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随着非常规油气勘探开发技术的发展和进步,页岩油气逐步成为我国油气勘探的重点领域(邹才能等,2010;郭彤楼,2014)。四川盆地作为我国页岩气勘探开发主战场,目前已在多套海相页岩层系中取得勘探开发突破,包括寒武系筇竹寺组、奥陶系五峰组、志留系龙马溪组、二叠系孤峰组等(董大忠等,2016;张金川等,2021;郭旭升等,2025)。“十四五”以来,DY1、FT1和LY1等井相继在大隆组取得页岩气勘探突破,彰显了上二叠统海相页岩气良好的勘探前景,并有望成为我国页岩油气增储上产的新层系(胡东风等,2023;明盈等,2023;杨雨等,2023;邹才能等,2024)。
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硅质矿物作为海相页岩中的重要矿物组成,往往形成于特定的地球化学条件和层位上,其成因及其硅质来源的研究,对于揭示古海洋、古气候和古构造具有重要意义(方雪等,2017;陈兰朴等,2025)。四川盆地上二叠统大隆组海相页岩主要分布于开江—梁平海槽内,周缘被生物礁灰岩所围绕,缺乏陆源物质输入,为典型的清水沉积环境(叶玥豪等,2024;马小刚等,2025;Xia Guodong et al.,2025)。前人针对大隆组富有机质硅质页岩成因机制做了大量研究,涉及生物成因、热液成因、交代成因和火山成因等多种成因(李红敬等,2009;周新平等,2012;方雪等,2017;杨雪等,2024),存在较大争议,特别是对于硅质形成过程中的硅质来源缺乏深入研究。
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海相页岩硅质成因与有机质富集之间的耦合机制对于评价页岩油气储层及勘探开发具有重要意义(遇昊等,2012)。前人针对奥陶系五峰组—志留系龙马溪组高陆源碎屑物质输入的典型“浑水沉积环境”下形成的硅质页岩认为其硅质成因与有机质富集之间存在一定耦合关系(卢龙飞等,2018),而对于研究区低陆源物质输入的典型“清水沉积环境”下形成的硅质页岩与有机质富集之间是否存在耦合关系尚不明确。
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为此,笔者等运用沉积学、矿物学、地球化学方法对川东地区DY1井大隆组硅质页岩开展研究,旨在讨论上二叠统大隆组硅质页岩成因和硅质来源,明确大隆组硅质形成与有机质富集之间的耦合关系,并建立硅质页岩发育模式,以期为川东地区上二叠统页岩气的勘探开发提供参考。
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1 区域地质概况
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晚二叠世Pangea大陆聚合达到鼎盛时期。华南板块位于Pangea大陆的东缘,古特提斯洋东南侧的中低纬度带(冯增昭等,1996)(图1a)。扬子板块夹于华夏板块和康滇古陆之间,此时期扬子板块主要以碳酸台地为主体,局部地区发育陆棚内盆地和滨海相沉积等。晚二叠世四川盆地位于扬子板块西北缘,该时期为四川盆地沉积充填与构造演化的重要阶段,古特提斯洋的扩张、峨眉山大火成岩省喷发(ELIP)和峨眉山地幔柱活动等一系列地质事件导致四川盆地发生强烈构造沉积分异,形成了隆凹格局的古地貌,并在盆地北缘形成一条北西—南东向裂陷槽(开江—梁平海槽)(何斌等,2003;马永生等,2006;王一刚等,2006;邱振等,2024)(图1b)。DY1井位于裂陷槽东侧(图1c),上二叠统自下而上依次发育吴家坪组和大隆组,其中大隆组地层厚约63 m,岩性从下至上发育硅质页岩、硅质灰岩、泥质灰岩和泥晶灰岩,下部硅质页岩为深水陆棚相沉积,上部泥质灰岩与泥晶灰岩为浅水陆棚相沉积(图1d)。
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图1 川东地区区域地质概况
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Fig.1 Overview of the regional geology of the eastern Sichuan Basin
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(a)二叠纪(约260 Ma)全球古板块再造图(据李江海等,2014修改);(b)华南板块乐平世古地理图(据何幼斌等, 2010修改);(c)川东地区长兴期古地理图(据文龙等,2025修改);(d)DY1井地层综合柱状图
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(a) Global palaeoplate reconstruction map of the Permian Period (ca.260 Ma) (modified from Li Jianghai et al., 2014&) ; (b) palaeogeographic map of the South China Block during the Lopingian Epoch (modified from He Youbin et al., 2010&) ; (c) palaeogeographic map of the Changhsingian age in the eastern Sichuan region (modified from Wen Long et al., 2025&) ; (d) comprehensive stratigraphic column of the Well DY1
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2 样品采集与实验方法
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2.1 样品采集
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笔者等研究样品采集自川东地区DY1井上二叠统大隆组取芯段岩芯(图1),共取岩芯样品20件,取样深度介于4330.0~4342.0 m,取样间隔约0.5 m/件。对20件所取样品开展总有机碳(TOC)分析、全岩X衍射(XRD)分析、主微量元素分析以及扫描电镜分析。
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2.2 实验方法
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薄片观察、扫描电镜和主微量分析测试在成都理工大学油气藏地质及开发全国重点实验室采用日本尼康公司E600型高级偏光显微镜、美国FEI公司Quanta250 FEG高分辨场发射扫描电子显微镜、荷兰帕纳科AXIOS Minerals(PANalytical)顺序式X射线荧光谱仪(XRF)和日本安捷伦Agilent 7500A型电感耦合等离子体质谱仪(ICP-MS)完成。
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TOC与全岩矿物测试在四川省科源工程技术测试中心有限责任公司采用Leco CS744碳硫分析仪与荷兰帕纳科X射线衍射仪(X’Pert MPD PRO)分别完成。
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2.3 数据分析方法
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对测试数据分析主要是为了对硅质页岩的元素异常、母岩分化和硅质成因进行分析,主要包括铈(Ce)异常、铕(Eu)异常值、富集系数、风化蚀变指数等。通过公式表示铈(Ce)异常;表示铕(Eu)异常; 为了排除陆源碎屑对微量元素的影响,采用Ixs =Isample-Alsample×来计算元素生物成因浓度(Algeo et al.,2011)。另外采用富集系数评价沉积岩中元素的富集程度(Tribovillard et al.,2006)。过量硅是指非碎屑来源的硅的总和,其包括了热液硅和生物硅,计算公式为(Holdaway et al.,1982):w(SiO2)EX(过量硅)=w(SiO2)Sample-。
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图2 川东地区DY1井大隆组一段主要矿物条形百分比分布图
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Fig.2 Percentage distribution of major minerals in Member 1 of the Dalong Formation from the Well DY1, eastern Sichuan Basin
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图3 川东地区DY1井大隆组一段岩相划分图 (改自叶玥豪等,2024)
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Fig.3 Lithofacies classification ofthe1st Member of the Dalong Formation in the Well DY1, eastern Sichuan Basin(modified from Ye Yuehao et al.,2024&)
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3 结果
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3.1 页岩岩相特征
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3.1.1 岩石矿物学特征
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通过对大隆组一段样品全岩X衍射实验分析可知:其矿物类型主要以石英为主,石英含量分布范围为17.2%~72.1%,平均为54.3%;方解石和黏土矿物含量次之,方解石矿物含量分布范围为5.7%~59.2%,平均为21.9%;黏土矿物含量分布范围为0~18.3%,平均为9.4%。此外,大部分页岩样品黄铁矿较发育,其含量为0~6.6%,平均为4.2%。纵向上,石英、黏土矿物等矿物含量在大一段中部分布较为平均;方解石含量在整体上具有随深度增加呈逐渐增大的趋势;斜长石含量则表现出随深度增加而减小的趋势(图2)。
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3.1.2 岩相特征
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笔者等采用页岩全岩矿物划分方案,结合薄片镜下鉴定,对大隆组一段页岩岩相进行划分,结果表明大隆组一段岩相主要以硅质页岩岩相为主,少数样品为钙质页岩岩相和混合质页岩岩相(图3)。
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硅质页岩颜色为黑色和深灰色(图4a),部分夹极薄的凝灰岩层(图4b、d)和钙质条带(图4c),薄片上可见大量硅质生物发育(硅质放射虫)(图4e—f),局部见方解石交代硅质放射虫壳体(图4f),未见石英脉体,扫描电镜下可见大量草莓状黄铁矿发育(图4j—l),硅质矿物类型以石英胶结物(图4k)和碎屑生物硅为主(图4l);混合页岩颜色为黑色—深灰色,薄片中见方解石脉体发育(图4g),钙质介壳生物和硅质生物零星发育(图4g);钙质页岩颜色为深灰色,主要以泥晶方解石为主,见钙球和介壳生屑,白云石零星发育(图4h—i),局部发生硅化(图4i)。
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3.2 地球化学特征
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3.2.1 有机质丰度
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川东地区DY1井大隆组一段岩芯样品总有机碳含量测试结果如表1所示,页岩样品TOC值分布范围为2.1%~15.8%,普遍大于2.00%,平均为7.26%,厚度约10 m,属于高富有机质页岩,纵向上大一段底部TOC含量低于大一段中上部(图7)。
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图4 川东地区DY1井大隆组一段典型页岩类型及硅质矿物特征
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Fig.4 Characteristics of typical shale types and siliceous minerals inthe1st Member of the Dalong Formation from the Well DY1, Eastern Sichuan Basin
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(a)黑色硅质页岩,DY1井,4334.70 m;(b)黑色硅质页岩夹薄层凝灰岩,凝灰岩层中黄铁矿十分发育,DY1井,4329.70~4329.82 m;(c)黑色硅质页岩夹钙质条带,钙质条带中黄铁矿零星发育,DY1井,4329.70~4329.82 m; (d)凝灰岩,DY1井,4340.70 m;(e)黑色含生屑硅质页岩,可见硅质放射虫,硅质壳体内有机质发育,DY1井,4331.10 m,单偏光;(f)硅质页岩,硅质放射虫发育,方解石交代放射虫壳体,DY1井,4341.31 m,单偏光;(g)混合质页岩,局部发生钙化,硅质生物和介壳生物零星发育,DY1井,4338.82 m;(h)钙质页岩,方解石钙球发育,DY1井,4298.75 m,单偏光;(i)黑色钙质页岩,零星可见白云石,介壳生物碎屑发育,DY1井,4331.42 m,单偏光;(j)硅质页岩,自生石英发育,石英与黏土矿物胶结,图中黄色十字为能谱点,DY1井,4330.57 m,ETD;(k)硅质页岩,石英胶结物,石英矿物边缘可见有机质,红色箭头所指为石英,DY1井,4331.10 m,BSED;(l)硅质页岩,生物石英发育,有机质与生物硅伴生,草莓状黄铁矿发育,DY1井,4336.70 m,BSED
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(a) Black siliceous shale, Well DY1, 4334.70 m; (b) black siliceous shale interbedded with thin tuff layers, with well-developed pyrite in the tuff layer, Well DY1, 4329.70~4329.82 m; (c) black siliceous shale interbedded with calcareous bands, with sporadically developed pyrite in the calcareous bands, Well DY1, 4329.70~4329.82 m; (d) tuff, Well DY1, 4340.70 m; (e) black bioclastic siliceous shale, showing siliceous radiolarians and organic matter developed within siliceous shells, Well DY1, 4331.10 m, PPL; (f) siliceous shale, with developed siliceous radiolarians, and calcite replacing radiolarian shells, Well DY1, 4341.31 m, PPL; (g) mixed shale, partially calcified, with sporadically developed siliceous organisms and shell organisms, Well DY1, 4338.82 m; (h) calcareous shale, with developed calcite spherulites, Well DY1, 4298.75 m, PPL; (i) black calcareous shale, sporadically containing dolomite, with developed shell bioclasts, Well DY1, 4331.42 m, PPL; (j) siliceous shale, with authigenic quartz developed and quartz cemented with clay minerals; the yellow cross in the image indicates the EDS point, Well DY1, 4330.57 m, ETD; (k) siliceous shale, quartz cement, with organic matter visible at the edges of quartz minerals; the red arrow points to quartz, Well DY1, 4331.10 m, BSED; (l) siliceous shale, with biogenic quartz developed, organic matter associated with biogenic silica, and developed framboidal pyrite, Well DY1, 4336.70 m, BSED
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3.2.2 主量元素
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DY1井大隆组一段硅质页岩主量元素分析在Al2O3—SiO2—CaO三端元图中显示SiO2(21.10%~66.98%,平均51.88%)和CaO(0.94%~24.25%,平均10.27%)是其最丰富的氧化物(图5),其次为Al2O3含量(均值为7.39%),然后依次为Fe2O3(均值为3.18%)、MgO(均值为1.87%)和K2O(均值为1.82%),其余主量元素含量均不足1%。总体上DY1井大隆组页岩具有较高的硅和相对较低的钙含量,这与页岩岩相划分结果具有一致性。Fe/Ti在5.46%~19.92%,均值为11.57%; Al/(Al+Fe+Mn)在0.46%~0.76%,平均0.62%; Al2O3/(Al2O3+Fe2O3)值为0.53%~0.83%,均值为0.70%; Fe2O3/TiO2在4.68%~17.07%,均值为9.91%(图7,表1)。在PAAS主量元素标准化元素富集系数图中,相对富集SiO2(均值为2.40)、Fe2O3(均值为1.18)、K2O(均值为1.24)、MgO(均值为3.63)、Na2O(均值为1.82),相对亏损TiO2(均值为0.85)(图6a)。
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图5 川东地区DY1井大隆组一段页岩Al2O3—SiO2— CaO三端元图(底图引自Wu Wei et al.,2021)
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Fig.5 Al2O3—SiO2—CaO ternary diagram for the shale from Member 1 of the Dalong Formation in Well DY1, Eastern Sichuan area (base map from Wu Wei et al., 2021)
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3.2.3 微量及稀土元素
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川东地区DY1井大隆组一段页岩样品在PAAS标准化微量元素标准化元素富集系数图中,显著富集Mo(MOEF均值为172.26),V、Cr、U、Ba、Ni、Cu、Zn和Rb等微量元素轻微富集(图6a)。ΣREE在41.04×10-6~202.11×10-6,均值为88.46×10-6,具有左倾型的PAAS标准化REE配分模式,轻稀土元素(LREE=32.13×10-6~167.95×10-6,均值为74.89×10-6)相对重稀土元素(HREE=6.66×10-6~34.16×10-6,均值为13.57×10-6)富集(图6b);(La/Yb)N在0.33~1.56,均值为0.66;(La/Ce)N在0.76~1.54,均值为1.06;具有轻微负Eu异常(δEu=0.40~1.12,均值为0.85),无明显Ce异常(δCe=0.73~1.26,均值为0.97)。
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4 讨论
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4.1 硅质页岩大地构造背景
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硅质页岩成岩作用可导致SiO2含量变化(Brueckner et al.,1987;Murray et al.,1991;邱振等,2011),但主量元素Al、Fe、Ti及稀土元素相对稳定,能较好恢复其大地构造背景(Murray et al.,1994)。判别图显示,研究区样品主要落于大陆边缘构造区域,少数位于远洋盆地与大陆边缘过渡带(图8a、b)。结合样品(La/Yb)N(均值0.66)、δCe(均值0.97)与大陆边缘硅质页岩平均值((La/Yb)N均值0.75;δCe均值1.03)接近(Murray et al.,1990)。晚二叠世时期,受到峨眉地幔柱活动的影响,开江—梁平海槽发生差异性沉降,形成了被动大陆边缘型裂陷槽(陈旭等,2022)。强烈拉张的构造背景有利于深部富硅流体扩散至海洋中,为海水整体富硅创造地质条件。
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图6 川东地区DY1井大隆组一段页岩主微量元素及稀土元素分布图: (a)大隆组硅质页岩PAAS标准化下的主量元素和微量元素富集系数(EF)图;(b)大隆组硅质页岩PAAS标准化稀土配分模式图
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Fig.6 Distribution of major elements, trace elements, and rare earth elements (REE) in the shale from the1st Member of the Dalong Formation, Well DY1, eastern Sichuan Basin: (a) Enrichment factor (EF) diagram of major and trace elements in PAAS-normalized siliceous shale from the Dalong Formation; (b) PAAS-normalized rare earth element (REE) distribution pattern of siliceous shale from the Dalong Formation
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图7 川东地区DY1井大隆组一段页岩总有机碳、微量及稀土元素分布
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Fig.7 Distribution of total organic carbon (TOC) , trace and rare earth elements in the shale fromthe1st Member of the Dalong Formation, Well DY1, eastern Sichuan Basin
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图8 川东地区DY1井大隆组一段硅质页岩构造背景判别图(底图引自Murray,1994):(a)Fe2O3/TiO2— Al2O3/(Al2O3+Fe2O3)交汇图;(b)LaN/CeN—Al2O3/(Al2O3+Fe2O3)交汇图
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Fig.8 Tectonic setting discrimination diagram for siliceous shale from Member 1 of the Dalong Formation in Well DY1, Eastern Sichuan Basin (base map from Murray, 1994) : (a) Fe2O3/TiO2—Al2O3/ (Al2O3+Fe2O3) binary diagram; (b) LaN/CeN—Al2O3/ (Al2O3+Fe2O3) binary diagram
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4.2 页岩硅质来源
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4.2.1 陆源物质来源
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陆源碎屑的输入被认为是重要的硅质来源之一(房双艺,2021)。从古地理背景来看,研究区硅质页岩沉积于海槽内深水陆棚环境,周缘被长兴组生物礁灰岩所围绕,远离古陆,暗示其沉积时期缺乏陆源物质供给,处于“清水沉积环境”(图1c)。结合薄片镜下及扫描电镜下特征显示陆源碎屑石英几乎不发育(图4),表明大隆组沉积时期陆源物质对硅质的贡献较为有限。从地球化学角度来看,TiO2、Al2O3和∑REE等指标的相关性分析一定程度上指示陆源物质在沉积过程中的供给程度(Lu Bin et al.,2018)。Al2O3含量大于0.5%的页岩样品易受到陆源碎屑的干扰,TiO2含量的高低可以指示陆源碎屑输入程度(Delvigne et al.,2012)。研究区样品Al2O3与∑REE关系图显示两者之间的相关性较弱(R2=0.13)(图9a),这说明陆源碎屑输入较少,且对硅质页岩的形成控制作用不强;Al2O3和TiO2的含量具有较高的正相关性(R2=0.92)(图9b),表明Ti来源于陆源碎屑,并以重矿物的形式赋存于黏土矿物中。Al2O3、TiO2与SiO2含量相关性较差(R2=0.0049,R2=0.0081)(图9c、d),陆源物质的增加对硅质含量无影响,表明硅质页岩中的Si为非黏土矿物来源,即陆源物质对研究区硅质页岩中硅质的贡献有限。结合古地理背景及地球化学特征分析,综合认为川东地区DY1井大隆组一段硅质页岩所受到的陆源碎屑的影响较小,陆源硅对硅质页岩中的硅质的贡献有限。
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图9 川东地区DY1井大隆组一段页岩硅质来源判别图解: (a)Al2O3—∑REE 交汇图;(b)Al2O3—TiO2 交汇图;(c)SiO2—Al2O3交汇图;(d)SiO2—TiO2交汇图
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Fig.9 Discrimination diagram for silica sources in the shale from Member 1 of the Dalong Formation, Well DY1, eastern Sichuan Basin: (a) Al2O3—ΣREE diagram; (b) Al2O3—TiO2 diagram; (c) SiO2—Al2O3 diagram; (d) SiO2—TiO2 diagram
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4.2.2 热液来源
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受峨眉地幔柱活动的影响,晚二叠世川东地区处于拉张背景,洋基底发生断裂为热液的发育和运移提供了通道,促进了硅组分溶解以及热液硅流体的上升,为硅质页岩中硅质的形成创造了条件(冯增昭等,1996;周永章等,2004;杜远生等,2006)。研究区岩石学特征显示大隆组一段没有明显的热液活动痕迹(图4)。热液来源硅稀土元素PAAS标准化配分模式曲线呈水平且具有LREE富集、δEu>1和LREE/HREE<1等特征(German et al.,1990;Murray et al.,1994),这些特征都与研究区左倾型稀土元素配分模式、亏损LREE、δEu(均值为0.85)<1和LREE/HREE(均值为5.74)>1的特征相悖。与典型的热液喷流沉积体系(显著Eu正异常且Ce负异常)存在成因机制的显著差异,表明研究区硅质与热液硅不具有亲缘性;此外,结合Al2O3/TiO2—Al/(Al+Fe+Mn)判别图进一步证实研究区硅质为非热液成因,属于正常海相沉积(图10a)。综上,认为研究区硅质页岩硅质来源几乎不存在热液活动的直接贡献。
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图10 川东地区DY1井大隆组一段页岩硅质成因判别图解: (a)Al2O3/TiO2—Al/(Al+Fe+Mn)图(底图引自黄虎等,2012);(b)Al—Fe—Mn三端元图解(底图引自Adachi et al.,1986);(c)Fe/Ti—Al/(Al+Fe+Mn)图解(底图引自王东安等,1995);(d)SiO2/Al2O3—Al2O3图解(底图引自黄虎等,2013)
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Fig.10 Discrimination diagram for the genesis of silica in the shale from Member 1 of the Dalong Formation, Well DY1, Eastern Sichuan Basin: (a) Al2O3/TiO2—Al/ (Al+Fe+Mn) diagram (base map from Huang Hu et al., 2012&) ; (b) Al—Fe—Mn ternary diagram (base map from Adachi et al., 1986) ; (c) Fe/Ti—Al/ (Al+Fe+Mn) diagram (modified from Wang Dongan et al., 1995&) ; (d) SiO2/Al2O3—Al2O3 diagram (base map from Huang Hu et al., 2013#)
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4.2.3 生物来源
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硅质生物的成岩转化是硅质重要的来源之一(Maliva et al.,1989)。研究区大隆组一段硅质页岩中含有丰富的放射虫,指示生物硅是大隆组硅质页岩硅质的重要来源之一(图4e、f)。主量元素(Mn、Fe、Al、Ti)受成岩作用影响较小,是区分热液成因和生物成因硅质的有效地球化学指标(Murray et al.,1994),Adachi等(1986)据此建立了Al—Fe—Mn三端元图解,图解显示大隆组硅质页岩多数分布于生物成因区域,极少数样品处于生物成因向热液成因过渡区域(图10b),表明硅质页岩主要受生物作用影响。王东安等(1995)通过研究现代海洋沉积物提出Fe/Ti和Al/(Al+Fe+Mn)比值来确定硅沉积水介质所处的环境状况。图解显示研究区样品主要落入生物成因硅质岩区域,明显受到生物化学沉积的影响(图10c)。由于Al2O3和TiO2受沉积、成岩和风化作用的影响较小,是判别硅质成因的重要地球化学指标,黄虎等(2013)在此基础上建立了SiO2/Al2O3—Al2O3和Al2O3/TiO2—Al/(Al+Fe+Mn)图解用于判别硅质成因。SiO2/Al2O3—Al2O3协变图解显示研究区样品偏离纯硅质岩与PAAS理论趋势线,硅化程度介于50%~70%,表明硅质形成受多种因素的影响,但生物作用的贡献占主导(图10d)。
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另外过量硅w(SiO2)EX是沉积物中生物硅的最佳判别指标之一(Dong Yixin et al.,2020),尽管可能包含陆源硅或热液硅的贡献(Gao Ping et al.,2020;Dong Tian et al.,2022),前文探讨了研究区硅质几乎不受热液影响,陆源硅贡献有限,因此,w(SiO2)EX值可有效约束生物硅含量。研究区大隆组硅质页岩样品的w(SiO2)EX值较高(均值12.79,占整体SiO2含量比例大于60%)进一步揭示硅质的形成以生物来源为主导。综合上述岩石学特征及地球化学特征表明研究区硅质页岩中硅质主要为生物成因硅,沉积方式以生物化学沉积为主。
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4.2.4 玄武岩淋滤
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在二叠系时期,由于峨眉山地幔柱事件,盆地内形成了大量峨眉山溢流玄武岩(韦恒叶等,2024)。玄武岩经过风化淋虑后形成硅酸后以溶液的形式注入水体并以非晶硅胶体的形式聚合沉淀,形成一定数量的硅质(杨康,2022)。前人研究认为硅质岩和玄武岩之间的亲缘关系通常通过对比两者之间的U、Th含量和U/Th比值来判别(周新平,2012)。峨眉山玄武岩U含量为1.0×10-6~1.97×10-6(均值1.57×10-6)、Th含量为4.63×10-6~8.1×10-6(均值7.13×10-6)和U/Th含量为0.16×10-6~0.32×10-6(均值0.22×10-6)(熊舜华等,1984)。研究区样品的U含量为3.29×10-6~29.36×10-6(均值14.97×10-6)、Th含量为2.15×10-6~39.40×10-6(均值8.30×10-6)和U/Th值为0.23×10-6~8.24×10-6(均值2.82×10-6)(表1),通过对比发现大隆组硅质页岩U含量变化范围大,与玄武岩均值差异显著,Th含量高于玄武岩中的含量。硅质页岩、玄武岩中的U、Th含量反映出硅质页岩与玄武岩亲缘性较差,表明玄武岩淋滤产生的硅源对硅质页岩中的硅质贡献较为有限。
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4.2.5 上升流
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上升流本身并不能形成硅质,但其作为硅质迁移的载体,可将深部富硅水体输送至陆架边缘表层,其溶解硅的含量通常高于其他环境一个数量级(周新平等,2012)。高磷硅含量的岩相组合与上升流活动也存在密切联系(Beauchamp et al.,2002),其作用机制体现在深部富硅流体经上升流输送至浅层氧化—还原水体时,通过吸附沉淀和胶结作用促进硅质生物沉积,并在成岩脱水过程中形成硅质富集层(杨康,2022)。研究区可见大量放射虫硅质页岩,部分放射虫和介壳生物在镜下以生物碎屑的形式聚集(图4l),表明这些生物生活在间歇性水动力的环境中,为上升流的存在提供了证据(葛小瞳,2024)。此外,基于研究区样品化学特征显示:大隆组Co×Mn值0.12~0.61(均值0.38)、Cd/Mo比值0.01~1.57(均值0.35)(表1),与Sweere等(2016)建立的上升流判别指标(Co×Mn<0.4且Cd/Mo>0.1)高度吻合,进一步表明研究区上升流活动的存在。上升流的发育一方面导致深部的硅质被带到浅层海水中,随后以吸附或胶体的方式沉淀;另一方面上升流发育区大量硅质生物死亡、沉淀,并在成岩过程中脱水,提供十分可观的硅质来源(杨康,2022)。
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4.2.6 火山活动
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火山活动是硅质的重要来源,一方面火山物质可直接输入硅质矿物,另一方面其将火山物质中的硅溶解于海洋中,提高海洋溶解硅浓度促进海洋中硅质生物的发育繁盛从而间接提供硅源(Zhang Bolin et al.,2023)。研究区上二叠统地层发育多期火山事件沉积(Shen Jun et al.,2014,2019; Wang Xiangdong et al.,2018,2019),大隆组硅质页岩段内可见凝灰岩层(图4b),表明这一时期存在火山活动,但确定火山活动对硅质的形成贡献需结合多指地球化学约束(Zr>160×10-6、Hf>2.8×10-6、Zr/Cr>1.0、10000 Zr/Al2O3>6.0、K2O/Rb>200×104、10000 V/Al2O3<20、10000 Ni/Al2O3<10和10000 Cr/Al2O3<10)(Yang Shengchao et al.,2022),通过对比发现尽管研究区硅质页岩层中偶见火山灰夹层(图7),但火山活动图解显示研究区硅质中几乎不含火山物质(图11a—f),揭示研究区硅质页岩中硅质来源于火山活动所产生的硅直接贡献较少,火山活动可能通过火山灰和富硅流体扩散至海洋中,使海洋富硅从而间接影响硅循环。
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综合以上分析,认为川东地区DY1井大隆组一段硅质页岩中硅质主要来源于硅质生物,受陆源硅的贡献较小,不存在热液硅、玄武岩淋滤硅和火山物质硅的直接贡献。硅质生物中的硅主要来源于上升流携带深部富硅水体至表层为硅质生物提供溶解硅供应,海洋富硅水体的形成可能为东特提斯洋硅质沉积事件(姚旭等,2013)、峨眉地幔柱活动(邱振等,2024)、洋基底断裂以及热液活动事件的叠加(邱振等,2011;赵振洋等,2020)。Fe/Ti和Al/(Al+Fe+Mn)等指标显示与扬子地区生物化学沉积硅质岩具有相似性(图9c),表明研究区硅质页岩主要通过生物化学沉积作用形成。
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图11 川东地区DY1井大隆组一段页岩火山活动判别图解(底图引自Yang Shengchao et al.,2022): (a)Zr—Hf关系图;(b)Zr/Al2O3—Zr/Cr关系图;(c)K2O/Rb—Zr/Cr关系图;(d)Cr/Al2O3—V/Al2O3关系图;(e)Cr/Al2O3—SiO2/Al2O3关系图;(f)Cr/Al2O3—Ni/Al2O3关系图
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Fig.11 Discrimination diagram for volcanic activity in the shale from Member 1 of the Dalong Formation, Well DY1, Eastern Sichuan Basin (the base map from Yang Shengchao et al., 2022) : (a) Zr—Hf diagram; (b) Zr/Al2O3—Zr/Cr diagram; (c) K2O/Rb—Zr/Cr diagram; (d) Cr/Al2O3—V/Al2O3 diagram; (e) Cr/Al2O3—SiO2/Al2O3 diagram; (f) Cr/Al2O3—Ni/Al2O3 diagram
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4.3 硅质页岩与有机质富集之间的耦合关系
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通过前文研究可知研究区硅质页岩成因主要以生物成因为主,因此,讨论硅质页岩与有机质富集之间的耦合关系实质上是讨论硅质生物与古生产力的关系(卢龙飞等,2018;Dong Tian et al.,2022)。
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上升流作为关键的古海洋动力学过程,通过底流垂向运移作用将富营养元素的深部水体输送至透光带,有效促进浮游生物勃发并显著提升初级生产力(马小刚等,2025)。笔者等采用校正后的Cuxs(均值87.23×10-6)和Nixs(均值242.56×10-6)作为古生产力指标,其与总有机碳(TOC)呈现正相关性(图12a、b),且与建峰剖面同期富硅层段生产力指标接近(葛小瞳,2024),表明大隆组高有机质丰度与上升流驱动的高初级生产力密切关联。古特提斯洋扩张诱发的区域性海侵事件为上升流发育提供了有利的古地理条件(Yu Yamin et al.,2021)。此外,Cd/Mo比值与w(SiO2)EX具有正相关性(图12c),表明上升流与生物硅之间具有一定耦合性。综上多种指标可以推测上升流通过运输富硅富营养的水体,致使硅质生物大量繁盛,创造高生产力环境。
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火山灰携带大量营养元素输入可提升海洋初级生产力,局部改变水温,促进生物勃发,为生物化学作用提供介质条件和地球化学域,增强有机质形成和富集(Lin et al.,2011;李登华等,2014;方雪等,2017;邱振等,2019),同时其释放的有毒物质(Cu、Zn)也可能导致初级生产力下降,产生的气溶胶会增强行星反照率及水体缺氧程度,间接影响有机质保存条件(谢浩然等,2023)。研究区火山活动层段与高富有机质硅质页岩层段并不同步(图7),表明火山活动和营养物质输入之间耦合性较弱,未能导致大量营养物质输入海槽内,这可能与火山活动所产生的少量有机质在沉降分解过程中受氧化还原条件的改变而被消耗,致使火山活动对这一时期海洋初级生产力的提高相对较弱(邱振等,2019)。因此,虽然火山活动具备营养物质供给潜力,但对大隆组沉积期间以硅质生物为主导的微生物繁盛贡献有限。此外,来源于陆源输入的少量营养物质同样可为以硅质生物发育提供物质基础,从而间接提高海洋初级生产力。除上述硅质生物与高生产力之间具有相关性能间接说明硅质页岩与有机质的耦合性之外。研究区硅质页岩层段与高有机质富集层段共生(图7),生物硅与有机质呈正相关(图12d),岩石学特征显示硅质生物与有机质伴生(图4e、k、l),都是硅质页岩与有机质富集之间具有一定耦合性的直接证据。
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图12 生物成因硅与有机质判别关系图
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Fig.12 Discrimination diagram of biogenic silica and organic matter
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古生产力判别图解(a)TOC—CuXS交汇图,(b)TOC—NiXS交汇图;上升流与过量硅判别图解(c)w(SiO2)EX—Cd/Mo交汇图; 有机质与生物硅含量关系图(d)w(SiO2)EX—TOC交汇图
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Discrimination diagrams for paleoproductivity and upwelling (a) TOC—CuXS diagram; (b) TOC—NiXS diagram; Discrimination diagrams for upwelling and excess silicon (c) w (SiO2) EX—Cd/Mo diagram; (d) w (SiO2) EX—TOC diagram
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综合研究表明,海洋表层生态系统中藻类与硅质生物的繁盛受多源营养供给体系的共同驱动。有限的陆源输入与火山活动贡献的营养物质,为藻类及硅质微生物的初级生产提供了部分物质基础,而上升流将富营养物质和溶解硅送至透光层,促进了硅质生物的繁盛,提高了海洋初级生产力。结合研究区硅质页岩层段与高有机质层段具有同步发育特征(图7),且生物硅含量与有机碳含量存在正相关性(图12d),以及岩石学特征,均表明研究区生物成因硅质页岩与有机质富集之间存在耦合关系。
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4.4 硅质页岩发育模式
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通过上述研究可知,研究区硅质页岩形成与峨眉山地幔柱主导的被动大陆边缘构造背景,硅质页岩以生物成因为主,硅质生物的繁盛与上升流携带的富硅、富营养海水有关,生物成因硅与有机质存在伴生关系,形成了上升流—生产力—有机质富集耦合机制。结合前人对于该地区的区域构造事件、以及沉积环境的研究,最终建立了研究区被动大陆边缘裂陷槽型硅质页岩发育模式(图13)。
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大隆组一段沉积时期,研究区海水整体呈现富硅特征,这主要受峨眉山大火成岩省(ELIP)(Zhang Bolin et al.,2023)、东特提斯硅质沉积事件(姚旭等,2016)、洋基底断裂及热液活动的影响。同期,古特提斯洋的扩张引发了上扬子台地的大规模海侵,导致裂陷槽水体加深,为上升流的发育提供了有利条件。上升流将深部富硅水体及大量营养物质携带至浅层,与经过长距离搬运后残存的火山灰及陆源碎屑营养物质共同作用,显著促进了浅层水体中硅质生物和浮游生物的繁盛。研究区温暖湿润的古气候环境(韦恒叶等,2023;雍锐等,2025)进一步为生物发育提供了支持,大幅提高了水体初级生产力(图13a)。上升流海水的溶解硅浓度显著高于正常海水,其携带的大量硅质主要被繁盛的硅质生物吸收利用,少部分则以吸附形式附着于胶体或质点表面,最终以石英胶结物的形式沉淀(图13b)。同时,随水体深度增加导致的温度下降降低了硅的溶解度,致使海水中的硅达到过饱和状态,从而发生无机沉淀(图13c)。持续的海平面上升促进了水体垂向分层,主导了中下部水体缺氧—硫化环境的形成(Xia Guodong et al.,2025)。微生物的大量死亡消耗了水体中的溶解氧,加剧了缺氧状况;研究区内广泛发育的“草莓状”黄铁矿(遇昊等,2012;马小刚等,2025)也为该缺氧—硫化环境提供了可靠证据。这种缺氧—硫化的还原环境极有利于硅质页岩中有机质的保存。最终,在碎屑生物硅质(主要来源)与自生硅(次要来源)的共同作用下,研究区形成了有利于硅质富集、保存及过饱和沉淀的沉积环境,从而形成了大隆组一段广泛稳定分布的富有机质硅质页岩。
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图13 川东地区上二叠统大隆组一段富有机质硅质页岩发育模式图
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Fig.13 Developmental model of organic-rich siliceous shale in Member 1 of the Upper Permian Dalong Formation, Eastern Sichuan Basin
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(a)川东地区大隆组一段黑色页岩富集模式图;(b)有机质与生物硅伴生沉积;(c)自生硅过饱和沉积
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(a) Enrichment model of black shale in the1st member of the Dalong Formation in the eastern Sichuan region; (b) syndeposition of organic matter and biogenic silica; (c) authigenic silica supersaturated sedimentation
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与同样具有高硅质含量的奥陶系五峰组—志留系龙马溪组海相页岩相比,研究区大隆组硅质页岩在有机质丰度(TOC)、优质烃源岩厚度、硅质成因、硅质来源及沉积环境等方面均存在显著差异。五峰组—龙马溪组页岩平均TOC为3.31%(郭彤楼,2025),优质烃源岩厚度介于5~90 m(谢武仁等,2024),其硅质页岩成因主要受陆源作用与生物作用控制,并伴有少量热液贡献(郑爱维等,2023;李娟等,2024);硅质来源包括陆源碎屑石英、生物成因石英及自生微晶石英等(韩豫等,2024),形成于陆源输入活跃的“浑水沉积环境”(Xia Guodong et al.,2025)。而研究区大隆组海相页岩平均TOC大于7%,优质烃源岩厚度为5~10 m,硅质成因以生物作用为主导,硅质主要来源于上升流携带的富硅、富营养盐海水,形成于陆源碎屑输入受限的“清水沉积环境”。上述截然不同的沉积环境是造成两组页岩陆源碎屑输入差异的关键,并最终导致其硅质页岩成因机制的本质区别。笔者等将为深入理解低陆源碎屑
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5 结论
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通过对川东地区上二叠统大隆组页岩进行岩石学、地球化学及硅质成因与有机质富集之间的关系研究,得出以下结论:
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(1)大隆组一段页岩岩性以硅质页岩为主,混合质页岩以及钙质页岩含量较少,有机质丰度较高,平均TOC达7.26%,矿物类型以石英为主,碳酸盐矿物次之,黏土矿物含量较低。
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(2)川东地区大隆组一段硅质页岩形成于峨眉山地幔柱事件主导的被动大陆边缘裂陷槽构造背景,硅质页岩中硅质来源以生物来源为主,几乎不存在陆源硅、热液硅、玄武岩淋滤硅以及火山硅的直接贡献。硅质生物的繁盛主要与富硅、富营养盐的上升流和区域构造事件引起的海水整体富硅有关。
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(3)上升流指标和生物硅含量指标均与生产力指标呈线性正相关,纵向上生物成因硅质页岩与高有机质丰度段相对应,以及镜下硅质生物与有机质的伴生关系等多种证据,揭示了研究区硅质页岩成因与有机质富集之间存在协同演化机制。
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(4)硅质页岩中有机质和硅质的富集同时受控于上升流驱动的原始海洋高初级生产力以及缺氧—硫化还原环境保存条件。
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摘要
二叠纪晚期受峨眉山地幔柱事件的影响,在四川盆地北缘开江—梁平海槽内沉积了一套富有机质硅质页岩,该套硅质页岩缺乏陆源物质输入,形成于典型的清水沉积环境,对其硅质成因及其与有机质富集之间的耦合关系进行研究,并在此基础上建立硅质页岩发育模式,以期为二叠系页岩气勘探开发提供参考。笔者等以川东地区上二叠统大隆组海相泥页岩为研究对象,开展了详细的岩芯观察、显微岩石学分析和全岩地球化学分析。结果表明:①大隆组富有机质泥页岩层段岩性以硅质页岩为主,有机质丰度较高,平均TOC达7.26%,矿物类型以石英矿物为主,碳酸盐矿物次之,黏土矿物含量较低;②硅质以生物来源为主,上升流带来的深部富硅水体与区域构造事件引起的海水整体富硅为硅质生物的繁盛提供了条件;③有机质富集与硅质的富集密切相关,硅质页岩中有机质和硅质富集同时受控于高初级生产力和缺氧—硫化还原环境保存条件,揭示出页岩硅质成因与有机质富集之间存在协同演化机制。
Abstract
Objectives: In the late Permian period, influenced by the mantle plume event of Mount Emei, a set of organic-rich siliceous shale was deposited in the Kaijiang—Liangping trough on the northern margin of the Sichuan Basin. This set of siliceous shale lacked the input of continental materials and was formed in a typical clear water sedimentary environment. The siliceous genesis of this set and its coupling relationship with organic matter enrichment were studied, and on this basis, the development model of siliceous shale was established. In order to provide a reference for the exploration and development of Permian shale gas. This paper takes the Marine shale of the Dalong Formation of the Upper Permian in the eastern Sichuan region as the research object and conducts detailed core observation, micro-petrological analysis and whole-rock geochemical analysis.
Results: ① The lithology of the organic-rich mud shale section of the Dalong Formation is mainly siliceous shale, with a relatively high organic matter abundance, an average TOC of 7.26%. The mineral types are mainly quartz minerals, followed by carbonate minerals, and the content of clay minerals is relatively low. ② Siliceous organisms mainly come from biological sources. The deep silicon-rich water bodies brought about by upwelling and the overall silicon-rich seawater caused by regional tectonic events provide conditions for the prosperity of siliceous organisms. ③ The enrichment of organic matter is closely related to the enrichment of siliceous matter. The enrichment of both organic matter and siliceous matter in siliceous shale is simultaneously controlled by high primary productivity and the preservation conditions of anoxic—sulfidation reduction environment.
Conclusions: It reveals that there is a coevolutionary mechanism between the siliceous genesis of shale and the enrichment of organic matter.
