Origin of Inorganic Carbon Isotope Excursions in Ediacaran Doushantuo Cap Dolostone at Jiulongwan Section in East Yangtze Gorges
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摘要:
峡东地区埃迪卡拉纪陡山沱组盖帽白云岩中异常偏负的无机碳同位素（δ13CV‒PDB<‒40‰），是甲烷释放的关键地质证据，但其具体成因机制尚不明确.对九龙湾剖面陡山沱组盖帽白云岩中白云岩和自生碳酸盐岩的碳、氧、硫、锶同位素及元素地球化学进行对比研究.自生碳酸盐岩极低的无机碳同位素值，极大的硫酸盐和黄铁矿硫同位素变化范围，较低的δ18O（CAS，Brt）-δ34S（CAS，Brt）斜率，Δ33Spyrite-δ34Spyrite具有的负相关性，指示古海洋冷泉环境下AOM-MSR作用参与；氧化还原敏感元素显示自生碳酸盐岩（JF1和JF2）形成于缺氧环境，整个盖帽白云岩形成于氧化（/贫氧）‒缺氧‒氧化（/贫氧）‒缺氧‒氧化（/贫氧）环境转变；古水深指标指示在JF1和JF2阶段海平面分别下降；主、微量元素及锶同位素表明，JF1和JF2阶段陆源风化物质输入增加.九龙湾地区埃迪卡拉纪早期两次海退形成的海底缺氧环境和水化学条件改变，是形成极负无机碳同位素组成的重要原因.
Abstract:Extremely negative inorganic carbon isotope values (δ13CV‒PDB<‒40‰) from the Ediacaran Doushantuo cap dolostone in East Yangtze Gorges were taken as key evidence for a methane release event, but the origin of the cap dolostone remain contested. Here we investigated carbon, oxygen, sulfur, and strontium isotopes, and major and trace element compositions in both authigenic carbonates and dolostones from the Doushantuo cap dolostone at the Jiulongwan Section. Authigenic carbonates show extremely negative inorganic carbon isotope values, remarkably wide ranges of sulfur isotope values for sulfates and pyrites, a positive δ18O(CAS, Brt)-δ34S(CAS, Brt) correlation with a low slope, and a distinctly negative Δ33Spyrite-δ34Spyrite correlation, which indicates that the extremely 13C-depleted carbonates were deposited from seawater via anaerobic oxidation of methane coupled to microbial sulfate reduction (AOM-MSR) at paleo-marine cold seeps. Redox-sensitive elements reveal that the authigenic carbonates (JF1 and JF2) were deposited in an anoxic condition, while the whole cap dolostone was deposited in transitional conditions of suboxic-anoxic-suboxic-anoxic-suboxic. Paleodepth indicators imply that the sea level in the Jiulongwan area dropped during the JF1 and JF2 stages, respectively. Results of major and trace elements and strontium isotopes demonstrate that the input of terrigenous weathered materials increased during the JF1 and JF2 stages. In Early Ediacaran Epoch, two regressions in the Jiulongwan area resulted in an anoxic environment and altered hydrochemical conditions, which is an important origin for the extremely negative inorganic carbon isotopes observed in the cap dolostone in this area.
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图 1 扬子板块埃迪卡拉纪沉积古地理（a、b）和黄陵背斜周缘地质简图（c）
a、b. 修改自Jiang et al.，2011；
魏昊明，2019 ；c. 修改自An et al.，2015Fig. 1. Paleogeographic map of Ediacaran depositional environment in the Yangtze Block (a, b) and sketch map around Huangling anticline (c)
图 2 九龙湾盖帽白云岩地层、岩石手标本和镜下照片
a. 九龙湾盖帽白云岩（C1+C2+C3）野外露头，南沱组冰碛砾岩与盖帽白云岩呈整合接触关系，照片中人身高1.75 m；b. 盖帽白云岩C2中顺层产出灰岩透镜体；c. HNYD06白云岩手标本，数据为微钻取样后测得的方解石胶结物无机δ13CV‒PDB值（‰）；d. HNYD27-2灰岩透镜体手标本，数据为微钻取样后测得的无机δ13CV‒PDB值（‰）；e.白云岩中方解石胶结物显微照片（正交偏光）；f. 灰岩透镜体中方解石脉显微照片（单偏光）
Fig. 2. Stratum, specimens and microscopic photographs of the cap dolostone at the Jiulongwan Section
图 3 九龙湾盖帽白云岩剖面及碳、氧、硫同位素组成变化
a. 碳酸盐无机碳同位素组成；b. 碳酸盐氧同位素组成；c. 硫酸盐（CAS和Brt）硫同位素组成；d. 硫酸盐（CAS和Brt）氧同位素组成. 剖面柱状图据Wang et al.，2008修改
Fig. 3. Stratigraphic column and carbon, oxygen and sulfur isotope profiles of the cap dolostone at Jiulongwan Section
图 4 九龙湾剖面盖帽白云岩碳、氧同位素及锶含量之间相关性
a. 白云岩碳、氧同位素相关性；b.自生碳酸盐岩碳、氧同位素相关性；c. 白云岩+自生碳酸盐岩的碳同位素与锶含量相关性；d. 白云岩+自生碳酸盐岩的氧同位素与锶含量相关性
Fig. 4. Correlations of carbon isotopes, oxygen isotopes and strontium contents of the cap dolostone at Jiulongwan Section
图 5 U、Mo、V含量与Al2O3、Th和Zr含量之间相关性
Fig. 5. Correlations between U, Mo, and V contents and Al2O3, Th, and Zr contents
图 6 九龙湾盖帽白云岩硫、氧同位素组成相关性
图a、b、c分别为白云岩、自生碳酸盐岩JF1和JF2的δ34S（CAS、Brt）与δ18O（CAS、Brt）相关性；图d、e、f分别为白云岩、自生碳酸盐岩JF1和JF2的δ34S（pyrite）与δ34S（CAS）相关性
Fig. 6. Correlations between sulfur isotopes and oxygen isotopes of the cap dolostone at Jiulongwan Section
图 8 九龙湾盖帽白云岩（a）与典型海水（b）的PAAS标准化稀土元素配分模式
Fig. 8. PAAS-normalized REE patterns in the cap dolostone at Jiulongwan section (a) and in typical seawater (b)
图 9 九龙湾盖帽白云岩无机碳同位素异常成因示意图
Fig. 9. Schematic diagram illustrating the origin of inorganic carbon isotope excursions in the cap dolostone at Jiulongwan Section
表 1 峡东九龙湾剖面盖帽白云岩硫、氧、锶同位素组成
Table 1. Sulfur, oxygen, and strontium isotopes of the cap dolostone at Jiulongwan Section
样品编号 岩性/矿物 δ34SCAS
（V-CDT, ‰）δ18OCAS
（V-SMOW, ‰）δ34SBrt
（V-CDT, ‰）δ18OBrt
（V-SMOW, ‰）δ34SPy
（V-CDT, ‰）$ \frac{{}^{87}\mathrm{S}\mathrm{r}}{{}^{86}\mathrm{S}\mathrm{r}}\left(1\sigma \right) $ HNYD01 白云岩 41.79 11.80 35.77 ‒ ‒ ‒ HNYD03 白云岩 39.52 ‒ 42.00 12.90 ‒ ‒ HNYD06 方解石胶结物 44.09 ‒ 42.10 12.24 26.07 0.711 50(1) HNYD07 方解石胶结物 31.73 14.54 27.44 ‒ 15.74 ‒ HNYD11 白云岩 29.17 15.73 ‒ ‒ 27.76 0.709 34(2) HNYD16-17 白云岩 29.85 ‒ ‒ ‒ 24.45 0.710 19(1) HNYD25 白云岩 30.16 15.11 ‒ ‒ 30.12 0.710 23(1) HNYD27-1 灰岩透镜体 46.72 13.34 39.83 ‒ ‒ ‒ HNYD27-2 灰岩透镜体 45.26 12.16 35.10 7.53 27.99 0.710 77(1) HNYD27-3 灰岩透镜体 49.54 ‒ 46.90 ‒ 11.62 0.710 53(1) HNYD28-1 灰岩透镜体 39.01 10.42 35.41 ‒ ‒ ‒ HNYD28-2 灰岩透镜体 54.31 ‒ 60.18 15.21 41.15 0.712 70(3) HNYD29-1 灰岩透镜体 52.33 12.12 52.96 ‒ 32.51 ‒ HNYD29-2 灰岩透镜体 44.27 10.91 47.03 10.87 8.18 ‒ HNYD31-32 白云岩 25.93 16.06 ‒ ‒ 33.41 0.709 35(1) JLW-C1-1 亮晶方解石脉和胶结物 79.3 20.1 ‒ ‒ 69.8 ‒ JLW-C1-1-2 亮晶方解石脉和胶结物 80.1 22.2 ‒ ‒ 73.4 ‒ JLW-C1-3 亮晶方解石脉和胶结物 58.2 19.7 ‒ ‒ 50.6 ‒ JLW-C1-4 亮晶方解石脉和胶结物 39.0 15.0 ‒ ‒ 38.4 ‒ JLW-C1-6 亮晶方解石脉和胶结物 58.8 16.1 ‒ ‒ 43.2 ‒ 注：JLW开头样品引自 Peng et al.（2022） ，其他数据为本文测定；“‒”表示该项分析未测或未测出.
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表 2 九龙湾剖面盖帽白云岩主、微量元素和有机碳含量及相关计算结果
Table 2. Results of major and trace element and total organic carbon contents of the cap dolostone at Jiulongwan Section
样品编号 岩性 主量元素（%） 微量元素（10-6） TOC
（%）U/Th Mn/Sr Zr/Al Sr/Ba V/(V+Ni) Al2O3 CaO MgO K2O MnO Fe2O3 U Mo V Th Ni Zr Sr Ba HNYD01 白云岩 4.01 35.68 2.28 0.61 0.52 3.50 1.11 1.62 16.20 3.22 18.70 49.80 357.0 2 000.0 0.072 0.34 11.2 23.5 0.18 0.46 HNYD06 自生碳酸盐岩 1.56 44.88 4.71 0.14 0.61 0.96 1.21 0.30 15.44 1.04 12.51 24.20 481.0 3 080.0 0.133 1.16 9.8 30.9 0.16 0.55 HNYD07 自生碳酸盐岩 1.00 32.41 13.22 0.24 0.33 1.03 1.00 0.37 10.31 0.70 12.42 19.00 141.0 525.0 0.044 1.43 18.2 36.0 0.27 0.45 HNYD11 白云岩 1.25 30.33 16.55 0.26 0.16 0.62 0.61 0.16 8.26 1.01 23.67 16.40 90.7 20.0 0.075 0.60 13.8 24.8 4.54 0.26 HNYD16-17 白云岩 1.22 31.43 16.71 0.26 0.27 0.76 0.77 0.22 9.92 1.97 20.91 16.00 101.0 25.4 0.076 0.39 20.8 24.8 3.98 0.32 HNYD25 白云岩 1.48 31.13 16.93 0.33 0.28 0.75 1.04 0.14 9.34 1.54 9.75 13.20 93.4 20.0 0.074 0.68 23.3 16.8 4.67 0.49 HNYD27-2 自生碳酸盐岩 0.84 44.54 1.89 0.21 0.93 1.05 2.18 0.25 65.90 0.45 17.04 15.10 197.0 209.0 0.126 4.84 36.5 34.1 0.94 0.79 HNYD28-2 自生碳酸盐岩 0.66 47.89 2.87 0.17 1.09 0.88 1.36 0.17 16.20 0.31 7.17 10.90 254.0 4 640.0 0.086 4.39 33.2 31.4 0.05 0.69 HNYD29-1 自生碳酸盐岩 0.75 43.71 3.34 0.20 1.13 1.10 2.07 0.22 26.20 0.21 7.68 24.80 198.0 396.0 0.182 9.86 44.2 62.4 0.50 0.77 HNYD31-32 白云岩 1.32 30.28 18.52 0.33 0.27 0.91 1.00 0.25 8.54 1.16 10.87 12.00 98.6 195.0 0.779 0.86 21.5 17.2 0.51 0.44
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表 3 九龙湾剖面盖帽白云岩稀土元素含量(10-6)及相关计算结果
Table 3. Results of rare earth element contents (10-6) of the cap dolostone at Jiulongwan Section
样品编号 岩性 La Ce Pr Nd Sm Eu Gd Tb Dy Y Ho Er Tm Yb Lu Y/Ho ΣREE+Y δCe δEu HNYD01 白云岩 16.58 38.45 4.54 19.31 3.95 1.07 3.42 0.50 2.64 15.59 0.46 1.06 0.15 0.90 0.13 33.54 108.77 1.02 1.47 HNYD06 自生碳酸盐岩 2.02 4.15 0.45 1.88 0.35 0.08 0.36 0.05 0.29 2.02 0.05 0.13 0.02 0.14 0.02 38.80 12.01 1.00 1.31 HNYD11 白云岩 2.19 4.67 0.53 2.23 0.48 0.11 0.41 0.07 0.39 3.27 0.08 0.22 0.03 0.23 0.03 41.38 14.95 1.00 1.17 HNYD16-17 白云岩 2.48 4.78 0.61 2.53 0.54 0.14 0.52 0.10 0.60 5.70 0.13 0.36 0.06 0.40 0.07 44.50 19.01 0.89 1.40 HNYD25 白云岩 1.76 3.64 0.40 1.81 0.37 0.09 0.36 0.06 0.37 2.89 0.08 0.20 0.03 0.24 0.03 34.51 12.35 0.99 1.24 HNYD27-2 自生碳酸盐岩 8.95 17.17 1.52 6.47 1.24 0.34 1.44 0.23 1.55 16.73 0.37 1.00 0.15 0.81 0.11 45.04 58.08 1.06 1.26 HNYD27-3 自生碳酸盐岩 14.34 31.59 3.32 14.50 3.02 0.62 3.36 0.61 4.44 38.22 0.99 3.00 0.49 3.15 0.42 38.46 122.07 1.05 0.92 HNYD28-1 自生碳酸盐岩 12.72 32.20 3.07 13.53 2.86 0.61 3.01 0.56 3.85 31.80 0.85 2.40 0.40 2.45 0.34 37.22 110.65 1.19 0.97 HNYD29-1 自生碳酸盐岩 5.66 10.26 0.88 3.61 0.68 0.22 0.77 0.12 0.78 7.26 0.18 0.47 0.07 0.42 0.06 40.47 31.45 1.03 1.61 HNYD31-32 白云岩 2.00 3.98 0.46 1.91 0.44 0.10 0.39 0.06 0.45 3.11 0.09 0.24 0.04 0.23 0.03 36.18 13.53 0.95 1.29 注：δCe=2CeN/（LaN+PrN），δEu=2EuN/（SmN+GdN），下标N代表稀土元素经澳大利亚后太古代页岩（PAAS）标准化之后的数值.
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