The Ore-forming Age of the Uranium Mineralization Associated with Precambrian Sedimentary-Metamorphic Iron Deposits in Eastern Liaoning Province and Reliability Analysis of Dating Results
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摘要:
辽东地区是中国成矿时代最古老的铀矿矿集区，有单铀型和铁矿伴生型两种，其中单铀型矿床成矿年龄已基本厘定，而铁矿伴生型铀矿成矿年龄尚不明确，制约了该类矿床的成因认识。晶质铀矿是铁矿伴生型铀矿中最主要的含铀矿石矿物，对其开展测年能够直接厘定铀矿成矿时代。本文对翁泉沟富蛇纹石磁铁矿矿石和弓长岭石榴子石蚀变岩中的晶质铀矿进行电子探针（EPMA）测年，并利用激光剥蚀电感耦合等离子体质谱法（LA-ICP-MS）对翁泉沟富蛇纹石磁铁矿矿石中的晶质铀矿进行U-Pb测年，两种测年结果相互验证，获得辽东地区铁矿伴生型铀矿的成矿时代为～1.85Ga，并在～1.78Ga遭受了后期热液事件的改造，与单铀型矿床成矿年龄一致，说明辽东地区单铀型和铁矿伴生型铀矿都形成于碰撞后伸展环境。辽东地区铁矿伴生型铀矿不同矿床的成矿热液在流体成分和温度上有差别，但都具有碱性和氧化的特征。
Abstract:BACKGROUND The eastern Liaoning Province represents the eldest hydrothermal uranium ore cluster area in China. Two ore types are classified, including independent uranium mineralization and uranium mineralization associated with Precambrian sedimentary-metamorphic iron deposits. The ore-forming age of the former type has been well constrained at ~1.85Ga, whereas the age of the latter type remains uncertain. Iron deposit-associated uranium mineralization developed in the Wengquangou B-Mg-Fe deposit, the Gaojiagou Fe deposit, and the Gongchangling Fe deposit. Geochronological studies on uraninite of the Wengquangou deposit yielded variable ages ranging from 2.0 to 1.8Ga[11-14], with some ages even older than the depositional ages of the hosting Liaohe Group (2.05 to 1.93Ga[15]). This inconsistency suggests that some uraninite grains used for dating are detrital in origin. The lack of reliable age constraints on the iron deposit-associated uranium mineralization has raised questions about its origin. It remains unknown whether the iron deposit-associated uranium mineralization resulted from the same hydrothermal process and formed at the same tectonic setting when compared with the independent uranium mineralization.
OBJECTIVES To determine the metallogenic age and verify the accuracy of the age in uranium.
METHODS The instrument JXA-iHP200F was used for analysis, and the age was calculated according to Ranchin’s empirical formula[38]. The analytical conditions were 20kV acceleration voltage, 50nA beam current, and 5μm beam spot size. A further LA-ICP-MS U-Pb dating method was used to verify the EPMA chemical ages of the uraninite, using a 193nm GeoLasPro and Agilent 7900 ICP-MS with a laser spot size of 16μm.
RESULTS The calculated age of the Wengquangou deposit ranges from 1899 to 1324Ma, but it is mainly concentrated from 1899 to 1741Ma. Two peaks at 1859Ma and 1784Ma are constrained by an age frequency distribution histogram. This result is younger than the deposition age of the Liaohe Group. The age of the Gongchangling deposit ranges from 1858Ma to 1715Ma, with two peaks at 1865Ma and 1743Ma constrained by an age frequency distribution histogram. In the Wengquangou deposit, the position for uraninite LA-ICP-MS U-Pb dating corresponds to EPMA analytical points. The weighted mean ages are grouped into 1840±16Ma (MSWD=2.0) and 1787±8Ma (MSWD=0.95), which are consistent with the results obtained by EPMA. The loss of Pb can result in disruption of U-Th-Pb isotope system and thus affect the calculated ages. The loss of Pb can be probed because it is generally considered to be positively correlated with Si, Ca and Fe contents. The SiO2+CaO+FeO contents of most measuring spots of uraninite of the two deposits is less than 1%, and show no correlation with Pb contents, indicating that the loss of Pb is negligible.
CONCLUSIONS The uranium mineralization associated with iron deposits has been constrained at ~1.85Ga and then experienced hydrothermal superposition at ~1.78Ga. The age results indicate that both the independent and iron ore-associated uranium mineralization in the eastern Liaoning Province was formed at ~1.85Ga, linking to a Proterozoic post-orogenic extensional environment in the eastern North China craton. The ore-forming fluids of different deposits of iron associated uranium deposits are all alkaline and oxidated but vary in fluid composition and temperature. This study highlights combined application of EPMA and LA-ICP-MS dating methods on uraninite, realizing the complementary advantages of spatial resolution and dating precision.
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图 5 （a） 翁泉沟矿床富蛇纹石磁铁矿矿石中晶质铀矿电子探针年龄与SiO2+CaO+FeO相关关系图; （b）翁泉沟矿床EPMA和LA-ICP-MS法对应点测年结果关系图
Figure 5.
表 1 翁泉沟富蛇纹石磁铁矿矿石和弓长岭石榴子石蚀变岩中晶质铀矿电子探针分析数据及年龄计算
Table 1. EPMA analytical results and age caculations of uraninites of the serpentine-enriched magnetite ore from the Wengquangou deposit and the garnet altered rock from the Gongchangling deposit
测点编号 UO2
(%)ThO2
(%)PbO
(%)SiO2
(%)CaO
(%)FeO
(%)Y2O3
(%)La2O3
(%)Ce2O3
(%)Nd2O3
(%)Total
(%)年龄
(Ma)WQG5-1 68.55 2.83 16.29 − 0.79 − 2.05 − 0.60 1.16 92.28 1862 WQG5-2 71.22 1.79 17.16 0.03 1.05 − 1.70 0.09 0.38 0.65 94.06 1899 WQG5-3 67.48 2.30 14.04 0.03 0.23 1.84 4.59 0.21 0.55 1.86 93.13 1635 WQG5-4 69.44 1.60 14.57 0.06 0.25 0.11 3.95 0.15 0.43 0.65 91.21 1655 WQG5-5 66.69 3.07 15.22 0.01 0.20 0.22 4.45 0.21 0.60 1.72 92.38 1785 WQG5-6 66.55 3.15 14.89 0.06 0.28 0.08 4.05 0.08 0.55 1.85 91.52 1749 WQG5-7 67.11 2.33 15.26 0.02 0.21 − 4.38 0.03 0.29 1.25 90.86 1786 WQG5-8.1 66.99 2.57 15.25 0.04 0.21 0.06 4.28 0.02 0.54 1.44 91.40 1785 WQG5-8.2 66.86 2.70 15.60 − 0.18 0.09 4.12 0.11 0.50 1.38 91.53 1828 WQG5-9.1 66.90 1.20 15.94 0.02 0.71 0.08 2.87 0.24 2.91 2.53 93.39 1882 WQG5-9.2 65.99 1.07 15.47 0.02 0.66 0.03 2.90 0.06 3.34 2.95 92.48 1854 WQG5-10 67.20 1.14 15.50 0.03 0.25 0.29 3.51 − 1.89 2.36 92.15 1823 WQG5-11 67.54 2.27 15.86 0.03 0.46 0.98 3.18 0.36 1.07 1.92 93.66 1845 WQG5-12 67.20 1.61 15.96 0.03 0.41 0.13 2.44 0.10 3.01 2.74 93.64 1872 WQG5-13.1 67.15 2.63 14.92 − 0.28 0.04 3.93 − 0.39 1.33 90.67 1741 WQG5-13.2 68.32 3.06 16.48 0.02 0.44 0.01 2.58 − 0.61 1.40 92.93 1888 WQG5-13.3 68.26 2.86 15.27 0.03 0.26 0.15 3.29 0.20 0.29 1.31 91.91 1752 WQG5-13.4 67.06 2.66 15.31 0.03 0.25 − 3.98 0.06 0.24 1.40 90.99 1790 WQG5-13.5 66.03 3.66 14.81 0.01 0.19 0.11 4.18 0.17 0.44 1.34 90.93 1748 WQG5-14.1 67.09 2.42 15.90 0.02 0.27 0.06 4.11 − 0.40 1.40 91.67 1860 WQG5-14.2 70.54 1.91 16.57 − 1.24 0.22 1.84 − 0.48 1.12 93.92 1850 WQG5-15 67.42 2.47 15.66 0.04 0.22 0.04 4.07 − 0.43 1.51 91.85 1822 WQG5-16 67.01 2.40 15.04 0.04 0.29 0.08 4.17 0.04 0.63 1.36 91.05 1762 WQG5-17 68.38 2.74 16.31 0.02 0.72 0.08 2.38 0.16 0.49 1.51 92.77 1869 WQG5-18.1 67.93 3.01 14.73 0.07 0.18 − 3.83 − 0.35 1.48 91.57 1697 WQG5-18.2 69.37 2.84 15.78 0.04 0.89 0.04 2.29 − 0.83 1.50 93.56 1782 WQG5-18.3 69.94 3.06 13.65 0.03 0.52 0.07 3.01 0.20 0.72 1.68 92.88 1528 WQG5-18.4 68.52 2.73 15.47 0.04 0.28 0.04 3.17 0.09 0.55 1.21 92.09 1769 WQG5-19 67.93 1.49 14.68 0.11 0.32 0.65 2.70 0.17 2.94 2.79 93.77 1705 WQG5-20 71.85 2.11 15.46 0.06 1.11 3.49 1.62 0.10 0.13 1.09 97.02 1694 WQG5-21.1 69.54 2.11 15.79 0.01 0.93 0.20 2.19 0.15 0.65 1.60 93.16 1786 WQG5-21.2 69.22 1.91 15.61 − 0.82 0.29 2.25 0.03 0.77 1.48 92.38 1775 WQG5-22 66.55 1.15 15.59 0.01 0.78 0.07 3.04 0.29 2.89 2.53 92.90 1851 WQG5-23 66.47 2.69 15.21 0.02 0.21 0.23 4.22 0.11 0.59 1.30 91.04 1793 WQG5-24 67.68 1.64 16.28 0.01 0.49 0.24 2.96 0.18 1.06 1.74 92.29 1896 WQG5-25 67.27 2.52 14.48 0.04 0.20 0.32 4.11 0.10 0.39 0.99 90.42 1689 WQG5-26 68.83 2.84 15.96 − 0.84 0.45 2.05 0.21 0.73 1.21 93.11 1816 WQG5-27 69.39 2.69 15.84 − 0.38 0.07 2.75 0.15 0.56 1.48 93.29 1790 WQG5-28 69.92 1.53 11.73 0.09 0.43 0.44 4.00 0.27 1.27 1.93 91.62 1324 WQG5-29 66.34 2.84 14.95 0.02 0.19 0.04 3.95 − 0.46 1.53 90.31 1765 WQG5-30 69.57 1.92 15.95 0.01 1.13 0.06 2.19 0.01 0.72 1.54 93.08 1805 WQG5-31 66.83 2.69 15.06 − 0.19 0.24 3.93 0.03 0.42 1.19 90.56 1766 WQG5-32 66.95 2.24 14.99 0.04 0.22 0.34 4.29 0.06 0.36 1.19 90.68 1760 WQG5-33 67.50 2.41 15.65 − 0.20 0.03 4.20 0.20 0.42 1.33 91.94 1820 WQG5-34.1 68.65 2.81 16.32 0.06 0.80 0.02 2.08 0.05 0.72 1.46 92.97 1863 WQG5-34.2 66.60 2.64 15.11 0.02 0.18 0.03 4.20 0.06 0.29 1.02 90.13 1778 WQG5-34.3 67.69 2.57 14.49 0.13 0.34 0.27 3.70 0.04 0.29 1.49 91.02 1679 WQG5-34.4 63.76 2.48 13.81 1.77 0.33 1.15 3.33 0.30 0.52 1.27 88.71 1698 GCL2-1 65.18 7.51 15.86 − 0.07 0.36 0.61 0.18 − 0.52 90.29 1858 GCL2-2 64.39 7.95 15.53 0.02 0.10 0.30 0.72 0.11 − 0.71 89.83 1837 GCL2-3 70.15 6.29 15.62 0.03 0.06 − 0.31 0.03 − 0.49 92.97 1715 GCL2-4 69.44 7.32 15.80 0.04 0.03 0.04 0.21 0.17 0.02 0.52 93.58 1743 GCL2-5 69.92 4.75 17.03 0.06 0.09 0.01 0.50 0.13 0.09 0.18 92.75 1891 GCL2-6 70.47 5.21 15.84 0.05 0.07 0.02 0.50 0.11 − 0.21 92.48 1741 GCL2-7 69.46 6.28 16.95 − 0.05 0.04 0.08 0.09 − 0.18 93.11 1879 GCL2-8 69.18 6.70 16.84 0.05 0.08 − 0.33 0.11 − − 93.27 1870 GCL2-9 69.46 5.85 15.79 0.07 0.03 0.04 0.67 0.21 0.12 0.54 92.79 1755 GCL2-10 67.61 7.35 16.44 0.04 0.02 0.02 0.27 0.06 0.17 0.35 92.33 1861 GCL2-11 70.97 4.27 16.57 − 0.13 0.03 0.02 0.13 0.19 0.27 92.57 1817 GCL2-12 68.81 5.56 16.32 − 0.08 0.27 0.21 0.22 − 0.53 92.00 1832 GCL2-13 69.06 5.34 16.07 − 0.21 0.33 0.18 0.12 − 0.44 91.73 1800 GCL2-14 65.22 5.18 14.67 − 0.03 1.09 0.16 0.16 − 0.43 86.93 1739 注：“−”表示实验结果未达到检测限。 
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表 2 翁泉沟富蛇纹石磁铁矿石中晶质铀矿LA-ICP-MS法U-Pb同位素分析结果和对应电子探针测试点
Table 2. LA-ICP-MS isotope dating results of uraninites of the serpentine-enriched magnetite ore from the Wengquangou deposit and corresponding EPMA analytical spots
测点编号 普通Pb
含量207Pb/206Pb 207Pb/235U 206Pb/238U 207Pb/206Pb 206Pb/238U 不谐和度
（%）对应电子
探针测点电子探针
年龄
（Ma）（μg/g） 比值 1σ 比值 1σ 比值 1σ 年龄
（Ma）1σ
（Ma）年龄
（Ma）1σ
（Ma）WQG5-01 53.9 0.1154 0.0007 4.7798 0.0593 0.3000 0.0030 1887 11 1691 15 10.4 WQG5-1 1862 WQG5-02 41.6 0.1150 0.0007 4.6733 0.0470 0.2953 0.0033 1880 16 1668 17 11.3 WQG5-2 1899 WQG5-03 96.5 0.1143 0.0007 4.6626 0.0506 0.2967 0.0041 1869 11 1675 20 10.4 WQG5-9.2 1854 WQG5-04 22.9 0.1116 0.0006 4.8099 0.0624 0.3129 0.0042 1826 9 1755 21 3.9 WQG5-9.1 1882 WQG5-05 20.2 0.1110 0.0013 4.4265 0.0509 0.2920 0.0048 1816 22 1651 24 9.1 WQG5-10 1823 WQG5-06 26.8 0.1145 0.0010 4.2651 0.0623 0.2706 0.0034 1872 17 1544 17 17.5 WQG5-11 1845 WQG5-07 38.2 0.1127 0.0006 4.7316 0.0588 0.3047 0.0038 1844 9 1715 19 7.0 WQG5-12 1872 WQG5-08 18.4 0.1119 0.0015 5.1489 0.0709 0.3358 0.0049 1831 24 1866 24 −1.9 WQG5-14.1 1860 WQG5-09 13.0 0.1141 0.0010 5.6601 0.0810 0.3596 0.0042 1866 15 1980 20 −6.1 WQG5-14.2 1850 WQG5-10 27.1 0.1120 0.0007 5.4790 0.0571 0.3548 0.0037 1832 10 1957 18 −6.8 WQG5-17 1869 WQG5-11 52.0 0.1145 0.0009 4.9450 0.0636 0.3136 0.0040 1873 15 1758 20 6.1 WQG5-7 1786 WQG5-12 60.3 0.1090 0.0007 4.5419 0.0625 0.3030 0.0046 1783 12 1706 23 4.3 WQG5-34.2 1778 WQG5-13 107.0 0.1093 0.0007 4.9063 0.0836 0.3257 0.0055 1788 12 1818 27 −1.7 WQG5-34.3 1679 WQG5-14 19.4 0.1091 0.0006 4.6320 0.0571 0.3079 0.0037 1784 9 1731 18 3.0 WQG5-16 1762 WQG5-15 91.3 0.1082 0.0010 4.8412 0.0861 0.3245 0.0050 1769 18 1812 24 −2.4 WQG5-6 1749 WQG5-16 35.8 0.1096 0.0008 4.8450 0.0550 0.3209 0.0036 1794 13 1794 18 0 WQG5-13.3 1752 WQG5-17 53.3 0.1082 0.0007 4.5799 0.0523 0.3073 0.0037 1770 11 1727 18 2.4 WQG5-13.4 1790 WQG5-18 49.5 0.1102 0.0007 4.5852 0.0578 0.3023 0.0038 1802 12 1703 19 5.5 WQG5-18.2 1782 WQG5-19 63.7 0.1099 0.0007 4.5958 0.0546 0.3040 0.0036 1798 11 1711 18 4.8 WQG5-8.1 1785 WQG5-20 35.9 0.1117 0.0007 4.2390 0.0521 0.2754 0.0033 1827 11 1568 17 14.2 WQG5-8.2 1828
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