氟、氯对热液钨、铜成矿的制约
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摘要
矿化剂在热液矿床成矿过程中的重要作用一直为人们所关注，矿化剂地球化学行为直接影响成矿元素的富集成矿，不同的矿化剂元素可能对金属成矿具有一定的专属性。本文以著名的江西德兴铜厂超大型斑岩铜矿床和大吉山钨矿床作为研究对象，研究F、Cl与W、Cu成矿的关系。主要的认识如下：
(1)F在花岗质岩浆中，可以降低岩浆的粘度、密度、固液相线温度、改变熔体结构，而Cl对熔体结构没有多大的影响。F在流体—花岗质熔体相间，绝大多数配分系数小于1.0，趋向于熔体相中配分，D_F随体系中F浓度的升高而增加。Cl在流体—花岗质熔体相间的配分系数均大于1.0，且D_(Cl)随体系中Cl浓度的升高而增大，Cl强烈地趋向富集于流体相中。
(2)Cu在流体—花岗质熔体作用过程中，铜总趋向于流体相中分布(D_(Cu)都大于1)。特别是在富Cl流体中Cu浓度较高，说明在富含Cl的热液流体能够从共存的熔体中活化迁移出大量的Cu，S的加入D_(Cu)有降低的趋势。钨趋向于熔体相中富集，其配分系数大多小于1.0。
(3)德兴铜厂花岗闪长斑岩属钙碱性系列岩石属Ⅰ型花岗岩类，具有埃达克岩的特征。岩浆来源于深部，在结晶演化过程中发生了围岩物质的混染，这种高铜含量围岩的混染使成矿物质在岩浆中得到富集，有利于铜的活化、迁移。在铜厂岩体不同的蚀变带中，SiO_2、K_2O、Cu、Mo等从新鲜斑岩甚至弱蚀变带中带出，而在强蚀变带强烈富集，Cl同样有在强蚀变岩石中富集的趋势；而Na_2O、Fe从斑岩体中带出，进入流体相中，流体中大量Fe的存在，有利于铜的沉淀、富集成矿。
(4)德兴铜厂斑岩体微量元素和稀土元素地球化学特征表明，该岩体发生了流体—熔体作用，分异出来的流体是一种相对富氯的流体，同时成矿流体的流向是从岩体中心向接触带方向流动。
(5)大吉山花岗岩具有高SiO_2、A／CNK值，显示过铝质特点。黑云母花岗岩是壳源花岗岩但又受到幔源岩浆或幔源流体的影响。随着花岗岩的演化(从Ⅰ→Ⅱ→Ⅲ)SiO_2、K_2O+Na_2O逐渐增加，∑Fe、Al_2O_3、CaO、F含量降低，为成矿提供了大量的矿化剂(F)和沉淀剂(Fe、Ca)。Eu负异常从Ⅰ至Ⅲ阶段花岗岩逐渐加强，表明该岩浆经历了高度的分异演化。
(6)大吉山花岗岩类稀士元素具有“四重效应”配分的特点以及微量元素
对KJRb、Y/Ho、Zr舰f以及Nb/Ta发生明显分异，暗示在花岗岩岩浆的演化过
程中，经历了充分的流体一熔体作用，同时分异出大量富含F、W等矿化剂元素
和成矿元素的热液流体，致使钨矿的形成。大吉山石英脉型钨矿的成矿年龄大约
在155 Ma。
(7)通过对成矿流体和花岗质岩石黑云母、白云母中卤素相对逸度的研究
(109担20/fH。忍l)flu，d、109(/Hr州el)fluid)发现，铜厂斑岩型铜矿床的成矿体系是
相对富氯体系，而大吉山石英脉型钨矿床成矿体系相对富氟，同时氟可能主要迁
移W、Sn、Nb、Ta等金属元素。
(8)结合斑岩型铜矿床成矿流体特征，铜主要以Cl的络合物形式存在和迁
移，迁移形式主要是CuCI。、cuC12一等。石英脉型钨矿床中，钨主要以钨酸、钨
酸盐及其离解j衫式存在和迁移，如wo42一、Hwo4’、NaHwo4、Nawo4’等;在高
度富氟的成矿流体中，钨的氟氧络合物(如wO3F一，woZF42一等)对钨迁移也具有
重要的作用。
因此，不同矿化剂类型具有一定的成矿专属性，热液铜矿床主要与Cl、S有
关，而热液钨矿床大多与F有关。
In recent years, people began to pay attention to the importance of mineralizer in the process of the metal elements ore-forming. Geochemical behaviors of mineralizer affect the metal elements to form deposits to some degree, and different mineralizers have its mineralization speciality to different ore-forming elements. Generally magmatic hydrothermal Cu and Au deposits enrich Cl and S, but W and Sn deposits are rich F systems.
In this paper, in order to study the relationship between the Cu, W and. Cl, S, F, Tongchang porphyry copper deposit and the Dajishan tungsten deposit are selected as the studying objectives, detailed investigations have been conducted into the geological and geochemical characteristics of the granitic rock, biotite, trace element and REE geochemistry, fluid inclusion geochemistry and the partitioning coefficients of the F, Cl, Cu, W. Based on these data, the following conclusions are drawn:
(1) Fluorine can reduce the viscosity and density of magma, temperature of solide-liquidus line and change the melt frame, but Cl has little effect on the melt. Chlorine tends to be partitioned into the fluid phase while fluorine shows a strong tendency to the melt phase. Df increases; with the fluorine content increasing, and so does the DCl.
(2) Between the granitic melts and coexisting aqueous fluids, Cu strongly partitions toward the fluid. In contrast, W strongly partitions toward the melt. In particular Dcu linearly increases with the Cl concentration in,the fluid, indicating that Cl can transport enough copper from the melt or other source bed to form the deposits. But Dcu decreases with the S added in experimental system.
(3) Tongchang granodiorite porphyry belongs to calc-alkali granite, also has characters of the Adakites. Magma materials coming from the mantle, duritig the fractional crystallization, there exists contamination of the wall-rock. This process was propitious to enrich, activate, transport the copper. In different alteration granodiorite porphyry, SiO2, K2O, Cu, Mo are depleted in the fresh and weakly altered rock, and are enriched in the strongly altered rock, Cl is also enriched in the strongly altered rock. But Na2O and Fe are extracted from the porphyry into the ore-forming fluid, especially the presence of Fe is in favor of Cu deposition.
(4) The trace elements and REE geochemistry of the Tongchang granodiorite porphyry indicate, there exists the reaction between the porphyry and the hydrothermal fluid. The hydrothermal fluid was Cl-enriched solution, and flowed from the porphyry center to contact zone.
(5) Dajishan granites have high SiO2 content and high A/CNK, show peraluminous granite characters. Granites belong to S-type granite, but the biotite granite was affected by the mantle or mantle fluid. With the evolution of the granitic complexes, the SiO2 and K2O+Na2O increase, but Fe. Al2O3, CaO and F decrease. It supplied more mineralizer(F) and precipitator(Fe,Ca) for mineralization. Strong negative 8 Eu shows the
granites are high evolved granite.
(6) The tetrad effect of REE and the obvious fractionation between K-Rb, Y-Ho, Zr-Hf, Nb-Ta, and Sr-Eu in the Dajishan granites indicate that, the aqueous fluid pays an important role in the evolution of the granites, as well as indicate that there exist enough interaction between peraluminous melt and aqueous magmatic fluid. Furthermore the fluorine played a very important role in this process.
(7) By studying of ore-forming fluid and the micas (using the F, Cl contents in micas to calculate the halogen fugacity of the hydrothermal fluid, eg. Log (fH2O/fHCl)fluid and log(fHF/fHCl)fluid), Tongchang porphyry copper deposit system is enriched in chlorine, however Dajishan tungsten deposit system is relatively enriched in fluorine, which transport W, Sn, Nb, Ta , et al.
(8) According to the characters of the porphyry copper deposits, copper is transported by chlorine, such as CuCl0 and CuCl2. For the tungsten deposits, tungsten
(1)F在花岗质岩浆中，可以降低岩浆的粘度、密度、固液相线温度、改变熔体结构，而Cl对熔体结构没有多大的影响。F在流体—花岗质熔体相间，绝大多数配分系数小于1.0，趋向于熔体相中配分，D_F随体系中F浓度的升高而增加。Cl在流体—花岗质熔体相间的配分系数均大于1.0，且D_(Cl)随体系中Cl浓度的升高而增大，Cl强烈地趋向富集于流体相中。
(2)Cu在流体—花岗质熔体作用过程中，铜总趋向于流体相中分布(D_(Cu)都大于1)。特别是在富Cl流体中Cu浓度较高，说明在富含Cl的热液流体能够从共存的熔体中活化迁移出大量的Cu，S的加入D_(Cu)有降低的趋势。钨趋向于熔体相中富集，其配分系数大多小于1.0。
(3)德兴铜厂花岗闪长斑岩属钙碱性系列岩石属Ⅰ型花岗岩类，具有埃达克岩的特征。岩浆来源于深部，在结晶演化过程中发生了围岩物质的混染，这种高铜含量围岩的混染使成矿物质在岩浆中得到富集，有利于铜的活化、迁移。在铜厂岩体不同的蚀变带中，SiO_2、K_2O、Cu、Mo等从新鲜斑岩甚至弱蚀变带中带出，而在强蚀变带强烈富集，Cl同样有在强蚀变岩石中富集的趋势；而Na_2O、Fe从斑岩体中带出，进入流体相中，流体中大量Fe的存在，有利于铜的沉淀、富集成矿。
(4)德兴铜厂斑岩体微量元素和稀土元素地球化学特征表明，该岩体发生了流体—熔体作用，分异出来的流体是一种相对富氯的流体，同时成矿流体的流向是从岩体中心向接触带方向流动。
(5)大吉山花岗岩具有高SiO_2、A／CNK值，显示过铝质特点。黑云母花岗岩是壳源花岗岩但又受到幔源岩浆或幔源流体的影响。随着花岗岩的演化(从Ⅰ→Ⅱ→Ⅲ)SiO_2、K_2O+Na_2O逐渐增加，∑Fe、Al_2O_3、CaO、F含量降低，为成矿提供了大量的矿化剂(F)和沉淀剂(Fe、Ca)。Eu负异常从Ⅰ至Ⅲ阶段花岗岩逐渐加强，表明该岩浆经历了高度的分异演化。
(6)大吉山花岗岩类稀士元素具有“四重效应”配分的特点以及微量元素
对KJRb、Y/Ho、Zr舰f以及Nb/Ta发生明显分异，暗示在花岗岩岩浆的演化过
程中，经历了充分的流体一熔体作用，同时分异出大量富含F、W等矿化剂元素
和成矿元素的热液流体，致使钨矿的形成。大吉山石英脉型钨矿的成矿年龄大约
在155 Ma。
(7)通过对成矿流体和花岗质岩石黑云母、白云母中卤素相对逸度的研究
(109担20/fH。忍l)flu，d、109(/Hr州el)fluid)发现，铜厂斑岩型铜矿床的成矿体系是
相对富氯体系，而大吉山石英脉型钨矿床成矿体系相对富氟，同时氟可能主要迁
移W、Sn、Nb、Ta等金属元素。
(8)结合斑岩型铜矿床成矿流体特征，铜主要以Cl的络合物形式存在和迁
移，迁移形式主要是CuCI。、cuC12一等。石英脉型钨矿床中，钨主要以钨酸、钨
酸盐及其离解j衫式存在和迁移，如wo42一、Hwo4’、NaHwo4、Nawo4’等;在高
度富氟的成矿流体中，钨的氟氧络合物(如wO3F一，woZF42一等)对钨迁移也具有
重要的作用。
因此，不同矿化剂类型具有一定的成矿专属性，热液铜矿床主要与Cl、S有
关，而热液钨矿床大多与F有关。
In recent years, people began to pay attention to the importance of mineralizer in the process of the metal elements ore-forming. Geochemical behaviors of mineralizer affect the metal elements to form deposits to some degree, and different mineralizers have its mineralization speciality to different ore-forming elements. Generally magmatic hydrothermal Cu and Au deposits enrich Cl and S, but W and Sn deposits are rich F systems.
In this paper, in order to study the relationship between the Cu, W and. Cl, S, F, Tongchang porphyry copper deposit and the Dajishan tungsten deposit are selected as the studying objectives, detailed investigations have been conducted into the geological and geochemical characteristics of the granitic rock, biotite, trace element and REE geochemistry, fluid inclusion geochemistry and the partitioning coefficients of the F, Cl, Cu, W. Based on these data, the following conclusions are drawn:
(1) Fluorine can reduce the viscosity and density of magma, temperature of solide-liquidus line and change the melt frame, but Cl has little effect on the melt. Chlorine tends to be partitioned into the fluid phase while fluorine shows a strong tendency to the melt phase. Df increases; with the fluorine content increasing, and so does the DCl.
(2) Between the granitic melts and coexisting aqueous fluids, Cu strongly partitions toward the fluid. In contrast, W strongly partitions toward the melt. In particular Dcu linearly increases with the Cl concentration in,the fluid, indicating that Cl can transport enough copper from the melt or other source bed to form the deposits. But Dcu decreases with the S added in experimental system.
(3) Tongchang granodiorite porphyry belongs to calc-alkali granite, also has characters of the Adakites. Magma materials coming from the mantle, duritig the fractional crystallization, there exists contamination of the wall-rock. This process was propitious to enrich, activate, transport the copper. In different alteration granodiorite porphyry, SiO2, K2O, Cu, Mo are depleted in the fresh and weakly altered rock, and are enriched in the strongly altered rock, Cl is also enriched in the strongly altered rock. But Na2O and Fe are extracted from the porphyry into the ore-forming fluid, especially the presence of Fe is in favor of Cu deposition.
(4) The trace elements and REE geochemistry of the Tongchang granodiorite porphyry indicate, there exists the reaction between the porphyry and the hydrothermal fluid. The hydrothermal fluid was Cl-enriched solution, and flowed from the porphyry center to contact zone.
(5) Dajishan granites have high SiO2 content and high A/CNK, show peraluminous granite characters. Granites belong to S-type granite, but the biotite granite was affected by the mantle or mantle fluid. With the evolution of the granitic complexes, the SiO2 and K2O+Na2O increase, but Fe. Al2O3, CaO and F decrease. It supplied more mineralizer(F) and precipitator(Fe,Ca) for mineralization. Strong negative 8 Eu shows the
granites are high evolved granite.
(6) The tetrad effect of REE and the obvious fractionation between K-Rb, Y-Ho, Zr-Hf, Nb-Ta, and Sr-Eu in the Dajishan granites indicate that, the aqueous fluid pays an important role in the evolution of the granites, as well as indicate that there exist enough interaction between peraluminous melt and aqueous magmatic fluid. Furthermore the fluorine played a very important role in this process.
(7) By studying of ore-forming fluid and the micas (using the F, Cl contents in micas to calculate the halogen fugacity of the hydrothermal fluid, eg. Log (fH2O/fHCl)fluid and log(fHF/fHCl)fluid), Tongchang porphyry copper deposit system is enriched in chlorine, however Dajishan tungsten deposit system is relatively enriched in fluorine, which transport W, Sn, Nb, Ta , et al.
(8) According to the characters of the porphyry copper deposits, copper is transported by chlorine, such as CuCl0 and CuCl2. For the tungsten deposits, tungsten
引文
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