Beruflich Dokumente
Kultur Dokumente
J. W. HEDENQUIST,
Department of Geology and Geological Engineering, Colorado School of Mines, Golden, Colorado 80401-1887
H. SATOH,
Geological Survey of Japan, AIST Tsukuba Central 7, 1-1-1 Higashi, Tsukuba 305-8567, Japan
AND
Y. MATSUHISA
Geological Survey of Japan, AIST Tsukuba Central 7, 1-1-1 Higashi, Tsukuba 305-8567, Japan
Abstract
Most skarn ore deposits are characterized by two distinctly different alteration styles. An early prograde stage
with anhydrous minerals, such as garnet and pyroxene, forms from relatively high-temperature, hypersaline liquid. A later retrograde stage with hydrous minerals, such as epidote, amphibole, and chlorite plus sulfide ore
minerals, forms from lower temperature, lower salinity fluids. These two alteration stages commonly have been
thought to reflect a dominance of magmatic and meteoric water, respectively, with relevance to the source of
ore metals. We report data from two different skarn systems, one being part of the worlds largest Cu-Au resource. Stable isotope compositions of anhydrous and hydrous alteration minerals from both deposits indicate
a magmatic source for both the prograde and retrograde stages: 18O averages 5.0 per mil for garnet (range,
3.47.2), 6.5 per mil for pyroxene (4.38.2), and 7.1 per mil for amphibole (4.38.7). The D values of
late amphibole are more complex, with magmatic values (77 to 78) for one deposit and both magmatic
and lighter values for another deposit that could be explained either by magmatic degassing or by limited mixing with meteoric water. We conclude that the differences in fluid compositionprograde versus retrograde
stagesresulted from a magmatic fluid that intersected its solvus during the early stage, creating vapor and hypersaline liquid, whereas in the later stage this magmatic fluid did not intersect its solvus because it followed
a different cooling path. This late, low- salinity liquid only boiled once its vapor-pressure curve was reached,
causing sulfide ore to precipitate during the retrograde stage.
Introduction
THE SOURCE of ore fluids is one of the most important topics
of applied geologic research (Hedenquist and Lowenstern,
1994; Pettke and Diamond, 1997; Harris and Golding, 2002).
Many studies have demonstrated multiple sources of fluids responsible for forming ore deposits. A variety of theories of ore
genesis invoke interactions among such fluids, particularly
those of magmatic and meteoric origin (Giggenbach, 1997;
and Taylor, 1997, respectively). Since most skarn ores have an
intimate spatial relationship with magmatic intrusions, their
minerals should provide a clear record of the fluid(s) that were
present in the intrusive environment during ore formation.
Skarn ore deposits are typically characterized by two distinct
alteration styles: an early prograde stage with anhydrous minerals, such as garnet and pyroxene, which forms from relatively high-temperature, hypersaline liquid (Kwak, 1986); and
a later retrograde stage which consists of hydrous minerals,
such as epidote, amphibole, and chlorite, and forms from lower
temperature, lower salinity fluids (Kwak, 1986). These two alteration stages commonly are thought to reflect a dominance
Corresponding
147
148
MEINERT ET AL.
Ertsberg District
50
Papua
New
Guinea
70
Ti
45
Irian Jaya
Lembah
Tembaga
Ti
25Cairns
Australia
*
S4
Tk
Grasberg
Tk
Pacific
Ocean
Kkel
Sydney
Tw
Yello
w Va
lley S
yncli
ne
Kucing
Liar
Fig. 2A
Big Gossan
GBT
*
* *
*
Dom
Ertsberg
70
45
Puncak
Jaya
4883m
70
Intrusion (Ti)
Thrust fault
Tertiary
carbonate rocks
Cretaceous
clastic rocks
0
km
Fig. 2B
40
75
60
E137
FIG. 1. Location and geology of the Ertsberg district, Irian Jaya, showing major deposits and location of cross sections of
Figure 2 (modified from Meinert et al., 1997).
and the third largest copper mine in the world. The deposits
of the Ertsberg district collectively constitute the worlds
largest Cu-Au resource. At the end of 2001, proven and probable reserves were estimated at 2,600 Mt of ore at an average
grade of 1.13 percent Cu, 1.05 g/t Au, and 3.72 g/t Ag, containing 23.8 Mt of recoverable copper, 64.5 Moz of recoverable gold, and 151.6 Moz of recoverable silver (Freeport McMoRan Annual Report, 2001).
The Big Gossan Cu-Au skarn deposit is the highest grade
copper deposit in the Ertsberg district, with current reserves
of 37.4 Mt grading 2.69 percent Cu, 1.02 g/t Au, and 16 g/t Ag
(Meinert et al., 1997). Ore is associated with a series of 3 to 4
m.y. granodioritic dikes (McMahon, 1994 a, b, c) that have intruded close to the near-vertical faulted contact between the
Shale Member of the Cretaceous Ekmai Formation and the
stratigraphically overlying carbonate sequences of the Paleocene Waripi and Eocene Faumai Formations. Most mineralized and altered sequences occur in the purer carbonate
rocks of the Waripi Formation, although biotite and calc-silicate hornfels alteration also occur in the clastic footwall rocks
adjacent to skarn ore. The scale of the Big Gossan skarn system is more than 1 km along strike, more than 500 m vertically (open at depth), and up to 200 m in width for an aggregate volume of more than 0.1 km3 (Fig. 2).
The calcic magnesian skarn assemblage in the Waripi Formation hosts the bulk of the Big Gossan orebody and is characterized by relatively coarse-grained garnet and pyroxene,
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with an average mineral ratio of about 1:2. The average composition of all analyzed garnets is andradite84.7grossularite13.5spessartine1.5pyrope0.3. Garnet higher in the deposit and
on the western and eastern margins shows a slight increase in
iron relative to that in deeper, more central locations. The
iron content of pyroxene is zoned in both space and time. The
pale, proximal, and early pyroxene is nearly pure diopside
(Di) and the dark green, distal, and late pyroxene ranges up
to 75 mole percent hedenbergite (Hd) with minor johannsenite (Jo). In agreement with general skarn zonation
patterns (Meinert, 1992, 1997), pyroxene becomes more ironand manganese-rich toward the margins of the known deposit, suggesting that the hydrothermal system was centered
in the middle of the deposit, coincident with the largest mass
of dike. A similar zonation occurs vertically; the average pyroxene composition for the highest third of the skarn system
is Di58Hd38Jo4, whereas the average for the deepest third is
Di86Hd13Jo1.
Amphibole in the Big Gossan skarn system ranges from
actinolite to cummingtonite, with the main substitution being
Fe-Mg-Mn for Ca. Most amphibole occurs as an alteration
product of pyroxene, typically with quartz, carbonate, anhydrite, and sulfides. Subcalcic amphiboles occur on the margins of skarn where pyroxene has been totally replaced. In
these occurrences, amphibole is intimately intergrown with
quartz and carbonate, the latter ranging in composition from
calcite to manganiferous siderite, suggesting that the location
148
149
SW
NE
SW
NE
Elev. (m)
BGU 14-2
BGU 10-1
2900
Ertsberg Intrusion
BGU 14-3
BGU 10-3
Intrusive Breccia
2800
BGU 14-6
2600
Marble (Tw)
Kkeh marker shale
BGU 10-5
Kembelangan Group
2500
BGU 14-7
BGU 10-6
2400
FIG. 2. Cross sections through the Big Gossan skarn system showing the distribution of garnet and pyroxene skarn. Locations shown in Figure 1.
percent KCl and 35 wt percent NaCl. By contrast, fluid inclusions in quartz and anhydrite associated with retrograde alteration average 7.1 wt percent NaCl equiv and spatially associated fluid inclusions homogenize to liquid and vapor at
370 to 380C (Fig. 3C, D ). This corresponds to boiling at a
pressure of 20 MPa, equivalent to a depth of 2 km below the
paleowater table under hydrostatic conditions. Since these
samples came from 600 m beneath the present surface, the
data indicate that at least 1.4 km of erosion has occurred in
the Ertsberg district over the past 4 m.y.
Mines Gasp, Quebec
Like the Ertsberg district, Mines Gasp in Quebec has both
porphyry and skarn ore (Fig. 4); however, the Devonian host
rocks and porphyritic quartz monzonite stocks have U-Pb zircon ages of 385 2.6 Ma (Stephenson et al., 1998), which is
much older than the ages at Ertsberg. The Mines Gasp district was discovered in 1921 and has produced more than 150
Mt of ore averaging 0.9 percent Cu (with production grades
up to 3.4% Cu). It has new drilled resources at Porphyry
Mountain of 200 Mt grading 0.73 percent Cu and 0.08 percent Mo (Hussey and Bernard, 1998). The scale of the Porphyry Mountain skarn system is more than 1 km in diameter
and more than 800 m vertically (open at depth) for an aggregate volume of more than 0.8 km3 (Fig. 5).
The Devonian host rocks at Mines Gasp have been gently
folded and consist of carbonaceous silty limestone, calcareous
149
150
MEINERT ET AL.
FIG. 3. Photomicrographs of inclusions in skarn minerals. A. Multiphase fluid inclusion in pyroxene containing vapor
bubble (V), halite (H), sylvite (S), hematite? (Hm), and unknown mineral (X). B. Multiphase fluid inclusion in pyroxene
containing vapor bubble (V), halite (H), sylvite (S), and chalcopyrite (Cpy). C. Vapor-rich fluid inclusion in quartz. D. Part
of a large pyroxene crystal which has been completely altered to amphibole (amph) and anhydrite. The anhydrite contains
hundreds of vapor-rich fluid inclusions, most of which homogenize to vapor.
Quebec
Mines
Gaspe
Maine
Boston
1 km
Atlantic
Ocean
Porphyry
Mtn
920A
923
890
905 886
793
904
20
900
909
Copper
Mtn A'
N65
Murdochville
Shiphead Fm.
15
metamorphic aureole
(limit of bleaching)
E6530
Forillon Fm.
FIG. 4. Location and geology of the Mines Gasp district (modified from Allcock, 1982). Crosshatched areas are surface
projections of porphyry plutons. Sample locations are surface projections of drill holes.
siltstone and shale, and minor marker tuff beds of the Forillon, Shiphead, and Indian Cove Formations (Gower and
Walker, 1993). These units were intruded by the Copper
Mountain stock and the Porphyry Mountain stock, the latter
encountered only in drill core. The margins of both stocks are
irregular, with numerous small dikes and sills intruded along
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150
151
-500 m
Cu
Mo
-1000 m
Fault subparallel to
Porphyry Brook
Fault Zone
A'
Sea
Level
Hornfels
Marble
Biotite hornfels
Quartz monzonite
porphyry
Limit of intense
K-silicate alteration
FIG. 5. Cross section with no vertical exaggeration through the Porphyry Mountain skarn system showing the distribution
of garnet and pyroxene skarn. Location (AA) shown in Figure 4. Top of cross section (sea level) is about 900 m below the
surface of Porphyry Mountain. Arrows indicate direction of increasing Cu and Mo grades relative to K silicate-altered core
of the intrusion. Gar = garnet, Pyx = pyroxene.
clastic-rich units were altered to dark- green pyroxene hornfels. With increasing distance from the intrusion, skarn in
limestone becomes more pyroxene rich and the calc-silicate
hornfels in more clastic-rich units becomes lighter in color.
All skarn was overprinted by veinlets and vein envelopes of
hydrous minerals such as amphibole, chlorite, and epidote,
usually associated with sulfide minerals. Surrounding the two
main mineralized stocks is a composite aureole of bleaching
and recrystallization marked by a relatively sharp transition
from recrystallized white marble to fine-grained, dark-gray
limestone about 10 to 200 m beyond the limit of skarn (Fig.
4). The distal thermal aureole can be detected for several
kilometers beyond visible alteration by a very subtle change in
illite crystallinity (Williams-Jones, 1986).
Previous fluid inclusion and stable isotope investigations of
the Copper Mountain porphyry copper deposit at Mines
Gasp did not distinguish prograde and retrograde alteration
stages but did find evidence for a predominance of magmatic
fluid, except for a relatively late, postmineralization influx of
meteoric water. The proximal porphyry ore at Copper Mountain formed from a fluid largely of magmatic origin (DH2O =
42 to 61, based on extraction of inclusion fluids; Shelton,
1983). Fluid inclusion results for skarn (Shelton, 1983)
indicate high temperatures (TH = 334506C) and high
salinities (1556 wt % NaCl equiv), similar overall to the values reported from the prograde stage of the Big Gossan copper skarn.
Stable Isotope Results
Recent advances in stable isotope analytical methods allow
analysis of considerably smaller samples (a few mg for laser
fluorination lines) than is required for conventional analyses
(tens to hundreds of mg). This is particularly important for
studies of skarn systems due to the finely intergrown nature of most skarn minerals and the complex reactions that
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152
MEINERT ET AL.
TABLE 1. Stable Isotope and Temperature Data for the Big Gossan and Mines Gasp Skarn Deposits
Big Gossan
Sample no.
Mineral
1-6-600
1-6-600
1-6-600
8-1-213
8-1-213
Actinolite
Actinolite, duplicate
Actinolite, duplicate
Actinolite#
Actinolite #, duplicate
9-5-340
10-3-78
23-2-122
23-4-420
14-6-400
Pyroxene
Pyroxene
Pyroxene
Pyroxene
Pyroxene
26-4-250
14-6-491
23-2-165
9-5-465
8-5-187
Garnet
Garnet
Garnet
Garnet
Garnet
Measured
18O(VSMOW)
()
Calculated
18Ofluid
()
Measured
D(SMOW)
()
Calculated
Dfluid
()
Measured
H2O
(wt %)
Flinc
T
(C)
8.6
8.6
8.7
11.1
10.9
9.6
9.6
9.7
12.1
11.9
78
24
2.6
350
77
23
1.9
350
350
350
7.0
7.0
7.3
7.5
8.2
8.8
8.7
9.0
9.2
10.1
455
445
445
445
490
5.5
5.6
5.7
6.2
7.2
pyx-gar = 1.3
8.1
8.2
8.3
8.8
9.8
400
400
400
400
400
370 70
Gasp
Porphyry Mtn
923-4859
900-5660-1
900-5660-2
900-5660-2
793-2990
Hornblende
Hornblende
Actinolite
Actinolite
Actinolite*
Actinolite
5.0
4.3
5.2
5.2
4.9
5.0
7.4
5.3
6.2
6.2
5.9
6.0
87
78
115
143
70
24
61
89
2.5
1.8
1.6
1.6
130
76
1.8
700
350
350
350
350
350
923-5008
904-4011
904-4011
890-4085
Pyroxene
Pyroxene
Pyroxene, duplicate
Pyroxene
4.3
5.4
5.6
6.0
6.2
7.3
7.5
7.9
500
500
500
500
909-4245B
905-3210
904-3995
886-4351
920-5012
909-4245A
Garnet
Garnet
Garnet
Garnet
Garnet
Garnet
3.4
3.6
3.6
4.3
4.5
5.6
pyx-gar = 1.1
6.2
6.4
6.4
7.1
7.3
8.4
450
450
450
450
450
450
450 100
Mineral separates were purified by a combination of heavy liquids and magnetic methods followed by hand picking under a binocular microscope; purity
was checked optically and by X-ray diffraction; all oxygen and all deuterium, except for the Porphyry Mountain sample, were analyzed at the Geological
Survey of Japan using analytical methods described in Hedenquist et al. (1998); deuterium of the Porphyry Mountain sample was analyzed at Oregon State
University using methods described by Bigeleisen et al. (1952); temperatures for Big Gossan pyroxene and amphibole are based on pressure-corrected fluid
inclusion measurements (Meinert et al., 1997); temperatures of skarn minerals at Mines Gasp are based on limited fluid inclusion and phase equilibria
data from Allcock (1982) and Shelton (1983); calculated fluid compositions for amphibole are based on fractionation factors of Bottinga and Javoy (1975)
and Suzuoki and Epstein (1976), and for garnet and pyroxene, the fractionation factors of Zheng (1993); the water content of amphibole was determined
by manometric measurement of H2 after reduction of the structural H2O released during stepwise heating to >1,000C, reproducible to 0.1 wt % H2O;
this does notinclude absorbed water, which was removed by outgassing under vacuum pumping for 12 h at ~150C; Flinc = fluid inclusion, # = calcite
inclusions, * = HCl leached
152
10
15
20
25
Big Gossan
Garnet
Amphibole
Amphibole
with calcite
inclusions
Gasp
Garnet
Pyroxene
Amphibole
Marine Carbonate
Pyroxene
Igneous
amphibole
Magmatic
fluid
-5
10
15
20
25
153
153
154
MEINERT ET AL.
25
-25
Gaspe igneous
amphibole
-50
Degassing
Initial water
dissolved in melt
-75
-100
-125
Present-day
Ertsberg meteoric
water, snow, & ice
-150
-175
-25
-20
-15
-10
-5
10
15
200
400
TC
600
800
Na:K = 1:1
Vapor
+
Liquid
Liquid
2
Skarn
Retrograde
alteration with
qtz-anhydrite,
amphibole,
and sulfides
0.5
10
%
wt
60
7
80
0.2
1.0
60
wt%
Pressure (MPa)
40
1 1
0.
80
100
t%
40 w
20
NaCl in liquid
Depth (lithostatic)
Vapor + Salt
Depth (hydrostatic)
20
6-8 wt%
NaCl
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1997). The highest temperature and lithostatic pressure deduced for the formation of these deposits during their prograde stage is 535C and 50 MPa, respectively (Meinert et al.,
1997). This is consistent with the steep isotherms around a
near-solidus magma that is exsolving an aqueous fluid (Shinohara and Hedenquist, 1997). A magmatic fluid with bulk
salinity of 7 wt percent NaCl will intersect its solvus at a 2-km
depth and separate into a 50 wt percent hypersaline liquid in
equilibrium with a vapor containing ~1 wt percent NaCl (Fig.
8). Based on the fluid inclusion evidence for temperature and
salinity, most prograde skarn formed from this hypersaline
liquid.
Upon aqueous phase separation, most of the SO2 and HCl
from the parent fluid will partition into the vapor phase (Candela and Piccoli, 1995; Scaillet et al., 1998; Keppler, 1999),
which being less dense forms a vapor plume overlying the
reservoir of hypersaline liquid that is generated (Henley and
McNabb, 1978). This creation of a hypersaline liquid with
high base metal solubilities and relatively low sulfur content
may have inhibited sulfide deposition during formation of the
prograde skarn, similar to Bodnars (1995) argument for porphyry deposits. Condensation of much of the vapor plume at
shallow depths would have formed a highly acidic, low-salinity liquid which most likely would have caused advanced
argillic alteration (Hedenquist, 1995) and dissolution of the
host carbonate rocks with attendant brecciation, again analogous to formation of volcanic-hosted lithocaps over porphyry
deposits (Hedenquist et al., 1998). This can be thought of as
the ground-preparation stage of a growing skarn system in
which the vapor plume produces cavernous porosity in carbonate rock, to be overrun subsequently by the high- salinity,
skarn-forming fluid as the system expands. Thus, the many
breccias that occur at both Big Gossan and Mines Gasp, as
well as at other skarn deposits in the porphyry environment
(Einaudi, 1982), are part of the normal early-stage hydrothermal evolution of such systems.
As the underlying vapor-saturated magma chamber continued to cool and crystallize, fluid continually exsolved, and this
later fluid may have been relatively similar in bulk Na-K-Cl
composition to that of the earlier stage fluid (Cline, 1995; Shinohara and Hedenquist, 1997). However, because of the lack
of concurrent dike intrusion and/or a sharply lower fluid flux
as the parent magma approached the end stages of stagnant
crystallization (Shinohara and Hedenquist, 1997), the ascending fluid followed a cooling path different from that of the
early stage. The lower rate of advection (Shinohara and
Hedenquist, 1997) meant that this late fluid cooled sufficiently during ascent so that it never intersected its solvus
(Fig. 8).
Cooling to a temperature below approximately 400C results
in a transition from ductile to brittle rock behavior, causing a
change from lithostatic to hydrostatic conditions (Fournier,
1991). Thus, even though the later stage fluid reached the
previously formed skarn at the same paleodepth of 2 km, the
pressure was 20 MPa under the hydrostatic conditions. A 7 wt
percent NaCl liquid at 20 MPa will intersect the saturated
vapor-pressure curve at 370C, resulting in boiling of the ascending liquid. Continued boiling and vapor loss will result in
progressive cooling accompanied by only a slight increase in
salinity due to vapor loss, e.g., from 7 to 10 wt percent NaCl
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