相山矿田西部铀钍矿床的成矿机理研究
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摘要
本论文以“全国钍资源调查与评价”项目为依托，以相山矿田西部火山热液型铀钍混合矿床—居隆庵、李家岭及邹家山矿床为研究对象，在总结、归纳大量国内外研究成果的基础上，对相山矿田西部的铀钍混合矿床进行蚀变岩石学、铀、钍矿物学、岩石化学、地球化学、流体包裹体、同位素及年代学进行系统研究，从而查明与钍矿化相关的蚀变特征，钍矿物的类型及钍的赋存状态，钍矿化样品的主、微量元素的地球化学特征，钍成矿期热液流体的成分、温度、盐度、密度等条件，钍矿化的形成时代，成矿过程中流体及矿化物质的来源，以及成岩与成矿过程的差异性，进而探讨热流体在钍矿化过程中的演化过程及钍成矿机理。
通过相山矿田西部铀钍混合矿床的蚀变岩石学的研究工作，查明了该地区矿化蚀变的特征：碱交代期发育碳酸盐化、钠长石化，是早期单铀型矿化蚀变；灰绿色水云母、绿泥石化蚀变带的范围最广，但矿化程度不高；晚期紫色萤石化、磷灰石化蚀变，是成矿期与钍成矿关系最密切的蚀变类型。通过大量的薄片观察及电子探针工作总结了该地区钍的赋存状态：①以独立钍矿物形式存在于钍石、铀钍石、方钍石中；②以类质同象形式存在于沥青铀矿、晶质铀矿、铀石、钛铀矿中；③以微量类质同象存在于副矿物磷灰石、锆石、独居石、金红石、磷钇矿中。
对蚀变及矿化样品分类统计对比表明，铀钍矿化程度高的样品具以下特征：富CaO、P_2O5，贫SiO_2；富集稀土元素，特别是重稀土元素，其LREE/HREE值低，轻、重稀土分异度大；富集Zr、Hf、Sm、Y、Yb等高场强元素，亏损Rb、Ba等大离子元素，同时由于矿化样品发育碳酸盐化与萤石化，导致其相对富Sr。矿化过程中形成大量的金属硫化物及副矿物导致相关微量元素的富集。
通过对成矿前及成矿期流体包裹体均一温度及冰点温度的测定，并利用激光拉曼分析法测定其成分，结果表明成矿期流体中的气相成分主要为N_2、CH_4、H_2、CO_2等代表地幔物质的气体，成矿流体为中低温、中低盐度、低密度的流体，成矿期流体的温度要低于前期成矿的流体温度，钍成矿期的流体温度为190℃~200℃，但成矿期流体的盐度要高于前期成矿及成矿后期流体的盐度，而热流体的密度随着时间的演化逐渐变小。
采用LA-ICP-MS对钍矿化期的铀钍矿物及钍矿化期伴生的磷灰石进行微区测年，首次获得了相山矿田西部铀钍混合矿床铀钍成矿的Th-Pb年龄97.5Ma，与相山第二期铀成矿的年龄99±6Ma非常接近，表明在这一成矿阶段，铀钍是共沉淀的。结合前人的Rb-Sr、Sm-Nd、Pb同位素研究资料，证明相山矿田火山岩-次火山岩主要是下地壳及基底早元古代-中元古代变质岩部分熔融的产物，同时也有地幔岩浆活动的参与，而铀、钍成矿期的萤石中的Sm-Nd同位素证据及铀、钍成矿期萤石中流体包裹体的成分表明，成矿热液中有地幔流体的成分。
矿化样品中的U、Th等不相容元素的含量均远大于正常地壳及地幔中的不相容元素。来自地幔的碱性热液流体含有丰富的矿化剂（CO_2、CO、CH_4、H_2S、H_2等），可以加强热液与围岩中物质运移的微循环，萃取围岩中的不相容元素，同时在深部地幔流体上升过程中，地幔流体本身的演化过程也是富集铀、钍及稀土等不相容元素的过程，最终形成了富含U、Th及REE的成矿热液。热流体运移过程中，温度、盐度、成分他及PH值的变化，是铀钍分离成矿的重要条件。碱性富CO_2的热液，有利于U的络合迁移，但不利于Th的络合迁移；而酸性热液在富F-离子的情况下，钍、铀可以与之形成络合物迁移，形成铀钍共沉淀，使铀钍混合矿化与早期单铀型矿化分离；同时富F-的热液流体增大了硅酸盐在水溶液及流体相中的溶解度，导致萤石化的矿样中磷灰石颗粒边缘生长了大量自形的钍石，而不是方钍石。
Depending on the project--“The investigation and appraisal of thorium resourcesin China”, taking the volcanic hydrothermal type deposits of western Xiangshan orefield—Julongan deposit, Lijialing deposit and Zoujiashan deposit as the researchobjects, and summarizing a large amount of foreign and domestic research andanalyzing materials, this dissertation does the analysis on the following aspects:alteration petrology, uranium-thorium mineralogy, petrochemistry, geochemistry, fluidinclusion, isotope and chronology, finds out a series of conclusions about the thoriumalteration characterization, thorium mineral types and its existing occurrences, majorand trace elements’ geochemical characterizations of thorium mineralized samples,compositions, temperature, salinity, and density of thorium metallogenetic epoch fluidinclusions, the epoch of thorium metallization, origin of fluid and metallogenicmaterial in the mineralized process, and the differences between diagenetic andmetallogenic process, and discusses the evolution process and the thoriummetallogenic mechanism.
Through the alteration petrology research of western Xiangshan ore field, itclarifies the alteration characters of this area：the alkali alteration phase developingcarbonation and albitizaiton is the the single uranium mineralization phase; the sagegreen hydromicazation and chloritization alteration zone spreads widely but alwayswith low grade mineralization; and the purple fluoritization and apatitization areintensely related with thorium mineralization. Studying detailedly macroscopicoccurrence and microscopic petrology characteristics of ore beraing thin sections, theauthor summarizes the occurrences of thorium in these deposits: existing asindependent thorium minerals-thorite, uranothorite, and thorianite; lying asisomorphous admixture in uranium minerals–pitchblende, uraninite, uranothorite,coffinite, and brannerite; occurring as microisomorphic form in accessory minerals-apatite, zircon, monazite, rutile, and xenotime.
Comparing the analyzing material of the alteration samples, it indicates thaturanium and thorium rich minerals have the characters as the following: rich in CaO, and P_2O5，poor in SiO_2; high content of REE especially HREE, low ratio ofLREE/HREE-high differentia degree of LREE and HREE; rich in high field intensityelements such as Zr, Hf, Sm, Y, and Yb, poor in large ion elements such as Rb, andBa, but due to the carbonation and fluoritization with relatively high content of Sr.Sulfides and accessory minerals are the main cause of the enrichment of some relativerare elements.
Testing the homogeneous temperatures and the freezing temperatures of the fluidinclusions in different metallogenetic phases, together with the components of thefluid inclusions testing by Laser-Roman spectrometry, the results show that the gasphase of fluid inclusions are composed of N_2,CH_4, H_2, CO_2and so on, which are thetypical components of mantle; the metallogenetic fluid is low-middle temperature,low-middle salinity, and low density; the temperature of metallogenetic phase is lowerthan the temperature of prior metallogenetic phase, but the salinity of metallogeneticfluid is higher than the prior metallogenetic fluid; and the temperature of thoriummineralization is190℃~200℃。.
Using LA-ICP-MS to testing the chronology data of uranium and thoriumminerals and the accompanied apatite, this paper obtain97.5Ma Th-Pb age ofmetallization for the first time which is similar to the second phase of Umetallization-99.0Ma. Combining with the previous isotopic research material ofRb-Sr、Sm-Nd、Pb, it proves that the volcanic-subvolvanic rocks of Xiangshan isderived from the part melting of low crust and early-middle Proterozoic metamorphicrocks, besides some mantle magma; at the mean time both the Sm-Nd isotopic dataand the fluid inclusion components of metallogenetic fluorite indicate themetallogenetic thermal fluid is partly composed of mantle substance.
The ore-forming substances partly are derive from mantle fluid, and partly comefrom wall rock which the fluid goes up through, abundant incompatible elements areextracted. Mineralized samples are richer in U,Th and other incompatible elementsthan normal crust and mantle.
Alkali thermal fluid come from mantle with plenty mineralizer (CO_2、CO、CH_4、 H_2S、H_2and so on), can promote the microcirculation of matter movement betweenthermal fluid and wall rock, and extract the incompatible elements from wall rock.when the mantle fluid uprising, the evolution of the mantle fluid also is the process ofthe enrichment of U, Th, REE and other incompatible elements, and finally forms theore-bearing thermal fluid rich in U, Th, and REE. In the process of metallogeneticfluid moving, the change of temperature, salinity, compositions and the PH is theimportant conditions, in which U,Th can precipitate separately. Alkali thermal fluidwith CO_2, is benefit for the migrating of U, but the thorium; in the other side acidicthermal fluid with F-is favorable for the migration of both uranium and thorium,therefore uranium and thorium can form ore-veins separately, and the thermal fluidrich in F-can enlarge the solubility of silicate in water solutions and fluids, leading thegrowth of thorite (not the thorianite) around the apatite in the alteration zone offluoritization.
通过相山矿田西部铀钍混合矿床的蚀变岩石学的研究工作，查明了该地区矿化蚀变的特征：碱交代期发育碳酸盐化、钠长石化，是早期单铀型矿化蚀变；灰绿色水云母、绿泥石化蚀变带的范围最广，但矿化程度不高；晚期紫色萤石化、磷灰石化蚀变，是成矿期与钍成矿关系最密切的蚀变类型。通过大量的薄片观察及电子探针工作总结了该地区钍的赋存状态：①以独立钍矿物形式存在于钍石、铀钍石、方钍石中；②以类质同象形式存在于沥青铀矿、晶质铀矿、铀石、钛铀矿中；③以微量类质同象存在于副矿物磷灰石、锆石、独居石、金红石、磷钇矿中。
对蚀变及矿化样品分类统计对比表明，铀钍矿化程度高的样品具以下特征：富CaO、P_2O5，贫SiO_2；富集稀土元素，特别是重稀土元素，其LREE/HREE值低，轻、重稀土分异度大；富集Zr、Hf、Sm、Y、Yb等高场强元素，亏损Rb、Ba等大离子元素，同时由于矿化样品发育碳酸盐化与萤石化，导致其相对富Sr。矿化过程中形成大量的金属硫化物及副矿物导致相关微量元素的富集。
通过对成矿前及成矿期流体包裹体均一温度及冰点温度的测定，并利用激光拉曼分析法测定其成分，结果表明成矿期流体中的气相成分主要为N_2、CH_4、H_2、CO_2等代表地幔物质的气体，成矿流体为中低温、中低盐度、低密度的流体，成矿期流体的温度要低于前期成矿的流体温度，钍成矿期的流体温度为190℃~200℃，但成矿期流体的盐度要高于前期成矿及成矿后期流体的盐度，而热流体的密度随着时间的演化逐渐变小。
采用LA-ICP-MS对钍矿化期的铀钍矿物及钍矿化期伴生的磷灰石进行微区测年，首次获得了相山矿田西部铀钍混合矿床铀钍成矿的Th-Pb年龄97.5Ma，与相山第二期铀成矿的年龄99±6Ma非常接近，表明在这一成矿阶段，铀钍是共沉淀的。结合前人的Rb-Sr、Sm-Nd、Pb同位素研究资料，证明相山矿田火山岩-次火山岩主要是下地壳及基底早元古代-中元古代变质岩部分熔融的产物，同时也有地幔岩浆活动的参与，而铀、钍成矿期的萤石中的Sm-Nd同位素证据及铀、钍成矿期萤石中流体包裹体的成分表明，成矿热液中有地幔流体的成分。
矿化样品中的U、Th等不相容元素的含量均远大于正常地壳及地幔中的不相容元素。来自地幔的碱性热液流体含有丰富的矿化剂（CO_2、CO、CH_4、H_2S、H_2等），可以加强热液与围岩中物质运移的微循环，萃取围岩中的不相容元素，同时在深部地幔流体上升过程中，地幔流体本身的演化过程也是富集铀、钍及稀土等不相容元素的过程，最终形成了富含U、Th及REE的成矿热液。热流体运移过程中，温度、盐度、成分他及PH值的变化，是铀钍分离成矿的重要条件。碱性富CO_2的热液，有利于U的络合迁移，但不利于Th的络合迁移；而酸性热液在富F-离子的情况下，钍、铀可以与之形成络合物迁移，形成铀钍共沉淀，使铀钍混合矿化与早期单铀型矿化分离；同时富F-的热液流体增大了硅酸盐在水溶液及流体相中的溶解度，导致萤石化的矿样中磷灰石颗粒边缘生长了大量自形的钍石，而不是方钍石。
Depending on the project--“The investigation and appraisal of thorium resourcesin China”, taking the volcanic hydrothermal type deposits of western Xiangshan orefield—Julongan deposit, Lijialing deposit and Zoujiashan deposit as the researchobjects, and summarizing a large amount of foreign and domestic research andanalyzing materials, this dissertation does the analysis on the following aspects:alteration petrology, uranium-thorium mineralogy, petrochemistry, geochemistry, fluidinclusion, isotope and chronology, finds out a series of conclusions about the thoriumalteration characterization, thorium mineral types and its existing occurrences, majorand trace elements’ geochemical characterizations of thorium mineralized samples,compositions, temperature, salinity, and density of thorium metallogenetic epoch fluidinclusions, the epoch of thorium metallization, origin of fluid and metallogenicmaterial in the mineralized process, and the differences between diagenetic andmetallogenic process, and discusses the evolution process and the thoriummetallogenic mechanism.
Through the alteration petrology research of western Xiangshan ore field, itclarifies the alteration characters of this area：the alkali alteration phase developingcarbonation and albitizaiton is the the single uranium mineralization phase; the sagegreen hydromicazation and chloritization alteration zone spreads widely but alwayswith low grade mineralization; and the purple fluoritization and apatitization areintensely related with thorium mineralization. Studying detailedly macroscopicoccurrence and microscopic petrology characteristics of ore beraing thin sections, theauthor summarizes the occurrences of thorium in these deposits: existing asindependent thorium minerals-thorite, uranothorite, and thorianite; lying asisomorphous admixture in uranium minerals–pitchblende, uraninite, uranothorite,coffinite, and brannerite; occurring as microisomorphic form in accessory minerals-apatite, zircon, monazite, rutile, and xenotime.
Comparing the analyzing material of the alteration samples, it indicates thaturanium and thorium rich minerals have the characters as the following: rich in CaO, and P_2O5，poor in SiO_2; high content of REE especially HREE, low ratio ofLREE/HREE-high differentia degree of LREE and HREE; rich in high field intensityelements such as Zr, Hf, Sm, Y, and Yb, poor in large ion elements such as Rb, andBa, but due to the carbonation and fluoritization with relatively high content of Sr.Sulfides and accessory minerals are the main cause of the enrichment of some relativerare elements.
Testing the homogeneous temperatures and the freezing temperatures of the fluidinclusions in different metallogenetic phases, together with the components of thefluid inclusions testing by Laser-Roman spectrometry, the results show that the gasphase of fluid inclusions are composed of N_2,CH_4, H_2, CO_2and so on, which are thetypical components of mantle; the metallogenetic fluid is low-middle temperature,low-middle salinity, and low density; the temperature of metallogenetic phase is lowerthan the temperature of prior metallogenetic phase, but the salinity of metallogeneticfluid is higher than the prior metallogenetic fluid; and the temperature of thoriummineralization is190℃~200℃。.
Using LA-ICP-MS to testing the chronology data of uranium and thoriumminerals and the accompanied apatite, this paper obtain97.5Ma Th-Pb age ofmetallization for the first time which is similar to the second phase of Umetallization-99.0Ma. Combining with the previous isotopic research material ofRb-Sr、Sm-Nd、Pb, it proves that the volcanic-subvolvanic rocks of Xiangshan isderived from the part melting of low crust and early-middle Proterozoic metamorphicrocks, besides some mantle magma; at the mean time both the Sm-Nd isotopic dataand the fluid inclusion components of metallogenetic fluorite indicate themetallogenetic thermal fluid is partly composed of mantle substance.
The ore-forming substances partly are derive from mantle fluid, and partly comefrom wall rock which the fluid goes up through, abundant incompatible elements areextracted. Mineralized samples are richer in U,Th and other incompatible elementsthan normal crust and mantle.
Alkali thermal fluid come from mantle with plenty mineralizer (CO_2、CO、CH_4、 H_2S、H_2and so on), can promote the microcirculation of matter movement betweenthermal fluid and wall rock, and extract the incompatible elements from wall rock.when the mantle fluid uprising, the evolution of the mantle fluid also is the process ofthe enrichment of U, Th, REE and other incompatible elements, and finally forms theore-bearing thermal fluid rich in U, Th, and REE. In the process of metallogeneticfluid moving, the change of temperature, salinity, compositions and the PH is theimportant conditions, in which U,Th can precipitate separately. Alkali thermal fluidwith CO_2, is benefit for the migrating of U, but the thorium; in the other side acidicthermal fluid with F-is favorable for the migration of both uranium and thorium,therefore uranium and thorium can form ore-veins separately, and the thermal fluidrich in F-can enlarge the solubility of silicate in water solutions and fluids, leading thegrowth of thorite (not the thorianite) around the apatite in the alteration zone offluoritization.
引文
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