Zircon Geochronology, Geochemistry and Stable Isotopes of the Wangв

Journal of Asian Earth Sciences 113 (2015) 695–710

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Journal of Asian Earth Sciences

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Zircon geochronology, geochemistry and stable isotopes of the Wang’ershan gold deposit, Jiaodong Peninsula, China ⇑ Yu-Jie Li a,b, Sheng-Rong Li a,b, , M. Santosh b, Sheng-Ao Liu b, Long Zhang b,c, Wen-Tao Li b, Ying-Xin Song b, Bi-Xue Wang b a State Key Laboratory of Geological Processes and Mineral Resources, China University of Geosciences, Beijing 100083, China b School of Earth Science and Resources, China University of Geosciences, Xueyuan Road, Haidian District, Beijing 100083, China c The 1th Gold Detachment of Chinese Armed Police Force, China article info abstract

Article history: The Early Cretaceous gold deposits of the Jiaodong Peninsula, eastern China, define China’s largest gold Received 11 December 2014 province with an overall endowment estimated more than 3000 t Au. The Wang’ershan gold deposit at Received in revised form 8 March 2015 the northern margin of the Jiaolai Basin in Jiaodong Peninsula of eastern China is located in the cen- Accepted 23 March 2015 tral-southern segment of the Wang’ershan fault zone. The major Mesozoic intrusions exposed in this Available online 30 March 2015 region are the Linglong granite and the Guojialing granodiorite to the northeast of the deposit. Both these intrusions show high-K and alkaline signature. The Linglong granite displays peraluminous feature Keywords: whereas the Guojialing granodiorite is metaluminous. Zircon U–Pb dating of the Linglong granite yields Zircon geochronology 206Pb/238U weighted mean age of 149.0 ± 1.3 Ma. The muscovite from the alteration zones associated with Stable isotopes Geochemistry mineralization in the Linglong granite yields a plateau age of 130.35 ± 0.96 Ma, representing the initial 34 Wang’ershan gold deposit phase of the hydrothermal activity. The d S values of pyrite from the gold mineralized veins range from 3 4 Jiaodong Peninsula 6‰ to 8.3‰ with the mean value of 7.66‰. The He/ He ratios of pyrite are in the range 1.58–2.71 Ra with a mean value at 2.168 Ra. The 40Ar/36Ar ratios show variation from 1220.3 to 1625.7 with an average of 1483.8. The d18O values of the mineralizing fluids show a range of 2.13‰ to 7.5‰, with an average of 18 2.4‰. The d Dw values are in the range of 97.5‰ to 61.4‰, with a mean at 82.6‰. Detailed elemental and isotopic data suggest that the hydrothermal fluids in early stage were mainly magmatic and derived from the Guojialing granodiorite, and the ore-forming fluids in the main ore-forming stages evolved into a mixture of magmatic and meteoric water. The ore-forming materials were primarily derived from crust, with minor input of mantle components. The ore-forming fluids might be related to the subduction of the paleo-Pacific slab beneath the North China Craton and the associated asthenosphere upwelling and consequent lithospheric thinning. Ó 2015 Elsevier Ltd. All rights reserved.

1. Introduction 2015). Some well-known type gold deposits, such as the Jiaojia- type and Linglong-type gold deposits, are named after this region The Jiaodong Peninsula currently ranks as the most important (Yang et al., 2006; Song et al., 2012; Li et al., 2015). The gold depos- gold producer in China (Zhang et al., 2015). Covering an area of its are mostly hosted by the Linglong granite or in the neighboring about 0.2% of the whole country, the gold production in this region zones of the Guojialing granodiorite, and are strongly controlled by reaches nearly one fourth of the total gold production of China. The NE-trending fault zones (Liu, 1987; Qiu et al., 2002). The ores are Jiaodong gold province is now famous for its large-scale granitoid- composed of either alteration type with disseminations and veinlet hosted ‘‘Jiaodong-type’’ gold deposits both in China and elsewhere sulfide (Jiaojia-type) or massive quartz-sulfide veins (Linglong- (Goldfarb and Santosh, 2013; Li et al., 2015; Groves and Santosh, type). The gold deposits of both two styles in Jiaodong have been dated by both direct and indirect means with ages concentrated between 130 and 110 Ma (Luo and Wu, 1987; Zhang et al., 1994, ⇑ 2003; Lu and Kong, 1993; Sun et al., 1995; Yang, 2000; Yang and Corresponding author at: State Key Laboratory of Geological Processes and Zhou, 2000a,b, 2001; Li et al., 2003a,b, 2006, 2008; H.M. Li et al., Mineral Resources, China University of Geosciences, Beijing 100083, China. Tel.: +86 010 82321732. 2003). Several models have been proposed for the formation of E-mail address: [email protected] (S.-R. Li). these gold deposits based on structural setting, mineralization http://dx.doi.org/10.1016/j.jseaes.2015.03.036 1367-9120/Ó 2015 Elsevier Ltd. All rights reserved. 696 Y.-J. Li et al. / Journal of Asian Earth Sciences 113 (2015) 695–710 style, and ore-forming fluid geochemistry, some workers suggested The basement rocks, belonging to the Late Archean Jiaodong that these deposits belong to the orogenic gold type (e.g., Kerrich Group, are exposed in Hongbu-Zhuqiang, Cikou-Xinzhuang and et al., 2000; Zhou and Lu, 2000; Goldfarb et al., 2001, 2005; Qiu Yaojia and form the hanging wall of the major fault plane in et al., 2002). However, many others noted that the tectonic setting Jiaojia. The Jiaodong Group is mainly composed of biotite gneisses and genetic characteristics of the Jiaodong gold deposits are differ- and marble. SHRIMP U–Pb dating of the inherited zircons captured ent from those of typical orogenic gold deposits (e.g., Groves et al., by the Mesozoic plutons indicate ages of 3.0–3.4 Ga for the 1998; Li and Santosh, 2014; Li et al., 2015), and classified these Jiaodong Group rocks (Wang et al., 1998). Mesozoic magmatic deposits as a unique ‘‘Jiaodong type’’ (e.g., Zhai and Santosh, rocks are widely developed in the area and range in age from 2013; Goldfarb and Santosh, 2013; Li et al., 2015). Late Jurassic and Early Cretaceous (Sang and You, 1992; Yang The relationship between granitoids and gold deposits and the et al., 2012, 2014c). The Late Jurassic Linglong granite is the main sources of the ore-forming materials and fluids are important to intrusion in the study area. The Early Cretaceous magmatic rocks understand the genesis of the gold mineralization in this region. which intrude the Late Jurassic granitoids are mainly composed In this study, we present results from zircon geochronology, and of the Guojialing granodiorite. elemental and isotope geochemistry from the Wang’ershan gold The regional structural architecture is dominated by the NE- deposit in an attempt to evaluate the sources of the ore-forming trending faults including the Jiaojia main fault and several sub- materials and fluids. faults which mainly consist of Wangershan, Hexi, Houjia and Qiujia faults. These faults served as the main pathway for the ore-forming fluids, and controlled the distribution and formation 2. Geological setting and ore field geology of gold deposits.

2.1. Geological setting 2.2. Geological characteristics of the Wang’ershan gold deposit The Jiaodong Peninsula is located in the southeastern margin of the North China Craton, and is one of the potential regions for gold The Wang’ershan gold deposit, with a resource of about 50 t Au mineralization in China. The Jiaojia gold mineralization belt, is located along the central-southern part of the Wang’ershan fault Sanshandao gold mineralization belt and Zhaoping gold mineral- zone that is the secondary fault of the major Jiaojia fault. ization belt are located in the northern Jiaodong Peninsula Cataclasites are dominant locally on both sides of the (Fig. 1), which are bound by a NNE-trending fault (Qiu et al., Wang’ershan fault. In the region of the Wang’ershan gold deposit, 2002). Among these, the Jiaojia gold mineralization belt mainly the NNE-trending fault is the principal ore-controlling structure. controlled by the Jiaojia fault is composed of several large gold Exposed in the eastern oreﬁeld, the Precambrian metamorphic deposits such as the Jiaojia, Xincheng, Hexi and Wang’ershan. rocks which constitute the basement in the area are characterized

Fig. 1. Regional geological map of the Laizhou gold field (modified from Song et al., 2011). Y.-J. Li et al. / Journal of Asian Earth Sciences 113 (2015) 695–710 697 by biotite plagioclase gneiss and the biotite-bearing amphibolite pyritization as well as sericitization (Fig. 4b and c), and carbon- facies gneisses. The Linglong granites in this orefield represent atization (Fig. 4d), with an obvious horizontal zoning from silicifi- about 80% of the outcrop of the Mesozoic granitoids, which is the cation, sericitization to K-feldspar alteration. The K-feldspar largest outcrop in this area. They constitute the footwall of alteration occurs mainly in the outermost part of the alteration the Wang’ershan gold deposit. The Guojialing granodiorite in the zone along the brittle fractures in granitic wall rocks, and former Wang’ershan gold deposit area is distributed at depth as revealed plagioclase was almost totally replaced by secondary K-feldspar from drill cores, with significant K-feldspar alteration and sericiti- in the area with strong alteration (Fig. 4a). Strong silicification zation. The nearest Guojialing granodioritic, the Shangzhuang replaced most former minerals by quartz (Fig. 4b), whereas in body, is exposed in the northeast, outside the Wang’ershan gold the weak silicification zone, parts of former minerals were replaced deposit. The other important rock types are mafic dikes, mainly by quartz, with remnant K-feldspar, sericite, plagioclase, and lamprophyres, emplaced within the Linglong granite. sulfide surrounded by newly formed quartz. With strong diffusive Around 10 Au-bearing ore bodies hosted in the Linglong granite sericitization, sericite almost replaced all the plagioclase and bio- have been identified in the Wang’ershan gold deposit and are tite, retaining pseudomorphs of plagioclase (Fig. 4b and c). Strong mostly controlled by N–W trending faults. Two ore bodies, thought pyrite alteration, which heavily overprinted former alterations, to be the largest so far, from the altered zones are named No. 1 and developed along cracks or other open spaces in altered wall rocks. No. 5 respectively. The No. 1 ore body is about 600 m in length, and Among these, the silicification and pyritization show a close 800 m in depth and 2–3 m in width, with an average gold grade of relationship with gold mineralization. 2–28 g/t. The No. 5 ore body is about 300 m in length, 360 m in depth and average 2.51 m in width, with an average gold grade 3. Analytical methods of 3–14 g/t. Both the No. 1 and No. 5 ore bodies are characterized by abundant quartz veins or veinlets than the barren altered rocks. 3.1. Sample preparation Based on mineral assemblage and textures, ore types in the Wang’ershan gold deposit are divided into alteration type and The field investigations and sampling in this study were aimed quartz-vein type. The mineralization is closely related to the alter- at: (1) to obtain unweathered representative samples; (2) to obtain ation. The ores are characterized by disseminated, banded, brec- all types of ores and wall rocks; and (3) to sample the ore samples ciated, block and mottled structures (Fig. 2), and granular, from ore bodies with cut-off grade of 2 ppm Au. cataclastic and enclave textures (Fig. 3). Sulfide minerals in the Muscovite quartz and pyrite were separated under a binocular deposit are mainly pyrite and minor sphalerite, galena, chalcopy- microscope from crushed rock fragments, and the mineral sepa- rite and arsenopyrite. The gangue consists primarily of quartz, ser- rates were pulverized to 200 mesh. H–O, S isotopes and He–Ar iso- icite, K-feldspar and plagioclase. Notably, gold occurs as discrete topes were measured at the Beijing Research Institute of Uranium electrum and native gold. Based on the ore textures, structures Geology. and the observed mineral assemblages, the hydrothermal period of ore formation is considered to include 4 stages (Wang et al., 3.2. Zircon U–Pb dating 2011; Guo et al., 2014): (I) pyrite-quartz-sericite stage, (II) quartz-pyrite stage, (III) quartz-polymetallic sulfide stage, and The zircon samples in this study were separated from fresh (IV) quartz-carbonate stage. Among these four stages, the quartz- sample of the Linglong granite. U–Pb dating was performed on a pyrite stage and quartz-polymetallic sulfide stage are the main laser ablation inductively coupled plasma mass spectrometry ore-forming stages. (LA-ICP-MS) at the National Key Laboratory of Continental Alteration around the mineralized fracture zone mainly consists Dynamics of Northwest University. The analytical procedures are of K-feldspar alteration (Fig. 4a), silicification (Fig. 4b), and described in previous studies (e.g. Yuan et al., 2004). In the

Fig. 2. Structures of ores from the Wang’ershan gold deposit. (a) Disseminated structure. (b) Block structure. (c) Band structure. (d) Mottled structure. Q – quartz, Py – pyrite, Gn – galena, Ccp – chalcopyrite. 698 Y.-J. Li et al. / Journal of Asian Earth Sciences 113 (2015) 695–710

Fig. 3. Ore texture of the Wang’ershan gold deposit. (a) Granular texture. (b) Cataclastic texture. (c) and (d) Enclave texture. Py – pyrite, Gn – galena, Ccp – chalcopyrite.

LA-ICP-MS method, the laser spot diameter and frequency were digestion using a mixture of HF and HNO3 acids in high-pressure 30 lm and 10 Hz, respectively. Zircon 91500 was employed as a ‘‘bombs’’ (Qi et al., 2000). Pure elemental standard solutions were standard and the standard silicate glass NIST was used to optimize used for external calibration and BHVO-1 and SY-4 were used as the instrument. Raw data were processed using the GLITTER pro- reference materials. The accuracies of the XRFS analyses are gram to calculate isotopic ratios and ages of 207Pb/206Pb, estimated at <2% for elements with concentrations greater than 206Pb/238U, 207Pb/235U, respectively. Data were corrected for com- 0.5 wt.% and 5% for those >0.1 wt.%. The uncertainties of the mon lead, according to the method of Anderson (2002), and calcu- ICP-MS analyses are estimated to be better than ±5% for most trace lated the ages by ISOPLOT 4.15 software (Yuan et al., 2004). elements with concentrations >10 ppm, and ±10% for those <10 ppm. 3.3. Ar–Ar ages 3.5. S, O and H isotopes Muscovite flakes (0.1–2.5 mm; >99% purity) were separated from the K-feldspar – quartz block mass from the drilling core Sulfur isotope compositions were determined with a Finnigan and were handpicked under a binocular microscope. The altered MAT 251 mass spectrometer in the Beijing Research Institute of granite is gray-red in color, with granoblastic texture. The altered Uranium Geology, following the procedures outlined by rock shows obvious K-feldspar alteration and silicification, consist- Glesemann et al. (1994). The precision for d34S is better than ing of quartz (about 35%), K-feldspar (about 35%), microcline ±0.2‰ and the data are reported relative to Vienna Canon Diablo (about 15%), muscovite (about 10%), and sericite (about 5%). Troilite (V-CDT) sulfide. Muscovite is about 2–8 mm in length and appears as gobbets The hydrogen isotopic compositions of fluid inclusion in quartz together with microcline and quartz. and oxygen isotopic compositions of quartz were determined with The muscovite and ZBH-25 biotite (standard sample) were a Finnigan-MAT253 mass spectrometer. Oxygen was extracted irradiated in the atomic reactor of Research Institute of Atomic from quartz by the BrF5 method (Clayton and Mayeda, 1963), Energy (Beijing, China) and set in the B4 hole for fast neutron and hydrogen isotope compositions of fluid inclusions were ana- irradiation. The 40Ar/39Ar analyses were performed at the lyzed using the Zn reduction method (Coleman et al., 1982). The Geologic Laboratories Center, China University of Geosciences, analytical precisions were better than ±0.2‰ for d18O quartz and Beijing, on a MM5400 Micromass spectrometer operating in a sta- ±1‰ for dD. The values of d18O and dD are reported as ‰ deviation tic mode. Samples were loaded in aluminum packets into a from SMOW and V-SMOW, respectively. Christmas tree sample holder and degassed at low temperature (250–300 °C) for 20–30 min before being incrementally heated in 3.6. He and Ar isotopes a double-vacuum furnace. The gases released during each step were purified by means of Ti and Al–Zr getters. He–Ar isotope compositions were determined with a MM5400 gases mass spectrometer (Micromass, GB) at the Beijing Research 3.4. Major and trace elements Institute of Uranium Geology. The analyses were performed with electric current of It4 = 800 lA, It 40 = 200 lA, and 9000 kV. Major oxides were determined by wavelength-dispersive X-ray Samples were weighed and transferred to aluminum foil, and fluorescence spectrometry of fused glass beads using a Philips loaded in an all-metal extraction system for noble gas analysis. PW2400 spectrometer at the Beijing Research Institute of The samples were preheated under high vacuum at 130 °C for at Uranium Geology. Trace elements, including REE, were determined least 24 h to eliminate adsorbed air. Before the analysis of each using a VG Plasma-Quad Excel ICP-MS after a 2 day closed beaker sample, the background value and the standard sample (air) were Y.-J. Li et al. / Journal of Asian Earth Sciences 113 (2015) 695–710 699

Fig. 4. Photomicrographs of alteration assemblages. (a) Magmatic plagioclase was almost totally replaced by K-feldspar. (b) Sericite and plagioclase in the earlier stage were replaced by quartz. (c) Plagioclase crystals were totally replaced by sericite. (d) Calcite formed veinlets filling in fractures. Qtz-quartz, Py-pyrite, Ser-sericite, Pl-plagioclase, Cal-calcite. measured. The samples were pyrolyzed at three steps (300 °C, other heating events are absent (Zeitler and Gerald, 1986). The 700 °C and 1600 °C), some of them were directly heated to sample also yields an inverse isochron ages of 129.3 ± 3.3 Ma 1600 °C and kept for 5 min. Gas purification was carried out, fol- (Fig. 7b), which is comparable with the plateau age. The accor- lowed by the separation of the helium and argon. The background dance suggests that the age is geologically meaningful. value for 1600 °C was 4He = 1.10 1014, 40Ar = 6.21 1013 in unit mol. The standard sample (air) for the experiments was from 4.3. Major and trace elements the summit of Gaolan Mountain, Lanzhou, China. The analytical precision for the noble gas isotopic measurements is better than Because the Guojialing granodiorite at depth in the Wang’ershan 10%, adopting procedures reported in earlier studies (Ye et al., gold deposit displays significant K-feldspar alteration and sericiti- 2007; Sun et al., 2009). zation, only fresh samples of the Guojialing granodiorite from the Shangzhuang body were selected for geochemical analysis. Representative major and trace element analysis on two types of 4. Results rocks are listed in Table 3. Compositionally the samples from the Linglong granite and the Guojialing granodiorite are monzonitic 4.1. Zircon ages granite and granodiorite, respectively (Fig. 8a). The granite samples from the Linglong granite and the Guojialing granodiorite show lit- The U–Pb data of the zircon from the Linglong granite are pre- tle chemical variation on major elements, and are characterized by sented in Table 1. The zircon crystals are mostly euhedral, trans- high contents of Al O (13.79–16.86%), Na O (3.70–5.00%) and K O parent, and colorless. The majority exhibit oscillatory or planar 2 3 2 2 (2.99–4.51%), with low MgO (0.17–1.18%) and TiO (0.17–0.40%). zoning in CL (Fig. 5). The thorium and uranium contents range from 2 The data highlight their high-K (Fig. 8d) and alkaline nature 16.9 to 254.2 ppm and 39.6 to 338.1 ppm respectively, with (Fig. 8c). The samples of Linglong granite display peraluminous corresponding Th/U ratios of 0.19–0.91. The high Th/U ratios indi- feature (A/CNK = 0.99–1.11, A/NK = 1.24–1.46; Fig. 8b); although cate their magmatic crystallization history. Thirteen spots yield the samples of Guojialing tend more toward metaluminous 206Pb/238U weighted mean age of 149.0 ± 1.3 Ma (95% conf., composition (A/CNK = 0.98–1.10, A/NK = 1.27–1.55; Fig. 8b). MSWD = 0.60; Fig. 6a), which is consistent with the concordia The Linglong granite and Guojialing granodiorite display similar age of 149.2 ± 3.5 Ma (Fig. 6b). This Late Jurassic age is considered chondrite-normalized REE patterns that are characterized by the to represent the formation age of the Linglong granite. enrichment of LREEs, with negative Eu anomalies (dEu = 0.48– 0.86; Fig. 9a and c). Primitive-mantle-normalized trace element 4.2. Ar–Ar ages patterns for both Linglong granite and Guojialing granodiorite show significant enrichment in large ion lithophile elements (Ba, The step heating analysis results of the muscovite are listed in Pb) and depletion in high field-strength elements (Ta, Nb, Zr and Table 2, where 39Ar% represents the percent release. Very little Hf) (Fig. 9b and d). 39Ar was released below 700 °C, and a large amount of 39Ar REE concentrations in pyrite samples are relatively low and (88.6%) was released between 850 and 1150 °C. No significant variations occur in the contents of REE in different types of pyrite 39Ar was released when the temperature exceeded 1400 °C. (Table 4 and Fig. 10). The pyrite samples from quartz–sericite– The step heating spectra show apparent age values of muscovite pyrite altered granite are characterized by obvious enrichment of in a small range of 128.80–132.3 Ma, with a plateau age of LREE, with negative Eu anomaly (dEu = 0.55–0.70). However, 130.35 ± 0.96 Ma (Fig. 7a). This is an ideal age spectrum, indicating LREEs and HREEs in pyrite from quartz vein are not much fraction- that the cooling process of the rock was rapid and effects of any ated, with only slight positive Eu anomaly (dEu = 1.42–1.87). 700 .J ie l ora fAinErhSine 1 21)695–710 (2015) 113 Sciences Earth Asian of Journal / al. et Li Y.-J.

Table 1 LA-ICP-MS zircon U–Pb isotopic dating of the Linglong granite in the Wang’ershan gold deposit.

Spot Conc. (ppm) Isotope ratio Age (Ma) Th U Th/U 207 Pb/206 Pb 1r 207 Pb/235 U1r 206 Pb/238 U1r 207 Pb/206 Pb 1r 207 Pb/235 U1r 206 Pb/238 U1r PG-2-5-01 16.89 39.63 0.426192279 0.04967 0.00835 0.16393 0.0273 0.02394 0.00055 179.4 350.59 154.1 23.81 152.5 3.49 PG-2-5-03 44.98 122.36 0.367603792 0.0494 0.00398 0.15721 0.01241 0.02308 0.00035 166.7 178.15 148.3 10.89 147.1 2.21 PG-2-5-05 68.34 117.36 0.582310838 0.05027 0.00343 0.16242 0.01083 0.02343 0.00031 207.4 151.07 152.8 9.46 149.3 1.94 PG-2-5-06 57.21 133.52 0.428475135 0.04841 0.00354 0.15413 0.01104 0.02309 0.00031 119.5 164.02 145.6 9.72 147.2 1.96 PG-2-5-09 28.57 50.22 0.568896854 0.04854 0.00962 0.16015 0.03139 0.02393 0.00072 125.6 409.53 150.8 27.47 152.4 4.54 PG-2-5-10 64.07 338.15 0.189472128 0.04927 0.00137 0.15768 0.00405 0.02321 0.00016 160.8 63.64 148.7 3.56 147.9 1.02 PG-2-5-11 60.52 102.38 0.59113108 0.04768 0.00428 0.1549 0.01365 0.02356 0.00036 82.4 200.89 146.2 12.01 150.1 2.27 PG-2-5-12 26.54 47.55 0.558149317 0.05603 0.00894 0.17923 0.02821 0.0232 0.00063 453.2 320.28 167.4 24.29 147.9 3.97 PG-2-5-14 30.68 64.45 0.476027929 0.04524 0.00592 0.14784 0.01913 0.0237 0.00046 0.1 248.19 140 16.92 151 2.9 PG-2-5-16 154.04 204.2 0.754358472 0.04818 0.00292 0.15498 0.00915 0.02333 0.00028 108.3 137.3 146.3 8.04 148.7 1.76 PG-2-5-17 41.17 99.09 0.415480876 0.05252 0.00602 0.16525 0.01864 0.02282 0.00044 308.2 241.8 155.3 16.25 145.4 2.78 PG-2-5-18 254.21 278.57 0.912553398 0.04989 0.00212 0.1622 0.00659 0.02358 0.00024 190 95.97 152.6 5.76 150.2 1.49 PG-2-5-24 47.72 104.91 0.454866076 0.05213 0.00465 0.16699 0.01459 0.02323 0.00039 291.2 191.05 156.8 12.7 148.1 2.43 Y.-J. Li et al. / Journal of Asian Earth Sciences 113 (2015) 695–710 701

Fig. 5. Cl images of zircons from the Linglong granite, showing the spot sits.

Fig. 6. Zircon U–Pb concordia plots (a) and recalculated weighted mean 206Pb/238U ages (b) for the Linglong granite.

Table 2 40Ar/39Ar analytical results of the Guojialing granodiorite.

40 39 (36 39 37 39 38 39 40 39 14 39 Stage T (°C) ( Ar/ Ar)m Ar/ Ar)m ( Ar/ Ar)m ( Ar/ Ar)m Ar (%) Ar (10 ) Ar% Age (Ma) 1 700 70.7464 0.213 7.4477 0.0713 11.76 0.13 0.86 42.5 ± 4.5 2 800 30.4075 0.0249 0.3156 0.0183 75.88 0.81 6.24 114.8 ± 1.2 3 850 31.0614 0.0177 0.5002 0.0158 83.22 0.69 10.87 128.1 ± 1.3 4 900 29.2701 0.0115 0.34 0.0149 88.42 1.13 18.4 128.2 ± 1.3 5 950 28.539 0.007 0.3642 0.014 92.88 3.51 41.86 131.2 ± 1.3 6 990 26.6358 0.0021 0.6639 0.0134 97.79 1.89 54.51 129.1 ± 1.3 7 1030 27.2138 0.0038 0.9215 0.0135 96.05 1.75 66.23 129.5 ± 1.3 8 1070 28.4497 0.0062 0.7705 0.0142 93.71 1.11 73.64 132 ± 1.3 9 1110 27.491 0.0026 0.3241 0.0134 97.26 2.93 93.23 132.3 ± 1.3 10 1150 26.6423 0.0011 1.3189 0.0131 99.08 0.8 98.55 130.8 ± 1.3 11 1200 27.4618 0.0063 1.5334 0.0155 93.59 0.14 99.49 127.5 ± 2.7 12 1400 51.0571 0.0273 18.8101 0.0181 86.79 0.08 100 217.4 ± 4.7

Note: Time of each step-heating is 10 min.

18 4.4. S, O and H isotopes 14.6‰, with a mean at 11.9‰, and the d Dw values are in the range of 97.5‰ to 61.4‰, with a mean at 82.6‰ (Table 6). Sulfur isotope analyses are presented in Table 5. The d34S values The O isotopic composition of the mineralizing ﬂuid can be calcu- of 10 samples range from 6‰ to 8.3‰ with the mean value of lated from that of quartz with the equation 1000lnaQ–W = 18 6 2 7.66‰. The d OQ values of quartz show a range of 10.0‰ to 3.38 10 T 3.40 (Clayton et al., 1972), where T represents 702 Y.-J. Li et al. / Journal of Asian Earth Sciences 113 (2015) 695–710

Fig. 7. Muscovite Ar–Ar ages of the Guojialing granodiorite. (a) 40Ar/39Ar age spectra, (b) Ar–Ar inverse isochron.

Table 3 Major elements (wt.%) and trace elements (106) composition of the Linglong granite and Guojialing granodiorite.

Rock type Linglong granite Guojialing granodiorite D17-1 D17-3 D17-6 D19-3 D24-1 D25-1 D35-1 D17-4 D24-5 D25-2 D29-7 D30-2 D30-3

SiO2 72.61 72.24 74.28 67.18 74.77 72.81 72.38 69.91 68.28 65.98 68.76 68.65 68.36

TiO2 0.20 0.21 0.17 0.30 0.17 0.24 0.23 0.30 0.40 0.35 0.34 0.35 0.35

Al2O3 14.00 13.98 14.31 14.44 13.79 14.68 15.01 15.33 16.86 14.81 16.19 15.57 15.39

Fe2O3 1.47 1.30 0.97 2.38 0.73 1.47 1.69 1.93 2.38 2.50 1.64 2.71 2.70 FeO 0.91 0.26 0.57 0.27 0.57 1.01 0.74 0.42 0.23 1.46 0.78 1.26 1.07 MnO 0.03 0.03 0.02 0.04 0.01 0.02 0.02 0.03 0.03 0.04 0.03 0.04 0.03 MgO 0.22 0.27 0.17 1.05 0.21 0.24 0.26 0.77 0.57 1.18 0.93 1.15 1.15 CaO 1.12 1.43 1.18 2.54 1.26 1.54 1.77 1.34 3.11 2.83 2.29 1.60 2.42

Na2O 3.98 3.70 3.85 3.93 3.77 3.95 4.38 5.00 4.65 3.84 4.58 4.38 4.09

K2O 3.82 4.36 4.01 3.17 4.51 4.33 3.88 3.56 2.99 3.32 4.45 3.75 3.90

P2O5 0.05 0.05 0.03 0.12 0.02 0.04 0.04 0.10 0.09 0.13 0.10 0.14 0.13 LOI 2.41 2.39 0.99 4.72 0.71 0.66 0.33 1.70 0.61 4.87 0.66 1.62 1.39 Total 100.82 100.21 100.54 100.14 100.51 100.98 100.73 100.39 100.20 101.30 100.75 101.21 100.99 V 9.16 8.42 2.30 30.20 4.49 2.20 4.33 27.70 13.40 34.20 20.20 33.40 36.30 Cr 2.75 1.77 0.57 21.70 1.03 0.51 0.46 19.80 1.82 20.30 19.70 22.80 26.90 Ni 1.09 0.80 0.55 8.44 0.44 0.31 0.47 6.85 1.48 7.94 11.50 8.33 9.97 Rb 97.50 106.00 97.80 89.10 71.20 76.00 92.70 88.10 60.50 80.40 87.90 86.40 83.80 Sr 427 409 777 450 895 743 905 790 1582 738 1832 867 1070 Y 10.70 9.63 4.79 7.48 3.17 3.53 2.72 6.56 9.89 7.49 8.32 10.50 9.95 Nb 8.53 8.38 5.50 7.00 2.66 4.96 3.41 5.90 10.30 6.63 6.51 8.00 7.92 Ba 1822 2286 2939 1010 2317 2845 2450 1714 3590 1900 3506 1871 2227 La 42.70 45.20 19.20 41.40 26.60 43.40 36.30 38.00 46.60 40.00 56.70 44.90 40.20 Ce 67.40 67.90 32.70 71.80 48.80 67.70 58.90 59.70 87.70 69.80 105.00 84.80 76.20 Pr 7.00 6.79 3.41 7.74 5.15 7.36 6.72 6.50 9.61 7.61 12.30 9.76 8.58 Nd 22.30 22.80 11.10 26.00 18.30 24.10 21.40 22.50 31.70 25.70 41.50 31.70 30.10 Sm 3.24 3.30 1.73 3.72 2.79 2.96 2.60 3.36 4.44 3.70 5.66 4.58 4.30 Eu 0.59 0.51 0.33 1.02 0.55 0.60 0.54 0.90 1.10 0.93 1.46 1.16 0.90 Gd 3.01 2.96 1.52 3.37 2.29 2.58 2.50 2.99 3.91 3.30 4.69 3.89 3.72 Tb 0.43 0.39 0.20 0.43 0.25 0.28 0.28 0.36 0.52 0.43 0.57 0.54 0.50 Dy 1.93 1.86 0.86 1.56 0.75 0.78 0.70 1.42 2.07 1.60 1.79 2.07 1.96 Ho 0.38 0.36 0.16 0.28 0.12 0.14 0.11 0.26 0.35 0.29 0.28 0.37 0.34 Er 1.15 1.04 0.49 0.86 0.41 0.51 0.39 0.76 1.08 0.86 0.94 1.08 1.05 Tm 0.20 0.18 0.08 0.13 0.05 0.07 0.04 0.11 0.15 0.13 0.11 0.17 0.16 Yb 1.23 1.17 0.50 0.83 0.32 0.39 0.26 0.71 0.88 0.82 0.70 1.00 1.01 Lu 0.18 0.18 0.07 0.12 0.05 0.05 0.04 0.10 0.11 0.12 0.09 0.14 0.15 Ta 0.67 0.61 0.35 0.50 0.20 0.20 0.08 0.42 0.58 0.45 0.37 0.53 0.54 Pb 25.40 33.00 34.10 11.60 28.60 22.60 33.70 20.50 24.10 29.20 36.10 17.30 31.00 Th 10.70 10.50 3.85 10.80 12.40 6.37 5.83 9.21 8.50 9.61 12.80 11.80 11.80 U 2.47 2.18 0.41 1.68 1.44 0.49 0.41 1.82 0.77 2.49 1.30 2.16 1.91 Zr 153.00 136.00 57.50 100.00 83.00 65.50 59.30 105.00 24.90 130.00 44.70 107.00 131.00 PHf 4.63 4.30 1.67 3.14 3.13 1.69 1.59 3.09 0.75 3.52 1.28 3.16 3.55 REE 151.73 154.62 72.35 159.26 106.42 150.91 130.77 137.66 190.23 155.28 231.79 186.15 169.17 dEu 0.57 0.48 0.61 0.86 0.65 0.65 0.64 0.85 0.79 0.80 0.84 0.82 0.67

LaN/YbN 24.90 27.71 27.33 35.65 60.38 80.03 102.11 38.23 37.90 35.16 58.52 32.37 28.55 A/NK 1.31 1.29 1.34 1.46 1.24 1.31 1.31 1.27 1.55 1.49 1.31 1.38 1.40 A/CNK 1.10 1.04 1.11 0.99 1.03 1.05 1.03 1.06 1.02 0.98 0.98 1.10 1.00 Y.-J. Li et al. / Journal of Asian Earth Sciences 113 (2015) 695–710 703

Fig. 8. Geochemical characteristics of the Mesozoic granites in the Wang’ershan gold deposit. (a) R1 vs. R2 diagram (after De la Roche et al., 1980); (b) A/NK vs. A/CNK plot;

Fig. 9. Chondrite normalized rare earth element patterns (a and c) and primitive mantle normalized spider diagrams (b and d) for the Mesozoic granites in the Wang’ershan gold deposit. Normalized values are from Sun and McDonough (1989). 704 Y.-J. Li et al. / Journal of Asian Earth Sciences 113 (2015) 695–710

Table 4 REE contents (106) of the pyrite from the Wang’ershan gold deposit.

Sample no. B01-9(1) B02-12(2) B01-8(1) B01-8(3) B04-2(4) B04-4(4) Host rock Altered granite Altered granite Altered granite Altered granite Quartz Quartz La 3.14 0.829 5.74 4.2 0.09 0.049 Ce 5.29 1.3 9.57 6.92 0.105 0.084 Pr 0.565 0.133 1.02 0.732 0.018 0.011 Nd 1.98 0.47 3.52 2.57 0.093 0.045 Sm 0.25 0.05 0.548 0.367 0.023 0.008 Eu 0.046 0.011 0.08 0.064 0.013 0.006 Gd 0.18 0.046 0.364 0.264 0.034 0.012 Tb 0.016 0.004 0.03 0.025 0.006 <0.002 Dy 0.078 0.012 0.074 0.062 0.042 0.011 Ho 0.014 0.003 0.009 0.007 0.005 <0.002 Er 0.031 0.008 0.019 0.022 0.018 0.006 Tm 0.007 <0.002 <0.002 <0.002 0.004 <0.002 Yb 0.039 0.008 0.013 0.008 0.031 0.006 Lu 0.007 <0.002 <0.003 <0.004 0.004 <0.002 Y 0.351 0.065 0.224 0.219 0.257 0.067 RREE 11.64 2.87 20.99 15.24 0.49 0.24 LREE 11.27 2.79 20.48 14.85 0.34 0.20 HREE 0.37 0.08 0.51 0.39 0.14 0.04 LREE/HREE 30.30 34.48 40.23 38.28 2.38 5.80 LaN/YbN 57.75 74.33 316.72 376.58 2.08 5.86 dEu 0.66 0.70 0.55 0.63 1.42 1.87 dCe 0.97 0.96 0.97 0.97 0.64 0.89

18 the temperature of ﬂuid inclusions in quartz. The d Ow values of the mineralizing ﬂuids show a range of 2.13‰ to 7.5‰, with an average of 2.4‰.

4.5. He and Ar isotopes

Helium and argon isotope data on the Wang’ershan gold deposit are listed in Table 7. The 3He/4He ratios of pyrite are in the range 1.58–2.71 Ra (Ra is the 3He/4He ratio of air = 1.4 106) with a mean value at 2.168 Ra. The results fall between the crust 3He/4He (0.01–0.05 Ra) and the mantle 3He/4He (6–7 Ra). The 40Ar/36Ar ratios show variation from 1220.3 to 1625.7 with an average of 1483.8, which is higher than the 40Ar/36Ar value of the atmosphere (295.5).

5. Discussion

5.1. Timing of gold mineralization

The Mesozoic intrusion exposed in the Wang’ershan gold deposit is mainly the Linglong granite, the zircons from which yield 206Pb/238U weighted mean age of 149.0 ± 1.3 Ma that is consistent with the late Jurassic granitic magmatism in the region (165– 149 Ma; Wang et al., 1998; Qiu et al., 2002; Mao et al., 2005; Jiang et al., 2012; Yang et al., 2012). The Guojialing granodiorite in the northwestern part of Jiaodong intruded the Linglong granite during Early Cretaceous (132–123 Ma; Goss et al., 2010; Liu et al., 2010; Wang et al., 2014). The muscovite from the K-feldspar – quartz alteration zone in this study yields a plateau age of 130.35 ± 0.96 Ma, which is older than the widely accepted period Fig. 10. Chondrite normalized REE distribution patterns of samples from the of the main gold mineralization event in the northwestern part Wang’ershan gold deposit. (a) Chondrite normalized REE patterns of altered rocks. of the Jiaodong gold province during the Early Cretaceous (b) Chondrite normalized REE patterns of quartz vein rocks. Normalized values are at120 ± 5 Ma (Li, 2004; Yang et al., 2014a; Goldfarb and Santosh, from Sun and McDonough (1989). 2013; Yang and Santosh, 2015). The hydrothermal sericite extracted from auriferous vein yielded a 40Ar/39Ar plateau age between 120.6 ± 0.3 Ma and 120.0 ± 0.4 Ma (Li et al., 2003a), which upwelling of hydrothermal ﬂuids resulted in the K-feldspar alter- is well within the gold mineralization period. ation, leading to the formation of the muscovite. The hydrothermal In our samples, muscovite appears as gobbets together with sericite in previous study was extracted from auriferous vein (Li K-feldspar and quartz, which might have formed during the transi- et al., 2003a) that formed during the main stage of hydrothermal tion between the formation of the Guojialing granodiorite and gold activity. These ages are both obtained by similar precise 40Ar/39Ar mineralization. At the initial stage of hydrothermal activity, the isotopic dating with small error. Provided that these ages are Y.-J. Li et al. / Journal of Asian Earth Sciences 113 (2015) 695–710 705

Table 5 REE patterns of the magmatic rocks and the pyrite from altered Sulfur isotopic composition of pyrite from the Wang’ershan gold deposit. granite, which suggests that the pyrite inherited the characteristics Sample no. Mineral d34 (‰) of the magmatic rocks because of the water–rock reaction between B01-8(1) Pyrite 7.6 ore-forming fluid and wall rocks. However, the REE characteristics B01-9(1) Pyrite 8.3 of pyrite from quartz veins are quite different and represent the B02-12(2) Pyrite 7.8 REE characteristics of ore-forming fluids during the main ore-form- B04-2(2) Pyrite 7.6 ing stage. B01-3(3) Pyrite 6 The isotope composition of hydrothermal sulfide is determined B01-8(3) Pyrite 7.8 B05-2(3) Pyrite 7.5 by total sulfur isotopic composition of the hydrothermal system B01-6(4) Pyrite 8.1 and the physicochemical conditions of mineralization (Sakai, B04-2(4) Pyrite 7.7 34 1968; OhmotoP and Rye, 1979; Hoefs, 1997). The d S value of total B04-4(4) Pyrite 8.2 sulfur (i.e., S) in the fluids is a proxy for the source (Ohmoto and Rye, 1979). The average d34S values of sulfide minerals approxi-

mate that of hydrothermal fluids in which H2S is the dominant sul- Table 6 fur species and when the mineral assemblage is simple (Ohmoto Oxygen and hydrogen isotopic compositions of quartz from the Wang’ershan gold and Rye, 1979; Rollinson, 1993). In the Wang’ershan gold deposit, deposit. the sulfur-bearing minerals are mainly sulfides (e.g., pyrite, pyr- 18 18 18 Sample Stage Mineral d OQ (‰) d OW (‰) d DQ (‰) T (°C) rhotite, and chalcopyrite) and the lack of oxidized phases (e.g., hematite) and sulfate minerals in the ore indicate a relatively sim- B02-8-5 I Quartz 12.8 7.5 72.8 350 34 B01-4-6 I Quartz 10 4.7 61.4 350 ple paragenesis, implying that the average d S values of pyrite B01-1-5 II Quartz 11.1 2.34 75.7 254 (the most abundant sulfide mineral) can directly represent the sul- B01-9-1 II Quartz 10.5 1.74 79.3 254 fur source. B01-7-4 III Quartz 11.3 1.86 90.3 240 The d34S values of pyrite from the Wang’ershan deposit display B04-2-4 III Quartz 12.2 2.76 91.8 240 B04-2-2 III Quartz 12 2.43 93 240 a narrow range (6‰ to 8.3‰, with a mean at 7.66‰), indicating a B04-6-3 IV Quartz 14.6 0.17 81.8 190 markedly homogeneous source. The Wang’ershan gold deposit is B05-2-3 IV Quartz 12.3 2.13 97.5 190 situated in the Jiaojia gold metallogenetic belt, with geologic features similar to the other gold deposits in this region such as the Jiaojia gold deposit and Xincheng gold deposit. The sulfur isotope characteristics are also similar, indicating same source of sulfur reliable, the age of 130.35 ± 0.96 Ma represents the beginning of for the deposits in this region (Huang, 1994; Zhang and Chen, the hydrothermal activity before gold mineralization, and the age 1999; Zhang et al., 2002; Mao et al., 2008; Li et al., 2013a). of ca. 120 Ma represents the timing of gold mineralization in the Previous studies show that the d34S values of samples from 40 39 Wang’ershan gold deposit. Yang et al. (2014b), based on Ar/ Ar Linglong granite formed during the main magmatic activity in geochronological constraints also concluded that the gold mineral- the region are in the range of 3.19‰ to 14.19‰, and the d34S values ization in the Dayingezhuang deposit in Jiaodong occurred of pyrite in the Guojialing granodiorite are between 2.17 to 10.1 between 134 and 126 Ma. (Wang, 1990; Huang, 1994; Wang et al., 2002). Moreover, the Li et al. (2003a) noted that cooling ages of the intrusion d34S values of pyrite in amphibolite and plagioclase-gneiss from (Guojialing granodiorite) from the Shangzhuang body at ca. the Jiaodong group also display a range of 1.3–7.8‰ (Li and Wu, 500 °C and 300–350 °C are 128.1–127.5 Ma and 124.4–124.1 Ma, 1995; Wang et al., 2002). The similar sulfur isotopic compositions respectively. The gold mineralization in the Wang’ershan gold of the Mesozoic Linglong granite, Guojialing granodiorite, and deposit occurred slightly after the cooling of the Guojialing gran- Jiaodong group rocks indicate the homogenization of sulfur iso- odiorite, which also indicates that the gold deposition might have topic system during crust-mantle interaction through geological link with the fluids expelled from the pluton during its cooling. time (Mao et al., 2008). Pyrite is an ideal mineral that preserves noble gases of mineral- 5.2. Sources of ore-forming materials and fluids ization from paleo-fluids (Hu et al., 1997; Zheng and Chen, 2000). The helium of the hydrothermal fluid can be well preserved in fluid As a good geochemical tracer, rare earth elements inherit the inclusions during the formation of mineral formed, as diffusivity of characteristics of ore-forming fluids in equilibrium with rocks dur- helium (Burnard et al., 1999). Because of the extremely low con- ing the mineralization, and their differential distribution is often tents, noble gases in atmosphere would not visibly contaminate interpreted as the change in source of fluid (H.M. Li et al., 2003; the helium composition in crustal fluid (Stuart et al., 1995). All Yang et al., 2003). Pyrite is the main gold-bearing mineral in the the samples analyzed in this study were collected from deep Wang’ershan gold deposit. The significant differences between underground mine workings, thus the possibility of existence of the chondrite-normalized REE patterns of pyrite indicate different cosmogenic 3He can be ruled out (Simmons et al., 1987; Stuart origins. There is no obvious difference in the chondrite-normalized et al., 1994). Moreover, the pyrite samples display no evidence

Table 7 Helium and argon isotopic compositions of the pyrite from the Wang’ershan gold deposit.

4 3 40 3 3 4 40 36 3 36 3 4 Sample Mineral He (cm STP/g) Ar (cm STP/g) He/ He Ar/ Ar 3He (cm STP/g) Ar (cm STP/g) F He Hemantle no. (107) (107) (106) (1012) (107) (%) B02- Pyrite 3.6 2.9 2.71 1604.5 0.9756 0.001807 12,035 24.5 12(2) B01-8(3) Pyrite 3.5 2.6 2.45 1625.7 0.8575 0.001599 13223.22 22.13 B01-6(4) Pyrite 9.9 5.5 1.58 1220.3 1.5642 0.004507 13272.15 14.21 B04-2(4) Pyrite 6 3.3 1.93 1484.6 1.158 0.002223 16309.8 17.4 706 Y.-J. Li et al. / Journal of Asian Earth Sciences 113 (2015) 695–710

Fig. 11. Sulfur compositions from Wang’ershan gold deposit, Linglong granite, Guojialing granodiorite and Jiaodong group compared with natural geological settings. (Range for natural geological settings from Hoefs, 1997).

Fig. 12. 3He–4He (a)and R/Ra-40Ar/36Ar(b) plots of inclusion-trapped fluids in sulfide mineral from the Wang’ershan gold deposit (modified from Winckler et al., 2001).

for later deformation, therefore, the helium and argon isotopic val- primary magmatic water (Taylor, 1974) and the magmatic water ues in the inclusions are thought to reflect the nature of ore-form- of the Guojialing granodiorite (Guo et al., 2014), indicating a poten- ing fluids trapped in the sulfide minerals (see Fig. 11) tial magmatic water source for the ore-forming fluid from stage I The 3He–4He data of fluid inclusions from the Wang’ershan gold (Fig. 13). The plots samples from stages II, III, and IV are distributed deposit (1.13–1.94 Ra) are distributed in the transition zone of between the area of metamorphic water in the eastern China crust (0.01–0.05 Ra) and mantle (6–9 Ra) (Fig. 12a; Stuart et al., (Zhang, 1985) and the meteoric water line (Taylor, 1974). 1995; Yamamoto et al., 2009). Plotted in R/Ra vs. 40Ar/36Ar diagram The oxygen and hydrogen isotopic composition in ore-forming (Fig. 12b), the data points are distributed between the crust and fluid is controlled by the isotopic compositions in both initial fluid mantle helium domains and away from the area of atmospheric and wall rock, the temperature, and the water/rock ratio (w/r) dur- saturation water. The percentage of mantle helium in hydrother- ing water–rock reaction. Based on the study of Taylor (1974),itis mal fluid in crust-mantle dual model can be calculated based on possible to calculate the amount of water involved in hydrother- the equation: Hemantle(%) = 100 (R Rc)/(Rm Rc), where Rm mal system as follows: (3He/4He in mantle) and Rc (3He/4He in crust) are set as i i f f 5 8 1.1 10 and 2 10 in this study, respectively (Tolstikhin, W dwater þ R drock ¼ W dwater þ R drock 1978; Kendrick et al., 2001; Stuart et al., 1995). The calculated per- where i = initial value; f = final value after exchange; W = atomic centage of mantle helium varies in the range of 18.13–31.69% with percent of water; R = atomic percent of exchangeable rock. Then: an average of 25.18%. The 40Ar/36Ar ratios show a range of 1220.3– 1625.7, much larger than that of atmospheric saturation water f i i f W=R ¼ðdrock drockÞ=½dwater ðdrock DÞ (40Ar/36Ar = 295.5). f f Oxygen and hydrogen isotopes are important monitors of the where D = d rock d water. In the Jiaodong region, drock at equilibrium 18 18 source and evolution of ore-forming fluids. The calculated d Ow is equal to the d Ovalue of plagioclase (An30) and the dD value of and dD values of quartz from stage I are close to those of the biotite (Zhai et al., 1995). Then the D can be calculated utilizing Y.-J. Li et al. / Journal of Asian Earth Sciences 113 (2015) 695–710 707

Fig. 13. Hydrogen and oxygen isotope compositions and water–rock isotope exchange evolutional curves of Wang’ershan gold deposit. Range for primary magmatic water from Taylor (1974); range for metamorphic water in the eastern China from Zhang (1985); values for the Linglong granite and the Guojialing granodiorite from Guo et al. (2014).

18 6 feldspar-H2O and biotite-H2O geothermometers (D O = 2.68 10 / in the dilution zones of the metamorphic water of the Jiaodong T2 3.53, DD=21.3 106/T2 2.8; O’Neil and Taylor, 1967). The Group and meteoric water and the magmatic water of the oxygen and hydrogen contents in rocks are approximately 50% and Guojialing granodiorite and meteoric water. It seems that meta- 1%, respectively. The W/R is the value of atomic ratio, therefore, the morphic and magmatic water contributed to the ore fluid. As mass ratio of rock and water can be calculated as w (W)/ shown in Fig. 13, the dD value of fluid increases with the decrease w(R) = 0.5W/R for d18O and w(W)/w(R) = 0.01W/R for dD. of mass ratio of rock and water (from 5 to 0.005). Therefore, during i18 i The d waterO and d waterD values in this region are 7.7‰ and the evolution, the dD value of fluid should not be less than the ini- i 47‰ for the magmatic water of the Guojialing granodiorite, tial dD value of fluid (d waterD). However, the minimum dD values of 9.9‰ and 62‰ for the metamorphic water of the Jiaodong ore-forming fluids of stages II, III, and IV are all less than the dilu- Group (Guo et al., 2014), and 16‰ and 120‰ for the tion values of the metamorphic water of the Jiaodong Group and i 18 Mesozoic meteoric water (Zhai et al., 1995). The drock O and meteoric water. Thus, the ore-forming fluids were mainly mag- i drockD values are 7‰ and 72‰ for the Linglong granite (Mao matic water of the Guojialing granodiorite mixed with meteoric et al., 2005), and 8.2‰ and 88.5‰ for the Jiaodong Group rocks water. The samples from stage IV plot closer to the evolution curve (Chen et al., 1995). The calculated water–rock isotope exchange of the Mesozoic meteoric water, indicating that the meteoric water evolutional curves at temperatures of 350 °C (stage I), 254 °C (stage contributed more to the formation of ore-forming fluid in stage IV. II), 240 °C (stage III), and 190 °C (stage IV) (Guo et al., 2014) with mass ratios of rock and water varying from 5 to 0.005 are shown 5.3. Tectonics associated with metallogeny in Fig. 13. The d18O and dD values of all the samples are much lower than The Wang’ershan gold deposit is located in and controlled by that of the Linglong granite, and therefore we exclude any mag- the Wang’ershan fault that is a secondary fault of the Jiaojia fault matic water derived from the Linglong granite. The values of sam- zone. The Jiaojia fault has been dated using K–Ar isotopic tech- ples from stage I are distributed along the water–rock isotope nique as 131.05–123.53 Ma (Song et al., 2010). The Zhaoping fault exchange evolutional curves of magmatic water of the Guojialing zone is another important regional ore-controlling fracture belt to granodiorite Linglong granite, and magmatic water of the the east of the Wang’ershan gold deposit, and the muscovite from Guojialing granodiorite Jiaodong Group at 350 °C, suggesting the tectonic schist in the Zhaoping fault zone yielded a 40Ar/39Ar the genetic relationship between the fluid and the magmatic water plateau age of 134.26 ± 0.34 Ma (Lin et al., 2000). The emplacement of the Guojialing granodiorite. The samples from stages II, III, and of the Guojialing granodiorite was approximately synchronous IV show a trend of migrating to the meteoric water, indicating with (or slightly later than) the formation of regional fault zones. the mixture of meteoric water in the ore-forming fluids. These Similar to the Wang’ershan gold deposit, previous studies have samples show much low d18O and dD values which are distributed obtained the ages of major gold deposits in this region located 708 Y.-J. Li et al. / Journal of Asian Earth Sciences 113 (2015) 695–710 along the Jiaojia fault zone (e.g., hydrothermal sericite and mus- (2) The hydrothermal fluids in early stage were mainly mag- covite 40Ar/39Ar plateau age of 121.0 ± 0.4–119.2 ± 0.2 Ma for matic and derived from the Guojialing granodiorite. The Jiaojia and Xincheng, Li et al., 2003b; pyrite Rb–Sr isochron age ore-forming fluids in main ore-forming stages evolved into of 122.3 ± 3.1 Ma for Hexi, Hou et al., 2006) and the Zhaoping fault a mixture of magmatic and meteoric water; the ore-forming zone (e.g., gold-bearing pyrite Rb–Sr isochron age of 122–120 Ma materials were primarily derived from crust, with minor for Dakaitou, Jiuqu, and Linglong, Yang and Zhou, 2000a,b, 2001). input of mantle materials. Moreover, the mineralization age of the Cangshang gold deposit, (3) The gold deposit was formed in the extensional setting in the westernmost margin, is dated at 121.3 ± 0.2 Ma by related to the subduction of the paleo-Pacific slab beneath hydrothermal sericite 40Ar/39Ar analyses (Zhang et al., 2003). the North China Craton (NCC) and the associated astheno- These ages represent the periods of the main phase of gold sphere upwelling and consequent lithospheric thinning. mineralization slightly after the crystallization of the Guojialing granodiorite. Given the potential duration of ore-forming hydrothermal activity, the gold mineralization is thought to be related to the emplacement of the Guojialing granodiorite. The cat- Acknowledgements aclasites along the Wang’ershan fault indicate the brittle deformation along the fault in the Linglong granite massif. The data from We thank Journal referees Ms Qiong-Yan Yang and an anony- Wang’ershan gold deposit suggest the beginning of hydrothermal mous reviewer for constructive and helpful comments. We also activity along the section of the fault zone at ca. 130 M, syn- thank Mr. Qingzhou Sun, Xu Li and Zhanshan Sun of the chronous with the intrusion of the Guojialing granodiorite. Wang’ershan Gold Company for their help at field work. We are Drastic changes in tectonic regime occurred during Mesozoic in grateful to the Master students from China University of eastern Asia, where the Late Permian-Early Triassic and the Geosciences, Mr. Zengda Li and Chonghao Liu for their support dur- Cretaceous periods witnessed the nappe-stacking and HP rocks ing our laboratory work and the manuscript preparation. This work burial, and large-scale extensional event, respectively (Charles was supported by the Key Programme of the National Natural et al., 2011). The gold mineralization event in the Jiaodong Science Foundation of China [90914002], China Geological Survey Peninsula is related to major plate shifts in the Pacific, especially [1212011220926], and the specialized research fund for the doc- the extensional crustal-scale structures developed through the toral programme of higher education [20130022110003]. Jiaodong Peninsula during the Early Cretaceous, which probably reflect the subduction of Pacific plate beneath the Eurasian plate References and the resulting transpressive regime along the edge of the conti- nent (Charles et al., 2011; Guo et al., 2013; Liu et al., 2014; Yang Anderson, T., 2002. Correction of common Pb in U–Pb analyses that do not report et al., 2014b). The subduction process led to crustal thinning and 204Pb. Chem. Geol. 192, 59–79. slab rollback and brought deep mantle materials to the upper man- Burnard, P.G., Hu, R., Turner, G., 1999. 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