Geochemical characteristics and geological implications of dark shale in the second submember of the first member of the Qiongzhusi Formation, Ziyang–Weiyuan area, China
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摘要: 四川盆地资阳−威远裂陷槽内下寒武统筇竹寺组作为深层—超深层页岩气勘探的重点层系，展现出巨大的资源潜力。为精确阐明其核心优质层段（筇一段2亚段⑤小层深色页岩）的古沉积环境、生产力演化及有机质富集主控因素，以Z201井的黑色页岩样品为研究对象，系统开展了岩石学分析，并结合总有机碳（TOC）、主微量元素及稀土元素等地球化学指标进行综合表征。结果表明，筇一段2亚段⑤小层页岩的地球化学组成在垂向上具有显著的阶段性差异。TOC含量呈“低—高—低”变化趋势，⑤-2亚小层为峰值，平均含量3.72%；主量元素中Al2O3和TiO2在⑤-2亚小层呈现低值谷，指示陆源输入最低；氧化还原敏感元素（U、Mo、V、Ni等）在⑤-2和⑤-3亚小层富集，U、Mo富集因子及协变模式指示了强还原滞留环境；古生产力指标P/Ti与过量硅（Siexc）变化一致，均在⑤-2亚小层达到最高，而生物成因钡（Babio）因受硫酸盐还原菌对重晶石的分解作用而信号失真；化学蚀变指数（CIA）、Sr/Cu及Rb/K等指标则指示了总体稳定的气候与半咸水的沉积环境。综合分析认为，⑤-2亚小层由于较高的初级生产力、强缺氧的底层水体与最低的陆源稀释作用的耦合，导致了该层段有机质的富集，形成了优质烃源岩；而其他亚小层则由于更高的陆源稀释作用和/或水体复氧导致的有机质保存条件恶化，抑制了有机质的富集。Abstract:
Objective The Lower Cambrian Qiongzhusi Formation, situated within the Ziyang–Weiyuan rift of the Sichuan Basin, represents a key target for deep to ultra-deep shale gas exploration and exhibits considerable resource potential. However, the high-resolution paleo-environmental evolution and the specific controlling mechanisms of organic matter (OM) enrichment within the core high-quality interval (dark shale of Bed 5, Submember 2, Member 1 of the Qiongzhusi Formation) remain insufficiently understood. This study aims to precisely reconstruct the paleo-depositional conditions—including climate, salinity, redox, water restriction, terrigenous input, and productivity—and to clarify the main factors controlling OM accumulation. Methods To precisely elucidate the paleo-depositional environment, productivity evolution, and controlling mechanisms of organic matter enrichment within this interval, a systematic geochemical investigation, including analyses of total organic carbon (TOC), major, trace, and rare earth elements, was conducted on black shale samples from Well Z201. Results The geochemical composition of the shales in Bed 5 exhibits significant vertical phasic heterogeneity. TOC abundance displays a ‘low–high–low’ trend, peaking in Bed 5-2 with an average of 3.72 %. Amongst major elements, Al2O3 and TiO2 show a distinct trough in Bed 5-2, indicating minimum terrigenous input. Redox-sensitive trace elements (e.g., U, Mo, V, Ni) are enriched in Beds 5-2 and 5-3, with U and Mo enrichment factors (EFs) and covariation patterns indicating a strongly reducing and restricted environment. Conclusion Based on the integrated analysis of these geochemical proxies, this study reconstructs the paleo-environmental evolution and elucidates the mechanism of organic matter enrichment. The shale deposition occurred under a stable warm–humid to semi-humid climate within a brackish and hydrographically restricted basin. The bottom water redox conditions fluctuated significantly, evolving from dysoxic in Bed 5-1 to strongly anoxic and euxinic in Beds 5-2 and 5-3, before reoxygenating to dysoxic conditions in Beds 5-4 and 5-5. Concurrently, terrigenous detrital input dropped to a minimum in Bed 5-2 but intensified significantly from Bed 5-3 upwards, while primary productivity peaked specifically in Bed 5-2. Consequently, the formation of the core high-quality source rock in Bed 5-2 resulted from the optimal convergence of high primary productivity, strong anoxic preservation, and weak terrigenous dilution. In contrast, organic matter accumulation in other intervals was suppressed by intensified terrigenous dilution and/or the deterioration of preservation conditions. [ Significance ] These findings clarify the complex coupling mechanism driving organic matter accumulation in deep shelf environments, highlighting that preservation conditions and sedimentation dilution are as critical as primary productivity. -
图 1 研究区位置及地层综合柱状图
a—研究区位置；b—地层综合柱状图
Figure 1. Location and comprehensive stratigraphic column of the study area
(a) Location of the study area; (b) Comprehensive stratigraphic column
图 2 筇一段2亚段⑤小层页岩岩石学典型特征
a—灰黑色页岩，夹粉砂质条带，发育粉砂岩透镜体，⑤-2亚小层，4611.01~4611.18 m；b—灰黑色页岩，夹粉砂质条带，发育黄铁矿结核，⑤-3亚小层，4593.69~4593.92 m；c—灰黑色页岩，可见高角度裂缝，⑤-4亚小层，4581.40~4581.65 m；d—灰黑色粉砂质页岩，均质构造，⑤-2亚小层，4589.4 m，单偏光；e—深灰色含粉砂质页岩，纹层发育，⑤-3亚小层，4594.45 m，单偏光；f—灰黑色粉砂质页岩，可见硅质纹层，⑤-4亚小层，4583.55 m，单偏光
Figure 2. Typical petrological characteristics of shale in Bed 5, Submember 2, Member 1 of Qiongzhusi Formation
(a) Grayish-black shale interbedded with silty bands, containing silts tone lenses, Bed 5-2, 4611.01–4611.18 m (b) Grayish-black shale interbedded with silty bands, showing pyrite nodules, Bed 5-3, 4593.69–4593.92 m; (c) Grayish-black shale with high-angle fractures, Bed 5-4, 4581.40–4581.65 m; (d) Grayish-black silty shale showing homogeneous texture, Bed 5-2, 4589.4 m, plane-polarized light; (e) Dark-gray silty shale with well-developed laminae, Bed 5-3, 4594.45 m, plane-polarized light; (f) Grayish-black silty shale with siliceous laminae, Bed 5-4, 4583.55 m, plane-polarized light
图 3 Z201井筇一段2亚段⑤小层各地化指标垂向变化
Figure 3. Vertical variations of geochemical proxies in Bed 5, Submember 2, Member 1 of Qiongzhusi Formation, Well Z201
图 4 Z201井筇一段2亚段⑤小层稀土元素配分图
Figure 4. Rare earth element distribution pattern of Bed 5, Submember 2, Member 1 of Qiongzhusi Formation, Well Z201
图 5 Z201井筇一段2亚段⑤小层古气候、古氧相、古盐度和古生产力判别图解
Figure 5. Cross-plot discrimination diagrams of palaeoclimate, palaeoredox conditions, palaeosalinity, and palaeoproductivity for Bed 5, Submember 2, Member 1 of Qiongzhusi Formation, Well Z201
图 6 Z201井筇一段2亚段⑤小层页岩水体滞留程度判别图版
a—Mo/TOC关系；b—U–Mo协变模式图 （Algeo and Tribovillard，2009）
Figure 6. Discrimination diagrams of water mass restriction for Bed 5, Submember 2, Member 1 of Qiongzhusi Formation, Well Z201
(a) Cross-plot of Mo versus TOC; (b) U–Mo covariation patterns (Algeo and Tribovillard, 2009)
图 7 Z201井筇一段2亚段⑤小层沉积演化模式（剖面位置见图1）
Figure 7. Depositional evolution model for Bed 5, Submember 2, Member 1 of Qiongzhusi Formation, Well Z201 (The profile location is indicated by the blue polyline in Fig. 1)
表 1 Z201井筇一2亚段⑤小层地球化学综合指标统计表
Table 1. Statistics of comprehensive geochemical indicators of Bed 5, Submember 2, Member 1 of Qiongzhusi Formation, Well Z201
指标 ⑤-1亚小层 ⑤-2亚小层 ⑤-3亚小层 ⑤-4亚小层 ⑤-5亚小层 ⑤小层 TOC/% 0.68~2.53/1.81 2.86~5.46/3.72 2.05~2.30/2.17 1.80~2.19/1.98 1.38~2.10/1.71 0.68~5.46/2.13 主量元素/% SiO2 64.53~68.35/66.12 63.10~69.28/66.68 67.53~67.79/67.70 62.10~69.15/65.64 60.84~65.96/63.69 60.84~69.28/65.19 Al2O3 11.00~13.21/12.12 10.17~12.39/10.99 11.11~11.71/11.39 11.02~12.95/12.21 12.27~14.90/13.36 10.17~14.90/12.45 Fe2O3 5.16~6.82/5.95 4.45~6.33/4.95 4.87~4.99/4.95 4.73~7.52/5.76 5.19~7.35/5.89 4.45~7.52/5.64 CaO 0.95~2.67/1.75 1.41~2.45/1.71 1.25~1.62/1.49 1.64~2.00/1.87 1.59~2.34/2.01 0.95~2.67/1.85 K2O 2.64~3.30/2.92 2.30~3.14/2.63 2.56~2.77/2.66 2.58~3.05/2.88 2.83~3.44/3.14 2.30~3.44/2.94 P2O5 0.16~0.22/0.19 0.21~0.25/0.23 0.22~0.23/0.22 0.17~0.20/0.18 0.15~0.25/0.20 0.15~0.25/0.20 TiO2 0.41~0.51/0.48 0.49~0.57/0.52 0.54~0.57/0.55 0.51~0.57/0.55 0.54~0.66/0.59 0.41~0.66/0.55 微量元素/（μg/g） V 89.52~210.35/132.23 118.74~551.13/236.27 155.68~548.25/341.97 123.30~245.13/170.25 127.36~168.05/145.19 89.52~551.13/180.39 Cr 59.15~109.49/76.30 54.18~106.13/84.75 67.59~82.73/76.49 71.64~105.55/85.86 59.68~117.45/98.70 54.18~117.45/89.14 Ni 35.59~97.78/66.29 87.87~151.05/120.00 126.00~128.88/127.72 57.92~103.03/76.92 52.19~89.33/70.31 35.59~151.05/84.33 Co 14.52~18.18/16.58 13.72~17.44/15.15 14.21~16.44/15.19 13.74~15.30/14.50 14.37~16.66/15.65 13.72~18.18/15.56 U 5.62~12.30/9.71 25.66~45.71/36.70 31.49~39.57/36.82 14.23~25.94/19.01 8.49~18.48/12.58 5.62~45.71/19.19 Th 9.54~10.89/10.49 10.86~12.62/11.82 10.89~12.15/11.44 9.51~10.32/9.85 9.59~11.12/10.35 9.51~12.62/10.68 Mo 8.04~14.35/11.24 21.62~35.55/27.82 23.72~24.41/24.09 16.13~20.67/17.84 9.12~17.64/12.24 8.04~35.55/16.42 Ba 1366.67~1437.41/1409.30 1340.74~1604.54/1437.87 1420.76~1527.75/1480.65 1476.99~1540.72/1506.84 1499.74~1677.91/1615.07 1340.74~1677.91/1526.98 Sr 111.51~147.03/127.73 131.55~151.70/136.94 122.67~133.37/129.35 127.22~133.82/131.29 124.27~144.07/132.63 111.51~151.70/132.07 Cu 33.69~45.52/38.88 37.88~42.46/40.14 39.93~46.06/42.67 38.83~57.34/45.22 40.78~56.67/44.33 33.69~57.34/42.65 稀土元素
（NASC标准化）La 1.15~1.34/1.25 1.06~1.32/1.23 1.26~1.46/1.35 0.95~1.12/1.06 1.02~1.32/1.16 0.95~1.46/1.20 Ce 1.03~1.15/1.09 0.92~1.14/1.07 1.08~1.24/1.16 0.85~0.98/0.93 0.93~1.13/1.02 0.85~1.24/1.05 Pr 1.28~1.40/1.35 1.17~1.40/1.32 1.29~1.52/1.41 1.02~1.19/1.13 1.09~1.38/1.21 1.02~1.52/1.26 Nd 1.16~1.24/1.20 1.13~1.30/1.23 1.20~1.41/1.30 0.94~1.11/1.04 1.00~1.23/1.14 0.94~1.41/1.17 Sm 1.31~1.53/1.39 1.39~1.55/1.45 1.37~1.56/1.47 1.08~1.27/1.17 1.16~1.53/1.29 1.08~1.56/1.34 Eu 1.39~1.66/1.51 1.49~1.63/1.56 1.58~1.70/1.64 1.42~1.51/1.46 1.47~1.97/1.70 1.39~1.97/1.62 Gd 1.24~1.48/1.34 1.31~1.49/1.39 1.35~1.51/1.45 1.11~1.28/1.19 1.11~1.45/1.27 1.11~1.51/1.31 Tb 1.25~1.58/1.40 1.36~1.60/1.47 1.41~1.57/1.52 1.18~1.36/1.26 1.22~1.51/1.33 1.18~1.60/1.38 Dy 1.03~1.30/1.15 1.14~1.34/1.24 1.20~1.33/1.28 1.00~1.18/1.07 1.05~1.32/1.13 1.00~1.34/1.16 Ho 0.83~1.01/0.90 0.90~1.08/0.97 0.91~1.04/1.00 0.79~0.93/0.85 0.84~1.02/0.90 0.79~1.08/0.91 Er 0.81~0.99/0.88 0.90~1.06/0.96 0.91~1.06/0.99 0.82~0.91/0.86 0.86~1.02/0.92 0.81~1.06/0.92 Tm 0.91~1.09/0.98 0.98~1.18/1.05 0.97~1.17/1.08 0.92~1.01/0.97 0.97~1.17/1.06 0.91~1.18/1.04 Yb 0.81~0.94/0.86 0.82~0.97/0.90 0.84~0.98/0.93 0.85~0.94/0.89 0.90~1.02/0.96 0.81~1.02/0.92 Lu 0.75~0.95/0.85 0.77~0.97/0.86 0.80~0.96/0.89 0.83~0.89/0.85 0.86~1.00/0.93 0.75~1.00/0.89 ΣREE/(μg/g) 164.61~176.16/170.88 151.73~180.93/170.46 169.78~196.54/183.03 134.33~153.96/147.21 145.04~174.96/160.87 134.33~196.54/164.98 地球化学指标 δCe 0.84~0.85/0.84 0.83~0.85/0.84 0.83~0.84/0.84 0.85~0.86/0.85 0.84~0.89/0.86 0.83~0.89/0.85 δEu 1.07~1.13/1.11 1.05~1.16/1.10 1.10~1.16/1.13 1.18~1.30/1.24 1.20~1.44/1.33 1.05~1.44/1.22 UEF 2.88~5.7/4.48 11.66~23.90/19.02 15.13~20.04/18.23 6.18~13.24/8.97 3.46~8.46/5.36 2.88~23.90/9.14 MoEF 10.09~16.58/12.79 29.35~47.33/34.98 28.78~29.49/29.22 17.20~25.88/20.45 9.33~19.85/12.75 9.33~47.33/18.88 CIA 52.38~60.20/56.45 51.89~56.87/55.49 56.53~58.59/57.57 54.50~58.76/56.83 57.10~61.27/58.98 51.89~61.27/57.62 Sr/Cu 2.45~4.36/3.36 3.10~3.68/3.42 2.66~3.31/3.05 2.22~3.45/3.01 2.37~3.38/3.02 2.22~4.36/3.14 C值 0.52~0.78/0.64 0.49~0.66/0.57 0.56~0.61/0.59 0.52~0.79/0.61 0.52~0.71/0.59 0.49~0.79/0.60 U/Th 0.59~1.13/0.92 2.05~3.90/3.14 2.59~3.62/3.24 1.50~2.51/1.91 0.86~1.93/1.22 0.59~3.90/1.76 V/Cr 0.98~2.42/1.79 1.12~6.71/2.89 2.30~6.93/4.37 1.17~3.42/2.12 1.24~2.47/1.55 0.98~6.93/2.15 Ni/Co 2.45~5.38/3.90 5.04~10.95/8.06 7.84~9.03/8.44 3.79~7.50/5.37 3.34~5.52/4.50 2.45~10.95/5.47 Sr/Ba 0.0777~0.1076/0.0908 0.0837~0.1111/0.0958 0.0821~0.0939/0.0875 0.0847~0.0899/0.0871 0.0741~0.0896/0.0822 0.0741~0.1111/0.0869 S/TOC 0.0048~0.0146/0.0087 0.0013~0.0054/0.0030 0.0053~0.0122/0.0099 0.0059~0.0118/0.0084 0.0045~0.0147/0.0092 0.0013~0.0147/0.0081 Rb/K 0.0042~0.0046/0.0044 0.0041~0.0045/0.0043 0.0043~0.0047/0.0044 0.0043~0.0045/0.0044 0.0041~0.0045/0.0043 0.0041~0.0047/0.0043 Mo/TOC /(μg·g−1·%−1) 4.33~14.95/7.46 5.79~11.11/7.77 10.50~11.91/11.15 7.64~11.48/9.14 5.94~8.39/7.16 4.33~14.95/7.91 Mo/U 0.99~1.43/1.19 0.50~1.23/0.80 0.60~0.78/0.66 0.80~1.13/0.97 0.77~1.53/1.00 0.50~1.53/0.96 P/Ti 0.26~0.32/0.29 0.26~0.36/0.33 0.28~0.31/0.29 0.22~0.29/0.24 0.18~0.30/0.24 0.18~0.36/0.27 Babio/(μg/g) 874.76~957.28/928.24 915.69~1154.70/1001.46 979.82~1062.86/1028.46 988.73~1039.34/1022.25 1012.60~1133.99/1084.76 874.76~1154.70/1032.91 注：表中数据格式为“范围/均值”；样品总数为30块 
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