Origin of marine barite deposits: Sr and S isotope characterization

Adina Paytan
Sarah Mearon
Department of Geological and Environmental Sciences, Stanford University, Stanford, California 94305-2115, USA
Kim Cobb
Miriam Kastner
Scripps Institution of Oceanography, La Jolla, California 92093-0212, USA

ABSTRACT
Barite can precipitate in microenvironments in the water column (marine barite),
from supersaturated pore fluids at the oxic-anoxic boundary within marine sediments and
where Ba-rich pore fluids are expelled and come into contact with sulfate-rich seawater
(diagenetic barite), or from hydrothermal solutions (hydrothermal barite). Barite is rela-
tively resistant to alteration after burial and has been used in paleoceanographic studies
to reconstruct seawater chemistry and productivity through time. For such applications
it is very important to determine the origin of the barite used, because both diagenetic
and hydrothermal barite deposits may not accurately record the open-ocean contempo-
raneous seawater chemistry and productivity. We show here that it is possible to distin-
guish between the different types of barite by using Sr and S isotopes along with crystal
morphology and size characteristics.

Keywords: barite, sulfur isotopes, strontium isotopes, paleoceanography.

INTRODUCTION for paleoceanographic studies (Church, 1979). A combination of S and

Barite in marine sediments is frequently used as a paleoproduc- Sr isotope analyses and crystal-morphology characterization is sug-
tivity proxy (Schmitz, 1987; Dymond et al., 1992; Gingele and Dahm- gested here to provide an indicator of the depositional environment of
ke, 1994; Paytan et al., 1996a; Dean et al., 1997) as well as to recon- a given barite. Sr and/or S isotope analyses have been previously ap-
struct the seawater Sr isotope curve (Paytan et al., 1993; Martin et al., plied to describe mechanisms and conditions of barite formation; how-
1995), to determine the S isotope ratio of marine sulfate (Cecile et al., ever, all previous studies were restricted to a single deposit or location
1983; Goodfellow and Jonasson, 1984; Strauss, 1997; Paytan et al., (Dean and Schreiber, 1977; Hannington and Scott, 1988; Kusakabe et
1998), and to characterize Holocene sedimentation rates by using ex- al., 1990; Torres et al., 1996b; Aquilina et al., 1997; Fu and Aharon,
cess 226Ra decay (Paytan et al., 1996b; van Beek and Reyss, 2001; van 1997; Aharon and Fu, 2000; Naehr et al., 2000; Breheret and Brum-
Beek et al., 2002). In all these applications it is assumed that the barite sack, 2000). Here we compare the isotope systematics and mineral-
crystals analyzed precipitated directly from seawater and thus recorded habit characteristics of a wide range of barite deposits and establish
contemporaneous seawater productivity and chemistry. Barite micro- criteria to distinguish between different modes of barite formation.
crystals have been observed in the water column (Dehairs et al., 1980;
Bishop, 1988), and there are indications that barite precipitates inor- ANALYTICAL METHODS
ganically directly from seawater in microenvironments containing Barite was separated from other minerals in the samples by a
decaying organic matter and other biogenic remains (Bishop, 1988; sequential leaching procedure (Paytan et al., 1993). All samples were
Dehairs et al., 1990; Ganeshram and Francois, 2002). This authigenic examined for purity by X-ray diffraction (XRD) and scanning electron
microscopy (SEM) with energy-dispersive spectrometry (EDS), and
marine barite (as defined here) precipitates as small crystals or aggre-
only samples that contained .95% barite were used. S isotope analyses
gates, ranging in size from 0.5 to 5 mm (Bishop, 1988; Dehairs et al.,
were done by continuous-flow mass spectrometry using a Carlo Erba
1980; Paytan et al., 1993).
NA 1500 elemental analyzer connected to a Micromass Isoprime mass
Barite may also precipitate in association with submarine hydro-
spectrometer. Samples of 4–8 mg were introduced in tin boats with
thermal activity (hydrothermal barite) (Zierenberg et al., 1984; Lons-
;5 mg vanadium pentoxide mixed in with each sample. A commercial
dale and Becker, 1985; Feely et al., 1987, 1990; Hannington and Scott,
tank of SO2 was used as a reference gas for d34S measurements, and
1988; Peter and Scott, 1988; Kusakabe et al., 1990; Moore and Stakes,
results are reported relative to the Canyon Diablo troilite standard, with
1990) as well as diagenetically at the oxic-anoxic boundary within
a standard deviation (2s) of 60.3‰. Barite samples were dissolved
sediments in association with sulfate-reducing conditions (Bolze et al.,
for Sr isotope analysis by using a resin chelation method (Paytan et
1973; Dean and Schreiber, 1977; Brumsack and Gieskes, 1983; Cecile al., 1993), and the Sr fraction was separated by standard ion-exchange
et al., 1983; Breheret and Brumsack, 2000) or when Ba-rich fluids from chromatography. Values of 87Sr/86Sr were determined on a VG-261
seeps or along fractures are expelled into seawater (diagenetic barite) mass spectrometer. The external precision of the analyses is 60.000 02.
(Lonsdale, 1979; Dia et al., 1993; Torres et al., 1996a; Aquilina et al., All values were normalized to an 86Sr/88Sr ratio of 0.1194. During the
1997; Naehr et al., 2000). These nonbiogenic barite deposits do not period of analysis, the mean 86Sr/87Sr ratio of the standard NBS 987
necessarily reflect the contemporaneous seawater conditions (chemistry was 0.710 24.
or productivity) and are therefore unsuitable for paleoceanographic
studies. RESULTS AND DISCUSSION
Criteria to distinguish between barite crystals that form via those The S and Sr isotope ratios of barite samples collected from dif-
distinct pathways are therefore required in order to utilize this phase ferent oceanic environments are given in Table 1 and Figure 1. Barite

q 2002 Geological Society of America. For permission to copy, contact Copyright Permissions, GSA, or [email protected].
Geology; August 2002; v. 30; no. 8; p. 747–750; 2 figures; 1 table. 747
 TABLE 1. Sr AND S ISOTOPE COMPOSITIONS OF MARINE BARITE
SAMPLES

Sample name 87
Sr/86Sr d34S Site and
(‰) sample
description*
Core tops# 0.709 175 21.1 1
Sediment traps** 0.709 170 20.9 2

JDFR##, sediment trap ER 270383 0.709 178 20.8 3

JDFR##, sediment trap ER 270388 0.706 077 21.1 3
JDFR##, Clam Bed Site, 2463-R7 0.704 460 20.7 4
JDFR***, East Wall ALV 1924-6-20 0.705 210 18.2 5
JDFR***, Casm Site ALV 2084-2A-1 0.706 251 19.5 5
JDFR***, ALV 1924-6-20 0.704 415 20.5 5
JDFR***, ALV 2945-4S2,245C 0.705 243 19.2 5
JDFR###, ALV 2254-21 0.705 162 20.9 5
JDFR###, ALV 2254-23-1 0.707 141 19.7 5
JDFR****, ALV 1461-5 0.704 512 21.0 6
JDFR****, ALV 1459-8 0.705 347 20.8 6
JDFR, Southern Site, ALV 1457 0.705 518 20.9 7
Mid-Atlantic Ridge####, ALV 2602-3 0.705 310 21.2 8
Mid-Atlantic Ridge####, ALV 2606-3 0.705 971 20.9 8
Mid-Atlantic Ridge####, ALV 2604-5 0.704 432 21.0 8
Mariana backarc 1830-R-1 0.704 172 21.2 9 Figure 1. Plot of Sr and S isotope values for barite samples sepa-
Mariana backarc 1831-R1-C 0.705 460 21.0 9 rated from different depositional environments. Green diamonds
Mariana backarc 1831-R2 0.703 991 21.1 9 (plotted as one point)—isotope values for all core-top and sediment-
Mariana backarc 1832-R2-C 0.704 762 20.9 9 trap samples (excluding Juan de Fuca Ridge [JDFR] trap) (i.e., ma-
East Pacific Rise 218N, 914-R1-A 0.704 275 20.8 10 rine barite). Blue circles—diagenetic barite samples. Red circles—
hydrothermal barite samples. Black dot within diamond—barite in
ODP Site 765C 34-1, 57–60 cm 0.710 892 24.2 11
<8 mm fraction of Juan de Fuca Ridge trap. Dotted lines pass
ODP Site 765C 34-2, 118–121 cm 0.710 817 23.7 11
Peru Margin SO 78/177 0.709 939 50.6 12 through present-day seawater Sr and S isotope ratios. CDT—Can-
Peru Margin NP 2/34 0.711 031 32.7 12 yon Diablo troilite (S isotope standard).
Peru Margin SO 78/180 0.710 621 45.2 12
Baja California, Ensenada, BC-1 0.708 801 28.9 13
Baja California, Ensenada, BC-2 0.708 701 29.0 13
Baja California, Ensenada, BC-3 0.708 810 29.6 13 curves (Burke et al., 1982; Paytan et al., 1998), and deviation from the
San Clemente Basin, 355 A 0.708 487 22.1 14 expected contemporaneous seawater values suggests nonseawater-
San Clemente Basin, 355 B 0.708 269 23.8 14
San Clemente Basin, 355 C 0.708 372 24.6 14
column origin (not marine barite).
Guaymas Basin 1170-16 0.706 037 24.2 15 The second category (blue circles in Fig. 1) includes barite sam-
Guaymas Basin 1172-6 0.706 251 25.7 15 ples with S isotope ratios higher than contemporaneous seawater val-
Guaymas Basin 1173-1 0.706 165 26.4 15
Guaymas Basin 1173-11 0.705 649 23.2 15 ues. For example, a recent massive barite deposit dredged in Baja Cal-
Monterey Canyon, tubeworm slump 0.708 182 26.7 N.D. ifornia (Lonsdale, 1979; Table 1) has a d34S isotope value of 29.0‰
Monterey Canyon 36.68N, 122.48W 0.708 163 31.3 16 and an Sr isotope ratio of 0.708 701, clearly different from those ex-
Monterey Canyon 36.68N, 122.48W 0.708 215 27.1 16
Gulf of Mexico (barite crusts) 0.708 587 28.5 17 pected for present-day seawater. These samples have precipitated from
Gulf of Mexico (barite crusts) 0.708 421 59.5 17 fluids that had some degree of sulfate loss due to bacterial sulfate
*References for site and sample description: 1, Paytan et al. (1993, 1998); 2, reduction (diagenetic barite). Sulfate reduction leads to enrichment of
Dymond and Collier (1988); 3, Dymond and Roth (1988); 4, Moore and Stakes the heavy S isotope (34S) in the residual sulfate in these fluids (Harrison
(1990); 5, Reyes et al. (1995); 6, Shanks and Seyfried (1987); 7, Feely et al. (1987);
8, Tivey et al. (1995); 9, Kastner et al. (1987); 10, Zierenberg et al. (1984); 11, and Thode, 1958). Barite precipitation may occur within the sedimen-
Gradstein et al. (1990); 12, Torres et al. (1996a) and Dia et al. (1993); 13, Legg tary column when Ba-rich fluids (from barite dissolution by the sulfate-
(1980); 14, Lonsdale (1979); 15, Lonsdale and Becker (1985); 16, Naehr et al. reduction process or from continental sources) migrate by diffusion or
(2000); 17, Fu and Aharon (1997).
#
Average value of 30 core-top samples. advection toward sulfate-rich sections in the sediment, typically at
**Average for 9 sediment-trap samples from the Pacific Ocean. oxic-anoxic fronts (Dean and Schreiber, 1977; Kastner et al., 1990;
##
Juan de Fuca Ridge (JDFR) Endeavour Segment.
***JDFR Axial Seamount.
Elderfield et al., 1990). Alternatively, barite could form at the sediment-
###
JDFR Middle Valley. water interface where these Ba-rich fluids are discharged through seeps
****JDFR South Explorer Ridge. or faults into sulfate-rich seawater, and barite saturation is exceeded
####
Lucky Strike.
(Torres et al., 1996a, 1996b; Naehr et al., 2000).
The Sr isotope ratio of these diagenetic barites depends on the Sr
isotope ratio of the water at the site of precipitation. The Sr could have
samples cluster into three groups depending on their origin. The first less 87Sr than the Sr that is typical of contemporaneous seawater if the
very tight cluster (represented by one green diamond in Fig. 1) includes pore fluids have been modified by Sr from less radiogenic sources like
barite samples separated from core-top sediments in the Pacific, Atlan- older marine sediments or the oceanic crust (as in San Clemente Basin
tic, and Indian Oceans (30 samples) and barite crystals separated from and Monterey Canyon); the Sr could have more 87Sr relative to con-
sediment-trap samples (9 samples). These barite samples have precip- temporaneous seawater if the pore-fluid Sr was derived from alteration
itated from seawater (marine barite) and record present-day Sr of radiogenic terrigenous material in the sediment or meteoric water
(0.709 17) and S (21.1‰) isotope ratios (as determined in our (Torres et al., 1996a; Kastner et al., 1990; Elderfield et al., 1990) (as
laboratory). in Peru Margin and Ocean Drilling Program Site 765C samples).
Because the seawater Sr and S isotope ratios have not remained A third group is composed of barite samples (red circles in Fig.
constant over time, the combination of Sr and S isotope ratios repre- 1) characterized by Sr isotope ratios that are between the modern sea-
senting contemporaneous seawater values is different for barite sepa- water value and the Sr isotope ratio of pure (mantle derived) hydro-
rated from sediments of different ages. Accordingly, the isotope ratios thermal fluids (estimated to be 0.703 50; Albarède et al., 1981). These
for any given barite sample of known age (independently derived) hydrothermal barite samples precipitate from fluids influenced by hy-
should be compared to the well-known seawater Sr and S isotope drothermal processes. Nonradiogenic Sr as well as Ba are leached from

748 GEOLOGY, August 2002

 most likely from hydrothermal solutions. However, in this sediment-
covered ridge system, the fluids are expelled into marine-sediment sec-
tions where sulfate reduction takes place, depleting the pore-water sul-
fate from the light S isotope and resulting in barite with S isotope
ratios slightly greater than seawater (Elsgaard et al., 1994).
In addition to the characteristic isotopic signatures of barite de-
posited in the different marine settings already described, the size and
morphology of barite crystals formed by those different precipitation
modes are distinct. Figure 2 shows SEM micrographs of typical barite
crystals separated from the different depositional environments. Marine
barite crystals precipitated in the water column and extracted from
sediment-trap samples (including the ,8 mm barite fraction from the
Juan de Fuca Ridge black smoker) or from marine sediments that have
not undergone extensive sulfate reduction are smaller than 5 mm and
are typically ellipsoidal in shape (Fig. 2, A–C). Hydrothermal barite
crystals are larger, 20–70 mm, and are typically precipitated as cross-
cutting tabular crystals commonly forming rosettes (Fig. 2, D–F). The
.8 mm barite crystals from the sediment trap above the Juan de Fuca
Ridge, as expected, have morphological features typical of hydrother-
mal precipitates. Diagenetic barite crystals are also large (20–700 mm),
flat, tabular-shaped crystals and appear as barite beds in the sedimen-
tary column. Diagenetic barite crystals that precipitate at the sediment-
water interface form mounds of highly porous barite with the layered
appearance of platy crystals that form diamond-shaped clusters (Fig.
2, G–H).

CONCLUSIONS
On the basis of crystal size and morphology and the Sr and S
isotope ratios of barite deposits, it is possible to distinguish between
the depositional environments and thus the origin of this mineral if the
age of the barite sample is independently determined. Careful exami-
nation of barite samples used for paleoceanographic studies would
eliminate any questions with respect to the authenticity of marine barite
origin and its fidelity in recording the seawater characteristics (pro-
ductivity and/or chemistry).
Figure 2. Scanning electron microscope images of barite crystals ACKNOWLEDGMENTS
from different oceanic settings. A: Marine barite, core-top sedi- We thank Peter Lonsdale, Debra Stakes, Billy Moore, Martha Torres, Mar-
ments, Pleiades expedition, core 77, 1.038N, 119.558W. B: Marine bar- garet Tivey, Richard Zierenberg, Thomas Naehr, Harmon Craig, Jack Dymond,
ite, Deep Sea Drilling Project Site 574C, 29.1 Ma. C: Marine barite, and Bob Collier for generously sharing their barite samples or sediment-trap
sediment trap, <8 mm fraction from Juan de Fuca Ridge black smok- material with us. We thank the Repositories of the Scripps Institution of Ocean-
er. D: Hydrothermal barite, Mariana backarc chimney 1831-R1-C. E: ography and Oregon State University (OCE-9102881) for providing core-top
Hydrothermal barite, Mid-Atlantic Ridge, chimney at Lucky Strike, samples for barite separation. Older marine barite samples were separated from
ALV 2602-3. F: Hydrothermal barite, sediment trap, >8 mm fraction Ocean Drilling Program and Deep Sea Drilling Project cores. Comments by P.
from Juan de Fuca Ridge black smoker. G: Diagenetic barite, Ocean van Beek greatly improved the manuscript. This work was supported by Na-
Drilling Program Leg 132, Site 765C 34-1, 47–60 cm, ca. 112 Ma. H: tional Science Foundation grants OCE-91-16010 and EAR-96-28479.
Diagenetic barite, San Clemente Basin, sea cliff 355A.
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