Geochemical Characteristics of Rare, Dispersed, and Rare Earth Elements in the Middle Jurassic Yan'an Formation of the Ningdong Coalfield and Their Indication for a Sedimentary Environment
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摘要:
稀有稀散稀土元素（三稀元素）因性能和作用特殊，是重要的战略资源，同时因其特有的地球化学属性，在研究古气候、古水体和古沉积环境、沉积物源等方面具有重要的意义。前人针对宁东煤田研究发现，煤系伴生稀散元素Ga轻度富集，而稀土元素含量偏低。本次研究选取灵武、积家井两个典型矿区，在钻孔岩心中开展系统采样，采用电感耦合等离子体质谱法（ICP-MS）对延安组泥岩、砂岩以及煤层顶（底）板开展三稀元素含量测试，探讨煤系三稀元素富集成矿可能性，同时讨论延安组古沉积环境特征及物源区岩石性质。结果表明：宁东煤田中侏罗统延安组煤系三稀元素整体含量水平较低（仅有Ga元素最高含量29.40μg/g，接近于30.00μg/g的最低工业品位）。稀有、稀散元素在延安组底部或细-粉砂岩、泥岩中的含量较高，与世界煤中的平均含量相比，稀有元素Li、Nb、Ta、Rb、Cs、Zr和稀散元素Ga、In、Sc、Hf为轻度富集或富集；REY（稀土元素+Y元素）属于LREY富集型，Eu呈明显的负异常。通过典型元素地球化学参数研究延安组古沉积环境，Rb、Sr和REY指示古气候条件温湿，Li、Sr、Ga指示为淡水沉积环境，Ce、Ce/La反映缺氧的还原环境；REY含量未受成岩作用影响，可以用于对原始沉积岩物源的判别。
Abstract:BACKGROUND Rare, dispersed, and rare earth elements are important strategic resources because of their special performance and function. At the same time, because of its unique geochemical properties, it is of great significance in the study of paleoclimate, paleo-water and paleo-sedimentary environment, and sediment sources. Previous studies have found that Ga in the Ningdong Coalfield is slightly enriched and rare earth element content is low.
OBJECTIVES To explore the possibility of enrichment and mineralization of rare, dispersed, and rare earth elements in the coal series of the Yan'an Formation of Middle Jurassic in the Ningdong Coalfield, and discuss the characteristics of paleosedimentary environment and properties of provenance rock.
METHODS Systematic sampling was carried out in the core of boreholes from the Lingwu and Jijiajing mining areas of the Ningdong Coalfield. ICP-MS was used to determine the content of rare, dispersed, and rare earth elements in mudstone, sandstone and top (bottom) plate of the Yan'an Formation.
RESULTS The overall content of rare, dispersed, and rare earth elements in the Yan'an Formation of the Ningdong Coalfield is low, which do not meet the requirements of the industrial indicators of the deposit and cannot be exploited comprehensively. The highest content of Ga is 29.40μg/g, which is close to the lowest industrial grade of 30.00μg/g. Compared with the average content of elements in world coal, rare elements Li, Nb, Ta, Rb, Cs, Zr and dispersed elements Ga, In, Sc, Hf are slightly enriched or enriched. The distribution of rare earth elements shows LREY type, and significant negative anomaly of Eu.
CONCLUSIONS Rb, Sr and REY indicate the humidity of paleoclimate conditions, Li, Sr and Ga represent the freshwater deposition environment, and Ce, Ce/La reflect the anoxic reducing environment. The REY content is not affected by diagenesis and can be used to discriminate the original sediment source.
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表 1 宁东煤田延安组样品稀有、稀散元素含量统计
Table 1. Statistics of rare and dispersed element contents in samples from Yan'an Formation, Ningdong Coalfield
元素类型 元素 积家井矿区 灵武矿区 最低值(μg/g) 最高值(μg/g) 平均值(μg/g) 最低值(μg/g) 最高值(μg/g) 平均值(μg/g) 稀有元素 Li 6.00 65.70 35.40 19.00 45.70 35.70 Be 0.72 6.66 2.70 1.52 3.27 2.35 Rb 14.70 140.00 105.60 52.60 140.00 112.70 Sr 91.50 308.00 159.10 116.00 279.00 165.70 Nb 3.17 21.00 13.70 8.15 19.80 16.30 Cs 1.00 9.72 6.10 2.68 14.10 8.10 Ta 0.28 1.73 1.10 0.60 1.64 1.30 Zr - - - 132.00 275.00 230.00 稀散元素 Sc 3.10 18.50 12.90 8.00 1.70 15.90 Ge 0.60 2.59 1.30 0.90 2.24 1.50 Ga 5.80 25.10 19.40 13.50 29.40 24.30 Cd 0.02 0.38 0.10 0.10 0.26 0.16 In 0.02 0.09 0.06 0.05 0.10 0.08 Tl 0.57 1.74 0.82 0.39 0.78 0.66 Hf - - - 4.03 8.33 6.89 Se 0.00 0.52 0.15 0.04 0.37 0.19 注：表中数据为本次实测结果，“-”表示未测试项目。 
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表 2 宁东煤田延安组样品稀有稀散元素平均富集系数
Table 2. Average enrichment coefficient of rare and dispersed elements in samples of Yan'an Formation, Ningdong Coalfield
元素 稀有稀散元素平均富集系数 元素 稀有稀散元素平均富集系数 积家井矿区 灵武矿区 平均值 积家井矿区 灵武矿区 平均值 Li 2.95 2.98 2.96 Sc 3.30 4.07 3.68 Be 1.70 1.47 1.58 Ge 0.58 0.68 0.63 Rb 7.54 8.05 7.79 Ga 3.35 4.18 3.75 Sr 1.45 1.51 1.48 Cd 0.57 0.75 0.65 Nb 3.71 4.39 4.04 In 2.03 2.51 2.26 Cs 6.07 8.10 7.06 Tl 1.31 1.05 1.18 Ta 4.05 4.50 4.27 Hf - 5.74 5.74 Zr - 6.39 6.39 Se 0.12 0.15 0.13 注：表中数据为本次研究样品实测元素含量除以世界煤中平均含量的比值；“-”表示该元素未测定。
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表 3 宁东煤田延安组样品稀土和钇元素含量
Table 3. Contents of REEs and yttrium in samples from Yan'an Formation, Ningdong Coalfield
序号 积家井矿区样品编号 采样深度(m) 样品岩性 元素含量(单位：μg/g) La Ce Pr Nd Sm Eu Gd Tb Dy Y Ho Er Tm Yb Lu 1 ND-SX01 531 炭质泥岩(煤层底板) 50.50 98.73 11.00 39.74 7.19 1.50 6.52 1.04 5.88 32.46 1.18 3.43 0.53 3.50 0.53 2 ND-SX02 607 中粒砂岩 50.60 98.80 11.19 40.91 7.70 1.65 6.82 1.11 6.07 33.65 1.19 3.39 0.53 3.33 0.52 3 ND-SX03 622 中-粗粒砂岩 42.69 82.80 9.53 35.99 6.66 1.51 5.94 0.92 4.97 24.35 0.93 2.48 0.42 2.47 0.39 4 ND-SX04 631 细砂岩 39.93 76.01 8.93 32.00 6.08 1.37 5.39 0.88 4.82 25.56 0.95 2.64 0.42 2.68 0.41 5 ND-SX05 655 中-粗粒砂岩 25.37 46.13 5.83 22.22 4.11 1.09 3.89 0.66 4.02 25.39 0.86 2.51 0.43 2.71 0.41 6 ND-SX06 681 粉砂岩(煤层顶板) 49.36 95.08 11.25 41.41 7.65 1.60 6.89 1.08 6.18 36.24 1.21 3.43 0.54 3.48 0.55 7 ND-SX07 691 中-粗粒砂岩 25.38 45.91 5.77 21.46 3.82 1.01 3.58 0.60 3.34 18.81 0.71 2.04 0.35 2.20 0.35 8 ND-SX08 717 细-粉砂岩 48.28 95.64 11.07 40.53 7.44 1.60 6.68 1.07 5.91 32.17 1.17 3.26 0.51 3.45 0.53 9 ND-SX09 717 细-粉砂岩 43.09 85.80 9.89 36.84 6.98 1.50 6.24 1.01 5.81 33.81 1.17 3.28 0.52 3.43 0.52 10 ND-SX10 751 粉砂岩 46.74 90.47 10.54 38.65 7.31 1.58 6.73 1.08 6.18 38.49 1.24 3.48 0.56 4.82 0.57 11 ND-SX11 766 中粒砂岩 18.80 36.90 4.29 15.10 2.60 0.73 2.33 0.36 1.98 10.34 0.37 1.04 0.21 1.15 0.21 12 ND-SX12 784 粉砂岩(煤层顶板) 49.40 97.92 11.14 40.53 7.49 1.61 6.83 1.06 6.01 32.91 1.18 3.35 0.52 3.42 0.51 13 ND-SX13 784 粉砂岩 42.93 85.36 9.89 36.53 6.74 1.50 6.21 1.01 5.68 31.15 1.13 3.14 0.50 3.29 0.51 14 ND-SX14 799 粗粒砂岩 12.65 21.22 2.67 10.52 1.83 0.65 1.63 0.29 1.58 9.75 0.33 0.94 0.19 1.06 0.18 15 ND-SX15 817 粉砂岩 74.05 148.60 16.33 58.62 10.91 2.29 9.67 1.46 7.61 37.13 1.41 3.80 0.56 3.63 0.55 16 ND-SX16 817 粉砂岩 48.18 93.54 10.75 39.23 7.13 1.58 6.43 1.03 5.65 36.01 1.53 3.10 0.49 3.08 0.48 17 ND-SX17 841 粗粒砂岩 46.55 82.93 8.88 30.70 5.16 1.05 4.80 0.78 4.79 30.62 0.99 2.98 0.50 3.28 0.50 18 ND-SX18 851 粉砂岩夹泥岩(煤层顶板) 15.62 25.25 3.09 11.37 1.78 0.58 1.53 0.25 1.21 7.71 0.27 0.80 0.18 1.00 0.18 19 ND-SX19 872 中粒砂岩 37.82 70.21 8.34 31.16 5.54 1.11 4.82 0.73 3.85 20.90 0.76 2.12 0.36 2.12 0.35 20 ND-SX20 895 粉砂岩 52.07 99.20 11.28 41.70 7.59 1.42 6.52 1.01 5.50 31.96 1.06 3.04 0.49 3.11 0.47 积家井矿区样品元素含量平均值 41.00 78.83 9.08 33.26 6.09 1.35 5.47 0.87 4.85 27.47 0.98 2.71 0.44 2.86 0.44 积家井矿区样品元素平均富集系数 3.73 3.43 2.6 2.77 3.04 2.86 2.03 2.73 2.31 3.27 1.82 2.92 1.42 2.86 2.18 序号 灵武矿区样品编号 采样深度(m) 样品岩性 元素含量(单位：μg/g) La Ce Pr Nd Sm Eu Gd Tb Dy Y Ho Er Tm Yb Lu 21 ND-SX21 335 泥岩(煤层底板) 33.06 61.29 6.63 24.86 4.13 1.23 3.58 0.52 2.47 12.28 0.46 1.29 0.23 1.30 0.25 22 ND-SX22 339 泥岩 49.94 97.24 11.30 42.85 8.03 1.76 6.68 1.09 6.43 33.85 1.28 3.43 0.54 3.55 0.55 23 ND-SX23 346 泥岩 36.76 68.15 8.14 31.51 6.06 1.25 5.31 0.93 5.83 36.02 1.22 3.30 0.53 3.35 0.53 24 ND-SX24 362 泥岩 62.08 127.31 14.10 54.83 9.98 2.13 8.32 1.33 7.93 39.95 1.54 4.14 0.63 4.15 0.62 25 ND-SX25 366 中粒砂岩 42.16 81.67 9.58 35.17 6.36 1.35 5.21 0.81 4.29 20.55 0.81 2.18 0.35 2.17 0.35 26 ND-SX26 409 泥岩(煤层顶板) 51.07 97.36 11.08 41.04 7.62 1.55 6.48 1.05 6.31 34.56 1.27 3.45 0.53 3.49 0.53 27 ND-SX27 410 粉砂岩 54.21 105.32 12.11 46.74 8.51 1.84 7.27 1.14 6.61 31.73 1.27 3.40 0.51 3.35 0.51 28 ND-SX28 415 粉砂质泥岩 52.15 100.99 11.78 45.71 8.31 1.74 6.93 1.11 6.40 31.26 1.25 3.37 0.52 3.41 0.52 29 ND-SX29 420 细粒砂岩 44.93 89.00 10.60 40.75 7.92 1.77 6.77 1.13 6.90 35.26 1.37 3.68 0.57 3.72 0.55 30 ND-SX30 493 炭质泥岩(煤层底板) 65.31 125.54 14.02 55.07 9.91 2.03 8.48 1.36 8.23 41.33 1.64 4.36 0.65 4.28 0.64 31 ND-SX31 497 炭质泥岩 48.87 94.56 10.96 41.20 7.68 1.65 6.37 1.01 5.90 29.56 1.22 3.14 0.49 3.21 0.49 32 ND-SX32 516 粉砂质泥岩(煤层底板) 46.26 90.57 10.37 39.00 7.26 1.53 6.20 1.01 6.12 32.61 1.26 3.28 0.52 3.56 0.52 33 ND-SX33 521 粉砂质泥岩 51.47 101.99 11.64 43.13 8.10 1.65 6.80 1.12 6.77 35.14 1.35 3.66 0.56 3.67 0.56 34 ND-SX34 572 粉砂质泥岩(煤层底板) 40.51 79.55 9.20 34.56 6.50 1.39 5.62 0.91 5.43 28.99 1.10 2.97 0.48 3.07 0.48 35 ND-SX35 574 粉砂质泥岩 46.12 89.81 10.29 38.02 7.07 1.48 6.05 0.99 5.77 29.62 1.14 3.03 0.48 3.09 0.47 36 ND-SX36 587 粉砂质泥岩(煤层底板) 50.78 96.84 11.04 40.76 7.62 1.59 6.55 1.05 6.21 32.12 1.23 3.36 0.52 3.39 0.52 37 ND-SX37 596 粉砂质泥岩(煤层底板) 50.26 89.46 11.08 41.68 7.59 1.56 6.35 1.00 5.78 29.02 1.15 3.14 0.49 3.23 0.49 38 ND-SX38 612 细粒砂岩 30.42 56.62 6.77 26.88 5.03 1.10 4.18 0.69 3.88 21.16 0.78 2.20 0.37 2.37 0.38 39 ND-SX39 617 粉砂质泥岩(煤层顶板) 35.90 62.74 6.82 24.83 4.10 0.76 3.63 0.59 3.36 19.32 0.70 2.05 0.36 2.33 0.38 灵武矿区样品元素含量平均值 46.96 90.32 10.39 39.40 7.25 1.54 6.15 0.99 5.82 30.23 1.16 3.13 0.49 3.19 0.49 灵武矿区样品元素平均富集系数 4.27 3.93 2.97 3.28 3.63 3.29 2.28 3.10 2.77 3.60 2.15 3.36 1.59 3.19 2.46 两矿区全部样品元素含量平均值 43.90 84.42 9.72 36.25 6.65 1.44 5.80 0.93 5.33 28.81 1.07 2.91 0.47 3.02 0.46 两矿区全部样品元素平均富集系数 3.99 3.67 2.78 3.02 3.33 3.07 2.15 2.91 2.54 3.44 1.98 3.13 1.50 3.02 2.31 注：表中数据为本次实测结果，富集系数为本次实测元素含量除以世界煤中平均含量得出，世界煤中平均含量引自文献[21]。
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表 4 宁东煤田延安组样品稀土和钇元素地球化学参数
Table 4. Geochemical parameters of REEs and yttriumin in samples from Yan'an Formation, Ningdong Coalfield
序号 积家井矿区样品编号 LREY MREY HREY REY (Gd/Lu)N (La/Lu)N (La/Yb)N (La/Sm)N (Gd/Yb)N δEu δCe Ceanom 1 ND-SX01 207.16 47.41 9.16 263.72 1.68 10.42 10.24 4.13 1.65 0.69 1.00 -0.04 2 ND-SX02 209.19 49.29 8.95 267.43 1.93 11.61 11.67 4.03 1.94 0.74 0.99 -0.04 3 ND-SX03 177.68 37.70 6.68 222.05 1.69 10.43 10.04 4.13 1.62 0.73 0.97 -0.05 4 ND-SX04 162.94 38.02 7.10 208.06 1.22 6.63 6.31 3.88 1.16 0.83 0.91 -0.08 5 ND-SX05 103.66 35.05 6.92 145.63 1.60 9.60 9.57 4.06 1.60 0.67 0.97 -0.05 6 ND-SX06 204.75 51.98 9.21 265.94 1.33 7.86 7.79 4.18 1.32 0.84 0.91 -0.07 7 ND-SX07 102.34 27.34 5.65 135.33 1.63 9.84 9.45 4.08 1.56 0.69 1.00 -0.03 8 ND-SX08 202.96 47.42 8.91 259.29 1.52 8.80 8.48 3.89 1.47 0.69 1.00 -0.03 9 ND-SX09 182.60 48.37 8.92 239.89 1.52 8.80 6.54 4.02 1.13 0.69 0.98 -0.04 10 ND-SX10 193.71 54.07 10.67 258.44 1.45 9.80 11.00 4.55 1.63 0.91 0.99 -0.03 11 ND-SX11 77.69 15.74 2.98 96.41 1.70 10.28 9.74 4.15 1.61 0.69 1.00 -0.03 12 ND-SX12 206.47 48.43 8.99 263.89 1.56 9.03 8.81 4.01 1.53 0.71 1.00 -0.03 13 ND-SX13 181.45 45.55 8.56 235.56 1.14 7.38 8.04 4.36 1.24 1.15 0.88 -0.10 14 ND-SX14 48.89 13.90 2.71 65.49 2.26 14.48 13.74 4.27 2.15 0.68 1.03 -0.02 15 ND-SX15 308.50 58.16 9.95 376.61 1.72 10.76 10.56 4.25 1.69 0.71 0.99 -0.04 16 ND-SX16 198.83 50.70 8.68 258.21 1.24 10.07 9.57 5.68 1.18 0.65 0.98 -0.05 17 ND-SX17 174.22 42.04 8.24 224.51 1.12 9.56 10.52 5.52 1.23 1.08 0.87 -0.10 18 ND-SX18 57.11 11.27 2.42 70.81 1.78 11.66 12.00 4.29 1.83 0.66 0.95 -0.06 19 ND-SX19 153.07 31.42 5.72 190.20 1.80 11.99 11.27 4.31 1.69 0.62 0.99 -0.04 20 ND-SX20 211.85 46.42 8.16 266.43 1.57 10.18 9.74 4.42 1.51 0.67 1.01 -0.03 积家井矿区平均值 168.25 40.01 7.43 215.70 1.57 9.96 9.75 4.31 1.54 0.76 0.97 -0.05 序号 灵武矿区样品编号 LREY MREY HREY REY (Gd/Lu)N (La/Lu)N (La/Yb)N (La/Sm)N (Gd/Yb)N δEu δCe Ceanom 21 ND-SX21 129.98 20.08 3.53 153.58 1.84 14.25 17.11 5.03 2.22 0.98 1.00 -0.05 22 ND-SX22 209.36 49.80 9.36 268.52 1.55 9.71 9.49 3.91 1.52 0.73 0.99 -0.04 23 ND-SX23 150.62 49.33 8.92 208.88 1.30 7.50 7.40 3.82 1.28 0.67 0.95 -0.07 24 ND-SX24 268.31 59.67 11.09 339.06 1.71 10.67 10.09 3.91 1.62 0.71 1.04 -0.02 25 ND-SX25 174.95 32.20 5.86 213.02 1.91 12.88 13.09 4.17 1.94 0.72 0.98 -0.04 26 ND-SX26 208.18 49.94 9.27 267.39 1.57 10.32 9.87 4.21 1.50 0.67 0.99 -0.04 27 ND-SX27 226.89 48.59 9.05 284.53 1.82 11.34 10.91 4.01 1.75 0.72 0.99 -0.05 28 ND-SX28 218.94 47.44 9.08 275.46 1.72 10.85 10.30 3.95 1.64 0.70 0.98 -0.05 29 ND-SX29 193.20 51.83 9.90 254.93 1.57 8.71 8.14 3.57 1.47 0.74 0.98 -0.04 30 ND-SX30 269.84 61.43 11.57 342.84 1.71 10.99 10.28 4.14 1.60 0.68 1.00 -0.05 31 ND-SX31 203.26 44.49 8.54 256.29 1.67 10.71 10.28 4.01 1.60 0.72 0.98 -0.04 32 ND-SX32 193.46 47.48 9.15 250.09 1.53 9.52 8.75 4.01 1.40 0.70 1.00 -0.04 33 ND-SX33 216.32 51.48 9.80 277.61 1.56 9.88 9.44 4.00 1.49 0.68 1.00 -0.03 34 ND-SX34 170.31 42.35 8.10 220.76 1.49 8.99 8.88 3.92 1.48 0.70 0.99 -0.04 35 ND-SX35 191.31 43.91 8.22 243.43 1.64 10.48 10.06 4.10 1.58 0.69 0.99 -0.04 36 ND-SX36 207.05 47.51 9.02 263.58 1.61 10.41 10.10 4.19 1.56 0.69 0.98 -0.04 37 ND-SX37 200.07 43.70 8.49 252.27 1.67 11.04 10.51 4.16 1.59 0.69 0.91 -0.08 38 ND-SX38 125.71 31.01 6.09 162.81 1.41 8.59 8.65 3.81 1.42 0.73 0.95 -0.07 39 ND-SX39 134.39 27.66 5.81 167.86 1.22 10.12 10.39 5.50 1.26 0.60 0.97 -0.07 灵武矿区平均值 194.32 44.73 8.47 247.52 1.61 10.37 10.20 4.13 1.57 0.71 0.98 -0.05 两矿区样品平均值 180.95 42.31 7.93 231.20 1.59 10.15 9.97 4.22 1.55 0.73 0.98 -0.05 注：δEu=EuN/(SmN×GdN)0.5；δCe= CeN/(LaN×PrN)0.5；Ce异常指数Ceanom=lg[3CeN/(2LaN+NdN)]，式中的CeN、LaN、NdN分别为CeN、LaN、NdN值与北美页岩标准化之后的值；每个矿区平均值为该矿区所采样品的算术平均值，全部样品平均值为两个矿区所有样品的算术平均值。
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