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作者简介:

陈彪,男,1993年生。工程师,从事白云鄂博矿床地质研究工作。E-mail:chen_biao202301@163.com。

通讯作者:

杨占峰,男,1963年生。教授,从事白云鄂博矿资源综合利用研究工作。E-mail:yang_zhanfeng@163.com。

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目录contents

    摘要

    白云鄂博矿床为一特大型Fe-REE多金属矿床,同时伴生有巨量的钍资源。然而,目前开发利用的矿种主要是铁和稀土资源,钍资源利用率几乎为零。查明矿床中钍资源的赋存状态和分布规律及揭示钍资源的富集过程及机制是今后钍资源开发利用的重要基础。本文依托近些年的系统采样及分析测试成果,对白云鄂博主、东、西矿区570个样品进行了详细的矿物学观察和全岩化学分析,在不同类型矿石中识别出以硅钍石为主的独立含钍矿物,硅钍石除少量呈现被稀土矿物包裹现象外,通常以细脉状穿插于稀土矿物内部,显示其明显滞后富集的特点。矿区ThO2平均品位达0.0322%,高出地壳钍克拉克值(9.6×10-6)30多倍,各种矿石类型中ThO2含量具有明显的差别,在云母型、闪石型、霓石型和萤石型矿石中具有高含量ThO2,而白云石型矿石中ThO2含量较低,指示矿区钍矿化主要形成于碱性热液交代和萤石化阶段。此外矿区随深度增加钍矿化作用加强,显示出矿床具有良好的钍资源成矿潜力。

    Abstract

    Bayan Obo deposit is a large Fe-REE polymetallic deposit with large thorium resources. However, iron and rare earth resources are the main minerals developed and utilized at present, while thorium resources are almost used up. For the development and utilization of thorium resources in the future, it is important to find the occurrence state and distribution law of thorium resources in ore deposits and reveal the enrichment process and mechanism of thorium resources. In this paper, based on the results of systematic sampling, analysis and testing in recent years, detailed mineralogical observation and whole-rock chemical analysis were carried out on 570 samples from Baiyunebozhu, East and west mining areas. Independent thorium minerals, mainly silicorite, were identified in different types of ores. Silicorite, except a small amount of which were coated by rare earth minerals, is usually interspersed in rare earth minerals in the form of veins. It shows the characteristics of lag enrichment. The average grade of ThO2 in the mining area is 0.0322%, which is more than 30 times higher than the Clark value of the crust (9.6×10-6). There are obvious differences in ThO2 content among various ore types, and high ThO2 content is distributed in mica, amphibole, girine and fluorite ores. The low content of ThO2 in dolomite ore indicates that thorium mineralization is mainly formed in alkaline hydrothermal metasomatism and fluorination. In addition, thorium mineralization is enhanced with the increase of depth, which indicates that the deposit has good thorium ore-forming potential.

  • 钍(thorium)是一种放射性元素,在元素周期表中属锕系元素。钍与铀具有类似的元素性质,但其具有比铀放射性衰变期更短、更安全的天然优势,因此也被当作为一种潜在的核燃料。我国在钍基熔盐堆核能系统(TMSR)研究方面已取得显著成果,甘肃省武威市建造的钍基熔盐堆也标志着我国成为世界上第一个对第四代核电技术进行商业化试验运营的国家(苏更林等,2022)。钍元素通常以+4价存在于方钍石(ThO2)和硅钍石(ThSiO4)等独立钍矿物中,有时也以类质同象的形式赋存于铈族矿物(如独居石等)中(孟艳宁等,2013a)。世界上目前发现的含钍矿物通常以伴生形式存在于稀有及稀土矿床内,以单一含钍矿物组成的钍矿床相对较少。钍矿资源按赋矿围岩可分为岩浆型、变质型和沉积砂矿型三大类,又可细分为碳酸岩型、正长岩型、热液脉型、砂矿型等20余种矿床亚类(Barthel et al.,1992孟艳宁等,2013a陈金勇等,2022)。

  • 世界上重要的钍资源多与火成碳酸岩相伴生,占比达总资源量的40%,主要富存在富含稀土和铌的矿石中,一些矿山把钍作为副产品回收,如美国的蒙顿·帕斯(REE)和巴西的阿腊夏(Nb)(Barthel et al.,1992)。另一重要的钍矿床是热液脉状矿床(占总资源量的31%),根据矿床脉石不同可进一步划分为石英-碱性长石-氧化铁矿脉、重晶石-萤石矿脉、石英-重晶石矿脉、方解石矿脉、磷灰石-石英矿脉和与碳酸岩共生的碳酸盐矿脉等6个亚种,典型的如美国的勒姆希·帕斯矿床(石英-长石-氧化带矿脉)等,该类矿床中钍以独立矿物硅钍石、方钍石的形式出现或赋存于与稀土元素共生的矿物(独居石、氟碳铈矿、磷钇矿等)中,矿床围岩多发生钠(钾)长石化、萤石化和重晶石化等蚀变(Barthel et al.,1992; 仉宝聚等,2005; 张书成等,2005)。我国已查明的钍(ThO2)资源量为28.6万t,仅次于居世界第一位的印度(34.3万t),与世界钍资源类型占比基本一致(徐光宪,2005),其中赋存于岩浆热液型中的钍矿床是目前最为丰富的类型之一,如新疆阿勒泰伟晶岩型钍矿床、白云鄂博钍-稀土矿床和相山中低温火山热液型铀钍混合矿床等(孟艳宁等,2013a)。

  • 内蒙古白云鄂博矿床是全球最大的碳酸岩型Fe-REE多金属共(伴)生矿床,除此之外,矿床内还蕴藏了巨量的钍资源,钍资源量为22.1万t,占全国已探明总量的77.3%(徐光宪,2005)。然而,目前只开发利用了其中的铁与部分稀土,已开采矿石中丰富的钍资源随工艺流程主要进入了尾矿库、由铁精矿产生的高炉渣和由稀土精矿产生的废渣中,致使白云鄂博矿钍资源至今利用率几乎为零(苏文清等,2005; 赵长有,2006a2006b; 程建忠等,2007)。白云鄂博矿床钍资源在不同矿区中的分布有所差异,全岩钍含量变化范围较大(1×10-6~9040×10-6; 中国科学院地球化学研究所,1988; 赵长有,2006a)。但是,这些结论均是根据有限的样品测试结果得出的,缺乏系统性的样品采集及归纳总结。另一方面,目前的研究认为矿床中钍资源以两种形式存在:① 类质同象的形式赋存于独居石、氟碳铈矿等稀土矿物及易解石、铌铁矿等铌矿物中;② 钍石或方钍石等独立钍矿物(赵长有,2006a2006b; 罗明标等,2010; 刘正义等,2016; 侯晓志等,2018a2018b2022; Hou Xiaozhi et al.,2020; 杨莉等,2021)。尽管这些研究明确了矿床中钍的赋存形式,但钍矿化与铁、稀土和铌矿化之间的联系仍然缺乏直接的证据。本研究基于近五年在主、东、西矿区大量的样品采集工作,利用偏光显微镜、场发射扫描电镜-能谱仪等设备,查明了白云鄂博矿床不同矿石类型钍资源的空间分布规律及其与铁、稀土形成的先后序次,并初步探讨了钍资源的富集机制,为下一步白云鄂博钍资源的开发利用提供科学依据。

  • 1 地质背景

  • 白云鄂博矿区位于内蒙古北部,距包头市北约150 km,东西长18 km,南北宽2~3 km,总面积约48 km2,大地构造位置上位于华北克拉通北缘狼山-渣尔泰-白云鄂博-化德裂谷系内,紧邻中亚造山带(图1),区域内一级断裂为乌兰宝力格深大断裂(白云鄂博-赤峰深断裂),次级断裂白银角拉克-宽沟断裂对区域的地层展布、构造-岩浆活动和成矿作用起主导作用(郝梓国等,2002)。矿区主要出露新太古界—古元古界色尔腾山群结晶基底、中元古界白云鄂博群以及新生代沉积物等(图1a)。色尔腾山群基底杂岩主要为斜长片麻岩、石英岩类等,白云鄂博群底部石英岩、长石砂岩不整合于其上。白云鄂博群主要是由石英岩、板岩及碳酸盐岩等组成的一套海相浅变质岩系,通常可划分为6个岩组和18个岩段(H1~H18)(白鸽等,1996; Yang Kuifeng et al.,2011; Fan Hongrui et al.,2016)。其中,矿区内的白云鄂博群以都拉哈拉组(H1、H2)、尖山组(H3~H5)、哈拉霍疙特组(H6~H8)和比鲁特组(H9、H10)为主,目前的研究认为铁、稀土矿化与赋矿的H8白云岩关系最为紧密(中国科学院地球化学研究所,1988; Lai Xiaodong et al.,2013)。

  • 区内断裂构造发育,以近东西向产出的逆冲推覆构造为突出特征,导致矿区岩石地层单元走向上不连续。此外,矿区内存在多期次不同性质的叠加褶皱构造,最主要的为宽沟背斜,轴向近东西向,轴长大于8 km,向西倾伏,古元古界组成背斜核部,背斜两翼由中元古界白云鄂博群组成,白云鄂博矿床处于其南翼(图1a; 王凯怡等,2002; 柯昌辉等,2021)。矿区附近分布有大量的火成碳酸岩墙,侵位时代在1300 Ma左右,主要分布在矿区主、东矿北侧宽沟背斜轴部(杨奎锋等,2010),以岩脉状侵位于基底杂岩及白云鄂博群(图1a)。根据主要造岩矿物组成可将碳酸岩脉划分为白云石型、白云石-方解石共存型和方解石型3种类型,其与赋矿白云岩之间存在紧密联系,属于碳酸岩岩浆演化不同阶段的产物,其中白云石型和白云石-方解石共存型对应于早期碳酸岩岩浆阶段,而方解石型碳酸岩脉则是晚期热液阶段结晶分异的产物(王凯怡等,2002)。长期的分离结晶作用使晚期碳酸岩岩浆中强烈富集Sr、Ba、Th、Nb和LREE等不相容元素(杨奎锋等,2010),热液阶段也是白云鄂博稀土矿化的主要成矿时代。矿区南部和东部还出露有大量岩浆岩体,且岩性种类较多,主要岩性为黑云母花岗岩、钾长花岗岩、花岗闪长岩和辉长闪长岩等,以岩基或岩株状侵入中元古界白云鄂博群板岩和砂岩、菠萝头山白云岩及太古宙—古元古代基底杂岩中(图1a),锆石LA-ICP-MS U-Pb年龄显示其侵位时代在二叠纪—三叠纪,与稀土矿床成因没有直接联系(范宏瑞等,2009; Ling Mingxing et al.,2014)。

  • 白云鄂博矿床中矿体依据全铁品位(Fe>45%富矿,45%~30%中矿,<30%贫矿)而圈定,主要包括主矿、东矿、西矿、东部接触带和东介勒格勒等主要矿段(郝美珍等,2018)。主、东矿段内矿体呈巨大的透镜状、厚层状产出,矿体发生了强烈的氟-钠(钾)矿化交代作用,氟主要以萤石出现,钠交代主要表现为霓石化、钠闪石化和钠长石化,钾交代主要表现为黑云母和金云母化。西矿段由16个大小不等的矿体组成,矿体在地表呈不规则的透镜体状或长条状,而在下部则通过向斜轴部相连,矿体发生了有限的氟-钠交代作用(白鸽等,1996Lai Xiaodong et al.,2013Yang Xiaoyong et al.,2017)。矿区放射性异常的分布与矿体东西走向一致,具有放射性的矿物主要有钍石、独居石、氟碳铈矿、易解石和黄绿石等,钍除以独立矿物钍石产出外,还以类质同象和分散状态与稀土铌矿物共生,铀则主要集中在易解石和黄绿石中,同时放射性强度的分布有时同褐铁矿化有密切关系,往往褐铁矿化发育的部位出现放射性异常(赵长有,2006a)。钍矿化的划分与铁、稀土的划分基本相同,钍矿化矿石类型主要为块状型、白云石型、萤石型、云母型、闪石型和霓石型等6种主要类型(刘正义等,2016),其中以块状型、云母型钍矿石和闪石型钍含量为最高,其次为霓石型和萤石型,而白云石型含量最低,云母型Th含量平均达到了0.0574%(0.0182%~0.0896%),闪石型钍含量平均为0.0331%(0.0100%~0.0600%)(中国科学院地球化学研究所,1988)。

  • 图1 白云鄂博矿区地质简图(a)(据Yang Kuifeng et al.,2011修改)及样品分布图(b,c)

  • Fig.1 Regional geological map of Bayan Obo deposit (a) (modified after Yang Kuifeng et al., 2011) and sample locations (b, c)

  • 2 样品与分析测试

  • 本次研究采用了主、东、西矿区采场境界范围内不同开采台阶的570个样品(图1b、 c),包含了白云石型、萤石型、云母型、闪石型和霓石型5种钍矿化矿石类型。其中钍矿化较好的云母型钍矿石主要产于西矿上部,在主、东矿上盘个别地段零星分布,矿石呈黑色块状构造,云母呈鳞片状分布,薄弱面处可见闪石石棉化现象,主要矿物为磁铁矿、黄铁矿、钍石及黑云母、钠闪石、萤石、白云石等脉石矿物(图2a~c);闪石型钍矿石主要分布于东矿上盘和西矿,主矿上盘有少量分布,且在西矿多分布于靠近黑云母化板岩地段,矿石呈灰黑色、墨绿色块状构造,主要矿物为磁铁矿、黄铁矿、独居石、氟碳铈矿、钍石及钠闪石、白云石、黑云母等脉石矿物(图2d~f)。

  • 样品测试在白云鄂博稀土资源研究与综合利用全国重点实验室完成。首先将采集样品进行详细岩性描述拍照后制成光薄片,剩下的矿样经颚式破碎机和盘式磨样机粗碎、细碎,磨成200目的粉末样品进行化学分析测试。利用偏光显微镜(ZEISS Axio Scope.A1 POL)重点对云母型和闪石型钍矿石光薄片进行详细观察,识别矿石的矿物组成及结构特征,挑选具有典型特征的光薄片表面喷镀铂金后应用能谱-扫描电镜法(EDS-SEM)进行点分析(EDS-point)、面分析(EDS-mapping),并结合背散射电子(BSE)图像确定主要矿物形貌特征和成分信息。场发射扫描电镜为德国(ZEISS)公司生产的Sigma-500型,能谱型号为(BRUKER XFlash 6160),工作条件为加速电压20 kV,分别率0.8 nm,工作距离8.5 mm,放大倍数50~100000,能量分辨率为20000 cps。钍(ThO2)含量利用电感耦合等离子体质谱仪(ICP-MS)测定,稀土(REO)含量利用电感耦合等离子体质谱仪(ICP-MS)和电感耦合等离子体发射光谱仪(ICP-AES)两种仪器共同测定,ICP-MS 型号为美国PE公司NEXion 300 Q,ICP-AES型号为安捷伦公司5110 VDV,TFe用重铬酸钾氧化还原滴定法测定(郝冬梅等,2003; 杜梅等,2014; 周凯红等,2022)。

  • 图2 白云鄂博矿床不同类型矿石手标本和镜下特征

  • Fig.2 Hand specimens and microscopic characteristics of different types ore in Bayan Obo deposit

  • (a,b,c)—云母型矿石;(d,e,f)—闪石型矿石;Mag—磁铁矿;REO—稀土矿物;Bas—氟碳铈矿;Dol—白云石;Cal—方解石;Rbk—钠闪石;Bt—黑云母;Fl—萤石;Sp—闪锌矿;Thr—钍石

  • (a, b, c) —mica-type ores; (d, e, f) —riebeckite-type ores; Mag—magnetite; REO—monazite; Bas—bastnaesite; Dol—dolomite; Cal—calcite; Rbk—riebeckite; Bt—biotite; Fl—fluorite; Sp—sphalerite; Thr—thorite

  • 3 分析结果

  • 3.1 独立钍矿物的岩相学特征

  • 通过大量的岩相学观察,本次研究在不同类型矿石中均发现了独立钍矿物,EDS分析结果表明这些钍矿物均为硅钍石(ThSiO4)。硅钍石在薄片中呈棕红色—棕褐色,多呈浑圆状和他形粒状,以星散状、浸染状、团簇状和细脉状产出,且在云母型、闪石型和萤石型矿石中含量居多。硅钍石多呈独立矿物赋存于云母、方解石和钠闪石等脉石矿物中(图3a~c),或与稀土矿物独居石、氟碳钙铈矿、氟碳铈矿等共(伴)生(图3d~f);硅钍石与稀土矿物独居石、氟碳钙铈矿、氟碳铈矿共(伴)生关系呈现多样性,赋存状态主要表现为:① 位于稀土矿物与其他矿物晶间(图3g、h);② 被独居石、氟碳钙铈矿、氟碳铈矿包裹(图3i、j);③ 呈细脉状穿插于独居石、氟碳铈矿晶体内(图3k、l);④ 部分浑圆状独居石、氟碳铈矿颗粒被硅钍石包裹(图3m、n),显示硅钍石的形成时代较稀土矿物成矿时代更为宽泛。此外,一些半自形—他形方铅矿颗粒呈细脉状充填于硅钍石粒间或呈“乳滴状”被钍矿物包裹(图3n、o),表明部分硅钍石的沉淀可能近同时或晚于方铅矿的形成。由于钍矿物具有放射性的特点,部分硅钍石显示非均质性现象(图3h)。

  • 此外,所有钍元素都显示出+4价,Th4+离子半径(1.02×10-10 m)与Ca2+(0.99×10-10 m)、REE3+(1.03×10-10 m)的离子半径很接近,容易被含钙矿物和+3价稀土元素矿物捕获发生类质同象置换,进入矿物晶格中(陈金勇等,2022),以类质同象形式赋存于独居石(图4a、b)、氟碳钙铈矿、氟碳铈矿(图4c、d)等稀土矿物、易解石(图4e、f)、褐钇铌矿等铌矿物和含铈硅酸盐矿物磷硅钙铈矿中(杨莉等,2021),且各矿物中钍含量关系为磷硅钙铈矿>褐钇铌矿>易解石>独居石>氟碳钙铈矿>氟碳铈矿(图5)。前人通过实验模拟等研究表明Th与独居石可通过以下任一方式结合(Stepanov et al.,2012):

  • CePO4+ThO2+SiO2 (Ce, Th) PO4, SiO22CePO4+ThO2+CaOThCaPO42+Ce2O3

  • 同时流体中Ca、Si和P的活性往往影响独居石中ThO2的含量(Stepanov et al.,2012)。能谱半定量测量结果显示部分云母型矿石中稀土矿物独居石钍含量高达6%,远高于矿区独居石中钍的平均含量(0.09%~0.46%,平均为0.26%)。

  • 3.2 不同类型矿石全岩地球化学组成

  • 主、东、西矿区570个岩石样品全铁(TFe)、稀土氧化物(REO)和氧化钍(ThO2)化学分析结果见表1。

  • 表1 白云鄂博矿床铁、稀土、钍品位表(%)

  • Table1 Grade (%) of iron, rare earth and thorium of Bayan Obo deposit

  • 注:TFe =Fe3++Fe2+

  • 主矿207个矿石样品全铁(TFe)平均含量为13.49%,稀土氧化物(REO)含量为3.70%,氧化钍(ThO2)含量为0.0350%(0.0001%~0.2276%);东矿128个矿石样品TFe含量为13.81%,REO含量为3.31%,ThO2含量为0.0329%(0.0003%~0.1934%);西矿235个矿石样品TFe含量为13.54%,REO含量为1.49%,ThO2含量为0.0277%(0.0002%~0.14%)。其中主矿和西矿云母型矿石具有高于矿区其他矿石类型的铁含量,东矿闪石型矿石TFe含量最高。对于REO而言,主矿REO含量最高,为西矿的2.5倍左右。云母型矿石是整个矿区各矿石类型中REO含量最低的,REO含量较高的矿石类型主要为霓石型和萤石型矿石,这也充分证实稀土的成矿聚集与矿区霓石化和萤石化具有密切的关系(Liu Shang et al.,2018a2018b)。

  • 矿区ThO2平均品位为0.0322%,高出地壳钍克拉克值(9.6×10-6)30多倍,含量箱线图表明(图6):主矿和西矿同类型矿石ThO2含量分布有很大的相似性,云母型矿石ThO2品位要高于同矿区其他矿石类型,平均为0.0485%和0.0453%,是地壳钍克拉克值近50倍,但数据波动性较大,标准差为0.05 左右;白云石型矿石ThO2含量最低,平均为0.0144%和0.0186%,但也高出地壳钍克拉克值近15倍;闪石型、萤石型和霓石型矿石ThO2含量居中。而东矿各矿石类型中ThO2含量与主、西矿分布规律有一定差异,云母型矿石ThO2含量最低,为0.0112%,但数据离散程度小,标准差为0.01;霓石型矿石ThO2含量最高,为0.0567%,高出地壳钍克拉克值(9.6×10-6)近60倍,也是本次研究中平均含量最高的矿石类型,但其含量分布较东矿其他矿石类型波动性大;萤石型、闪石型和白云石型矿石ThO2含量居中。纵观整个矿区的矿石类型,可以发现钍(ThO2)主要还是集中分布在硅酸盐类矿石(云母型、霓石型、闪石型)或萤石型矿石中,而白云石型矿石中含量较低。同时不管是云母型矿石,还是霓石型矿石,其虽具有较高含量的ThO2,但数据波动性也较大,说明含钍矿物在矿石中的分布也并不均一。

  • 图3 白云鄂博矿床钍矿物偏光显微镜和背散射图像

  • Fig.3 Polarizing microscope and backscattered scanning electron microscope images of thorium minerals in Bayan Obo deposit

  • (a)—云母型矿石中赋存于云母中的钍石;(b)—云母型矿石中赋存于云母和方解石中的钍石;(c)—闪石型矿石中赋存于方解石中的钍石;(d)、(e)—云母型矿石中赋存于独居石粒间和边缘的钍石,部分呈条带状分布;(f)—闪石型矿石中赋存于氟碳钙铈矿、氟碳铈矿和白云石粒间的钍石;(g)—云母型矿石中独居石粒间钍石;(h)—闪石型矿石中氟碳铈矿边缘钍石;(i)—霓石型矿石中氟碳钙铈矿包裹钍石;(j)—云母型矿石中独居石包裹钍石;(k)—云母型矿石中细脉状钍矿物穿插独居石;(l)—闪石型矿石中细脉状钍矿物穿插氟碳铈矿;(m)—云母型矿石中钍石包裹独居石;(n)—云母型矿石中钍石包裹氟碳铈矿,钍石边缘生长有方铅矿;(o)—云母型矿石中钍石包裹“乳滴状”方铅矿;Mag—磁铁矿;Mnz—独居石;Bas—氟碳铈矿;Par—氟碳钙铈矿;Dol—白云石;Cal—方解石;Thr—钍石;Rbk—钠闪石;Bt—黑云母;Gn—方铅矿

  • (a) —thorite occurring in mica of mica-type ores; (b) —thorite occurring in mica and calcite of mica-type ores; (c) —thorite occurring in calcite of riebeckite-type ores; (d) , (e) —thorite occurring between and along the edges of monazite grains, partly banded in mica-type ores; (f) —thorite occurring between parisite, bastnaesite and dolomite grains in riebeckite-type ores; (g) —thorite between grains of monazite in mica-type ores; (h) —thorite at the edge of bastnaesite in riebeckite-type ores; (i) —thorite encased in parasite of aegirine-type ore; (j) —thorite encased in monazite of mica-type ores; (k) —veined thorium intersperse monazite in mica-type ores; (l) —veined thorium intersperse bastnaesite in riebeckite-type ores; (m) —monazite encased in thorite of mica-type ores; (n) —bastnaesite encased in thorite and galena grows on the edge of thorite of mica-type ores; (o) —thoriite envelops galena in “milky drops” of mica-type ores; Mag—magnetite; Mnz—monazite; Bas—bastnaesite; Par—parisite; Dol—dolomite; Cal—calcite; Thr—thorite; Rbk—riebeckite; Bt—biotite; Gn—galena

  • 图4 白云鄂博矿床独居石、氟碳铈矿和易解石的背散射图像和Th元素分布图

  • Fig.4 Backscattered scanning electron microscope images of monazite, bastenite and aeschynite in Bayan Obo deposit

  • (a)—云母型矿石中的独居石和钍石矿物;(b)—(a)视域Th元素分布图;(c)—霓石型矿石中氟碳钙铈矿、氟碳铈矿和钍石;(d)—(b)视域Th元素分布图;(e)—霓石型矿石中易解石和氟碳钙铈矿;(f)—(e)视域Th元素分布图;Mnz—独居石;Bas—氟碳铈矿;Par—氟碳钙铈矿;Aeg—霓石;Aes—易解石;Thr—钍石;Bt—黑云母

  • (a) —monazite and thorite in mica-type ores; (b) —Th element distribution map in the (a) horizon; (c) —parisite, bastnaesite and thorite in aegirine-type ores; (d) —Th element distribution map in the (b) horizon; (e) —aeschynite and parasite in aegirine-type ores; (f) —Th element distribution map in the (e) horizon; Mnz—monazite; Bas—bastnaesite; Par—parisite; Aeg—aegirine; Aes—aeschynite; Thr—thorite; Bt—biotite

  • 4 讨论

  • 4.1 钍与稀土、铁相关关系

  • 白云鄂博矿作为铁-稀土-铌-钍等多金属共(伴)生矿床,其各元素、各矿种的相关性一直受到研究者的关注,前人也进行了大量的研究(章雨旭等,2009; Hou Xiaozhi et al.,2020)。本次矿区570个矿样化验分析数据皮尔逊相关系数(r)(余建英等,2003)表明(表2),矿区各类型矿石中TFe和REO相关系数除主、东矿云母型外,其余都表现为弱相关(|r|<0.3),TFe和REO表现了明显的解耦现象,白云鄂博矿区铁和稀土这种分离富集的倾向可能是其元素性质的差异导致了它们在运移、富集、沉淀过程的分异。章雨旭等(2009)研究显示REE与Th关系密切,可能发生了同步富集,且钍较多赋存于贫铁矿石中。本次测试结果中ThO2和REO相关分析除东矿云母型表现为中度相关外,其余大多数表现为弱相关或低度相关,稀土含量高的矿石钍含量不一定高(Hou Xiaozhi et al.,2020)。相比而言,ThO2和TFe相关系数更好,多数具有中度相关性,可能暗示了二者经历了相似的迁移、富集过程,尤其是西矿云母型和闪石型表现出较好的中度相关性,且Hou Xiaozhi et al.(2020)也发现在云母型和闪石型矿石中ThO2和TFe具有很好的正相关性,ThO2在铁矿物中的分布比例较高,而REO含量很低,所以在选铁过程中遇到的Fe和Th难分离问题可能是白云鄂博矿床的成因影响。此外,纵观整个矿区白云石型、萤石型、云母型、闪石型和霓石型铌稀土铁矿石来看,云母型铌稀土铁矿石中TFe-REO-ThO2三者相关系数要好于其他4种类型,矿区的钾交代蚀变可能促进了不同元素的相似富集成矿。

  • 表2 白云鄂博矿床不同矿石类型TFe、REO和ThO2 相关系数分析表

  • Table2 Correlation coefficients of TFe, REO and ThO2 for different ore types in Bayan Obo deposit

  • 注:0.8≤|r|表示高度相关,0.5≤|r|<0.8表示中度相关,0.3≤|r|<0.5表示低度相关,|r|<0.3表示弱相关或基本不相关。

  • 图5 白云鄂博矿床部分矿物钍含量EDS点分析测试结果

  • Fig.5 EDS point analysis and test results of some minerals in Bayan Obo deposit

  • 图6 白云鄂博矿床不同矿石类型ThO2含量分布箱线图

  • Fig.6 Distribution characteristics of ThO2 content of different ore types in Bayan Obo deposit

  • 4.2 钍富集作用及其成矿机制探讨

  • 碱性岩岩浆-热液系统蕴藏着广泛的矿床,这些类型的矿床多是在岩浆阶段后期经历蚀变、交代和热液填充作用等形成(Deng Jun et al.,2018Qiu Kunfeng et al.,2021),大量的地球化学实验表明岩浆演化程度与成矿作用密切相关,演化程度高的岩浆在成矿元素的迁移和初步富集中起着重要作用,岩浆后阶段的流体通常含有高含量的挥发性成分和高浓度的成矿元素(Lichtervelde et al.,2010Deng Jun et al.,20162021)。钍在岩浆作用阶段是一种强不相容元素,由于其在熔浆中的质量分数及分配系数(<1)较低,因此不易进入到早期结晶的矿物相中,而通常富集于残余熔浆或热液中;随着岩浆的演化,残余熔体或热液中的钍元素含量不断增加,最终形成大量的钍石、独居石等含钍矿物(仉宝聚等,2005; Huang Yaqi et al.,2022)。在岩浆后期的高温热液阶段钍主要呈胶体形式(如钍石ThSiO2)搬运或以络合物的形式迁移,如氟络合物((ThF)3+,(ThF22+,﹝Th(F,Cl)n-(2n-4))和碳酸盐络合物(﹝Th(CO3n-(2n-4))(张书成等,2005)。富含稀土H2O-CO2-Cl-F的富碱碳酸岩流体具有黏度低、迁移性高的特点,在高温条件下具有较强的搬运不相容元素的能力(仉宝聚等,2005; 张书成等,2005; 陈金勇等,2022),目前发现的世界上富碱碳酸岩常常富含钍石、方钍石等含钍矿物,流体中钍的质量分数最高可达到1600×10-6陈金勇等,2022)。本次测试结果显示白云鄂博矿区白云石型矿石相比较其他4种矿石类型钍含量最低,但也达到了184×10-6,5种矿石中钍平均含量达260×10-6,最高为2600×10-6,也充分证实碳酸岩流体中富集有大量的REE、Th等不相容元素,为含钍矿物的沉淀提供了物质来源。

  • 白云鄂博矿床中铁、稀土及铌资源都不同程度经历了漫长的富集过程。在1.3 Ga左右,白云鄂博地区发生了强烈碳酸岩岩浆作用,形成H8白云岩和区内广泛发育的碳酸岩墙。富H2O-CO2-NaCl(F-REE)碳酸岩熔体经历了岩浆—岩浆热液—热液等3个阶段,在晚期的热液阶段,碳酸岩岩浆分异出的富水、富碱、富氟热液上涌,发生强烈碱性蚀变和萤石化作用(Yang Xiaoyong et al.,2017; Liu Shang et al.,2018a2018b; She Haidong et al.,2021),后续一直持续到晚古生代经历了多期大规模的热液交代蚀变演化作用(Li Xiaochun et al.,2021; 邓淼等,2022)。强烈的蚀变演化促进矿区REE、Fe等元素迁移—沉淀,形成独居石、氟碳铈矿等主要稀土矿物(Song Wenlei et al.,2018),磁铁矿等铁矿物,萤石、霓石、钠闪石、黑云母等脉石矿物(肖荣阁等,2012)和一些细脉状硫化物(She Haidong et al.,2021)。其中热液中REE的运移—沉淀主要受高含量的F-控制,而铁以Fe-Cl络合物形式迁移,Cl和Na、K一样在流体的最后阶段依然活跃,从而铁主要沉淀在霓石、闪石和云母等为主的矿石中(Tian Pengfei et al.,2021)。

  • 矿区全岩分析显示钍矿化矿石类型多样,具有明显的不均一性,不同矿石的矿物含量具有显著差异。硅酸盐型(霓石、闪石和云母型)矿石钍矿化作用强烈,富含大量的含钍矿物,萤石型居中,而白云石型矿石钍元素积累量很低,所以白云鄂博矿区钍的成矿富集同典型岩浆热液型钍矿床一样,钍矿化受制于强烈的钾钠交代和萤石化作用(Barthel et al.,1992孟艳宁等,2013b)。白云鄂博赋矿白云岩的母岩浆是富含F、Cl、P挥发分以及REE、Na、K、Th和Fe这些元素的(王凯怡等,2018),在矿区强烈的钠钾交代过程中,围岩中大量的硅也被带入到溶液中。由于Th4+可以与Cl-形成络合物ThCl3+张书成等,2005),在交代过程中大量的挥发分Cl依然很活跃,可以携带Fe、Th4+等迁移更远的距离,持续向压力更低的上部移动,由于碱度的降低,流体中的Fe-Cl、ThCl+3络合物溶解度会降低和分解(王凯怡等,2018),大量的铁氧化物和硅酸盐钍矿物(ThSiO4)沉淀出来,所以矿区的钍也主要沉淀在最晚形成的碱交代矿石中,表现出和铁类似的迁移规律,这也正好可以解释矿石中TFe-ThO2的良好相关性。此外,云母型矿石中显示出异常的钍和铁富集现象,大量自形—半自形磁铁矿和呈细脉状、浸染状的独立硅钍石嵌布于黑云母、金云母、方解石矿物粒间或边部(图3a、b),表现为典型的热液成因的矿物学特征,同时稀土矿物独居石中的Th含量也要远远高于矿区的平均值,充分说明矿区的钾交代作用可能对钍和铁的富集起到更积极的作用。BSE图像还观察到部分硅钍石与方铅矿、黄铁矿、雌黄铁矿等硫化物共生,揭示还原环境可能有利于钍矿物的沉淀富集(孟艳宁等,2013b)。

  • 通过对稀土矿物独居石和氟碳铈矿的Sm-Nd和原位Th-Pb定年,以及霓石和钠闪石等蚀变矿物的Ar-Ar测年工作,目前的研究揭示出矿床中稀土的成矿作用主要发生在中元古代(~1.3 Ga)和晚古生代(~440 Ma)两个时期,早期形成的稀土矿物多数受到了后期热液流体的改造作用(Zhu Xiangkun et al.,2015; Li Xiaochun et al.,2021)。Huang Xiaowei et al.(2015) 在矿床中识别出了两类磁铁矿,两类磁铁矿具有明显不同的稀土含量,并进一步提出两期的稀土矿化可能同时伴随了铁的富集成矿作用。白云鄂博矿床中铌矿物的富集与稀土的晚期成矿作用可能具有一定的时间关联(~430 Ma),或与更晚期的海西期花岗岩体侵入有关,只有少量铌矿物沉淀于中元古代(Liu Shang et al.,2020)。以上前人的研究表明矿床中的铁、稀土、铌矿化具有较为一致的时间演化历史。矿区不同矿石类型中钍矿物BSE图像显示钍矿物共(伴)生关系复杂多样,早期形成的稀土矿物多被钍矿物细脉穿插,或呈交代残余体赋存于钍矿物内部,同时也有部分钍矿物被独居石、氟碳铈矿等包裹,这些矿物学特征表明矿床中少量钍矿物形成时代要早于稀土矿物,而大量钍的富集作用要滞后于稀土成矿作用。另一方面,矿床中金属硫化物的形成通常认为晚于铁、稀土的成矿作用,主要形成于古生代热液期(Smith et al.,2015),本次研究识别出方铅矿呈包裹体赋存于钍石内部,这也说明了矿区钍的富集作用要晚于矿床中大规模的铁-稀土矿化时代。

  • 综合可知,白云鄂博矿床中碳酸岩流体为含钍矿物的沉淀奠定了物质基础,结晶分异形成少量钍矿物,而后期多期次的热液交代如K-Na化、萤石化和硫化物化等促使成矿物质进一步活化—迁移—富集—再沉淀,其中钾交代可能扮演了更重要的角色。同时,矿区钍矿化作用并非一期完成,而是经历了较长矿化阶段以及多期次矿化作用。结合本次研究工作,在前人对矿物学、岩石学和年代学等全面细致基础工作上(Smith et al.,2015She Haidong et al.,2021),确立了矿区主要矿物演化序列(图7)。

  • 4.3 钍的空间分布及资源勘查前景

  • 通过大量的全岩分析可知,矿区的钍主要分布在云母型和闪石型矿石中,在水平上分布并不均匀,主要集中在云母型和闪石型矿带,而在纵深方向上,从不同台阶的钍含量趋势图(图8)可以看出,主、东、西矿体钍品位随矿体深度加深钍矿化有加强的趋势,尤其西矿体更加明显。

  • 白云鄂博矿经过几十年的露天开采,主矿和东矿已接近设计开采深度,近年来包钢集团对主、东矿体深部开展了多次钻探验证,完成多个大于1000 m的深孔,均显示良好铁矿层,钻孔ZK-15-3-1和ZK15-3-2矿体厚度超过100 m,主矿14线和东矿15线、15-03线深部的矿体均变厚,且14线向东、15线向西,矿体均未封闭(李以科等,2022),未见随深度而发生矿化减弱或尖灭的趋势,找矿效果显著。东矿最深孔WK20-02(1775.4 m)钻孔柱状图显示在矿体深部依然存在磁铁矿和独居石、氟碳铈矿、氟碳钙铈矿等稀土矿物,化验分析数据显示1000 m深度后TFe、REO品位仍然很高,部分TFe总量达到40%,REO达10%以上(图9)(Tang Haiyan et al.,2021),东矿深部铁、稀土、铌、钍等元素含量平均品位分别达27.45%、5.49%、0.11%、0.035%,明显高于矿石边界品位(侯晓志等,2022),重力-航磁-电法等地球物理勘探也证实主矿和东矿深部及其两侧具有巨大的资源前景(范宏瑞等,2022; 李以科等,2022)。

  • 图7 白云鄂博矿床主要矿物生成序列

  • Fig.7 Main mineral formation sequence of Bayan Obo deposit

  • 本次研究显示各矿体深部依然存在品位ThO2>0.10%的矿石(图8),充分证明矿体深部钍资源同铁、稀土一样,仍然具有较大的成矿潜力。此外,从元素成矿相关性及蚀变岩性角度来看,受到Na、K、F、S等交代后的碱性蚀变、萤石化和硫化物化等蚀变作用区带存在巨大的找矿潜力。

  • 图8 白云鄂博矿区钍(ThO2)含量变化趋势图

  • Fig.8 Trend of thorium (ThO2) content in Bayan Obo deposit

  • 图9 白云鄂博东矿勘探线剖面图(a)和东矿WK20-02钻孔1000 m以下TFe和REO含量变化趋势图(b)(据Tang Haiyan et al.,2021修改)

  • Fig.9 Profile of exploration line (a) and trend of TFe and REO content below 1000 m in borehole WK20-02 (b) in east Bayan Obo deposit (modified after Tang Haiyan et al., 2021)

  • 5 结论

  • (1)白云鄂博矿床各类型矿石中都不同程度赋存有以硅钍石为主的独立钍矿物,部分钍以类质同象的形式存在于独居石、氟碳铈矿、氟碳钙铈矿等稀土矿物和易解石、褐钇铌矿等铌矿物中,与稀土矿物、晚期硫化物共生关系复杂,表现出成矿多期性的特征。从矿石类型上来看,钍主要集中在硅酸盐类(云母型、霓石型、闪石型)和萤石型矿石中,而白云石型矿石中含量较低,稀土含量高的矿石中钍含量不一定高,此外,在云母型和闪石型矿石中ThO2与TFe显示出良好的正相关性。

  • (2)白云鄂博Fe-REE-Th矿床初始成矿物质来源于~1.3 Ga的火成碳酸岩岩浆,后期多期次的钾钠化-萤石化-硫化物化等热液蚀变使初始碳酸岩经历改造,成矿物质Th发生进一步活化、迁移、富集和再沉淀,演化形成现今钍矿化现象。

  • (3)白云鄂博矿体中的钍在水平上分布并不均匀,主要集中在云母型和闪石型矿带,而各矿体钍含量随深度加深存在钍矿化加强的趋势,矿体深部具有良好的钍资源开发潜力,后续需对钍矿化进行勘查和圈定,实现矿区钍资源的综合开发利用。

  • 致谢:谨以此文庆祝包头稀土研究院60周年华诞!衷心祝愿稀土院在未来的征程中再创佳绩!祝愿白云鄂博矿在新一轮的找矿行动中再创辉煌!样品采集过程中得到了包钢集团首席专家赵永岗、包头稀土研究院刘建军副院长、刘国卿工程师、梁小龙工程师、白云铁矿刘峰总工、郭宾工程师和巴润矿业公司崔凤总工等专家的大力帮助与支持,分析测试工作得到了包头稀土研究院王振江高工的帮助,在此深表感谢!

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