Titanite Mineralogy and Its Implications for Nb Enrichment Mechanism of Alkaline Volcanic-Rock Hosted Nb Deposit in NW Hubei Province
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摘要: 位于南秦岭武当地区的天宝铌矿床是我国典型的碱性火山岩型铌矿床，但其岩浆成因、演化及成矿机理等方面的研究十分薄弱.天宝碱性火山岩主要分为粗面质岩石和碱性玄武岩两大类，两者在空间上紧密共生.在详细的岩（矿）相学及榍石显微结构研究的基础上，利用LA-ICP-MS分析技术对天宝粗面质火山岩中的榍石进行原位U-Pb定年，并利用EPMA对不同岩性中不同产状的榍石进行原位地球化学成分分析，从而反演岩浆演化过程及铌富集过程.粗面质岩石中榍石原位U-Pb定年的结果为432.4±4.4 Ma（n=30，MSWD=2.4），这与区域上其他粗面岩、基性岩、碳酸岩-碱性岩杂岩体形成年龄基本一致，说明研究区在早志留世发生过大规模的碱性岩浆活动.碱性玄武岩和粗面岩中榍石均可以分为岩浆榍石及捕获榍石.不同类型的榍石具有明显的产状和地球化学特征上的差异，其中岩浆榍石以自形、粒度大、振荡环带发育为主要特征，也有部分以微小粒状的形式产于基质或斑晶榍石周围，其通常具有贫Al和低Al/Fe的特点；而捕获榍石以破碎程度高、多产在岩屑内部及周围为典型特征，部分以晶屑的形式弥散状分布，且具有富Al及高Al/Fe的特点.早期形成的碱性玄武岩中的岩浆榍石具有相对较低Nb2O5（< 0.47%）、Na2O（< 0.05%）和REE2O3（< 0.87%）的特征，但Al2O3+Fe2O3的含量变化较大（0.80%~2.91%），说明早期玄武质岩浆的Nb含量相对较低.而粗面岩中的岩浆榍石明显富集Nb2O5（0.19%~1.50%）及REE2O3（0.02%~4.06%），结合镜下观察到微细铌铁矿、易解石等铌矿物发育在粗面质岩石中，指示了碱性岩浆从玄武质到粗面质演化的过程中，Nb的含量发生了明显的提高并最终在粗面岩中富集成矿.Abstract: The Tianbao niobium deposit, located in the Wudang area of the South Qinling belt, is a typical alkaline volcanic-rock hosted Nb deposit in China. However, the research on the origin and evolution of alkaline magma as well as the enrichment mechanism of Nb is lacking. The alkaline volcanic rocks in Tianbao can be divided into trachyte series and alkaline basalt series, which are spatially associated. In this study, it presents detailed petrography observation combined with in-situ U-Pb dating of titanite by LA-ICP-MS, and in-situ element analyses of different types of titanite by EPMA, to reveal the magma evolution and the Nb enrichment processes. The trachyte rocks have titanite U-Pb age of 432.4±4.4 Ma(n=30, MSWD=2.4), which is consistent with the zircon U-Pb age of other trachytes, mafic dykes, and carbonatite-alkaline complexes in the South Qinling belt, indicating that the study area had large-scale alkaline magmatism activation in the Early Silurian. The titanite from both trachyte and alkaline basalt rock are of magmatic and detrital origins based on their occurrences and geochemical characteristics. Most magmatic titanite grains are euhedral and coarse, and have oscillating zoning, while some grains are present in the form of small particles around the titanite phenocrysts. They have lower Al contents and Al/Fe ratios compared to detrital titanites, which are typically fragmented. The magmatic titanites in the early basaltic rock have lower concentrations of Nb2O5 (< 0.47%), Na2O (< 0.05%) and REE2O3 (< 0.87%), but have a large variety of Al2O3+ Fe2O3 (0.80%-2.91%), indicating that the Nb content in the early basaltic magma is relatively low. The magmatic titanites in the trachyte are obviously enriched in Nb2O5 (0.19%-1.50%) and REE2O3 (0.02%-4.06%). Trachytes also contain fine-grained other Nb minerals such as pyrochlore, columbite, and aeschynite, indicating that the contents of Nb are significantly increased during magma fractionation from basalt to trachyte, and eventually lead to ore-grade mineralization in trachyte.
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图 1 秦岭位置的大地构造简图（a）和南秦岭区域地质图（b）
图a据张成立等（2007）修改，图b据Wang et al.（2017）修改
Fig. 1. Schematic diagram of the structure of Qinling belt (a) and geological map of South Qinling belt (b)
图 2 天宝碱性火山岩型铌矿床矿区地质图
据刘万亮等（2015）修改
Fig. 2. Geological map of Tianbao alkaline volcanic-rock hosted Nb deposit
图 3 天宝碱性火山岩型铌矿床钻孔2001岩性柱状图
Fig. 3. Lithology column of ZK2001 in the Tianbao alkaline volcanic-rock hosted Nb deposit
图 4 粗面质岩石手标本及镜下照片
a.长石呈斑晶产出在粗面岩中；b.钾长石斑晶；c.钾长石冷阴极发光照片显示钾长石发生了明显的钠化；d.褐帘石呈斑晶产出；e.粗面岩中具有明显核边结构的磷灰石；f.铌矿物和锆矿物以微细粒状分布在基质中；g.铌矿物产出在榍石、黑云母斑晶矿物的周围及裂隙中；h.粗面质凝灰岩手标本照片；i.粗面质凝灰岩阴极发光图像. Ab.钠长石；Ap.磷灰石；Ase.易解石；Cal.方解石；Kf.钾长石；Ilm.钛铁矿；Ksp.长石；Ttn.榍石；Zr.锆石
Fig. 4. Hand specimen and microscope photos of trachyte
图 5 碱性玄武岩手标本及镜下照片
a.玄武质角砾岩手标本照片；b，c.玄武质角砾岩镜下照片；d.玄武质凝灰岩镜下照片；e.发育有热液边的磷灰石；f.玄武质凝灰岩中的榍石；Ap.磷灰石；Px.辉石族；Ttn.榍石
Fig. 5. Hand specimen and microscope photos of alkaline basalt
图 6 天宝碱性火山岩岩中不同产状的榍石BSE镜下照片
a~c.粗面质岩石中的斑晶榍石；d.粗面质岩石中的基质榍石；e.粗面质岩石中的捕获榍石；f，g.碱性玄武岩中的岩浆榍石；h~i.碱性玄武岩中的捕获榍石
Fig. 6. BSE photos of different types of titanite in the Tianbao alkaline volcanic rock
图 7 天宝粗面岩榍石U-Pb年龄
a.反协和关系图；b.铅校正后加权平均年龄
Fig. 7. U-Pb age of titanate from Tianbao trachyte
图 8 天宝碱性岩榍石Fe-Al(a)和Al-Ti(b)含量（apfu）图解
Ttn1-1. 粗面岩中的斑晶榍石；Ttn1-2. 粗面岩中的基质榍石；Ttn1-3. 粗面岩中的捕获榍石；Ttn2-1. 碱性玄武岩中的斑晶榍石；Ttn2-2. 碱性玄武岩中的捕获榍石（下同）
Fig. 8. Illustrations of Fe-Al (a) and Al-Ti (b) content (in atoms per formula unit) of titanite fromTianbao alkaline rocks
图 9 天宝碱性岩中榍石元素含量（apfu）协变图解
Fig. 9. Compositional variations (in atoms per formula unit) of titanite from Tianbao alkaline volcanic rocks
图 10 南秦岭地区早古生代碱性岩浆岩年龄汇总
Fig. 10. Age summary of alkaline magmatic rocks from the South Qinling belt
表 1 天宝粗面岩LA-ICP-MS榍石U-Pb定年结果
Table 1. LA-ICP-MS titanite U-Pb dating results of trachyte from Tianbao
分析点号 Pb Th U 207Pb/206Pb 207Pb/235U 206Pb/238U 206Pb/238U (10-6) Ratio 1σ Ratio 1σ Ratio 1σ Age (Ma) 1σ B20-01 3.45 80.5 10.50 0.396 6 0.05 4.265 6 0.35 0.099 0 0.00 386.9 23.7 TB20-02 3.76 85.1 10.50 0.280 7 0.03 3.963 7 0.30 0.118 2 0.00 499.1 27.7 TB20-03 3.85 90.1 10.60 0.298 5 0.03 3.823 5 0.31 0.110 0 0.00 464.5 27.7 TB20-04 3.49 79.5 10.50 0.310 7 0.03 3.774 3 0.25 0.110 3 0.01 458.1 26.8 TB20-05 3.49 76.6 10.30 0.316 0 0.03 3.832 2 0.37 0.108 4 0.01 449.9 26.7 TB20-06 3.96 105.9 11.90 0.295 4 0.03 3.634 4 0.32 0.104 8 0.00 451.4 28.8 TB20-07 3.62 82.1 10.70 0.388 2 0.07 4.290 4 0.31 0.108 6 0.00 413.0 22.4 TB20-08 3.99 100.9 10.60 0.402 2 0.05 4.613 6 0.31 0.109 6 0.01 408.6 21.6 TB20-09 3.68 88.8 10.20 0.321 6 0.03 4.261 6 0.31 0.114 3 0.01 462.2 25.4 TB20-10 3.40 81.4 10.40 0.401 4 0.06 4.367 9 0.33 0.107 6 0.00 404.6 21.9 TB20-11 3.83 90.1 10.60 0.394 4 0.04 4.961 3 0.37 0.111 4 0.00 416.3 21.7 TB20-12 3.66 89.0 10.70 0.347 3 0.03 4.556 6 0.35 0.108 7 0.00 433.6 24.7 TB20-13 3.64 85.0 10.50 0.402 2 0.05 4.298 3 0.31 0.106 6 0.00 402.0 22.1 TB20-14 3.64 80.2 10.10 0.396 3 0.06 4.626 7 0.44 0.110 3 0.01 412.9 21.7 TB20-15 4.14 95.0 10.30 0.348 2 0.04 4.721 3 0.32 0.127 5 0.01 477.3 21.7 TB20-16 3.45 75.0 9.45 0.405 0 0.04 4.914 0 0.40 0.108 9 0.00 405.8 21.5 TB20-17 3.12 79.7 9.91 0.425 8 0.07 4.201 6 0.39 0.094 2 0.00 364.1 23.2 TB20-18 3.05 71.9 9.84 0.400 5 0.05 3.862 7 0.29 0.100 6 0.00 389.0 23.2 TB20-19 3.51 80.6 10.80 0.432 2 0.05 4.766 5 0.32 0.101 1 0.00 377.2 21.6 TB20-20 4.17 81.5 10.10 0.420 6 0.04 6.413 3 0.52 0.134 7 0.01 448.2 17.2 TB20-21 3.89 92.5 11.50 0.291 4 0.03 3.741 6 0.32 0.108 7 0.00 465.1 28.4 TB20-22 3.92 96.6 11.10 0.313 4 0.03 4.212 6 0.31 0.104 5 0.00 440.6 27.6 TB20-23 3.75 86.5 11.40 0.300 6 0.02 3.930 2 0.25 0.107 5 0.00 456.2 27.9 TB20-24 4.01 78.6 10.90 0.310 1 0.02 5.077 6 0.35 0.133 1 0.01 516.5 23.4 TB20-25 3.41 75.0 10.00 0.407 8 0.06 4.146 0 0.38 0.108 5 0.01 403.7 21.5 TB20-26 3.24 72.2 9.56 0.320 4 0.05 3.709 8 0.41 0.109 5 0.01 450.3 26.2 TB20-27 3.67 75.9 10.50 0.346 6 0.03 4.809 1 0.31 0.115 3 0.00 450.2 23.7 TB20-28 4.18 97.7 11.60 0.333 5 0.04 4.593 3 0.35 0.121 7 0.01 473.3 23.5 TB20-29 4.05 108.0 11.10 0.228 3 0.03 2.971 0 0.32 0.104 9 0.01 493.5 34.4 TB20-30 3.47 83.4 10.80 0.353 1 0.03 4.555 4 0.35 0.105 7 0.00 423.1 24.9 注：利用在线Isoplot（http://www.isoplotr.com/isoplotr/）中等时线型普通铅（Isochron）法进行普通铅校正. 
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表 2 天宝碱性火山岩中榍石主微量元素分析结果（均值：%）
Table 2. Major and trace element compositions (%) of titanite from Tianbao alkaline volcanic rocks (average)
岩性 粗面质岩石 碱性玄武岩 类型 Ttn1-1 Ttn1-2 Ttn1-3 Ttn2-1 Ttn2-2 样品编号（数量） TB14、ZK37、ZK51（N=28） ZK51（N=5） TB14（N=8） TB8、ZK116（N=22） TB3、TB8（N=15） Al2O3 1.05 0.73 3.70 0.94 3.24 TiO2 34.60 36.80 32.80 38.10 33.90 CaO 26.90 27.50 29.60 29.50 29.60 Y2O3 0.25 0.19 0.02 0.07 0.01 Ta2O5 0.00 0.00 0.00 0.00 0.00 MnO 0.18 0.05 0.01 0.03 0.01 Nd2O3 0.57 0.21 0.07 0.10 0.04 Na2O 0.27 0.72 0.05 0.02 0.05 MgO 0.09 0.05 0.08 0.03 0.11 SiO2 29.60 31.00 31.60 30.60 31.50 Nb2O5 1.00 0.81 0.70 0.24 0.15 Fe2O3 2.35 1.91 1.48 0.84 1.47 Pr2O3 0.18 0.06 0.03 0.06 0.02 Ce2O3 1.31 0.07 0.00 0.08 0.00 La2O3 0.46 0.01 0.01 0.03 0.01 F 0.15 0.12 0.60 0.03 0.32 Cl 0.00 0.01 0.00 0.00 0.01 总量 98.60 100.00 100.40 100.60 100.20
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