Research status and prospect of the evolution mechanism of ore-forming fluids for carbonatite-hosted REE deposits
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摘要:
与碱性岩有关的碳酸岩型内生稀土矿床在中国乃至世界上轻稀土资源储量中占有极为重要的地位，诸如我国内蒙古的白云鄂博稀土矿床、川西冕宁—德昌稀土成矿带中的牦牛坪、大陆槽等稀土矿床、山东微山县郗山稀土矿床以及美国的Mountain Pass稀土矿床等都属于这种类型的稀土矿床。当前，对于这类稀土矿床的成矿流体演化机制，学界主要存在结晶分异作用、不混溶作用(熔体-熔体不混溶、熔体-流体不混溶以及流体-流体不混溶)以及热液交代蚀变作用之间的分歧。结晶分异作用可以使具有不相容性的稀土元素在残余熔体相中逐渐富集，直至形成稀土矿物。不混溶作用能够使稀土元素在不混溶后形成的两相或多相中的某一相中发生选择性富集，形成稀土矿化。成矿流体演化晚阶段的热液流体对早期生成的矿物或围岩进行交代蚀变，使其释放出能与稀土元素在热液中形成络合物的F-、(CO3)2-以及(SO4)2-等阴离子(团)，并最终在合适的构造控矿部位和外界环境条件下，重结晶或沉淀出稀土矿物。上述3种观点各有其理论依据，但是在解释一些碳酸岩型稀土矿床地质现象或实验地球化学模拟结果的时候都或多或少存在一定程度上的不足。前人的研究结果表明，碳酸岩型稀土矿床中发育了大量的熔体包裹体、熔体-流体包裹体以及富CO2的流体包裹体，以往在利用Linkam TS1400XY以及Linkam THMS600等这类常规高温热台，在101325 Pa条件下对其进行热力学测温时，这些包裹体大多在尚未达到完全均一状态前就已发生爆裂或泄露，极大制约了人们对这类稀土矿床在高温岩浆阶段和中高温岩浆-热液阶段成矿流体演化过程的认知。另外，对于稀土元素在成矿流体演化过程中的含量变化特征及其地球化学行为的研究，目前主要是通过包裹体成分组成的拉曼光谱分析，以及对矿体和围岩进行的全岩地球化学分析，尚缺乏单个包裹体中元素含量的原位微区分析方面的数据。未来，对碳酸岩型稀土矿床中发育的熔体包裹体、熔体-流体包裹体和富CO2的流体包裹体，利用热液金刚石压腔开展高温高压原位均一实验模拟研究，以及对单个包裹体中微量元素的含量利用LA-ICP-MS进行原位微区分析，将是揭示该类稀土矿床成矿流体演化机制的关键。
Abstract:Carbonatite-hosted endogenetic rare earth element (REE) deposits related to alkaline rocks are very important in light rare earth resources in China and even in the world. At present, controversies for the evolution mechanism of ore-forming fluids for carbonatite-hosted REE deposits are mainly among crystallization differentiation, liquid immiscibility (melt-melt, melt-fluid and fluid-fluid immiscibility) and hydrothermal metasomatic alteration. Crystallization differentiation can gradually enrich the incompatible REEs in the residual melt phase until the REE minerals are formed. Immiscibility can lead to selective enrichment of REEs in one of the two or multiple-phases formed after immiscibility, resulting in REE mineralization. The hydrothermal fluids formed in the late stage of ore-forming fluids evolutionary process have metasomatic reaction with the early-formed minerals or surrounding rocks and release anions (anion clusters) such as F-, (CO3)2- and (SO4)2-, which can form complexes with REEs in the hydrothermal aqueous solution, and finally recrystallize or precipitate REE minerals in appropriate ore-hosting structures under suitable external conditions. Each of the above three viewpoints has its own theoretical basis, but they are more or less inadequate in the explanation of some geological phenomena or experimental geochemical simulation results of carbonatite-hosted REE deposits. The previous study results shown that there are a large number of melt inclusions, melt-fluid inclusions and CO2-rich fluid inclusions in carbonatite-hosted REE deposits. In the past, most of these inclusions decrepitated or were leaked before reaching the total homogenization status when heated at 101325 Pa by using conventional high temperature heating stages, such as Linkam TS1400XY and Linkam THMS600, which greatly restrict our understanding of the evolutionary process of ore-forming fluids in high temperature magmatic stage and medium-high temperature magmatic-hydrothermal stage for this type of REE deposits. In addition, studies on the contents variation characteristics and geochemical behavior of REEs in the ore-forming fluid evolutionary process is mainly through the Raman spectroscopy analysis of the components of inclusions, as well as the whole rock geochemical analysis of ore bodies and surrounding rocks, and there is still a lack of in-situ microanalysis data about the element contents of individual inclusions. In the future, for melt inclusions, melt-fluid inclusions, and CO2-rich fluid inclusions that trapped in this type of deposits, in-situ high temperature and high pressure microthermometry experiments by employing hydrothermal diamond-anvil cell together with in-situ LA-ICP-MS microanalysis of trace elements contents in individual inclusions, are supposed crucial to reveal its evolution mechanism of ore-forming fluids.
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1. 研究目的（Objective）
松科二井，获取了从基底—火石岭组—沙河子组—营城组—登娄库组下部连续完整的原位岩心。本文对松科二井沙河子组上部的孢粉化石进行研究，为研究白垩纪地球温室气候和环境变化，建立服务“百年大庆”目标和基础地质研究的“金柱子”提供基础资料。
2. 研究方法（Methods）
孢粉样品采自松科二井3395.46~3901.35 m，岩性为黑色、灰黑色泥岩、粉砂质泥岩，层位为沙河子组上部。孢粉分析鉴定在吉林大学古生物学与地层学研究中心完成，具体过程为：每个样品取过筛的干样50 g，进行盐酸→氢氟酸→氢氧化钾→盐酸→硝酸→氢氧化钾→盐酸等分析处理，用筛选法将样品中的孢粉化石集中在试管中，制2个固定片在生物显微镜下鉴定。
3. 研究结果（Results）
依据松科二井3395.46~3901.35 m井段的孢粉化石演化特征，划分出两个孢粉组合。
（1）Leiotriletes sp.- Cyathidites australis - Chasmatosporites sp.组合（简称LCC组合），分布在3832.94~3901.35m井段。蕨类孢子占绝对优势，裸子类花粉较低，未见被子类花粉。蕨类孢子含量最高的是Cyathidites australis，其次是Leiotriletes sp.和Cyclogranisporites sp.，有时代意义的还有Cicatricosisporites exilis、C. minutaestriatus、C. splendidus、C.australiensis、Klukisporites sp.、Maculatisporites sp.、Triporoletes singularis、Trilobosporites tribotrys、Aequitriradites sp.和Polycingulatisporites reduncus等；裸子类花粉含量最高的是Chasmatosporites sp.，其次是Psophosphaera sp.，有时代意义的类型有Parvisaccites sp.、Erlianpollis minisculus、Paleoconifersp.、Pseudowalchia sp.和Classopollis sp.等。
（2）Klukisporites triangulus- Aequitriradites sp.- Pristinuspollenites sp.组合（简称KAP组合），分布在3395.46~3613.62 m井段。裸子类花粉百分含量（53.03%~72.13%）较高，其次为蕨类孢子（27.87% ~46.97%），未见到被子类花粉。裸子类花粉中含量最高的是Alisporites parvus，其次是Piceaepollenites sp.，含量较高的类型还有Chasmatosporites sp.、Pinuspollenites divulgatus和P. sp.等，有时代意义的还有Parvisaccites otagoensis、Erlianpollis minisculus、E. mediocris、Jiaohepollis sp.和Classopollis classoides等。蕨类孢子含量最高的是Klukisporites sp.，其次是Leiotriletes sp.和Cyathidites australis，含量较高的类型还有Cyclogranisporites sp.等，有时代意义的有Cicatricosisporites exilis、C.apiteretus、C. australiensis、Klukisporites triangulus、K.variegatus、Pilosisporites scitulus、Impardecispora sp.、Levisporites wulinensis、Triporoletes singularis、Trilobosporites humilis、Aequitriradites sp.和Schizaeoisporites sp.等。
含有早白垩世特有或在早白垩世繁盛的分子：Cicatricosisporites、Klukisporites、Pilosisporites、Maculatisporites、Impardecispora、Levisporites、Triporoletes、Trilobosporites、Aequitriradites、Schizaeoisporites、Polycingulatisporites、Parvisaccites、Paleoconiferus、Erlianpollis、Foveotriletes.和Classopollis等（图 1）。
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图 1 松科二井沙河子组部分孢粉化石（1-Cicatricosisporites exilis，样品号：SK2-375；2. -Cicatricosisporites minutaestriatus，标品号：SK2-385；3-Cicatricosisporites splendidus，标品号：SK2-385；4-Cicatricosisporites australiensis，样品号(sample number)：SK2-375；5-Levisporites wulinensis，样品号(sample number)：SK2-205；6. Aequitriradites sp.，样品号(sample number)：SK2-389; 7-Trilobosporites tribotrys，样品号(sample number)：SK2-389；8- Classopollis classoides，标品号：SK2-97；9-Erlianpollis minisculus，样品号(number)：SK2-395; 10. Parvisaccites sp.，样品号：SK2-395；11. Pilosisporites scitulus，标品号：SK2-201；12-Triporoletes asper，标品号(specimen number)：SK2-219；13. Foveotriletes subtriangulularis，样品号：SK2-219；14-Klukisporites triangulus，样品号(sample number)：SK2-205；15-Impardecispora sp.，样品号：SK2-201; 16-Schizaeoisporites polaris，样品号：SK2-173；17-Polycingulatisporites reduncus，标品号：SK2-395；18-Maculatisporites sp.，样品号：SK2-391。19-Chasmatosporites sp.，样品号：SK2-389; 20-Paleoconiferae sp.，样品号(sample number)：SK2-391;线段比例尺为10 μm, the scale of the line segment is 10 μm）Figure 1. Spores and pollen from the Lower Cretaceous Shahezi Formation in Well SK2上述2个孢粉组合分布在，属沙河子组上部，LCC组合蕨类孢子百分含量占绝对优势，裸子类花粉较少，从组合特点来看，可以与高瑞琪等人建立的沙河子组上部Granulatisporites-Lophotriletes-Cicatricosisporites组合大致对比，但上部的KAP组合层位显然高于高瑞琪等人建立的孢粉组合。与高瑞琪等人建立的孢粉组合相比，当前孢粉组合出现的有时代意义的孢粉类型更多且时代更新。
4. 结论（Conclusions）
两个孢粉组合海金砂科孢子繁盛，类型多样化，没有发现早期被子植物花粉；虽在蕨类孢子与裸子类花粉的百分含量及属种构成上明显不同，但出现的有时代意义的化石类型基本相同，其时代均为早白垩世早期。
5. 致谢（Acknowledgement）
本文为国家自然科学基金项目（41790451)和中国地质调查局项目（DD20190097）共同资助。孢粉化石由张淑琴研究员鉴定。
致谢: 本文在成文过程中得到了中国地质科学院矿产资源研究所李建康研究员的大力帮助; 两位审稿专家以及编辑对论文提出了宝贵的修改意见，在此一并表示衷心的感谢！ -
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图 1 上地幔橄榄岩低度部分熔融形成的初始岩浆在结晶分异作用下REE进行富集的模型(据Cullers and Medaris, 1977)
实心圆代表上地幔橄榄岩部分熔融产生的初始熔体中REE的含量；点虚线代表初始熔体中单斜辉石和石榴石以99∶1的比例结晶50% 后所产生的剩余熔体中的REE预测含量；虚线代表霓辉岩中的REE含量；实线代表霓辉质的初始熔体(磷灰石：榍石：单斜辉石：不透明矿物：霞石：黑云母=2.2∶3.8∶46.7∶5.5∶33.4∶8.4)结晶40%后，所产生的剩余熔体中的REE含量。通过以上几种结晶分异作用所产生的熔体中的REE含量均达不到碳酸岩中的REE含量
Figure 1. Fractional crystallization model for the enrichment of REE from low degree partial melting of peridotite in the upper mantle (after Cullers and Medaris, 1977)
Initial melt for the fractional crystallization model (solid circle); predicted melt after 50% crystallization of clinopyroxene∶garnet = 99∶ 1 from the initial melt (dot- dashed line); actual ijolite (dashed line). Forty percent fractional crystallization of the ijolite in the ratio of apatite∶sphene∶clinopyroxene∶opaques∶nepheline∶biotite = 2.2∶3.8∶ 46.7∶5.5∶33.4∶8.4 yields a REE content of the ijolite (solid line), and the REE content will never become similar to that of the carbonatite
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图 2 碱土、碱性元素在碳酸盐-硅酸盐不混溶熔体间的分配系数
Figure 2. Distribution coefficients of alkaline earth and alkaline elements in carbonate-silicate immiscible melts
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图 3 REE在共生的碳酸盐-硅酸盐两相中的分配系数
Figure 3. Distribution coefficients of REE elements between immiscible carbonate and silicate phases (after Veksler et al., 2012)
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图 4 Kalkfeld碳酸岩及其出溶盐流体中REE和其他微量元素的含量(据Bühn and Rankin, 1999)
Figure 4. REE and other trace elements in Kalkfeld carbonatite and the exsolution salt fluid (after Bühn and Rankin, 1999)
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图 5 牦牛坪REE矿床成矿流体演化P-T轨迹示意图(据Xie et al., 2009)
Ⅰ—熔体包裹体组合代表的碳酸岩阶段；Ⅱ—熔-流体包裹体组合代表的伟晶岩阶段；Ⅲ—富CO2流体包裹体组合代表的重晶石-氟碳铈矿阶段；Ⅳ—富水溶液流体包裹体组合代表的方解石阶段。图中阴影区根据实际包裹体测温数据绘制，阴影区之外的椭圆部分是根据含CO2流体包裹体、含CO2且含子矿物的流体包裹体以及熔体-流体包裹体的未均一测温结果而推测的其可能均一温度和压力范围
Figure 5. Schematic T-P path for evolution of the ore-forming fluid in the Maoniuping REE deposit (after Xie et al., 2009)
Ⅰ-Carbonatite stage, melt inclusion assemblage; Ⅱ-Pegmatite stage, melt- fluid inclusion assemblage; Ⅲ- Barite- bastnaesite stage, CO2- rich fluid inclusion assemblage; Ⅳ- Calcite stage, aqueous rich fluid inclusion assemblage. Shaded ellipse represents T-P range based on microthermometry data, unshaded ellipse shows estimated range based on unhomogenized inclusion data for aqueous- liquid CO2 fluid inclusions, aqueous daughter minerals-liquid CO2 fluid inclusions and melt-fluid inclusions
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图 6 深源岩浆在缓慢冷却和结晶过程中发生的两相碳酸盐-硅酸盐熔体不混溶以及多相碳酸盐-盐类熔体不混溶过程示意图(据Panina and Motorina, 2008修改)
Figure 6. Flow chart illustrating the mechanism of two-phase carbonate-silicate liquid immiscibility and polyphase carbonate-salt liquid immiscibility in deep-seated magmas during their slow cooling and crystallization in the Earth's crust (modified from Panina and Motorina, 2008)
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