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义马盆地中侏罗世2-3号煤层元素地球化学及沉积环境分析

高迪, 郭慧玲, 王佳慧

高 迪,郭慧玲,王佳慧. 义马盆地中侏罗世2-3号煤层元素地球化学及沉积环境分析[J]. 煤炭科学技术,2023,51(5):174−183

. DOI: 10.13199/j.cnki.cst.2021-1395
引用本文:

高 迪,郭慧玲,王佳慧. 义马盆地中侏罗世2-3号煤层元素地球化学及沉积环境分析[J]. 煤炭科学技术,2023,51(5):174−183

. DOI: 10.13199/j.cnki.cst.2021-1395

GAO Di,GUO Huiling,WANG Jiahui. Geochemical characteristics and sedimentary environment of coal during Middle Jurassic in Yima Basin[J]. Coal Science and Technology,2023,51(5):174−183

. DOI: 10.13199/j.cnki.cst.2021-1395
Citation:

GAO Di,GUO Huiling,WANG Jiahui. Geochemical characteristics and sedimentary environment of coal during Middle Jurassic in Yima Basin[J]. Coal Science and Technology,2023,51(5):174−183

. DOI: 10.13199/j.cnki.cst.2021-1395

义马盆地中侏罗世2-3号煤层元素地球化学及沉积环境分析

基金项目: 

国家自然科学基金资助项目(41402094);油气资源与探测国家实验室开放课题基金资助项目(PRP/open-2008)

详细信息
    作者简介:

    高迪: (1980—),男,河南周口人,副教授,硕士生导师,博士。E-mail:gaodi@hpu.edu.cn

  • 中图分类号: P595

Geochemical characteristics and sedimentary environment of coal during Middle Jurassic in Yima Basin

Funds: 

National Natural Science Foundation of China (41402094); National Laboratory of Petroleum Resources and Exploration (PRP/open-2008)

  • 摘要:

    为研究华北板块西南缘中侏罗世煤层地球化学特征及其沉积环境,以义马盆地中侏罗世义马组2-3号煤层为研究对象,借助X射线荧光光谱仪、等离子体质谱仪等手段,运用地球化学理论和方法,详细研究了煤中地球化学特征及其所反映的沉积环境。研究结果表明:研究区常量元素含量与中国煤相比,SiO2、P2O5和K2O显著偏高,而Al2O3含量较低;微量元素中Cs富集,Sb、Nb、Ta、Zr、Hf亏损;稀土元素整体为轻微富集,δEu负异常,而δCe正异常,表明采样煤层未受岩浆、热液、海水影响,物源主要是陆源碎屑;Th/U、V/ (V+Ni)、Ce异常、Sr/Cu及气候指数分析表明,采样煤层古泥炭堆积于还原环境,成煤期整体处于半干旱气候。

    Abstract:

    In order to study the geochemical characteristics and sedimentary environment of the Middle Jurassic coal seam in the southwestern margin of the North China Plate, taking the coal of Yima Formation in Yima Basin as the research object to study the geochemical characteristics and sedimentary environment of Middle Jurassic coal seams in the southwest margin of the North China plate, based on the data from X-ray fluorescence spectrometer and plasma mass spectrometer. The results show that: The content of major element of SiO2, P2O5 and K2O are significantly higher, while the content of Al2O3 is lower compared with Chinese coals. Enrichment of Cs and deficit of Sb, Nb, Ta, Zr and Hf in trace elements. The rare earth elements are slightly enriched as a whole, with negative Eu anomalies and positive Ce anomalies, indicating that the coal seam was not affected by magma, hydrothermal and seawater, and the provenance is mainly terrigenous clastic. It shows that the coal forming environment in reductive environment, and the whole coal forming period is in semi-arid climate environment by the analysis of Th/U, V/ (V+Ni), Ce anomaly, Sr/Cu and climate index.

  • 煤作为重要的化石能源,在我国能源结构中占据主导地位,随着碳达峰碳中和愿景目标的提出,如何清洁利用煤炭是我们面临的严峻挑战。煤中元素运移特点、富集的物化特性和物源供给的不同,控制着不同成煤区、不同成煤期、不同地质背景下元素富集规律[1-2]。研究区义马组是河南省唯一具有工业价值的中生代煤系,前人开展了部分研究工作。义马盆地是晚太古代结晶基底和元古代—古生代—早中生代褶皱基底之上的中新生代断陷—拗陷盆地[3];认为义马组沉积环境具有冲积扇−湖滨三角洲−半深湖−滨浅湖−半深湖的演化特征[4-5];义马组各煤层分别发育在扇前冲积平原、湖滨三角洲和滨浅湖泊相[6-7];盆地产生于构造活动期,发展于稳定成煤期,结束于活动期,经历了氧化−还原−氧化的环境[8]。前人研究侧重于沉积环境及构造演化、成煤机制等,煤层元素地球化学特征及其所反映的沉积环境研究工作尚未见到公开报道。

    义马煤田位于河南省西部,东西长25 km,南北宽2.5~11 km,面积约150 km2[5, 7]。构造上位于华北板块西南缘,东秦岭—大别山构造带北缘,是在华北地台基础之上发育起来的中新生代叠合盆地[9]图1a)。古生代古秦岭洋俯冲消减,华北古板块和扬子古板块碰撞形成以近东西向构造,中新生代特提斯洋俯冲、消减,印度板块与欧亚板块碰撞和太平洋板块俯冲对盆地复杂大地构造背景具有深远影响[3],中生代时期盆地物源区主要为南侧的秦岭−大别山造山带[10]。义马盆地整体处于渑池向斜的轴部,发育在被岸上断层、扣门山断层和硖石−义马断层控制的渑池义马断块之上(图1b)。

    图  1  研究区构造位置和义马组地层柱状图[11-12]
    Figure  1.  Tectonic location map of Yima Basin and stratigraphic histogram of Yima Formation[11-12]

    研究区主要发育三叠系、侏罗系、白垩系、古近系、新近系和第四系地层,中侏罗世义马组2-3号煤是主采煤层(图1c),煤厚0.24~14.08 m,平均7.73 m。

    选取义马盆地东北部北露天矿中侏罗世义马组2-3号煤层,从底至顶按20 cm的间隔采集31块煤样(编号为BLT1~BLT31)。煤样采取严格按照GB/T482—2008执行,样品采集后立刻放入密封袋中。主量元素测试方法依据《GB/T 14506.14—2010 硅酸盐岩石学化学分析方法 第14部分:氧化亚铁量测定》和《GB/T 14506.28—2010 硅酸盐岩石学化学分析方法第28部分:16个主次成分测定》,测试仪器采用荷兰生产的Axios mAX X射线荧光光谱仪。微量元素和稀土元素测试方法依据《GB/T 14506.30—2010 硅酸盐岩石化学分析方法 第30部分:44个元素量测定》,测试仪器采用美国Thermo Fisher公司生产的Element XR等离子体质谱仪。以上分析测试均在核工业地质分析测试研究中心完成。测试及计算结果见表1(微量元素)、表2(常量元素)、表3(稀土元素)。

    表  1  义马盆地中侏罗世煤样微量元素分析结果
    Table  1.  Content of trace elements in middle Jurassic coal from Yima Basin
    项目含量/(μg·g−1
    LiBeScVCrCoNiCuZnGaRbSrMoCdInSbCsBaWReT1PbBiThUNbTaZrHfSr/CuTh/UV/(V+Ni)
    BLT-197.504.40019.534717144.389.749.917227.411571.11.440.2450.090.10810.61370.0540.0030.66313.70.2628.231.20.1920.0074.430.1481.426.860.79
    BLT-216.002.8806.2835.721.61014.614.225.17.6232.33113.640.2340.0320.1184.051160.7720.0032.377.640.1072.571.530.180.0055.490.17821.901.680.71
    BLT-335.602.3606.433621.814.71714.210510.940.23472.90.260.0340.1475.101640.3130.0031.1415.90.2268.13.030.2190.00415.80.47424.442.670.68
    BLT-410.702.2705.8126.423.28.3912.111.612.66.2631.83813.590.2260.0250.1644.762951.10.0050.3924.990.0941.970.8060.2940.0046.770.1932.842.440.69
    BLT-561.804.79016.614962.217.440.915.326.314.21643982.630.1150.0670.03821.12310.1910.0033.114.90.2026.552.110.0680.0056.60.17126.013.100.78
    BLT-610.103.4406.0821426.614.435.49.5733.75.9631.34074.760.1450.0150.083.351321.59<0.0021.992.950.051.490.5650.1740.0034.540.12242.532.640.86
    BLT-760.905.81015.910356.219.346.519.131.813.31266102.330.1420.0650.03719.410460.0920.0022.315.50.2377.022.440.0540.00590.29431.942.880.69
    BLT-819.805.45010.147.832.94.858.9312.610.28.9640.341762.560.0740.0580.0426.139890.4450.0070.30635.20.2675.461.110.1210.00813.60.484331.434.920.84
    BLT-97.231.0403.8929.715.95.88.518.68.674.61211972.940.0630.0160.0991.963770.8940.0030.1291400.4651.230.5550.280.0094.940.177139.192.220.78
    BLT-107.371.2004.2428.317.34.648.38.698.044.2367763.250.0290.0210.0983.963080.9120.0030.2214.850.0731.720.6940.3440.0057.110.23989.302.480.77
    BLT-113.141.3203.0818.512.24.67.756.719.33.5225.36584.560.0690.0130.0583.173620.810.0030.2182.770.0651.180.4460.2460.0045.930.17498.062.650.70
    BLT-1241.605.07015.112056.934.581.820.262.913.265.68754.250.1930.0740.1357.953380.2350.0033.6623.90.2275.732.550.1580.005170.49843.322.250.59
    BLT-1326.503.79011.866.143.324.441.618.912613.582.912845.550.2950.0550.19910.94730.6550.0041.5833.60.2674.522.240.2950.00515.50.48667.942.020.61
    BLT-1410.704.59013.289.333.340.778.81926.21446.815455.410.260.0340.346.175831.2<0.0025.539.370.1622.653.30.7620.00716.60.48781.320.800.53
    BLT-1519.005.17014.133150.95.6711.215.610.512.842.813953.30.0790.030.1865.744840.7610.0040.1995.280.092.351.390.3410.00411.70.32189.421.690.97
    BLT-167.623.1709.251423730.4711634.71019.99917.280.3340.0440.3412.964021.440.0030.6327.830.0981.982.860.6110.00615.20.47761.940.690.67
    BLT-1727.105.35014.482.341.56.61161720.312.732.232323.210.1330.050.1014.4112610.2750.0040.83611.90.1793.751.770.2350.00614.20.452190.122.120.84
    BLT-1812.202.3504.1444.314.65.098.610.310.64.1512.46675.350.0780.0150.1222.663031.090.0030.0972.40.0440.9950.6160.3940.0055.470.16464.761.620.84
    BLT-1915.801.9303.6322922.35.7924.39.414.22.8110.38624.290.1090.0090.1671.403081.050.0080.05616.20.070.5240.5750.5520.0153.840.10791.700.910.90
    BLT-2018.602.48012.1147431356.112.912.914.627.86774.930.1040.0330.2684.363021.060.0021.2411.80.1023.234.120.5530.00716.20.48352.480.780.72
    BLT-2147.103.46011.924360.119.127.322.320.214.778.513312.930.1160.0540.12610.38310.4150.0020.98112.20.2134.772.290.2920.00320.40.56959.692.080.90
    BLT-2232.005.08010.227446.16.3911.411.810.29.3347.315913.040.0940.0250.0776.829180.6530.0030.4386.380.0822.31.070.1530.0058.820.244134.832.150.96
    BLT-2328.806.55021.73787918.623.8195823.341.47815.470.2820.0380.3425.143351.18<0.0020.8479.840.1113.584.410.5910.00525.90.65841.110.810.94
    BLT-24193.006.78022.111483.811.232.626.255.930.32016902.040.1030.1490.02923.73990.0460.0032.1829.60.4215.32.120.0560.00511.70.36126.347.220.78
    BLT-2541.6012.7003021691.39.7616.423.519.91722.11 86111.90.1460.0890.3762.7810130.6390.0030.573260.236.844.510.4990.00624.30.63879.191.520.93
    BLT-2688.803.65013.411359.69.3521.519.636.323.11688752.260.1760.1050.05619.44320.1920.0021.4925.50.38211.31.430.0320.00410.50.31844.647.900.84
    BLT-2732.907.89026.95831125.9518.210.549.827.140.41 4224.160.0660.0360.4994.277811.720.0030.3124.220.0493.962.570.4970.0048.470.221135.431.540.97
    BLT-2814.007.82016.825453.631.333.716.612320.833.12 1347.790.2150.0420.2953.4910240.8510.0030.810.80.1543.326.080.540.00818.90.557128.550.550.88
    BLT-2941.209.62019.390.566.59.0116.518.218.614.46915712.640.0790.0770.0359.168920.1220.0040.93922.40.2297.772.350.120.0088.530.28786.323.310.85
    BLT-30107.006.81017.919172.58.7721.235.513727.81953080.9150.2830.1440.06222680.057<0.0021.8827.30.40313.92.990.0660.0068.60.258.684.650.90
    BLT-3137.603.60014.958.451.58.8519.820.375.620.41432132.140.0720.0880.0416.31880.047<0.0021.5324.10.33510.92.770.0480.017.210.26310.493.940.75
    均值37.854.6112.93154.8850.9614.6129.7317.2044.0513.9665.601085.073.980.160.050.158.18506.190.67<0.0031.2518.680.195.012.150.290.0111.400.3475.402.680.79
    地壳23.01.7316.0143.0127.024.781.356.076.316.7108.0382.01.430.1770.0970.511.23463.01.130.7314.00.197.62.0718.31.6148.04.5
    中国煤值31.802.114.3835.1015.407.0813.7017.5041.406.559.25140.003.080.250.050.841.13159.001.080.4715.100.795.482.439.440.6289.503.71
    世界煤值12.001.603.9025.0016.005.1013.0016.0023.005.8014.00110.002.200.220.030.921.00150.001.100.637.800.973.302.403.700.2836.001.20
    中国J-K煤5.002.403.0013.0012.008.0011.009.0033.004.007.0079.002.000.100.901.80150.001.900.409.000.304.002.008.000.5039.001.00
    富集系数(R11.192.182.954.413.312.062.170.981.062.137.097.751.290.641.000.187.243.180.622.661.240.240.910.880.030.020.130.09
    富集系数(R23.152.883.326.203.192.862.291.081.922.414.699.861.810.731.670.168.183.370.611.982.390.201.520.900.080.040.320.28
    富集系数(R37.571.924.3111.914.251.832.701.911.333.499.3713.741.991.600.174.543.370.353.132.080.631.251.080.040.020.290.34
    富集系数(R41.652.660.811.080.400.590.370.310.580.840.612.842.780.900.520.296.651.090.591.711.331.000.661.040.020.010.080.08
    富集系数(EF2.043.301.001.340.500.730.450.380.711.030.753.513.441.120.640.368.231.350.732.121.651.240.821.290.020.010.100.09
    注: “—” 表示无数据;中国煤及世界煤数据据文献[13,17],中国J-K煤数据据来自文献[18],地壳数据据文献[19];EF=(Cx/CSc)e/(Cx/CSc)dCx为煤中某种元素平均含量值;CSc为煤中钪元素平均含量值;C'x为地壳中某元素平均含量值;C'Sc为地壳中钪元素平均含量值。
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    表  2  义马盆地中侏罗世煤样常量元素分析结果
    Table  2.  Content of major elements in middle Jurassic coal from Yima Basin %
    样品编号
    12345678910111213141516171819202122232425262728293031平均值中国煤
    SiO262.935.3910.985.8629.563.9229.8711.763.544.463.4916.3816.056.407.103.558.782.621.183.959.958.425.3648.466.2055.096.565.1818.1854.5567.3716.878.47
    Al2O315.242.655.361.6710.241.4810.394.541.461.551.185.415.232.092.481.354.230.910.491.894.523.712.4118.703.4217.493.282.386.4518.0716.635.715.98
    Fe2O39.502.121.960.993.913.452.740.482.450.710.923.602.413.820.641.510.791.3835.151.962.451.111.392.751.052.301.122.451.637.462.943.464.85
    MgO2.690.420.480.450.710.280.930.650.480.450.410.630.610.530.530.460.590.461.170.440.550.570.510.870.600.660.500.550.750.910.770.660.22
    CaO1.701.271.220.990.941.191.031.801.191.000.911.171.061.201.171.011.380.919.590.940.910.980.890.531.320.472.431.361.330.410.191.371.23
    Na2O0.160.080.270.100.170.090.160.100.130.080.100.110.090.090.080.080.100.100.080.090.140.140.100.150.100.150.110.090.110.160.180.120.16
    K2O2.580.190.260.211.390.151.260.030.130.180.140.530.750.240.230.120.210.080.050.170.430.380.232.090.152.450.270.180.553.474.680.770.19
    MnO0.070.010.010.020.010.010.010.010.020<0.00400.0100.010<0.00400.2000.010.01000.010.010.010.010.010.020.020.020.015
    TiO20.970.080.140.090.430.070.470.230.070.090.070.290.290.130.140.090.170.060.030.080.150.130.110.760.110.780.100.100.330.830.850.270.33
    P2O50.130.020.040.020.030.080.040.920.280.140.070.070.270.280.280.160.760.060.080.030.090.250.070.130.300.260.200.370.230.100.060.190.092
    SiO2/Al2O34.132.032.053.512.892.652.872.592.422.882.963.033.073.062.862.632.082.892.432.092.202.272.222.591.813.152.002.182.823.024.052.691.42
    注:中国煤数据据来自文献[13],BLT代表北露天矿。
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    表  3  义马盆地中侏罗世煤样稀土元素分析结果
    Table  3.  Content of rare earth elements in middle Jurassic coal from Yima Basin ug/g
    项目含量/(μg·g−1
    LaCePrNdSmEuGdTbDyHoErTmYbLuY∑REYδCeδEu(La/Yb)N(La/Sm)N(Gd/Yb)N
    BLT-133.560.57.4428.75.361.074.650.7563.420.5941.460.2151.20.15433.9149.020.920.6618.823.933.13
    BLT-29.5418.427.861.480.2821.290.2161.160.2290.6040.1030.6540.08814.143.911.010.629.834.051.59
    BLT-311.623.12.549.51.730.3331.490.2491.210.2270.6110.10.5920.08213.553.361.020.6313.214.222.03
    BLT-46.8913.61.626.531.340.3161.190.2141.170.2240.6080.1060.6520.09113.234.550.980.777.123.231.47
    BLT-530.760.36.8626.74.740.8673.80.62.680.4661.250.1921.130.14926.2140.431.000.6218.324.072.71
    BLT-66.12131.576.741.470.3191.440.2671.480.2880.7610.1230.7450.10218.734.431.010.675.542.621.56
    BLT-730.663.37.2928.65.081.144.170.6773.090.5381.370.2091.220.15730.7147.441.020.7616.913.792.76
    BLT-817.2344.0617.94.110.9423.360.58630.5231.290.1861.050.13830.888.350.980.7811.042.632.58
    BLT-95.110.81.315.550.9790.2580.8560.1490.7470.1410.3870.0660.3940.0558.9526.791.010.868.733.281.75
    BLT-103.919.471.346.361.210.2871.010.180.9280.1770.4710.0780.4760.06311.025.961.000.795.542.031.71
    BLT-114.319.331.084.390.970.2640.870.1540.8550.1620.4450.0750.4550.06210.723.421.040.886.392.791.54
    BLT-1215.928.13.1512.52.720.5712.330.4312.260.4161.10.1791.060.14424.270.860.960.6910.113.681.77
    BLT-1327.859.16.6124.44.170.8233.640.5672.630.4651.20.1861.130.14725.0132.871.050.6516.594.192.60
    BLT-1425.758.16.5324.14.020.8363.730.6033.020.5391.410.2181.350.16928.6130.331.080.6612.834.022.23
    BLT-1520.444.74.9418.13.210.6912.890.4842.360.4211.060.1731.030.1325.4100.591.070.6913.354.002.26
    BLT-166.6414.41.798.431.880.4531.580.2991.660.3160.830.1370.8350.11118.839.361.010.805.362.221.53
    BLT-1766.512812.543.46.941.436.150.8613.660.5571.420.1811.060.13530.3272.791.070.6742.306.034.68
    BLT-182.726.630.9434.180.8470.2350.8280.1640.9310.190.5190.0880.5430.07511.818.891.000.863.382.021.23
    BLT-194.3710.21.134.190.7670.2030.7230.1350.6610.1250.3360.0570.3440.0478.8123.291.000.838.563.581.70
    BLT-204.549.381.064.191.160.3061.100.2421.490.3060.8410.1520.9570.13416.125.861.030.833.202.460.93
    BLT-2114.125.82.8110.21.940.531.760.3031.60.3050.8330.140.8530.11717.261.290.990.8811.144.571.66
    BLT-2216.735.94.518.83.590.8493.060.5062.410.431.090.1710.9950.12926.689.131.000.7811.322.932.48
    BLT-238.7220.12.278.712.070.5072.050.4352.520.51.320.231.390.18929.251.011.090.754.232.651.19
    BLT-2442.277.79.0934.96.261.134.790.7583.310.5661.480.2151.290.15730.4183.850.950.6322.064.243.00
    BLT-2543.7859.1933.15.111.124.720.7733.620.6441.660.2551.520.19637.6190.611.020.7019.385.382.51
    BLT-2646.483.39.435.16.041.084.780.7162.990.491.210.1650.9940.1226.5192.790.960.6131.474.833.88
    BLT-2713.827.23.1112.12.310.5992.060.3852.060.3871.080.1811.150.15923.566.581.000.848.093.761.45
    BLT-2861.81231344.96.91.356.230.8813.820.6461.660.2491.490.19934.5266.131.040.6327.965.633.37
    BLT-2938.778.58.230.35.611.154.780.7833.850.6931.810.2831.670.22637176.561.060.6815.624.342.31
    BLT-3058.110712.447.48.321.57.041.084.520.731.840.2531.490.19143.1251.860.960.6026.294.393.81
    BLT-3152.795.211.141.36.851.185.500.8083.30.541.350.1811.030.12627.5221.170.950.5934.504.844.31
    均值23.5846.235.1919.653.520.733.030.492.340.411.070.170.990.1323.67149.021.010.7214.493.762.31
    中国煤22.5046.706.4222.304.070.844.650.623.7418.200.961.790.640.382.08136.00
    世界煤11.0023.003.5012.002.000.472.700.322.108.400.540.930.310.201.0068.47
    富集系数(CC)2.142.011.481.971.761.551.121.531.110.0491.980.183.190.6523.672.18
    注:中国煤数据与世界煤数据来源于文献[13],$\delta \text{Ce}\text{=}{\text{Ce}}_{\text{N}}/\sqrt{{\text{La}}_{\text{N}}\text{×}{\text{Pr}}_{\text{N}}} $,CeN、LaN、PrN为Ce、La、Pr元素球粒陨石标准化值;$\delta \text{Eu}\text{=}{\text{Eu} }_{\text{N} }/\sqrt{ {\text{Sm} }_{\text{N} }\text{×}{\text{Gd} }_{\text{N} } }$,EuN、SmN、GdN为元素球粒陨石标准化值[20];球粒陨石数据据文献[21];富集系数(CC)为样品中稀土元素含量/世界煤中稀土元素含量;“—” 为无数据。
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    煤样常量元素SiO2和P2O5平均含量是中国煤的1.99倍,K2O含量为4.03倍;SiO2/Al2O3值是中国煤[13]的1.9倍,高岭石(1.18)[14-15]的2.3倍;其余值整体和中国煤相当(表2)。常量元素中SiO2占主导地位,Al2O3含量仅为中国煤的95%,和Si含量不具有一致性。

    煤样微量元素含量相对于中国煤、世界煤、中国侏罗−白垩纪煤、地壳丰度的比值(R1R2R3R4)见表1。其中,比值>2表示富集,介于0.5 ~ 2表示正常含量,小于0.5表示贫化[16]。同时,煤以有机质为主,无机质含量低。因此,选择地壳中化学性质稳定的Sc元素作为基准计算富集系数(FE),FE>10为强烈富集,FE>5为富集,0.5< FE<5为正常,FE< 0.5为亏损[16]

    结果显示(表2图2),研究所用煤样与中国煤相比(R1),Be、Sc、V、Cr、Co、Ni、Ga、Rb、Sr、Cs、Ba、Tl为富集;与世界煤(R2)和中国侏罗煤(R3)相比,Li、Sc、V、Cr、Ga、Rb、Sr、Cs、Ba为富集,且后者比值整体偏大。与Sc元素相比,EF值大于5 的只有Cs元素。同时按照GLUSKOTER等提出的煤中微量元素高于地壳克拉克值6倍以上为富集的原则(R4[22-23],也只有Cs元素。

    图  2  煤样稀土元素富集系数
    Figure  2.  Histogram of REE enrichment on coal samples

    煤中Cs常与黏土矿物、云母和长石等富钾矿物结合,与常量元素中K异常富集具有一致性[18]。在所有富集系数中,Sb、Nb、Ta、Zr、Hf值均远小于0.5,属于亏损元素。Nb和Ta属于强的亲氧元素,常赋存于角闪石、黑云母等含钽矿物中;Hf赋存在锆矿物中,和Zr具有一致性,本次研究两元素同样含量较低;Sb属于亲铜元素,常来源于热液[18]

    综合分析富集元素和亏损元素分布情况,研究区煤层未受岩浆、热液影响。

    研究煤样稀土元素(REY)总体含量整体较高,介于1.09 ~ 272.79 μg/g,均值为149.02 μg/g,略大于中国煤均值[13],为世界煤[13]均值的2.18倍(表3)。稀土元素总量富集系数为1.10,表明整体为轻微富集。其中,Y(CC=23.67)十分富集,La(CC=2.14)、Ce(CC=2.01)轻微富集,Ho(CC=0.049)、Tm(CC=0.18)显著亏损,其余元素均接近世界煤均值。

    对煤样稀土元素测值进行标准化处理,并绘制配分曲线(图3)。结果表明,除样品BLT-31之外,其他样品稀土元素的分布模式相近,整体呈左高右低的“V”型曲线,轻稀土较为富集,重稀土相对亏损。煤样(La/Yb)N范围为3.20~42.30,均值为14.49,说明轻、重稀土元素整体分异程度较高;(La/Sm)N范围为2.02~6.03(均值3.76),(Gd/Yb)N范围为0.93~4.68(均值2.31),说明轻、重稀土均较为富集。

    图  3  煤样稀土元素分布曲线
    Figure  3.  Curves of REE distribution on coal samples

    一般情况下,δEu负异常是由陆源碎屑继承而来[24]。煤样δEu范围为0.59~0.88,均值为0.72,整体呈现出显著负Eu异常,表明采样煤层沉积期物源来自于陆源碎屑。一般δCe负异常为海相环境[18, 25],煤样δCe范围为0.92~1.09,均值为1.01,呈现出正Ce异常,表明古泥炭沼泽未受海水影响,即陆相沉积。

    鉴于微量元素和稀土元素的良好稳定性,常被作为物源的指示剂,以及用来研究沉积环境[24]。但是煤内的微量元素富集受各种因素的影响,只有具有沉积成因的微量元素才可以进行沉积环境分析[26]

    Th和U在还原状态下化学性质相似,但在氧化环境下有较大差别[27]。在陆表环境下Th为+4价,十分稳定,不易溶解。U在强还原环境下为+4价,在沉积物中富集;强氧化环境下为+6价,极易溶解,导致沉积物中U减少。一般认为,ωTh/ωU值为0~2时,表现为贫氧环境,达到8时为强氧化环境[28]。煤样Th/U比变化在0.55~7.9(图4),均值为2.68,整体为弱还原环境。

    图  4  煤样地化特征反映的泥炭沼泽介质氧化还原环境演化
    Figure  4.  Evolution of redox environment of peat swamp reflected by geochemical characteristics of coal samples

    Ni在还原状态和碱性条件下易于富集,V在缺氧状态下以有机络合物形式沉淀[29]ωV/ω(V+Ni)>0.84时,为水体分层强的厌氧环境;比值处于0.6~0.84时,水体分层较弱的厌氧环境;比值处于0.46~0.60时,水体分层弱的贫氧环境[30-31]。煤样V/(V+Ni)范围为0.53~0.97,多数样品在0.53~0.85,均值0.79,反映采样煤层沉积期可能处于水体分层较弱的厌氧环境。

    Elderfield等提出的Ce异常参数Ceanom也广泛用来判别古氧化还原条件[32]

    $$ \text{}{\text{Ce}}_{\text{anom}}\text={\text{lg{3}\text{Ce}}_{\text{N}}/\text{(2}{\text{La}}_{\text{N}}\text+{\text{Nd}}_{\text{N}}\text{)}} $$

    式中,N为稀土元素的北美页岩标准化值。Ceanom>−0.1时,指示还原环境;Ceanom<−0.1时,指示氧化环境。煤样Ceanom介于−0.07~0.02,平均−0.03,均大于−0.1,指示其为还原环境,CeN、LaN、NdN分别代表本论文Ce、La、Nd测试的数据与北美页岩该元素标准值的比值。

    从地化特征分析,采样煤层古泥炭沼泽经历了3阶段氧化还原环境演化(图4)。

    根据已有研究成果,喜湿型元素有Cr、Ni、Mn、Cu、Co、Cs、Hf等,喜干型元素有B、Mo、Mg、Zn、Na、Ca等,而喜干型元素Sr与喜湿型元素Cu之间的比值更能指示温暖潮湿的气候和炎热干燥的气候[33-34]ωSr/ωCu的比值为1~10时指示温暖潮湿气候,比值大于10时指示炎热干燥气候[35-36]。研究区煤层中ωSr/ωCu的变化范围基本在30~200,只有少量样品在1~10(图5),平均值为75.4,表明义马盆地成煤时处于炎热干燥的气候。

    图  5  煤样地化特征反映的古气候环境演化
    Figure  5.  Evolution of palaeoclimate environment reflected by geochemical characteristics of coal samples

    赵增义等[37]提出了气候指数C值:

    $$ \begin{split} {{C}}=& \sum\omega({\rm{Fe}}+{\rm{Mn}}+{\rm{Cr}}+{\rm{Ni}}+{\rm{V}}+{\rm{Co}})/ \\ &\sum\omega({\rm{Ca}}+{\rm{Mg}}+{\rm{Sr}}+{\rm{Ba}}+{\rm{K}}+{\rm{Na}}) \end{split} $$

    C值与气候的对应关系为:0~0.2干旱,0.2~0.4半干旱,0.4~0.6半干旱−半潮湿,0.6~0.8半潮湿,0.8~1潮湿。煤样C值介于0.02~3.07,平均0.31,整体处于半干旱的气候环境,从地化特征分析,采样煤层沉积期经历多期次小规模的气候变化(图5)。

    中侏罗世早期,我国古气候具有明显的分带性,北方以温暖潮湿气候为主,如吐哈盆地、塔里木盆地、柴达木盆地及鄂尔多斯盆地[38-39],东南部以半干旱−半潮湿为主,如四川盆地北部、合肥盆地等[39],西南为干旱气候区,如羌塘盆地、昌都盆地等[39-40],研究结果与前人基本一致。

    1)义马盆地中侏罗世煤常量元素含量与中国煤相比,SiO2和P2O5平均含量是中国煤的1.99倍,K2O含量为4.03倍,而Al2O3含量仅为中国煤的95%,和Si含量不具有一致性。

    2)微量元素中Cs富集,Sb、Nb、Ta、Zr、Hf亏损,表明研究区煤层未受岩浆、热液影响;稀土元素整体为轻微富集,δEu负异常,而δCe正异常,表明研究区物源主要来自于陆源碎屑,且成煤期未受海水影响。

    3)通过ωTh/ωUωV/ω(V+Ni)及Ceanom分析表明,研究区成煤期处于还原环境,且经历了3次大的氧化还原环境的演化过程;Sr/Cu和气候指数分析表明,研究区成煤期整体处于半干旱的环境,且经历了多期次的小规模的气候变迁过程。

  • 图  1   研究区构造位置和义马组地层柱状图[11-12]

    Figure  1.   Tectonic location map of Yima Basin and stratigraphic histogram of Yima Formation[11-12]

    图  2   煤样稀土元素富集系数

    Figure  2.   Histogram of REE enrichment on coal samples

    图  3   煤样稀土元素分布曲线

    Figure  3.   Curves of REE distribution on coal samples

    图  4   煤样地化特征反映的泥炭沼泽介质氧化还原环境演化

    Figure  4.   Evolution of redox environment of peat swamp reflected by geochemical characteristics of coal samples

    图  5   煤样地化特征反映的古气候环境演化

    Figure  5.   Evolution of palaeoclimate environment reflected by geochemical characteristics of coal samples

    表  1   义马盆地中侏罗世煤样微量元素分析结果

    Table  1   Content of trace elements in middle Jurassic coal from Yima Basin

    项目含量/(μg·g−1
    LiBeScVCrCoNiCuZnGaRbSrMoCdInSbCsBaWReT1PbBiThUNbTaZrHfSr/CuTh/UV/(V+Ni)
    BLT-197.504.40019.534717144.389.749.917227.411571.11.440.2450.090.10810.61370.0540.0030.66313.70.2628.231.20.1920.0074.430.1481.426.860.79
    BLT-216.002.8806.2835.721.61014.614.225.17.6232.33113.640.2340.0320.1184.051160.7720.0032.377.640.1072.571.530.180.0055.490.17821.901.680.71
    BLT-335.602.3606.433621.814.71714.210510.940.23472.90.260.0340.1475.101640.3130.0031.1415.90.2268.13.030.2190.00415.80.47424.442.670.68
    BLT-410.702.2705.8126.423.28.3912.111.612.66.2631.83813.590.2260.0250.1644.762951.10.0050.3924.990.0941.970.8060.2940.0046.770.1932.842.440.69
    BLT-561.804.79016.614962.217.440.915.326.314.21643982.630.1150.0670.03821.12310.1910.0033.114.90.2026.552.110.0680.0056.60.17126.013.100.78
    BLT-610.103.4406.0821426.614.435.49.5733.75.9631.34074.760.1450.0150.083.351321.59<0.0021.992.950.051.490.5650.1740.0034.540.12242.532.640.86
    BLT-760.905.81015.910356.219.346.519.131.813.31266102.330.1420.0650.03719.410460.0920.0022.315.50.2377.022.440.0540.00590.29431.942.880.69
    BLT-819.805.45010.147.832.94.858.9312.610.28.9640.341762.560.0740.0580.0426.139890.4450.0070.30635.20.2675.461.110.1210.00813.60.484331.434.920.84
    BLT-97.231.0403.8929.715.95.88.518.68.674.61211972.940.0630.0160.0991.963770.8940.0030.1291400.4651.230.5550.280.0094.940.177139.192.220.78
    BLT-107.371.2004.2428.317.34.648.38.698.044.2367763.250.0290.0210.0983.963080.9120.0030.2214.850.0731.720.6940.3440.0057.110.23989.302.480.77
    BLT-113.141.3203.0818.512.24.67.756.719.33.5225.36584.560.0690.0130.0583.173620.810.0030.2182.770.0651.180.4460.2460.0045.930.17498.062.650.70
    BLT-1241.605.07015.112056.934.581.820.262.913.265.68754.250.1930.0740.1357.953380.2350.0033.6623.90.2275.732.550.1580.005170.49843.322.250.59
    BLT-1326.503.79011.866.143.324.441.618.912613.582.912845.550.2950.0550.19910.94730.6550.0041.5833.60.2674.522.240.2950.00515.50.48667.942.020.61
    BLT-1410.704.59013.289.333.340.778.81926.21446.815455.410.260.0340.346.175831.2<0.0025.539.370.1622.653.30.7620.00716.60.48781.320.800.53
    BLT-1519.005.17014.133150.95.6711.215.610.512.842.813953.30.0790.030.1865.744840.7610.0040.1995.280.092.351.390.3410.00411.70.32189.421.690.97
    BLT-167.623.1709.251423730.4711634.71019.99917.280.3340.0440.3412.964021.440.0030.6327.830.0981.982.860.6110.00615.20.47761.940.690.67
    BLT-1727.105.35014.482.341.56.61161720.312.732.232323.210.1330.050.1014.4112610.2750.0040.83611.90.1793.751.770.2350.00614.20.452190.122.120.84
    BLT-1812.202.3504.1444.314.65.098.610.310.64.1512.46675.350.0780.0150.1222.663031.090.0030.0972.40.0440.9950.6160.3940.0055.470.16464.761.620.84
    BLT-1915.801.9303.6322922.35.7924.39.414.22.8110.38624.290.1090.0090.1671.403081.050.0080.05616.20.070.5240.5750.5520.0153.840.10791.700.910.90
    BLT-2018.602.48012.1147431356.112.912.914.627.86774.930.1040.0330.2684.363021.060.0021.2411.80.1023.234.120.5530.00716.20.48352.480.780.72
    BLT-2147.103.46011.924360.119.127.322.320.214.778.513312.930.1160.0540.12610.38310.4150.0020.98112.20.2134.772.290.2920.00320.40.56959.692.080.90
    BLT-2232.005.08010.227446.16.3911.411.810.29.3347.315913.040.0940.0250.0776.829180.6530.0030.4386.380.0822.31.070.1530.0058.820.244134.832.150.96
    BLT-2328.806.55021.73787918.623.8195823.341.47815.470.2820.0380.3425.143351.18<0.0020.8479.840.1113.584.410.5910.00525.90.65841.110.810.94
    BLT-24193.006.78022.111483.811.232.626.255.930.32016902.040.1030.1490.02923.73990.0460.0032.1829.60.4215.32.120.0560.00511.70.36126.347.220.78
    BLT-2541.6012.7003021691.39.7616.423.519.91722.11 86111.90.1460.0890.3762.7810130.6390.0030.573260.236.844.510.4990.00624.30.63879.191.520.93
    BLT-2688.803.65013.411359.69.3521.519.636.323.11688752.260.1760.1050.05619.44320.1920.0021.4925.50.38211.31.430.0320.00410.50.31844.647.900.84
    BLT-2732.907.89026.95831125.9518.210.549.827.140.41 4224.160.0660.0360.4994.277811.720.0030.3124.220.0493.962.570.4970.0048.470.221135.431.540.97
    BLT-2814.007.82016.825453.631.333.716.612320.833.12 1347.790.2150.0420.2953.4910240.8510.0030.810.80.1543.326.080.540.00818.90.557128.550.550.88
    BLT-2941.209.62019.390.566.59.0116.518.218.614.46915712.640.0790.0770.0359.168920.1220.0040.93922.40.2297.772.350.120.0088.530.28786.323.310.85
    BLT-30107.006.81017.919172.58.7721.235.513727.81953080.9150.2830.1440.06222680.057<0.0021.8827.30.40313.92.990.0660.0068.60.258.684.650.90
    BLT-3137.603.60014.958.451.58.8519.820.375.620.41432132.140.0720.0880.0416.31880.047<0.0021.5324.10.33510.92.770.0480.017.210.26310.493.940.75
    均值37.854.6112.93154.8850.9614.6129.7317.2044.0513.9665.601085.073.980.160.050.158.18506.190.67<0.0031.2518.680.195.012.150.290.0111.400.3475.402.680.79
    地壳23.01.7316.0143.0127.024.781.356.076.316.7108.0382.01.430.1770.0970.511.23463.01.130.7314.00.197.62.0718.31.6148.04.5
    中国煤值31.802.114.3835.1015.407.0813.7017.5041.406.559.25140.003.080.250.050.841.13159.001.080.4715.100.795.482.439.440.6289.503.71
    世界煤值12.001.603.9025.0016.005.1013.0016.0023.005.8014.00110.002.200.220.030.921.00150.001.100.637.800.973.302.403.700.2836.001.20
    中国J-K煤5.002.403.0013.0012.008.0011.009.0033.004.007.0079.002.000.100.901.80150.001.900.409.000.304.002.008.000.5039.001.00
    富集系数(R11.192.182.954.413.312.062.170.981.062.137.097.751.290.641.000.187.243.180.622.661.240.240.910.880.030.020.130.09
    富集系数(R23.152.883.326.203.192.862.291.081.922.414.699.861.810.731.670.168.183.370.611.982.390.201.520.900.080.040.320.28
    富集系数(R37.571.924.3111.914.251.832.701.911.333.499.3713.741.991.600.174.543.370.353.132.080.631.251.080.040.020.290.34
    富集系数(R41.652.660.811.080.400.590.370.310.580.840.612.842.780.900.520.296.651.090.591.711.331.000.661.040.020.010.080.08
    富集系数(EF2.043.301.001.340.500.730.450.380.711.030.753.513.441.120.640.368.231.350.732.121.651.240.821.290.020.010.100.09
    注: “—” 表示无数据;中国煤及世界煤数据据文献[13,17],中国J-K煤数据据来自文献[18],地壳数据据文献[19];EF=(Cx/CSc)e/(Cx/CSc)dCx为煤中某种元素平均含量值;CSc为煤中钪元素平均含量值;C'x为地壳中某元素平均含量值;C'Sc为地壳中钪元素平均含量值。
    下载: 导出CSV

    表  2   义马盆地中侏罗世煤样常量元素分析结果

    Table  2   Content of major elements in middle Jurassic coal from Yima Basin %

    样品编号
    12345678910111213141516171819202122232425262728293031平均值中国煤
    SiO262.935.3910.985.8629.563.9229.8711.763.544.463.4916.3816.056.407.103.558.782.621.183.959.958.425.3648.466.2055.096.565.1818.1854.5567.3716.878.47
    Al2O315.242.655.361.6710.241.4810.394.541.461.551.185.415.232.092.481.354.230.910.491.894.523.712.4118.703.4217.493.282.386.4518.0716.635.715.98
    Fe2O39.502.121.960.993.913.452.740.482.450.710.923.602.413.820.641.510.791.3835.151.962.451.111.392.751.052.301.122.451.637.462.943.464.85
    MgO2.690.420.480.450.710.280.930.650.480.450.410.630.610.530.530.460.590.461.170.440.550.570.510.870.600.660.500.550.750.910.770.660.22
    CaO1.701.271.220.990.941.191.031.801.191.000.911.171.061.201.171.011.380.919.590.940.910.980.890.531.320.472.431.361.330.410.191.371.23
    Na2O0.160.080.270.100.170.090.160.100.130.080.100.110.090.090.080.080.100.100.080.090.140.140.100.150.100.150.110.090.110.160.180.120.16
    K2O2.580.190.260.211.390.151.260.030.130.180.140.530.750.240.230.120.210.080.050.170.430.380.232.090.152.450.270.180.553.474.680.770.19
    MnO0.070.010.010.020.010.010.010.010.020<0.00400.0100.010<0.00400.2000.010.01000.010.010.010.010.010.020.020.020.015
    TiO20.970.080.140.090.430.070.470.230.070.090.070.290.290.130.140.090.170.060.030.080.150.130.110.760.110.780.100.100.330.830.850.270.33
    P2O50.130.020.040.020.030.080.040.920.280.140.070.070.270.280.280.160.760.060.080.030.090.250.070.130.300.260.200.370.230.100.060.190.092
    SiO2/Al2O34.132.032.053.512.892.652.872.592.422.882.963.033.073.062.862.632.082.892.432.092.202.272.222.591.813.152.002.182.823.024.052.691.42
    注:中国煤数据据来自文献[13],BLT代表北露天矿。
    下载: 导出CSV

    表  3   义马盆地中侏罗世煤样稀土元素分析结果

    Table  3   Content of rare earth elements in middle Jurassic coal from Yima Basin ug/g

    项目含量/(μg·g−1
    LaCePrNdSmEuGdTbDyHoErTmYbLuY∑REYδCeδEu(La/Yb)N(La/Sm)N(Gd/Yb)N
    BLT-133.560.57.4428.75.361.074.650.7563.420.5941.460.2151.20.15433.9149.020.920.6618.823.933.13
    BLT-29.5418.427.861.480.2821.290.2161.160.2290.6040.1030.6540.08814.143.911.010.629.834.051.59
    BLT-311.623.12.549.51.730.3331.490.2491.210.2270.6110.10.5920.08213.553.361.020.6313.214.222.03
    BLT-46.8913.61.626.531.340.3161.190.2141.170.2240.6080.1060.6520.09113.234.550.980.777.123.231.47
    BLT-530.760.36.8626.74.740.8673.80.62.680.4661.250.1921.130.14926.2140.431.000.6218.324.072.71
    BLT-66.12131.576.741.470.3191.440.2671.480.2880.7610.1230.7450.10218.734.431.010.675.542.621.56
    BLT-730.663.37.2928.65.081.144.170.6773.090.5381.370.2091.220.15730.7147.441.020.7616.913.792.76
    BLT-817.2344.0617.94.110.9423.360.58630.5231.290.1861.050.13830.888.350.980.7811.042.632.58
    BLT-95.110.81.315.550.9790.2580.8560.1490.7470.1410.3870.0660.3940.0558.9526.791.010.868.733.281.75
    BLT-103.919.471.346.361.210.2871.010.180.9280.1770.4710.0780.4760.06311.025.961.000.795.542.031.71
    BLT-114.319.331.084.390.970.2640.870.1540.8550.1620.4450.0750.4550.06210.723.421.040.886.392.791.54
    BLT-1215.928.13.1512.52.720.5712.330.4312.260.4161.10.1791.060.14424.270.860.960.6910.113.681.77
    BLT-1327.859.16.6124.44.170.8233.640.5672.630.4651.20.1861.130.14725.0132.871.050.6516.594.192.60
    BLT-1425.758.16.5324.14.020.8363.730.6033.020.5391.410.2181.350.16928.6130.331.080.6612.834.022.23
    BLT-1520.444.74.9418.13.210.6912.890.4842.360.4211.060.1731.030.1325.4100.591.070.6913.354.002.26
    BLT-166.6414.41.798.431.880.4531.580.2991.660.3160.830.1370.8350.11118.839.361.010.805.362.221.53
    BLT-1766.512812.543.46.941.436.150.8613.660.5571.420.1811.060.13530.3272.791.070.6742.306.034.68
    BLT-182.726.630.9434.180.8470.2350.8280.1640.9310.190.5190.0880.5430.07511.818.891.000.863.382.021.23
    BLT-194.3710.21.134.190.7670.2030.7230.1350.6610.1250.3360.0570.3440.0478.8123.291.000.838.563.581.70
    BLT-204.549.381.064.191.160.3061.100.2421.490.3060.8410.1520.9570.13416.125.861.030.833.202.460.93
    BLT-2114.125.82.8110.21.940.531.760.3031.60.3050.8330.140.8530.11717.261.290.990.8811.144.571.66
    BLT-2216.735.94.518.83.590.8493.060.5062.410.431.090.1710.9950.12926.689.131.000.7811.322.932.48
    BLT-238.7220.12.278.712.070.5072.050.4352.520.51.320.231.390.18929.251.011.090.754.232.651.19
    BLT-2442.277.79.0934.96.261.134.790.7583.310.5661.480.2151.290.15730.4183.850.950.6322.064.243.00
    BLT-2543.7859.1933.15.111.124.720.7733.620.6441.660.2551.520.19637.6190.611.020.7019.385.382.51
    BLT-2646.483.39.435.16.041.084.780.7162.990.491.210.1650.9940.1226.5192.790.960.6131.474.833.88
    BLT-2713.827.23.1112.12.310.5992.060.3852.060.3871.080.1811.150.15923.566.581.000.848.093.761.45
    BLT-2861.81231344.96.91.356.230.8813.820.6461.660.2491.490.19934.5266.131.040.6327.965.633.37
    BLT-2938.778.58.230.35.611.154.780.7833.850.6931.810.2831.670.22637176.561.060.6815.624.342.31
    BLT-3058.110712.447.48.321.57.041.084.520.731.840.2531.490.19143.1251.860.960.6026.294.393.81
    BLT-3152.795.211.141.36.851.185.500.8083.30.541.350.1811.030.12627.5221.170.950.5934.504.844.31
    均值23.5846.235.1919.653.520.733.030.492.340.411.070.170.990.1323.67149.021.010.7214.493.762.31
    中国煤22.5046.706.4222.304.070.844.650.623.7418.200.961.790.640.382.08136.00
    世界煤11.0023.003.5012.002.000.472.700.322.108.400.540.930.310.201.0068.47
    富集系数(CC)2.142.011.481.971.761.551.121.531.110.0491.980.183.190.6523.672.18
    注:中国煤数据与世界煤数据来源于文献[13],$\delta \text{Ce}\text{=}{\text{Ce}}_{\text{N}}/\sqrt{{\text{La}}_{\text{N}}\text{×}{\text{Pr}}_{\text{N}}} $,CeN、LaN、PrN为Ce、La、Pr元素球粒陨石标准化值;$\delta \text{Eu}\text{=}{\text{Eu} }_{\text{N} }/\sqrt{ {\text{Sm} }_{\text{N} }\text{×}{\text{Gd} }_{\text{N} } }$,EuN、SmN、GdN为元素球粒陨石标准化值[20];球粒陨石数据据文献[21];富集系数(CC)为样品中稀土元素含量/世界煤中稀土元素含量;“—” 为无数据。
    下载: 导出CSV
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出版历程
  • 收稿日期:  2022-07-08
  • 网络出版日期:  2023-05-07
  • 刊出日期:  2023-05-30

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