Mineralium Deposita (2001) 36: 93100
LETTER
Peter J. Pollard
Sodic(calcic) alteration in Fe-oxideCuAu districts: an origin via
unmixing of magmatic H2OCO2NaCl CaCl2KCl uids
Received: 26 May 1999 / Accepted: 8 June 2000
Abstract Iron-oxideCuAu deposits, particularly those formed in
deeper level (plutonic) environments, are commonly characterized
by regional scale sodic(calcic) alteration, which typically formed
pre- or syn-CuAu mineralization. The sodic(calcic) assemblages
include albite, scapolite, pyroxene, actinolite, apatite, titanite, epi-
dote and calcite. The consistent presence of coexisting hypersaline
aqueous and CO2-rich uids in minerals from sodic(calcic) alter-
ation and associated Fe-oxideCuAu deposits is the result of
unmixing of H2OCO2NaCl CaCl2KCl magmatic uids. Ex- quences, a process capable of resulting in the addition of these
perimental evidence indicates that the Na/(Na + K) ratio of uids
in equilibrium with two alkali feldspars in CO23 -bearing parent
uids would be signicantly higher than in unmixed chloride-
bearing aqueous uids. Therefore, uid unmixing caused by de-
creases in temperature and/or pressure, will result in albitization of
wall rocks, as is observed in most deeper level Fe-oxideCuAu
deposits. This alteration style may be succeeded by K-feldspath-
ization with decreasing temperature because of the increase in
equilibrium Na/(Na + K) in chloride-bearing uids buered by
alkali feldspars.
Introduction
Regional scale alteration systems dominated by Na- and Ca-rich
minerals, which include albite, scapolite, actinolite, clinopyroxene,
apatite, titanite, epidote and calcite, are a feature of many districts
that host Fe-oxideCuAu deposits (Williams and Blake 1993;
Barton and Johnson 1996; Frietsch et al. 1997). Mineralogically
similar alteration is also recognized in porphyry-related CuAu
deposits (e.g. Carten 1986). The mechanism of formation of sodic(
calcic) alteration and its relationship to CuAu mineralization is of
special interest, as models that envisage a dominantly magmatic
source for uids and metals (Perring et al. 1999, 2000) will lead to
quite dierent exploration strategies than those that consider
contributions from evaporitic host rocks (e.g. Barton and Johnson
1996). In either case, large volumes of rock are commonly aected
by sodic(calcic) alteration, and large amounts of metals may be
Editorial handling: R. R. Large
P. J. Pollard
Economic Geology Research Unit, School of Earth Sciences,
James Cook University, Townsville,
Queensland 4811, Australia
e-mail: peter.pollard@jcu.edu.au
Tel.: +61-7-47815050; Fax: +61-7-47251501
Springer-Verlag 2001
mobilized from some rock types into the uid phase and be
available for subsequent mineralization (e.g. Dilles and Einaudi
1992).
The introduction of signicant amounts of Na and Ca during
sodic(calcic) alteration is commonly attributed to feldsparuid
exchange occurring when externally-derived uids are heated as
they are drawn toward magmatic heat sources (Dilles and Einaudi
1992). The hot uids may also interact with evaporite-bearing se-
elemental species that contribute to later alteration (Barton and
Johnson 1996).
Examination of paragenetic relationships, uid inclusions and
stable isotope data for sodic(calcic) altered rocks and Fe-oxide
CuAu mineralization, particularly in the Mt. Isa Inlier, Australia
(Fig. 1), suggests that alteration results from the unmixing of H2O
CO2NaCl CaCl2KCl uids derived from granitoid magmas.
It does not require the presence of evaporitic rocks and/or heating
of externally-derived uids for introduction of sodium and calcium
into the hydrothermal system, although these processes may also
contribute to alteration.
Fe-oxideCuAu districts and sodic(calcic) alteration
Hitzman et al. (1992) proposed a new iron oxide [CuUAurare
earth element (REE)] class of ore deposits. This includes `Kiruna-
type' iron ore deposits in northern Sweden, Cu U Au
REE deposits that include Olympic Dam in Australia, and Fe
CuAu deposits in the coastal batholith of Chile. These deposits
are commonly dominated by iron oxides (magnetite and/or he-
matite), and occur in alteration zones of variable character. At the
district-scale, alteration tends to be dominated by sodic alteration
at depth, potassic alteration at intermediate to shallow levels, and
sericitic and silicic alteration at very shallow levels (Hitzman et al.
1992). Among the CuAu deposits, magnetite-dominated systems
are common in deeper environments such as characteristic of the
Mount Isa eastern fold belt (also referred to as the Cloncurry
district), Australia (Williams 1998; Fig. 1), where the granitoids
that are broadly contemporaneous with mineralization were em-
placed at 1015 km depth (Pollard et al. 1998). Hematite-domi-
nated systems are common in shallower (subvolcanic)
environments such as at Olympic Dam (Reeve et al. 1990) and in
the coastal batholith of Chile (e.g. Espinoza et al. 1996).
In deeper level Fe-oxideCuAu districts, sodic(calcic) altera-
tion is commonly present as a very widespread alteration style
(Hitzman et al. 1992; De Jong and Williams 1995; Freitsch et al.
1997) in a variety of host rocks (Table 1). Sodic(calcic) assemblages
are commonly accompanied by CuAu mineralization (Table 1), but
in some cases mineralization was associated with potassic alteration
94

b deformation (De Jong and Williams 1995; Oliver 1995; Rubenach
Fig. 1 Geology of the eastern part of the Mt. Isa Inlier showing the
distribution of the mineral deposits discussed in the paper. (Modied
from Blake 1987)
(biotite and/or K-feldspar) that overprinted earlier sodic(calcic)
alteration. Sodic(calcic) alteration is present in all documented Cu
Au deposits in the Mount Isa eastern fold belt. Some of these deposits
have pre-ore and/or ore-stage assemblages dominated by sodic-
(calcic) minerals, e.g. Mount Elliott (pyroxene, scapolite, actinolite,
magnetite, titanite; Wang and Williams 1996), Osborne (albiteac-
tinolitemagnetite; Adshead 1995), Lightning Creek (pyroxene, al-
bite, magnetite, quartz, titanite; Perring et al. 1999), and Great
Australia (carbonate, amphibole, magnetite; Cannell and Davidson
1998). However, mineralization in other deposits was accompanied
by potassic alteration that overprinted pre-ore sodic(calcic) altera-
tion (e.g. Greenmount: Krcmarov and Stewart 1998; Starra: Roth-
erham et al. 1998; and Ernest Henry: Mark and Crookes 1999).
Styles of sodic(calcic) alteration in the Mt. Isa
eastern fold belt
Sodic(calcic) alteration occurs within and adjacent to a wide va-
riety of brittle and ductile structures in the Mount Isa eastern fold
belt (Fig. 2). In some cases, there is evidence for multiple, over-
printing stages of sodic(calcic) alteration. The most common types
of structural controls for sodic(calcic) alteration include brittle
ductile shear zones, ductile fabrics (cleavages) linked to regional
95
and Barker 1998), breccia complexes (De Jong and Williams 1995;
Mark 1998), and brittle fracture systems (veins).
Large volumes of rock with sodic(calcic) alteration are asso-
ciated with the formation of breccia complexes that are particularly
well-exposed along the Cloncurry fault (e.g. De Jong and Williams
1995; Mark 1998). These breccias occur predominantly in the roof
zones and margins of the Williams and Naraku batholiths and, at
least in part, were developed during multiple episodes of granitoid
intrusion (Mark and De Jong 1996; Mark 1998). Breccia zones
from tens to hundreds of metres across commonly consist of clasts
of albitized host rocks (metasediment, calc-silicate rock, granitoid,
amphibolite) in a matrix composed of sodic(calcic) minerals. Clast
sizes vary considerably in the breccias, with large clasts (metres
across) being mainly subangular to angular, whereas the smaller
clasts are commonly more rounded. The presence of rounded clasts
of mixed rock types in a matrix of secondary minerals suggests that
the sodic(calcic) breccias are, in part, hydrothermal intrusive
breccias. Brecciation of this type is commonly formed by upward
escape of a magmatic vapour phase that promotes fracturing and
milling of intrusion roof rocks, with alteration of clasts and matrix
by later high-salinity magmatic uids (e.g. Grant et al. 1980).
Pervasive clinopyroxenealbite titanite calcite alteration
overprints monzodiorite and monzogranite at the Lightning Creek
prospect (Perring et al. 1999, 2000). No uid channel-ways have
been observed to be associated with this alteration, and uid
movement appears to have been controlled predominantly by grain
boundaries and microfractures. Quartz and feldspar from the
sodic(calcic) altered granitoids have similar oxygen isotope com-
positions to those in the unaltered granitoids, which has been

Table 1 Sodic(calcic) alteration and inll assemblages from Fe-oxideCuAu districts

Host rock Host lithology Sodic(calcic) alteration Inll assemblage References

age assemblage

Mary Kathleen Proterozoic Calc-silicate rocks Albiteamphibolecalcite Calcite Oliver et al. (1993)
fold belt, titanite clinopyroxene quartz clinopyroxene
Australia biotiteapatite amphiboledolomite
chalcopyritepyrrhotite
Metadolerite Albiteamphibolecalcite Calcite Oliver et al. (1993)
titanite clinopyroxene quartz clinopyroxene
amphiboledolomite
chalcopyritepyrrhotite
Mt.Isa eastern Proterozoic Tonalite Albitemagnetite Albitemagnetitequartz Mark (1998)
fold belt, quartz titanite calcite
Australia actinolite
Metabasite, calc Albitic plagioclase(An5-15) De Jong and Williams
silicate rocks, actinolitetitanite (1995)
metapelite, apatite quartz
granitoid magnetiteclinopyroxene
Quartz Albiteclinopyroxene Perring et al. (1999)
monzodiorite, titanitecalcite
monzogranite
Pahtohavare, Proterozoic Metabasite Albite Dolomitecalcitequartz Lindblom et al. (1996)
Sweden scapolite biotitealbite
Bidjovagge, Proterozoic Graphitic schist, Albitecalcitescapolite- Quartzcarbonate Bjorlykke et al. (1987);
Norway diabase amphibolebiotite actinolitemagnetite Ettner et al. (1993)
pyritepyrrhotite
chalcopyrite apatite
muscovite
Punta Del Cretaceous Dacitic rock Albite Marschik and
Cobre district, Fontbote (1996)
Chile
El Algarrobo, Cretaceous Diorite Sodic plagioclasequartz Menard (1995)
Chile rutiletitanite
96
Fig. 2 Cartoon to illustrate geological environments of sodic(calcic)
alteration and Fe-oxideCuAu deposits in the Mount Isa eastern
fold belt (Cloncurry district)
interpreted to indicate that the uid responsible for alteration was
hot (600650 C) and of similar isotopic composition to primary
magmatic uids (Perring et al. 1999).
Subhorizontal granitic sills cut the pervasive sodic(calcic) al-
teration at the Lightning Creek prospect. They display a transition
from magmatic crystallization to hydrothermal uid exsolution as
supported by localized albitization of the sills and development of
magnetiteclinopyroxenealbitequartzapatitetitanite pyrite Kathleen fold belt. Results suggested that >80% of the uid re-
veins (Perring et al. 1999). Proton-induced X-ray emission (PIXE)
analysis of hypersaline uid inclusions in quartz from a magnetite-
rich portion of one of the sills indicates that the uids are rich in Cl
(40 wt%), Na (halite present at room temperature), K (6
16 wt%), Ca (5 wt%), Fe (10 wt%), Ba (0.51.0 wt%) and Cu
(>1 wt%; Perring et al. 1999, 2000).
Mechanism for development of sodic(calcic) alteration
The K/Na ratio of chloride-bearing uids in equilibrium with two
alkali feldspars increases with increasing temperature (Orville
1963). A uid that is heated as it is drawn into a convective system
would, therefore, be capable of causing albitization, with K-feld-
spar alteration at lower temperatures. This temperature-dependent
exchange model has been used by Dilles and Einaudi (1992),
Hitzman et al. (1992) and De Jong and Williams (1995) to explain
sodic(calcic) alteration. Barton and Johnson (1996) proposed that
the uids related to Fe-oxide (REECuAuU) deposits gain Cl
and Na from coeval or ancient evaporites along uid ow pathways
to cause albitization in downwelling parts of the system, and in
upwelling parts where water/rock ratios are high.
Stable isotope investigations in the Mary Kathleen fold belt and
Mount Isa eastern fold belt (Oliver et al. 1993; Aslund et al. 1995;
Mark et al. 1999; Perring et al. 1999) suggest that sodic(calcic)
assemblages were formed at high temperatures (>500 C, and
commonly >600 C) from magmatic-hydrothermal uids. Oliver
et al. (1993) modelled carbon and oxygen isotope data for calcite
from sodic(calcic) alteration/inll zones in the 200-km-long Mary
sponsible for alteration was magmatic, with a small proportion
possibly derived from, and in isotopic equilibrium with, the calc-
silicate rocks.
Fluid inclusion data from Fe-oxideCuAu districts (Table 2)
commonly indicate the presence of both hypersaline aqueous and
low-salinity CO2-rich uids during alteration and mineralization.
These are commonly interpreted to have formed by unmixing of an
original H2OCO2NaCl CaCl2 uid (Ettner et al. 1993; Oliver
1995; Adshead et al. 1998). Perring et al. (1999) found that similar
uids were exsolved during crystallization of granitic sills at the
Lightning Creek prospect in the Mount Isa eastern fold belt. This is
consistent with a magmatic origin for the uids responsible for
sodic(calcic) alteration and Fe-oxideCuAu mineralization, in
agreement with the stable isotope data referred to above.
The presence of anionic species other than Cl in hydrothermal
uids has a signicant eect on feldspar-uid equilibria (Iiyama
1965). In experiments at 600 C and 1 kbar, Iiyama (1965) showed
that CO23 -bearing uids are signicantly enriched in sodium with
respect to Cl-bearing uids. Equilibrium Na/(Na + K) expressed
 97

Table 2 Fluid inclusion data from Fe-oxideCuAu deposits and districts. Hypersaline is used to refer to uid inclusions containing
multiple solid phases where the total salinity has not been specied

Deposit/district Host minerals Primary uid inclusion types References

Punta Del Cobre, Chile Post-ore calcite 3034 wt% eq. NaCl Marschik and Fontbote (1996)
Salobo, Brazil Quartz 1. CO2 CH4 Lindenmayer and Teixeira (1999)
2. 3952 wt% eq. NaCl
Bidjovagge, Norway Quartz 1. CO2 CH4N2 Ettner et al. (1993);
2. CH4 Ettner et al. (1994)
3. H2ONaClCaCl2 CO2CH4
(CuAu mineralization 25 wt% NaCl + CaCl2,
AuCu mineralization 3045 wt% eq. NaCl)
Pahtohavare, Sweden Quartz 1. CO2 Lindblom et al. (1996)
2. Hypersaline
3. H2ONaClCaCl2
Mary Kathleen fold Quartz 1. CO2 Oliver (1995)
belt, Australia 2. CO2H2OCaCl2 (35 wt% eq. CaCl2)
3. NaClH2OCaCl2KCl (>30 wt% eq. NaCl)
Mt. Isa eastern fold belt, Australia
Osborne Quartz 1. CO2 Adshead et al. (1998)
2. Hypersaline
3. 2037 wt% eq. NaCl
Starra (ironstone) Quartz 1. CO2 Rotherham et al. (1998)
2. 3452 wt% eq. NaCl
Lightning Creek Quartz 1. CO2 Perring et al. (1999)
2. hypersaline
Eloise Quartz 1. CO2 + H2O Baker (1998)
2. Hypersaline
3. 3047 wt% eq. NaCl

as concentrations of salts (molarity) in solution is 0.79 in Cl-rich

uids and 0.96 in CO23 -rich uids (Iiyama 1965; Fig. 3). An H2O
CO2 uid containing a high concentration of Cl, and in equilib-
rium with alkali feldspar-rich rock (e.g. granitoid) should, there-
fore, have a Na/(Na + K) value greater than that of an aqueous
uid in equilibrium with the same rock.
Fluid unmixing resulting from decreases in pressure and/or
temperature causes partitioning of CO2 to the vapour phase and
salts to the liquid phase (Bowers and Helgeson 1983). It may cause
an increase in pH of the liquid phase because of displacement of
reaction (1) to the right by CO2 escape from the aqueous phase
(Reed and Spycher 1985).
HCO3 H ! H2 O CO2
1
aq aq aq gas
This initially causes the concentration of CO23 to increase because
the increase in pH displaces reaction (2) to the right (Reed and
Spycher 1985), but will eventually be reversed by removal of CO2
from the original uid (see Fournier 1985).
HCO3 ! H CO23 2
Following unmixing, the CO2-poor aqueous-rich uid will have a
Na/(Na + K) value greater than the equilibrium value for a Cl-
bearing uid in equilibrium with two alkali feldspars. In order to
approach equilibrium, the uid must contribute sodium to, and
gain potassium from, the wall rocks (albitization).
The timing and mechanism of uid saturation in the magmas
and subsequent uid unmixing has not been well-established in
Fe-oxideCuAu districts. The low solubility of CO2 in granitic
magmas (Holloway 1976) suggests that pressure decrease during
upward intrusion of the magmas may cause CO2 saturation, Fig. 3 Exchange equilibria between alkali feldspars and KNa
although the addition of CO2 from devolatilization of carbonate- solutions with Cl)1 and CO23 anions at 600 C and 1 kbar. The
bearing host rocks could also be signicant. Saturation of the NamA/(NamA + KmA) values are concentrations in solution, where
magma in CO2 would result in partitioning of water, chlorine A is the anionic species and m is the number of cations. (Modied
and metals to the uid phase. from Iiyama 1965)
98
Fluid unmixing via isothermal pressure decrease would result in
a large miscibility gap between liquid and vapour (Bowers and
Helgeson 1983), leading to maximum albitization, while isobaric
temperature decrease would result in progressive unmixing. Per-
vasive alteration, such as that described at the Lightning Creek
prospect, could reect early, essentially isobaric unmixing in the
magma chamber, where the uids interact with previously crys-
tallized granitoid during inltration along grain boundaries and
microfractures.
Fluid saturation in crystallizing magmas and subsequent exso-
lution and unmixing of these uids results in volume expansion that
can cause brecciation (Burnham and Ohmoto 1980). The extensive
hydrothermal intrusive breccias associated with sodic(calcic) al-
teration in the Mt. Isa eastern fold belt could be formed by this
mechanism, where brecciation was primarily caused by escape of
the CO2-rich vapour phase, and albitization was primarily caused
by later inltration of the salt-rich liquid phase.
Albitization, caused by unmixing of H2OCO2NaCl
CaCl2KCl uids as outlined above, will give way at lower tem-
peratures to K-metasomatism because equilibrium Na/(Na + K)
in the uid phase increases with decreasing temperature in Cl-
bearing uids (Orville 1963; Lagache and Weisbrod 1977). This can
explain the early albitization in Fe-oxideCuAu districts that is
commonly overprinted by K-rich metasomatism with the devel-
opment of K-feldspar and/or biotite. A 0.01 increase in equilibrium
Na/(Na + K) is equivalent to a temperature decrease of 25 C in
the chloride system (Lagache and Weisbrod 1977).
Calculation of the possible eects of unmixing of H2OCO2
NaCl uids is severely hampered by a lack of information on uid
compositions prior to unmixing and the Na/(Na + K) equilibrium
ratio in uids with multiple anionic species. Assuming 40 wt%
NaCl + KCl (see Table 2) and equilibrium (molar) Na/
(Na + K) 0.91 for an initial uid composition, the uid contains
35 wt% NaCl and 5 wt% KCl. Following unmixing and removal of
the CO2-rich vapour phase, the equilibrium Na/(Na + K) changes
to 0.79 (Iiyama 1965) and the new equilibrium composition of the
saline liquid phase will be 29.9 wt% NaCl and 10.1 wt% KCl. Each
kilogram of uid would need to contribute 20 g Na to the wall
rocks to reach equilibrium. Mass balance calculations for sodic-
(calcic) alteration in the Mount Isa eastern fold belt and Mary
Kathleen fold belt suggest that the altered rocks gained between
10 g (granite) and 34 g (psammitic schist) of Na per kg of rock
(Williams 1994; Aslund et al. 1995; Mark 1998). Each kilogram of
uid would therefore have the capacity to alter 0.5 to 2 kg of
rock. If, as seems likely, the shift in equilibrium Na/(Na + K)
caused by unmixing is less than the maximum 0.11 used above
(0.910.79), the amount of uid required to alter a given rock
volume will increase proportionately. For example, a change of
0.01 in equilibrium Na/(Na + K) would require 1.8 g of Na to
be contributed to the rock. Similarly, if the salinity of the original
uid was greater than the 40 wt% assumed above, the amount of
uid required for alteration would be lower.
In order to examine the capacity of magmatic-hydrothermal
uids to have caused sodic(calcic) alteration hosting Fe-oxideCu
Au deposits in the Mount Isa eastern fold belt, an estimate of the
amount of uid exsolved from the granitoids is required. The
crystallization of amphibole, magnetite and plagioclase within the
intrusions suggests water contents in the magmas of 4.56.5 wt%
(see Dall'Agnol et al. 1999). If it is assumed that 4 wt% H2O was
expelled during crystallization (40 g/kg of granite), and the salinity
was 40 wt% Na + K salts as in the example above, 1 kg of uid is
produced from each 15 kg of magma. Thus, in the case where un-
mixing causes a 0.11 shift in equilibrium Na/(Na + K), 7.530 kg
of granite is required for each kilogram of sodic(calcic) altered
rock. The 200 km2 of rocks dominated by sodic(calcic) alteration
in the southern part of the Eastern fold belt (De Jong and Williams
1995) would, therefore, require 1500 to 6000 km2 of granitoid to
provide sucient uid volume. The real extent of granitoids of the
Williams batholith is 2100 km2. However, the granitoids are also
continuous beneath the Proterozoic metasedimentary rocks (Well-
man 1992) and are also likely to be vertically extensive beneath
zones of sodic(calcic) alteration (e.g. Wyborn 1992).
The above calculations are necessarily simplistic given the un-
certainties in many of the variables, but they do serve to indicate
that unmixing of a magmatic CO2H2ONaCl uids can produce a
hypersaline aqueous uid capable of major amounts of sodic-
(calcic) alteration. This mechanism is also consistent with stable
isotope and uid inclusion data from such altered rocks and ex-
plains why uids originally in equilibrium with potassic magmas
can cause albitization during temperature drops.
Discussion
Unmixing of magmatic uids to produce sodic(calcic) alteration,
as outlined here, could also be applicable to chemically similar
uids derived from other sources. For example, uids derived by
devolatilization of carbonate-evaporite sequences during prograde
metamorphism contain high (but variable) concentrations of NaCl
and CO2. However, the preservation of large volatile activity gra-
dients at outcrop scales in the Mary Kathleen fold belt requires that
individual layers did not reach equilibrium with uid produced by
other layers to any signicant degree, and that the rocks were not
inltrated by any signicant volume of externally derived uid
(Oliver et al. 1992). This suggests that any alteration caused by an
unmixed hypersaline aqueous uid derived from the carbonate-
evaporite sequences themselves may be very localized. This is in
marked contrast to sodic(calcic)-altered rocks in the same region
that require large volumes of isotopically homogeneous uids
probably released from crystallizing magmas (Oliver et al. 1993).
The common occurrence of sodic(calcic) altered rocks sur-
rounding deeply formed Fe-oxideCuAu deposits can be ex-
plained by the unmixing of H2OCO2NaCl CaCl2KCl
magmatic uids. This is consistent with the spatial and temporal
association with intrusive rocks, and uid inclusion and stable
isotope data for the altered rocks. However, some sodic(calcic)
alteration in Fe-oxideCuAu districts may have resulted from
other suggested processes such as uid heating and/or interaction
of uids with evaporitic rocks. Because of the economic signicance
of the Fe-oxideCuAu deposits, it is important for exploration
modelling to discriminate between these dierent processes and
determine the signicance of each within given districts.
Acknowledgements This project was funded by the Australian
Mineral Industries Research Association (P438) and the Australian
Research Council Collaborative Research Grants Scheme. Pat
Williams, Geordie Mark, Nick Oliver and Roger Taylor are
thanked for numerous discussions on the origins of sodic(calcic
alteration). Scott Wood, Pat Williams, Roger Taylor and two
Mineralium Deposita reviewers are thanked for their comments on
the manuscript.
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