Application of EPMA and LA-ICP-MS to Study Mineralogy of Arsenopyrite from the Haoyaoerhudong Gold Deposit, Inner Mongolia, China
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摘要:
毒砂的主微量元素组成可以用于判断元素的赋存状态，探讨元素在不同阶段的活化迁移行为。内蒙古浩尧尔忽洞金矿床是产自白云鄂博群黑色岩系中的一个超大型金矿，发育重要载金矿物毒砂和斜方砷铁矿。前人利用传统粉末溶样法对矿石进行同位素分析，探讨了成矿物质来源，但金的迁移富集机制尚未获得解决。为探讨该矿床金迁移富集过程，本文在矿相学的基础上，对不同类型的毒砂进行电子探针(EPMA)和电感耦合等离子体质谱(ICP-MS)测试。所测得的电子探针数据经ZAF程序校正，LA-ICP-MS数据采用“无内标-基体归一法”进行定量计算，可以有效地分析微区成分。结果显示：毒砂(Apy)内部发育斜方砷铁矿(Lo)，可分为递进剪切变形阶段的Apy-Ⅰ1、Apy-Ⅰ2、Lo-Ⅰ和后剪切变形阶段的Apy-Ⅱ1、Apy-Ⅱ2、Lo-Ⅱ。各世代毒砂主元素组成稳定，含有少量Co、Ni和微量Sb、Te、Bi、Pb、Au、Ag。其中，Co在Apy-Ⅱ1和Apy-Ⅱ2中偏高，微量元素Au、Bi、Pb、Te在Apy-Ⅰ1中明显富集。斜方砷铁矿富As(64.06%~67.87%)，含Co(0.33%~4.98%)、Ni(1.23%~6.37%)，微量元素Au、Te、Bi、Pb、Ag在Lo-Ⅱ中更富集。研究表明，Lo-Ⅱ是最主要的载金矿物，温度和硫逸度的变化导致了斜方砷铁矿和自然金的沉淀，自然金是由早期毒砂和斜方砷铁矿的“不可见金”经活化再迁移沉淀形成。
Abstract:BACKGROUND The composition of major and trace elements in arsenopyrite can be used to identify the occurrence of elements and explore the remobilization and migration behaviour of elements in different stages. The Haoyaoerhudong gold deposit in Inner Mongolia is a super large gold deposit hosted in the black shales of the Bayan Obo Group. Gold-bearing minerals such as arsenopyrite and loellingite are present. Previous researchers have used the traditional powder dissolution method to analyze the isotope of the ore and discussed the source of ore-forming materials, but the migration and enrichment mechanism of gold has not been unraveled.
OBJECTIVES To understand the gold migration and enrichment process of this deposit.
METHODS Based on mineralogy, different types of arsenopyrite were analyzed by electron probe microanalyzer (EPMA) and inductively coupled plasma-mass spectrometry (ICP-MS). The data measured by EPMA was corrected by ZAF program, and the data measured by LA-ICP-MS was quantitatively calculated by "no internal standard-matrix normalized calibration".
RESULTS The results showed that loellingite was developed in arsenopyrite. They can be divided into Apy-Ⅰ1, Apy-Ⅰ2, Lo-Ⅰ in progressive shear deformation stage and Apy-Ⅱ1, Apy-Ⅱ2 and Lo-Ⅱ in post shear deformation stage. The major element composition of arsenopyrite in different generations was stable, with a small amount of Co and Ni and a trace amount of Sb, Te, Bi, Pb, Au and Ag. Cobalt was higher in Apy-Ⅱ1 and Apy-Ⅱ2, whereas Au, Bi, Pb and Te were obviously enriched in Apy-Ⅰ1. Loellingite was rich in As (64.06%-67.87%), Co (0.33%-4.98%), Ni (1.23%-6.37%). Trace elements such as Au, Te, Bi, Pb and Ag were more enriched in Lo-Ⅱ.
CONCLUSIONS Lo-Ⅱ is the most important gold-bearing mineral. The changes of temperature and sulfur fugacity lead to the precipitation of loellingite and native gold. Native gold is precipitated by remobilization and migration of "invisible gold" in early arsenopyrite and loellingite.
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表 1 毒砂和斜方砷铁矿的EPMA测试条件
Table 1. EPMA analytical conditions of arsenopyrite and loellingite
元素 分析晶体 特征X射线 计数时间(s) 标样矿物 检出限(μg/g) 峰位 背景 As TAP Lα 10 5 砷化镓(GaAs) 53~105 Sb PETH Lα 10 5 硫化锑(Sb2S3) 270~294 Pb PETJ Mα 10 5 方铅矿(PbS) 110~136 S PETJ Kα 10 5 黄铜矿(CuFeS2) 18~39 Ag PETH Lα 10 5 硫砷银矿(Ag3AsS3) 190~246 Fe LIF Kα 10 5 黄铁矿(FeS2) 138~186 Cu LIF Kα 10 5 黄铜矿(CuFeS2) 339~473 Au PETH Mα 10 5 金(Au) 146~192 Co LIF Kα 10 5 钴(Co) 294~374 Ni LIFH Kα 10 5 硫化镍(NiS) 111~155 Zn LIF Kα 10 5 闪锌矿(ZnS) 203~437 
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表 2 毒砂、斜方砷铁矿电子探针分析结果
Table 2. Electron probe microanalysis of arsenopyrite and loellingite
测点编号 矿物 元素含量(%) As Sb Pb S Ag Fe Cu Au Co Ni Zn 总计 B228(2)-1-3 毒砂
(Apy-Ⅰ1)45.78 - 0 18.51 0 34.87 - - 0.465 0.5 0 100.16 B228(2)-2-1 45.81 0.029 0.017 18.96 0 34.94 - 0 0.491 0.506 0 100.76 B228(2)-2-3 45.85 0.08 0.07 19.09 0.037 34.25 0 0 0.356 0.438 0 100.16 B241(1)-1-1 45.27 - 0.1 19.86 - 33.92 0 0.049 0.243 0.145 - 99.61 B241(1)-1-3 45.55 0.039 0.214 18.61 0 34.48 0 0 0.357 0.284 0 99.53 B241(1)-2-4 45.32 - 0 19.41 0 34.46 0 0 0.373 0.23 0 99.79 B241(2)-1-1 45.99 0.043 0.074 19.01 - 34.06 0 0 0.26 0.424 0 99.87 B241(1)-1-2 毒砂
(Apy-Ⅰ2)45.53 0.044 - 18.91 0 34.48 0 0.038 0.388 0.166 0 99.56 B241(1)-2-1 45.21 0 0 19.32 0 34.52 - 0.088 0.271 0.154 0 99.56 B228(2)-1-1 45.64 - 0 18.99 0.035 34.36 0 0 0.361 0.375 0 99.79 B228(2)-1-2 斜方砷铁矿
(Lo-Ⅰ)66.05 0.048 0.132 2.41 0 28.27 - 0 0.541 2.584 - 100.04 B228(2)-2-2 67.63 0.047 0 1.00 - 27.14 0 0 0.607 3.152 0.034 99.60 B241(1)-2-2 64.06 - 0.033 2.34 0 29.53 0 0 0.483 1.233 0 97.70 B241(2)-1-2 65.98 0 0 2.65 0 28.98 0 0 0.332 2.146 0 100.09 B241(2)-1-3 66.17 0 0.066 2.27 - 28.85 0 0 0.342 2.237 0 99.95 B183-5 毒砂
(Apy-Ⅱ1)45.37 0 0 19.00 - 33.86 0 0.133 0.431 0.506 0 99.31 B352-3-2 45.18 - 0 18.11 0 33.81 0 - 3.346 0.213 0 100.68 B219-1-2 45.29 - 0 18.40 0.033 34.37 0 0 2.03 0.562 0 100.69 B263(2)-1-3 45.58 0 0.018 18.60 0 33.84 0.031 0 1.242 0.878 0 100.19 B263(2)-2-2 45.31 0 0.035 19.30 - 33.97 0 0.088 1.282 0.675 0 100.66 B263(2)-2-3 45.61 0 0 18.96 0 33.87 0 0.022 1.255 0.727 0 100.44 B183-1 毒砂
(Apy-Ⅱ2)44.97 0 0.065 19.58 0 34.20 0 0 0.379 0.444 0.089 99.72 B352-1-1 44.46 0 0 18.70 - 34.69 - 0 2.212 0.201 0 100.29 B219-2-1 44.36 - 0.013 18.64 - 34.68 0 - 1.943 0.372 0 100.04 B263(1)-1-2 44.03 - 0 18.65 - 35.08 0 0.033 1.463 0.424 0 99.70 B263(2)-1-1 45.56 0 - 17.26 0 34.74 0 0 1.128 0.856 0 99.54 B263(2)-2-1 45.43 0 0 19.11 0.026 34.01 0 - 1.32 0.617 0 100.53 B263(1)-2-2 45.35 - 0.119 18.82 0 34.05 0 0.04 1.418 0.538 - 100.36 B263(1)-3-1 44.30 0 0 18.99 0.026 34.95 0 0 1.28 0.431 0 99.98 B183-2 斜方砷铁矿
(Lo-Ⅱ)66.26 0 0.033 1.52 0.019 26.27 0 0 0.639 3.846 0 98.59 B183-4 66.55 0 0 2.02 - 26.82 - 0.085 0.612 3.615 - 99.75 B352-1-2 67.80 0 0 0.97 0 24.44 0 0 4.951 1.807 0 99.96 B352-3-1 66.20 0 0.122 2.34 0 25.26 0 0.078 4.977 1.592 0 100.57 B219-1-1 67.87 0 0.081 1.08 0 24.79 0 0 2.763 3.471 0 100.04 B219-2-3 67.48 - 0.066 0.74 0.019 24.46 - 0 2.952 3.434 0 99.16 B263(1)-1-1 67.07 0.09 0.071 1.67 0 25.55 0 0.049 2.001 3.441 0 99.94 B263(1)-2-1 66.96 0.028 0.071 1.81 - 25.77 - 0.03 1.997 3.53 0 100.21 B263(1)-3-2 66.29 0 0.061 2.24 - 26.27 0 0.036 1.72 3.152 0 99.77 B263(2)-1-2 66.29 0 0.043 1.69 0 22.80 0 0 1.624 6.371 0 98.83 B263(2)-2-4 66.41 0 0.104 1.82 0.05 23.55 0 0 1.76 5.822 0 99.51 B263(2)-2-5 66.52 0 0 1.63 0.047 23.44 0 0 1.731 5.965 0 99.34 注：“-”表示元素含量低于检测限。
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表 3 毒砂、斜方砷铁矿LA-ICP-MS分析结果
Table 3. LA-ICP-MS analysis of arsenopyrite and loellingite
测点编号 矿物 元素含量(μg/g) Au Co Ni Sb Te Bi Pb Se Ag Cu Zn Ba Al Ti Mn B190(3)-3 毒砂
(Apy-Ⅰ1)0.08 5267 1510 196.32 14.64 91.05 12.82 11.88 3.00 45.41 3.97 0.27 591.27 3.93 660.59 B171(2)-3 0.70 13596 1147 274.62 15.32 47.47 2.53 6.07 0.23 0.64 1.48 2.64 441.49 20.06 2.75 B164(2)-5 0.81 10505 5034 135.60 22.13 78.42 7.06 9.54 0.73 0 1.80 3.63 876.66 17.84 9.28 B241(1)-1 12.37 1205 860 195.60 64.66 32.62 1.17 16.66 0.17 0.23 0.69 1.65 259.60 17.47 1.66 B241(1)-2 1470.74 1443 1756 206.00 656.40 3117.29 7.23 13.06 170.77 0.87 2.71 9.67 1724.68 159.63 15.98 平均 3.49 6403 2061 201.63 154.63 673.37 6.16 11.44 1.03 11.79 2.13 3.57 778.74 43.79 138.05 B241(1)-3 毒砂
(Apy-Ⅰ2)0.34 1102 766 174.65 46.74 0.35 - 12.58 0.39 0.44 7.11 0.03 0 - 0.51 B171(2)-2 0.06 13157 1258 276.13 11.36 0.26 0.01 4.01 0 0 - 0.02 - - 0 B190(3)-1 0.11 9867 2265 191.93 14.86 3.19 0.42 9.70 0 93.52 - 0.45 47.13 6.98 1.76 B164(2)-1 0.28 9999 1261 149.34 12.46 9.89 0.30 9.23 0.31 - 2.75 3.69 251.98 21.95 7.06 平均 0.20 8531 1388 198.01 21.36 3.42 0.24 8.88 0.35 0.44 4.93 1.05 149.56 14.46 3.11 B241(1)-4 斜方砷铁矿
(Lo-Ⅰ)125.15 1334 4459 147.69 319.25 1554.98 2.79 12.68 15.53 1.02 0.52 0.03 21.99 0.98 1.89 B171(2)-4 58.60 9186 6214 163.44 78.14 1119.76 1.28 3.64 5.81 0 4.11 3.84 632.47 40.12 10.77 B256-1-1 29.24 12952 12024 140.24 42.62 37.02 - 6.97 0.56 0.02 13.93 - 10.36 0 1.01 B256-1-3 14.04 10047 11280 100.19 56.19 7.72 - 9.51 0 0 0 0.50 143.01 6.59 - B228-02-1 13.18 1787 11037 152.43 39.56 43.50 0.53 13.78 0 0 - 1.31 217.67 9.66 - B228-02-3 22.28 1387 10094 118.66 35.84 1.06 - 18.71 - 0 - 0 1.59 0 0 B241-2-1 27.01 920 8199 132.52 32.12 0.37 0 - 0 0 0 0 - - - 平均 41.36 5373 9044 136.45 86.24 394.92 1.53 10.88 7.30 0.52 6.19 1.42 171.18 14.34 4.55 B352-2 毒砂
(Apy-Ⅱ1)0.57 17114 1092 153.23 40.96 24.42 3.85 4.56 0.16 0.93 - - 3.51 0.64 - B352-7 0.32 11992 721 119.16 36.29 15.07 1.28 4.74 0.31 0.38 - 1.69 60.37 2.68 1.67 B263(2)-2 0.60 5037 5010 98.64 35.92 13.75 1.12 12.64 0.06 0.36 1.38 3.55 281.94 22.32 9.60 B263(1)-5 0.49 8908 3354 153.76 60.67 11.58 1.62 7.91 0.04 - - 0.11 20.45 1.67 9.32 平均 0.50 10763 2544 131.20 43.46 16.20 1.97 7.46 0.15 0.56 1.38 1.78 91.57 6.83 6.86 B217(1)-2 毒砂
(Apy-Ⅱ2)0.24 12235 2189 326.33 23.79 1.05 0.08 6.38 0 0.58 0 0.12 12.46 3.15 0.98 B217(1)-4 0.48 9847 2474 333.20 28.18 4.86 3.16 9.31 - 0 0.68 - 3.98 - 0 B352-6 0.49 14627 1052 134.01 38.19 0.65 0.43 5.20 0 496.77 8.59 0.03 2.75 0 0.40 B352-4 0.23 11925 774 150.47 41.84 1.61 0.12 3.09 0.10 0 0.82 0.70 144.42 21.98 7.88 TB352-4 0.09 13060 1318 129.57 18.92 1.89 0.25 5.42 0.04 0 1.02 0.12 33.97 3.76 2.05 B263(1)-4 0.31 7470 3269 151.74 51.00 0.58 0.03 5.81 0.01 0.51 - 0.03 0.75 - - B263(2)-1 0.22 4231 3724 80.48 26.58 0.77 0.03 11.00 0 0.26 0.48 0.01 0.32 - 0.37 B263(1)-1 0.27 7235 2892 152.93 50.82 1.96 0.17 6.24 0 0 0 0.02 0 0.96 0 B263(3)-1 0.06 2438 630 77.99 26.29 0.34 - 9.52 0 - 0.40 0 0 - 0.33 平均 0.26 9230 2036 170.75 33.96 1.52 0.54 6.89 0.05 0.45 2.00 0.15 28.38 7.46 2.00 B352-5 斜方砷铁矿
(Lo-Ⅱ)1496.33 9874 4873 484.41 1733.03 15908.75 41.76 5.13 124.75 2.11 1.62 5.91 927.91 19.31 3.74 B217(1)-3 1409.11 12145 15303 368.04 475.07 9073.09 27.33 5.41 40.30 1.91 709.43 0.73 44.05 18.14 2.71 B217(1)-5 108.76 4033 5251 204.96 454.37 5936.41 29.02 6.65 8.77 0 - 0.20 79.98 2.41 2.69 B183-1 1656.97 1692 11690 619.91 1721.39 39714.13 34.69 - 23.97 - 125.53 212.27 16689.82 1215.42 198.35 B183-2 75.96 1964 12500 100.47 143.48 1163.09 5.57 22.49 7.11 0 30.90 33.54 4176.58 538.89 110.59 B183-4 45.45 2414 14312 106.73 66.05 735.19 - 24.11 2.62 0 0 0.18 31.67 35.64 0 B263(3)-2 12.30 8167 5492 56.77 51.68 53.85 0.48 9.43 3.46 23.39 1.62 3.61 509.77 19.40 11.39 B263(1)-2 11.89 6697 12912 123.14 71.23 1.00 0.26 3.95 - 10.83 5.91 - - 1.64 0 平均 602.10 5873 10292 258.05 589.54 9073.19 19.87 11.02 30.14 9.56 145.84 36.63 3208.54 231.36 41.18 注：“-”表示元素含量低于检测限。
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