Lithos 202–203 (2014) 207–226

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Lithos
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Highly fractionated S-type granites from the giant Dahutang tungsten

deposit in Jiangnan Orogen, Southeast China: geochronology,
petrogenesis and their relationship with W-mineralization
Lan-Chun Huang a, Shao-Yong Jiang a,b,c,⁎
a
State Key Laboratory for Mineral Deposits Research, School of Earth Sciences and Engineering, Nanjing University, Nanjing 210093, China
b
State Key Laboratory of Geological Processes and Mineral Resources, China University of Geosciences, Wuhan 430074, China
c
Faculty of Earth Resources and Collaborative Innovation Center for Exploration of Strategic Mineral Resources, China University of Geosciences, Wuhan 430074, China

a r t i c l e i n f o a b s t r a c t

Article history: The Dahutang deposit is a newly discovered tungsten deposit, which is within the largest ones in the world with
Received 30 November 2013 an estimated WO3 reserve of 2 million tones. W-mineralization is considered to be related with the Late Mesozoic
Accepted 31 May 2014 granites in the district. However, the precise emplacement ages, sources of these granites, and their relationship
Available online 9 June 2014
with mineralization are not well understood. In this study, four mineralization-related granite bodies (G1 to G4)
were identified in the Dahutang mining area, including the porphyritic-like two-mica granite (G1) (the size of its
Keywords:
Early Cretaceous
phenocrysts is from 0.2 × 0.2 cm2 to 0.7 × 0.3 cm2), middle- to fine-grained muscovite granite (G2), porphyritic
U–Pb geochronology two-mica granite (G3) (the size of its phenocrysts is from 0.3 × 0.2 cm2 to 0.9 × 0.6 cm2), and fine-grained two-
W-mineralization mica granite (G4). LA-ICP-MS U–Pb dating of zircon grains from these four granite bodies yields emplacement
S-type granite ages of 144.0 ± 0.6 Ma, 133.7 ± 0.5 Ma, 130.3 ± 1.1 Ma and 130.7 ± 1.1 Ma, respectively. Granites contain quartz,
Jiangnan Orogen K-feldspar and plagioclase as the principal phases, accompanied by muscovite, minor biotite and accessory
Southeast China minerals. Geochemically, the granites are strongly peraluminous, have high contents of alkalis, high Ga/Al ratios,
enrichment in LILEs (such as Rb) and depletion in HFSEs (such as Zr, Nb, Ti). The granites formed at relatively low
temperatures (679 °C to 760 °C) according to zircon saturation temperatures. Geochemical fractionation trends
recorded by whole rocks and minerals permit to distinguish and model the two fractional crystallization series G1
and G2–G4. Fractional crystallization of orthoclase and albite in G1 and G4, and orthoclase and oligoclase in G2
and G3 was the principal process of magmatic differentiation that controlled Rb, Sr and Ba concentrations,
whereas rare earth elements were fractionated by accessory minerals, such as apatite, zircon and monazite.
The geochemical data suggest that the rocks are highly fractionated S-type granites. The granites show bulk
rock εNd(t) values in the range of − 9.37 to − 5.92 and zircon εHf(t) values from − 8.44 to − 2.13, with late
Mesoproterozoic TCDM ages for both Nd and Hf isotopes. Geochemical and isotopic data suggest that these highly
fractionated S-type granites G1 and G2–G4 were originated from two episodes of partial melting of different
protoliths which have analogous components of metamorphosed pelitic rocks from the Neoproterozoic
Shuangqiaoshan Group, which are enriched in tungsten. Extreme fractional crystallization resulted in further
enrichment of tungsten in the evolved granitic magma. The new presented data together with previously pub-
lished data suggest that the Dahutang granitic complex was likely to be formed during lithospheric thinning
and asthenospheric upwelling process in Eastern China.
© 2014 Elsevier B.V. All rights reserved.

1. Introduction
The occurrence of tungsten mineralization is generally related to
granitic intrusions of both S- and A-type granites, such as the S-type
granites related with the tin–tungsten mineralization in the Khuntan
⁎ Corresponding author at: State Key Laboratory for Mineral Deposits Research, School
of Earth Sciences and Engineering, Nanjing University, Nanjing 210093, China. Tel.: +86
13952003223.
E-mail addresses: shyjiang@cug.edu.cn, shyjiang@nju.edu.cn (S.-Y. Jiang).
Batholith, northern Thailand (Yokart et al., 2003) and the nearly
contemporaneous A- and S-type granites related with tin-tungsten
mineralization in the Krušné hory/Erzgebirge Mts., Central Europe
(Breiter, 2012). These granites are usually enriched in tungsten, tin or
molybdenum well above Clarke values and are termed as tungsten-
bearing or tin-bearing granites (Hua et al., 2007; Lehmann, 1987,
1990; Mao et al., 2007; Neiva, 1984). The intrusions are commonly
emplaced at shallow crustal levels and possess alkaline to peraluminous
characteristics, with enrichments in volatile elements such as F, Li, and
sometimes B (Fogliata et al., 2012; Xie et al., 2009; Zhao et al., 2001).

http://dx.doi.org/10.1016/j.lithos.2014.05.030
0024-4937/© 2014 Elsevier B.V. All rights reserved.
208 L.-C. Huang, S.-Y. Jiang / Lithos 202–203 (2014) 207–226
Several models have been proposed for the role of magmatic evolution
in tungsten enrichment: (i) transfer of the rare metals by a fluid to the
top of a silicic magma chamber (Kovalenko and Kovalenko, 1984),
(ii) extreme fractional crystallization of magma (Breiter, 2012; Gomes
and Neiva, 2002; Raimbault et al., 1995), (iii) post-magmatic hydrother-
mal alteration processes, such as greisenization (Neiva, 2002), which
promote the release of metals from biotite, hornblende and other min-
erals in the granite (Zhao et al., 2005). Here we present new geological,
geochemical and isotopic data that shed new light on the origin of
the world's largest tungsten ore deposit and related granites in the
Dahutang area of the Jiangnan Orogen, Southeast China.
Southeast China is renowned for widespread magmatism and
mineralization in the Late Mesozoic, and its richness in ore deposits of
W, Sn, U, Nb–Ta, Cu, Pb, Zn and the REE (Hua et al., 2007; Mao et al.,
2007; Sun et al., 2012). Most mineralization belts in South China are
considered to be genetically and spatially associated with Late Jurassic
to Early Cretaceous intrusive granites (Chen et al., 1993; Wang et al.,
2012a,b; Xie et al., 2012a,b; Mao et al., 2006; Wu et al., 2012). In recent
years, several Late-Yanshanian granite-related W and W–Mo deposits
with ages between 143 and 137 Ma have been discovered and exploited
in the transition zone between the Lower Yangtze River Valley and the
Gan-Hang Belt (Mao et al., 2013; Qin et al., 2010; Song et al., 2012,
2013), with the Dahutang deposit having an estimated tungsten re-
source of up to 2.0 million tons of WO3 and an established tungsten re-
serve that exceeds 1.1 million tons of WO3 (Mao et al., 2013). However,
little is known about the petrogenesis of the ore-related granites.
In this study, we present precise zircon U–Pb ages of four granite
bodies which are spatially related to tungsten mineralization, togeth-
er with geological and mineralogical chemistry and petrographic,
whole rock geochemical and Nd isotopic and Hf isotopic data, in an
attempt to better understand the petrogenetic processes and their re-
lationship with mineralization as well as the tectonic evolution of the
region.
2. Geological setting and sampling
2.1. Geological setting
The Southeast China includes the Yangtze Block in the northwest
and Cathaysia Block in the southeast, and is surrounded by the North
China Craton in the north, the Tibetan Plateau in the west, the Indochina
Block in the southwest and the Philippine Sea Plate in the east. Different
tectonic histories and crustal ages support a distinction between the
Yangtze and Cathaysian blocks (e.g., Qiu et al., 2000; Xu et al., 2007;
Zheng et al., 2006). The ca. 1500 km long ENE-trending Proterozoic
Jiangnan Orogen is located along the southeastern margin of the
Yangtze Block and adjacent to the Cathaysian Block (Fig. 1a). It has
been widely accepted that the area of Jiangnan Orogen was outlined
mainly based on the distribution of Proterozoic magmatic rocks and
meta-sedimentary sequences between the two blocks (Shu and Charvet,
1996).
There are two series of metasedimentary rocks separated by an
unconformity in the Jiangnan Orogen. Sedimentary rocks below the un-
conformity comprise the Shuangqiaoshan Group in northwestern Jiangxi
Province, which are mainly pelitic and sandy metasedimentary rocks
with few metavolcanic rocks (Huang et al., 2003). The Shuangqiaoshan
Group is equivalent to the Tongchang Group in the northeastern Jiangxi
Province and the Shangxi Group in the southern Anhui Province.
Sedimentary rocks above the unconformity comprise the Dengshan
Group in Jiangxi Province, equivalent to the Xiuning Formation in
Anhui Province (Wang and Li, 2003), and show approximate upright,
open folds (BGMRJX, 1984; Wang et al., 2007a,b). These two suits of
low-grade metasedimentary rocks are considered to have been formed
separately in the Meso- and Neoproterozoic (Ma et al., 1984; Zhang
et al., 1984). However, recent studies have indicated that the
Shuangqiaoshan Group below the unconformity was deposited during
the Neoproterozoic (Gao et al., 2008, 2012; Q. Wang et al., 2007a,b,
2008). In the Dahutang area, strata of the Shuangqiaoshan Group
occur in the form of a suite of thick greenschist facies turbidite
metasedimentary rocks. These metasedimentary rocks can be further
subdivided into four formations from oldest to youngest: Hengyong,
Jilin, Anlelin and Xiushui formations (Gao et al., 2008; Liu, 1997). Local-
ly, the Shuangqiaoshan Group consists mainly of tuffaceous sandstone,
phyllite, tuff, phyllite slate and lesser spilite and quartz-keratophyre
(BGMRJX, 1984; Liu, 1997).
The Dahutang area is located in the northern part of the Jiuling
Mountain in the center of the Jiangnan Orogen, and surrounded by the
Jiurui region of Middle-Lower Yangtze Valley Mineralization Belt in
the north and the Xiangshan district of Gan-Hang Belt in the south
(Fig. 1a). The Jiuling Mountain, a Neoproterozoic granitic intrusion, is
the largest composite granitoid complex in south-eastern China with
an outcrop area greater than 2500 km2 (Zhong et al., 2005), intruded
in the aforementioned basement sequences of the Shuangqiaoshan
Group. The Late Mesozoic granitic rocks consist predominately of
porphyritic-like two-mica granite (G1), middle- to fine-grained musco-
vite granite (G2), porphyritic two-mica granite (G3) and fine-grained
two-mica granite (G4). These granitic rocks can be roughly divided
into two stages (Fig. 2a; Cao, 2011). In the early stage, G1 granitic rocks
occur as sills and dykes mostly, showing the north–south trending
lengths from one hundred meters to several hundred meters and
thicknesses from several meters to tens of meters, intruded in the
Neoproterozoic granodiorite batholith or in the low-grade metamor-
phic rocks of Shuangqiaoshan Group (Figs. 1b; 2b). In the late stage,
G2 G3 and G4 granitic rocks sharply cut granite G1 and Neoproterozoic
granodiorite batholith as stocks, cones and pipes (Fig. 2a). Granites G2
G3 and G4 were occasionally encountered in boreholes drilled at depths
of several hundreds of meters below the surface, so the geological inter-
relations among G2–G4 are not clear at this stage. In this area, the
pegmatite with salmon-pink K-feldspar phenocrysts (the size of its
phenocrysts is up to 2.5 cm × 1.2 cm) is around these granites and the
tungsten-ore body at margin. Ore veins surround the crest of the Late
Mesozoic granite complex, cutting G1 granitic rocks and being cut by
G2 granitic rocks (Fig. 2a, b). Wolframite and scheelite are the main
ore minerals in the Dahutang tungsten ore deposit. The tungsten miner-
alizations can occur in quartz veins, dip-dying veinlets, altered granites,
greisens and cryptoexplosive breccias. Previous researchers have noted
the episodic nature of the Mesozoic intrusions and their relations with
the W-mineralization in the Dahutang area (Lin et al., 2006a,b).
2.2. Petrography
Samples for this study have been collected from drill cores and
underground tunnels in the Dahutang mining area. The mineralogical
and petrographic features and sampling depth of the samples are
summarized in Table 1. The sample locations are briefly described as
follows.
The samples of G1 (zk0-26-1 to zk0-26-3) were collected from bore-
hole zk0-26 in the south part of the Dahutang mining area. The samples
of G2 were collected from drill cores zk108 (zk108-2-1, zk108-2-2,
zk108-2-4) and zk11-5 (zk11-5-25, zk11-5-27, zk11-2-12) in the
north part of the Dahutang mining area and from zk11-2 in the south
part of the Dahutang mining area. All the samples of G3 (zk1-4, zk1-6,
zk1-9, zk1-11 and zk1-13 were collected from 726 m to 893 m in bore-
hole zk1 in the south part of the Dahutang mining area. The samples of
G1 (81#-12) and G4 (81#-23 to 81#-26) were collected from under-
ground tunnels in the northern Dahutang mining area, the depth of
these samples were less than 20 m to the surface.
The main minerals in these granites are quartz, orthoclase, muscovite,
albite in G1 and G4, and oligoclase in G2 and G3. The feldspars are not
zoned. The phenocrysts consist of quartz, orthoclase, albite or oligoclase.
The sizes of G1 and G3 granitic phenocrysts are from 0.2 cm × 0.2 cm to
0.7 cm × 0.3 cm and 0.3 cm × 0.2 cm to 0.9 cm × 0.6 cm, respectively.
 L.-C. Huang, S.-Y. Jiang / Lithos 202–203 (2014) 207–226 209

Fig. 1. (a) Distribution of Mesozoic granites and volcanic rocks in South China (modified after Zhou et al., 2006). The South China Block is comprised of two blocks: Yangtze Block and
Cathaysia Block. The approximate position of the Jiangnan Orogenic Belt is also outlined in the map, which is in the edge of Cathaysia Block and belongs to Yangtze Block; (b) Simplified
geological map of the Dahutang tungsten deposit (modified after Cao, 2011).

Accessory minerals include monazite, ilmenite, magnetite, apatite,
zircon, scheelite and wolframite. All the samples contain minor biotite.
Granites G1 and G2 show porphyritic-like texture. Granites G3 and G4
show granitic texture and porphyritic texture. In addition, some samples
contain miarolitic cavities which suggest that they were emplaced at
shallow levels after extensive fractional crystallization. Quartz is the
main filler in the miarolitic cavities, associated with a small amount of
apatite and scheelite. Cordierite was not observed in any of our samples.
Instead, the Dahutang samples display plagioclase ± muscovite assem-
blages. The four types of granites from the Dahutang area do not contain
mafic minerals such as arfvedsonite and riebeckite, which are sometimes
found in alkaline granites. The scheelite and wolframite have been
found in the granitic rocks of G1–G4, showing irregular shapes from
10 μm × 5 μm to 70 μm × 30 μm and existing in quartz, orthoclase or
oligoclase (Fig. 3a, b, c, d). In Fig. 3a, the scheelite has a paragenetic
relationship with wolframite in the matrix of G1 granitic rocks. In
Fig. 3c, the scheelite is associated with fluorite and pyrite inhering in
the oligoclase of granite G3. The scheelite and wolframite, showing no
signs of alteration or veinlets cutting around them, are directly grown
in the rock-forming minerals. They should be crystallized directly
from the granitic magmas and no later than the formation time of the
rock forming minerals.
210 L.-C. Huang, S.-Y. Jiang / Lithos 202–203 (2014) 207–226

analyses for the samples were carried out in the State Key Laboratory for
Mineral Deposits Research, Nanjing University. Whole-rock major ele-
ment analyses were determined by Thermo Scientific ARL 9900 X-ray
Fluorescence (XRF) on fused glass, following a procedure described by
Norrish and Hutton (1969). The precisions are better than 1% with the
elemental abundances N1%, while the precisions are about 10% with
the elemental abundances b 1%. For trace element analyses, about
50 mg of powered sample was dissolved in high-pressure Teflon bombs
using an HF + HNO3 mixture. Rh was used as an internal standard to
monitor signal drift during ICP-MS measurements. The trace elements
were measured by a Finnigan Element II inductively coupled plasma
mass spectrometry (ICP-MS). The analytical precisions were estimated
to be better than 10% for all trace elements according to standards and
duplicated analyses. Detailed analytical procedures for trace elements
are described by Gao et al. (2003).

3.2. Sr–Nd isotopic analyses

Sr and Nd isotopic compositions were measured using a Neptune

Fig. 2. Geological sections along exploration line 8 (a) and exploration line 5 (b) of
the Dahutang tungsten deposit showing the major ore bodies, hosted mainly by the
Neoproterozoic biotite granodiorite and Early Cretaceous porphyritic-like two-mica
granite (G1). The late stage middle- to fine-grained muscovite granite (G2) cuts across
the tungsten ore body and the granite G1. (a, b, modified after Cao, 2011).
Plus MC-ICP-MS at the State Key Laboratory for Mineral Deposits
Research, Nanjing University, following the procedures of Pu et al.
(2005). About 50 mg samples were dissolved in the same way as for
trace element analyses. Complete separation of Sr was achieved by a com-
bination of cation-exchange chromatography in H+ form and pyridinium
form with the DCTA complex. Nd was then separated from the REE frac-
tions by cation-exchange resin using HIBA as eluent. After purification,
the separated Sr and Nd were respectively dissolved in 1 ml of 5%
HNO3 for the 87Sr/86Sr and 143Nd/144Nd analysis on MC-ICP-MS. During
the period of laboratory analysis, measurements of NIST SRM-987 Sr
standard yielded 87Sr/86Sr ratio of 0.710280 ± 0.000005 (2σ), and the
JNdi-1 Nd standard yielded 143Nd/144Nd ratio of 0.512086 ± 0.000004
(2σ). Total analytical blanks were 5 × 10−11 g for Sm and Nd and (2 ~
5) ×10−10 g for Rb and Sr. For the calculation of (87Sr/86Sr)i, εNd(t) and
Nd model ages, the following parameters were used: λRb = 1.393 ×
10− 11 year−1 (Nebel et al., 2011); λSm = 6.54 × 10− 12 year− 1
(Lugmair and Marti, 1978); (147Sm/144Nd)CHUR = 0.1967 (Jacobsen and
Wasserburg, 1980); (143Nd/144Nd)CHUR = 0.512638 (Goldstein et al.,
1984); (143Nd/144Nd)DM = 0.513151, (147Sm/144Nd)DM = 0.2136 (Liew
and Hofmann, 1988). The 147Sm/144Nd value of 0.118 (Jahn and Condie,
1995) was used for a two-stage model age calculation (TCDM).

3.3. Zircon U–Pb analysis

3. Analytical methods
3.1. Major and trace element analyses
Samples for whole-rock geochemical analyses were crushed to fine
powders of 200-mesh using an agate mill. The major and trace element
Individual zircon grains were separated from samples through
crushing, conventional magnetic and heavy liquid separation methods
followed by hand picking under a binocular microscope. The zircon
grains were mounted on adhesive tape, enclosed in epoxy resin, and
then polished to section the crystals in about half for analysis. The

Table 1
Lithology and mineralogy of the four granite rock types from the Dahutang mining area.

Samples Rock types Lithology Color Texture Mineralogy Sampling depth (meter)

ZK0-26-1 to G1 Porphyritic-like two-mica Gray Porphyritic-like texture Quartz, alkali feldspar, plagioclase, ≤20, 128 and 524
ZK0-26-3 granite (from 0.2 × 0.2 cm2 to 0.7 × 0.3 cm2), muscovite with minor biotite
81#-12 fine-grained granitic texture for groundmass
ZK108-2-1, G2 Middle- to fine-grained Gray Porphyritic-like texture, fine-grained Quartz, alkali feldspar, plagioclase, 248–341 m, 314–315 m
ZK108-2-2 muscovite granite granitic texture for groundmass muscovite with minor biotite and 557 m
ZK108-2-4
ZK11-5-25,
ZK11-5-27
ZK11-2-12
ZK1-4 to ZK1-6 G3 Porphyritic two-mica Light grey Porphyritic texture Quartz, alkali feldspar, plagioclase, 726-893
ZK1-9 to granite (from 0.3 × 0.2 cm2 to 0.9 × 0.6 cm2), muscovite with minor biotite
ZK1-11 felsitic or microcrystalline texture.
ZK1-13
81#-23 to G4 Fine-grained two-mica Gray Granitic texture Quartz, alkali feldspar, plagioclase, ≤20
81#-26 granite muscovite with minor biotite
 L.-C. Huang, S.-Y. Jiang / Lithos 202–203 (2014) 207–226
Fig. 3. Electron backscattered photos for wolframite and scheelite of the G1–G4 granites. The photos a, b, c, and d from the samples of ZK0-26-2, ZK108-2-1, ZK1-4 and 81#-23 represent
granites G1, G2, G3, and G4 from the Dahutang area.
transmitted and reflected light images of the zircon grains were docu-
mented, and cathodoluminescence (CL) images of the zircon grains
were photographed in order to study their structure and morphology
and selecting spots for U–Pb dating and Lu–Hf analysis. The CL images
of zircon samples were taken using a Gantan CL detector attached to a
JMS6510 scanning electron microscope (manufactured by Japan Elec-
tron, Japan) at Beijing Geoanalysis Company. Zircon U–Pb analyses
were taken at the State Key Laboratory of Ore Deposit Geochemistry,
Institute of Geochemistry, Chinese Academy of Sciences, Guiyang. A
Geo-Las-Pro laser-ablation system (Lamda Physik, Gottingen, Germany)
and an Agilent 7700x ICP-MS (Agilent Technologies, Tokyo, Japan) were
used for U–Pb dating. The 193 nm ArF excimer laser, homogenized by
a set of beam delivery systems, was focused on the surfaces of zircon
samples with an energy density of 10 J/cm2. The ablation protocol
employed a spot diameter of 25 μm at 5 Hz repetition rate for 40 s (equat-
ing to 200 pulses). Helium was applied as carrier gas to efficiently trans-
port aerosol to ICP-MS.
Zircon 91500 was used as external standard to correct instrumental
mass discrimination and elemental fractionation (Wiedenbeck et al.,
1995, 2004). Zircon GJ-1 and Plešovice zircon were used for quality
control (Jackson et al., 2004; Sláma et al., 2008). The Pb abundances of
zircons were externally calibrated against NIST SRM 610 with Si as
internal standard, while Zr was used as an internal standard for other
trace elements (Liu et al., 2010a). Raw data reduction was performed
off-line by using the ICPMSDataCal software (Liu et al., 2010a,b).
The results are presented in Supplemental electronic data Table 1. A
summary of data for all the dated magmatic rocks in the Dahutang area
is listed in Table 2. Some zircon analyses had unstable signals, presum-
ably due to micro-cracks or inclusions. In other cases, 206Pb/238U ages
and 207Pb/235U ages are discordant (corrected ratio lower than 95%),
which were not included in the discussion, but have been listed in
Supplemental electronic data Table 1. Errors on individual analyses are
cited as 1σ, and the weighted mean of the 206Pb/238U ages are quoted
at the 95% confidence level.
211
3.4. Lu–Hf isotope analysis
In situ Lu–Hf isotope analyses of zircons were carried out by means
of 193 nm laser attached to a Neptune multi-collector ICP-MS (LA-
MC-ICP-MS) at the State Key Laboratory for Mineral Deposits Research
of Nanjing University, China. The techniques were described in detail
by (Wu et al., 2006). Most in situ Hf isotope analyses were carried out
in Ar carrier gas with a beam diameter of 28 μm and a 6 Hz repetition
time. For the calculation of εHf values we have adopted the chondritic
values of (Blichert-Toft and Albarède, 1997).
The measured 176Lu/177Hf ratios and the 176Lu decay constant of
1.87 × 10− 11 yr−1 reported by Söderlund et al. (2004) were used to
calculate initial 176Hf/177Hf ratios. The chondritic values of 176Lu/177Hf
(0.0336) and 176Hf/177Hf (0.282785) reported by Bouvier et al. (2008)
were used for the calculation of εHf values. The depleted mantle Hf
model ages (TDM) were calculated using the measured 176Lu/177Hf ratios
of zircon based on an assumption that the depleted mantle reservoir
has a linear isotopic growth from 176Hf/177Hf ratio of 0.279718 at
4.55 Ga to 0.283250 at present, with a 176Lu/177Hf ratio of 0.0384
(Griffin et al., 2000). We also present a two-stage model age (TCDM) for
each zircon, which assumes that its parental magma was produced
from an average continental crust (176Lu/177Hf = 0.015) that originally
was derived from the depleted mantle (Griffin et al., 2002). Hf isotopic
results are reported with 2σ errors in Supplemental electronic data
Table 2.
3.5. Electron microprobe analysis
All elemental analyses of biotite and muscovite were obtained from
polished thin sections using a JEOL JXA-8100 electron microprobe at
State Key Laboratory for Mineral Deposits Research at Nanjing University,
China. The elemental analyses of feldspar were acquired from polished
thin sections using a JEOL JXA-8230 electron microprobe at Testing
Center of Shandong Bureau of China Metallurgy and Geology, China.
212 L.-C. Huang, S.-Y. Jiang / Lithos 202–203 (2014) 207–226

Table 2
Summary of age dating results and Hf isotopic compositions of zircons from the Dahutang granites.

Sample no. Lithology Method U (ppm) Th (ppm) Th/U Age (Ma) εHf (t) TCDM (Ma)

ZK0-26-3 Porphyric-like two-mica granite (G1) LA-ICP-MS 562 ~ 22,280 35 ~ 11,692 0.01 ~ 1.41 144.0 ± 0.6 −8.44 ~ −2.13 1301 ~ 1698 Ma
ave = 7690 ave = 1379 ave = 0.26 ave = −5.20 ave = 1494 Ma
ZK11-5-27 Middle- to fine-grained muscovite granite LA-ICP-MS 186 ~ 7599 82 ~ 2649 0.04 ~ 0.97 133.7 ± 0.5 −8.16 ~ −2.30 1304 ~ 1672 Ma
(G2) ave = 4025 ave = 358 ave = 0.13 ave = −4.31 ave = 1430 Ma
ZK1-4 Porphyritic two-mica granite (G3) LA-ICP-MS 173 ~ 10,993 32 ~ 327 0.02 ~ 0.80 130.3 ± 1.1 −7.56 ~ −3.65 1386 ~ 1632 Ma
ave = 6239 ave = 200 ave = 0.14 ave = −4.97 ave = 1469 Ma
81#-23 Fine-grained two-mica granite (G4) LA-ICP-MS 163 ~ 2891 62 ~ 5237 0.06 ~ 1.57 130.7 ± 1.1 −8.02 ~ −3.03 1347 ~ 1661 Ma
ave = 984 ave = 2365 ave = 0.47 ave = −4.98 ave = 1470

Element determinations (Si, Al, Fe-Total, Mg, Ti, Mn, Ca, Ba, Na, K, F
and Cl) of biotite and muscovite and (Sn, Sr, W) of muscovite were
carried out using a beam size of 1 μm, an accelerating potential voltage
of 15 kV, and a probe current of 15 nA. Standards used were natural
minerals and synthetic compounds, including hornblende (Si, Na, Mg,
Al, Ca, Ti), apatite (F), barium chlorapatite (Cl), fayalite (Fe, Mn),
K-feldspars (K), cassiterite (Sn), barium strontium phosphate (Sr, Ba),
scheelite (W). Matrix effects were corrected using the ZAF software
provided by JEOL. The accuracy of the reported values for the analyses
is 1%–5% depending on the abundance of the element. Element determi-
nations (Si, Al, Fe-Total, Mg, Ti, Mn, Ca, Na, K, Rb and P) of feldspar were
carried out using a beam size of 1 μm–2 μm, an accelerating potential
voltage of 15 kV, and a probe current of 20 nA. Standards used were
natural minerals and synthetic compounds, including jadeite (Si, Na),
almandine garnet (Al, Fe), olivine (Mg), rutile (Ti), rhodonite (Mn),
diopside (Ca), sanidine (K), apatite (P) and rubidium titanyl phosphate
(Rb). Matrix effects were corrected using the ZAF software provided by
JEOL. The accuracy of the reported values for the analyses is 1%–5%
depending on the abundance of the element.
4. Results
4.1. Zircon U–Pb geochronology
U–Pb concordia diagrams for the analytical data are shown in Fig. 4.
Representative zircon CL images of the sample candidates for U–Pb
dating are also inserted in Fig. 4.
The zircon grains of Dahutang granitic complex are euhedral, mostly
around 100 μm in length and elongation ratios of 2:1 to 4:1. Most of
them are transparent and colorless under the optical microscope. Con-
centric zoning typical of magmatic zircon is common and some inherited
cores have been observed in CL images. The magmatic zircons have
highly variable U contents from 1248 ppm to 22,281 ppm. The inherited
zircons have lower U contents from 163 ppm to 4862 ppm, and most of

Fig. 4. Representative Cathodoluminescence (CL) images of zircon grains and zircon U–Pb concordia diagrams. The images a, b, c, and d from the samples of ZK0-26-3, ZK11-5-27, ZK1-4
and 81#-23 represent granites G1, G2, G3, and G4 from the Dahutang area. The scale bar is 50 μm.
 L.-C. Huang, S.-Y. Jiang / Lithos 202–203 (2014) 207–226
them are in the hundreds of ppm range (Supplemental electronic data
Table 1).
The zircons from G1 were previously dated by LA-ICP-MS at Nanjing
University, yielding a weighted mean 206Pb/238U age of 144.2 ± 1.3 Ma
(Huang and Jiang, 2012). This sample has been re-analyzed in this study
by LA-ICP-MS, at Guiyang, in order to confirm the reliability of this age.
The weighted mean 206Pb/238U age of granite G1 is 144.0 ± 0.6 Ma
(Fig. 4a). The zircons from G2, G3 and G4 yield weighted mean
206
Pb/238U ages of 133.7 ± 0.5 Ma, 130.3 ± 1.1 Ma and 130.7 ±1.1 Ma,
respectively (Fig. 4b, c, d).
4.2. Major and trace element geochemistry
A total of 21 samples were analyzed for major and trace element
compositions and the results are listed in Table 3. Major element con-
centrations have been recalculated volatile free using loss on ignition
(LOI) data for plotting in the Q'-ANOR diagram of Streckeisen and Le
Maitre (1979), in order to distinguish different types of granitoids
(Fig. 5). In general, the four types of granites all belong to alkali-
feldspar granite (Fig. 5), rich in SiO2 (72.52 to 75.19 wt.%) and alkalis
(alkalinity ratio (A.R.) [Al2O3 + CaO + (Na2O + K2O)]/[Al2O3 + CaO −
(Na2O + K2O)] of 3.09 to 3.80), with high K2O contents of 4.09–
5.09 wt.% and P2O5 contents of 0.15–0.36 wt.% (Table 3). They are strongly
peraluminous with Al2O3 content of 13.50 to 14.80 wt.% and A/CNK ratio
[Al2O3/(CaO + Na2O + K2O)] of 1.16 to 1.29 (Table 3). The calculated
zircon saturation temperatures (TZr) are 679 to 760 °C (Table 3) according
to the zircon saturation thermometry provided by Watson and Harrison
(1983).
The potentially information about the processes and/or physical
conditions of magma evolution can be revealed by the differentiation
trends within the four granites. Förster et al. (1999) and Breiter (2012)
considered this index superior to SiO2 to indicate the differentiation
paths of granitic melts. Because Ti is less easily remobilized by secondary
effects, TiO2 contents in whole rock decrease smoothly and continuously
with progressive differentiation (Förster et al., 1999). Thus, Fig. 6
presents a series of variation diagrams for petrogenetically important
elements with 1/TiO2 as an index of differentiation. Selected major
and trace elements plot on two distinct curvilinear trends defined by:
a) granite G1; b) granite G2, G3 and G4. The two trends start from a
point of origin, but have different directions of differentiation trends.
Compared with granites G2–G4, granite G1 has more sharply differenti-
ation trends in Ba, Sr, Rb, U, Y and Pb contents (Fig. 6d, e, f, h, i), but less
differentiation trends for distinctly higher Fe2O3, MgO, Zr, La and Th
contents (Fig. 6b, c, g, j, l). In the curvilinear trend of G2–G4 (Fig. 6),
G3 as an endmember has higher K2O, Fe2O3, MgO, Ba, Sr, Zr, Y, La and
Th, but distinctly lower Rb and U contents with indistinguishable differ-
entiation, compared with that in G2 and G4. The differentiation trends
of the elements in granite G2 are more obvious than the other three
granites. The concentration of the major and trace elements in granite
G2 decreases steadily, except for Rb and U contents increasing smoothly
alone with the differentiation (Fig. 6). The degree of differentiation in
granite G4 is between the granites G2 and G3.
The Dahutang granites display typical trace element distributions
with low Ba, Sr and high Rb (Table 3). Contents of Sr range from 14.3
to 62.5 ppm. Contents of Rb are relatively high from 387 to 804 ppm
(Table 3). They also have high 10,000*Ga/Al ratios of 2.60–4.46
(Table 3), low contents of high field strength elements (HFSE) such as
Zr, Nb, Ce, Y and relatively low zircon saturation temperatures (679–
760 °C) (Table 3).
The REE contents are relatively low (24–124 ppm). Chondrite-
normalized REE patterns (Fig. 7a, c, e, g) display light REE (LREE) enrich-
ment with strong negative Eu anomalies (Eu/Eu* = 0.13–0.46). The REE
patterns of G1 and G3 each display a relatively narrow range, with
(La/Yb) N of 9.5–11.6 and 11.1–11.9, respectively. In contrast, the REE
patterns of G2 and G4 show a more variable (La/Yb)N ratio of 5.3–18.3
and 15.1–23.3 (Fig. 7c). The four granite types (G1 to G4) exhibit similar
213
trace element patterns, and they have similar negative anomalies in Ba,
Nb, Sr, Ti, Zr and positive anomalies in Rb, U, Ta as shown in the primitive
mantle-normalized trace-element diagrams (Fig. 7b, d, f, h).
4.3. Whole rock Sr–Nd and zircon Hf isotopic compositions
The Sr–Nd isotopic analytical results for Dahutang granites are given
in Table 4. Initial Sr–Nd isotopic compositions depending on the different
lithologies were calculated at t = 144 Ma (for G1), t = 134 Ma (for G2),
and t = 130 Ma (for G3 and G4), respectively. Calculated initial 87Sr/86Sr
ratios range from 0.680113 to 0.788563. The wide range of initial 87Sr/
88
Sr ratios and some unreasonably low ratios reflect the large range
and sometimes very high 87Rb/86Sr ratios (22 to 118). The high Rb/Sr
ratios of the samples can lead to the analytical uncertainty considerably
larger, especially for samples with very low Sr contents (e.g. b 20 ppm)
(Romer et al., 2012). Therefore, all the samples of G1–G4 do not yield
meaningful initial Sr-isotopic compositions because of their high Rb/Sr
ratios (8–41). The four granitic bodies show a range of εNd(t) values of
− 9.4 to − 5.7, with most εNd(t) values ranging between − 7.9 and
− 7.0. The corresponding Nd model ages (TCDM) of G1 to G4 range
between 1406 Ma and 1689 Ma, with most TCDM between 1500 Ma and
1580 Ma.
The Hf isotopic analytical results of zircons for granites G1 to G4
are presented in Supplemental electronic data Table 2. The εHf(t) values
range from −8.44 to −2.13, whereas the averages are of −5.20 (G1),
− 4.31 (G2), − 4.97 (G3) and − 4.98 (G4) (Table 2, Fig. 8a, c, e, g),
showing Mesoproterozoic to Paleoproterozoic TCDM ages, from 1301 Ma
to 1698 Ma (Fig. 8b, d, f, h). The Hf model ages of G1 to G4 show nearly
normal distributions and TCDM age peaks occur at 1500–1550 Ma (G1)
and 1400–1450 Ma (G2 to G4) (Fig. 8b, d, f, h).
4.4. Mineral compositions
4.4.1. Mica
Representative electron microprobe analyses and chemical formulae
calculated for biotite and muscovite from granites G1 to G4 are listed in
Supplemental electronic data Tables 3 and 4, respectively. All of the
Dahutang biotites are rich in Fe with high Fe/(Fe + Mg) ratios of
0.604–0.783. The biotites from these granites display high TiO2 contents
(1.88%–4.32%), F contents (up to 3.89 %) but low Cl contents (0.00%
~ 0.05%), with relatively wide range of Fe3+/(Fe2+ + Fe3+) ratio from
0.017 to 0.227 and Mg/(Mg + Fe2+ + Fe3+) of 0.22–0.40 corresponding
to biotites of aluminous-potassic rock series (Nachit et al., 1985). The
muscovites of granites G1–G4 are relatively rich in Fe (Fe/(Fe + Mg)
ratios of 0.52–0.81). They have high TiO2 (up to 0.85) and Al2O3 (up to
37.98) and low MgO, corresponding to primary muscovite according to
the criteria of Miller et al. (1981) and Monier et al. (1984). The content
of SiO2 in biotite increases with the degree of fractionation of granites
G1–G4, while the content of FeO (total) and Al2O3 decreases (Fig. 9a, b).
The content of FeO (total) and F in micas of granite G1 changes little
(Fig. 9c). However, the micas of granites G2–G4 evolve with fractionation,
along with a steady increase in F from 0 to 3.30 and from 0 to 3.89 respec-
tively in the muscovite and biotite (Fig. 9c).
4.4.2. Feldspar
The compositions of K-feldspar and plagioclase phenocryst from
granites G1–G4 are given in supplemental electronic data Tables 5 and
6, respectively. The orthoclase contents of the four granitic rocks are
similar (94 to 98 mol%). The content of Rb2O in the orthoclase pheno-
cryst of G1–G4 generally does not exceed 0.1 wt%. The content of P2O5
in the orthoclase phenocryst of G1–G4 varies from 0 to 0.24 wt%. The
anorthite content of phenocryst from G1 and G4 is higher than the
anorthite content of phenocryst from G2 and G3. Plagioclase in granites
G1 and G4 varies from An9 to An20. Nearly pure end-member, albite
(An0 to An1) forms the plagioclase phenocryst in granites G2 and G3.
The content of P2O5 in plagioclase from G1 and G4 (0.11–0.20 wt%) is
 214
L.-C. Huang, S.-Y. Jiang / Lithos 202–203 (2014) 207–226
Table 3
Major (wt.%) and trace element (ppm) compositions from the Dahutang granites.

Sample 81#-12 ZK0-26-1 ZK0-26-2 ZK0-26-3 ZK108-2-1 ZK108-2-2 ZK108-2-4 ZK11-2-12 ZK11-5-25 ZK11-5-27 ZK-1-4 ZK-1-5 ZK-1-6 ZK-1-9 ZK-1-10 ZK-1-11 ZK-1-13 81#-23 81#-24 81#-25 81#-26

Rock type G1 G1 G1 G1 G2 G2 G2 G2 G2 G2 G3 G3 G3 G3 G3 G3 G3 G4 G4 G4 G4

SiO2 74.00 72.52 72.88 73.33 73.50 72.94 73.62 74.31 73.03 73.89 73.48 73.79 73.08 73.30 73.90 74.07 73.00 74.87 73.80 75.19 73.98
TiO2 0.15 0.17 0.18 0.16 0.05 0.08 0.06 0.11 0.16 0.17 0.16 0.16 0.15 0.16 0.15 0.15 0.16 0.10 0.11 0.13 0.13
Al2O3 13.91 14.21 14.27 14.02 14.54 14.80 14.67 14.31 14.61 14.34 14.02 13.99 13.92 13.62 13.74 14.11 14.47 13.59 13.98 13.50 13.85
Fe2O3(total) 1.25 1.36 1.47 1.50 0.79 1.10 0.80 1.02 1.26 1.35 1.34 1.33 1.33 1.31 1.29 1.28 1.35 1.01 1.04 1.28 1.16
FeO 0.88 1.10 1.12 1.10 0.68 0.79 0.70 0.78 0.95 1.06 1.10 0.94 1.12 0.69 1.08 1.15 1.16 0.87 0.90 1.02 0.97
MnO 0.04 0.04 0.04 0.04 0.05 0.05 0.04 0.06 0.03 0.03 0.03 0.03 0.03 0.03 0.03 0.03 0.03 0.03 0.03 0.04 0.03
MgO 0.33 0.32 0.30 0.31 0.21 0.25 0.21 0.28 0.35 0.34 0.37 0.33 0.36 0.37 0.36 0.34 0.36 0.24 0.26 0.32 0.29
CaO 0.74 0.75 0.59 0.73 0.54 0.65 0.56 0.73 0.82 0.85 0.71 0.70 0.72 0.45 0.67 0.72 0.71 0.63 0.67 0.61 0.82
Na2O 2.91 3.70 3.69 2.92 3.87 3.40 3.71 3.63 3.45 3.35 3.42 3.23 3.48 3.24 3.28 3.43 2.95 3.01 2.96 2.51 2.89
K2O 4.97 4.39 4.27 4.77 4.09 4.73 4.15 4.36 4.70 4.42 4.74 4.72 4.62 4.96 4.80 4.75 5.00 4.66 5.07 4.84 5.09
P2O5 0.23 0.29 0.29 0.25 0.36 0.32 0.30 0.35 0.23 0.25 0.22 0.22 0.23 0.21 0.22 0.23 0.22 0.19 0.18 0.18 0.15
LOI 1.34 1.50 1.56 1.59 1.37 1.45 1.47 1.27 1.60 1.59 1.46 1.27 1.35 1.78 1.84 1.51 1.88 1.20 1.31 1.37 1.36
Total 99.86 99.24 99.56 99.61 99.37 99.78 99.59 100.43 100.24 100.58 99.96 99.76 99.27 99.43 100.28 100.61 100.13 99.52 99.40 99.97 99.75
A.R. 3.32 3.35 3.31 3.18 3.24 3.22 3.13 3.26 3.23 3.09 3.49 3.35 3.48 3.80 3.55 3.46 3.20 3.34 3.42 3.18 3.39
A/CNK 1.21 1.16 1.21 1.24 1.23 1.24 1.26 1.19 1.19 1.21 1.16 1.20 1.16 1.18 1.16 1.16 1.25 1.22 1.21 1.29 1.18
Li 712 270 301 233 412 656 522 478 615 736 153 164 158 127 164 150 563 165 192 129 182
Be 7.51 19.1 12.9 10.1 2.80 11.4 4.06 27.9 7.71 6.17 8.71 9.23 8.43 8.05 9.61 9.16 34.1 18.2 3.96 3.93 3.05
Sc 3.75 4.49 4.97 4.41 3.14 3.48 3.93 4.35 3.49 3.80 4.26 3.96 4.40 4.05 4.46 3.46 4.14 2.74 3.56 2.35 3.43
Ti 1398 1492 1685 1487 438 718 730 1034 1364 1561 1459 1378 1434 1438 1409 1230 1374 713 965 739 1096
V 10.6 11.9 12.7 11.6 1.72 3.82 4.71 9.72 13.5 14.5 12.8 11.9 12.1 12.2 12.9 10.9 12.4 6.71 8.43 8.25 12.1
Cr 6.76 6.09 10.0 6.67 6.91 3.35 5.41 6.53 49.8 12.2 13.2 10.3 16.6 10.4 10.3 6.51 5.80 9.44 13.2 11.1 10.4
Mn 346 325 359 333 374 457 440 475 250 254 254 237 259 252 256 198 220 186 269 196 249
Co 1.47 1.62 1.67 1.67 0.37 0.63 0.74 1.23 2.23 2.02 1.93 1.94 1.84 1.80 1.94 1.56 1.69 1.00 1.86 1.23 1.99
Ni 3.51 2.72 4.65 3.40 3.38 1.59 2.78 3.20 24.80 6.04 6.95 6.11 8.39 6.35 4.89 2.97 2.57 6.05 6.82 5.68 4.51
Cu 93.4 103.1 6.07 395 171 89.7 98.8 62.1 54.0 107 4.10 3.76 3.82 5.18 3.31 0.99 3.23 138 556 174 98.0
Zn 97.0 96.1 75.9 158 133 95.5 125 48.9 91.3 114 53.3 194 58.9 54.5 55.5 42.9 42.8 47.6 68.5 48.5 76.5
Ga 26.4 30.4 33.7 32.3 27.2 28.6 33.2 26.4 28.3 30.1 27.5 26.3 28.1 24.5 26.5 24.3 25.4 20.4 27.8 18.6 25.1
Rb 804 616 571 707 532 621 730 790 618 653 472 458 488 457 473 447 499 473 575 387 519
Sr 40.3 24.9 21.7 36.7 14.3 15.3 27.4 48.2 39.0 33.5 46.1 55.6 41.7 55.3 46.2 42.0 65.2 29.7 39.9 29.7 49.9
Y 9.29 12.6 13.3 11.5 6.85 8.31 9.69 9.99 9.60 9.69 13.3 13.5 14.0 12.9 13.1 12.2 13.5 7.03 9.31 6.34 9.87
Zr 87.8 91.1 98.3 88.5 33.5 38.4 45.8 55.0 90.0 91.2 80.8 82.4 86.3 82.1 86.0 75.5 83.6 39.9 50.0 43.7 61.7
Nb 14.6 18.5 19.6 16.6 11.7 15.1 15.9 15.9 8.45 9.28 12.1 11.9 12.9 11.6 11.2 11.2 11.3 11.5 12.9 8.01 11.0
Mo 1.31 1.22 1.86 0.97 0.39 0.54 5.39 0.87 0.61 1.27 1.77 0.92 0.96 0.78 1.02 0.59 0.54 0.87 2.91 11.5 71.8
 Cd 0.28 0.47 0.16 0.89 0.27 0.17 0.17 0.19 0.15 0.20 0.10 0.11 0.09 0.08 0.09 0.07 0.08 0.12 0.33 0.14 0.21
Sn 78.2 81.6 52.7 65.8 83.7 51.3 88.9 90.6 82.7 108 22.2 23.8 23.9 19.3 23.0 21.5 23.1 40.1 53.5 37.5 40.0
Cs 246 184 178 177 218 258 245 421 265 334 92.0 97.8 94.0 139 105 119 406 112 100 55.0 60.0
Ba 174 79.6 45.2 136 25.9 26.8 74.1 127 135 132 160 148 150 166 166 142 167 97.3 145 101 161
La 22.7 21.3 23.3 22.5 4.05 7.12 7.79 11.1 18.8 21.8 18.5 16.8 17.3 17.6 18.5 14.6 16.7 8.02 10.9 8.39 12.2
Ce 48.9 50.4 54.0 53.4 9.48 16.5 18.2 24.1 42.8 48.0 43.1 40.7 41.6 41.3 43.5 34.9 39.2 17.5 24.4 18.0 28.0
Pr 5.54 5.61 6.26 5.89 1.10 1.83 1.99 2.55 4.67 5.32 4.74 4.45 4.72 4.68 4.84 3.94 4.11 1.87 2.58 1.96 2.99
Nd 20.0 20.6 23.5 20.9 3.85 6.53 7.15 9.38 17.2 19.4 17.9 16.8 17.4 17.0 17.6 14.4 14.4 6.67 9.34 7.05 11.20
Sm 4.43 4.94 5.46 5.00 1.34 1.88 2.07 2.19 3.77 4.15 4.58 4.31 4.51 4.32 4.57 3.74 3.75 1.60 2.34 1.66 2.46
Eu 0.40 0.28 0.21 0.35 0.07 0.09 0.18 0.30 0.32 0.35 0.38 0.35 0.37 0.36 0.41 0.30 0.36 0.22 0.34 0.24 0.35
Gd 3.22 3.72 4.15 3.46 1.38 1.88 2.08 1.92 2.75 3.05 3.85 3.61 3.81 3.69 3.76 3.16 3.42 1.50 2.12 1.51 2.23
Tb 0.40 0.49 0.57 0.43 0.24 0.30 0.35 0.29 0.36 0.40 0.53 0.51 0.54 0.53 0.56 0.45 0.51 0.24 0.32 0.23 0.34
Dy 2.29 2.94 3.36 2.71 1.61 1.87 2.18 2.05 2.01 2.22 3.23 3.05 3.28 3.13 3.14 2.77 2.95 1.53 2.08 1.42 2.03
Ho 0.37 0.51 0.57 0.46 0.25 0.31 0.37 0.38 0.37 0.41 0.57 0.54 0.59 0.55 0.56 0.49 0.53 0.27 0.37 0.25 0.35
Er 0.89 1.26 1.39 1.10 0.63 0.77 0.90 1.02 0.95 1.06 1.42 1.31 1.40 1.34 1.45 1.19 1.32 0.65 0.90 0.61 0.91
Tm 0.12 0.17 0.18 0.14 0.09 0.11 0.13 0.15 0.13 0.14 0.19 0.17 0.19 0.18 0.19 0.16 0.17 0.09 0.13 0.09 0.12
Yb 0.70 1.01 1.04 0.85 0.55 0.64 0.75 0.91 0.81 0.85 1.14 1.06 1.12 1.10 1.12 0.94 1.04 0.61 0.81 0.52 0.77
Lu 0.10 0.13 0.15 0.12 0.07 0.09 0.10 0.13 0.12 0.13 0.16 0.15 0.16 0.16 0.16 0.14 0.16 0.09 0.11 0.08 0.11
Hf 3.19 3.44 3.84 3.25 1.74 1.89 2.23 2.20 3.18 3.38 3.27 3.13 3.35 3.20 3.26 2.89 3.07 1.62 2.21 1.60 2.26
Ta 3.59 5.58 6.11 4.53 3.77 4.57 5.28 10.18 2.71 2.88 2.59 2.45 2.67 2.34 2.52 2.56 2.33 5.74 7.29 3.44 5.10
W 58.1 33.1 27.9 102 355 103 228 41.1 115 280 9.62 12.0 8.35 9.34 11.3 7.44 188 12.2 10.6 13.9 24.9
Pb 31.0 22.7 20.0 25.7 18.7 22.5 27.7 22.7 27.3 26.0 29.4 26.3 29.3 25.5 29.8 26.9 32.3 29.0 40.0 20.8 39.4
Bi 1.83 5.93 4.06 7.45 0.57 2.88 8.11 2.78 0.88 1.81 1.77 4.12 3.11 1.51 2.84 0.49 1.61 22.5 15.8 20.7 10.5

L.-C. Huang, S.-Y. Jiang / Lithos 202–203 (2014) 207–226

Th 20.1 19.4 21.1 20.3 3.40 6.23 5.97 7.50 16.3 17.5 15.3 13.3 14.3 13.8 15.0 12.3 14.3 5.99 7.69 5.26 8.82
U 11.6 17.6 18.1 15.9 19.6 16.8 18.2 17.3 15.2 12.4 13.4 12.3 13.6 13.0 13.1 13.2 13.1 11.4 13.7 7.59 12.0
Rb/Sr 20 25 26 19 37 41 27 16 16 20 10 8 12 8 10 11 8 16 14 13 10
Zr/Hf 28 26 26 27 19 20 21 25 28 27 25 26 26 26 26 26 27 25 23 27 27
U/Th 0.6 0.9 0.9 0.8 5.8 2.7 3.1 2.3 0.9 0.7 0.9 0.9 0.9 0.9 0.9 1.1 0.9 1.9 1.8 1.4 1.4
Y/Ho 25 25 23 25 27 27 26 26 26 24 23 25 24 23 23 25 26 26 25 26 28
10,000*Ga/Al 3.59 4.05 4.46 4.35 3.53 3.65 4.28 3.48 3.66 3.96 3.71 3.55 3.81 3.40 3.64 3.25 3.31 2.83 3.76 2.60 3.42
ΣREE 110 113 124 117 24.7 39.9 44.2 56.4 95.0 107 100 93.9 97.1 95.9 100 81.1 88.6 40.9 56.8 42.0 64.1
LaN/YbN 23.3 15.1 16.0 19.0 5.32 7.94 7.47 8.71 16.7 18.3 11.6 11.3 11.1 11.5 11.9 11.1 11.5 9.46 9.72 11.6 11.4
Eu/Eu* 0.31 0.19 0.13 0.24 0.17 0.15 0.27 0.43 0.29 0.28 0.27 0.27 0.26 0.27 0.29 0.26 0.30 0.42 0.45 0.46 0.45
M 1.17 1.24 1.19 1.15 1.16 1.16 1.13 1.20 1.21 1.18 1.23 1.19 1.24 1.20 1.22 1.23 1.15 1.15 1.17 1.08 1.20
TZr(°C) 751 750 760 754 679 689 704 713 751 754 741 745 745 744 746 736 749 693 708 704 721

LOI is loss of ignition; A.R. = [Al2O3 + CaO + (Na2O + K2O)]/[Al2O3 + CaO − (Na2O + K2O)] (wt.% ratio); A/CNK = Al2O3/(CaO + Na2O + K2O) (molar ratio).
Eu/Eu* is a measure of the Eu anomaly when compare to Sm and Gd. Eu/Eu* = EuN/[(SmN) × (GdN)]0.5.
T Zr (°C) = 12,900/(2.95 + 0.85 × M + lnDZr, zircon/melt) (Watson and Harrison, 1983), where DZr, zircon/melt is the ratio of Zr concentrations (ppm) in zircon to that in the saturated melt, M = cation ratio (Na + K + 2 × Ca)/(Al × Si). The geothermometer is
calibrated for M = 0.9 to 1.7.

215
216 L.-C. Huang, S.-Y. Jiang / Lithos 202–203 (2014) 207–226

more than that from G2 and G3 (0–0.02 wt%). Both feldspars in granites
G1–G4 are P-free (0–0.24 wt% of P2O5, Fig. 10).

5. Discussion

5.1. Petrogenesis of the Dahutang granites

5.1.1. Genitic type

Fig. 5. Q’-ANOR normative composition diagram (after Streckeisen and Le Maitre, 1979)
for classification of the Dahuatang granites, where Q’ = 100 × Q/(Q + Or + Ab + An)
and ANOR = 100 × An/(Or + An).
The Dahutang granites with characteristics of strongly peraluminous,
alkaline, P-enriched and Zr, Th, Y, HREE-poor are typical S-type rocks
(Champion and Bultitude, 2013; Chappell and White, 1992, 2001;
Clemens, 2003; Collins and Richards, 2008; Healy et al., 2004). These
granites exhibit strongly elevated concentrations of Li, Rb, Cs, Ta, Sn
and W; but of very low Ca, Ti, Mg, Sr, Ba, Hf and rare earth elements.
The highest tungsten values (up to 355 ppm) are found in granites
G1–G4 that contain accessory wolframite and scheelite (Fig. 3). G4
with tungsten values around 10 ppm is also found to contain accessory
wolframite. Che et al. (2013) attest the hypothesis that wolframite can

Fig. 6. Diagrams of chemical compositions of granites G1, G2, G3, and G4 from the Dahutang area. The 1/TiO2-parameter is the most robust indicator of the fractionation paths of granitic melts.
 L.-C. Huang, S.-Y. Jiang / Lithos 202–203 (2014) 207–226 217

Fig. 7. Chondrite-normalized REE patterns (a, c, e, and g normalization values are from Boynton, 1984) and primitive mantle-normalized trace element patterns (b, d, f, and h normalized
values are from McDonough and Sun, 1995) for the Dahutang granites (a, b for G1. c, d for G2. e, f for G3. g, h for G4).

occur as a magmatic mineral. Wolframite has also been found in Li-mica
granite in Variscan Erzgebirge (Förster et al., 1999), Podlesi pegmatite
(Breiter et al., 1997) and residual melt inclusions from Ehrenfriedersdorf
(Webster et al., 1997). In addition to the above features, these granites
are relatively poor in biotite and contain primary muscovite (Table 1
and Supplemental electronic data Table 4) (Miller et al., 1981; Monier
et al., 1984). These S-type granites belong to muscovite-bearing granit-
oids (MPG-type), usually resulting from ‘wet’ anatexis of crustal rocks
(Barbarin, 1996, 1999). Zircon saturation temperatures (TZr) could
represent the temperature of early stage of magma evolution (Ferreira
et al., 2003). In this case, the lower limits of calculated zircon saturation
temperatures (TZr) (Table 3) are of 750 °C, 693 °C, 735 °C and 679 °C as
the maximum temperatures of magma for G1, G2, G3 and G4, because
there are rare inherited zircons. Therefore, it seems that the muscovite-
bearing Dahutang granites formed under a high water activity and low
magmatic temperature environment. The Tzr is higher for G1 than for
G2, G3 and G4, indicating a higher degree of partial melting for G1
(Miller et al., 2003).
G1–G4 have high 10,000*Ga/Al ratios (most values range from 3.25
to 4.46) analogous to the characteristic of typical A-type granites.
Whalen et al. (1987) noted that highly fractionated felsic I- and S-type
granites can have major and trace element compositions overlapping
those of typical A-type granites. Previous studies also have shown that
highly differentiated I-type granites and some S-type granites in the
Lachlan Fold Belt display overlapping compositions (Chappell and
White, 1992; Chappell et al., 2012). Clearly, the four granites are highly
fractionated S-type tungsten-rich granites, tending to show major
element and mineral compositions converging to haplogranitic compo-
sitions (King et al., 1997). The highly fractionated property of these
granites can also be reflected in the indicators of differentiation,
218 L.-C. Huang, S.-Y. Jiang / Lithos 202–203 (2014) 207–226

Table 4
Nd and Sr isotopic compositions of the Dahutang granites.
147
Sample/NO. Rock type Sm Nd Sm/144Nd 143
Nd/144Nd 2σ εNd εNd TCDM Rb Sr 87
Rb/86Sr 87
Sr/86Sr 2σ (87Sr/86Sr)i
(ppm) (ppm) (0) (t) (Ma) (ppm) (ppm)

81#-12 G1 4.43 20.0 0.134 0.512174 0.000003 −9.05 −7.89 1578 804 40.3 57.8 0.805423 0.000020 0.689458
ZK0-26-1 G1 4.94 20.6 0.145 0.512202 0.000007 −8.51 −7.55 1550 616 24.9 71.6 0.828931 0.000017 0.685182
ZK0-26-2 G1 5.46 23.5 0.140 0.512190 0.000004 −8.74 −7.71 1563 571 21.7 76.1 0.832992 0.000021 0.680113
ZK0-26-3 G1 5.00 20.9 0.144 0.512190 0.000008 −8.74 −7.78 1569 707 36.7 55.8 0.801814 0.000047 0.689803
ZK108-2-1 G2 1.34 3.85 0.210 0.512170 0.000014 −9.13 −9.37 1689 532 14.3 108 0.905059 0.000026 0.703522
ZK108-2-2 G2 1.88 6.53 0.174 0.512183 0.000006 −8.88 −8.49 1618 621 15.3 118 0.901788 0.000046 0.682258
ZK108-2-4 G2 2.07 7.15 0.175 0.512227 0.000010 −8.02 −7.65 1550 730 27.4 77.2 0.932722 0.000438 0.788563
ZK11-2-12 G2 2.19 9.38 0.141 0.512140 0.000008 −9.71 −8.77 1641 790 48.2 47.4 0.802112 0.000026 0.713491
ZK11-5-25 G2 3.77 17.2 0.133 0.512206 0.000004 −8.43 −7.33 1524 618 39.0 45.9 0.793049 0.000013 0.707250
ZK11-5-27 G2 4.15 19.4 0.129 0.512218 0.000004 −8.19 −7.04 1501 653 33.5 56.4 0.799105 0.000019 0.693667
ZK-1-4 G3 4.58 17.9 0.155 0.512231 0.000008 −7.94 −7.25 1514 472 46.1 29.6 0.768154 0.000015 0.714454
ZK-1-5 G3 4.31 16.8 0.155 0.512299 0.000015 −6.61 −5.92 1406 458 55.6 23.8 0.760997 0.000011 0.717804
ZK-1-6 G3 4.51 17.4 0.156 0.512251 0.000010 −7.55 −6.88 1484 488 41.7 33.8 0.773064 0.000006 0.711710
ZK-1-9 G3 4.32 17.0 0.154 0.512233 0.000004 −7.90 −7.19 1510 457 55.3 23.9 0.770447 0.000012 0.727041
ZK-1-10 G3 4.57 17.6 0.157 0.512231 0.000006 −7.94 −7.28 1517 473 46.2 29.7 0.766922 0.000010 0.713132
ZK-1-11 G3 3.74 14.4 0.157 0.512240 0.000007 −7.76 −7.11 1503 447 42.0 30.9 0.76946 0.000013 0.713526
ZK-1-13 G3 3.75 14.4 0.158 0.512220 0.000004 −8.15 −7.51 1536 499 65.2 22.2 0.760324 0.000006 0.720166
81#-23 G4 1.60 6.67 0.145 0.512214 0.000005 −8.27 −7.42 1528 473 29.7 46.0 0.792343 0.000018 0.708934
81#-24 G4 2.34 9.34 0.152 0.512203 0.000007 −8.49 −7.74 1554 575 39.9 41.7 0.793233 0.000067 0.717718
81#-25 G4 1.66 7.05 0.142 0.512220 0.000006 −8.15 −7.25 1514 387 29.7 37.7 0.785084 0.000011 0.716685
81#-26 G4 2.46 11.2 0.133 0.512240 0.000005 −7.76 −6.71 1470 519 49.9 30.1 0.778592 0.000027 0.724015

Fig. 8. Histogram of εHf(t) values and Hf model ages (TCDM) of G1 (a, b), G2 (c, d), G3 (e, f) and G4 (g, h).
 L.-C. Huang, S.-Y. Jiang / Lithos 202–203 (2014) 207–226
Fig. 9. Evolution of chemical compositions of micas during fractionation of the Dahutang
granites. (a) Relations between FeO (total) and SiO2 in biotite. (b) Relations between
Al2O3 and SiO2 in biotite. (c) Relations between F and FeO (total) in biotite and primary
muscovite.
considered as Rb/Sr ratio (8–41), Zr/Hf ratio (19–28) and U/Th ratio
(0.6–5.8), and shown in the variation diagrams (Fig. 6). Strong correla-
tions between some major and trace elements vs. 1/TiO2 exist on two
distinct curvilinear trends defined by: a) granite G1; b) granite G2, G3
Fig. 10. The whole-rock CaO/P2O5 plot of the Dahutang granites (after Breiter, 2012). At
excess of Ca, in S-type magmas oligoclase crystallized at the same time as apatite; at excess
of P, apatite crystallized together with P-bearing alkali feldspars. In the granites G1–G4,
apatite is abundant and feldspars are P-free.
219
and G4, suggesting significant fractionations during two different
magmas evolutions (Fig. 6).
5.1.2. Origin
It is generally accepted that strongly peraluminous (S-type) granites
are derived largely by partial melting of metasedimentary protoliths
(Jiang et al., 2011; Koester et al., 2002). The aluminum enrichment in
magma can be generated by three processes: fractional crystallization
of amphibole, despite source rocks not being saturated in Al (Chappell
et al., 2012; Zen, 1986); partial melting of basaltic to andesitic rocks
under crustal conditions (Ellis and Thompson, 1986); and partial melting
of aluminium-rich metasedimentary rocks (e.g., schists and phyllites)
(Nabelek and Glascock, 1995; Sylvester, 1998). However, the magma
produced by the first two processes are usually weakly peraluminous
or metaluminous, and tend to have high Sr abundances (Gaudemer
et al., 1988; Zen, 1986), which are contrary to our observations. The
Dahutang granites are strongly peraluminous (S-type) granites with
low Sr abundances from 14.3 to 65.2 ppm (Table 3). Thus, the magma
that produced the four types of granites was most likely derived from
aluminium rich metasedimentary protoliths in the crust. This is supported
by high Rb contents, suggesting sources rich in mica (Liu et al., 1984).
Experiments show that strongly peraluminous granites will inherit
different CaO/Na2O ratios by partial melting of different source compo-
sitions: metapelite-derived S-type granite melts tend to have lower
CaO/Na2O ratios (b 0.3) than metapsammite-derived S-type granite
melts (Jung and Pfänder, 2007; Sylvester, 1998). The four granite types
at Dahutang have lower CaO/Na2O (b 0.3) and higher Rb/Ba, typical of
pelitic-rich sources. Thus, they show the typical features of a metapelite-
derived peraluminous granite melt (Fig. 11). Pelitic-rich sediments tend
to have smaller quantities of detrital zircons than coarse clastic sedimen-
tary rocks (Patchett et al., 1984). The low Zr contents of the studied
granites further support the notion that they were likely derived from
an pelitic source.
The Nd isotopic composition of the Shuangqiaoshan Group meta-
sediments (including slates, phyllites, tuffs and greywackes) was
defined by previous studies (Chen and Jahn, 1998; Li, 1996; Ling et al.,
1992; Ma and Xiang, 1993; Zhang et al., 2000). Notably, the Nd isotopic
data (mostly from −8.77 to −6.71) for the Dahutang granites lie within
the range of Nd isotopic evolution envelop of the Shuangqiaoshan
Group rocks, but they are more radiogenic than those of the Proterozoic
crust in South China (Fig. 12a). The low εHf(t) and εNd(t) values in
Fig. 12b indicate that the granite samples have compositions close to
the field of global sediments. The whole rock Nd isotopic compositions
of the four types of granites show a relatively narrow range (with few
exceptions). The initial Hf isotopic values of zircon grains of the
Dahutang granites vary from −8.44 to −2.13, showing nearly normal
distributions with distribution peaks of εHf(t) (Fig. 8a, c, e, g). Although
the εNd(t) values of G1–G4 are in the same range, the peak values of
εHf(t) (− 5 to − 3) in the granites G2–G4 are higher than the peak
values of εHf(t) (−6 to −5) in granite G1. Lu–Hf isotope data from sin-
gle zircons can give a more precise identification of continental crustal
evolution than Sm–Nd isotopic data of a whole rock (Hawkesworth
and Kemp, 2006; Teixeira et al., 2011). The εHf(t) can be more effective
to indicate the differences in the source region of the four granites than
the εNd(t) values. Seemingly, granite G1 has more evolved upper crustal
source than G2, G3 and G4. The absence of published Hf isotope data
for the Shuangqiaoshan Group metasedimentary rocks precludes a
direct comparison with our data. Hafnium model ages of zircons (TCDM)
in G2–G4 are mainly distributed in the range between 1350 Ma and
1450 Ma, slightly younger than that of G1 between 1500 Ma and
1550 Ma (Fig. 8b, d, f, h). Most Nd model ages (TCDM) overlap with the
range of Hf model ages indicating that the sources of the granites
were likely derived from late Mesoproterozoic depleted mantle.
The four types of Dahutang granites show relatively consistent
Nd and Hf isotopic compositions and likely have been formed by
partial melting of pelitic rocks from Shuangqiaoshan Group. This
220 L.-C. Huang, S.-Y. Jiang / Lithos 202–203 (2014) 207–226
Fig. 11. Rb/Sr vs. CaO/Na2O and Rb/Ba ratios for the Dahutang granites (after Sylvester,
1998).
conclusion is supported by abundant inherited zircons recorded in the
early Neoproterozoic ages (around 824 Ma) (Supplemental electronic
data Table 1), which are regarded as the time of deposition of the
Shuangqiaoshan Group (Gao et al., 2008, 2012). Compared with the
Nd isotope data (mostly from − 8.77 to − 6.71) for G1–G4 (Table 4),
Variscan S-type W-rich or Sn + W-rich granites, such as S-type granite
of the older intrusive complex granites (OIC-S) and Li-mica granites in
the Erzgebirge and the two-mica granites from the Carrazeda de Ansiães
area in the Central Iberian Zone, separately exist εNd(t) values as −1.8
to − 5.2 (t = 325 Ma) (Breiter, 2012), − 4.5 to − 7.4 (t = 320 Ma)
(Förster et al., 1999) and − 6.2 to − 9.1 (t = 319–330 Ma) (Teixeira
et al., 2012). OIC-S granites and Li-mica granites have more primitive
isotopic characteristics than the Dahutang granites. The Nd isotope
data of the two-mica granites have a similar range as our data. The
protolith of these granites in the Erzgebirge is considered as a mixture
of fertile quartzo-feldspathic rocks (orthogneisses) with micaceous
metapelites (Breiter, 2012; Förster et al., 1999). However, the Dahutang
granitic rocks and two-mica granites from the Carrazeda de Ansiães
area correspond to magmas completely formed by partial melting of
metasedimentary materials (Table 4; Fig. 12a; Teixeira et al., 2012),
thus having lower εNd(t) values. The initial εHf in magmatic zircons of
S-type granites from the Spanish Central System (SCS) in the European
Variscan Belt and the Carrazeda de Ansiães areas of the Iberian Variscan
Belt are separately in the ranges of −6 to −2 (Villaseca et al., 2012) and
−8 to −4 (Teixeira et al., 2011). The initial Hf isotopic values of zircon
grains of the Dahutang granites vary from −8 to −2 (Fig. 8; Table 2),
less radiogenic than that of S-type granites from the SCS but showing a
larger variation than that of S-type granites in the two regions. Probably,
the Dahutang granites showing a larger variation of εHf(t) values
Fig. 12. (a) Evolution of εNd(t) (from bulk rock Nd isotopic composition). Data of Nd
isotopic compositions of Shuangqiaoshan Group are cited from previous researchers
(Chen and Jahn, 1998; Li, 1996; Ling et al., 1992; Ma and Xiang, 1993; Zhang et al.,
2000). The εNd isotopic evolution envelop of Proterozoic crust in South China has been
determined by Wang et al. (1994). (b) Whole-rock εNd vs. zircon εHf diagram for the
Dahutang granites. Also shown are the fields for MORB, OIB and Global sediments
(Vervoort and Blichert-Toft, 1999).
were derived from magmas formed by many distinct pulses of partial
melting of heterogeneous metasedimentary materials, predominantly
in metapelite from the Shuangqiaoshan Group.
Granites G1 and G2, G3 and G4 have some similar geochemical char-
acteristics as described above, including all the εNd(t) values in the same
range. Granites G2, G3 and G4 that are pretty close in the emplacement
age show the closest Nd and Hf isotopic compositions (Table 4; Table 2;
Fig. 7) and the same evolved trends in the variation diagrams (Fig. 6),
which define a homogenous magmatic differentiation ruled by fractional
crystallization. However, the major and trace elements variation and
different peak values of εHf(t) suggest that G1 and G2–G4 correspond
to distinct origin materials (Figs. 6; 8). This is confirmed by the higher
content of REE (Fig. 7), higher TZr in G1, higher content of FeO (total)
and Al2O3 in biotite and P2O5 in K-feldspar and plagioclase of G1, com-
pared with the other three types of granites (Fig. 9a, b; Supplemental
electronic data Tables 5 and 6). In addition, G1 is more than 10 Myr.
older than G2, G3 and G4. The high Cs content in granite indicates
that the derivation of magmas from a source has not experienced a pre-
vious episode of melting, because the highly incompatible Cs would
have been lost (London, 1995). Thus, granites G1, G2, G3 and G4 with
extremely high Cs contents (55–421 ppm) (Table 3) rule out these
magmas sequential partial melting from the same crustal source. There-
fore, the two episodes of granitic magmas were likely derived from the
different protoliths which have analogous components. In the late
episode, the magmas of G2, G3 and G4 were likely derived from the
same magmatic chamber.
5.2. Geodynamic implication
The Jiangnan Orogen is located between the Middle-Lower Yangtze
Valley Mineralization Belt and the Shi-Hang Belt (Fig. 1a). The
 L.-C. Huang, S.-Y. Jiang / Lithos 202–203 (2014) 207–226
geochronology of the Dahutang granites indicates that magmatic
activity in the region lasted from 144 Ma to 130 Ma. The formation of
S-type granites in Dahutang area occurred later than the intrusion
of I-type granites of the nearby Jiurui district (148–142 Ma) in the
Middle-Lower Yangtze Valley Mineralization Belt (Fig. 1a; Ding et al.,
2006; Li et al., 2010; Yang et al., 2011), and slightly earlier than the
A-type granites of Xiangshan district (137–135 Ma) in the Gan-Hang
Belt (Yang et al., 2010a,b, 2012). These S-type granites belong to
MPG-type granites which were affected mainly by major crustal shear
or overthrust structures in orogenic zones during continental collision,
as demonstrated by Barbarin (1996). However, it seems unlikely that
the Jiangnan Orogen was in a continental collisional setting during
the Early Cretaceous because regional deformation corresponded
to northwestward compression that only occurred during the Early
and Middle Jurassic in the area (Wang et al., 2012a,b), or even
continued until 155 Ma (Zhu and Liu, 2000). In the Early Cretaceous,
Basin and Range Province had been formed in southeastern
China (Gilder et al., 1991). A-type granitic and within-plate basaltic
magmatism from 140 to 90 Ma suggests a dominant extensional envi-
ronment in the region (Huang and Jiang, 2012; Jiang et al., 2011; Li,
2000; Yang et al., 2012). In addition, the Yanshanian granites in the Jiurui
district and in the Xiangshan area were considered to be associated with
an extensional regime, lithosphere thinning and asthenosphere upwell-
ing since the Early Cretaceous (Li et al., 2010, 2013; Wu et al., 2012; Xie
et al., 2012a,b; Xu et al., 2002; Zhou and Li, 2000; Zhou et al., 2006).
Therefore, the Dahutang granites likely also formed within this general
extensional tectonic regime taking into account their ages. The Jiangnan
Orogen contained several kilometers thick wedges of Proterozoic
metasedimentary rocks, which have been affected by post-orogenic
crustal and lithosphere thinning and asthenospheric upwelling that con-
tributed for the partial melting of upper crustal sedimentary rocks
(Huang et al., 2003).
The Late Mesozoic lithospheric extension in Middle-Lower Yangtze
Valley Mineralization Belt was previously considered to be related to
lower-crustal delamination of thickened crust (Q. Wang et al., 2007a,
b; Xu et al., 2002), or a slab window formed by ridge subduction (Ling
et al., 2009; Sun et al., 2007). The southeastern ward roll-back of the
Palaeo-Pacific plate was invoked for explaining back-arc extension in
Gan-Hang Belt (Jiang et al., 2011). Other models like oblique subduction
of the Paleo-Pacific Ocean (Wang et al., 2011) or rollback and delamina-
tion of the subducted Paleo-Pacific slab (Li and Li, 2007; Wong et al.,
2009) also have been proposed to interpret Cretaceous lithosphere ex-
tension in SE China. Based on decreasing ages of granitic magmatism
from Jiurui to Xiangshan districts and evidence for a Late Cretaceous
(92–97 Ma) extension episode in the coastal area of SE China (Lapierre
et al., 1997; Qiu et al., 2004), it seems likely that the regional extension
gradually migrated from east towards the coastal area.
5.3. Fractionation process
The two episodes of granites G1 and G2, G3 and G4 were derived
from partial melting of the different protoliths which have analogous
components in the Shuangqiaoshan Group (as discussed in 5.1.2). The
metasedimentary rocks in Shuangqiaoshan Group contain higher
∑REE contents (171 to 365 ppm) than granites G1–G4 (24–124 ppm).
The metasedimentary rocks have much lower Rb/Sr (0.25 to 2.67) and
(La/Yb)N (0.03 to 1.40) ratios than granites G1–G4 (Rb/Sr ~8 to 41 and
(La/Yb)N ~ 5.3 to 18.3), according to data from Zhang et al. (2000). In
addition, Primitive Archean Australian shale-normalized REE patterns
of these metasedimentary rocks exhibited positive Eu anomalies and
LREE substantially equal to HREE (Zhang et al., 2010). The Dahutang
granites, with strongly elevated concentrations of Li, Rb, Cs and Ta, but
very low Ti, Mg, Sr, Ba, Hf and rare earth elements, show no evidence
of a “geochemical signature” inherited from the source materials.
Therefore, the variations in trace elements of the Dahutang granites
221
are the results of differentiation processes ruled by fractional crystalli-
zation mechanisms.
Marked negative Eu anomalies (Fig. 7a, c, e, g) and depletion of Sr
(Fig. 7b, d, f, h) in these granites require partial melting of source
rocks within the stability field of plagioclase, rather than garnet as a
residual phase resulting in positive Eu anomaly. Therefore, the decrease
in the MREE and HREE of the granites G1–G4 (Fig. 7a, c, e, g) may have
been dominantly affected by apatite and zircon fractionation (Bea,
1996; Henderson, 1984). However, in strongly peraluminous melts,
apatite has an increased solubility (Cuney and Friedrich, 1987; Montel
et al., 1988), while zircon has significantly reduced solubility (Cuney
and Friedrich, 1987; Montel, 1986; Montel et al., 1988; Rapp et al.,
1987; Watson and Harrison, 1984). Then, the influence of apatite frac-
tionation on the decrease in the MREE can be reduced, whereas the
zircon fractionation can strengthen the decrease in the HREE. The total
contents of REE (24–124 ppm) of the Dahutang granites are lower
than those of source rocks within the Shuangqiaoshan Group, maybe
due to fractionation of accessory minerals such as monazite, apatite
and zircon, and/or mobilization of REE through complex Cl-REE and
F-REE in late post-magmatic fluids (Irber, 1999; Taylor et al., 1981).
Granites G2, G3 and G4 seem to define a magmatic differentiation
series as G3 grades into G4 and finally into G2 and their ages are roughly
identical at 130–134 Ma (Fig. 4b, c, d). Granite G1 can be considered as
an independent pulse within its age at 144 Ma (Fig. 4). Granites G1 and
G2, G3 and G4 define different curvilinear trends in major and trace
elements diagrams (Fig. 6), and show fractionation trends for biotite
and muscovite (Fig. 9a, b, c) and subparallel whole rock REE patterns
within each series (Fig. 7). In the series b, the decrease in LREE from
G3 to G4 and finally to G2 can be explained by fractionation of monazite
(Bea, 1996), while the decrease in the MREE can be due to apatite
fractionation (Henderson, 1984), and the decrease in HREE to zircon
fractionation (Bea, 1996). The fact that LREE decreases greater than
HREE in the series b can be explained by higher degrees of monazite
fractionation than those of zircon fractionation.
In log–log diagrams of Ba vs. Eu, Sr vs. Eu, Ba vs. Sr and (La/Yb)N vs. La
(Fig. 13), the sample ZK1-13 from granite G3 may even be close to the
initial composition of the magma. Element variations indicate that
plagioclase and K-feldspar fractionation is also required after partial
melting of G1–G4 (Fig. 13a, b, c). The fractionation of plagioclase can
result in negative Sr and Eu anomalies and the fractionation of
K-feldspar leads to negative Ba and Eu anomalies (Fig. 7). In addition,
the high Rb/Sr ratios of these granites also indicate high degrees of
fractionation of plagioclase (EI Bouseilly and EI Sokkary, 1975). A
more extensive feldspar and accessory mineral fractionation is detected
in G2, while the fractional crystallization of G3 is not obvious and a
moderate degree of fractional crystallization of G4 is between G2 and
G3 (Fig. 13). The crystal fractionation of zircon in G1 and apatite, allanite
and/or monazite in G2, G3 and G4 controls the variation in La and Yb
contents (Fig. 13d). The granite G2 seems to be controlled by higher
and variable degrees fractionation of allanite and/or monazite (Fig. 13d),
resulting in a wider range in the LREE pattern of G2 (Fig. 7c). The samples
of G3 have analogous degrees of crystal fractionation of feldspar,
apatite, allanite and/or monazite (Fig. 13), originating a very narrow
variation of the pattern in Fig. 7e, f. In addition, the negative Ti anoma-
lies of the Dahutang granites (Fig. 7) may indicate the fractionation of
Fe–Ti oxides (ilmenite) and/or fractionation of micas occurred in
magma evolution.
5.4. Concentration and transportation of tungsten and its relationship with
the granites
The Dahutang tungsten deposit has been estimated as one of the
world’s largest tungsten deposits. Feng et al. (2012) reported Re–Os
isochron ages of molybdenite of 143.7 ± 1.2 Ma and 140.9 ± 3.6 Ma
for this deposit. Similar Re–Os model ages (138.4 Ma to 143.8 Ma)
were also obtained for molybdenite by Mao et al. (2013). These data
222 L.-C. Huang, S.-Y. Jiang / Lithos 202–203 (2014) 207–226

Fig. 13. (a) Ba vs. Eu, (b) Sr vs. Eu, (c) Ba vs. Sr diagrams, showing that fractionation process of feldspar plays an important role in the formation of the Dahutang granites. Partition
coefficients of Ba and Sr are from Philpotts and Schnetzler (1970), and Eu is from Arth (1976). (d) (La/Yb)N vs. La diagram, showing the change of REE patterns by separation of accessory
minerals. Partition coefficients are from Fujimaki (1986) for apatite, Mahood and Hildreth (1983) for zircon and allanite, and Yurimoto et al. (1990) for monazite. Pl: plagioclase; Kf:
K-feldspar; Bt: biotite; Aln: allanite; Mnz: monazite; Ap: apatite; Zrn: zircon.

are consistent with a zircon 206Pb/238U age from granite G1 of 144.0 ±
0.6 Ma. Field observations and the ages of granite G1 and tungsten ore
bodies clearly indicate that they are spatially and temporally associated
with each other. The ages of G2–G4 granites are 133.7 ± 0.5 to 130.3 ±
1.1 Ma. Seemingly, these intrusions occurred after the W-mineralization.
However, G1 and G2–G4 granites have unusually high tungsten con-
tents, typically several tens of ppm, but sometimes as high as several
hundreds of ppm (Table 3). These tungsten contents are much higher
than average upper crustal and lower crustal values (1.9 ppm and
0.6 ppm, respectively) (Rudnick and Gao, 2004). The question that
arises is why these highly fractionated S-type granites contain so
much more tungsten than normal crust, but only granite G1 has a
genetic relationship with the tungsten mineralization.
Metapelite-derived magma that underwent a process of fractional
crystallization can be connected with tungsten-rich zones (Breiter,
2012; Fogliata et al., 2012; Teixeira et al., 2012; Xu and Chen, 1987). In
fact, Breiter (2012) argued that some micaceous metapelites are
enriched in LILE, Sn and W. Tungsten concentration data on metapelitic
rocks within the Shuangqiaoshan Group indicate high abundances (up
to 12 ppm), much higher than tungsten contents of typical crustal
rocks, which are in the 1–2 ppm range (Rudnick and Gao, 2004).
These tungsten-rich metasediments are the most likely source of the
tungsten in the granites and related ore deposits.
Tungsten is a strongly incompatible lithophile element with strong
enrichment in the crust compared to the mantle (Ertel et al., 1996).
Partial melting in the presence of favorable complexing agents can
lead to additional enrichment of such metals (Liu et al., 1994). In addi-
tion, fractional crystallization would have led to further enrichment of
W–Sn in the magma (Fogliata et al., 2012; Teixeira et al., 2012). This
differentiation process has been described for granites of the Jalama
batholith, Portugal (Ruiz et al., 2008), in northern and central Portugal
S-type granitic rocks (Neiva, 2002), and in some granites of Krušné
hory/Erzgebirge Mountains, Central Europe (Breiter, 2012). However,
the mechanism controlling the degree of concentration of tungsten
during fractional crystallization process is different from that of tin.
The valence state of tin is controlled by the oxygen fugacity of the
magma and it can be concentrated in the residual melt or be removed
in the crystallizing phases depending on its valence state as Sn2 + or
Sn4+ (Cobbing et al., 1986; Linnen et al., 1996; Zhao et al., 2005). Tung-
sten dissolves predominantly as W6 + at all oxygen fugacities above
IW-3.6 (the iron-wüstite [IW] buffer) in silicate magma (Wade et al.,
2013). A possible contribution from W4+ may be only at the very lowest
oxygen fugacity accessible to the experimental method in melt (Che
et al., 2013; O'Neill et al., 2008; Wade et al., 2013). As shown in the
Fe3+-Fe2+-Mg diagram (Fig. 14), the oxygen fugacities of G3 and G2
estimated by the biotite compositions are above Ni-NiO (NNO) buffer,
that of G4 is between NNO and QFM buffers, and that of G1 is below
the Fe2SiO4-SiO2-Fe3O4 (QFM) buffer. The granite G1 crytallized under
lower oxygen fugacity condition than granites G2 to G4. Hence the pre-
dominant valence state of tungsten in the four types of granitic magmas
is likely to be hexavalent, independent of oxygen fugacity over a log ƒO2
range of above the IW-3.6 buffer.
In an early stage of granitic magma evolution, tungsten is compatible
in rutile included in accessory minerals, whereas in a late stage it is
associated with the rock-forming minerals, like micas (Linnen and
Cuney, 2005) and accessory wolframite and scheelite (Che et al., 2013;
Fig. 3). Liu et al. (1984) considered the tungsten content in muscovite
and rutile is up to 96 ppm and 2000 ppm, respectively. Breiter et al.
 L.-C. Huang, S.-Y. Jiang / Lithos 202–203 (2014) 207–226
Fig. 14. The oxygen fugacity of the Dahutang granites estimated by biotite compositions
(after Wones and Eugster, 1965).
(2007) reported tungsten contents up to 3.6 wt% WO3 in rutile from
peraluminous granites. In the early stages of crystallization, W6+ can
substitute Ti4+, accompanied by a double substitution of Fe to maintain
charge balance (Rice et al., 1998), which will bring large quantities of
W6+ into rutile, thus giving rise to a relatively low tungsten concentration
in later crystallization stages. However, granites usually contain ilmenite
or titanomagnetite rather than rutile as the main accessory Ti-bearing
mineral (Haggerty, 1976). Rutile appears to be stable only in highly
fractionated granites that are impoverished in Mg and Fe content and
approach haplogranitic composition (Keppler, 1993). Granites G1–G4
contain 0.79–1.5 wt% Fe2O3t and 0.21–0.37 wt% MgO in the normal
range of MgO-, Fe2O3t-content of low calcium granitic rocks (Turekian
and Wedepohl, 1961). Therefore, rutile may be not the early mineral
phase in the four granitic melts. However, fractional crystallization pro-
cesses could rise up substantially the tungsten accumulated in the resid-
ual melts. On the other hand, the experiments performed by Mengason
et al. (2011) have shown that: (i) the partition coefficients of tungsten
among silicate melt and sulfur phases will not vary significantly with
changes in the fugacities of oxygen and sulfur; (ii) sulfur phases addi-
tion or removal is not expected to exert a significant influence on the
tungsten budget of magma (Mengason et al., 2011; Sun et al., 2004).
On the other hand, many studies of geological field relations, fluid
inclusions and isotopic geochemistry have shown that the magma can
be concentrated in mineral deposits within the magmatic hydrothermal
paradigm (Candela and Bouton, 1990; Ishihara, 1977; Linnen and
Cuney, 2005; Maulana et al., 2013). The tungsten mineralizations are
generally associated to reduced granitic magmas that typically belong
to ilmenite series (Ishihara, 1977), such as those of Ryoke metamorphic
belt in Japan (Sato, 1980), granitic rocks from Sulawesi, Indonesia
(Maulana et al., 2013), and Leinster granite batholith in SE Ireland
(Gallagher, 1989). During the late stages of magmatic evolution the
oxygen fugacity can exert a control on the relative efficiencies of removal
of tungsten from magma into hydrothermal ore-forming fluids. This
view has been demonstrated by the experiments of tungsten in fluid/
mineral partition coefficients (Bali et al., 2012; Candela and Bouton,
1990), which have shown that low oxygen fugacity conditions can pro-
mote the accumulation of tungsten in the hydrothermal fluids. Further-
more, Ague and Brimhall (1988) also found conditions of formation of
tungsten-rich deposits with the oxygen fugacity below QFM buffer.
The studied G1 granite is the only one type with oxygen fugacity
below QFM buffer; the other three types of G2 to G4 granites have a
higher oxygen fugacity than G1 (Fig. 14). The lower oxygen fugacity of
granite G1 provides a possibility to remove substantial tungsten from
magma to the hydrothermal fluids. Taking into account the geological
field relations between granite G1 and the tungsten ore bodies and
the coincident, the G1 granitic magma may be the source of ore mate-
rials in the Dahutang tungsten deposit. The granites G2 to G4 have a
higher oxygen fugacity leading to retain tungsten in rock-forming min-
erals (such as micas) in the late stages of evolution of granitic magma,
and their relationship with tungsten mineralization in the district
needs further inversitigation. Granites G1 to G4 derived from the partial
melting of tungsten-rich metasedimentary rocks of the Shuangqiaoshan
Group and underwent the processes of highly fractional crystallization,
223
leading to the very high W contents in these granites. Although the
tungsten in granite G1 had been removed for mineralization, it still
has a high content of tungsten as 28–102 ppm.
6. Conclusions
Results of this work indicate that granites G1, G2, G3 and G4
from the Dahutang area are silica-rich, strongly peraluminous S-type
granites, formed by ‘wet’ anatexis at low formation temperatures. The
granites have high contents of alkali elements, high Ga/Al, relatively
low abundances of REE contents, low Ba, Sr, Zr contents and high Rb
contents. Geochemical and isotopic data suggest that these highly
fractionated S-type granites G1and G2–G4 were mainly originated
from two episodes of partial melting of different protoliths which
have analogous components of metamorphosed pelitic rocks from the
Neoproterozoic Shuangqiaoshan Group. Chondrite-normalized REE
patterns with negative Eu anomalies indicate partial melting of source
rocks within the stability field of plagioclase. In the primitive mantle
normalized variation diagrams, negative anomalies in Ba, Nb, Sr, Ti, Zr
and positive anomalies in Rb, U, Ta indicate that they have underwent
highly fractional crystallization of plagioclase, K-feldspar, monazite,
apatite and zircon. Two series can be distinguished: G1 and G2–G4.
The major and trace elements variation diagrams and the fractional
crystallization modeling of Sr, Eu and Ba show that the samples of G3
are close to the initial composition of the magma and G2 and G4 can be
derived from the G3 magma. In situ zircon U–Pb dating indicates that
magmatic activity took place in the early Cretaceous (130–144 Ma).
Multiple phases of intrusions extracted tungsten from tungsten-rich
protoliths. Fractional crystallization resulted in further enrichment of
tungsten. Therefore, granites G1–G4 all have high contents of tungsten.
However, at the present stage we only know that the granite G1 has a
close relationship with W-mineralization and this granite possesses a
lower oxygen fugacity below QFM. Its magma may be the source of
ore substance in the Dahutang tungsten deposit. The formation and
emplacement of the granites in the Dahutang area must be viewed in
the context of extensional tectonic processes in eastern China during
the Early Cretaceous. These processes resulted in lithosphere thinning, as-
thenospheric upwelling, and coeval partial melting of metasedimentary
rocks of the upper crust.
Supplementary data to this article can be found online at http://dx.
doi.org/10.1016/j.lithos.2014.05.030.
Acknowledgements
We are grateful to Dr. Karel Breiter and an anonymous reviewer for
the thoughtful reviews. Their constructive and stimulating comments
helped to significantly improve the manuscript. We thank the editor-
in-chief Nelson Eby and journal manager Rohini Shivaram for seasonable
feedbacking the information of status of review on our paper. We also
thank Dr. Wen-Lan Zhang, Ming-Lan Hou, and Pei-Jun Lin for the help
with electron microprobe analyses, Liang Li and Bin Wu with LA-ICP-
MS U–Pb dating, Li Liu with zircon CL image, An-Jun Lin and Shui-Yuan
Yang with LA-MC-ICP-MS Lu–Hf analyses, Gang Zeng with major
element analyses, Qian Liu with trace element analyses and Wei Pu
with Sr–Nd isotopic analyses. This work was supported by a Major State
Basic Research 973 Program of China (2012CB416706) and a project
from the China National Science Foundation (No. 41072055).
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