https://doi.org/10.1130/G48348.

Manuscript received 20 May 2020

Revised manuscript received 1 September 2020
Manuscript accepted 16 October 2020

© 2020 Geological Society of America. For permission to copy, contact [email protected].

Fluid compositions reveal fluid nature, metal deposition

mechanisms, and mineralization potential: An example at the
Haobugao Zn-Pb skarn, China
Qihai Shu1,2*, Zhaoshan Chang2,3 and John Mavrogenes4
1
State Key Laboratory of Geological Processes and Mineral Resources, School of Earth Sciences and Resources, China University
of Geosciences, Beijing 100083, China
2
Economic Geology Research Centre, James Cook University, Townsville, Queensland 4811, Australia
3
Department of Geology and Geological Engineering, Colorado School of Mines, Golden, Colorado 80005, USA
4
Research School of Earth Sciences, Australian National University, Canberra, Australian Capital Territory 2601, Australia

ABSTRACT other skarns that contribute to the world’s supply

Fluid inclusion compositions obtained from laser ablation–inductively coupled plasma– of W, Sn, Zn-Pb, Mo, Cu, Au, and Fe (Meinert
mass spectrometry at the Haobugao Zn-Pb skarn in northeastern China provide constraints et al., 2005; Chang et al., 2019).
on fluid origin, evolution, and metal deposition mechanisms and an example of evaluating
mineralization potential. Metal concentrations in the prograde fluids were high (up to 1.4 wt% DEPOSIT GEOLOGY
Zn and 1.8 wt% Pb) but remained in solution, likely due to the high temperatures (440–575 °C) The Haobugao skarn deposit (44°37’N,
and salinities (35.4–45.3 wt% NaCl equivalent). Absolute concentrations of elements (e.g., Rb 119°16’E) in Inner Mongolia, northeastern
and Na) and mass ratios (e.g., Zn/Na and K/Na) reveal that the early, prograde fluids were China (Fig. 1A) contains 0.29 Mt Zn averag-
magmatic, consistent with the oxygen isotope composition of fluids (δ18OH2O = 5.5‰–8.5‰). ing 4.24% Zn, 0.15 Mt Pb (2.25% Pb), and
Later mixing with a meteoric fluid caused dilution and Zn-Pb deposition, as revealed by 2.91 Mt Fe (28.7% Fe), with subordinate Cu
lowered element concentrations and Pb/(Na + K) and Zn/(Na + K) ratios in the sulfide-stage and Ag and minor newly discovered Mo and
fluid inclusions. Elevated Ca/K ratios in sphalerite-hosted inclusions indicate fluid-carbonate Sn (Sun et al., 2018). The Haobugao deposit is
reactions that buffered fluid pH, also facilitating Zn-Pb precipitation. Although cassiterite and related to an Early Cretaceous biotite granite
molybdenite occur locally at Haobugao, mass balance calculation shows low metal endowment porphyry stock that emplaced into intercalated
(maximum 2900 t Sn and 2200 t Mo) of the system. Furthermore, the generally unchanged siltstone and/or shale and limestone of the Perm-
Sn/(Na + K) and Mo/(Na + K) ratios from pre- to late-mineralization fluids suggest that the ian Dashizhai Formation (Fig. 1B). The skarn is
fluids were never saturated in Sn and Mo. Therefore, finding much Sn or Mo at Haobugao is an ∼800-m-long, ∼900-m-deep, steeply dipping
unlikely. This demonstrates a potential tool for evaluating the metal endowment of a mineral tabular body. It fully replaced the limestone bed
prospect, which may guide exploration. near the intrusion and partially replaced it at dis-
tal locations along the limestone-siltstone and/or
INTRODUCTION the usage of fluid compositions determined by shale boundary (Fig. 1B; Fig. S1 in the Supple-
Compositions of single fluid inclusions (FIs) LA-ICP-MS to examine the full fluid evolution mental Material1). The paragenesis includes a
measured by proton-induced X-ray emission of the Haobugao Zn-Pb skarn system in north- pre-mineralization prograde garnet-pyroxene
(Ryan et al., 1991) and laser ablation–induc- eastern China from the early pre-mineralization stage, followed by an Fe (magnetite) mineral-
tively coupled plasma–mass spectrometry (LA- prograde stage through the sulfide stage to the ization stage accompanied by retrograde amphi-
ICP-MS; Audétat et al., 1998; Heinrich et al., final post-ore stage. The examination reveals the bole-epidote-ilvaite-quartz alteration, a sulfide
1999) have been used to investigate magmatic proportion of different fluids (e.g., magmatic, (sphalerite-galena-pyrite and minor chalcopy-
hydrothermal fluid compositions (e.g., Audé- meteoric, and formation) in the hydrothermal rite) mineralization stage with further retrograde
tat, 2019), to infer fluid types (e.g., Samson system over time, the metal deposition mecha- chlorite-quartz-calcite alteration, and a post-ore
et al., 2008) or pulses (e.g., Baker et al., 2004; nisms, and the resource potential of some less- stage of barren calcite veins (Figs. 1C–1E; Figs.
Kouzmanov et al., 2010), to define hydrother- abundant metals. The Haobugao deposit evolved S2 and S3). Minor molybdenite and cassiterite
mal processes (e.g., Audétat et al., 1998; Hein- from an early high-temperature (∼575 °C) pro- were deposited in the late Fe stage and early
rich, 2005), and for thermodynamic modeling grade stage through to a retrograde low-temper- sulfide stage. The prograde stage is zoned, with
(e.g., Bertelli et al., 2009). This study expands ature post-ore overprinting mineral assemblage a garnet-dominant zone near the intrusion, an
(∼150 °C), making it suitable for such a study. intermediate pyroxene-rich zone, and a distal
*E-mail: [email protected] The approach presented here may also apply to wollastonite ± siderite zone at the marble front
1
Supplemental Material. Methods, results, Figures S1–S6, and Tables S1–S6. Please visit https://doi.org/10.1130/GEOL.S.13262843 to access the supplemental
material, and contact [email protected] with any questions.

CITATION: Shu, Q., Chang, Z., and Mavrogenes, J., 2021, Fluid compositions reveal fluid nature, metal deposition mechanisms, and mineralization potential:
An example at the Haobugao Zn-Pb skarn, China: Geology, v. 49, p. XXX–XXX, https://doi.org/10.1130/G48348.1

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 A C D E Figure 1. (A) Location
of the Haobugao skarn
deposit, northeastern
China. (B) Schematic
cross section of Haobugao
(details are provided in
Figure S1 [see footnote 1]).
grt—garnet; pyx—pyrox-
B ene; wo—wollastonite;
sd—siderite. Geologic
F G H unit ages: 1—lower Perm-
ian Dashizhai Formation;
2—142.9 ± 1.6 Ma (zircon
U-Pb; Liu et al., 2018);
3—140.3 ± 3.4 Ma (molyb-
denite Re-Os; Wan et al.,
2014), 139.6 ± 0.9 Ma (cas-
siterite U-Pb, Liu et al.,
2018). (C,D) Garnet-pyrox-
ene skarn postdated by
I J K later calcite (cal)–sphaler-
ite (sp)–galena (gn) veins
or interstitial filling. (E)
Massive ore composed
of sphalerite and calcite.
(F) Primary brine (type
B) fluid inclusion assem-
blages (FIAs) in pyroxene.
(G) Primary vapor (type
V) FIAs in pyroxene. (H,I)
Primary type L FIAs in sphalerite. (J) Primary type L FIA in sulfide-stage calcite. (K) Secondary (type SL) FIAs along trails (dashed lines) in
sulfide-stage calcite.

(Fig. 1B; Fig. S1). The Fe mineralization is rela- similar phase ratios and microthermometric calcite-hosted FIAs being 12–1266 ppm and
tively proximal and the Zn-Pb ores distal; chal- measurements are also treated as a FIA in this 27–1558 ppm, respectively. Zinc in calcite-
copyrite, where present, occurs mainly between study (Figs. 1F–1H and 1J). hosted FIAs is 57–1220 ppm. Molybdenum and
the Fe and Zn-Pb orebodies. Such zoning pat- Sn in type L FIAs are 1–13 ppm and 2–22 ppm,
terns are similar to those of many other Zn-Pb RESULTS respectively.
skarns worldwide (e.g., Meinert, 1987; Meinert Sample information, analytical details, and Type SL (secondary) FIAs in calcite (n = 5)
et al., 2005; Chang et al., 2019). the microthermometric and fluid composition have lower Th (152–204 °C) and salinities (1.2–
We analyzed FIs in prograde pyroxene and data are available in the Supplemental Material. 4.2 wt% NaCl equivalent). They are depleted in
later sulfide-stage sphalerite and calcite (Figs. 1 Brine (type B) inclusions in pyroxene homog- most elements (e.g., <31 ppm Zn and <22 ppm
F–1 K; Table S1 in the Supplemental Material). enize to liquid after halite disappearance, with Pb), with Mo and Sn below detection limits.
FIs in other minerals were not used due to their homogenization temperatures (Th) of 421–575 For the boiling assemblages with both brine
scarcity and small size (commonly <5 μm). FIs °C for the 19 FIAs, and salinities of 35.4– and vapor inclusions (types B and V) in pyrox-
in pyroxene are of two types: brine (type B) 45.3 wt% NaCl equivalent. LA-ICP-MS analy- ene, calculated trapping pressures (Steele-
that contains vapor, liquid, and a halite ± syl- ses show that they contain 0.5–1.4 wt% Zn and MacInnis et al., 2012) are 500–525 bar (average
vite ± tiny opaque daughter crystal (Fig. 1F); 0.5–1.8 wt% Pb. Concentrations of Mo and Sn 513 bar). The high-temperature prograde stage
and rare vapor inclusions (type V) containing are significantly lower; 21–84 and 27–122 ppm, was likely under near-lithostatic conditions
>80 vol% vapor bubbles (Fig. 1G). Locally, respectively (Tables S2–S4; Fig. S4). Three (Fournier, 1999), therefore the formation depth
types B and V FIs occur in one assemblage (Fig. vapor (type V) FIAs in pyroxene yielded Th of is estimated at ∼1.9 km. This depth is similar to
S2H), indicating boiling. In the sulfide stage, FIs 448–491 °C and salinities of 3.9–7.1 wt% NaCl the ∼2.0 km emplacement depth of the causative
in sphalerite and calcite typically contain liquid equivalent. Vapor inclusions contain lower con- intrusion, calculated using a hornblende geoba-
and vapor phases (type L), and the bubbles are centrations of most analyzed elements than brine rometer (Ridolfi et al., 2010; Table S5). For the
<50 vol% of each FI (Figs. 1H–1J). Secondary inclusions, but similar elemental mass ratios to brine FIAs without coexistent vapor inclusions,
FIs (type SL) in calcite (Fig. 1K) are interpreted Na + K, except for As and Li, whose ratios to the pressure (513 bar)–corrected trapping tem-
to postdate sulfide precipitation. No detectable Na + K are significantly higher (Fig. 2A). This peratures are typically 1–19 °C higher than the
CO2 or other non-aqueous gases were identified could be due to the volatility of As and Li, which measured Th (Table S2).
in any FIs based on laser Raman analysis. All partition more favorably into vapor (Heinrich The pressures calculated from type L FIAs
analyzed FIs have round, elongate, or negative- et al., 1999). in sulfide stage are 38–192 bar (n = 20), which
crystal shape and range in size from 10 to 40 μm Type L inclusions in sphalerite and calcite should be lower than the trapping pressures.
across. homogenize to liquid. Such FIAs in sphalerite The highest estimate, 192 bar, could be the best
Groups of individual FIs in a particular (n = 11) have Th of 240–369 °C and salinities approximation of the trapping pressure. It indi-
growth zone of the host mineral or in the same of 3.0–9.5 wt% NaCl equivalent. The primary cates a depth of ∼1.9 km assuming hydrostatic
pseudosecondary trails are considered a fluid FIAs in syn-ore calcite (n = 9) have compara- conditions, which is identical to the estimated
inclusion assemblage (FIA; Goldstein and Reyn- ble Th (257–360 °C) and salinities (2.2–6.2 wt% depth for the prograde skarns. This agrees with
olds, 1994). Where growth zones and pseudo- NaCl equivalent). Their compositions are also the observation that many Zn-Pb stage minerals
secondary trails are absent, FIs in a cluster with similar (Fig. S5), with Pb in sphalerite- and and prograde minerals occur in the same samples

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 Figure 2. (A) As/(Na + K)
A B
and Li/(Na + K) ratios of
type B, L, and SL fluid
inclusion assemblages
(FIAs) in the Haobugao
skarn deposit, northeast-
ern China, are different
from that of type V FIAs.
Reconstructed values
for initial fluid are based
on compositions of
prograde-stage brine
and vapor inclusions,
assuming that they are
the boiling product of
10 wt% NaCl equivalent
single-phase fluid. pyx—
pyroxene; sp—sphalerite;
cal—calcite. (B) Fluid Ca/K
mass ratios of formation
C D water, skarn deposits, and
porphyry deposits. In the
plot, boxes show the inter-
quartile range (IQR) of the
data. IQR is defined as the
difference between the
75th percentile and the
25th percentile. Bold hori-
zontal lines represent the
median, and diamonds
represent the means of
the data. Horizontal lines
at the end of each whis-
ker represent the ends of
the 1.5 IQR range beyond
the IQR. Open circle below
the box for Baiyinnuo’er is
an outlier that exceeds the
IQR by a factor of 1.5 to
3. (C,D) Comparison of Haobugao fluids with typical formation water on Rb versus Na and Zn/Na versus K/Na plots. Gray arrows show fluid
evolution trends from prograde to post-ore stage, which are not explainable by mixing with formation water. Compiled fluid compositions for
B–D are from basins and skarn or porphyry deposits from: 1—North America and the Gulf of Thailand (Samson et al., 2008, and references
therein); 2—western Honduras (Samson et al., 2008); 3—northern Finland (Niiranen et al., 2005); 4—northern and central Mexico (Haynes and
Kesler, 1988); 5—northeastern China (Shu et al., 2017, and references therein); 6—northeastern China (this study); 7—northern Mexico (Bertelli
et al., 2009); 8—Bristish Columbia, Canada (Quan et al., 1987); 9—the island of Bougainville, Papua New Guinea (Eastoe, 1978); 10—Colorado,
USA (Audétat, 2015); 11—Utah, USA (Vanko et al., 2001).

(Figs. 1C and 1D), suggesting formation at simi- lower concentrations of the elements, such as brine FIAs but different from the ratios of vapor
lar paleodepths. A pressure correction of 2–12 meteoric water, and indicates that these elements FIAs (Fig. 2A). They are also unlikely to be a
°C has been made using the trapping pressure remained undersaturated during this stage, likely single-phase fluid exsolved from the magma that
192 bar for the type L FIAs (Table S2). due to the high temperatures and salinities main- never boiled (e.g., Shinohara and Hedenquist,
The measured oxygen isotope compositions taining high solubilities of the elements. The 1997; Baker and Lang, 2003) because the As/
(δ18O) of prograde pyroxene and garnet are δ18OH2O values of the fluids (5.5‰–8.5‰) indi- (Na + K) and Li/(Na + K) ratios of the Zn-Pb-
3.7‰–6.7‰, and the calculated δ18OH2O values cate a magmatic origin (Meinert et al., 2003), mineralizing fluids are significantly lower than
are 5.5‰–8.5‰ (Table S6). The measured δ18O which is consistent with the near-lithostatic con- the reconstructed As/(Na + K) and Li/(Na + K)
values for magnetite in Fe mineralization stage ditions under which external fluid involvement ratios of the initial single-phase fluid before boil-
are −5.5‰ to −3.4‰, corresponding to δ18OH2O was unlikely. ing (Fig. 2A). The cooling gradually drove the
values of 1.9‰–4.4‰ (Table S6). The δ18O val- The sulfide-stage fluids have significantly system into a brittle state (Fournier, 1999) and
ues for the sulfide stage calcite and quartz are lower salinities (2.2–9.5 wt% NaCl equivalent) the prograde skarns had abundant interstitial
5.9‰–8.4‰, with the calculated δ18OH2O values than the prograde fluids. They are likely the mix- spaces between the crystals (e.g., Figs. 1C and
being −0.4‰ to 3.2‰ (Table S6). ing product of the prograde brine and meteoric 1D), both of which permitted mixing.
water, as indicated by the gradual decrease Mixing was an important Zn-Pb deposition
FLUID SOURCES, EVOLUTION, AND in the δ18OH2O values from the prograde flu- mechanism. During the Zn-Pb stage, the decreas-
METAL DEPOSITION ids (5.5‰–8.5‰) through the Fe stage fluids ing concentrations of both Zn-Pb and other non-
The fluid salinities (35.4–45.3 wt% NaCl (1.9‰–4.4‰) to the sulfide-stage fluids (−0.4‰ precipitation elements (e.g., Na, K, Cs, and Rb)
equivalent) and element (e.g., Na, K, Rb, Cs, to 3.2‰; Fig. S6). They are unlikely to be the along with the drop in temperatures indicate the
Zn, Pb, Sn, and Mo) concentrations of the contracted prograde-stage vapor (e.g., Heinrich, occurrence of mixing, while the stronger deple-
prograde-stage brine remain nearly constant 2005), as revealed by the As/(Na + K) and Li/ tion of Zn-Pb than other elements, as revealed
over the temperature range of >550–440 °C (Na + K) ratios of the Zn-Pb-mineralizing flu- by the decreasing Zn/(Na + K) and Pb/(Na + K)
(Fig. 3A). This excludes mixing with fluids with ids, which are similar to those of the prograde ratios whereas other elements’ ratios to Na + K

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 assume that all the removed Zn is in sphalerite,
A then the total brine needed to generate the ∼0.29
Mt Zn is ∼38 Mt. If all the Sn and Mo in the
∼38 Mt brine were eventually precipitated, then
maximum ∼2900 t Sn and ∼2200 t Mo could
have been deposited. However, Sn/(Na + K) and
Mo/(Na + K) ratios show little variation from
the early brine to the later sulfide-stage fluids,
in contrast to the significant drop of Zn/(Na + K)
and Pb/(Na + K) ratios (Fig. 3B). This indicates
Figure 3. Evolution of
element concentrations
that there was no significant loss of Sn and Mo
(A) and mass ratios X/ from the fluids. Therefore the precipitated Sn
(Na + K) (B) for Haobugao and Mo tonnages should be far lower than the
skarn deposit (northeast- above estimated maximum possible values, and
ern China) fluid inclusion it is then unlikely that Haobugao contains Sn or
assemblages (FIAs)
from prograde stage Mo ores of economic significance. This study
through sulfide stage demonstrates a potentially powerful tool when
B to post-ore stage. pyx— evaluating the metal endowment of a given min-
pyroxene; sp—sphalerite; eral prospect, which may help guide exploration.
cal—calcite.
ACKNOWLEDGMENTS
This work was funded by the National Natural Science
Foundation of China (grants 41602083 and 41973043),
the 111 Project (grant BP0719021), and the MOST
Special Fund from the State Key Laboratory of Geo-
logical Processes and Mineral Resources, China
University of Geosciences (grant MSFGPMR201804).
We thank Yong Lai, Yi Hu, Johannes Hammerli, and
Jan-Marten Huizenga for their assistance with anal-
yses. The manuscript benefitted considerably from
discussions with and comments from Rich Goldfarb,
insightful reviews by three anonymous reviewers, and
editorial handling by Gerald Dickens.
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