Ore-Forming Fluid and Thermochemical Sulfate Reduction in the Wusihe Lead-Zinc Deposit, Sichuan Province, China
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摘要: 四川乌斯河铅锌矿床是赋存于震旦系灯影组白云岩中的大型铅锌矿床.本次研究结合最新的野外地质现象发现该矿床除存在前人所强调的沉积成矿作用以外，热液成矿作用非常明显.对该矿床流体包裹体进行细致的岩相学、显微测温和激光拉曼研究，揭示成矿流体特征，并探讨成矿机制.研究结果显示该矿床包裹体类型较为单一，以气液两相为主，均一温度主要集中于120~260 ℃，平均盐度为10.0% NaCl eqv，压力为32~68 MPa，成矿流体为中-低温、中等盐度.激光拉曼测试显示包裹体气相成分含有CH4、H2S、C2H6、C2H2、N2和NH3，为多元共存的流体体系.在热驱动力下(120~260 ℃)，流体混合作用提供了物质基础(SO42-)、催化剂(Mg2+)和还原剂(有机质、CH4和H2S)促使硫酸盐热化学还原反应(TSR)启动.TSR反应过程中流体pH发生变化，进一步促进了金属硫化物沉淀.Abstract: The Wusihe lead-zinc deposit, hosted in the Dengying Formation, is a large lead-zinc deposit in the Sichuan Province, China. The previous research noted the Wusihe deposit was classified as a sediment-hosted stratiform lead-zinc deposit. However, our field survey result suggests that hydrothermal ore-forming processes are crucial to lead-zinc mineralization. In this paper, we present a detailed petrographic, microthermometric and laser Raman spectroscopy study of fluid inclusions from the Wusihe deposit reveals the characteristics of ore-forming fluids and mineralization mechanism. Primary fluid inclusions (FIs) in dolomite, quartz, calcite, fluorite and sphalerite are mainly two phases (L+V type). Microthermometric data show the homogenization temperatures range from 120 ℃ to 260 ℃, and the average of salinity is 10.0% NaCl eqv. The estimated trapping pressures are 32 MPa to 68 MPa. The laser Raman spectroscopy shows that the gas components have a certain amount of CH4, H2S, C2H6, C2H2, N2 and NH3. The mixed ore-forming fluids offer heat, SO42-, and Mg2+ to provoke the thermochemical sulfate reduction (TSR). The TSR could be a key factor for sulfur source and H+. The change of pH value leads to the precipitation of metallogenic elements.
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图 1 扬子地块西缘铅锌矿床分布略图
据成都地质矿产研究所(2003).云贵川渝1:250万地质图，略有简化
Fig. 1. Regional geological and distribution map of lead-zinc deposits on western margin of the Yangtze block
图 2 乌斯河铅锌矿床地质简图
1.第四系；2.奥陶系－二叠系碎屑岩、碳酸盐岩；3.寒武系碎屑岩、碳酸盐岩；4.上震旦统观音崖组碎屑岩－灯影组白云岩；5.南华系苏雄组陆相火山岩、碎屑岩；6.中元古界峨边群变质岩；7.铅锌矿(化)层；8.断层；9.地质界线；10.河流；11.晋宁期花岗岩；据四川地矿局207地质队(2006) 略有修改
Fig. 2. Geological sketch of the Wusihe lead-zinc deposit
图 3 不同成矿期成矿阶段野外照片
a.沉积期形成的纹层-条带状矿石；b.热液期多金属硫化物将沉积期形成的纹层状矿石角砾胶结；c.热液期第Ⅱ阶段形成的矿石被第Ⅲ阶段的方铅矿脉切穿；d.第Ⅲ阶段切层和顺层的方铅矿脉；e.热液期第Ⅱ、Ⅲ阶段形成的矿脉破碎后，呈角砾状，被第Ⅳ阶段沥青+方解石+石英胶结; f.热液期第Ⅳ阶段的沥青粗脉；Bit.沥青；Cc.方解石；Dol.白云石；Gn.方铅矿；Py.黄铁矿；Q.石英；Sp.闪锌矿
Fig. 3. Photographs showing different stages of the Wusihe deposit
图 4 乌斯河矿床流体包裹体特征
a.热液期第Ⅰ阶段的闪锌矿和白云石中包裹体发育；b.热液期第Ⅱ阶段，浅黄-浅黄白相间闪锌矿发育生长环带，L+V型原生流体包裹体沿生长环带发育，次生包裹体呈线状切穿生长环带; c.热液期第Ⅲ阶段，红棕色闪锌矿内部发育有定向排列的L+V型流体包裹体；d.热液期第Ⅲ阶段方解石内两种成分不同的L+V型；e.热液期第Ⅲ阶段，淡紫色萤石内的L+V型流体包裹体，包裹体颜色为无色透明，边缘清晰；f.热液期第Ⅱ阶段石英中的V型流体包裹体
Fig. 4. Photomicrographs of fluid inclusions in the Wusihe deposit
图 5 流体包裹体的均一温度-盐度直方图
a.沉积期，闪锌矿、白云石和石英中流体包裹体均一温度直方图；b.沉积期流体包裹体盐度直方图；c.热液期第Ⅰ成矿阶段，闪锌矿、白云石和石英中流体包裹体均一温度直方图；d.热液期第Ⅰ成矿阶段流体包裹体盐度直方图；e.热液期第Ⅱ成矿阶段，闪锌矿和石英中流体包裹体均一温度直方图；f.热液期第Ⅱ成矿阶段流体包裹体盐度直方图；g.热液期第Ⅲ成矿阶段，闪锌矿、方解石、萤石和石英中流体包裹体均一温度直方图；h.热液期第Ⅲ成矿阶段盐度直方图; i.热液期第Ⅳ成矿阶段，方解石和石英中流体包裹体均一温度直方图；j.热液期第Ⅳ成矿阶段流体包裹体盐度直方图
Fig. 5. Histograms of microthermometric and salinity for each stage
图 6 乌斯河矿床包裹体激光拉曼图谱
a.闪锌矿内包裹体，含有CH4和N2，其中CH4特征峰值为2 914.8 cm-1，N2特征峰值为2 327.5 cm-1；b.闪锌矿内包裹体，含有C2H2和H2O，其中C2H2特征峰值为1 961.6 cm-1，H2O特征峰值为3 386.9 cm-1；c.石英内包裹体，含有CH4和H2O，其中CH4特征峰值为2 914.7 cm-1，H2O特征峰值为3 544.3 cm-1；d.石英内包裹体，含有NH3和H2O，其中NH3特征峰值为3 339.7 cm-1，H2O特征峰值为3 618.2 cm-1；e.闪锌矿内包裹体，含H2S，特征峰值为2 614.4 cm-1；f.白云石内包裹体，含有C2H6，其中C2H6特征峰值为2 975.2 cm-1
Fig. 6. Raman spectra of fluid inclusions from the Wusihe deposit
图 7 乌斯河矿床成矿压力估算
a.热液期第Ⅰ成矿阶段，闪锌矿包裹体的等容线分布在ρ=0.90和ρ=0.79之间的红色区域，结合平均温度250 ℃投影，获得的最小捕获压力为32 MPa；b.热液期第Ⅱ成矿阶段，闪锌矿包裹体的等容线分布在ρ=0.97和ρ=0.87之间的红色区域，结合平均温度207 ℃投影，获得的最小捕获压力为58 MPa；c.热液期第Ⅲ成矿阶段，闪锌矿包裹体的等容线分布在ρ=1.07和ρ=0.92之间的红色区域，结合平均温度172 ℃投影，获得的最小捕获压力为68 MPa
Fig. 7. Estimation for the metallogenic pressure of Wusihe deposit
表 1 各成矿阶段流体包裹体显微测温数据
Table 1. Summary of fluid inclusion data from each stage of mineralization
成矿期成矿阶段(测试个数) 寄主矿物 初熔温度(℃) 均一温度(℃) 冰点(℃) 盐度(% NaCl eqv) 密度(g/cm3) 沉积期
n=36白云石 -33.8 181~221 -6.5~-2.9 3.6~9.9 0.90~0.97 闪锌矿 -21.6~-19.1 132~223 -10.8~-4.1 6.5~14.8 0.91~1.02 石英 191~194 / / / 热
液
期Ⅰ
n=73白云石 -41.6 216~266 -8.7~-7.2 10.7~12.5 0.87~0.93 石英 -16.3 203~291 -18.9~-4.2 6.7~21.6 0.84~0.97 闪锌矿 -23.8~-17.8 217~282 -10.3~-3.3 5.4~14.3 0.79~0.90 Ⅱ
n=79石英 178~269 -9.0~-2.5 4.2~12.9 0.85~0.96 闪锌矿 -25.1~-19.7 168~238 -9.1~-4.3 6.9~13.0 0.87~0.98 Ⅲ
n=65萤石 159~227 -9.2~-3.9 6.3~14.0 0.94~1.00 闪锌矿 -25.4~-20.6 133~211 -19.2~-4.8 7.6~21.8 0.92~1.07 方解石 208~218 -14.5~-10.1 14.0~18.2 0.96~0.99 石英 154~229 -8.2~-5.0 7.9~11.9 0.91~0.97 3Ⅳ
n=35石英 -18.1 141~199 -10.4~-1.6 2.7~14.4 0.90~1.01 方解石 -22.4 102~197 -13.5~-3.0 5.0~15.2 0.89~1.02 
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表 2 热液期流体包裹体激光拉曼测试结果
Table 2. Raman spectra of fluid inclusions from the hydrothermal stage
序号 成矿阶段 主矿物 包裹体类型 测试对象 成分 拉曼特征峰(cm-1) 采样位置 1 第Ⅰ阶段 石英 L+V型 气相 N2 2 339.4 角砾岩带 2 第Ⅰ阶段 石英 L+V型 气相 C2H6 2 974.0 角砾岩带 3 第Ⅰ阶段 白云石 L+V型 气相 C2H6 2 975.2 麦地坪上矿段 4 第Ⅰ阶段 白云石 L+V型 气相 CH4 2 912.3 麦地坪上矿段 5 第Ⅰ阶段 白云石 L+V型 气相 N2 2 330.5 麦地坪上矿段 6 第Ⅰ阶段 闪锌矿 L+V型 气相 CH4和N2 2 914.8和2 327.5 麦地坪上矿段 7 第Ⅱ阶段 闪锌矿 L+V型 气相 C2H2和H2O 1 961.6和3 386.9 麦地坪上矿段 8 第Ⅱ阶段 闪锌矿 L+V型 液相 H2O 3 443.3 麦地坪上矿段 9 第Ⅱ阶段 闪锌矿 L+V型 气相 N2 2 329.2 麦地坪上矿段 10 第Ⅱ阶段 石英 L+V型 气相 CH4和H2O 2 914.7和3 544.3 麦地坪上矿段 11 第Ⅱ阶段 石英 L+V型 气相 NH3和H2O 3 339.7和3 618.2 麦地坪上矿段 12 第Ⅲ阶段 闪锌矿 L+V型 气相 H2S 2 614.4 麦地坪上矿段 13 第Ⅲ阶段 闪锌矿 L+V型 气相 CH4 2 914.7 麦地坪下矿段 14 第Ⅲ阶段 石英 V型 气相 CH4 2 915.9 麦地坪下矿段
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表 3 乌斯河铅锌矿床金属硫化物硫同位素
Table 3. δ34S values of sulfides in the Wusihe lead-zinc deposit
样品编号 矿物 δ34SCDT(‰) 资料来源 送样号 矿物 δ34SCDT (‰) 资料来源 Hx001 闪锌矿 +14.83 Hx003 方铅矿 +14.41 Hx003 闪锌矿 +14.53 Hx006 方铅矿 +13.99 Hx005 闪锌矿 +12.65 Hx015 方铅矿 +13.92 Hx006 闪锌矿 +14.82 Hx001 方铅矿 +11.78 林方成，2005b Hx052 闪锌矿 +12.82 Hx044 方铅矿 +12.07 Hx044 闪锌矿 +10.48 林方成，2005b Hx052 方铅矿 +8.85 Hx055 闪锌矿 +10.43 Hx055 方铅矿 +11.20 Hx020 闪锌矿 +8.52 Wh-1 闪锌矿 +8.61 Hx021 闪锌矿 +7.48 Wh-2 闪锌矿 +14.05 李同柱等，2007 Hx025 闪锌矿 +13.13 Wh-3 闪锌矿 +13.75 Hx041 黄铁矿 +15.51
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