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作者简介:

丁绵绵,女,1998年生。硕士研究生,矿物学、岩石学、矿床学专业。E-mail:MG21290002@smail.nju.edu.cn。

通讯作者:

车旭东,男,1982年生。副教授,主要从事稀有金属成矿研究。E-mail:xdche@nju.edu.cn。

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周新民, 李武显. 2000. 中国东南部晚中生代火成岩成因: 岩石圈消减和玄武岩底侵相结合的模式. 自然科学进展, (3): 50~57.
目录contents

    摘要

    稀有金属铌钽在我国华南存在多时代成矿特征,前人对其最晚成矿期晚白垩世成矿事件报道较少。本文以浙东南的吴小垟铌矿床为研究对象,结合野外调查、岩石学、矿物原位微区分析和同位素年代学等研究,确定矿床铌成矿岩体为细粒黑云母花岗岩,成岩成矿年龄分别为89.2±0.8 Ma和86.5±1.0 Ma,揭示了该区存在晚白垩世花岗岩侵位及其相关铌成矿事件。铌除了以独立矿物的形式赋存在铌铁矿、铌铁金红石、铅烧绿石中,还有部分铌赋存于黑云母中。在岩浆-热液作用下,云母类型发生了从铁云母→黑鳞云母→铁锂云母的变化。铁云母Nb含量最高可达1253×10-6,黑鳞云母-铁锂云母铌含量最高至794×10-6,黑云母极度富铌的特征,指示该花岗岩具有非常好的铌找矿潜力,富铌黑云母可以作为一种铌钽找矿指示性矿物。综合上述矿物学特征,得出吴小垟矿床存在两阶段铌成矿事件:岩浆期原生铌铁矿族矿物、原生富铌黑云母和铌铁金红石的形成;以及后期热液作用下铌从岩浆和原生含铌矿物中迁移出形成次生的含铌氧化物。

    Abstract

    The rare mental niobium-tantalum has multi-epoch metallogenic characteristics in South of China, and the Late Cretaceous metallogenic event as the latest metallogenic stage is rarely reported by predecessors. This paper focuses on the Wuxiaoyang Niobium deposit in southeast of Zhejiang Province. By combining field investigation, petrology, in situ microzone analysis of minerals and isotopic chronology, we determined that the main body of niobium mineralization is fine-grained biotite granite. The diagenetic and metallogenic ages are 89.2±0.8 Ma and 86.5±1.0 Ma respectively, revealing an important Late Cretaceous granite emplacement and niobium mineralization event in this area. Niobium occurs in the form of independent minerals in columbite group mineral, rutile and plumbopyrchlore. In addition, part of niobium occurs in biotite. Under magma-hydrothermal interaction, the mica evolved from annite to protolithionite to zinnwaldite; the highest Nb-content of annite was 1253×10-6, and the highest Nb-content of protolithionite and zinnwaldite was 794×10-6. As the extremely Nb-rich characteristics of biotite indicate that the deposit has a very well niobium prospecting potential, the Nb-rich biotite can be used as an indicator mineral for niobium-tantalum prospecting. Based on the above mineralogical characteristics, there are two stages of niobium mineralization events in this deposit: firstly, the formation of primary columbite group minerals, Nb-rich biotite and rutile in magmatic stage; secondly, niobium migrates from magma and primary Nb-bearing minerals to form secondary niobium-containing oxides under late hydrothermal action.

  • 稀有金属铌(Nb)、钽(Ta)由于良好的耐热性与延展性、较高的熔点与热导率等特性,是电子、航天航空、化工等产业的重要原料,在国防科技、高新技术和医疗等领域具有不可替代性(谭东波等,2018)。因此,铌和钽被视为重要的战略性关键金属(侯增谦等,2020)。

  • 世界上的铌钽矿床分为内生型、外生型两大类,以内生型为主。内生型铌钽矿床主要与过铝或者准铝质花岗岩或花岗伟晶岩和碱性—过碱性花岗岩、伟晶岩及碳酸岩有关(Linnen and Cuney,2005)。中国的铌钽资源主要产自过铝质花岗岩和花岗伟晶岩中,华南是中国重要的铌钽成矿地区,其Nb-Ta矿化通常与高分异花岗岩、花岗伟晶岩相关(王汝成等,2020)。近期研究发现,华南许多超大型铌钽矿床的形成与富铌黑云母花岗岩密切相关,如与江苏苏州善安浜铌钽矿床相关的苏州花岗岩岩体中的铁云母Nb平均含量为100×10-6~769×10-6,而含锂铁云母Nb含量更高,可达1426×10-6,平均含量为720×10-6Tian Ennong et al.,2021),赣东北黄山铌矿床相关的黄山岩体的中粒花岗岩中黑鳞云母Nb平均含量为884×10-6,而铁云母Nb平均含量可达1347×10-6Zhu Zeying et al.,2018)。

  • 基于铌铁矿族矿物U-Pb定年和地球化学研究,Che Xudong et al.(2019)等将华南地区Nb-Ta成矿划分为多期矿化事件,最后一期铌钽矿化事件发生在晚白垩世(约90 Ma),是发现铌钽矿床最少的一期,代表性矿床是湖南的界牌岭矿床(Xie Lei et al.,2016),成岩成矿时间被限制在91~89 Ma。先前研究对于华南地区白垩纪铌钽成矿重点停留在早白垩世(毛景文等,2008王汝成等,2020赵正等,2022),随着华南地区铌钽成矿研究的深入,晚白垩世成矿受到更多的关注。例如:Zhao Zhuang et al.(2021)报道的南岭地区上堡矿床,成岩成矿时间分别为87.3±0.9 Ma、86.83±0.8 Ma,同样揭示华南地区存在晚白垩世岩浆活动、花岗岩侵位及相关Nb-Ta矿化。中国东南沿海地区广泛发育一条中生代火山-侵入杂岩带,具有良好的稀有金属成矿潜力 (杜杨松等,1990饶灿等,2022),但目前对于东南沿海地区铌钽成矿的研究并不多。因此本次研究重点关注东南沿海地区的晚白垩世铌成矿。

  • 吴小垟矿床是近些年来新发现的铌矿床,位于浙江省温州市平阳县。该矿床位于平阳山门火山洼地,围绕该破火山边缘及中心分布着铌钽、黄铁矿、铜铅锌多金属等多个矿点(徐厚倜,2015)。浙江省第十一地质大队(2019)对该区域的普查中报道了吴小垟铌矿,铌矿化发生在细粒黑云母花岗岩中,简述了矿床地质、成因和找矿前景分析,未对其年代学、矿物学及成矿机理等方面开展系统的研究工作。本次研究基于全岩主微量元素分析、锆石和铌铁矿U-Pb定年、含铌氧化物矿物原位微区分析等工作,厘定吴小垟矿床的成矿时代,探讨其矿床成因,并评估其铌钽成矿潜力,进一步讨论富铌黑云母对铌钽成矿作用的指示意义,并促进对华南地区晚白垩世花岗岩Nb-Ta成矿的认识。

  • 1 区域地质背景

  • 中生代期间,中国东南部岩浆活动强烈,火山-岩浆作用在中国东南沿海地区形成一条广泛分布的火山岩带(图1),该带是环太平洋火山-侵入岩带的重要组成部分。中国东南沿海地区中生代火山岩浆活动起始于早侏罗世,在早白垩世达到高峰,结束于晚白垩世早期(邢光福等, 2009)。统计显示,这些火山岩、花岗岩形成在中侏罗世(180~160 Ma)的约占13.5%;形成在晚侏罗世(159~140 Ma)的约占19.4%;形成在早白垩世(139~97 Ma)的约占57.2%;形成在晚白垩世(96~65 Ma)的约占9.8% (李武显和周新民,2000)。此外,此火山岩带显著的特征是,主要以酸性岩浆岩(花岗岩、流纹岩)为主(王德滋等,2000)。

  • 目前研究认为,东南沿海地区中生代火山岩形成于伸展构造背景,与古太平洋板块的俯冲作用有关(Li Zhengxiang and Li Xianhua,2007邢光福等,20082009)。区域内晚中生代大规模酸性岩浆活动可能与玄武岩底侵作用引起的陆壳部分熔融有关(Zhou Xinmin et al.,2006Guo Feng et al.,2012),壳幔混合作用和岩浆混合作用是该火山岩带形成的重要原因(周新民和李武显,2000)。

  • 这条火山岩带具有同源、同时、同空间和同步迁移和喷发-侵入相交替的特征,因此被称为东南沿海火山-侵入杂岩体(王德滋等,2000)。地球化学数据表明该火山侵入杂岩体中富含稀有金属元素(谢学锦,2012),其中发育许多与花岗岩有关的中生代稀有金属(W-Sn-Nb-Ta-Li-Be)矿床,例如:浙江青田铍矿、福建霞浦大湾铍矿、浙江平阳地区张基铍多金属矿与吴小垟铌矿、福建平和福里石铍矿、浙江千亩田铍矿、浙江铜山铍矿、广东大坑铌铁矿、广东泰美铌铁矿、广东大方铌钽矿、浙江河桥锂铍铌钽矿床(徐厚倜,2015黄新鹏,2016;胡庆海,2017;饶灿等,2022),大规模稀有金属成矿主要集中于早白垩世(135~125 Ma)和早白垩世—晚白垩世(105~90 Ma)(李晓峰等,2021)。这些稀有金属矿床的分布受区域性断裂控制,成矿类型主要为花岗岩型、伟晶岩型和火山岩型;东南沿海地区中生代稀有金属富集与区域内大规模的火山活动、花岗质岩浆的侵入及其侵入后的热液作用密切相关(毛景文等,2008)。

  • 2 矿床地质背景

  • 晚中生代强烈的火山-岩浆活动在整个区域内形成一条北东-南西向展布的曹门-张基花岗斑岩脉,与矿区相邻(图2)。前人勘探结果表明,研究区内共发现矿点约8个,主要分布在平阳县吴小垟村—瑞安市张基村,分别是:吴小垟铌矿、吴小垟铍多金属矿、百尖高岭土矿、张基铍矿、张基多金属矿床、毛竹坑多金属矿、赤馏铅锌矿和黄岭头铜铅矿等。张基铍矿与张基多金属矿出露于下白垩统馆头组,其他矿床均出露于下白垩统朝川组。钨锡铍矿、铌铁矿、磷钇矿主要分布在地区西北部的龙尾—张基一带,近曹门-张基花岗斑岩体;而铜、银、铅锌多金属矿多分布于南部、东部地区,离曹门-张基花岗斑岩体相对较远。

  • 以江山-绍兴断裂为界,浙西北地区属扬子地块,而浙东南地区属华夏地块,矿区隶属于浙东南地区(崔玉荣等,2010)。矿区内发育多条断裂,为成矿提供了良好的空间;泰顺-黄岩大断裂从勘查区西北侧约20 km处通过,温州-镇海大断裂从勘查区东南侧约22 km处通过,松阳-平阳大断裂从勘查区北东部通过(图3a)。研究区位于山门沉积型火山洼地东部的内部边缘和双尖山破火山的北缘(图3b),矿点往往围绕该山门火山洼地和破火山边缘及中心分布。

  • 图1 我国东南沿海地区火山-侵入岩及矿床分布简图(改自Jiang Yaohui et al.,2015饶灿等,2022

  • Fig.1 Distribution of volcano-intrusive rocks and deposit in southeast coastal area of China (modified after Jiang Yaohui et al.,2015Rao Can et al.,2022

  • 浙东南沿海火山活动带是中国东南部中生代火山岩带的重要组成部分,构造上隶属浙闽沿海中生代活动大陆边缘(董传万和彭亚鸣,1994),吴小垟矿床就位于该火山活动带。该成矿区位于环西太平洋活动大陆边缘,中生代以来火山活动强烈,形成巨厚的火山-沉积岩系,同时伴生岩浆侵入作用,发育火山构造、断裂构造。区内中生代火山岩主要活动时代为140~105 Ma,为早白垩世;而从晚白垩世开始,火山喷发的强度逐渐减弱,并且喷发中心发生了从浙西到浙东沿海的转移变化(李坤英,1982)。浙东南地区晚中生代火山岩地层为磨山石群(自下而上分别为大爽组、高坞组、西山头组、茶湾组、九里坪组)和永康群(自下而上分别为馆头组、朝川组、小平田组、泰顺组)(段政,2013)。矿区出露的地层主要为下白垩统永康群的一套杂色湖相沉积岩夹火山碎屑岩,出现的永康群为馆头组(K1g)、朝川组(K1c)。本区馆头组岩性为河湖相沉积岩,局部出露玄武岩-流纹岩双峰式火山岩;而朝川组为紫红色陆相沉积岩夹酸性火山碎屑岩。

  • 吴小垟矿床出露于下白垩统朝川组(K1c),前人对朝川组的黑云母进行K-Ar稀释法定年,测得结果为111 Ma(李坤英等,1989),代表朝川组火成岩的结晶年龄,因此也可以代表火成岩的形成年龄。前人将浙东南燕山期中生代火山活动分为四个旋回,第一旋回形成的火山岩年龄为200~165 Ma;第二旋回火山岩形成年龄为165~145 Ma,第三旋回火山岩形成年龄为145~115 Ma,第四旋回火山岩形成年龄为115~85 Ma(余明刚等,2021),吴小垟矿床赋存的下白垩统朝川组形成在中生代火山活动的第四旋回。

  • 图2 吴小垟矿区地质简图(据浙江省第十一地质大队,2019修改)

  • Fig.2 Geological schematic map of the Wuxiaoyang deposit (modified after Zhejiang Province Eleventh Team, 2019

  • 浙江省第十一地质大队前期普查资料显示,吴小垟铌矿出露面积0.023 km2,地表宽度3.0~40.7 m不等,Nb2O5的品位为0.043%~0.091%,铌矿化主要矿石矿物为铌铁矿,赋存在细粒黑云母花岗岩中。发现其含矿花岗岩向底部变深变宽,Nb2O5品位达到0.025%以上的岩体厚度近30 m,其特点为低品位和厚度大,该地区具有一定的铌成矿潜力。

  • 3 样品和分析方法

  • 本次研究在吴小垟矿床采到3套样品,分别是细粒黑云母花岗岩(样品WXY1-2-2)、矿区不成矿细粒二云母花岗岩围岩(样品WXY2-1)以及曹门-张基花岗斑岩脉(样品NSY-1)。样品手标本及薄片照片如图4所示。铌铁矿族矿物和含铌氧化物主要赋存在细粒黑云母花岗岩中。所有样品在手标本和显微镜下均能观察到明显的蚀变现象。

  • 细粒黑云母花岗岩(图4a~c),粒径介于0.2~0.4 mm之间,主要矿物组合为石英(~45%)、钾长石(~40%)、钠长石(~10%)、黑云母(~5%),副矿物包括铌铁矿、铌铁金红石、锆石、萤石、赤铁矿和磷灰石等。

  • 细粒二云母花岗岩(图4d~f),成矿岩体的围岩,粒径介于0.4~1 mm之间。主要矿物组合为石英(~25%)、钾长石(~30%)、钠长石(~30%)、黑云母(~5%),白云母(~2%),副矿物包括锆石、萤石、钛铁氧化物等。

  • 花岗斑岩(脉),斑状结构,基质呈微—细粒结构;斑晶主要为蚀变钾长石、石英,斑晶自形程度较高,含量约为45%;基质主要由钠长石(~15%)、石英(~15%)、钾长石(~15%)组成(图4g~i);副矿物为锆石、赤铁矿等铁氧化矿物、萤石和高岭土等。

  • 图3 吴小垟矿区区域构造图

  • Fig.3 Simplified geological map of the Wuxiaoyang deposit

  • (a)—矿区构造图(据浙江省第十一地质大队,2019);(b)—山门洼地火山构造位置图(据徐厚倜,2015

  • (a)—structural map of mining area (after Zhejiang Province Eleventh Team,2019); (b)—volcanic structure location of Shanmen depression(after Xu Houti,2015)

  • 3.1 全岩主微量元素分析

  • 全岩主量元素分析在南京大学内生金属矿床成矿机制研究国家重点实验室X荧光光谱(XRF)实验室完成,仪器为Thermo Scientific ARL 9900型X射线荧光光谱仪,测试条件为电压40 kV,电流70 mA,每个元素扫描时间为20 s,使用标样BHVO-2和BCR-2,相对误差在元素丰度>1.0%时为±1%,元素丰度<1.0%时为±10%。

  • 全岩微量元素分析在聚谱检测科技有限公司(南京)使用ICP-MS完成,仪器型号是Agilent7700X,详细分析方法见Qi Liang et al.(2000)。使用美国地质调查局USGS的BHVO-2、AGV-2和W-2,以及GeoPT9的OU-6标样用于校正,微量元素分析精度优于10%。

  • 3.2 EPMA原位微区主量元素分析

  • 背散射电子图像(BSE)和矿物主量元素分析在南京大学内生金属矿床成矿机制研究国家重点实验室使用电子探针JEOL JXA-8230完成。工作条件为:加速电压15 kV,电子束电流20 nA,云母测试束斑直径为3 μm,铌铁矿族矿物及铌氧化物矿物测试束斑直径为1 μm,矿物主要元素峰位设定为10 s,次要元素峰位时间设定为20 s,背景测定时间为峰位时间的一半。分析矿物为云母(主要组成元素为Si、Al、Fe、K、F,次要组成元素为Mn、Ti、Mg、Ca、Na、Nb、Ta)、铌铁矿族矿物(主要组成元素为Nb、Ta、Fe,次要组成元素为Sc、W、Mn、Sn、Ti)和铌氧化物矿物。云母分析使用如下标样:角闪石、铁橄榄石、金红石、黑云母、磷灰石、黄玉和铌钽铯合成金属。铌铁矿族矿物和铌氧化物矿物采用以下标样:合成Fe2O3、铌钽铯合成金属、白钨矿、铁橄榄石和合成的化合物(SnO2和MnTiO3),测试数据统一进行ZAF矫正。

  • 3.3 锆石、铌铁矿U-Pb定年

  • 从成矿细粒黑云母花岗岩中挑选锆石、铌铁矿,及从曹门张基-花岗斑岩中选取锆石用于U-Pb年代学测定。在河北省廊坊市诚信地质服务有限公司对锆石、铌铁矿进行分选:将样品洗净并碎至60~80目后用淘洗法选出纯度较高的单矿物,在双目镜下挑选出形态完整的锆石和铌铁矿颗粒。将待测矿物晶体固定制靶、抛光,并对靶中的锆石做阴极发光(CL)图像拍摄,对铌铁矿做背散射电子(BSE)图像拍摄。锆石、铌铁矿U-Pb定年分析在南京大学内生金属矿床成矿机制研究国家重点实验室使用激光剥蚀-电感耦合等离子体质谱仪(LA-ICP-MS)完成,该仪器由Thermo Fisher Scientific公司的i-Cap Q 型的电感耦合等离子体质谱仪和 Australian Scientific Instruments公司的RESOlution S-155型激光剥蚀系统组成。

  • 图4 吴小垟矿床岩石手标本、显微照片以及背散射电子(BSE)图像

  • Fig.4 Hand specimen photographs, microscopic features and back-scattered electron (BSE) images of rocks in the Wuxiaoyang deposit

  • (a~c)—样品WXY1-2-2,细粒黑云母花岗岩;(d~f)—样品WXY2-1,细粒二云母花岗岩(部分位置有萤石脉穿插);(g~i)—样品NSY-1,花岗斑岩;Bt—黑云母;Qtz—石英;Kfs—钾长石;Fl—萤石;Ab—钠长石;Hem—赤铁矿;Ms—白云母;Zrn—锆石

  • (a~c)—sample WXY1-2-2,fine-grained biotite granite; (d~f)—sample WXY2-1,fine-grained two-mica granite (fluorite veins inserted in some locations); (g~i)—sample NSY-1,granite porphyry;Bt—biotite;Qtz—quartz;Kfs—K-feldspar;Fl—fluorite;Ab—albite;Hem—hematite; Ms—muscovite; Zrn—zircon

  • 锆石激光剥蚀工作参数:激光脉冲频率5 Hz,脉冲能量密度~3.3 J/cm2,熔蚀微区直径为29 μm;总计数时间为90 s,其中背景值测定40 s,峰位测定50 s。每8个样品点测试中,插入2次国际标准锆石91500(1065.4±0.3 Ma)(Wiedenbeck et al.,1995)作为定年标样,2次锆石PLE作为定年监测标样,2次SRM610和1次SRM612作为微量元素分析标样。

  • 铌铁矿激光剥蚀工作参数:激光脉冲频率4 Hz,脉冲能量密6 J/cm2,熔蚀微区直径为43 μm;总计数时间为90 s,其中背景值测定40 s,峰位测定50 s。在每8个样品测点中插入2次铌铁矿标样Coltan 139(506.2±5.0 Ma)(Melcher et al.,2015)作为定年标样,1次铌铁矿RL、SN3作为定年监测标样(Xiang Lu et al.,2023),2次SRM610作为微量元素分析标样,1次BCR-2G、GSE-1G作为微量监测标样。具体实验流程参考Che Xudong et al.(2015)

  • 对分析数据的离线处理(包括对样品和空白信号的选择、仪器灵敏度漂移矫正、元素含量及U-Th-Pb同位素比值和年龄计算)采用软件ICPMSDataCal完成(Liu Yongsheng et al.,20082010)。锆石和铌铁矿样品的U-Pb年龄谐和图绘制和年龄权重平均计算均采用Isoplot/Ex_ver3完成(Ludwig,2003)。

  • 3.4 LA-ICP-MS微量元素分析

  • 云母和铌铁矿的微量元素分析在南京大学内生金属矿床成矿机制研究国家重点实验室使用激光剥蚀-电感耦合等离子体质谱仪(LA-ICP-MS)完成。铌铁矿族矿物分析条件同U-Pb定年条件;云母工作参数如下:激光脉冲频率4 Hz,脉冲能量密度~3.6 J/cm2,熔蚀微区直径为29 μm;总计数时间为80 s,其中背景值测定40 s,峰位测定40 s。实验过程中采用美国国家标准技术研究院的标准玻璃NIST SRM 610和NIST SRM 612作外标,美国地质调查局玄武岩玻璃BCR-2G和GSE-1C作监测标样来校准元素灵敏度并确认测试的准确性(Gao Jianfeng et al.,2013)。数据统一使用ICPMSData Cal程序离线处理(Liu Yongsheng et al.,2008),云母使用29Si、铌铁矿使用55Mn作为内标来矫正仪器漂移,含量相对偏差优于±10%。

  • 4 结果

  • 4.1 全岩地球化学特征

  • 表1列出了细粒黑云母花岗岩、细粒二云母花岗岩围岩、花岗斑岩(脉)全岩主、微量元素分析结果。区域内样品均呈现出高硅(SiO2 = 75.31%~77.06%)、富铝(Al2O3 =12.50%~13.40%)、富碱(K2O=3.70%~5.23%,Na2O = 1.51%~4.31%)和低钙(CaO < 0.20%)的特征,地球化学特征均为过铝质(图5a)。对比未成矿的样品,细粒黑云母花岗岩具有更高的铝 (Al2O3=13.40%)和碱含量(K2O=5.23%,Na2O=4.31%)

  • 微量元素分析结果显示,细粒黑云母花岗岩相比于未成矿的样品具有较高的Nb(114×10-6)、Ta(10.2×10-6)含量、较低的Nb/Ta(11.11)和Zr/Hf(22.41)比值。细粒黑云母花岗岩、细粒二云母花岗岩围岩和花岗斑岩(脉)中稀土元素总量相差较大,前者的稀土总量为50.1×10-6,后两者的稀土总量为133×10-6~327×10-6;球粒陨石标准化的稀土元素配分曲线均为大致水平的“海鸥式”形状,成矿细粒黑云母花岗岩具有更明显的Eu负异常(δEu=0.03)(图5b)。

  • 4.2 铌元素的赋存状态

  • 自然界中铌元素主要以独立矿物、类质同象和微细包裹体的形式存在(马驰等,2011)。为探明吴小垟矿区中铌元素的赋存状态,我们对样品进行背散射电子(BSE)图像观察、EMPA电子探针定量分析以及LA-ICP-MS微量元素分析。研究发现,吴小垟矿区铌元素以独立矿物的形式赋存在铌铁矿族矿物、铌铁金红石、铅烧绿石中,部分铌还以类质同象的形式赋存在黑云母中。

  • (1)铌铁矿族矿物(Fe,Mn)(Nb,Ta)2O6:是吴小垟矿床中分布最广泛的铌矿物。其背散射电子图像如图6所示。铌铁矿族矿物按照晶形可分为两种类型:① 呈自形的板状、柱状晶形,粒径为50~120 μm(图6a、b),分布在造岩矿物中;② 铌铁矿受蚀变呈不规则晶形,粒径较小,为5~20 μm(图6c、d),多呈星散状嵌布在造岩矿物中。铌铁矿族矿物的共生矿物有钾长石、钠长石、石英、萤石、锆石、黑云母等。明显自形、原生的板-柱状铌铁矿族矿物可见明显的岩浆变化环带,具有核边结构。核、边部的FeO、MnO含量变化不大;边部区域Nb2O5含量在65.25%~70.09%,Ta2O5含量在4.50%~10.35%,而核部区域Nb2O5含量在73.98%~76.12%,Ta2O5含量在1.49%~3.09%,边部铌低钽高,而核部铌高钽低;其他元素含量未见明显差异(表2)。边部、核部的Ta/(Ta+Nb)比值分别为0.037~0.087和0.013~0.014,Mn/(Fe+Mn)比值分别为0.099~0.114和0.086~0.0160。铌铁矿族矿物还含少量的TiO2、WO3,此外还有痕量的Sc、Sn,其氧化物含量大多低于0.1%或低于检测线。在成分分类图解中,矿区内铌铁矿族矿物均落在铌铁矿的范围内(图7)。铌铁矿稀土元素分析结果见表2,其稀土元素配分曲线具明显的左倾斜特征,为重稀土元素富集型;ΣHREE为2217×10-6~7376×10-6,ΣLREE为27.4×10-6~229×10-6,稀土总量ΣREE为2244×10-6~7605×10-6;配分曲线呈现出明显的Eu负异常(图8)。

  • 图5 吴小垟矿床岩石地球化学特征

  • Fig.5 Whole-rock geochemistry characteristics of the Wuxiaoyang deposit

  • (a)—A/CNK-A/NK图解;(b)—稀土元素球粒陨石标准化配分图解(标准化数据引自McDonough and Sun,1995

  • (a)—diagram of A/CNK-A/NK; (b) —chondrite-normalized REE patterns (chonrite REE values are from McDonough and Sun, 1995

  • 表1 吴小垟矿床样品全岩主量(%)和微量(×10-6)元素分析结果

  • Table1 The results of major elements (%) and trace elements (×10-6) of the samples from the Wuxiaoyang deposit

  • 注:A/CNK=Al2O3/(CaO+Na2O+K2O),A/NK=Al2O3/(Na2O+K2O),均为分子(摩尔)比;ΣREE为稀土总量;δEu为铕的异常程度,δEu=EuN/(SmN×GdN)(详细的计算方法见Taylor and McLenan,1985)。

  • (2)铌铁金红石(Ti,Nb,Fe)O2:铌铁金红石的背散射图像如图9a~d所示,呈他形粒状,粒径约50~100 μm,分布在造岩矿物(黑云母)中,通常被包裹在造岩矿物中。电子探针分析主量元素成分数据见表3;背散射图片下个别颗粒发育明显的环带(图9c、d);其中环带亮处的铌铁金红石主量元素成分相比于暗处铌铁金红石展现出铌高、铁高和钛低的特点,Nb2O5含量为10.28%~18.74%,FeO含量为5.65%~8.50%,TiO2含量为71.68%~82.87%;环带暗处铌铁金红石Nb2O5含量为2.71%~5.77%,FeO含量为2.16%~3.28%,TiO2含量为88.42%~94.54%,此外还有微量的W、Ta、Mn、Sn。

  • 表2 吴小垟矿床细粒黑云母花岗岩中铌铁矿主量元素(%)和微量元素(×10-6)成分特征

  • Table2 Compositions of major elements (%) and trace elements (×10-6) of columbite from fine-grained biotite granite of the Wuxiaoyang deposit

  • 注:“-”表示低于检测限。

  • (3)铅烧绿石(Pb,Y,Ca,U)2-xNb2O6(OH):铅烧绿石的背散射电子(BSE)图像见图9e、f,铅烧绿石呈不规则粒状,很小,粒径仅几个微米,其常常呈零星嵌布于他形铌铁矿中。电子探针主量元素分析结果见表4;铅烧绿石的Nb2O5含量为34.36%~43.37%,而Ta2O5含量在6.37%~15.69%,此外还有微量的Fe、Ti。

  • 图6 吴小垟矿床细粒黑云母花岗岩中铌铁矿背散射电子(BSE)图像

  • Fig.6 Back-scattered electron (BSE) images of columbite from fine-grained biotite granite of the Wuxiaoyang deposit

  • Bt—黑云母;Qtz—石英;Kfs—钾长石;Ab—钠长石;Zrn—锆石;Clb—铌铁矿

  • Bt—biotite;Qtz—quartz;Kfs—K-feldspar;Ab—albite;Zrn—zircon; Clb—columbite

  • 图7 吴小垟矿床细粒黑云母花岗岩中铌铁矿族矿物成分分类图解

  • Fig.7 Compositional classification of columbite group mineral from fine-grained biotite granite of the Wuxiaoyang deposit

  • (4)云母:少量铌元素还以类质同象的形式赋存在黑云母中。吴小垟矿床成矿细粒黑云母花岗岩中明显存在3种黑云母,云母主量元素分析结果见表5、成分分类图解见图11,确定分别为铁云母、黑鳞云母和铁锂云母,铁云母、黑鳞云母属于Li-Fe系列云母,铁锂云母属于Li-Al系列云母。图10为3种云母的背散射电子(BSE)图像,图10a、b为原生铁云母,具有完整片状晶形,背散射图片下显示出成分均一,并且沿着解理发育铁氧化物。图10c、d为黑鳞云母和铁锂云母,一阶段黑鳞云母(Prl-1)具有较好晶形,二阶段黑鳞云母(Prl-2)沿着原生黑鳞云母的边部发育,铁锂云母沿着黑鳞云母内部或裂隙生长。吴小垟矿床中的云母类型显示出“铁云母→黑鳞云母→铁锂云母”的变化,相应出现FeO含量降低,SiO2、Al2O3、Li2O和MgO含量升高的变化 (图12)。云母EPMA电子探针元素分析结果(表5)表明,铁云母Nb2O5含量为0.15%~0.23%,一阶段黑鳞云母Nb2O5含量为0.14%~0.21%,二阶段黑鳞云母Nb2O5含量为0.03%~0.1%,而铁锂云母Nb2O5含量最高仅为0.02%或低于检测限;表明云母是富铌的、Nb2O5随着云母类型的变化而降低。

  • 图8 吴小垟矿床细粒黑云母花岗岩中铌铁矿稀土元素球粒陨石标准化配分图解(标准化数据引自 McDonough and Sun,1995

  • Fig.8 Chondrite-normalized REE patterns of columbit from fine-grained biotite granite of the Wuxiaoyang deposit(chonrite REE values are from McDonough and Sun,1995

  • 图9 吴小垟矿床细粒黑云母花岗岩中铌铁金红石和铅烧绿石背散射电子(BSE)图像

  • Fig.9 Back-scattered electron (BSE) images of rutile and plumbopyrchlore from fine-grained biotite granite of the Wuxiaoyang deposit

  • Bt—黑云母;Qtz—石英;Kfs—钾长石;Ab—钠长石;Zrn—锆石;Rtl—铌铁金红石;Ppcl—-铅烧绿石;Clb—铌铁矿

  • Bt—biotite;Qtz—quartz;Kfs—K-feldspar;Ab—albite;Zrn—zircon; Rtl—rutile; Ppcl—plumbopyrchlore; Clb—columbite

  • 表3 吴小垟矿床细粒黑云母花岗岩中铌铁金红石主量元素(%)成分特征

  • Table3 Compositions (%) of major elements of rutile from fine-grained biotite granite of the Wuxiaoyang deposit

  • 表4 吴小垟矿床细粒黑云母花岗岩中铅烧绿石主量元素(%)成分特征

  • Table4 Compositions (%) of major elements of plumbopyrochlore from fine-grained biotite granite of the Wuxiaoyang deposit

  • 图10 吴小垟矿床细粒黑云母花岗岩中云母背散射电子(BSE)图像

  • Fig.10 Back-scattered electron (BSE) images of mica from fine-grained biotite granite of the Wuxiaoyang deposit

  • Qtz—石英;Kfs—钾长石;Fl—萤石;Ab—钠长石;Hem—赤铁矿;Zrn—锆石;Ann—铁云母;Prl-1—一阶段黑鳞云母;Prl-2—二阶段黑鳞云母;Znw—铁锂云母

  • Qtz—quartz; Kfs—K-feldspar; Fl—fluorite;Ab—albite; Hem—hematite; Zrn—zircon; Ann—lepidomelane; Prl-1—protolithionite of first stage; Prl-2—protolithionite of secend stage; Znw—zinnwaldite

  • 图11 吴小垟矿床细粒黑云母花岗岩中云母成分分类图解 (底图改自Tischendorf et al.,1997

  • Fig.11 Compositional classification of mica from fine-grained biotite granite of the Wuxiaoyang deposit (base map modified from Tischendorf et al.,1997

  • 成矿细粒黑云母花岗岩中云母的微量元素分析结果见表6。由于铁锂云母常沿着黑鳞云母的解理发育、粒度较小呈不规则晶形,因此在LA-ICP-MS实验过程中未将二者分开。云母铌含量很高:铁云母铌含量最高可达1253×10-6,黑鳞云母-铁锂云母铌含量为562×10-6~794×10-6,这与我们对云母主量元素测定时发现的云母富Nb、且从“铁云母→黑鳞云母→铁锂云母”Nb含量降低的结果一致。为了对比,我们也对细粒二云母花岗岩围岩中的黑云母进行了微量元素分析,其云母铌含量很低,仅为n×10-6。所有云母的稀土元素含量较低,大多低于检测限,有些仅为n×10-6~10n×10-6

  • 表5 吴小垟矿床细粒黑云母花岗岩中云母主量元素含量(%)

  • Table5 Compositions (%) of major elements of mica from fine-grained biotite granite of the Wuxiaoyang deposit

  • 注: Ann—铁云母;Prl-1—一阶段黑鳞云母;Prl-2—二阶段黑鳞云母;Znw—铁锂云母;-表示低于检测限;T-site为硅氧四面体层中阳离子数;Y-site为八面体层中阳离子数;X-site为云母结构层中大阳离子数;Z-site为附加阴离子数;H2O*和LiO2*根据Tindle and Webb(1990)计算;Fe2+和Fe3+的原子根据林文蔚和彭丽君(1994)计算。

  • 表6 吴小垟矿区云母微量元素含量(×10-6

  • Table6 Compositions (×10-6) of trace elements of mica from the Wuxiaoyang deposit

  • 注: Ann—铁云母;Prl—黑鳞云母; Znw—铁锂云母。

  • 4.3 锆石、铌铁矿U-Pb定年

  • 细粒黑云母花岗岩中锆石阴极发光(CL)图像显示,锆石粒径在50~100 μm,蚀变严重,未见完整晶形,多数为他形粒状,曲晶石化严重,绝大部分颗粒在阴极发光(CL)图像上呈现出全黑。分析区域选择阴极发光中非全黑以及透射光中透明的锆石颗粒的核部,共测试32个锆石,选取落于谐和线附近且谐和率大于90%的11个锆石颗粒,其Th和U含量分别为1207×10-6~2173×10-6、2446×10-6~3604×10-6,Th/U=0.40~0.65(表7),均属于岩浆锆石,最终得到加权平均年龄为89.2±0.8 Ma(2SD;MSWD=0.4)(图13a~c),该年龄代表吴小垟细粒黑云母花岗岩的结晶年龄。

  • 细粒黑云母花岗岩中的铌铁矿背散射电子(BSE)图像显示,铌铁矿粒径在70~150 μm,多呈自形、板柱状,部分颗粒发育核边结构。分析区域选取均匀的、无孔洞的核部,共测试40个铌铁矿,最终选定17个落在谐和线附近且谐和率大于90%的矿物颗粒,其U、Th和Pb含量分别为65.0×10-6~682×10-6、2.72×10-6~235×10-6和0.96×10-6~10.9×10-6,U/Th比值介于3.16~72.72之间(表8),206Pb/238U年龄范围在82.1~89.4 Ma之间,得到铌铁矿U-Pb加权平均年龄为86.5±1.0 Ma(2SD;MSWD=0.94)(图13d~f),该年龄代表吴小垟细粒黑云母花岗岩的铌成矿年龄。

  • 曹门-张基花岗斑岩中锆石阴极发光(CL)图像显示,锆石颗粒明显不同于细粒黑云母花岗岩中的锆石,其粒径均大于100 μm,具明显的振荡韵律环带。分析区域选取均匀、无孔洞的核部,共测试32个锆石颗粒,最终选定16个落在谐和线附近且谐和度大于90%的锆石颗粒,其Th和U含量分别为136×10-6~906×10-6和151×10-6~701×10-6,Th/U = 0.61~2.73(表7),均属于岩浆锆石,最后得到锆石U-Pb加权平均年龄为97.5±0.4 Ma(2SD;MSWD = 0.6)(图13h~g),该年龄代表曹门-张基花岗斑岩的成岩年龄。

  • 表7 吴小垟矿区细粒黑云母花岗岩和花岗斑岩LA-ICP-MS锆石U-Pb定年分析结果

  • Table7 LA-ICP-MS zircon U-Pb dating of fine-grained biotite granite and granite porphyry in the Wuxiaoyang deposit

  • 表8 吴小垟矿区细粒黑云母花岗岩LA-ICP-MS铌铁矿U-Pb定年分析结果

  • Table8 LA-ICP-MS columbite U-Pb dating of fine-grained biotite granite in the Wuxiaoyang deposit

  • 图12 吴小垟矿床细粒黑云母花岗岩中云母的元素含量变化特征

  • Fig.12 Plots of variation characteristics of element content of micas from fine-grained biotite granite of the Wuxiaoyang deposit

  • 5 讨论

  • 5.1 吴小垟矿床成岩成矿年代学特征

  • 吴小垟矿床细粒黑云母花岗岩中锆石的U-Pb年龄为89.2±0.8 Ma,铌铁矿族矿物U-Pb年龄为86.5±1.0 Ma;铌铁矿族矿物U-Pb年龄为结晶年龄,同样代表吴小垟铌矿的成矿年龄;锆石U-Pb年龄为锆石的结晶年龄,代表细粒黑云母花岗岩的成岩年龄;考虑到分析的误差以及不同矿物定年方法的差异,吴小垟矿床的成岩成矿年龄基本一致,属晚白垩世。贯穿区域的曹门-张基花岗斑岩中锆石U-Pb年龄为97.5±0.4 Ma,花岗斑岩的成岩年龄要早于吴小垟矿床成岩成矿年龄,两者不是同期岩浆活动的产物。

  • 华南地区以发育大规模、多时代、多旋回花岗岩类和独特的中生代钨锡铍铌钽等大规模稀有金属成矿作用而闻名。华南地区的岩浆作用主要发生在加里东期、印支期和燕山期,华南花岗岩中最具经济意义的是燕山期造山运动形成的燕山期花岗岩(李晓峰等,2021)。华南地区燕山期岩浆活动主要分为以下3个阶段:180~152 Ma、130~120 Ma、107~87 Ma(Wang Yuejun et al.,2013),多金属矿化主要分为以下3个时期:170~150 Ma、140~126 Ma、110~80 Ma(Mao Jingwen et al.,2006),矿化作用与区域内岩浆事件密切相关。华南地区燕山期的Nb-Ta矿化同样受控于构造-岩浆事件,被划分为3期(Che Xudong et al.,2019):① 160~150 Ma,代表性矿床有湖南的尖峰岭矿床、赖子岭矿床和金竹垄矿床等(轩一撒等,2014毛禹杰等,2021);②~130 Ma,代表性矿床是江西灵山花岗岩体附近的松树岗矿床、黄山矿床(Che Xudong et al.,2015Xiang Yuanxin et al.,2017);③~90 Ma,目前已报道的有湖南的界牌岭矿床、上堡矿床,成矿年龄分别是91~89 Ma、86.83±0.8 Ma(Xie Lei et al.,2016Zhao Zhuang et al.,2021)。吴小垟铌矿床的成矿年龄为86.5±1.0 Ma,是华南地区最后一期的Nb-Ta成矿的产物。

  • 受古太平洋板块俯冲的影响,中生代中国东南部火山作用强烈,自晚侏罗世到白垩纪,东南沿海火山和构造活动被分为3个阶段:中—晚侏罗世(165~145 Ma)东南沿海由古太平洋俯冲挤压转变为俯冲后伸展,发育全区广泛分布的钨钼锡等多金属矿床和叶腊石等非金属矿床;白垩纪开始,伴随着华南进入古太平洋板块俯冲挤压后的伸展阶段,古太平洋板块的俯冲角度的变化,导致了大规模的岩石圈减薄,东南沿海地区发育大面积的火山-侵入活动,早白垩世(145~115 Ma)阶段发育浅成低温热液型金属、非金属和稀土矿产;晚白垩世(115~85 Ma)的火山活动和成矿作用是早白垩世的延续,伴生以浅成低温热液型为主的金属矿产、叶腊石和明矾石等非金属矿产(Mao Jingwen et al.,2013董长春等,2023)。中国东南沿海地区晚中生代形成的花岗质火山-侵入杂岩体与太平洋板块向中国东南大陆的俯冲消减、由此引发的玄武岩浆的底侵作用密切相关(王德滋等,2000)。吴小垟地区细粒黑云母花岗岩侵位及伴生的Nb-Ta矿化是在中国东南部地区岩石圈伸展、板块扩张裂解、火山岩浆活动频发的地球动力学背景下发生的。

  • 图13 吴小垟矿床中定年矿物颗粒照片及U-Pb年龄谐和图

  • Fig.13 Photographs and U-Pb concordia diagrams of dated mineral grains of the Wuxiaoyang deposit

  • (a~c)—细粒黑云母花岗岩中锆石的阴极发光(CL)图像、锆石LA-ICP-MS U-Pb谐和图、锆石加权平均U-Pb年龄图;(d~f)—花岗斑岩锆石的阴极发光(CL)图像、锆石LA-ICP-MS U-Pb谐和图、锆石加权平均U-Pb年龄图;(g~i)—细粒黑云母花岗岩中铌铁矿的背散射电子(BSE)图像、铌铁矿LA-ICP-MS U-Pb谐和图、铌铁矿加权平均U-Pb年龄图

  • (a~c)—cathodoluminescence(CL)images,U-Pb concordia diagrams determined by LA-ICP-MS,weighted average U-Pb age diagrams of zircon from fine-grained biotite granite; (d~f)—cathodoluminescence(CL)images,U-Pb concordia diagrams determined by LA-ICP-MS,weighted average U-Pb age diagrams of zircon from granite porphyry; (g~i)—back scattered electron (BSE) images,U-Pb concordia diagrams determined by LA-ICP-MS,weighted average U-Pb age diagrams of columbites from fine-grained biotite granite

  • 5.2 云母与铌成矿的关系

  • 云母是层状硅酸盐矿物,由于结构的特殊性,层间可以容纳其他离子或基团,碱金属稀有元素Rb和Cs可以替代K;在八面体位置上,Li、Nb、Ta、Sn等稀有金属元素可以部分替代Al、Fe、Mg。因此,云母是稀有金属重要的载体,成为稀有金属元素矿床中重要的指标矿物(王汝成等,2019)。

  • 云母的成分反映云母结晶时熔体或流体的成分,铁云母是极度富铁的,同时铁氧化物矿物沿着铁云母的解理发育(图10a),反映形成铁云母的体系环境是富铁的。云母的成分变化能够反映云母结晶过程中熔体或流体成分变化,岩浆演化、岩浆混合作用和热液交代作用都可能导致体系成分变化从而导致云母成分发生变化。吴小垟矿床中的含矿细粒黑云母花岗岩样品中存在不同阶段的云母,显示出明显岩浆-热液演化及流体活动的痕迹:早期云母为自形片状的铁云母,而晚期为非自形的黑鳞云母和铁锂云母,云母的成分呈Fe降低、Li和Al升高的变化。铁云母通常是自形的,分布在钠长石、钾长石和石英的间隙中,在背散射电子图像(BSE)中、成分均一未见分区(图10a、b,表5),因此认为其是岩浆期结晶的产物;而背散射电子图像下的黑鳞云母、铁锂云母的非自形晶形以及成分分析显示明显的成分不均一、铁锂云母常沿着黑鳞云母的裂隙或解理发育的现象(图10c、d,表5),显示其均为后期热液成因。

  • 云母在花岗岩铌钽成矿中发挥着重要作用(Stepanov et al.,2014);前人关于云母和花岗质熔体间Nb-Ta分配行为的实验表明,岩浆结晶的云母可以在一定条件下赋存一定量的Nb、Ta(Nash and Crecraft,1985Stepanov and Hermann,2013)。尤其是近些年来对天然样品的研究发现,黑云母也可以相当富铌。例如黄山岩体的中粒黑鳞云母花岗岩中黑鳞云母Nb平均含量可达884×10-6,而铁叶云母Nb平均含量更高,为1347 ×10-6Zhu Zeying et al.,2018),是超大型黄山铌矿床铌极端富集的体现。吴小垟矿床细粒黑云母花岗岩中岩浆结晶的原生铁云母Nb含量最高可达1253×10-6,其Nb含量已经接近黄山岩体铁云母中的Nb含量,铁云母中这么高的Nb含量,指示该细粒黑云母花岗岩有着非常好的铌找矿潜力。

  • 富铌黑云母常常存在于华南地区的花岗岩中,Yang Zhaoyu et al.(2023)罗列了富铌黑云母的Nb含量及Nb/Ta比值,如黄山花岗岩(Nb:1209×10-6,Nb/Ta:29)、苏州花岗岩(Nb:1426×10-6,Nb/Ta:17)、赵井沟花岗岩(Nb:805×10-6,Nb/Ta:31),这些铌钽矿床中的富铌黑云母具有高Nb/Ta比值的特征。图14为黄山铌矿床和吴小垟矿床中云母Nb-Ta的含量和比值,黄山岩体数据来源于Zhu Zeying et al.(2018),吴小垟矿床中的铁云母与黄山岩体中的云母相比具有相似高Nb含量和更高的Nb/Ta比值(Nb:1253×10-6,Nb/Ta:386),而黑鳞云母-铁锂云母与黄山岩体的云母相似(Nb:562×10-6~794×10-6,Nb/Ta:32~42)。因此,富铌、高Nb/Ta比值的黑云母可以作为一种新的找矿指示性矿物。黑云母是常见的造岩矿物,对其的研究成熟而完整,特征性黑云母若作为新兴的铌钽找矿指示性矿物,能对于未来的铌钽找矿勘查工作提供更简便的方法和新的方向。此外,吴小垟细粒黑云母花岗岩中从早期铁云母到晚期黑鳞云母-铁锂云母,Nb、Ta含量降低,与热液有关的云母其Nb、Ta含量会显著降低(王汝成等,2019)。Yang Zhaoyu et al.(2020)提出在岩浆期后热液作用中,黑云母产生的Nb、Ta可与Ca、Ti、Si、Fe、F结合形成钛铁矿、金红石、榍石等含铌矿物和Nb-Ta氧化物,Yang Zhaoyu et al.(2023)的高温高压实验复现了以上现象。花岗岩中的富铌云母经受热液蚀变淋滤出的铌,对于后期铌成矿具有重要意义(Zhu Zeying et al.,2018)。富铌黑云母可以为岩浆-热液作用下的铌钽成矿提供Nb、Ta(Zhu Zeying et al.,2018),在本区域,广泛发现富铌黑云母,可能为次生铌铁氧化物的形成提供了Nb。

  • 图14 吴小垟和黄山岩体云母的Ta-Nb图解

  • Fig.14 Ta-Nb diagram of the Huangshan and Wuxiaoyang micas

  • 5.3 岩浆过程和热液作用中铌的富集、迁移和成矿

  • 一般认为稀有金属元素富集的原因是岩浆结晶、花岗质熔体的高度演化和分异(Huang Xiaolong et al.,2002Teresa et al.,2017);高度结晶分异的花岗岩经历岩浆热液演化过程形成了含稀有金属花岗岩(Wu Fuyuan et al.,2017Yin Rong et al.,2019)。本次研究的成矿细粒黑云母花岗岩具有高硅、富碱和强过铝质的特征;微量元素在分异演化过程中较主量元素更加敏感(Bau,1997),对比矿区内的不成矿花岗岩,成矿细粒黑云母花岗岩显示更明显的Eu负异常(图5b)、更低的Zr/Hf和Nb/Ta比值(表1),成矿细粒黑云母花岗岩对比区域内未成矿花岗岩具有更高的演化程度,岩浆的高度演化对火成岩系统中稀有金属的富集至关重要。

  • 吴小垟矿床铌成矿受岩浆过程、热液作用等因素的制约,是一个复杂的过程。Nb、Ta具有很低的流体/熔体分配系数,因此更倾向保留在熔体中(Linnen and Cuney,2005)。随着岩浆的高度演化,逐渐结晶出自形的铌铁矿族矿物和含铌氧化物矿物。细粒黑云母花岗岩中原生铌铁矿呈自形柱状,粒径在100 μm以上,背散射图像显示不太明显的核边成分分带(图6a、b),是明显岩浆期结晶的产物;同样的,呈现明显的成分环带的被造岩矿物包裹的铌铁金红石(图9a、b)、自形的富铌铁云母(图10a、b),均呈现岩浆期结晶的特征。

  • 此外,热液作用也可能影响铌钽成矿(Li Jie et al.,2015),晚期富F、H2O热液流体对稀有金属成矿起改造作用。蚀变的铌铁矿呈他形粒状,粒径大约在10 μm左右(图6c、d),其晶形的变化表明铌铁矿经历了热液流体作用。铁云母到黑鳞云母、铁锂云母的过程中,热液流体作用同样显得至关重要(图10c、d),铅烧绿石常与铌铁矿共生在一起(图9e、f),展现出热液成因的特征。

  • 综上,吴小垟矿床存在两阶段的铌成矿:第一阶段铌成矿发生在岩浆期,结晶自形铌铁矿、原生富铌云母和铌铁金红石;而第二阶段铌成矿发生在岩浆期后,伴随着热液流体的活动,铌从富铌花岗质岩浆、原生含铌矿物中迁移出来富集形成次生含铌氧化物。

  • 6 结论

  • (1)吴小垟矿床成矿岩体为细粒黑云母花岗岩,其锆石U-Pb年龄为89.2±0.8 Ma,铌铁矿U-Pb年龄为86.5±1.0 Ma,均为晚白垩世,进一步完善和佐证华南地区存在晚白垩世岩浆作用、花岗岩的侵入和相关Nb-Ta成矿事件。

  • (2)吴小垟矿床存在两阶段稀有金属成矿:早阶段在岩浆期缓慢结晶出原生含铌矿物;晚阶段受岩浆期后热液作用,铌从富铌花岗质岩浆和原生含铌氧化物矿物迁移出,形成次生含铌氧化物矿物。

  • (3)黑云母极度富铌,在岩浆-热液演化过程中发生铁云母→黑鳞云母→铁锂云母的变化,该过程中黑云母Fe、Nb的含量降低,Al、Li、Mg、Si含量增高。虽然目前该矿已探明的储量有限,但原生黑云母极度富铌的特征,指示该矿区仍有很好的铌找矿潜力。

  • 致谢:衷心感谢两位匿名审稿专家和编委对本文质量的严格把关,为本文提出的建设性意见和建议!

  • 注释

  • ❶ 浙江省第十一地质大队.2019. 浙江省平阳县龙尾-瑞安市张基地区铍多金属矿普查报告(浙地基评[2019]5号).

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