New Recognition of Carbonate Nodules Genesis in Sinian Doushantuo Formation in Zigui Area and Its Geological Implication
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摘要: 扬子克拉通秭归地区震旦系陡山沱组第四段黑色泥页岩中广泛发育具明显δ13C负异常的碳酸盐岩结核，其是否与古甲烷天然气水合物渗漏有关值得深入研究.对该碳酸盐岩结核开展的沉积结构构造、岩相学和地球化学研究表明，碳酸盐岩结核具典型韵律环带结构，普遍发育有亮晶球体结构、草莓状黄铁矿，以及与渗漏系统有关的凝块组构，δ13C具明显负异常(-5.65‰~-6.76‰)，U、Mo元素强烈富集(UEF=8~26，MoEF=99~320)，Y/Ho比值为31.05~37.31，稀土配分型式为平缓左倾，主微量元素K、Sc、V、Cr、Co、Ni、Rb、Sr、Ba、Th、U和Mo等总体显示为缺氧-硫化环境，与冷泉碳酸盐岩的形成环境和特征一致.碳酸盐岩结核环带SiO2、MgO、CaO、CO2等地球化学元素含量呈阶段性连续增减变化，显示碳酸盐岩结核形成经历了初始形成、成岩-交代、成岩后改造3个连续演化阶段.据此，提出碳酸盐岩结核是新元古代末噶斯奇厄斯冰期(582~551 Ma)结束温度回暖，黑色泥页岩中低温封存固态天然气水合物发生分解释放和成岩-交代形成的冷泉碳酸盐岩结核，也是古天然气水合物存在的重要地质记录和标志，这一新认识为华南扬子克拉通在震旦系和下古生界沉积盖层中寻找页岩气(甲烷天然气)储集层位提供了重要地质依据.Abstract: The carbonate nodules with strongly negative δ13C anomalies are widely developed in the black muddy shale in the forth member of the Doushantuo Formation from the Sinian System in the Zigui area, Yangtze Craton. Whether they were related to leakage of gas hydrate deserves further studies. Studies of sedimentary structure, petrography and geochemistry of these carbonate nodules show that these nodules have typical oscillatory zoning, sparry sphere structure, framboidal pyrite and agglomerate fabrics, which are related to venting system. The carbonate nodules display obvious negative δ13C anomalies (-5.65‰ to -6.76‰), strong enrichment of U and Mo elements (UEF=8-26, MoEF=99-320) and Y/Ho ratios between 31.05 and 37.31. Their REE distributions display gentle left-sloping patterns and their major and trace elements such as K, Sc, V, Cr, Co, Ni, Rb, Sr, Ba, Th, U and Mo indicate a hypoxia and sulfidic setting, which is consistent with characteristics and formation environment of cold seep carbonates. SiO2, MgO, CaO and CO2 contents of oscillatory zoning within the nodules show continuously increase or decrease changes, respectively. They reflect three stages of continuous evolution processes including primary formation, subsequent diagenesis-metasomatism and final diagenetic reworking. Accordingly, it can be proposed that these carbonate nodules were ultimately developed as decomposition, diagenesis and metasomatism of the low temperature stored solid gas hydrate sediment in the black muddy shale when the temperature became higher after the Neoproterozoic Gaskiers glaciation (582-551 Ma). This study provides an important record that confirms existence of the ancient natural gas hydrate and offers an important geological evidence for exploring shale gas (methane gas) reservoirs in the Sinian System and Lower Paleozoic sedimentary covers in the Yangtze Craton of South China.
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图 1 鄂西黄陵穹隆地区地质简图
Fig. 1. Geological sketch of the Huangling dome in western Hubei
图 2 秭归地区岩石地层层序、同位素年代及冰期时代综合对比
数据来源：① Condon et al.(2005)；② Zhang et al.(2005)；③ 刘鹏举等(2009)；④ 刘鸿允(1991)；⑤ Bowring et al.(2003)；⑥ Halverson et al.(2005)；⑦ Macdonald et al.(2010)；⑧ Fanning and Link(2004)；⑨ Hoffman(1999)；⑩ Frimmel et al.(1996)
Fig. 2. Comprehensive comparison for the stratigraphic sequence, isotopic age and glacial epoch in Zigui area
图 3 碳酸盐岩结核野外及显微照片
a.碳酸盐岩结核野外宏观特征；b、c.红圈表示碳酸盐岩结核A和B的钻孔取样位置；d.白云石球状构造(单偏光)，圆圈内白云石集合体近圆形，方框中白云石集合体近方形；e.草莓状黄铁矿集合体(反射光)；f.不同期次裂隙之间的切割关系(单偏光)；g.凝块石沉积组构(单偏光)；h.亮晶球体结构(单偏光)
Fig. 3. Field and micrograph photographs of the carbonate nodules
图 4 碳酸盐岩结核中SiO2与MgO、CaO、CO2含量相关性
Fig. 4. SiO2 and MgO, CaO, CO2 contents for correlation of carbonate nodules
图 5 碳酸盐岩结核澳大利亚后太古宙沉积岩标准化REE配分模式
Fig. 5. PAAS-nomalized REE distribution pattern of the carbonate nodules
图 6 碳酸盐岩结核形成环境地球化学判别
a.Sr/Ba-Rb/K判别图解，数据来源于Campbell and Williams(1965)、王益友等(1979)、郑荣才和柳梅青(1999)；b.V/(V+Ni)-V/Cr判别图解，数据来源于Hatch and Leventhal(1992)、Jones and Manning(1994)、Wingnall(1994); c.V/(V+Ni)-Th/U判别图解，数据来源于Hatch and Leventhal(1992)、Jones and Manning(1994)、Wingnall(1994).(图例同图 5)
Fig. 6. Geochemical discrimination diagrams of formation environment for the carbonate nodules
表 1 碳酸盐岩结核主量元素(%)组成
Table 1. Major elements (%) composition of the carbonate nodules
样品号 碳酸盐岩结核A 碳酸盐岩结核B 取样位置 内核带 过渡带 边缘带 内核带 过渡带 边缘带 取样编号 A-1-2 A-1-3 A-1-7 A-2-9 A-3-1 A-4-1 B-1-3 B-1-6 B-2-2 B-3-7 B-4-5 SiO2 72.80 81.77 51.58 14.39 8.40 7.04 56.99 49.06 9.92 7.01 5.88 TiO2 0.08 0.07 0.06 0.05 0.04 0.07 0.06 0.04 0.04 0.04 0.07 Al2O3 1.66 1.65 1.11 0.97 0.82 1.28 1.11 0.83 0.63 0.74 1.24 Fe2O3 2.92 2.71 2.50 0.63 0.53 1.40 1.90 1.34 0.44 0.50 1.51 FeO 0.37 0.30 0.37 0.12 0.10 0.10 0.67 0.60 0.15 0.07 0.08 MnO 0.07 0.04 0.07 0.12 0.13 0.11 0.08 0.08 0.12 0.11 0.10 MgO 3.74 1.86 8.23 16.37 17.41 17.80 7.80 9.75 17.29 18.03 17.96 CaO 5.90 3.01 13.39 25.67 27.57 27.00 11.65 14.44 26.43 27.42 26.97 Na2O 0.16 0.15 0.19 0.16 0.16 0.19 0.20 0.19 0.17 0.16 0.19 K2O 0.61 0.55 0.42 0.45 0.40 0.66 0.41 0.28 0.29 0.35 0.60 P2O5 0.17 0.11 0.15 0.09 0.06 0.07 0.19 0.12 0.06 0.05 0.03 H2O+ 1.82 1.86 1.44 1.10 1.00 1.17 1.42 1.22 1.22 1.19 1.32 CO2 8.19 4.05 18.50 39.49 42.33 41.86 17.54 21.40 42.02 43.12 42.48 Total 98.49 98.13 98.01 99.61 98.95 98.75 100.02 99.35 98.78 98.79 98.43 
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表 2 碳酸盐岩结核微量元素(10-6)组成
Table 2. Trace elements (10-6) composition of the carbonate nodules
样品号 碳酸盐岩结核A 碳酸盐岩结核B 取样位置 内核带 过渡带 边缘带 内核带 过渡带 边缘带 取样编号 A-1-2 A-1-3 A-1-7 A-2-9 A-3-1 A-4-1 B-1-3 B-1-6 B-2-2 B-3-7 B-4-5 Be 0.53 0.43 0.45 0.73 0.70 0.90 0.35 0.45 0.57 0.50 0.78 Sc 2.44 2.14 1.91 2.08 1.82 5.04 1.67 1.58 1.46 1.58 2.61 V 165.0 139.0 135.0 189.0 175.0 278.0 93.8 88.4 147.0 160.0 177.0 Cr 21.4 17.0 26.1 14.6 10.1 15.5 15.7 17.0 9.2 8.0 11.3 Co 3.94 3.22 2.85 2.18 1.97 2.95 3.10 2.60 1.72 1.88 2.75 Ni 35.0 28.4 24.6 23.8 20.2 28.2 18.9 17.4 18.7 19.3 12.4 Cu 31.0 25.1 20.2 9.2 8.6 12.6 15.3 13.3 6.5 6.1 13.1 Zn 90.6 98.7 57.7 29.7 42.1 46.5 32.7 19.1 29.5 33.2 11.1 Ga 2.86 2.92 2.03 1.68 1.46 2.34 1.85 1.56 1.18 1.37 1.81 Rb 16.10 14.90 10.70 9.74 8.15 13.10 10.20 7.37 5.85 7.37 12.60 Sr 70.0 59.6 212.0 92.3 107.0 93.7 89.2 123.0 118.0 94.4 110.0 Y 9.90 6.96 9.33 10.10 9.77 15.20 9.21 6.78 6.93 7.02 9.53 Zr 18.80 17.40 12.70 10.90 8.51 13.50 11.80 8.88 6.79 8.12 12.60 Nb 1.84 1.68 1.24 1.06 0.87 1.39 1.20 0.87 0.67 0.82 1.39 Mo 28.1 23.3 19.30 19.8 14.0 23.7 18.0 15.3 15.6 16.3 14.3 Sn 1.95 1.11 1.16 0.56 0.41 0.59 1.98 1.14 0.38 0.47 0.58 Cs 0.75 0.71 0.50 0.41 0.33 0.57 0.48 0.37 0.26 0.34 0.56 Ba 538 541 3 504 142 162 201 1 201 2 181 1 429 500 141 La 9.38 6.80 8.76 10.30 9.66 12.80 10.10 7.57 7.26 7.55 8.57 Ce 14.90 10.90 12.30 13.80 13.20 19.60 14.70 10.20 9.43 10.30 13.10 Pr 1.87 1.36 1.48 1.64 1.54 2.40 1.74 1.19 1.10 1.14 1.58 Nd 6.89 4.96 5.51 5.91 5.45 8.58 6.36 4.23 3.92 4.18 5.85 Sm 1.33 1.03 1.02 1.08 1.01 1.68 1.16 0.82 0.69 0.75 1.13 Eu 0.31 0.24 0.55 0.23 0.20 0.35 0.33 0.35 0.31 0.20 0.24 Gd 1.37 0.95 1.11 1.23 1.07 1.76 1.15 0.86 0.81 0.89 1.09 Tb 0.21 0.15 0.17 0.19 0.18 0.30 0.19 0.14 0.13 0.13 0.19 Dy 1.27 0.96 1.07 1.13 1.08 1.96 1.11 0.77 0.78 0.84 1.17 Ho 0.29 0.21 0.25 0.27 0.28 0.46 0.27 0.19 0.20 0.21 0.30 Er 0.75 0.54 0.74 0.78 0.77 1.29 0.68 0.49 0.60 0.55 0.84 Tm 0.10 0.09 0.09 0.11 0.11 0.21 0.09 0.07 0.08 0.09 0.13 Yb 0.68 0.48 0.63 0.69 0.81 1.41 0.54 0.42 0.54 0.62 0.83 Lu 0.09 0.07 0.09 0.11 0.13 0.21 0.08 0.07 0.09 0.09 0.14 Hf 0.49 0.46 0.32 0.28 0.22 0.37 0.33 0.24 0.17 0.22 0.33 Ta 0.15 0.13 0.10 0.09 0.09 0.12 0.10 0.08 0.07 0.08 0.12 Pb 13.90 11.70 14.30 5.29 5.70 9.77 7.02 29.00 7.30 5.61 6.35 Th 2.33 2.10 1.57 1.39 1.14 1.88 1.53 1.09 0.88 1.05 1.81 U 5.12 3.40 4.44 6.43 4.84 7.89 5.51 4.17 3.41 4.16 6.93 ∑REE 49.30 35.67 43.14 47.59 45.30 68.17 47.66 34.15 32.88 34.58 44.71
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表 3 碳酸盐岩结核碳同位素(‰)分析结果
Table 3. Carbon isotope (‰) analytical results of the carbonate nodules
样品号 碳酸盐岩结核A 碳酸盐岩结核B 取样位置 内核带 过渡带 边缘带 内核带 过渡带 边缘带 取样编号 A-1-2 A-1-3 A-1-7 A-2-9 A-3-1 A-4-1 B-1-3 B-1-6 B-2-2 B-3-7 B-4-5 δ13C -6.51 -6.63 -6.71 -6.16 -6.11 -5.65 -6.76 -6.72 -6.12 -5.97 -6.37
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