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Stable isotope geochemistry and Re–Os ages of theYinan gold deposit, Shandong Province, northeasternChinaYang Liua, M. Santosha, Sheng-Rong Liab & Pu Guoa

a School of Earth Sciences and Resources, China University of Geosciences, Beijing, Chinab State Key Laboratory of Geological Processes and Mineral Resources, China University ofGeosciences, Beijing, ChinaPublished online: 10 Feb 2014.

To cite this article: Yang Liu, M. Santosh, Sheng-Rong Li & Pu Guo (2014) Stable isotope geochemistry and Re–Os agesof the Yinan gold deposit, Shandong Province, northeastern China, International Geology Review, 56:6, 695-710, DOI:10.1080/00206814.2014.886167

To link to this article: http://dx.doi.org/10.1080/00206814.2014.886167

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Stable isotope geochemistry and Re–Os ages of the Yinan gold deposit,Shandong Province, northeastern China

Yang Liua, M. Santosha, Sheng-Rong Lia,b* and Pu Guoa

aSchool of Earth Sciences and Resources, China University of Geosciences, Beijing, China; bState Key Laboratory of GeologicalProcesses and Mineral Resources, China University of Geosciences, Beijing, China

(Received 7 November 2013; accepted 19 January 2014)

The Yinan gold deposit in the Luxi area of Shandong Province in northeastern China is a skarn-type ore deposit. In thisarticle, we present results from sulphur, lead, carbon–oxygen, and helium–argon isotope chemistry to characterize the oregenesis and source features. We also present rhenium–osmium ages from molybdenite to evaluate the timing of oreformation. The δ34S values of pyrite from the ore deposit range from 0.7‰ to 5.60‰ with a mean at 2.70‰, close tomantle and meteorite sulphur. Among Pb isotopes, 206Pb/204Pb values range from 18.375 to 18.436, 207Pb/204Pb values from15.694 to 15.8, and 208Pb/204Pb values from 38.747 to 39.067. The δ13C values of calcite associated with the ores rangefrom −0.2‰ to −0.5‰ and their δ18O values show variation from 9.4‰ to 12.6‰, suggesting a mixed fluid source. The3He/4He and 40Ar/36Ar ratios of fluids trapped in pyrite are in the range of 0.27–1.11 Ra and 439.4–826, respectively, withcalculated proportion of the mantle-derived He ranging from 3.25% to 14.03% and atmosphere argon ranging from 35.8%to 67.3%. The data suggest that the ore-forming fluids were derived from the crust and were mixed with a distinctcontribution of mantle helium. The Re and Os values vary from 32 × 10−6 to 93.02 × 10−6 and from 0.01 × 10−9 to0.34 × 10−9, respectively. The model ages of molybdenite range from 126.96 ± 1.82 Ma to 129.49 ± 2.04 Ma, with aweighted mean age of 128.08 ± 0.75 Ma and isochron age of 130.3 ± 3 Ma. These ages are close to the age of the associatedquartz diorite porphyrite pluton, suggesting a close relationship between Cretaceous magmatism and metallogeny in NEChina. A comparison of the Yinan gold deposit in the Luxi area with those of the Jiaodong area shows that the contrast inmetallogenic features between the two are linked with the tectonic and geodynamic history.

Keywords: Re–Os geochronology; isotope geochemistry; Yinan gold deposit; Jiaodong gold deposits; NE China

1. Introduction

The North China Craton (NCC) is a collage of at leastthree major crustal blocks (Figure 1(a); Guo et al. 2014)which has been in focus in recent studies associated withcraton destruction, large-scale magmatism, and metallo-geny (e.g. Zhai and Santosh 2011; Guo et al. 2013; Liet al. 2013; Zhang et al. 2013). The magmatism in theNCC attained its peak during the Cretaceous period (Liet al. 2013) and was accompanied by the formation of avariety of mineral deposits (Shen et al. 2013a).

Gold is one of the most important mineral resources inthe NCC. The major gold deposits are located in theJiaodong peninsula (eastern margin of the NCC) withages in the range 130–110 Ma; the Xiaoqinling andXiong’ershan regions (southern margin of the NCC) withages between 128 and 126 Ma; and, in addition, Jibeiregion (northern margin of the NCC) with ages from239–175 Ma (Li and Santosh 2013).

Shandong Province along the southeastern margin of theNCC is the largest gold producing region in China. The goldreserves in this region occupy more than 25% of the totalreserve of the country and yield about 30 t bullions per year,with 90% of the gold deposits concentrated in the Jiaodong

area (Zhai et al. 2001; Zhou et al. 2002; Fan et al. 2005; Liet al. 2006; Guo et al. 2013; Yang et al. 2013). The region isdivided into two sectors, the Jiaodong to the east and Luxi tothe west, by the Tan-Lu Fault. The Jiaodong gold depositscan be divided into three main types: altered rock type(Sanshandao, Jiaojia, Xincheng, Dayigezhuang), quartzvein type (Linglong, Denggezhuang, Rushan), and interstra-tified breccia type (Pengjiakuang, Fayunkuang) (Li 2002; Liet al. 2007a, 2007b). The Luxi area has much less goldcompared with the Jiaodong area, both in the number ofdeposits and their size. The mineralization in the Luxi areaincludes cryptoexplosive breccia type (Guilaizhuang,Zhuojiazhuang), skarn type (Yinan), ancient karst type,layered disseminated limestone type, quartz vein type, andporphyry altered rock type (Zeng et al. 1999). The goldmineralization mainly occurs along the margin of the volca-nic complex or within the volcanic-breccia-related pipe, suchas those of the Guilaizhuang and Yinan gold deposits; thesetwo gold deposits are the most typical gold deposits in theLuxi area. The available age data from Jiaodong area showthat the ages from the granitoids can be divided into twogroups. The first group is between 165 and 150 Ma, asrepresented by the Linglong, Luanjiahe, Duogushan, and

*Corresponding author. Email: lisr@cugb.edu.cn

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Wendeng batholiths. The second group shows ages concen-trated in the 130–110 Ma range, such as the Guojialing,Weideshan, Sanfushan, Aishan, and Laoshan batholiths.Similarly, the dioritoids from the Luxi area also show twoage groups: the Tongshi complex with ages in the range190–175 Ma and the Tongjing and Jinchang complexeswith ages in the range 135–113 Ma. The ages of miner-alization of the Jiaodong area are between 137 and 71 Ma,with the majority of data converging around 120 ± 10 Ma(Guo et al. 2013), such as the Linglong gold deposit (123–122 Ma), Jiaojia gold deposit (120 Ma), Xincheng golddeposit (120 Ma), Denggezhuang gold deposit (117.5 Ma),and so on (Li and Santosh 2013). The ages of mineralizationin Luxi area mainly include two stages: 180–170 Ma(Guilaizhuang gold deposit) and 133–128 Ma (Yinan golddeposit) (Guo et al. 2013). Whereas considerable work hasbeen done on the Jiaodong area with respect to gold miner-alization and crustal evolution history (e.g. Guo et al. 2013;Yang et al. 2013, and references therein), information on theLuxi region is sparse.

Magmatic rocks related to mineralization of skarn-typegold deposits in China were mainly formed in the lateYanshanian (J–K), the ore bodies are mainly distributedin or near the contact zone of the intrusion and surround-ing rocks. The skarn-type gold deposits in China aremainly concentrated in the eastern region, such as theNCC, the middle and lower reaches of the Yangtze

River, and eastern coastal areas. In tectonic setting, thesegold deposits are mainly distributed in the continentalcollision orogenic belt, epicontinental active belt, andintracontinental fracture magmatic belt (Chen et al.1997). The Yinan gold deposit, which is located in theeast margin of the Luxi area and adjacent to the Tan-Lufault, belongs to a typical skarn deposit (Dong 2008).Previous studies in this area focused on the relationshipbetween magmatism and mineralization, metallogeniccharacteristics, fluid inclusions, stable isotopes, and geo-chronology (Chen et al. 1995; Qiu et al. 1996; Zhen andLuo 1996; Dong 2008; Gu et al. 2008; Li et al. 2009; Liuet al. 2009; Hu et al. 2010; Wang 2010). However, theprecise mineralization age of this deposit has not beenreported as yet and a comparison of the ore systemsbetween Luxi and Jiaodong has also not been attempted.

In this article, we present isotope geochemistry andmolybdenite Re–Os ages in understanding the ore genesisand timing of ore formation. We also attempt to evaluatethe distinction between the Yinan gold deposit and thosein the Jiaodong gold deposits.

2. Geological setting and ore deposit characteristics

2.1. Regional geology

Shandong Province is located at the southeastern marginof the NCC and is part of the Mesozoic circum-Pacific

Figure 1. (a) Major tectonic units of the NCC (modified after Xu et al. 2009; Zhai and Santosh 2011; Shen et al. 2013b). (b) Thelocation of Yinan gold deposit within Shandong Province: WB, Western Block; EB, Eastern Block (modified after Xu et al. 2009; Zhaiand Santosh 2011; Shen et al. 2013b). (c) Sketch map of the geology and major mineral deposits of Shandong Province (modified afterXu et al. 2002; Guo et al. 2013).

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tectonic and metallogenic belt (Goldfarb et al. 2013). TheTan-Lu fault, a major corridor of fluids and magmas dur-ing the Mesozoic, divides the Shandong region into theJiaodong sector to the east and the Luxi sector to the west(Figure 1, Liu et al. 2004; Guo et al. 2013).

The basement rocks of the Luxi area are made up ofthe Neoarchaean Taishan Group and Palaeoproterozoicgranitoids. The Taishan Group is mainly composed ofplagioclase amphibolites, biotite granulites, and TTGgranitoids (Song et al. 2001). These rocks are overlainby Palaeozoic, Mesozoic and Cenozoic carbonate, clastics,and volcanic rocks. The Palaeozoic strata includeCambrian–Ordovician carbonate rocks, Carboniferous–Permian marine strata, and continental coal-bearing clasticrocks. The Mesozoic sequence, in which Triassic forma-tions are absent, is dominated by Jurassic and Cretaceouscontinental clastic rocks. The Cenozoic sequences aremainly terrigenous clastic sedimentary rocks capped byvolcanic rocks (Niu et al. 2004).

2.2. Ore deposit characteristics

The Yinan gold deposit consists of three ore districts, theTongjing, Jinlong, and Jinchang, which are located on thewestern side of the Yishu fault zone along the southeasternmargin of the Luxi block. The Jinlong area is located inthe axial of the Tongjing anticline. The Yinan gold depositis obviously controlled by faults; the ore-controlling faultsprovided the pathways for ore-bearing hydrotherm upwel-ling and the space for mineralization. The Tongjing andJinlong regions occur at the intersection of the NNETangwu-Gegou fault and the NW Majiawo-Tongjingfault. The Jinchang region is located at the conjunctionof the NNE Zaolinzhuang fault and the NW Mamuchi-Jinchang fault. Cambrian strata invaded by magmatic

intrusions are well developed in this area, a setting favour-able for ore mineralization (Figures 1 and 2).

Because of the tiny stratigraphic inclination angle, theoutcrop in the ore district is not complete, only the upperstrata were exposed. The strata in the Yinan gold depositmainly include the Quaternary and Cambrian sedimentaryrocks. The major sedimentary units in the Jinchang oredistrict are the Gushan limestone, shale, Zhangxia lime-stone, and Mantou limestone, sandstone, and shale. TheJinchang intrusive complex is mostly composed of mon-zonitic granite, granite porphyry, quartz diorite porphyry,and hornblende granite porphyry. The sedimentary rocksin the Tongjing ore district are mainly composed of theZhangxia limestone and Zhushadong limestone. TheTongjing intrusive complex is mainly quartz diorite por-phyry, and the formation of quartz diorite porphyry isearlier than other magmatic rocks in the Yinan area(Table 1, Figure 3).

The ore bodies mainly occur in the contact zone ofthe intermediate-acidic intrusive bodies (which is mainlyquartz diorite porphyry) and the surrounding rocks, andalso in the interlayer slip zone and the unconformitysurface of the strata (Figure 4(a)). They are small–medium in scale, with bedded, lenticular, and other com-plex shapes. Most of the ore bodies extend for about140–200 m in length and their lengths along the dippingdirection are about 100–150 m. The thicknesses of theore bodies range from 0.49 to 11.61 m. The ore bodiesare enriched in Au–Cu–Fe, and the average gold grade is1.13–5.03 g t−1, the average copper grade is 0.49–0.81 g t−1,and the average iron grade is 27.04–33.43 g t−1 (Figure 4(b)).The wall rock alteration has mainly three types: (1) ther-mal contact metamorphism– hornfels and marble, whichare formed by the thermal metamorphism; (2) contactmetasomatism– skarn, which is widely developed in

Figure 2. Regional geological sketch map of the Yinan gold deposit.

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contact zone of the intrusion and the calcareous rocks; and(3) hydrothermal alteration distributed in a wide range,particularly in the tectonic developed zone, whichincludes chloritization, carbonatation, etc.

The typical ore types in the Yinan gold deposits aremainly magnetite with gold and copper (Figure 7).Metallic minerals in the ore mainly include native gold,pyrite, chalcopyrite, and magnetite, followed by bornite,

molybdenite, and specularite. The non-metallic mineralsare mainly garnet, diopside, epidote, quartz, calcite, andchlorite (Figures 5 and 6).

Ore structures include granular, metasomatic, reactiontype, fillings, and residual or emulsion type. Among these,granular structure is the most common (Figures 5 and 6).The ore textures are mainly massive, disseminated,mottled, veined, brecciated, and banded (Figure 7).

Table 1. Isotopic ages of the major intrusions in the Yinan gold deposit.

Pluton name Test objects Test method Age (Ma) References

Tongjing complex Diorite K–Ar 125.5 Zheng and Luo (1996)Diorite porphyry K–Ar 117.5Quartz diorite K–Ar 121.5 The Eighth Geological Team of Shandong Province (1981)Quartz diorite porphyry U–Pb 128 Guo et al. (2014)Quartz diorite porphyry U–Pb 128–129 Wang et al. (2011)

Jinchang complex Granodiorite K–Ar 125.5 The Eighth Geological Team of Shandong Province (1981)Monzonitic granite porphyry K–Ar 116.8Gabbro K–Ar 121.5 Wang and Wang (1987)Granodiorite porphyry K–Ar 116.4Granite porphyry K–Ar 105.4

Figure 3. (a) Geological sketch map of the Jinchang ore district (modified after Dong 2008). (b) Geological sketch map of the Tongjingore district (modified after Dong 2008).

Figure 4. (a) Schematic profile map of the Yinan gold deposit. (b) Sketch profile map of the typical ore body in the Yinan gold deposit(modified after Dong 2008).

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Based on the ore textures, structures, and mineralassociations, we divide the ore-forming processes intofive stages. (I) skarn stage: mainly output some anhydroussilicate minerals, including grossular, andradite, diopside,etc. (II) Retrograde alteration stage: mainly formed epidoteand a small amount of diopside. (III) Oxide stage: theformed metallic minerals are magnetite and haematite,and non-metallic minerals are mainly a little of quartzand epidote. (IV) Quartz-sulphide stage: a great deal ofpolymetallic sulphide was produced in this stage, such aspyrite, chalcopyrite, and bornite; non-metallic minerals aremainly quartz, chlorite, and calcite. (V) Supergene stage:mainly formed haematite, malachite, limonite, quartz, and

calcite. Stages I, II, and IV are ore-being, but Stage IV isthe main ore-forming stage.

3. Samples and analytical methods

Samples for this study were collected mainly fromunderground mine workings. The samples for Re–Osisotopes were collected from drill core ZK7-3 at adepth of 716–726 m in the Jinchang ore district andall of these samples are euhedral flaky or crumbymolybdenite distributed in skarn. The samples forsulphur isotopes and lead isotopes were collected from+29 m and −230 m levels in the Jinlong ore district.

Figure 5. Representative photomicrographs showing the major metallic minerals of Yinan gold deposit. (a) Gold distributed within oraround grain margins of euhedral pyrite. (b) Native gold occurring in the internal or cracks of euhedral pyrite. (c) Euhedral flakymolybdenite distributed in skarn. (d) Flaky specularite embedded in chalcopyrite. (e) Euhedral tabular magnetite distributed inchalcopyrite. (f) Euhedral–subhedral magnetite occuring with chalcopyrite; the grain margin of magnetite is replaced by haematite.Mineral abbreviations: Ccp, chalcopyrite; Mag, magnetite; Py, pyrite; Au, gold; Ht, specularite; Hem, haematite; Mo, molybdenite.

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The samples for helium–argon isotopes were collectedfrom +29 m of tunnel in the Jinlong ore district and thesamples for carbon–oxygen isotopes were collectedfrom Tongjing ore district, +29 m of tunnel in Jinlongore district, and core samples of drill ZK7-3 in Jinchangore district. The samples for suphfur isotopes, lead iso-topes, and helium–argon isotopes are skarn and magne-tite with gold and copper, the samples for carbon–oxygen isotopes are magnetite with gold and copper,marble, limestone, and hornfels. The locations for allsamples are listed in Table 2.

After crushing and sieving of the representative sam-ples, we selected separated mineral grains of 0.2–1 g from

40–60 mesh under a binocular microscope, ensuring purityof more than 99%. The mineral separates were ground inthe agate mortar to less than 200 mesh. Re–Os isotopeanalysis was performed at the National GeologicalExperiment Centre of the Chinese Academy ofGeological Sciences. The other isotope analyses wereperformed at the Nuclear Industry Beijing GeologicalResearch Analysis and Test Research Centre.

Re–Os analyses involved sample decomposition, dis-tillation separation of Os, extraction and separation of Re,and mass spectrometry. The chemical processing of thesamples and mass spectrometry techniques followed thosedescribed in Du et al. (1994, 2001).

Figure 6. Representative photomicrographs showing the major non-metallic minerals of Yinan gold deposit. (a) Euhedral granulargarnet showing zoned structure with the cracks in the surface. (b) Euhedral granular garnet with anomalous extinction. (c) Euhedral–subhedral granular diopside; the mineral is locally replaced by chalcopyrite. (d) Grain margin replacement of granular garnet by chlorite.(e) Euhedral–subhedral granular epidote. (f) Laths of phlogopite replaced by chlorite, together with fluorite, scheelite, molybdenite, andother mineral. Mineral abbreviations: Ccp, chalcopyrite; Mo, molybdenite; Grt, garnet; Ad, andradite; Di, diopside; Ep, epidote; Chl,chlorite; Cal, calcite; Phl, phlogopite; Fl, fluorite; Sch, scheelite.

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Sulphur isotope composition was obtained by measuringSO2, after grinding the sulphide minerals and reacting themwith cuprous oxide in a specific proportion (pyrite is 1:10,chalcopyrite is 1:8). The samples were placed in a porcelainboat and processed at high temperatures. These were thenintroduced into a quartz tube and heated in vacuum condi-tions for oxidation (2.0 × 10−2 Pa, 980°C). The SO2 wasanalysed using a Delta V Plus gas isotope mass spectrometeronline system, and the analysis results were reported withrespect to CDT, with a precision of ±0.2‰.

The samples of pyrite and chalcopyrite from thequartz–sulphide phase were used for lead isotope analysis.The powdered sulphide fraction was acid treated with amixture of HF + HClO4. After decomposition and drying,HCl was added and dried again, and finally 0.5 mol/l HBr

was added to dissolve the samples for the separation oflead using the anion exchange resin procedure (Li et al.2009). Thermal surface ionization mass spectrometry wasused to analyse the lead isotope using an IsoProbe-T massspectrometer.

Carbon and oxygen isotopic compositions of carbo-nates were obtained by measuring the CO2. The samplepowders were treated with 100% phosphoric acid invacuum under constant temperature for 4 hours. Pureseparation water generated by the freezing method col-lected the pure CO2 gas, which was separated and ana-lysed with a MAT 253 mass spectrometer. The results ofthe analysis were reported on the basis of PDB andSMOW for carbon and oxygen isotopes, respectively,and the analytical precision is better than ±0.2‰.

Table 2. The location (latitude and longitude) for all samples.

Samples Location Longitude Latitude

Sulphur isotope Jinlong ore district 118° 28′ 42.79 35° 35′ 36.09Lead isotope Jinlong ore district 118° 28′ 42.83 35° 35′ 36.11Re–Os isotopes Drill ZK7-3 118° 23′ 43.67 35° 35′ 33.61Carbon–oxygen isotopes Jinlong ore district 118° 28′ 42.63 35° 35′ 36.02

Tongjing ore district 118° 28′ 52.13 35° 36′ 4.39Drill ZK7-3 118° 23′ 43.67 35° 35′ 33.61

Helium–argon isotopes Jinlong ore district 118° 28′ 42.79 35° 35′ 36.09

Figure 7. Photographs of different ore types and mineral assemblages in the Yinan gold deposit. (a) Dense disseminated chalcopyrite ingarnet skarn. (b) Taxitic chalcopyrite and quartz, and calcite veins in magnetite ore. (c) Polymetallic sulphide and quartz, and calcite veinsin magnetite ore. (d) Banded epidote and magnetite in ore. Mineral abbreviations: Ccp, chalcopyrite; Py, pyrite; Ep, epidote; Grt, garnet;Qtz, quartz; Cal, calcite.

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He–Ar isotopes analyses were performed on fluidinclusions in pyrite of the quartz–sulphide stage. Themineral fractions were ultrasonically cleaned with acetone,heated to 120°C, and degassed for 24 hours in a vacuum.The mineral grains were crushed to release the gases,which were then purified by titanium sponge pump, zirco-nium aluminum pump, active carbon, and freezing byliquid nitrogen. The He and Ar extracted by standardtechniques (e.g. Cai et al. 2008) were analysed in aHelix SFT inert gas mass spectrometer.

4. Results

4.1. Rhenium–osmium isotopes and chronology

The results of Re–Os isotope analysis of molybdenite fromthe Yinan gold deposit are listed in Table 3. The Re andOs values range from 46.32 × 10−6 to 93.02 × 10−6 and0.01 × 10−9 to 0.34 × 10−9. The model ages of sevenmolybdenite samples range from 126.96 ± 1.82 to129.49 ± 2.04 Ma.

4.2. Sulphur isotopes

Sulphur isotope analyses are presented in Table 4. Theδ34S values of 29 samples (seven samples from this study,and the rest compiled from previous studies) range from0.7‰ to 5.60‰ with the mean value of 2.70‰.

4.3. Lead isotopes

Lead isotope data from the Yinan gold deposit are listedin Table 5. The results show 206Pb/204Pb values of18.375–18.436 (average 18.405); 207Pb/204Pb values of15.694–15.8 (average 15.736); and 208Pb/204Pb valuesof 38.747–39.067 (average 38.876).

4.4. Carbon–oxygen isotopes

Carbon and oxygen isotope analyses of carbonate fromthe Yinan gold deposit are listed in Table 6. The δ13Cvalues of calcite range from −0.2‰ to −0.5‰ with an

Table 3. Rhenium and osmium isotopic composition of the Yinan gold deposit.

Re (ng/g)Common Os

(ng/g) Re187 (ng/g) Os187 (ng/g)Model age

(Ma)

Sample Weight (g) Value 2σ Value 2σ Value 2σ Value 2σ Value 2σ

ZK73-2 0.03051 47624.461 425.448 0.1604 0.0081 29932.927 267.408 63.3806 0.4938 126.96 1.82ZK73-4 0.02047 50979.228 560.561 0.1318 0.0149 32041.465 352.337 67.9599 0.5514 127.18 2.02ZK73-8 0.02026 51317.644 608.769 0.1889 0.0147 32254.165 382.639 69.2264 0.5429 128.69 2.11ZK73-9 0.02048 93015.289 1091.682 0.0127 0.0284 58461.970 686.171 125.5227 0.9907 128.74 2.10ZK73-10 0.02111 74129.966 957.912 0.3420 0.0152 46592.166 602.094 99.2468 0.7822 127.72 2.19ZK73-13 0.02016 67999.075 741.698 0.2365 0.0150 42738.779 466.189 92.2978 0.7344 129.49 2.04ZK73-14 0.02021 46329.682 511.389 0.0133 0.0149 29119.132 321.430 62.2036 0.4892 128.09 2.02

Table 4. Sulphur isotope composition of the Yinan gold deposit.

Sample Mineral δ34SCDT‰ Reference

JL-29-1 Pyrite 0.7JL-29-2 Pyrite 1.4JL-29-5 Pyrite 1.3JL-29-6 Pyrite 0.8 This studyJL-29-7 Pyrite 1.5JL-230-1 Pyrite 1.7JL-230-4 Chalcopyrite 0.9

TJ30-12 Pyrite 2.5KS50-12 Pyrite 3.6ZK66-1-42 Pyrite 3.5ZK24-20-107 Pyrite 3.0DJSB3-2 Pyrite 1.5TJ30-12 Chalcopyrite 2.7Kg30-8 Chalcopyrite 4.3 Dong (2008)KS10-4 Chalcopyrite 2.6KS50-12 Chalcopyrite 4.1MW280-B1 Chalcopyrite 3.0ZK67-1-22 Chalcopyrite 3.8DJSB3-2 Chalcopyrite 2.0

JC-8 Pyrite 3.4JC-40 Pyrite 2.8JC-25 Chalcopyrite 1.9 Qiu et al. (1996)JC-32(1) Chalcopyrite 3.5JC-47(3) Chalcopyrite 2.0JC-49(1) Chalcopyrite 3.4

S-1 Pyrite 4.1S-2 Pyrite 5.6 Wan (1992)S-3 Pyrite 2.1S-4 Pyrite 4.7

Table 5. Lead isotope composition and parameters of the Yinangold deposit.

Sample Mineral 206Pb/204Pb 207Pb/204Pb 208Pb/204Pb

JL-29-1 Pyrite 18.375 15.694 38.747JL-29-6 Pyrite 18.392 15.698 38.767JL-29-2 Pyrite 18.400 15.715 38.819JL-230-5 Pyrite 18.386 15.724 38.827JL-230-1 Chalcopyrite 18.428 15.753 38.932JL-230-4 Chalcopyrite 18.417 15.749 38.913JL-29-7 Pyrite 18.408 15.757 38.934JL-29-5 Pyrite 18.436 15.800 39.067

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average of −0.36‰. The δ18O values range from 9.4‰ to12.6‰ with an average of 10.52‰. The δ13C values ofmarble range from −0.3‰ to −0.6‰ with an average of−0.45‰, the δ18O values range from 18.9‰ to 19.2‰ withan average of 19.05‰. The δ13C values of limestone rangefrom −0.1‰ to −0.2‰ with an average of −0.15‰, theδ18O values range from 18.5‰ to 19.7‰ with an averageof 19.1‰. The δ13C value of hornstone is −0.4‰, the δ18Ovalues is 19.3‰. δ18OSMOW values were calculated basedon the equation 18OSMOW = 1.03086 × 18OPDB + 30.86(Friedman and O’Neil 1977).

4.5. Helium–Argon isotopes

Helium and argon isotope data on the Yinan gold depositare listed in Table 7. The 3He/4He ratios of pyrite are inthe range 0.27–1.11 Ra (Ra is the 3He/4He ratio ofair = 1.4 × 10−6) with a mean value at 0.62 Ra. The resultsfall between the crust 3He/4He (0.01–0.05 Ra) and themantle 3He/4He (6–7 Ra). The 40Ar/36Ar ratios show varia-tion from 439.4 to 826 with an average of 575.3, which isclose to the 40Ar/36Ar value of the atmosphere (295.5).

5. Discussion

5.1. The ore-forming age of Yinan gold deposit and therelation to magmatism

In skarn-type ore deposits, the timing of mineralization isbroadly coincident with the time of magma emplacement(Shen et al. 2013a). From Table 3, the model ages of

molybdenite range from 126.96 ± 1.82 to 129.49 ± 2.04Ma, with the weighted mean age at 128.08 ± 0.75 Ma[MSWD = 0.84]. The isochron age is 130.3 ± 3 Ma(Figure 8) [MSWD = 0.96]. The isochron age is closelycomparable with the weighted mean age within the errorrange, which shows the reliability of our data. In addition,common osmium content in the samples is very low, closeto zero, illustrating that the 187Os in our samples is theproduct of the decay of 187Re, confirming the validity ofthe model age. We interpret the Re–Os weighted mean ageto represent the timing of mineralization in the Yinan golddeposit at 128.08 ± 0.75 Ma. Previous studies haveobtained many K–Ar ages of Tongjing complex andJinchang complex (Table 1). The Re–Os age obtainedfrom molybdenite in the skarn ore of the present study ismarkedly consistent with the U–Pb ages of 128.0 ± 5.4 Ma(Guo et al. 2014) and 128–129 Ma (Wang et al. 2011)obtained from zircons in the quartz dioritic porphyritepluton. The ages of the granitoids are significantly laterthan the quartz dioritic porphyrite. This suggested theclose link between the formation of the Yinan gold depositand the emplacement of the quartz dioritic porphyrite, butthe granitoids seemed to be less associated with goldmineralization.

5.2. The evidence for crust–mantle input

The rhenium content in the molybdenite can be used totrace the source of ore-forming materials (Stein et al.1997; Mao et al. 1999a, 1999b). Based on a comprehen-sive analysis and comparison of the Re content in molyb-denite of various types of molybdenum deposit in China,Mao et al. (1999b) observed a range from mantle source tocrust–mantle mixed source to crust source. The Re contentof molybdenite in the Yinan gold deposit ranges from46.32 × 10−6 to 93.02 × 10−6 with an average of61.62 × 10−6, suggesting that the ore-forming materialsare dominated by a mixed crust–mantle source.

The sulphide minerals in Yinan gold deposit aremainly pyrite and chalcopyrite. In the frequency histogram(Figure 9(a)), the sulphur isotopic composition is locatedin a narrow range representing equilibrium sulphur isotopefractionation and a dominantly single source. The δ34Svalues in the range 2–4‰ are comparable to the valuesof magmatic sulphur. Taking the maximum δ34S value(30‰) of early Palaeozoic sea-water sulphate as one of

Table 6. Carbon and oxygen isotopic composition of the Yinangold deposit.

Sample Test objectδ13CV-

PDB‰δ18OV-

PDB‰δ18OV-

SMOW‰

TJ-5 Calcite −0.5 −19.9 10.4TJ-6 Calcite −0.4 −20.6 9.6TJ-7 Calcite −0.4 −20.8 9.4JL-29-1 Calcite −0.3 −19.7 10.6JL-29-3 Calcite −0.2 −17.8 12.6ZK7-3-21 Marble −0.6 −11.4 19.2ZK7-3-22 Marble −0.3 −11.6 18.9ZK7-3-23 Limestone −0.2 −12.1 18.5ZK7-3-24 Limestone −0.1 −10.9 19.7ZK7-3-25 Hornstone −0.4 −11.3 19.3

Table 7. Helium and argon isotopic composition of the Yinan gold deposit.

Sample Mineral

4He(cm3STP · g−1)(10−7) 40Ar/36Ar

40Ar(cm3STP · g−1)(10−7)

3He(cm3STP · g−1)(10−13) 3He/4He R/Ra

JL-29-2 Pyrite 1.80 826 2.07 2.81 15.60 1.11JL-29-5 Pyrite 5.86 439.4 1.10 3.94 6.72 0.48JL-29-7 Pyrite 4.33 460.4 2.28 1.63 3.77 0.27

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the endmembers (Hoefs 1997) and sulphur from mantle asanother endmember (0‰), we calculated the ratio of thecontribution of these two kinds of sulphur sources. Thesulphur sourced from early Palaeozoic sea-water sulphateis 2.3–18.7% and the sulphur sourced from mantle is81.3–97.7%. The sulphur isotopic composition of Yinangold deposit suggested that the sulphur was derived frommantle and mixed with crustal material.

We plot the lead isotope data of pyrites and chalco-pyrite from the Yinan gold deposit on lead isotope evolu-tion diagrams (Zartman and Doe 1981; Li and Santosh2013). In the Pb208/Pb204–Pb206/Pb204 diagram (Figure10(b)), all of the data are located between the mantleand lower crust evolution line, illustrating that the leadin these ores mainly comes from a deep source. However,in the Pb207/Pb204–Pb206/Pb204 diagram (Figure 10(a)),all samples plot outside the upper crust evolution line,suggesting crustal contamination. These are commonfeatures of skarn deposits, indicating that the metallo-genic components are derived from both magmatic andsedimentary sources.

In the carbonate δ18OV-SMOW and δ13CV-PDB composi-tion diagram (Liu et al. 1997; Liu et al. 2004, Figure 11),four data from the hydrothermal calcite samples fall in thegranite source area and one falls between granite andmarine carbonate. The data suggest that the source ofore-forming fluid is mainly magmatic, with a minor mix-ing with the marine carbonate strata into which the magmaintruded.

The data of two marble samples and two limestonesamples are close to the data of hornfels samples, fallingbetween granite and marine carbonate, and illustrating thatthe host rocks of the ore bodies (limestone) or marble andhornfels were affected by the magmatic hydrothermal event.The oxygen isotope values show obvious loss of 18O cor-responding isotopic exchange between the magmatic fluidsand surrounding calcareous sedimentary rocks.

5.3. The source of ore-bearing fluids

The initial isotopic composition of helium and argontrapped within fluid inclusions in pyrite is mainly

Figure 8. (a) Re–Os isochron plot for molybdenite samples from the Yinan gold deposit. (b) Weighted average Re–Os ages of themolybdenites from Yinan gold deposit.

Figure 9. (a) Histogram of sulphur isotopic composition of the Yinan gold deposit. (b) Sulphur isotope compositions from the Yinangold deposit compared with the Jiaodong gold ore system and other major geological settings. Range for geological settings from Hoefs(1997). Range for Jiaodong gold ore system from Li and Santosh (2013).

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influenced by the analytical methods, ore-forming fluids,diffusion loss, and radioactive helium, argon, and cosmo-genic 3He (Hu et al. 1998). The inclusions in pyrite in thisstudy are mainly native inclusions, and the samples werecollected from underground tunnels, which exclude thepossibility of the influence from the factors above.Therefore, we believe that the data obtained can be takento represent the characteristics of the ore-forming fluidwhen the fluid inclusions were captured.

The noble gases in hydrothermal fluids may have threedifferent sources for helium and argon isotopes with dis-tinct ratios (Simmons et al. 1987; Stuart et al. 1995; Huet al. 1998, 2004). It is usually considered that the He–Arisotopic composition in the atmospheric saturated water isthe same as that in the surface atmosphere, with 3He/

4He = 1 Ra (Ra of the atmosphere 3He/4He ratio is1.4 × 10–6), 40Ar/36Ar = 295.5, and the 40Ar/4He ratioapproximately 0.001 (Simmons et al. 1987; Stuart et al.1995; Hu et al. 1999). Mantle fluid is characterized byhigh 3He, with 3He/4He in the range 6–9 Ra, 40Ar/36Ar > 20,000, and 40Ar/4He ratio of 0.33–0.56(Simmons et al. 1987; Hu et al. 1999; Cai et al. 2004).However, the 3He/4He ratio in typical crust is usually lessthan 0.1 Ra, the majority of cases even only 0.01–0.05 Ra,40Ar/36Ar often exceeds 45,000, and the 40Ar/4He ratio isgenerally in the range 0.16–0.25 (Simmons et al. 1987;Stuart et al. 1995; Hu et al. 1999; Feng et al. 2006).

The 3He/4He ratios of the Yinan gold deposit in therange 0.27–1.11 with a mean value of 0.62 are slightlyhigher than that of the crust (0.01–0.1 R/Ra), but markedly

Figure 10. Lead isotope diagrams for the Yinan gold deposit and the Jiaodong gold ore system. (a) and (b) based on Zartman and Doe(1981) and, Li and Santosh (2013).

Figure 11. Carbonate δ13C–δ18O composition diagram for the Yinan gold deposit (after Liu et al. 1997; Liu et al. 2004).

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lower than that of the mantle (6–9 R/Ra). According to thecrust–mantle mixing model, the proportion of mantle heliumcan be calculated by Hemantle (%) = [(3He/4He)samples

– (3He/4He)crust]/[(3He/4He)mantle – (3He/4He)crust] × 100

(Xu et al. 1995). Among these, 3He/4He ratios of crust are2 × 10−8 and the 3He/4He ratios of mantle are 1.1 × 10−5

(Stuart et al. 1995). Our calculations show that the proportionof the mantle-derived He in the pyrite from the Yinan golddeposit ranges from 3.25% to 14.03% with an average of7.74%. In the 3He–4He diagram (Figure 12(a)), all data fall inthe crust–mantle transition zone, close to the helium line ofcrust evolution.

The 40Ar/36Ar ratios in the range of 439.4–826 are higherthan that of the atmosphere (40Ar/36Ar = 295.5). The radio-genic Ar can be determined by Ar = [(40Ar/36Ar)samples– 295.5]/(40Ar/36Ar)samples. Calculation shows that the con-tent of radiogenic Ar ranges from 32.7% to 64.2% withan average of 44.2%. As a result, the contribution ofatmospheric Ar ranges from 35.8% to 67.3% with anaverage of 55.8%. Thus, the contribution of atmosphericAr is slightly higher than the radiogenic Ar, but the

difference is not big. In the R/Ra–40Ar/36Ar diagram(Figure 12(b)), the samples are all located between crustfluid and mantle fluid, and close to the region of airsaturated water.

In summary, our He–Ar isotope data indicate that theore-forming fluid of the Yinan gold deposit was mainlysourced from the crust and was mixed with a distinctcontribution of mantle helium.

5.4. Comparison of the Yinan gold deposit with theJiaodong gold ore system

A comparison of the sulphur isotopic composition of sometypical gold deposits in the Luxi and Jiaodong areas showsthat the δ34S values of Luxi gold deposits show lowervalues when compared with those of the Jiaodong golddeposits (Figure 9(b)). For example, in the Guilaizhuangexplosive breccia-type gold deposit of Luxi, δ34S valuesrange from 0.71‰ to 2.99‰ with a mean at 2.44‰ (Huet al. 2006), and the δ34S values of Yinan skarn-type golddeposit range from 0.7‰ to 5.60‰ with an average of

Figure 12. He and Ar isotopic composition diagrams of the fluids trapped in sulphide minerals from the Yinan gold deposit and theJiaodong gold ore system (modified from Winckler et al. 2001; Li and Santosh 2013). M, mantle-derived fluid field; C, crustal fluids field;and ASW, atmospheric saturated water.

Figure 13. (a) Plate tectonic sketch showing the petrogenesis of magmatism in Shandong Province (modified after Guo et al. 2013). (b)Metallogenic model of the Yinan gold deposit showing that its ore forming materials probably derived from crust–mantle mixed fluids.

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2.70‰. In contrast, δ34S values of quartz vein-type golddeposits in Jiaodong are 6.8–9.3‰, those of altered rock-type gold deposits are 8.5–12.5‰, and the δ34S values ofbreccia ores are 9.9–12.7‰, this suggests that the ore-forming minerals in Jiaodong gold deposits were probablysourced from a common reservoir of crust–mantle interac-tion (Mao et al. 2008). Therefore, the sulphur isotopiccomposition indicates that the ore-forming materials inLuxi and Jiaodong are different and the mantle contribu-tion in the Luxi area is greater than the jiaodong area. The206Pb/204Pb data on eight samples of sulphide mineralsfrom the Yinan gold deposit range from 18.375 to18.436 with an average of 18.405, 207Pb/204Pb valuesfrom 15.694 to 15.8 with an average of 15.736, and208Pb/204Pb values from 38.747 to 39.067 with an averageof 38.876. These data are distinctly different from the dataon the quartz vein-type and fracture alteration-type golddeposits in Jiaodong area (Pb206/Pb204 values of 16.40–-17.92 with an average of 17.13, 207Pb/204Pb values of15.20–15.72 with a mean at 15.45, and 208Pb/204Pb valuesof 37.26–38.60 with an average of 37.70), but similar tothe data of the strata-bound gold deposits (Li and Santosh2013). Lead isotope compositions of sulphides from theYinan gold deposits and those from Jiaodong gold oresystem show that Pb is mainly derived from the lowercrust and partly from a mantle source (Figure 10(a) and(b)), but in the Yinan gold deposit, which is a skarn-typedeposit, Pb contribution also comes from the sedimentarystrata. The carbon and oxygen isotopes data of calcitefrom the Yinan gold deposit show that the δ13C valuesrange from −0.2‰ to −0.5‰ with an average of −0.36‰,the δ18O values range from 9.4‰ to 12.6‰ with anaverage of 10.52‰. The values are similar to those ofbreccia-type ores in the Jiaodong area (the δ13C valuesare −0.1‰ to −4.8‰ with an average of −2.2‰, the δ18Ovalues are 2.9–12.4‰ with an average of 8.5‰), whereascompared with the quartz vein ores (the δ13C and δ18Ovalues average of −4.4‰ and 10.4‰) and altered rock-type ores (the δ13C and δ18O values average of −5.5‰ and12‰) (Mao et al. 2008), the values of Yinan gold depositare lower in δ18O but higher in δ13C. The carbon andoxygen isotopic composition also suggests that the ore-forming material comes from a mixture of crust and man-tle, obviously mixed with the carbonate rock. Helium andargon isotopic data on fresh pyrite samples from the Yinangold deposit show that the proportion of mantle sourcevaries from 3.25% to 14.03% with an average at 7.74%,which is greater than the mantle helium involved in thequartz vein-type gold mineralization of the Jiaodongpeninsula with an average of 6% and the mantle heliuminvolved in the strata-bound type of gold mineralizationwith an average of 4% (Li and Santosh 2013). The heliumand argon isotopes studies of the pyrite from the Yinangold deposit and Jiaodong gold ore system indicate thatthe ore-forming fluid was derived from the crust and

mantle source (Figures12(a) and (b)), but the contributionof mantle material in the Yinan gold deposit is signifi-cantly more than the Jiaodong gold ore system. Withregard to the magmatic rocks closely linked with goldmineralization, many studies have suggested that theGuojialing granodiorite in the Jiaodong area is formedby the interaction of partial melting of lower crust andthe upwelling of mantle (Hou et al. 2007; Jiang et al.2009), while the dioritoid in the Luxi area mainly derivedfrom the mantle (Wang et al. 2011). It also suggests thatthe contribution of mantle material in the Luxi area ismore than the Jiaodong area. However, the ages of mag-matism of these two regions are similar, such as the agesof Guojialing granodiorite in the Jiaodong area, which are inthe range of 126–130 Ma (Wang et al. 1998), and the ages ofquartz dioritic porphyrite in the Yinan area, which are around128 Ma, this shows that the mineralization in these tworegions may be the same issue of metallogenic events.

The differences between the Yinan gold deposit andJiaodong gold ore system are possibly related to thecontrast in the geological, structural, and geodynamicsettings of Luxi and Jiaodong. In terms of geologicalbackground, the magmatic units of Jiaodong area arefar more complex than those of Luxi area. Whereasabundant crustally derived granitoids are distributedwidely in Jiaodong, only small scattered dioritic plutonsare present in Luxi. In terms of geological structure, thedistribution of faults in Jiaodong is broadly similar to theYishu fault zone, trending mainly in a NE–NNE direc-tion, whereas the faults in Luxi area trend mainly in theNW direction. In addition, the Jiaodong area is moreclose to the margin of North China plate than the Luxiarea, and therefore witnessed more intense tectoniceffects from the Triassic continental collision and subse-quent Pacific-plate subduction from the east, thus favour-ing more metallogenic potential. As the Jiaodong area ismore close to the Pacific plate subduction zone, crust–mantle interaction is more strong beneath this region,with effective fluid and melt transfer from depth beingadjacent to the Tan-Lu fault zone (Xu et al. 2002; Guoet al. 2013). Moreover, previous studies (Guo et al. 2013)have shown that the mantle beneath the Luxi area ismainly of EM1 type, whereas the mantle beneath theJiaodong area is mainly of EM2 type, implying thatthere is more ancient lithospheric mantle beneath theLuxi area, whereas the Jiaodong region is characterizedby modified lithospheric mantle and asthenosphere input.So the mineralization differences between Jiaodong areaand Luxi area may be related to the different geodynamicsettings. Luxi area, which is located in the intraplateenvironment, witnessed less magmatism and metallogenycompared with Jiaodong Peninsula.

The various types of gold mineralization may be asso-ciated with the different sedimentation and denudationhistory in these two regions.

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We proposed a model in Figure13(a) to explain thepetrogenesis of magmatism in Shandong Province. Duringthe Early Cretaceous (130‒110 Ma), the Pacific plate sub-duction beneath the Eurasian plate led to dehydration ofthe underthrusted crust and large-scale mantle convectionin the asthenosphere, which transferred the mantle materi-als (fluid and melt) to the upper mantle and lower crust.The heat input into the bottom of the lithosphere from theupwelling asthenosphere caused the melting of lithospheremantle, and the modified mantle was underplated beneaththe lower crust of the Tan-Lu fault, channelling maficmagmas on both sides of the fault. The Jiaodong area,characterized by shallower lithosphere depth, witnessedmore asthenosphere mantle input, which induced extensivecrust–mantle interaction and voluminous felsic magmatism.In Luxi area, the mafic magmas generated the intermediate(calc-alkaline) and felsic magmatism as a result of crust–mantle mixing. However, compared with the Jiaodong area,the Luxi area is located in the intraplate environment, andthe lithosphere thickness here shows a sharp increase fromthe Jiaodong area (An et al. 2009; Guo et al. 2013).Therefore, the presence of more ancient mafic crust in thisregion is the dominant reason for the origin of mafic com-plexes in the Luxi area. In Figure 13(b), the Tongjingcomplex of the Yinan gold deposit formed accompaniedby a variable degree of crust and mantle mixing throughmantle-derived mafic magmatic intrusions. As recordedfrom our field investigations, the magmatic fluids producedat the later stage of complex formation mixed with thegroundwater, and crustal fluid caused the skarn forming,such as the thermal contact metamorphism, and the contactmetasomatism located in the contact zone of complex andsurrounding rock as well as its nearby, hydrothermal altera-tion effect are mainly distributed in the neck of the complexand within the contact zone.

6. Conclusions

(1) We report a molybdenite Re–Os age of128.08 ± 0.75 Ma, marking the timing of miner-alization in the Yinan gold deposit. The age com-pares well with the U–Pb zircon data from theassociated quartz dioritic porphyrite pluton, thuscorrelating the Yinan deposit with the dioriticmagmatism.

(2) The S, Pb, He–Ar, and C–O isotopic studies showthat the ore-forming materials of Yinan golddeposit were derived from mixed crust–mantlesources.

(3) According to the comparison of stable isotopes inthese two regions, we inferred that the contributionof mantle material in the Luxi area is significantlymore than the Jiaodong area.

FundingThis work was supported by the Key Programme of the NationalNatural Science Foundation of China [90914002], ChinaGeological Survey [1212011220926], and the specializedresearch fund for the doctoral programme of higher education[20130022110003]. This study also contributes to the TalentAward to M. Santosh under the 1000 Talents Plan of theChinese Government.

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