大别山千鹅冲钼矿区花岗岩的SHRIMP锆石U-Pb年龄、Hf同位素组成及微量元素特征**

高阳 叶会寿 李永峰 罗正传 李法岭 熊必康 孟芳GAO Yang, YE HuiShou*, LI YongFeng, LUO ZhengZhuan, LI FaLing, XIONG BiKang and MENG Fang

1. 中国地质科学院矿产资源研究所，国土资源部成矿作用与资源评价重点实验室，北京 1000372. 河南省有色金属地质矿产局，郑州 4500163. 河南省地矿局第三地质调查队，信阳 4640004. 中国地质大学，北京 1000831. MLR Key Laboratory of Metallogeny and Mineral Assessment, Institute of Mineral Resources, Chinese Academy of Geological Sciences, Beijing 100037, China2. Henan Provincial Non-ferrous Metals Geological and Mineral Resources Bureau, Zhengzhou 450016, China3. No. 3 Geological Survey, Henan Bureau of Geology and Mineral Resources, Xinyang 464000, China4. China University of Geosciences, Beijing 100083, China2013-09-02 收稿, 2013-12-07 改回.

1 引言

千鹅冲钼矿床位于秦岭-大别造山带东部的大别山地区，是东秦岭-大别钼矿带近年来发现的一处超大型钼矿床，已探明钼资源量60万吨，平均品位0.08%(李法岭，2011；Maoetal., 2011a)。2006年开始，河南省第三地质调查队在千鹅冲地区实现了找矿突破，发现了矿区南部南湾组片岩中的千鹅冲隐伏岩体及其上部的隐伏矿体，最终确定其为超大型规模，并且是大别山地区发现的第一个超大型钼矿床。千鹅冲钼矿床的发现不仅结束了大别山地区无超大型矿床的历史，同时对区域上找矿勘探也具有十分重要的指导意义。

自千鹅冲钼矿发现以后，多位学者就其成矿成岩时代、成矿流体特征等进行了研究。研究结果表明，千鹅冲钼矿辉钼矿Re-Os同位素年龄为128±8Ma(李法岭，2011；杨梅珍等，2010)，成矿作用发生在早白垩世；成矿流体为高温、高盐度、贫子晶、富CO2的流体系统(Yangetal., 2013)。钻探工程揭露矿体下部存在隐伏岩体，并且与矿体具有紧密的空间关系，所以对千鹅冲隐伏岩体进行年代学研究对于揭示成岩成矿关系及成矿机制都具有重要意义。本次研究对矿体下部隐伏的二长花岗岩和花岗斑岩进行了SHRIMP锆石U-Pb同位素定年，从而精确厘定了千鹅冲隐伏岩体的形成时代，并通过锆石原位Hf同位素及锆石微量元素分析，浅析千鹅冲隐伏岩体的成因、构造背景及与成矿的关系，同时为深入研究大别山地区白垩纪钼成矿作用与区域大规模花岗质岩浆作用的关系提供了重要依据。

2 区域地质背景

大别造山带是秦岭-大别-苏鲁造山带的组成部分，形成于三叠纪华北与华南两板块的碰撞拼合(图1)(张国伟等，2001；Hackeretal., 1998；Lietal., 2001；Ratschbacheretal., 2003)。大别造山带西起河南桐柏山，向西以南阳盆地为界与秦岭造山带相望，东侧为郯城-庐江断裂，此断裂使大别造山带和苏鲁造山带之间位移约500km。大别造山带南北边界分别为襄樊-广济断裂和栾川-明港-固始断裂。

大别造山带以商城-麻城断裂为界可分为东大别和西大别两部分。东大别从北到南分别以晓天-磨子潭断裂(XMF)、五河-水吼断裂(WSF)和太湖-马庙断裂(TMF)为边界可划分出4个岩石-构造单元(Lietal., 2001；向必伟，2009)：(1)北淮阳构造带，主要包括一套在华南板块向华北板块俯冲时刮削下来所形成的低级变质地体(Zhengetal., 2005)，变质岩原岩具有700～800Ma的锆石U-Pb年龄(Hackeretal., 2000；Chenetal., 2003)；(2)北大别杂岩带，主要由大规模白垩纪花岗岩及少量镁铁-超镁铁质侵入岩、新元古代TTG片麻岩和角闪岩、三叠纪榴辉岩、少量变质沉积岩和麻粒岩以及少量橄榄岩组成(Hackeretal., 2000；Bryantetal., 2004；Liuetal., 2005；Xuetal., 2000；Zhengetal., 2003)；(3)南大别高压-超高压变质带，以产出含柯石英和金刚石榴辉岩为特征(Wangetal.,1989)，主要包括榴辉岩、含石榴石橄榄岩、硬玉石英岩、大理岩、石榴石-二云母片岩及片麻岩(Hackeretal., 1998, 2000；Xuetal., 2003)；(4)宿松杂岩带，主要包含中-新元古代变质沉积岩和变质火山岩以及震旦纪大理岩(Youetal., 1996)。西大别具有与东大别相似的岩石-构造单元组成，不同的是西大别缺少与“北大别杂岩带”相对应的构造单元。

大别山地区发育大量中生代岩浆岩，其显著特点是全部形成于早白垩世，主要包括大量中酸性侵入岩及少量镁铁-超镁铁质岩和火山岩(Fanetal., 2004；Heetal., 2011, 2013；Huangetal., 2008；Wangetal., 2007；Zhaoetal., 2005)。早白垩世花岗岩类侵位时间为117～143Ma(Heetal., 2011；Wangetal., 2007)，可分为两期，早期岩体(130～143Ma)通常具有高的Sr/Y和La/Yb比值，而晚期岩体则通常不具备这一特征(Wangetal., 2007；Xuetal., 2007)。火山岩主要分布在北淮阳构造带内，主要包括玄武质粗安岩、粗安岩及粗面岩等(Fanetal., 2004)。镁铁-超镁铁质侵入岩主要发育在北大别杂岩带内，时代为123～130Ma，主要包括辉石岩、角闪石岩、辉长岩等(Daietal., 2011；Huangetal., 2007；Wangetal., 2005；Zhaoetal., 2005)。

目前在大别山地区发现的斑岩型钼矿床主要分布在中西部的北淮阳构造带及临近地区(图1)。斑岩钼矿与早白垩世中酸性小斑岩体具有紧密的时空关系，其产出明显受网格状断裂构造的控制。

图1 桐柏-大别山地区地质图(据Ratschbacher et al., 2003修改)白垩纪花岗岩及镁铁-超镁铁质岩引自Ratschbacher et al., 2003；He et al., 2011；Zhao et al., 2005. ZXF, GMF, XMF, TSF, DSHF, SMF, WSF, TMF and TLF分别代表朱阳关-夏馆断裂、龟山-梅山断裂、晓天-磨子潭断裂、桐柏-商城断裂、陡山河断裂、商城-麻城断裂、五河-水吼断裂、太湖-马庙断裂及郯城-庐江断裂Fig.1 Generalized geological map of the Tongbai-Dabie area in East China (modified after Ratschbacher et al., 2003)Cretaceous granites and mafic-ultramafic intrusive rocks are from Ratschbacher et al., 2003; He et al., 2011; Zhao et al., 2005. ZXF, GMF, XMF, TSF, DSHF, SMF, WSF, TMF and TLF represent the Zhuyangguan-Xiaguan Fault, the Guishan-Meishan Fault, the Xiaotian-Mozitan Fault, the Tongbai-Shangcheng Fault, the Doushanhe Fault, the Shangcheng-Macheng Fault, the Wuhe-Shuihou Fault, the Taihu-Mamiao Fault and Tancheng-Lujiang Fault, respectively

3 矿床地质特征

千鹅冲钼矿床位于西大别北淮阳构造带内，区域性桐柏-商城断裂带北侧(图1)。矿区出露地层比较简单，绝大部分为泥盆系南湾组(Dn)浅变质云母石英片岩系，另外在矿区西南部边界分布少量震旦系-下奥陶统肖家庙岩组(Z-O1x3)地层以及沟谷中出露的第四系(图2)。区内地层走向北西西，与区域构造线一致。肖家庙岩组与南湾组以桐-商韧性剪切带为界，呈构造接触，构造带以南为肖家庙岩组地层，以北为南湾组地层。

矿区内无大的褶皱构造，构造主要为断裂构造。断裂构造分为韧性断裂和脆性断裂。韧性断裂为区域性桐(柏)-商(城)韧性剪切带的一部分，出露于矿区南部，为肖家庙岩组与南湾组地层的分界(图2)，韧性剪切带内的构造岩以云英质构造片岩为主，次为长英质变晶糜棱岩。脆性断裂是矿区内的主要构造形态，主要发育在矿区中部南湾组地层中，主要为北西西向和近南北向两组。地表沿断裂分布一系列构造蚀变岩带，带内岩石发生较强硅化、钾长石化、碳酸盐化及褐铁矿化，部分地段发现钼、铜、铅锌、银矿化。

千鹅冲矿区地表无大岩体出露，经钻探验证，在矿区中南部存在隐伏岩体(图2b)，钻孔揭露其顶部标高为-512.71～-751.29m，岩体呈起伏状与围岩侵入接触，局部有震碎现象。钻孔控制隐伏岩体平面投影面积约0.262km2。该岩体为矿区钼矿的成矿母岩，其与围岩接触带可见强弱不等的蚀变，类型主要有硅化、钾长石化、绢云母化和黄铁矿化，并伴生钼矿化，但矿化强度弱于上部围岩。岩体主要由花岗斑岩和二长花岗岩组成，钻孔中揭露的花岗斑岩含量远多于二长花岗岩，二长花岗岩只在局部可见。除此之外，区内燕山晚期中酸性小型脉岩较发育，按岩石类型可分为闪长玢岩脉、煌斑岩脉、石英斑岩脉和花岗斑岩脉。

除少量矿体产于隐伏岩体内接触带，绝大部分矿体产于南湾组片岩中。赋矿岩石主要为绿帘黑云石英片岩、绿帘黑云片岩、含绿帘二云石英片岩、黑云斜长石英片岩、黑云石英片岩等，矿体与围岩均呈渐变过渡关系，无明显界限。金属矿物主要为辉钼矿、黄铁矿、黄铜矿、方铅矿、闪锌矿、磁铁矿、赤铁矿等；脉石矿物主要为石英、钾长石、绿帘石、方解石、黑云母、绢云母、白云母、绿泥石、萤石。主要的矿石结构包括自形-半自形-他形结晶结构、交代结构、压碎结构、固溶体出溶结构等。矿石构造类型主要有脉状构造、浸染状构造、角砾状构造等。矿区内常见的围岩蚀变有硅化、钾长石化、黄铁矿化、绢云母化、绿帘石化、绿泥石化、碳酸盐化等，多叠加出现，强弱不等。以硅化、钾长石化、黄铁矿化、绢云母化发育较强。

图2 千鹅冲钼矿地质简图及勘探线剖面图(据河南省地矿局第三地质调查队，2011*河南省地矿局第三地质调查队. 2011. 河南省光山县千鹅冲钼矿勘探报告)

Fig.2 Simplified geological map and cross-section of the Qian’echong Mo deposit

图3 千鹅冲岩体手标本及显微照片(a)-二长花岗岩与花岗斑岩的侵入接触关系；(b)-二长花岗岩；(c)-花岗斑岩. Q-石英；Kf-钾长石；Pl-斜长石；Bi-黑云母；Chl-绿泥石Fig.3 Hand specimens and photomicrographs showing petrology of Qian’echong stock(a)-intrusive contact relationship of monzogranite and granite porphyry; (b)-monzogranite; (c)-granite porphyry. Q-quartz; Kf-K-feldspar; Pl-plagioclase; Bi-biotite; Chl-chloritic

4 样品描述及分析方法

本次研究所采集的二长花岗岩(QEC-7)和花岗斑岩(QEC-8)来自ZK005钻孔985m处，可见花岗斑岩在与二长花岗岩的接触部位有冷凝边(图3a)，其形成晚于二长花岗岩。其中，二长花岗岩为灰白色，细粒结构，块状构造(图3b)。主要矿物为石英(20%～25%)、正长石(35%～40%)、斜长石(30%～35%)；次要矿物为黑云母，含量2%～4%；副矿物主要有锆石、磷灰石、榍石、磁铁矿、钛铁矿等，含量1%～3%。大部分岩石发生较强的硅化。花岗斑岩，肉红色-暗红色，斑状结构，块状构造(图3c)。斑晶含量15%～20%，主要为正长石(40%～50%)、石英(35%～40%)、斜长石(15%～20%)及少量黑云母；基质含量约为80%，矿物组成同斑晶，粒度0.1～0.4mm；副矿物主要有磁铁矿、钛铁矿、锆石、磷灰石等，含量为1%～5%。岩石普遍发生较强烈的钾硅酸盐化及硅化蚀变。

图4 千鹅冲钼矿二长花岗岩和花岗斑岩代表性锆石阴极发光图像及测点位置、U-Pb年龄和εHf(t)值Fig.4 Cathodoluminescence (CL) images of representative zircon of monzogranite and granite porphyry from the Qian’echong Mo deposit with analytical numbers, U-Pb ages and εHf(t)

将岩石样品破碎，经重力和磁选后在双目镜下挑选出锆石颗粒，并与标准锆石一起置于环氧树脂做成样品靶，进行锆石透、反射光、阴极发光照相，以及SHRIMP定年、Lu-Hf同位素分析和锆石微量元素测试。

锆石分选工作在廊坊市地源矿物测试分选技术服务有限公司完成。锆石阴极发光(CL)照相在中国地质科学院地质研究所北京离子探针中心完成。锆石U-Pb年龄数据是在中国地质科学院地质研究所北京离子探针中心的网络虚拟实验室，通过SHRIMP远程共享控制系统(SHRIMP Remote Operation System, SROS)远程控制位于澳大利亚Curtin理工大学(Curtin University of Technology)的SHRIMP II仪器获得的，详细测试方法见Williams(1998)。SHRIMP远程共享控制系统(SROS)由北京离子探针中心、中国计量科学研究院和吉林大学共同研发，可以实现通过Internet公共网络，远程控制SHRIMP II仪器、远程选取样品待测点和实时远程实验数据输出打印等功能。数据处理采用SQUID和ISOPLOT程序(Ludwig, 2003)。

锆石Lu-Hf同位素测试是在中国地质科学院矿产资源研究所国土资源部成矿作用与资源评价重点实验室Neptune多接收等离子质谱和Newwave UP213紫外激光剥蚀系统(LA-MC-ICP-MS)上进行的，实验过程中采用He作为剥蚀物质载气，剥蚀直径为55μm，测试时采用锆石国际标样GJ1作为参考物质，分析点与U-Pb定年分析点为同一位置。相关仪器运行条件及详细分析流程见侯可军等(2007)。分析过程中锆石标准GJ1的176Hf/177Hf测试加权平均值为0.282015±28(2σ,n=10)，与文献报道值(侯可军等，2007；Elhlouetal., 2006)在误差范围内完全一致。

锆石原位微量元素测试在国家地质实验测试中心(NRCGA)完成，采用激光剥蚀等离子质谱(LA-ICP-MS)方法。使用仪器为Thermo Element II 等离子质谱仪，激光剥蚀系统为New Wave UP-213。实验中采用He 作为剥蚀物质的载气，激光波长213nm、束斑40μm、脉冲频率10Hz、能量0.176mJ、密度23～25J/cm2，测试过程中首先遮挡激光束进行空白背景采集15s，然后进行样品连续剥蚀采集45s，停止剥蚀后继续吹扫15s 清洗进样系统，单点测试分析时间75s。等离子质谱测试参数为冷却气流速(Ar)15.55L/min；辅助气流速(Ar)0.67L/min；载气流速(He)0.58L/min；样品气流速0.819L/min，射频发生器功率1205W。数据测试标样使用NIST-610。用于计算Ce4+和Ce3+在锆石-熔体中的分配系数所用到的全岩微量元素含量测试在国家地质实验测试中心完成，检测仪器为等离子体质谱仪ICP-MS(X-series)，测试精度优于5%。

5 分析结果

5.1 SHRIMP锆石U-Pb年龄

二长花岗岩(QEC-7)和花岗斑岩(QEC-8)中的锆石多呈柱状，长度一般为100～200μm，长宽比大多为2:1～3:1，无色透明，具清晰震荡环带，裂纹不发育，显示岩浆成因特征(Rubatto and Gebauer, 2000)(图4)。本次研究中，对样品QEC-7和QEC-8分别选择了14个和16个点进行测试，锆石U-Pb定年结果列于表1。两件样品中绝大部分锆石Th/U比值变化在0.56～1.99之间，属典型岩浆锆石特征(Belousovaeta., 2002)。QEC-7的14个测试点和QEC-8的15个测试点分别得到206Pb/238U年龄为130±2Ma(MSWD=1.4)和129±2Ma(MSWD=1.9)(图5)，分别代表二长花岗岩和花岗斑岩的结晶年龄。另外，样品QEC-8中的一个测点3.1得到了1943±37Ma的年龄，没有参与加权平均年龄的计算。以上测年结果显示千鹅冲隐伏岩体中的二长花岗岩和花岗斑岩形成于同一岩浆事件。

表1千鹅冲钼矿床二长花岗岩(QEC-7)和花岗斑岩(QEC-8)的SHRIMP锆石U-Pb同位素定年结果

Table 1 Results of SHRIMP zircon U-Pb dating of monzogranite (QEC-7) and granite porphyry (QEC-8) from the Qian’echong Mo deposit

SpotNo.U(×10-6)Th(×10-6)Th/U206Pb*(×10-6)206Pbc(%)207Pb*235U±%(1σ)207Pb*206Pb*±%(1σ)206Pb*238U±%(1σ)206Pb238UAge(Ma)±Ma(1σ)QEC-7-1.116829440.5829.50.150.13522.90.04812.20.02041.9130.22.4QEC-7-2.1124816461.3622.71.130.14207.60.04917.30.02101.9133.62.5QEC-7-3.1127510780.8723.0—0.14672.40.05061.50.02101.9134.12.5QEC-7-4.12423471.484.21.720.11028.80.04068.50.01972.1125.82.6QEC-7-5.13654941.406.11.230.1150170.0431170.01932.2123.12.7QEC-7-6.12421730.744.2—0.16374.30.05873.80.02022.1129.12.7QEC-7-7.1150120471.4126.80.260.14153.30.04962.70.02071.9132.02.5QEC-7-8.184914101.7215.30.360.13314.30.04623.90.02091.9133.32.5QEC-7-9.1154816051.0727.30.310.14383.00.05092.30.02051.9130.72.4QEC-7-10.1101518511.8917.7—0.15704.30.05563.90.02051.9130.62.5QEC-7-11.11763391.993.11.720.1100190.0391190.02042.3130.13.0QEC-7-12.15004010.838.60.500.12777.40.04647.10.02002.0127.42.5QEC-7-13.11772451.433.10.990.1210150.0438150.02002.3127.82.9QEC-7-14.1151011180.7726.70.380.13563.90.04793.50.02051.9131.02.4QEC-8-1.174841.161.38.04————0.01934.0123.24.9QEC-8-2.14083320.847.1—0.172100.06149.80.02042.1130.02.7QEC-8-3.158330.5817.4—6.47007.70.13347.40.35172.2194337QEC-8-4.146700.008.50.820.14256.90.04906.60.02112.0134.52.6QEC-8-5.127800.005.01.350.1110130.0388120.02072.1132.12.7QEC-8-6.179800.0013.2—0.13443.30.05042.50.01932.2123.42.7QEC-8-7.146500.007.80.400.17293.30.06482.70.01942.0123.52.4QEC-8-8.16437491.2011.10.480.12813.80.04673.30.01991.9127.12.4QEC-8-9.19188901.0016.00.310.13495.60.04845.30.02021.9129.02.4QEC-8-10.1118415411.3420.7—0.13893.00.04942.40.02041.9130.12.4QEC-8-11.14512460.567.60.900.1240110.0461100.01952.0124.72.5QEC-8-12.1126510850.8921.90.260.13372.80.04822.10.02011.9128.52.4QEC-8-13.1166815390.9529.50.470.12794.30.04543.90.02051.9130.52.4QEC-8-14.14502930.677.8—0.15113.70.05453.10.02012.0128.32.5QEC-8-15.19399551.0516.9—0.14152.60.04901.80.02091.9133.62.5QEC-8-16.1219015140.7140.73.450.13317.20.04636.90.02091.9133.12.5

注：Pb*和Pbc分别代表放射铅和普通铅，锆石中的普通铅用实测204Pb校正; —表示未检出

图5 SHRIMP锆石U-Pb年龄谐和图及加权平均年龄Fig.5 Zircon U-Pb isotope concordian diagrams and weighted average ages

表2千鹅冲钼矿床二长花岗岩(QEC-7)和花岗斑岩(QEC-8)锆石Hf同位素分析结果

Table 2 Zircon Hf isotopic composition of monzogranite (QEC-7) and granite porphyry (QEC-8) from the Qian’echong Mo deposit

SpotNo.176Yb/177Hf176Lu/177Hf176Hf/177Hf±2σ(176Hf/177Hf)iAge(Ma)εHf(t)tDM1(Ma)tDM2(Ma)QEC-7-1.10.0811110.0013290.2821490.0000200.282146130-19.315682408QEC-7-2.10.1339350.0024110.2822950.0000220.282289134-14.214032086QEC-7-3.10.1650890.0039830.2823200.0000230.282310134-13.414282037QEC-7-4.10.0844470.0017510.2822340.0000270.282229126-16.414652224QEC-7-5.10.1246460.0018570.2822780.0000210.282273123-14.914062127QEC-7-6.10.1003610.0019910.2822740.0000260.282270129-14.914172132QEC-7-7.10.1256450.0016860.2823460.0000300.282342132-12.313031969QEC-7-8.10.1561120.0020790.2826180.0000330.282612133-2.79251362QEC-7-9.10.0870800.0013110.2821590.0000280.282155131-18.915532385QEC-7-10.10.0745100.0012960.2820010.0000240.281997131-24.517742736QEC-7-11.10.0871600.0012340.2825000.0000280.282497130-6.910711624QEC-7-12.10.1355800.0031620.2821250.0000290.282118127-20.416832470QEC-7-13.10.0963390.0013780.2823760.0000310.282373128-11.312501902QEC-7-14.10.1195740.0029890.2822250.0000200.282218131-16.715282245QEC-8-1.10.1184460.0016410.2823300.0000250.282326123-13.113242010QEC-8-2.10.0818730.0012790.2821590.0000220.282156130-18.915512385QEC-8-3.10.0133800.0001960.2809940.0000190.2809871,943-19.830723787QEC-8-4.10.0663240.0011100.2822670.0000190.282264135-15.013942142QEC-8-5.10.0392970.0006000.2823350.0000250.282334132-12.612811988QEC-8-6.10.1079880.0021290.2823230.0000220.282318123-13.313512027QEC-8-7.10.0798330.0011540.2822810.0000210.282279124-14.713752116QEC-8-8.10.0699900.0010970.2823790.0000180.282376127-11.212361895QEC-8-9.10.0714910.0011840.2822350.0000210.282233129-16.214412215QEC-8-10.10.1084380.0019960.2823690.0000190.282364130-11.612811921QEC-8-11.10.1021630.0015780.2823730.0000240.282370125-11.512601912QEC-8-12.10.0750580.0013390.2823140.0000190.282311129-13.513362041QEC-8-13.10.0810800.0015310.2822200.0000180.282216131-16.814762250QEC-8-14.10.0844270.0012380.2823700.0000240.282367128-11.512531915QEC-8-15.10.1351150.0030770.2822740.0000250.282266134-14.914602136QEC-8-16.10.1051810.0017560.2822080.0000260.282204133-17.215022276

注：εHf(t)=10000×{[(176Hf/177Hf)S-(176Lu/177Hf)S×(eλt-1)]/[(176Hf/177Hf)CHUR,0-(176Lu/177Hf)CHUR×(eλt-1)]-1};tDM1=1/λ×ln{1+[(176Hf/177Hf)S-(176Hf/177Hf)DM]/[(176Lu/177Hf)S-(176Lu/177Hf)DM]};tDM2=1/λ×ln{1+[(176Hf/177Hf)S, t-(176Hf/177Hf)DM, t]/[(176Lu/177Hf)c-(176Lu/177Hf)DM]}+t; (176Lu/177Hf)S和(176Hf/177Hf)S为样品测定值; (176Hf/177Hf)CHUR,0=0.282772, (176Lu/177Hf)CHUR=0.0332, (176Hf/177Hf)DM=0.28325, (176Lu/177Hf)DM=0.0384 (Blichert-Toft and Albarède, 1997; Griffinetal., 2000); λ=1.867×10-11/a (Soderlundetal., 2004); (176Lu/177Hf)c=0.015;t为锆石结晶时间

5.2 锆石Hf同位素

在SHRIMP锆石U-Pb定年的基础上，对样品QEC-7和QEC-8进行了锆石微区Hf同位素测定，分析结果见表2和图6。大部分锆石的176Lu/177Hf比值小于0.002，说明锆石在形成后具有很少的放射成因Hf的积累，所测定的176Hf/177Hf比值基本代表了其形成时体系的Hf同位素组成。样品QEC-7共分析14个点，176Hf/177Hf比值变化于0.282001～0.282618，εHf(t)值变化于-24.5～-2.7(绝大部分集中在-24.5～-11.3之间)，两阶段模式年龄(tDM2)变化于1362～2736Ma。样品QEC-8共分析16个点，176Hf/177Hf比值变化于0.280994～0.282379，εHf(t)值较均一，变化于-19.8～-11.2，除一颗继承锆石的两阶段模式年龄(tDM2)为3787Ma外，其他变化于1895～2385Ma之间(图6)。

表3千鹅冲钼矿二长花岗岩和花岗斑岩锆石微量元素LA-ICP-MS测试结果(×10-6)

Table 3 Zircon trace element data of monzogranite and granite porphyry in the Qian’echong Mo deposit (×10-6)

测点号LaCePrNdSmEuGdTbDyHoErTmYbLuThUHfQEC-7(二长花岗岩)10.0226.00.050.752.561.0910.83.4551.920.810620.228658.583.43421743120.411220.898.5112.84.4257.815.619496.144271.076016996118882168432.8382.31.709.3611.33.0340.813.018876.235862.571215167317381941640.2094.40.363.296.481.9434.810.314768.136367.7738168106616231924452.731333.6524.123.46.6774.921.724190.742285.7853190126920861851560.0993.80.292.373.381.4723.38.0710148.228750.25191187788581682270.0532.30.090.591.631.068.612.8535.216.777.613.513731.61171941937780.961320.736.5913.23.7045.712.914761.624938.937870.611439551472893.841672.1811.411.74.5351.917.221587.943782.78641871657241517589101.001180.839.1614.05.6557.618.419672.530855.758010372774111072111.1347.90.846.528.292.2133.89.8512954.024041.641289.5385133617901122.641562.0819.227.210.612231.634412755690.879614399889112897130.291511.1413.325.35.4094.926.229311449578.97521521350129514638142.034612.2318.229.210.412330.231313357581.7640117233295714226154.471261.5510.317.66.7851.214.218377.728746.5534121953132119386160.2381.01.0712.425.510.086.921.024795.438257.258612034439616506176.031952.319.0411.45.2354.914.415368.528538.233759.269137916054全岩60.494.49.0329.03.870.692.630.301.510.220.660.100.490.0822.94.354.69QEC-8(花岗斑岩)10.1874.20.9514.127.47.6472.021.925790.931952.153398.73872461222320.1469.80.222.074.951.8821.15.8078.537.118829.934078.33213801792330.0421.00.131.342.900.6311.52.9434.314.965.99.5686.717.235.680.718603410236531.310729.87.3051.813.714652.225646.949880.97809321311450.1120.70.638.0911.33.6742.310.210744.617729.925545.61141101268866.561331.478.8812.53.7052.915.520589.739660.65761255956271531473.7791.24.2817.79.542.6930.28.0598.342.422535.835977.845165215181845.319323.976.724.83.1154.112.514661.127241.639378.739782617922912537335.712632.46.1460.014.116372.431949.242690.6411446150051041.61429.7541.822.24.3255.216.120673.729149.950292.130532010863114.5184.21.6810.611.33.0745.813.416367.330956.251992.3427452129261229.51237.2129.615.02.0746.715.318666.128453.256592.0962126011256135.661104.2818.118.05.9251.313.514869.832452.854914173693822108140.1437.30.324.097.030.5830.29.2812448.622036.638075.530259214122150.5545.10.332.863.881.6019.66.0083.848.725545.4528145680147419242166.3278.52.1011.78.412.6928.48.4010944.021138.442898.6642103914575171.9574.31.3412.116.44.2172.420.622081.136161.457610047648913029180.5958.30.403.264.991.8626.68.3010444.422338.735566.033337014067193.6768.92.0210.910.33.1740.511.313758.627745.244493.272980914297205.1239.52.8216.517.80.6979.319.219272.833957.447177.633856215152全岩41.667.76.5321.03.080.562.300.341.760.290.850.140.920.1726.97.464.77

图6 二长花岗岩和花岗斑岩锆石εHf(t)统计直方图(a)和二阶段模式年龄(tDM2)统计直方图(b)Fig.6 Histogram of εHf(t) (a) and two stage mode ages (tDM2) (b) of zircons from monzogranite and granite porphyry

表4千鹅冲钼矿二长花岗岩和花岗斑岩锆石Ce3+和Ce4+的分配系数及比值

Table 4 Partition coefficients and ratios of Ce3+and Ce4+of zircons from monzogranite and granite porphyry in the Qian’echong Mo deposit

测点号DCe3+DCe4+Ce4+/Ce3+Ce/Ce*Eu/Eu*QEC-7(二长花岗岩)10.00070341.5393.7234.60.6320.00600803.5215.349.70.5030.00529720.2164.09.20.4340.00157847.4636.185.50.3950.01730896.380.610.30.4960.00062758.91606145.20.5170.00053384.2639.3115.10.8780.01533870.390.638.70.4690.00462999.4382.514.10.56100.01202739.6103.131.80.61110.00481584.7104.512.10.40120.03290823.749.416.40.57130.02630938.360.063.90.34140.046001103.9105.753.20.53150.01552808.585.311.80.69160.03346551.624.740.20.65170.01412708.2145.812.80.64QEC-8(花岗斑岩)10.15925541.95.943.70.5320.00648508.1158.498.20.5630.01032226.729.175.70.3340.21304652.224.51.60.5750.05883344.04.219.70.5160.02666617.872.910.50.4470.02364576.756.15.60.4980.15398521.417.61.40.2690.22445543.423.81.40.43100.11094483.717.91.70.38110.02921548.741.77.50.41120.05154745.434.42.10.24130.04518673.234.95.50.59140.01412490.238.042.90.12150.00213675.9311.325.90.56160.01469658.578.05.30.53170.05755584.118.111.30.37180.00824497.5103.629.50.49190.02369662.042.06.20.47200.08648499.75.72.50.06

注：锆石和熔体之间Ce4+和Ce3+的分配系数DCe3+、DCe4+及Ce4+/Ce3+比值计算方法据Ballardetal. (2002)；Eu/Eu*=EuN/(SmN×GdN)1/2；Ce/Ce*=CeN/(LaN×PrN)1/2

图7 锆石稀土元素球粒陨石标准化配分曲线(球粒陨石标准化值据Sun and McDonough, 1989)Fig.7 Chondrite-normalized REE patterns of zircons (chondritite values after Sun and McDonough, 1989)

5.3 锆石微量元素特征

锆石中稀土元素及Th、U、Hf元素含量见表3。测试结果显示，二长花岗岩中锆石的稀土总量为358.9×10-6～2536×10-6，平均为1604×10-6；花岗斑岩中锆石的稀土总量为268.8×10-6～1893×10-6，平均为1279×10-6。锆石稀土元素球粒陨石标准化配分曲线(图7)显示，二长花岗岩和花岗斑岩具有较一致的稀土元素特征，亏损LREE且富集HREE。

锆石Ce4+和Ce3+在锆石-熔体间的分配系数DCe4+、DCe3+及Ce4+/Ce3+比值见表4。计算结果显示，二长花岗岩和花岗斑岩都具有变化较大的Ce4+/Ce3+比值，但二长花岗岩总体上具有相对花岗斑岩更大的Ce4+/Ce3+比值。二长花岗岩和花岗斑岩中的锆石均显示正Ce异常和Eu负异常(图7)，但样品QEC-8中部分锆石具有更强负Eu异常(图7b)，锆石Ce/Ce*分别变化于9.2～234.6和1.4～98.2之间，Eu/Eu*变化范围分别为0.34～0.87(平均0.55)和0.06～0.59(平均0.42)。

6 讨论

6.1 成岩成矿时代

本次研究得到千鹅冲钼矿中隐伏的二长花岗岩和花岗斑岩SHRIMP锆石U-Pb年龄分别为130±2Ma和129±2Ma，二者在误差范围内一致。这一结果与李法岭(2011)和杨梅珍等(2010)报道的千鹅冲钼矿床的辉钼矿Re-Os同位素年龄(128±7Ma)及成矿后花岗斑岩脉的年龄(129±3Ma)也具有比较好的一致性，说明千鹅冲斑岩型钼矿床的成岩成矿作用发生在早白垩世。

鉴于前人(李法岭，2011；杨梅珍等，2010)报道的千鹅冲钼矿辉钼矿Re-Os等时线年龄误差较大(±7Ma)，最近，作者运用辉钼矿Re-Os同位素定年重新厘定了千鹅冲钼矿的成矿时代，6件辉钼矿样品得到了一条理想的等时线，其Re-Os等时线年龄为129±2Ma(MSWD=0.63)(数据待发表)。这一结果与本文获得的千鹅冲矿区二长花岗岩和花岗斑岩的SHRIMP锆石U-Pb年龄非常一致，说明千鹅冲钼矿成岩成矿时限较短，约为128～130Ma。

近年来，东秦岭-大别钼矿带钼矿床年代学研究表明，虽然有少量钼矿床形成于中生代以前(如寨凹和龙门店，李厚民等，2009；魏庆国等，2009)，但总体上以中生代成矿作用大爆发为显著特征(李永峰等，2005；毛景文等，2005；叶会寿等，2006)。Maoetal.(2008，2011a)比较全面地统计了东秦岭-大别钼矿带钼矿床成矿时代，将中生代钼矿床作用划分为三个期次：晚三叠(221～233Ma)、晚侏罗-早白垩(138～148Ma)、早-中白垩(112～131Ma)。与东秦岭多期次钼成矿作用不同，除个别侏罗纪年龄外，绝大多数大别山地区钼矿床的成矿作用发生于早白垩世(黄凡等，2011；李毅等，2013，及其中引文)，此时代跨度与大别山碰撞后岩浆作用时限基本一致(Heetal., 2011；Wangetal., 2007)。

6.2 岩浆源区及相对氧逸度

6.2.1 岩浆源区

锆石Lu-Hf同位素体系具有较高的封闭温度(Schereretal., 2000)，能有效地揭示岩浆演化过程和源区性质(Griffinetal., 2000；Beloisovaetal., 2006)。由于Hf属于不相容元素，当寄主岩浆不断发生部分熔融和结晶分异作用时，亏损地幔源区具有更高的176Hf/177Hf比值，使得熔融物和寄主岩浆发生176Hf/177Hf比值的解耦，即大陆地壳相对于亏损地幔具有更低的176Hf/177Hf比值和εHf(t)值(Patchettetal., 1981)。

表2和图8显示，千鹅冲钼矿中二长花岗岩和花岗斑岩中的锆石具有低的εHf(t)值和古老的Hf模式年龄，并且所有Hf同位素数据点均落于球粒陨石Hf同位素演化线之下(图8)，表明千鹅冲岩体主要来源于古老的地壳物质。大别造山带的深部地壳和岩石圈地幔是否存在华北物质存在争议(Huangetal., 2007；Li and Yang, 2003；Wangetal., 2005)，但基于对大别造山带超高压变质岩及早白垩世高Sr/Y花岗岩的地球化学性质的详细研究，多数学者认为大别造山带的地壳物质基本来自华南板块(Heetal., 2013；Zhengetal., 2003；Zheng and Zhang, 2007；Zhaoetal., 2007；Zhao and Zheng, 2009)。所以千鹅冲花岗岩应来源于华南板块北缘的古老地壳。

图8 锆石εHf(t)-Age图解资料来源：北大别片麻岩引自Zhao et al. (2008)；太古代崆岭片麻岩和混合岩以及古元古代崆岭花岗岩引自Zhang et al. (2006)，Zheng et al. (2006)，Xiong et al. (2008)；亏损地幔演化线据Nowell et al. (1998)Fig.8 εHf(t) vs. Age plots for zirconsData sources: The granitic gneiss from North Dabie from Zhao et al. (2008); Archean gneiss and migmatite and Paleoproterozic granite from the Kongling Complex from Zhang et al. (2006a); Zheng et al. (2006b); Xiong et al. (2008). The evolutionary line of depleted mantle after Nowell et al. (1998)

千鹅冲花岗岩的锆石Hf同位素特征与大别造山带碰撞后花岗岩的锆石Hf同位素特征具有相似性(Zhaoetal., 2011)，暗示它们具有一致的来源。对大别造山带内碰撞后花岗岩类的研究表明，它们与造山带地表出露的原岩为新元古代的双峰式火成岩的高压-超高压变质岩(Liu and Xue, 2007；Zhengetal., 2003)有相似的地球化学特征(Bryantetal., 2004；Heetal., 2011, 2013；Wangetal., 2007；Zhangetal., 2002；Zhaoetal., 2011)，说明这些花岗岩来自大别造山带高压-超高压变质岩的部分熔融(Heetal., 2013；Wangetal., 2007；Zhaoetal., 2011)。虽然对于大别造山带后碰撞花岗岩具体来自镁铁质榴辉岩还是中酸性大别片麻岩存在较大分歧(Heetal., 2011, 2013；Wangetal., 2007；Zhaoetal., 2011；Xuetal., 2013)，但是古元古-太古代的继承锆石、古元古-太古代的Nd和Hf的模式年龄都指示这些花岗岩的原岩混入了不同比例的更古老的地壳物质(如太古代崆岭杂岩)(Heetal., 2013；Zhaoetal., 2011)。千鹅冲花岗斑岩中发现了年龄为1943Ma的古元古代继承锆石，其与崆岭杂岩内的古元古代花岗岩具有相似的Hf同位素特征(图8)，也说明了其原岩混入了类似崆岭杂岩的古老地壳物质。虽然两个样品中大部分锆石的εHf(t)值为较低的负值，但是变化范围较大的εHf(t)值和二阶段模式年龄暗示其源区可能混入了不同比例的年轻地幔组分，尤其是二长花岗岩(图6)。大别山地区白垩纪超基性岩浆作用开始于～130Ma(Jahnetal., 1999；Wangetal., 2005)，说明此时地幔上涌不仅为花岗岩原岩部分熔融提供了热源，也注入了少量幔源组分。

6.2.2 相对氧逸度

实验表明，Mo在流体中的溶解度与流体的氧逸度关系密切(Balietal., 2012)。岩浆中的Ce常呈3价和4价，在氧化条件下，锆石中的Zr4+容易被Ce4+离子取代。另外，Ce3+和Ce4+的分异能力很强，对岩浆的氧化还原状态具有较高的敏感度，因此可以通过Ce4+/Ce3+比值来判断岩浆氧逸度的相对高低(Ballardetal., 2002；Bolharetal., 2008；Burnham and Berry, 2012；Trailetal., 2012)。Eu在岩浆中呈Eu2+和Eu3+两种价态，当Ce4+稳定存在时，Eu应呈三价。实验表明，Eu的异常一般与Ce的异常呈正相关关系，并且也可用来指示熔体的氧逸度(Burnham and Berry, 2012；Trailetal., 2012)。

千鹅冲钼矿花岗斑岩中的锆石比二长花岗岩中的锆石具有更低的Eu/Eu*比值，即更强的Eu异常，可能是由于斜长石的分离结晶作用(Hoskin and Schaltegger, 2003)。随着岩浆的演化，在锆石达到饱和之前，Eu2+优先进入斜长石，从而造成了演化程度更高的花岗斑岩中的锆石具有更强的Eu异常。二长花岗岩和花岗斑岩中的锆石的Ce4+/Ce3+比值平均值分别为287.4和55.9。二长花岗岩中的锆石中具有较高的Ce4+/Ce3+比值，与西藏玉龙和冈底斯地区以及智利东部的斑岩铜矿具有相似的特征(Ballardetal., 2002；Liangetal., 2006；辛洪波和曲晓明，2008)，相比之下，花岗斑岩中锆石的Ce4+/Ce3+比值明显低于这些斑岩铜矿。钻孔中揭露的花岗斑岩远多与二长花岗岩且形成晚于二长花岗岩，推测成矿流体更可能来自花岗斑岩。已有研究表明，岩浆的氧逸度不是控制钼成矿的决定因素，岩浆中铁和钛的含量、岩浆流体含量以及岩浆上升过程中的对流机制都是影响钼富集的重要因素(Keppler and Wyllie, 1991；Shinogaraetal., 1995；Tacker and Candela, 1987)。

6.3 动力学背景

大别造山带形成于三叠纪华南与华北板块之间的碰撞对接(Lietal., 1993；Hackeretal., 1998)，关于造山带内含柯石英和金刚石的超高压变质岩的研究显示大量的华南陆壳物质曾深俯冲到超过100km的深度(Wangetal., 1989)。然而，地震资料表明该造山带现今地壳的平均厚度约为35km，且缺少基性下地壳，暗示曾经发生了加厚山根的拆沉作用(Gaoetal., 1998a, b)。

大别造山带发育的大量白垩纪花岗岩在约130Ma发生明显的地球化学特征变化，即>130Ma形成的花岗岩具有高Sr/Y和(La/Yb)N比值以及低Y含量的特征，而形成于130Ma之后的花岗岩则不具备这一特征(Heetal., 2011；Wangetal., 2007)。研究表明，早期花岗岩(130～143Ma)来自石榴石为主要残留相的加厚下地壳的部分熔融(Heetal., 2011)。花岗岩地球化学特征在130Ma左右发生的转变指示大别造山带在约130Ma发生了下地壳的拆沉作用，所以之后形成的花岗岩来自减薄地壳的部分熔融(Heetal., 2011；Wangetal., 2007；Xuetal., 2007)。另外，北大别广泛分布的形成于123～130Ma的镁铁-超镁铁质岩的地球化学特征显示，它们具有明显的陆壳物质特征属性，可能由拆沉的下地壳熔体交代上地幔或岩石圈地幔形成(Huangetal., 2007)。所以，大别造山带在早白垩世发生了下地壳的拆沉作用(Gaoetal., 1998a, b)。

碰撞造山带的演化一般都要经历从挤压缩短向伸展减薄的构造体制的转换过程(Leech, 2001；Vanderhaeghe and Teyssier, 2001)。大别造山带早白垩世下地壳拆沉作用可能导致造山带的去山根作用、软流圈上涌及大规模地壳伸展(Ratschbacheretal., 2000, 2003；Bryantetal., 2004；Hackeretal., 2004；Liuetal., 2004)。Wuetal.(2007)通过对北大别混合岩的研究认为，大别山地区构造体制由挤压向伸展转换的时间约为145Ma。另外，大别造山带于早白垩世侵位的A型花岗岩也进一步证明了当时的伸展环境(王强等，2000；谢智等，2004)。

综上所述，千鹅冲钼矿的成岩成矿作用发生在大别山地区早白垩世的伸展构造背景下。事实上，整个中国东部在早白垩世总体处在伸展的构造体制下(Maoetal., 2011b；Wangetal., 2012)。在这一时期，不仅形成了东秦岭-大别钼矿带这一世界级钼多金属成矿省(Maoetal., 2008, 2011a)，而且在中国东北地区(Yangetal. 2003；孙景贵等，2012)、华北克拉通内部(翟明国，2010；毛景文等，2005)、长江中下游地区(Duanetal., 2012；Maoetal., 2011c；Xieetal., 2008, 2011, 2012；袁顺达等，2010)以及华南地区(Maoetal., 2013)均发育了大规模的构造-岩浆-成矿事件(Maoetal., 2011b；Wangetal., 2012；Wuetal., 2005)，它们均与中国东部乃至亚洲东北部晚中生代大规模地壳伸展的构造背景密切相关(Maoetal., 2003；Wangetal., 2012)。

7 结论

(1)千鹅冲钼矿区隐伏岩体中的二长花岗岩和花岗斑岩的SHRIMP锆石U-Pb年龄分别为130±2Ma和129±2Ma，与辉钼矿Re-Os年龄一致，为早白垩世，成岩成矿作用发生在一个很短的时限内(128～130Ma)。

(2)锆石Hf同位素特征显示千鹅冲岩体的物质来源主要为华南陆块北缘的古老地壳及少量年轻地幔组分，原岩中含有古元古代-太古代的基底岩石，二长花岗岩相比花岗斑岩具有更高的氧逸度。

(3)千鹅冲钼矿床形成于早白垩世的伸展构造体制下。大别造山带于早白垩世发生的下地壳拆沉作用导致的软流圈上涌及壳幔相互作用不仅形成了大规模的岩浆作用，也为斑岩型钼矿床提供了物质来源。

致谢中国地质科学院地质研究所刘建辉、矿产资源研究所郭春丽和国家地质实验测试中心孙东阳分别在SHRIMP锆石测年、锆石Hf同位素测试及锆石微量元素测试过程中提供了大量帮助，在此一并表示感谢。

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