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Re-Os-Isotope Systematics of Sulfides

from Base-Metal Porphyry and Manto-
Type Mineralization in Chile
a a a a
Joaquin Ruiz , Claire Freydier , Tom Mccandless , John Chesley
b
& Francisco Munizaga
a
Department of Geosciences , University of Arizona, Tucson,
Arizona, 85721
b
Departamento de Geologia , Universidad de Chile, Santiago, Chile
Version of record first published: 06 Jul 2010.

To cite this article: Joaquin Ruiz , Claire Freydier , Tom Mccandless , John Chesley & Francisco
Munizaga (1997): Re-Os-Isotope Systematics of Sulfides from Base-Metal Porphyry and Manto-Type
Mineralization in Chile, International Geology Review, 39:4, 317-324

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 international Geology Review, Vol. 39, 1997, p. 317-324.
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Re-Os-Isotope Systematics of Sulfides from Base-Metal Porphyry

and Manto-Type Mineralization in Chile1
JOAQUIN RUIZ, CLAIRE FREYDIER, TOM MCCANDLESS, JOHN CHESLEY,
Department of Geosciences, University of Arizona, Tucson, Arizona 85721

AND FRANCISCO MUNIZAGA

Departamento de Geologia, Universidad de Chile, Santiago, Chile

Abstract
Chile is a major world producer of copper, most of which occurs in base-metal porphyry and in
manto deposits. A fundamental difference between these two types of deposits is the relative
importance of intrusions spatially associated with the mineralization. The porphyry deposits are
set within Mesozoic to Tertiary intrusive complexes. The manto-type deposits are restricted to
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volcanic and volcano-sedimentary sequences of Middle-Late Jurassic, Early Cretaceous, Late

Cretaceous, and Early Tertiary times. Large intrusive centers are not spatially associated with
these deposits, although minor intrusions are common. A central question in the metallogenesis
of these deposits is the source of ore-forming components, in particular the ore metals. Initial
187
Os/ 188 Os isotopic data from sulfides from the El Teniente, La Disputada, and Andacollo base-
metal porphyry deposits range from 0.19 to 1. These data indicate that the Os (and, by inference,
Cu) is mostly crustally derived, since it is more radiogenic than that of the mantle, which has a
187
Os/ 186 Os ratio of —0.12. The isotopie data for El Soldado, which is an important example of
manto-type mineralization, are significantly more radiogenic, with 187 Os/ 188 Os ratios greater
than 3. These radiogenic values require that the Os come from a crustal reservoir with a high R e /
Os ratio, such as black shales. The Os-isotopic data indicate that the source for these two types of
base-metal deposits is different, but that both Os reservoirs reside in the crust.

Introduction measured in gangue minerals, because they are

A FUNDAMENTAL QUESTION in metallogenesis is
lithophile elements, requiring further assump­
the source of ore-forming components, in par­ tions about the relationship between ore and
ticular the ore metals. The relative importance associated minerals. In contrast, Re and Os are
of associated magmas, country rocks, and chalcophile and therefore are concentrated in
underlying basement have been discussed by sulfides (Drake and Jones, 1983; Fleet and
many (e.g., Norton, 1979; Ruiz et al., 1980; Stone, 1991). If one assumes that Os is a good
Kesler et al., 1983; Cumming et al., 1979) but proxy for the major ore-forming metals, Os
the overall constraints on the question are few. becomes a significant tracer for the source of
In addition to physical and chemical models the base-metal sulfides.
(e.g., Norton, 1977), previous studies have Chile is a major world producer of copper,
addressed source rocks and source paths with most of which occurs in base-metal porphyry
stable and radiogenic isotopes, specifically Sr, and in manto deposits. A fundamental dif­
Nd, and Pb isotopes. Of these isotopie systems, ference between these two types of deposits is
Pb is the only one that is an ore-forming ele­ the relative importance of intrusions spatially
ment in sulfide deposits. However, Pb-isotope associated with the mineralization. The por­
data in many cases do not yield uniquely con­
phyry deposits are set within Mesozoic to
strained results. Sr and Nd isotopes usually are
Tertiary intrusive complexes where large hydro-
thermal systems with prolonged interaction
between fluids in the intrusive magmas and
'This paper is one of a series of contributions (Marcos
Zentilli, compiler) to Project No. 342, Age and Isotopes of
country rocks concentrated metals at well
South American Ores, of the International Geological Cor­ above average crustal values. The Chilean
relation Program. manto-type deposits are restricted to volcanic

0020-6814/97/257/317-8 $10.00 317

 318 RUIZ ET AL.
FIG. 1. Location of deposits.
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and volcano-sedimentary sequences of Middle-
Late Jurassic, Early Cretaceous, Late Creta­
ceous, and Early Tertiary times. Large intrusive
centers are not spatially associated with these
deposits, although minor intrusions of dioritic
composition are common. Here we study the
Andacollo and El Teniente deposits as examples
of porphyry-related deposits and El Soldado as
an example of a manto (Fig. 1).
Information on the source of ore-forming
elements in these two types of ore deposits
would provide constraints on the processes that
form the ore. For example, ore-forming metals
may originate from associated magmas or from
country rocks. In the case of those deposits
whose metals come from associated magmas,
determining the proportion of mantle and
crustal components in the magma would estab­
lish which reservoir played the greatest role in
the ore formation. These constraints are of
academic as well as economic importance, since
identifying source rocks and source paths of the
metals can be useful in exploration. It should be
emphasized that there is a paucity of data that
constrain the source of metals in porphyry
deposits. This study attempts to address these
questions with respect to the Re-Os-isotope
system.
Re-Os Isotopes in Ore Deposits
The potential applicability of Re-Os isotopes
to geological problems has been recognized for
decades (Herr and Merz, 1955; Herr et al.,
1967; Schindler, 1975; Allègre and Luck, 1980;
Luck and Allègre, 1982), but only in the past
FIG. 2. Re-Os isochrons for different samples from the
Andacollo deposit (from Freydier et al., submitted).
few years has this potential begun to be realized.
Several features make the Re-Os-isotope sys­
tem uniquely suitable for metallogenetic stud­
ies. Re and Os are chalcophile (Hart and
Ravizza, 1993; Martin et al., 1993); therefore
the Re-Os system can be applied directly to
sulfide mineralization in base-metal porphyry
deposits, rather than to associated silicate
phases.
Re-Os-isotopic dating of molybdenite has
been shown to be very robust (McCandless et
al., 1993; McCandless and Ruiz, 1993; Yin et
al., 1993), but few studies have attempted to
analyze other sulfides from felsic igneous rocks
because of their low Os and Re concentrations
(Morgan et al., 1968; Schindler, 1975; Stein et
al., 1993). Recent work by Freydier et al. (sub­
mitted) shows that isochrons can be obtained
from common sulfides such as chalcopyrite,
bornite, and pyrite. That study yielded Re-Os
isochrons with ages for the Andacollo deposit
(Fig. 2) that are consistent with K-Ar ages for
magmatic and alteration minerals (Munizaga et
al., 1985), indicating that the Re-Os isotopic
system can be used to date common sulfides in
ore deposits associated with intermediate and
felsic rocks.
An important aspect of the Re-Os isotopic
system for tracer studies of magmas and ore-
forming solutions is that Os is compatible to
highly compatible relative to Re in partial melt­
ing of the mantle (Walker, 1988; Walker et al.,
1989). The high Re/Os ratios in the products of
mantle melting evolve to greatly elevated
187
Os/ 188 Os ratios over time, because of the
 RE-OS-ISOTOPE
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FIG. 3. Osmium-isotope evolution of the mantle (bold line) and possible evolution paths for Proterozoic and
Mesozoic oceanic lithosphere (diagonal lines). The upper boundary of each envelope is a path for oceanic crust with
187
Re/ 1 8 8 Os ratios of 500; the lower boundary is for
decay of 187Re to l87 Os (Fig. 3). Thus, Re-Os
isotopes are a potentially powerful tool for doc­
umenting interactions between the crust and
mantle. The results presented here demonstrate
the efficacy of Re-Os isotopes in metallogenic
studies.
Analytical Techniques
Approximately 1-g samples of bornite, chal-
copyrite, pyrite, and sphalerite were digested
overnight in a Carius tube at 240°C in a 1:2
solution of HCl:HNO 3 . The Carius tube solu­
tion was treated in a two-stage distillation pro­
cedure similar to that described by Shirey and
Walker (1995) but also modified for sulfides to
ensure complete oxidation of Os to a volatile
species when present in a sulfur-rich solution.
This is critical for achieving equilibrium of the
spike during the digestion process and for mobi­
lizing the Os during the distillation stages. The
oxidation was accomplished by using 30 ml of
15M HNO 3 and 11 ml of H 2 O 2 rather than
H 2 SO 4 -H 2 O 2 in the first distillation stage. The
second distillation stage was the same as that of
Shirey and Walker (1995), in which Os is
trapped either in HBr or in a 3:1 mixture of 10M
HCl:ethanol. The Os accumulated in the second
trap was heated at 70°C overnight in a sealed
Savillex beaker to ensure that the Os was in the
SYSTEMATICS 319
187
Re/ 188 Os ratios of 100.
reduced hexachloride or bromide form before
drying the sample. The residue was brought
back into solution in 0.1M HCl and loaded
on micro-columns for additional purification
(R. A. Creaser, pers. commun., 1995).
The Re remained in solution in the first flask
of the first distillation. The Re-rich solution
was dried-down and the cake redissolved in a
0.1M HNO 3 solution, which then was loaded on
a 1-ml anion column (AG-1 X8, 200-400 mesh).
The procedure was similar to that described by
Morgan et al. (1991) and Morgan and Walker
(1989), except that their first-stage Re-column
chemistry used H 2 SO 4 instead of HNO 3 . This
procedure was repeated using 0.1-ml anion
resin.
The samples were loaded on platinum fila­
ments and analyzed by negative thermal-ioniza-
tion mass spectrometry (NTIMS) on a VG 54
mass spectrometer (Chesley and Ruiz, 1997).
Total Re blanks ranged from 14 to 36 pg; total
Os blanks were 4 pg. The technique employed
here yielded total Re and Os contents from 50
pg to 1 ng to be analyzed by NTIMS, with errors
of 0.5 to 1% in most cases.
Geologic Setting
The basement where base-metal porphyry
and manto-type deposits occur in northern
Chile is a collage of sedimentary, igneous, and
 320 RUIZ ET AL.
nietamorphic rocks that were accreted along the
Chilean margin from the late Proterozoic to
Late Cretaceous (Davidson and Mpodozis,
1991; Sillitoe, 1991). A convergent setting has
existed since the Precambrian, but stresses in
the continental lithosphere have shifted from
compressive to extensional in character, the
latter case being attributed to a steeper angle of
subduction of the oceanic plate (Mariana-type
subduction) (Davidson and Mpodozis, 1991).
Magmatic arcs have migrated eastward since the
Upper Jurassic and are the settings in which the
major base-metal porphyry deposits formed.
Most of the deposits are associated with fast,
oblique plate-convergence velocities that are
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believed to have existed from the Paleocene to
the early Oligocene (Pardo Casas and Molnar,
1987; Davidson and Mpodozis, 1991). With
respect to country rocks, the Chilean deposits
are dominantly emplaced in igneous rocks of
Mesozoic and Paleozoic age, unrelated to the
porphyry magmatism. However, the deposits
sampled here are emplaced mostly in Creta­
ceous and Tertiary igneous rocks.
The porphyry deposits are set within intru­
sive complexes. The main copper mineral in
base-metal porphyry deposits is chalcopyrite,
which commonly is accompanied by lesser
bornite. Another important economic mineral
is m o l y b d e n i t e , and gold is a c o m m o n
byproduct. The evolution of these deposits is
complex and includes protracted hypogene and
subsequent supergene enrichment. Hypogene
mineralization is accompanied by K-silicate,
sericitic, or advanced argillic alteration. The
magmatism associated with the mineralization
is associated with subduction (Sawkins, 1990).
However, mineralization occurs at specific time
intervals (Sillitoe, 1988) within the more gen­
eral magmatism associated with subduction. In
Chile and Peru, large porphyry base-metal
deposits of the main Cordillera were formed
during the periods of 65 to 51 Ma, 41 to 31 Ma,
and 16 to 5 Ma (Ambrus, 1979; Sillitoe, 1981,
1988; Clark et al., 1983; Warnaars et al., 1985;
Cuadra, 1986; Zentilli et al., 1994). One impor­
tant deposit in the coastal region, Andacollo,
was formed at ~100 Ma.
The manto-type deposits are high grade
(~1.5% Cu) and occur in volcanic and volcano-
sedimentary sequences of Middle-Late Juras­
sic, Early Cretaceous, Late Cretaceous, and
Early Tertiary time (Munizaga et al., 1995;
Zentilli et al., 1997). Although large intrusive
centers are not spatially associated with these
deposits, minor dioritic intrusions are common.
Much of the sulfide mineralization in the
manto-type deposits is present as finely dis­
seminated grains and as open-space fillings in
vugs or stockwork veinlets. Hypogene mineral­
ization typically involves a chalcocite, born­
ite, and chalcopyrite, with ubiquitous specu­
lante. A typically Na-rich alteration assem­
blage consisting of albite-quartz-chlorite or
sericite and calcite accompanies manto-type
mineralization.
Results and Discussion
In this study we analyzed sulfides from El
Teniente, La Disputada, and Andacollo, exam­
ples of base-metal porphyry deposits, and from
the El Soldado deposit, which is an important
example of manto-type mineralization. The por­
phyry base metals selected are examples of the
youngest (El Teniente and La Disputada) and
oldest (Andacollo) base-metal porphyry miner­
alization in Chile. Analysis of sulfides from
these deposits permits the evaluation of secular
Os-isotopic ratios of porphyry mineralization
over time. The young age of the sulfides from El
Teniente and Disputada also requires minimal
Re corrections, reducing uncertainties in the
initial 187 Os/ 188 Os ratios that may arise because
of analytical errors. This makes it possible to
evaluate the Os-isotopic evolution of the miner­
alizing fluids, and to determine the distribution
coefficients of Re and Os between different
phases and h y d r o t h e r m a l fluids. The
TEN-11-95 samples (Table 1) represent a series
of chalcopyrite, sphalerite, bornite, and pyrite
separates of a single hand specimen. The
TEN-2-95 series are bornite and chalcopyrite
from a different hand sample, and TEN-4-95
and TEN-8-95 are from other hand samples.
The Re contents of these separates range from
0.05 to 0.18 ppb and the Os contents range from
0.04 to 1 ppb. The separates have a large range
in values (Table 1), suggesting that crystallo-
graphic constraints do not control the distribu­
tion of these elements since the sulfide
separates appear to be cogenetic. The pyrite
sample from Disputada has a higher concentra­
tion of Re than any sample from El Teniente,
but the Os concentration is similar to those of
El Teniente (Fig. 3).
 RE-OS-ISOTOPE SYSTEMATICS 321

TABLE 1. Re- and Os-Isotopic Composition of Sulfides from Chile

187
Sample name1 Total Os, ppb Total Re, ppb ( 87 Os/ 188 Os)m Re/ 188 Os ( 187 Os/ l88 Os)i

El Teniente
TEN11-95-cpy (27) 0.082 0.116 0.19383 7.80499 0.19318
ΤΕΝ11-95-cpy (17) 0.874 0.053 0.19624 0.31783 0.19621
TEN11-95-cpy (607) 0.153 0.085 0.18081 2.71784 0.18058
TEN11-95-sphal (606) 0.044 0.078 0.18752 9.46598 0.18674
TEN-2-95-bornite (19) 0.087 0.061 0.22286 3.76793 0.22255
TEN2-95-bornite (604) 0.042 0.180 0.17286 21.79200 0.17104
TEN8-95-cpy (605) 1.051 0.062 0.34794 0.30200 0.34792
TENll-95-pyrite(610) 0.176 0.094 0.88458 2.93663 0.88433

Andacollo
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Andacollol-pyrite (26) 0.016 6.190 6.87525 3578.21652 0.90897

Andacollol -pyrite (606) 0.915 5.617 1.17208 37.06557 1.11027
Andacollo2-pyrite (608) 1.732 4.921 0.19110 15.16400 0.16582
Andacollo3-pyrite (608) 1.982 99.990 0.70457 290.29114 0.22054
Andacollo3-pyrite (610) 0.224 56.319 3.06995 1923.29100 -0.13693

El Soldado-cpy (605) 65.355 15.409 3.95264 1.72300 3.94977

Disputada1-pyrite (731) 6.110 0.249 0. 17668 0.20300 0.17666

1
Numbers in parentheses indicate numbers of samples collected.

Samples from Andacollo are more enriched
in Re than those of El Teniente (5 to 100 ppb),
but are unremarkable in Os (0.016 to 2 ppb). As
at El Teniente, the sulfides exhibit variable Re
and Os concentrations, and pyrite separates
have a very large range of 187 Re/ 188 Os ratios.
The heterogeneities in Re and Os contents may
be explained by a "nugget effect," because Re
and Os might be concentrated in micro-phases
that are not equally distributed, or by a fluid
with rapidly evolving Re and Os concentrations.
This can be turned to an advantage during the
use of sulfides for Re-Os geochronology
because large variations in Re/Os ratios are
obtained from separates from the same mineral
phase, as shown in Figure 3.
The l87 Os/ 188 Os ratios of the sulfides from
porphyry base-metal deposits range from 0.18
to 0.88. In all cases, the elevated 187 Os/ 188 Os
ratios of the samples indicate a crustal compo­
nent of Os, since the mantle has a 187 Os/ 188 Os
ratio of approximately 0.13 (Fig. 2), which is
one to two orders of magnitude greater than the
crust (Ivanov et al., 1972; Luck and Allègre,
1991). The variations in the Os-isotopic ratios
of the sulfides indicate that the hydrothermal
fluids that precipitated the ore acquired the Os
from different reservoirs.
The initial 187 Os/ 188 Os ratio of pyrite from El
Soldado, which is the example of manto-type
deposits studied here, is much more radiogenic
than that of the base-metal porphyry deposits
(Fig. 4). The initial Os-isotopic ratio of 3.9
shows that the Os (and by inference the other
ore-forming metals for this deposit) has a
crustal component greater than that of the
porphyry deposits. This is not entirely surpris­
ing, since the deposit is not as intimately associ­
ated with large magmatic systems as is the case
with base-metal porphyry deposits.
There has been considerable debate on the
origin of manto-type deposits (Carter, 1960;
Ruiz and Ericksen, 1962; Losert, 1974; Lortie
and Clark, 1974; Camus, 1980; Espinoza and
Palacios, 1982; Sato, 1984; Holmgren, 1985;
Sillitoe, 1988; Munizaga et al., 1995). The pres­
ence of some calc-silicates has been used to
argue that mantos are distal skarns. The pres­
ence of oil droplets has been the basis for the
contention that the fluids are associated with
organics (Zentilli et al., 1994, 1997), and the
ubiquitous presence of sodic alteration has
been used to argue for fluids modified by inter­
actions with evaporites. Although Os reservoirs
in the crust are imperfectly understood, black
shale is one crustal reservoir with high Re/Os
ratios that can account for the high 187 Os/ 188 Os
ratios of the El Soldado sulfides. This inter-
 322
FIG. 4. 1 8 7 Os/ 1 8 8 Os ratios of Chilean ore deposits and
probable mantle and crustal reservoirs.
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pretation is further supported by the observa­
tions by Zentilli et al. (1994, 1997), who have
demonstrated the existence of oil-rich inclu­
sions within the ore.
Conclusions
The Re-Os-isotopic data clearly show that Os
(and by inference base metals) in Chilean por­
phyry base-metal and manto-type deposits is
too radiogenic to be derived solely from mantle
sources. The very low abundances of Re and Os
in the crust compared to those in the mantle
further suggest that the source of the ore-
forming metals is largely crustal. The average
187
Os/ 188 Os of the sulfides from porphyry base-
metal deposits is ~ 0 . 2 , whereas that of El Sol-
dado, which is an example of a Chilean-type
manto, is much more radiogenic at ~3. This
indicates that the crustal sources for the por­
phyry base-metal and manto-type deposits are
different. The large difference in the isotopic
ratios of these deposits also may prove a useful
indicator in exploration programs.
Acknowledgments
This work was possible because of funds
provided by BHP, Cambior, CODELCO-Chile,
Phelps Dodge, The W.M. Keck Foundation, and
the National Science Foundation through
grants EAR 9406259 and EAR 9628150 and
Chile's FONDECYT 194-041. We are especially
grateful to Drs. Bruce Bouley, Hugo Dummett,
Michael Gustin, Greg McKelvey, and Alvaro
Puig for their support. This paper is a contribu­
RUIZ ET AL.
tion to IGCP Project No. 342, on the Age and
Isotopes of South American Ores.
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