Geochemical, U-Pb Age and Nd-Isotopic Characteristics of Titanite in Alkaline Rocks from Dazhuang Nb-REE Deposit in Southern Margin of North China Craton
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摘要: 位于华北克拉通南缘河南省方城县的大庄铌-稀土矿是近年来新发现的一例具有中型规模的铌-稀土矿床.该矿床赋存于新元古代双山碱性侵入岩中，黑云母正长岩和角闪霞石正长岩是铌-稀土矿的主要赋矿岩石.通过电子探针与LA-ICP-MS等方法对大庄铌-稀土矿碱性岩中的榍石开展了主量、微量元素、U-Pb年代学和微区Nd同位素研究.大庄铌-稀土矿碱性岩中榍石的SiO2（28.597%~31.169%）、CaO（25.492%~28.949%）、TiO2（34.126%~38.940%）平均含量明显低于理论值，含有相对较高的F（0.141%~1.086%）、Al2O3（1.573%~2.817%）和FeO（0.446%~2.147%）.榍石具有极高的稀土元素总量（∑REE=781.47×10-6~31 766.59×10-6），球粒陨石标准化稀土配分曲线呈明显的右倾型，轻重稀土分馏明显，样品具有明显的负δEu异常（0.27~0.86）和不明显的δCe异常（0.97~1.22），Th/U值介于1.40~11.86，暗示大庄铌-稀土矿碱性岩中榍石为岩浆成因榍石，榍石Zr温度计获得大庄碱性岩的形成温度为667~964 ℃，平均为933 ℃.大庄铌-稀土矿碱性岩中的榍石具有极高的Nb和REE含量，表明榍石是大庄铌-稀土矿的重要成矿矿物，铌、稀土等元素是伴随岩浆演化逐步富集的结果.富铌榍石样品获得848±35 Ma、849±22 Ma、843±30 Ma、845±20 Ma、845±24 Ma和849±40 Ma的形成年龄，限定大庄铌-稀土矿化富集的时代为新元古代，与Rodinia超大陆裂解事件相关.榍石具有较为均一的Nd同位素值（εNd（t）=-3.25~-0.66），表明方城地区霞石正长岩的原始岩浆形成于富金云母的地幔源区.Abstract: The Dazhuang deposit is a newly discovered medium-scale Nb-REE deposit which is located at the Fangcheng County of Henan Province on the southern margin of the North China craton. The Nb-REE orebodies are hosted in biotite syenite and hornblende nepheline syenite of Neoproterozoic Shuangshan alkaline pluton. In this paper, major and trace elements, U-Pb geochronology and in-situ Nd isotope studies were carried out on the titanite from the alkaline rocks by EPMA and LA-ICP-MS. The average contents of SiO2 (28.597%-31.169%), CaO (25.492%-28.949%) and TiO2 (34.126%-38.940%) in titanite are significantly lower than the theoretical values, whereas it contains relatively high contents of F (0.141%-1.086%), Al2O3 (1.573%-2.817%) and FeO (0.446%-2.147%). The titanite in Dazhuang deposit has a very high total amount of REE (∑REE=781.47×10-6-31 766.59×10-6). In the chondrite-normalized REE patterns, the rare earth distribution curve is obviously right-leaning, and the light and heavy rare earth fractionation is obvious. There are obvious negative δEu anomalies (0.27-0.86) and inconspicuous δCe anomalies (0.97-1.22), with Th/U values ranging from 1.40 to 11.86, suggesting that the titanite is magmatic origin. The formation temperature of Dazhuang alkaline rocks obtained by the titanite Zr thermometer is 667-964 ℃, with an average of 933 ℃. The titanite in Dazhuang deposit has very high Nb and REE contents, indicating that the titanite is an important ore-bearing mineral, and the Nb and REE are the result of the gradual enrichment of magma evolution. Formation ages of 848±35 Ma, 849±22 Ma, 843±30 Ma, 845±20 Ma, 845±24 Ma, and 849±40 Ma were obtained from the Nb-rich titanite samples, constraining that the mineralization age of Dazhuang Nb-REE deposit is Neoproterozoic, of which related to the breakup of the Rodinia supercontinent. Titanite has a relatively uniform Nd isotope (εNd(t)=-3.25 to -0.66) value, indicating that the original magma was derived from mantle where rich in phlogopite.
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图 1 方城县大庄铌-稀土矿大地构造图和区域地质图
图a据Dong et al., 2011修改；图b据张哨波等，2020修改
Fig. 1. Simplified tectonic map and reginal geological map of Dazhuang Nb-REE deposit, Fangcheng County
图 3 方城县大庄铌-稀土矿区地质图（据李山坡等，2020修改）
Fig. 3. Geological map of the Dazhuang Nb-REE deposit in Fangcheng County (modified after Li et al., 2020)
图 4 大庄铌-稀土矿床各类岩石野外照片
a.黑云母正长岩；b.角闪霞石正长岩；c.黑云角闪正长岩；d.片麻状含磁铁矿黑云母正长岩
Fig. 4. Field photos of various rocks in the Dazhuang Nb-REE deposit
图 5 大庄铌-稀土矿15线（a）和0线（b）勘探线剖面简图（据张哨波等，2020修改）
Fig. 5. No.15 (a) and No.0 (b) exploration line sections of the Dazhuang Nb-REE deposit (modified after Zhang et al., 2020)
图 6 大庄铌-稀土矿碱性岩中榍石的显微特征
Mc.微斜长石；Or.正长石；Ne.霞石；Ab.钠长石；Bt.黑云母；Ttn.榍石；Am.角闪石；Mag.磁铁矿；Ap.磷灰石；Cal.方解石；Ms.白云母；Agt.霓辉石
Fig. 6. Micrographs of titanite in alkaline rocks from Dazhuang Nb-REE deposit
图 7 大庄铌-稀土矿碱性岩中榍石的BSE图像
Fig. 7. BSE images of titanites in alkaline rocks from the Dazhuang Nb-REE deposit
图 8 大庄铌-稀土矿碱性岩中榍石球粒陨石标准化稀土配分图（a）和原始地幔标准化微量元素蛛网图（b）（标准化值据Sun and McDonough, 1989）
Fig. 8. Chondrite-normalized REE patterns (a) and primitive mantle-normalized trace element patterns (b) for titanite in alkaline rocks from the Dazhuang Nb-REE deposit (normalized data after Sun and McDonough, 1989)
图 9 大庄铌-稀土矿碱性岩中榍石的REE与Th、U、Nb、Ta、Zr、Hf、La、Y、Th/U、Nb/Ta关系图解
Fig. 9. Plots of REE vs. Th, U, Nb, Ta, Zr, Hf, La, Y, Th/U and Nb/Ta for titanite in alkaline rocks from the Dazhuang Nb-REE deposit
图 10 大庄铌-稀土矿碱性岩中榍石的Nb-Ta、Th-U、Zr-Hf和Sm-Nd图解
Fig. 10. Plots of Nb vs. Ta, Th vs. U, Zr vs. Hf and Sm vs. Nd for titanite in alkaline rocks from the Dazhuang Nb-REE deposit
图 11 大庄铌-稀土矿碱性岩中榍石LA-ICP-MS U-Pb年龄Tera-Wasserburg谐和图
Fig. 11. LA-ICP-MS Tera-Wasserburg concordia diagrams for titanite in alkaline rocks from the Dazhuang Nb-REE deposit
图 12 大庄铌-稀土矿碱性岩中榍石（Al2O3+Fe2O3）-TiO2 (a)和（Al2O3+Fe2O3）-F(b)图解
Fig. 12. Diagrams of (Al2O3+Fe2O3) vs. TiO2 (a) and (Al2O3+Fe2O3) vs. F (b) for titanite in alkaline rocks from the Dazhuang Nb-REE deposit
表 1 华北克拉通南缘及秦岭造山带新元古代岩浆活动记录
Table 1. Neoproterozoic magmatic activity records in the southern margin of North China craton and Qinling orogenic belt
构造背景 样品岩性 采样位置 时代(Ma) 方法 资料来源 同碰撞 花岗质脉体 北秦岭牛角山岩体 929±25 SHRIMP锆石U-Pb 王涛等，2005 片麻状花岗岩 北秦岭牛角山岩体 955±13 SHRIMP锆石U-Pb 二云母花岗片麻岩 北秦岭牛角山岩体 954.6±5.1 TIMS锆石U-Pb 陈志宏，2004 花岗闪长质片麻岩 北秦岭西涝峪 956±8 TIMS锆石U-Pb Chen et al., 2006 黑云母二长片麻岩 北秦岭德河岩体 923±23 LA-ICP-MS锆石U-Pb Wang et al., 2011a 964.4±5.2 TIMS锆石U-Pb 陈志宏，2004 943±18 SHRIMP锆石U-Pb 黑云斜长片麻岩 948.1±8.9 SIMS锆石U-Pb 刘丙祥等，2013 花岗质糜棱岩 北秦岭方庄岩体 933.4±9.2 SIMS锆石U-Pb 闪长岩 北秦岭拉鸡庙 973±60 LA-ICP-MS锆石U-Pb 刘军锋等，2009 石英二长片麻岩 北秦岭郭家坪 953.4±14 SHRIMP锆石U-Pb 陆松年等，2005 二云母花岗片麻岩 北秦岭卢氏狮子坪 954.6±5.1 TIMS锆石U-Pb 陈志宏，2004 黑云母花岗闪长质片麻岩 北秦岭李家庄 937±21 SHRIMP锆石U-Pb 花岗闪长质片麻岩 北秦岭西峡石槽沟 955.5±8.4 TIMS锆石U-Pb 黑云母花岗片麻岩 北秦岭西峡寨根 914±10 SHRIMP锆石U-Pb 花岗质片麻岩 西秦岭新阳岩体 981±5 LA-ICP-MS锆石U-Pb 丁仨平等，2006 938±4 黑云母花岗闪长质片麻岩 978.5±4.8 LA-ICP-MS锆石U-Pb 裴先治等，2007 黑云母二长花岗质片麻岩 935.5±3.5 LA-ICP-MS锆石U-Pb 花岗质片麻岩 西秦岭元龙岩体 924.2±2.7 LA-ICP-MS锆石U-Pb 刘会彬等，2006 黑云母二长花岗质片麻岩 914.7±7.6 LA-ICP-MS锆石U-Pb 裴先治等，2007 后碰撞 花岗闪长岩 北秦岭蔡凹岩体 889±10 LA-ICP-MS 张成立等，2004 二长花岗片麻岩 北秦岭两河口岩体 851.8±1.9 TIMS锆石U-Pb 陈隽璐等，2004 蚀变角闪辉绿（辉长）岩 中秦岭小茅岭复式岩体 864.4±1.7 LA-ICP-MS锆石U-Pb 刘仁燕等，2011 蚀变闪长岩 中秦岭小茅岭复式岩体 846.7±2.7 LA-ICP-MS锆石U-Pb 蚀变石英闪长岩 中秦岭小茅岭复式岩体 859.4±1.7 LA-ICP-MS锆石U-Pb 蚀变二长闪长岩 中秦岭小茅岭复式岩体 861.1±1.8 LA-ICP-MS锆石U-Pb 板内裂解 变辉长岩 华北克拉通南缘栾川软玉矿 849.5±5.1 SIMS锆石U-Pb Ling et al., 2015 辉长岩 华北克拉通南缘栾川群 830±6 LA-ICP-MS锆石U-Pb Wang et al., 2011b 830±7 LA-ICP-MS锆石U-Pb 826±34 LA-ICP-MS/SHRIMP锆石U-Pb 霓辉正长岩 华北克拉通南缘双山岩体 844.3±1.6 SHRIMP锆石U-Pb 包志伟等，2008 粗面岩 华北克拉通南缘栾川群 840±4 LA-ICP-MS锆石U-Pb 胡国辉等，2019 845±5 846±6 854±8 李振生等，2020 霞石正长岩 华北克拉通南缘大庄铌-稀土矿 848±35 LA-ICP-MS榍石U-Pb 本文 849±22 843±30 845±20 845±24 849±40 
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