (1999)
123
1009 Page 4 of 8 Contrib Mineral Petrol (2014) 167:1009

Table 2 Partitioning coefficients used for fractionation modelling proposed that the lower solubility of columbite relative to
presented at Fig. 2 tantalite might be the driving force behind fractionation of
DTi DNb DTa References Abundance Nb from Ta in evolved melts (Linnen and Keppler 1997;
in model % Linnen 1998; Chevychelov et al. 2010; Bartels et al. 2010;
Fiege et al. 2011). This idea is supported by dissolution
Biotite 15 3.6 1.2 (Nash and 10
Crecraft 1985) experiments of natural columbite (Chevychelov et al. 2010)
Muscovite 19 3.5 0.4 (Raimbault and 10 where Nb appeared more compatible than Ta (i.e. DNb/
Burnol 1998) DTa [ 1 for columbite) and increasing Ta/Nb in colum-
Magnetite 40 2.2 2.5 (Nash and 5 bite–tantalite during fractionation of pegmatites (London
Crecraft 1985) 2008). However, compositional trends in granites and
Titanite 21 7.6 19.6 (Green and 7 measured solubilities argue against a major role for col-
Pearson 1987) umbite–tantalite in Nb–Ta fractionation. The crystalliza-
Rutile 115 61 112 (Xiong et al. 2 tion of Nb minerals should decrease Nb contents in the
2011)
melts. Conversely in the Beauvoir granite (Raimbault et al.
Ilmenite 117 73 86 (Nash and 2
Crecraft 1985)
1995), Nb contents increase with fractionation (Raimbault
et al. 1995). Experimental solubility studies demonstrate
Amphibole 8.8 1.6 1.0 (Tiepolo et al. 10
2000) that columbite and tantalite are highly soluble in granitic
melts (100 s ppm to weight %, Linnen and Keppler 1997;
Abundance % is amount of mineral used in the modelling of frac-
tional crystallization at Fig. 2
Linnen 1998; Chevychelov et al. 2010) and hydrosilicate
liquids (Smirnov et al. 2012). Solubilities of thousands of
ppm of Ta and Nb observed in experimentally and mea-
biotite. Empirical estimates of partition coefficients also sured in pegmatite melt inclusions (Thomas et al. 2011) are
demonstrate DNb [ DTa and DNb/DTa as high as 8.7 (Rai- comparable to, or exceed Ta concentrations in economic
mbault and Burnol 1998). Additional evidence is supplied by Ta deposits (Table 1). Therefore, it is likely that tantalite–
published trace element compositions of micas in granites. columbite saturation of melts occurs only in the most
Muscovite in granites and pegmatites from the Barroso–Alvão fractionated granitic melts and is not the primary control on
pegmatite field, Portugal, have high Nb (43–220 ppm) and Ta enrichment. Petrographic evidence also points to late sat-
(3–44 ppm) and relatively low Ta/Nb (0.06 in granites and uration of Ta–Nb minerals (Van Lichtervelde et al. 2007;
0.07–0.11 in pegmatites, compare with crustal Ta/Nb of 0.08) Černý et al. 2012).
(Martins et al. 2012). In the Tanco pegmatite, magmatic micas
have high concentrations of Nb (17–120 ppm) and Ta
(36–360 ppm) and Ta/Nb from 1 to 3.5 (Lichtervelde et al. Discussion
2008), which are substantially lower than the bulk Tanco
pegmatite (Ta/Nb of 5.4, Table 1). These data demonstrate Nb–Ta fractionation in the melt sources
that muscovite in evolved granites have high Nb and Ta
concentrations and a strong preference for Nb relative to Ta. Granitic melts form by partial melting of the lower crust
Modelling of Rayleigh fractional crystallization predicts through vapour-absent melting reactions that consume
that 90 % crystallization of granite with 10 % biotite muscovite (phengite at high pressure), biotite and amphi-
would increase Ta/Nb by 30 % in the residual melt, bole (Vielzeuf and Holloway 1988; Vielzeuf and Montel
whereas muscovite crystallization would double Ta/Nb. 1994). The upper continental crust has Ta/Nb of 0.08–0.1
Crystallization of 99.9 % of melts precipitating 10 % of and around 1 ppm Ta (Barth et al. 2000). Anatexis of
muscovite might increase Ta/Nb by a factor of 8 and crustal rocks results in higher Ta/Nb in partial melts
concentrate Ta to 760 ppm in the residual melt. Fractional compared to their protolith due to the effect of residual
crystallization of biotite and muscovite reproduces the biotite (Stepanov and Hermann 2013). The Ta/Nb of
decrease in Ti content and the increase in Ta/Nb observed 0.17–0.25 observed in anatectic melts (Acosta-Vigil et al.
in granites (Fig. 2). The high partitioning coefficients for 2010) are close to the Ta/Nb of the least evolved granites in
Ti in biotite and muscovite cause a rapid decrease in Ti a fractionated granitic series (Fig. 2). Therefore, elevated
content in the residual melt. This suppresses saturation of Ta/Nb is a normal feature of crustal granitic melts, and
Ti-bearing oxides during crystallization and precludes a biotite-present melting represents the first stage in the
decrease in Ta content in the melt due to the crystallization generation of Ta-rich melts. If anatexis occurs at higher
of these phases. temperature at which micas are completely consumed, then
The primary ore mineral in Ta deposits is columbite– the main hosts for Nb and Ta become Ti-bearing oxides
tantalite (Linnen et al. 2012). A number of studies (titanite, rutile and ilmenite), which all partition Ta relative

123
Contrib Mineral Petrol (2014) 167:1009
to Nb (Nash and Crecraft 1985; Prowatke and Klemme
2005; Xiong et al. 2011; Olin and Wolff 2012). Hence,
high-temperature anatexis produces lower Ta/Nb partial
melts than their source, and such melts are unlikely to
evolve into Ta-rich magmas. High-temperature melts are
also likely to have high Ti and low water contents. These
features favour saturation in Ti-oxides over biotite, and
hence, melts evolve to low Ta concentrations.
Tantalum-rich melts are unlikely to form from low
degrees of partial melting, which is commonly invoked in
the formation of melts rich in very incompatible elements
(e. g. Turner et al. 1996). This is because of the inevitable
presence of Ti-rich minerals in which Ta can be compatible
in crustal rocks. Granitic melts with elevated Ta/Nb are
formed by means of melting in the presence of residual
biotite; however, Ta enrichment is yet to occur.
Origin of pegmatite types
Pegmatites form two distinct compositional classes: the
LCT type characterized by enrichment in Li, Cs and Ta,
and the NYF type, which are high in Nb, Y (and HREE)
and F (Černý and Ercit 2005). Given that one is named for
Ta (LCT type) and the other for Nb (NYF Type), an
understanding of the fractionation of these two elements
should clarify the origin of these two classes.
LCT-type pegmatites are derived from hydrous granitic
magmas often derived from sedimentary protolith (S-type).
The hydrous composition and low temperatures of these
melts favour fractionation of biotite and muscovite, which
results in high Ta concentrations and elevated Ta/Nb. The
characteristic feature of the LCT pegmatites is low LREE
contents and fractionated REE patterns with negative Nd
anomalies. These features can be explained by fraction-
ation of monazite (Stepanov et al. 2012). Another feature
of LCT-type pegmatites and Ta-rich intrusives is low Zr
contents and low Zr/Hf (Zaraisky et al. 2009) related to
fractionation of zircon from granitic melt (Linnen and
Keppler 2002; Claiborne et al. 2006). Formation of Ta-rich
melts by biotite and muscovite fractionation is consistent
with the association of Ta deposits with biotite-bearing
granites, (Kostitsyn et al. 2004).
The NYF-type pegmatites tend to form from higher
temperature melts, which results in less biotite fraction-
ation and late saturation of accessory monazite and zircon.
Therefore, fractionation of feldspars and quartz results in
enrichment in REE, Nb and Ta. In these granites, amphi-
bole fractionation could affect Nb/Ta, which occurs, for
instance, in arfvedsonite-bearing granites from Africa
(Schmitt et al. 2002; Ogunleye et al. 2005). In these
granites, Nb enrichment is extreme (up to 0.3 wt%) but
Ta/Nb varies little. This is due to the low DNb and DNb/DTa
Page 5 of 8 1009
close to unity for melt–amphibole (Tiepolo et al. 2000;
Stepanov and Hermann 2013). Interestingly, large Ta
deposits are associated only with LCT-type pegmatites,
while pegmatites of NYF type are not significant Ta and
Nb sources.
Fractionation in natural systems
This contribution discusses results of modelling of Ray-
leigh fractional crystallization of Ti-bearing minerals on
the evolution of Ti, Nb and Ta concentrations in melts. In
natural systems, fractionation is more complex due to
variations in partitioning coefficients and abundances of
minerals. Additionally, Rayleigh fractionation assumes
infinitely fast diffusion in the melt and infinitely slow
diffusion in solids or immediate separation of solids and
melt upon crystallization.
The partitioning coefficients between melt and solids can
vary with temperature, pressure and melt/mineral composi-
tion. The availability of partitioning coefficients differs for
different minerals. Quality experimental data are available
for rutile and titanite and indicate that DNb and DTa increase
with decreasing temperature and DNb/DTa increase at lower
temperatures (Xiong et al. 2011). For amphiboles, Nb and Ta
partitioning coefficients are available only for basaltic melts
(Tiepolo et al. 2000). For biotite, Stepanov and Hermann
(2013) demonstrated that the range of DNb and DTa exceeds
analytical uncertainty; however, the dataset is insufficient for
estimation of the effect of various parameters on D’s. For
muscovite, the only available DNb and DTa are from natural
rock (Raimbault and Burnol 1998). Therefore, while mod-
elling in Fig. 2 presents vectors of melt evolution, additional
experimental data on partitioning and constraints on mech-
anisms of separation of melts and cumulates would be nec-
essary for precise modelling of fractional crystallization.
Zonation of Nb–Ta minerals in pegmatites
Ta and Nb minerals are often zoned in pegmatites. The most
common zonation in minerals of the columbite–tantalite
series is increasing Ta/Nb from core to rim. This trend results
from preferential partitioning of Nb into tantalite–columbite
(Linnen and Keppler 1997; Chevychelov et al. 2010).
However, some columbite–tantalite minerals show sudden
increase in Nb contents in the outer zones of crystals, and this
zonation is attribute to either addition of high Nb melt or
complex fluid–melt interaction (Černý et al. 1986; Zhang
et al. 2004; London 2008). On contrary, this ‘‘reversed
zoning’’ can be explained by a release of Nb from recrys-
tallized magmatic mica. Additionally, recrystallization of
primary magmatic mica might produce columbite in rocks,
which were not initially columbite saturated.
123
1009 Page 6 of 8
Conclusions
The genetic model proposed by this study emphasizes the
importance of biotite and muscovite fractionation in the
formation of Ta-rich granitic melts. Economic concen-
trations of Ta in pegmatites and leucogranites should be
expected only in the vicinity of fractionated biotite-
bearing granitic intrusions. Granites that experience sig-
nificant fractionation of rutile, ilmenite and titanite lose a
large fraction of their Ta and Nb in the early stages of
crystallization and are unlikely to develop high Ta con-
tents. Modelling of fractional crystallization predicts that
only small fractions of the original liquid will acquire
high Ta/Nb and Ta contents. Extraction of these volu-
metrically minor melts from host intrusions becomes
possible due to the low viscosities of the volatiles-rich
melts (Thomas et al. 2012). Possibly, several stages of
melt extraction and fractional crystallization are required
for the formation of melts with economic concentrations
of Ta. In order to produce such intrusions, and to pro-
duce sufficient melt to form an economic deposit, the
starting intrusion needs to be large. Regions with large,
fractionated granitic intrusions with biotite in their early
stages and muscovite in their late stage differentiates
are predicted to be the most prospective for Ta
mineralization.
Acknowledgments We thank D. H. Green, I. C. Campbell, M.
T. Sweetapple, J. A. Halpin, D. R. Cooke, S. Z. Smirnov, V.
Kamenetsky and reviewers by R. Linnen and A. Hack for constructive
comments that significantly improved the manuscript.
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