Experimental Study on Possibility of Deep Uranium-Rich Source Rocks Providing Uranium Source in Ordos Basin
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摘要:
鄂尔多斯盆地上三叠统延长组长7段石油优质烃源岩以富铀为特色，而盆地侏罗-白垩纪地层以赋存大量砂岩型铀矿而著称. 为探索深部长7富铀烃源岩为浅部砂岩型铀矿形成提供铀源的可能性，选择盆地南部的富铀烃源岩、油样以及具有代表性的碳酸铀酰作为反应物，在中-高温高压还原条件下分别进行烃源岩生排烃-排铀模拟实验和油-铀关系模拟实验. 结果表明，铀元素可随烃源岩排烃过程一同排出，30~200℃和2~5 MPa内温压的增高有利于生烃量和排铀量的增加；且铀携出率随生烃量增加而增大，一般为55%~75%. 其中水溶性铀占比约12%，由生烃作用叠加导致的铀携出率为43%~48%. 本实验发现铀迁移形式特殊，为四价（UO2）、六价（UO3）、四价与六价的混合价态（U3O8）及水合物胶体形式（UO3·H2O、U6O7（OH）2O），主要是被低温油气流体吸附而随之迁移，且铀吸附量随温度的增加和压力的降低呈增加的趋势. 因此，低温热液含铀的油-水流体往浅部地层迁移时对铀矿形成是有利的. 综合研究认为鄂尔多斯盆地深部的长7富铀烃源岩可大量释放或排出铀元素，铀以四价、六价、混合价态等形式被低温油气吸附，并且随油水流体一起沿断裂通道向上迁移，从而为盆地浅部砂岩型铀矿的形成提供铀源.
Abstract:The high quality source rocks of the Chang 7 Member in Yanchang Formation of the Upper Triassic in the Ordos Basin are characterized by uranium enrichment, while the Jurassic-Cretaceous strata of the basin are famous for hosting a large number of sandstone-type uranium deposits. To analyze the possibility of source rocks providing uranium source for shallow sandstone type uranium deposits, the uranium-rich source rocks, oil samples from the Chang 7 Member and representative uranyl carbonate were selected as reactants, and simulation experiments of hydrocarbon generation and expulsion of uranium from source rocks and oil-uranium relationship were carried out respectively under the reduction conditions of medium-high temperature and high pressure. The results show that uranium can be discharged along with the process of hydrocarbon expulsion from source rock, and the increase of temperature and pressure at 30-200 ℃ and 2-5 MPa is conductive to the increase of hydrocarbon generation and uranium discharge. The discharged rate of uranium increases with the increase of hydrocarbon generation and is generally 55%-75%. Among them, the proportion of soluble uranium from itself is about 12%, and the discharged rate of uranium caused by the superposition of hydrocarbon generation is 43%-48%. The uranium migration forms found in this experiment are special, such as tetravalent (UO2), hexavalent (UO3), mixed valence (U3O8) and hydrate colloid form (UO3·H2O, U6O7(OH)2O), which are mainly adsorbed by low-temperature oil-gas fluid, and the uranium adsorption capacity shows an increasing trend with the increase of temperature and the decrease of pressure. Thus, it is beneficial for uranium ore formation when low temperature uranium-bearing oil-hydrothermal fluids migrate to shallow strata. Based on the above analyses, it is considered that the source rocks of Chang 7 Member in the southern Ordos Basin can release or discharge a large amount of uranium, which can be adsorbed by low-temperature oil-gas in the form of tetravalent, hexavalent and mixed valence. Subsequently, the adsorbed uranium moves upwards along with the oil-water fluid through the fracture, providing partial material source for the formation of shallow sandstone-type uranium deposits of the basin.
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图 1 鄂尔多斯盆地构造单元及长7段烃源岩厚度分布示意图（a）和长7段伽玛异常强度平面分布（b）
Fig. 1. The schematic diagram of tectonic units and the thickness distribution of source rocks in the Chang 7 Member (a) and planar distribution of anomalous gamma intensity in the Chang 7 Member (b)
图 2 延长组长7段优质烃源岩伽玛异常段典型曲线形态（a）、长7段地层综合柱状图(b)和露头照片(c)
图a修改自刘池洋等，2020；图c在陕西铜川瑶曲镇聂家河村南村口所摄
Fig. 2. Gamma abnormal pattern of high-quality source rocks in Chang 7 Member (a), comprehensive strata columnar (b) and outcrop photograph (c) of the Chang 7 Member
图 3 烃源岩生排烃-排铀(a)和铀-油关系(b)模拟实验的操作流程
Fig. 3. Operation procedures of the experimental simulation of hydrocarbon generation and expulsion-uranium expulsion in source rock (a) and the experimental simulation of uranium-oil relationship (b)
图 4 200 ℃不同压力条件下实验前后的铀携出量（a）、铀携出率（b）、甲烷生成量(c)、烃类成分及含量（d）和总烃量（e）变化
Fig. 4. Changes of discharged content of uranium (a), discharged rate of uranium (b), methane production (c), types and productions of hydrocarbon (d) and total hydrocarbon production (e) after reaction under different pressures at 200 ℃
图 5 2 MPa不同温度条件下样品实验前后的铀携出量(a)和铀携出率(b)变化
Fig. 5. Changes of discharged content (a) and discharged rate (b) of uranium after reaction under different temperatures at 2 MPa
图 6 200 ℃不同压力条件下石油与碳酸铀酰混合的反应产物的X射线衍射图
Fig. 6. The X-ray diffraction pattern of the reaction product of petroleum mixed with uranyl carbonate after reaction under different pressures at 200 ℃
图 8 200 ℃不同压力下反应后的铀酰离子浓度变化
Fig. 8. The relation between uranyl ion concentration and experimental pressure after reaction at 200 ℃
图 9 3 MPa不同温度条件下石油与碳酸铀酰混合的反应产物的X射线衍射图
Fig. 9. The X-ray diffraction pattern of the reaction product of petroleum mixed with uranyl carbonate after reaction under different temperatures at 3 MPa
图 10 3 MPa不同温度下反应后的铀酰离子浓度变化
Fig. 10. The relationship between uranyl ion concentration and experimental temperature after reaction under different temperatures at 3 MPa
图 11 盆地西南部深部石油运移至浅部直罗组及其与浅部砂岩铀矿的空间关系
Fig. 11. Spatial relationship between deep oil migration to the Zhiluo Formation and shallow sandstone uranium deposits in southwestern Ordos Basin
表 1 鄂尔多斯盆地长7段烃源岩热解分析数据
Table 1. Pyrolysis analysis data of the Chang 7 Member source rocks in Ordos Basin
样品 有机碳TOC（%） 最高峰温Tmax（℃） 可溶烃S1（mg/g） 热解烃S2（mg/g） 有机CO2 S3（mg/g） 产油潜力S1+S2（mg/g） 产率指数Ip 干酪根类型 氢指数IH 降解率D（%） 烃指数IHC（mg/g） 长7段油页岩 16.38 427.0 4.66 29.51 4.21 34.17 0.14 ⅡB 175 2.84 27.69 注：热解分析在西北大学大陆动力学实验室完成. 
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表 2 模拟实验中设定的温压条件
Table 2. Temperature and pressure conditions set in the simulation experiment
实验名称 对比类型 温度（℃） 压力（MPa） 实验名称 对比类型 温度（℃） 压力（MPa） 烃源岩排烃-排铀实验 相同温度不同压力 200 2 中高温高压及还原条件的油-铀关系 相同温度不同压力 200 2 3 3 4 4 5 5 相同压力不同温度 30 2 相同压力不同温度 30 3 100 100 150 150 200 200
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表 3 200 ℃不同压力条件下实验前后的铀含量和烃类成分及含量变化
Table 3. The changes of uranium content and hydrocarbon type and content after reaction under different pressure at 200 ℃
压力(MPa) 铀质量百分比ω(10-6) 样品质量（g） 携出量(10-4 g) 携出率(%) 甲烷 乙烷 丙烷 异丁烷 正丁烷 异戊烷 正戊烷 乙烯 丙稀 总烃 反应前 反应后 反应前 反应后 生成量 占比(%) 生成量 占比(%) 生成量 占比(%) 生成量 占比(%) 生成量 占比(%) 生成量 占比(%) 生成量 占比(%) 生成量 占比(%) 生成量 占比(%) 生成量 占比(%) 2 281 120 50 47.4 83.62 59.52 27.04 55.54 3.74 7.68 2.67 5.48 0.86 1.76 1.92 3.94 0.87 1.78 1.12 2.30 6.94 14.25 3.51 7.20 48.69 100 3 281 87.8 50 46.8 99.41 70.75 34.70 53.26 5.15 7.90 2.80 4.30 1.08 1.66 2.02 3.10 1.13 1.73 1.61 2.47 8.93 13.71 7.73 11.86 48.69 100 4 281 80.8 50 42.2 106.40 75.72 36.05 51.95 8.27 11.92 5.28 7.61 1.02 1.47 2.44 3.52 1.35 1.95 1.36 1.96 7.39 10.65 6.24 8.99 69.40 100 5 281 72.8 50 46.8 108.43 77.75 37.98 49.75 6.10 7.99 3.48 4.56 1.20 1.57 2.38 3.12 1.37 1.79 1.97 2.58 14.55 19 7.31 9.58 76.34 100 注：反应物分析测试在核工业二〇三研究所完成.
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表 4 2 MPa不同温度条件下的样品实验前后铀和烃类成分及含量变化
Table 4. The changes of uranium content and hydrocarbon type and content after reaction under different temperatures at 2 MPa
温度(℃) 铀质量百分比ω(10-6) 样品质量（g） 携出量(10-4 g) 携出率(%) 甲烷 乙烷 丙烷 异丁烷 正丁烷 异戊烷 正戊烷 乙烯 丙稀 总烃 反应前 反应后 反应前 反应后 生成量 占比(%) 生成量 占比(%) 生成量 占比(%) 生成量 占比(%) 生成量 占比(%) 生成量 占比(%) 生成量 占比(%) 生成量 占比(%) 生成量 占比(%) 生成量 占比(%) 30 281 268 50 45.9 17.53 12.48 - - - - - - - - - - - - - - - - - - - - 100 281 132 50 46.2 79.52 56.60 20.27 55.93 3.02 8.33 1.63 4.50 2.72 7.51 1.03 2.84 0.52 1.43 0.72 1.99 3.61 9.96 2.72 7.51 36.24 100 150 281 124 50 47.5 81.60 58.08 23.83 57.48 3.46 8.35 2.05 4.94 0.82 1.98 1.39 3.35 0.94 2.27 1.09 2.63 4.92 11.87 2.96 7.14 41.46 100 200 281 120 50 47.4 83.62 59.52 27.04 55.56 3.74 7.69 2.67 5.49 0.86 1.77 1.92 3.94 0.87 1.79 1.12 2.30 6.94 14.26 3.51 7.21 48.67 100 注：反应物分析测试在核工业二〇三研究所完成，“-”代表未检测到.
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表 5 200 ℃不同压力条件下石油与碳酸铀酰混合的反应产物及产量与溶液中铀酰离子浓度变化
Table 5. The reaction product and yield of mixture of petroleum and uranyl carbonate and the change of uranyl ion concentration in solution after reaction under different pressures at 200 ℃
压力（MPa） 2 3 4 5 固态产物 类型 U3O8 U3O8 UO3 UO3 产量（g） 0.13 0.10 0.06 0.02 铀酰离子 Abs 1.057 1.326 1.592 1.737 C（mol/L） 0.004 9 0.007 6 0.010 2 0.011 7
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表 6 不同浓度的铀酰离子的吸光度
Table 6. The absorbance of uranyl ions at different concentrations
C(mol/L) 0 0.001 25 0.002 5 0.005 0 0.007 5 0.010 0 Abs 0.526 0.695 0.816 1.161 1.331 1.515
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表 7 3 MPa不同温度条件下石油与碳酸铀酰混合的反应产物及产量与溶液中铀酰离子浓度变化
Table 7. The reaction product and yield of mixture of petroleum and uranyl carbonate and the change of uranyl ion concentration in solution after reaction under different temperatures at 3 MPa
温度（℃） 30 100 150 200 固态产物 类型 UO3·H2O UO3·H2O UO3·H2O, U6O7(OH)2O UO3 产量（g） 0.09 0.16 0.21 0.01 铀酰离子 Abs 1.542 1.243 3.000 1.057 C（mol/L） 0.009 7 0.006 7 0.004 9 0.024 0
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