Paleoclimate Evolution and Uranium Mineralization during the Deposition of Uranium-Bearing Rocks in the Southwest of Songliao Basin
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摘要: 含铀岩系沉积时的古气候条件对铀成矿起着重要的控制作用，但是长期以来未引起人们足够重视.以松辽盆地西南部HLJ地区含矿目的层姚家组下段为研究对象，通过对代表性钻孔岩心的泥岩样品进行全岩主、微量元素和TOC测试，采用K/Na、aAlNa、CPA、CIX、PIA、CIW、CIA等多项化学风化指标来判断样品化学风化作用强度，重建其沉积时期古气候条件.同时，结合U和TOC含量及Fe2+/Fe3+比值来探讨含铀岩系沉积时的古气候条件对铀成矿的制约.结果表明，目的层碎屑岩经历了由弱-强-弱的化学风化作用，显示其沉积时的古气候由相对寒冷干旱-相对温暖潮湿-相对寒冷干旱的演变规律.这种古气候变化导致了铀储层砂体中TOC含量低（平均值0.05%），层间氧化带发育规模大，铀矿体主要形成于远离蚀源区的盆地腹部；形成于潮湿气候条件下的暗色泥岩具有更高TOC（平均值0.61%）和U含量（最高可达885×10-6），其沉积时发生了强烈的预富集作用而成为后期成矿过程中重要铀来源之一，其成岩期排泄出还原性孔隙水可能是铀储层砂体中构建氧化-还原屏障的主要因素.沉积时的温暖潮湿气候增强了蚀源区化学风化作用强度，有利于母岩铀元素活化和淋漓及沉积区泥岩铀的预富集作用.Abstract: Although, the paleoclimate plays an important role in controlling uranium mineralization during the deposition of uranium-bearing rocks, it has not attracted enough attention of uranium geologists for a long time. The lower member of Yaojia formation is the ore bearing target layer in the southwest of Songliao basin. Taking the lower member of Yaojia formation as the research object, the contents of the main and trace elements and total organic carbon of mudstone samples from representative boreholes were tested. A number of chemical weathering indexes, such as K/Na ratio, aAlNa, chemical proxy of alteration (CPA), modified chemical index of alteration (CIX), plagioclase index of alteration (PIA), chemical index of weathering (CIW), chemical index of alteration (CIA), are used to judge the intensity of chemical weathering of the samples, and reconstruct the paleoclimate conditions during the depositional period. At the same time, combined with the contents of U and TOC and the ratio of Fe2+/Fe3+, the constraints of paleoclimate conditions on uranium mineralization during the deposition of uranium-bearing rock series in the study area are discussed. The results show that the clastic rocks in the study area have experienced the change of chemical weathering intensity from weak to strong to weak, indicating that the evolution law of paleoclimate from relative cold and drought to relative warm and humidity to relative cold and drought. This paleoclimate change leads to low TOC content in uranium reservoir sand bodies (average value 0.05%) and large-scale development of interlayer oxidation zone, so uranium ore bodies are mainly located in the hinterland of the basin far away from the erosion source area. Dark mudstone formed in humid climate has higher TOC (average 0.61%) and U content (up to 885×10-6). It has become one of the important sources of uranium due to its strong preconcentration during deposition. The discharge of reducing pore water during diagenesis may be the main factor for the construction of oxidation-reduction barrier in uranium reservoir sand bodies. During deposition, the warm and humid climate enhances the intensity of chemical weathering in the source area, which is conducive to the activation and leaching of uranium in the parent rock and the uranium preconcentration of mudstone in the sedimentary area.
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图 2 松辽盆地西南部姚家组下段典型野外钻孔岩石颜色照片
a.钻孔ZK48-30，489.4~492.5 m，灰白色砂岩与暗色泥岩呈紧密伴生关系；b.为图a中对应点位①局部放大照片；c.钻孔ZK80-8，521.6 m，红色砂岩中发育红色泥砾；d.钻孔HLJ-15，641 m，灰白色砂岩中发育灰色泥砾；e.钻孔ZK40-8，560 m，浅红色砂岩中发育灰色和红色泥砾
Fig. 2. Rock color photos of typical field boreholes in the lower member of Yaojia Formation in the southwest of Songliao basin
图 3 研究区钻孔HLJ-15姚家组下段泥岩样品Sc/Th、CIW与CIA交会图
Fig. 3. cross plot of Sc/Th, CIW and CIA of mudstone samples from the lower member of Yaojia Formation of Borehole HJL-15 in the study area
图 4 研究区钻孔HLJ-15姚家组下段泥岩样品A-CN-K图解
Fig. 4. A-CN-K diagram of mudstone samples in the lower member of Yaojia Formation of Borehole HLJ-15 in the study area
图 5 研究区钻孔HLJ-15姚家组下段泥岩代表性化学风化指标纵向变化曲线
Fig. 5. Longitudinal variation curve of representative chemical weathering indexes of mudstone from the lower member of Yaojia Formation of Borehole HLJ-15 in the study area
图 6 研究区钻孔HLJ-15姚家组下段碎屑岩U含量、Fe2+/Fe3+、TOC含量变化曲线
Fig. 6. Variation curve of U content, Fe2+/Fe3+ and TOC content of clastic rocks in the lower section of Yaojia Formation from Borehole HLJ-15 in the study area
图 7 研究区钻孔HLJ-15姚家组下段碎屑岩U含量与Fe2+/Fe3+和TOC含量交会图
Fig. 7. Cross plot of U content, Fe2+/Fe3+ and TOC content of clastic rocks in the lower member of Yaojia Formation from Borehole HLJ-15 in the study area
图 8 松辽盆地西南部HLJ地区铀成矿模式（修改自焦养泉等，2015）
Fig. 8. Uranium metallogenic model of HLJ area in the southwest of Songliao basin (modified from Jiao et al., 2015)
表 1 松辽盆地西南部HLJ地区钻孔HLJ-15碎屑岩样品主、微量及化学风化指标值
Table 1. Main, trace and chemical weathering index values of clastic rock samples from Borehole HLJ-15 in HLJ area in southwest Songliao basin
样品号 HPL-1 HPL-2 HPL-3 HPL-4 HPL-5 HPL-6 HPL-7 HPL-8 HPL-9 HPL-10 HPL-11 HPL-12 HPL-13 HPL-14 HPL-15 HPL-17 HPL-18 HPL-19 HPL-20 岩性 红色泥岩 红色砂岩 红色泥岩 红色砂岩 红色砂岩 红色砂岩 暗色泥岩 灰色砂岩 灰色砂岩 灰色砂岩 暗色泥岩 暗色泥岩 灰色砂岩 灰色砂岩 灰色砂岩 红色泥岩 灰色砂岩 灰色砂岩 暗色泥岩 深度（m) 720 714 708 705 702 700 690 686 680 676 674 672 670 668 660 656 652 650 646 SiO2(%) 56.13 66.48 61.23 73.56 81.01 78.46 65.29 77.39 76.47 76.76 59.64 56.57 76.28 79.27 69.09 64.53 68.83 78.12 62.24 Al2O3(%) 13.59 10.12 13.28 12.58 10.17 10.01 16.95 11.44 8.92 10.12 20.43 22.04 10.43 10.47 16.81 15.33 11.77 10.79 20.27 TFe2O3(%) 4.47 1.48 3.96 2.02 1.42 1.46 3.41 1.56 1.83 1.25 3.26 3.36 1.60 1.26 2.23 7.48 2.23 1.17 2.33 MgO(%) 2.770 2.980 1.840 0.307 0.195 0.626 0.943 0.424 0.924 0.861 1.180 1.350 0.712 0.395 0.582 0.860 1.460 0.492 0.953 CaO(%) 5.510 4.990 4.670 2.080 0.296 1.380 0.736 0.859 2.470 1.980 0.539 0.569 1.750 0.829 0.209 0.340 3.340 1.010 0.197 Na2O(%) 1.300 1.270 1.340 1.380 1.170 1.080 1.120 1.200 0.831 0.869 0.853 0.858 0.901 0.942 1.030 0.548 0.980 0.936 0.710 K2O(%) 2.51 2.33 2.54 2.78 2.87 2.91 3.31 3.32 2.69 2.90 3.51 3.74 3.24 3.27 3.43 2.87 3.07 3.49 3.68 MnO(%) 0.158 0.081 0.098 0.039 0.011 0.049 0.024 0.024 0.098 0.062 0.027 0.022 0.057 0.033 0.014 0.058 0.074 0.019 0.016 TiO2(%) 0.622 0.347 0.616 0.375 0.427 0.244 0.778 0.301 0.253 0.358 0.876 0.915 0.237 0.263 0.804 0.725 0.496 0.241 0.928 P2O5(%） 0.143 0.086 0.092 0.084 0.096 0.072 0.154 0.073 0.085 0.100 0.216 0.242 0.069 0.075 0.123 0.232 0.095 0.065 0.116 Sc 12.30 10.10 8.28 10.90 12.50 12.50 10.40 Th 7.58 8.22 12.20 17.00 18.10 13.00 14.30 烧失量（%） 12.77 9.84 10.11 4.77 1.94 3.68 7.24 3.32 5.36 4.71 9.47 10.31 4.64 3.12 5.65 6.89 7.56 3.57 8.49 FeO(%) 0.44 0.40 0.24 0.45 0.35 0.58 0.72 0.59 1.41 1.05 1.34 1.09 1.37 1.00 1.4 2.12 1.76 0.93 1.22 有机C(%) 0.069 0.081 0.072 0.045 0.033 0.032 0.208 0.036 0.031 0.043 0.214 0.213 0.044 0.033 0.040 0.125 0.076 0.048 0.981 U 1.61 1.16 1.60 1.22 2.42 2.16 6.64 2.93 14.70 260.00 6.97 885.00 19.00 5.60 3.76 2.84 11.60 5.91 4.49 Fe2+/Fe3+ 0.123 0.431 0.072 0.330 0.379 0.794 0.308 0.728 6.070 14.625 0.845 0.566 20.790 7.647 2.328 0.462 7.294 7.750 1.401 K/Na 2.16 2.12 3.31 4.60 4.88 5.86 5.80 αALNa 2.68 2.54 3.88 6.14 6.59 10.06 7.32 CPA 86.40 85.76 90.20 93.57 93.98 94.45 94.55 CIX 73.65 72.80 75.72 79.67 80.12 79.24 79.71 PIA 72.23 71.26 82.61 89.87 90.58 92.69 92.87 CIW 76.48 75.78 85.77 91.60 92.18 94.09 94.19 CIA 66.32 65.48 72.58 78.24 78.80 78.99 79.45 Sc/Th 1.62 1.23 0.68 0.64 0.69 0.96 0.73 样品号 HPL-23 HPL-24 HPL-25 HPL-26 HPL-27 HPL-29 HPL-30 HPL-31 HPL-32 HPL-33 HPL-34 HPL-36 HPL-37 HPL-39 HPL-40 HPL-48 HPL-55 HPL-56 HPL-58 岩性 灰色砂岩 灰色砂岩 灰色砂岩 暗色泥岩 灰色砂岩 红色泥岩 红色砂岩 红色砂岩 红色砂岩 红色砂岩 红色砂岩 红色砂岩 红色泥岩 红色泥岩 红色砂岩 暗色泥岩 红色泥岩 红色泥岩 红色泥岩 深度（m) 636 632 629 625 623 622 616 610 607 604 602 600 594 592 591 590 586 580 578 SiO2(%) 79.98 70.94 77.65 53.67 77.12 65.9 78.08 77.22 77.51 75.16 71.54 74.19 64.68 62.37 73.05 52.94 62.49 63.5 66.39 Al2O3(%) 9.29 13.00 10.68 23.07 11.37 15.10 12.05 11.79 12.26 13.07 13.05 13.24 16.48 16.12 12.98 14.96 16.1 16.21 15.26 TFe2O3(%) 1.34 2.57 1.43 3.75 1.30 4.63 1.32 2.55 1.76 2.54 3.69 2.94 5.34 6.45 2.11 5.8 6.17 6.11 5.42 MgO(%) 0.537 0.379 0.542 1.54 0.492 0.854 0.221 0.22 0.205 0.29 0.62 0.365 0.789 1.02 0.674 1.99 1.01 0.957 0.796 CaO(%) 1.200 2.280 1.200 0.593 1.030 1.430 0.245 0.245 0.200 0.180 1.050 0.213 0.202 0.212 0.795 3.01 0.177 0.173 0.352 Na2O(%) 0.881 1 0.987 1.02 1.25 0.802 1.54 1.52 1.59 1.49 1.38 1.47 1.32 1.36 1.53 1.42 1.43 1.4 1.42 K2O(%) 3.10 3.32 3.36 3.98 3.50 3.00 3.74 3.35 3.61 3.54 3.19 3.36 3.56 3.94 3.56 2.81 3.89 3.84 3.84 MnO(%) 0.035 0.074 0.027 0.021 0.036 0.07 0.008 0.017 0.012 0.011 0.062 0.015 0.018 0.023 0.024 0.073 0.031 0.024 0.018 TiO2(%) 0.183 0.511 0.319 0.918 0.298 0.688 0.323 0.546 0.360 0.507 0.723 0.543 0.721 0.699 0.446 0.566 0.684 0.687 0.632 P2O5(%） 0.050 0.158 0.070 0.160 0.055 0.250 0.082 0.100 0.070 0.095 0.111 0.089 0.146 0.167 0.088 0.128 0.118 0.098 0.071 Sc 13.30 14.00 9.61 9.03 12.40 11.80 12.10 7.53 Th 18.00 12.60 17.90 15.60 11.90 17.10 17.80 14.10 烧失量（%） 3.38 5.71 3.70 11.26 3.45 7.13 2.29 2.35 2.36 3.02 4.55 3.56 6.66 7.62 4.69 16.23 7.81 6.92 5.79 FeO(%) 0.99 0.98 1.05 0.92 0.62 0.77 0.50 0.46 0.34 0.35 0.44 0.36 0.34 0.59 0.47 1.98 0.63 0.58 0.49 有机C(%) 0.046 0.065 0.066 0.536 0.044 0.053 0.059 0.050 0.030 0.052 0.042 0.052 0.039 0.056 0.043 1.850 0.117 0.078 0.084 U 2.01 3.22 2.46 4.06 1.78 3.41 1.77 1.90 1.62 1.78 2.20 2.66 1.99 2.06 1.70 3.05 2.38 2.38 2.46 Fe2+/Fe3+ 4.657 0.739 4.500 0.376 1.134 0.227 0.730 0.252 0.274 0.181 0.153 0.158 0.076 0.113 0.330 0.614 0.128 0.118 0.112 K/Na 4.36 4.18 3.02 3.24 2.21 3.04 3.07 3.02 αAlNa 5.80 4.83 3.20 3.04 2.70 2.89 2.97 2.76 CPA 93.22 91.96 88.36 87.81 86.49 87.25 87.56 86.72 CIX 79.37 76.75 73.20 71.22 73.53 71.01 71.47 70.12 PIA 88.77 83.51 85.20 84.05 73.13 83.23 83.47 79.82 CIW 90.68 86.59 88.26 87.76 77.37 87.06 87.17 84.47 CIA 77.52 72.97 73.13 71.19 66.83 70.88 71.22 68.64 Sc/Th 0.74 1.11 0.54 0.58 1.04 0.69 0.68 0.53 注：TFe2O3（%)表示样品中以Fe2O3形式的全铁总含量；K/Na、αAlNa、CPA、CIX、PIA、CIW和CIA计算公式参照表 2；Sc、Th和U单位为μg/g；HPL-9，HPL-10，HPL-11，HPL-12，HPL-13，HPL-14样品来自含矿层段. 
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表 2 化学风化指数及其计算公式
Table 2. Chemical weathering index and its calculation formula
风化指标 计算公式 参考文献 K/Na (K2O×0.83)/(Na2O×0.74) Guo et al., 2018 aAlNa (Al/Na)样品/(Al/Na)UCC Garzanti et al., 2013 CPA 100×(Al2O3)/(Al2O3+Na2O) Cullers, 2000 CIX 100×(Al2O3)/(Al2O3+Na2O+K2O) Garzanti et al., 2014 PIA 100×(Al2O3－K2O)/(Al2O3+CaO*+Na2O－K2O) Fedo et al., 1995 CIW 100×Al2O3/(Al2O3+CaO*+Na2O) Harnois, 1988 CIA 100×Al2O3/(Al2O3+CaO*+Na2O+K2O) Nesbitt and Young, 1982 注：K/Na和aAlNa式中化学分子式代表质量百分比，其他式中分子式代表摩尔百分比；UCC代表上陆壳；CaO*是指硅酸盐中CaO含量.
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表 3 研究区钻孔HLJ-15姚家组下段碎屑岩U含量、Fe2+/Fe3+和TOC含量
Table 3. Statistical data of U content, Fe2+/Fe3+ and TOC content of clastic rocks in the lower member of Yaojia Formation from Borehole HLJ-15 in the study area
区域 岩性 有机碳含量（%） Fe2+/Fe3+ U（×10-6） 范围 平均值 范围 平均值 范围 平均值 松辽盆地HLJ地区 红色泥岩 0.04~0.13 0.08 0.07~0.46 0.16 1.60~3.41 2.30 红色砂岩 0.03~0.08 0.05 0.15~0.79 0.40 1.16~3.22 1.98 暗色泥岩 0.21~1.85 0.61 0.31~2.56 0.95 3.05~885 131.97 灰色砂岩 0.03~0.08 0.05 0.73~20.79 7.05 1.78~260 29.98 伊犁盆地洪海沟 铀矿石带（砂岩） — 0.58 — 1.59 — 544.26 注：伊犁盆地洪海沟地区数据引自陈奋雄等（2016）.
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