魏世林, 焦鑫, 柳益群, 李红, 周鼎武, 吕亦然. (2024). 陆内裂谷湖相火山-热液沉积型白云岩研究进展* [J]. 古地理学报, 26(5): 1037-1057.
WEI Shilin, JIAO Xin, LIU Yiqun, LI Hong, ZHOU Dingwu, LÜ Yiran. (2024). Progress on volcanic-hydrothermal sedimentary dolostone in intracontinental lacustrine rift basin[J]. Journal Of Palaeogeography, 26(5): 1037-1057.   
Doi: 10.7605/gdlxb.2024.05.077
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陆内裂谷湖相火山-热液沉积型白云岩研究进展*
魏世林1, 焦鑫1, 柳益群1, 李红1, 周鼎武2, 吕亦然3
1 大陆动力学国家重点实验室,西北大学地质学系,陕西西安 710069
2 山东科技大学地球科学与工程学院,山东青岛 266590
3 中国科学院地质与地球物理研究所,北京 100029
通讯作者简介 焦鑫,男,1985年生,副教授,主要从事沉积岩石学、火山-热液沉积学、页岩油研究工作。E-mail: jxin807@163.com。

第一作者简介 魏世林,男,2000年生,硕士研究生,主要从事沉积学研究工作。E-mail: wsl1924@163.com。

收稿日期:2024-02-21 改回日期:2024-04-08
基金资助:*国家自然科学基金青年项目(编号: 41802120)与陕西省自然科学基础研究计划项目(编号: S2024-JC-YB-1766)联合资助
摘要

以富有机质黑色页岩为代表的页岩油、页岩气资源近年来成为全球范围内油气勘探、开发领域的研究热点。该岩性在中国陆相湖盆中主要为来源复杂的细粒沉积岩,其中发育有一类特殊的纹层状泥晶白云岩。该类白云岩的岩石学、矿物学微观特征和地球化学特征既区别于常见的次生白云石化成因白云岩,又与微生物成因白云岩不同,被定义为一类新型的火山-热液沉积型白云岩。在研读大量国内外文献的基础上,综述了现代湖相白云石全球分布及形成环境特征,并展示了白云岩成因模式研究进展。重点选择了均在拉张构造背景下所形成的三塘湖盆地和准噶尔盆地芦草沟组、酒西盆地下沟组和二连盆地腾格尔组发育的火山-热液沉积型白云岩为研究对象,并进行对比研究。发现该类白云岩的特征: (1)保留有完好的原始微米级纹层结构和微晶晶体,后期受到的成岩作用较弱; (2)与半深—深湖黑色泥页岩互层且缺乏蒸发作用特征,并含有不同比例的火山-热液矿物; (3)锶同位素显示成岩流体具有深源(壳-幔混合)特征; (4)含有丰富的有机物质,并与油气分布展现出较强的耦合关系。最后,提出应加强该类白云岩研究、 利用其蕴含的特殊地质信息进行构造背景示踪及探讨其与油气生成关系。

关键词: 白云岩成因; 湖相泥晶白云岩; 热液沉积; 黑色页岩; 裂谷盆地
中图分类号:P531 文献标志码:A 文章编号:1671-1505(2024)05-1037-21
Progress on volcanic-hydrothermal sedimentary dolostone in intracontinental lacustrine rift basin
WEI Shilin1, JIAO Xin1, LIU Yiqun1, LI Hong1, ZHOU Dingwu2, LÜ Yiran3
1 State Key Laboratory of Continental Dynamics,Department of Geology,Northwest University,Xi’an 710069,China
2 College of Earth Science and Engineering,Shandong University of Science and Technology,Shandong Qingdao 266590,China
3 Institute of Geology and Geophysics,Chinese Academy of Sciences,Beijing 100029,China
About the corresponding author JIAO Xin,born in 1985,is an associate professor in Northwest University. His research interests include sedimentary petrology,volcanic-hydrothermal sedimentology,and shale oil. E-mail: jxin807@163.com.

About the first author WEI Shilin,born in 2000,is a master degree candidate in Northwest University. He is engaged in sedimentology. E-mail: wsl1924@163.com.

Fund:Youth Program of the National Nature Science Foundation of China(No.41802120)and the Natural Science Basic Research Program of Shaanxi(No. S2024-JC-YB-1766)
Abstract

Organic-rich black shales,which represent shale oil and gas resources,have become a research hotspot in the field of oil and gas exploration and development in China and around the world in recent years. These lithologies consist mainly of complexly sourced fine-grained sedimentary rocks in continental lacustrine basins in China,among which a special type of laminated microcrystalline dolostone is developed. The petrological,mineralogical micro-features,and geochemical characteristics of this type of dolostone are distinct from the commonly dolostones formed by dolomitization and are also different from microbial mediated dolostones. Hence,the dolostones have been defined as a new type of volcanic-hydrothermal sedimentary dolostone. Based on extensive review of domestic and foreign literature,this paper summarizes the global distribution and environmental characteristics of modern lacustrine dolomites and presents the research progress on the models of origins of dolostone. The focus is on the comparative study of volcanic-hydrothermal sedimentary dolostones found in the Lucaogou Formation in Santanghu and Junggar Basins, the Xiagou Formation in Jiuxi Basin,and the Tengger Formation in Erlian Basin,all of which are formed in an extensional tectonic setting. Four characteristics are summarized as follows: (1)These dolostones are well-preserved with μm-scale laminated structure and microcrystallized,indicating latterly weak diagenesis. (2)They contain a variety of volcanic-hydrothermal minerals,and are interbedded with semi-deep to deep lacustrine black shale. Evaporite characteristics are lacking. (3)Strontium isotopes indicate that the diagenetic fluid has a deep source(crust-mantle mixed)characteristic. (4)They are rich in organic matters and show a strong coupling relationship with hydrocarbon distribution. Finally,it is recommended to enhance research on this type of dolostone,utilize its unique geological information for tracing tectonic backgrounds,and explore its relationship with hydrocarbon generation as future research directions.

Key words: dolomite origin; lacustrine microcrystalline dolostone; hydrothermal sedimentology; black shale; rift basin

随着世界范围内常规油气产量的不断下降, 以黑色页岩为主要代表的非常规油气资源在勘探开发中取得了一系列突破(邹才能等, 2020, 2023a; 姜在兴等, 2023; 金之钧等, 2023; 赵文智等, 2023)。自2010年以来, 中国在非常规油气资源领域发展迅速, 以湖相细粒沉积岩为主要岩性的富有机质黑色页岩, 作为非常规油气资源重要的生油岩和储集层因具有非常可观的油气勘探开发价值, 因而受到广泛关注(邹才能等, 2010; 贾承造等, 2012; Yu and Yuan, 2013; 李昌伟等, 2015)。统计发现, 中国多套重要的黑色页岩均分布于拉张作用下形成的被动大陆边缘盆地和裂谷盆地内(邹才能等, 2023b), 而在这些富有机质黑色页岩中均含有一类特殊的泥晶白云岩, 其岩石学、矿物学和地球化学特征既区别于常见的次生白云石化成因白云岩, 又与微生物成因形成的原生白云岩不同(柳益群等, 2010, 2011; 文华国等, 2014; 焦鑫等, 2017; 郑荣才等, 2018)。整体表现为: (1)保留有完好的原始微米级纹层结构和微晶晶体, 后期受到的成岩作用较弱; (2)与泥页岩互层且缺乏蒸发作用特征, 其矿物组分中含有不同比例的火山-热液矿物; (3)锶同位素显示成岩流体具有深源(壳-幔混合)特征; (4)含有丰富的有机物质, 并白云岩分布特征与油气资源展现出较强的耦合关系。因此, 无论是对解决“ 白云石问题” 等科学问题, 还是指导非常规油气勘探、开发的生产问题, 该类白云岩均具有极高的研究价值。郑荣才等(2003, 2006)最早在酒西盆地白垩系下沟组发现并报道了首例湖相“ 白烟型” 喷流沉积白云岩; 随后柳益群等(2010)在三塘湖盆地二叠系芦草沟组发现了热水沉积白云岩, 认为其形成与幔源热液活动密切相关; 钟大康等(2015)在二连盆地白音查干凹陷下白垩统腾格尔组发现湖相热水沉积白云岩, 认为其形成可能与火山活动和湖底热液作用有关; 张帅等(2018, 2020)在准噶尔盆地东部吉木萨尔凹陷中二叠统芦草沟组中发现热液喷流沉积白云岩, 认为其形成与幔源流体相关。

通过研读并梳理了大量前人资料, 综合归纳了近年来关于富有机制黑色页岩中的这类泥晶白云岩研究成果。通过对比国内外白云岩成因模式、全球湖相白云石的分布以及国内火山-热液型白云岩研究进展等方面, 旨在引起更多学者讨论该类白云岩成因, 探索其与页岩油气生成和构造背景示踪方面的科学问题。

1 白云岩成因模式

作为一种化学成分简单(CaMg[CO3]2)且地质时期分布广泛的矿物类型, 白云石自从其被发现并命名之后的200余年里, 其成因始终存在争议。由于厚度大且白云石成分较纯的白云岩(massive dolostone)主要分布于古生界和前寒武系, 而较新的地层中很少被发现(Given and Wilkinson, 1987; Warren, 2000)。该差异使得白云石被认为是一种典型的次生交代成因矿物。在实验室常温条件下模拟白云石生成的失败(Land, 1998), 表明在地表条件下白云石成核和沉淀存在动力学障碍。地质时期白云石的大量沉积与它现代沉积的缺失及不能在实验条件下模拟生成明显矛盾, 这就是著名的“ 白云石问题(dolomite problem)” (Petrash et al., 2017; Chang et al., 2020)。

目前关于白云岩成因主要为次生和原生成因2类(表 1; 表 2)。次生成因包括6类。根据白云石化的物理化学条件、Mg2+来源以及流体动力学机制可分为蒸发模式(Pray and Murry, 1965; Hsü and Siegenthaler, 1969)、渗透回流模式(Adams and Rhodes, 1960; Pray and Murry, 1965)、海水模式(Land, 1985)、混合水模式(Badiozamani, 1973)、埋藏模式(Zenger et al., 1980; Wierzbicki et al., 2006)和热液改造模式(Hardie, 1991; Smith, 2006; 赫云兰等, 2010)。不难看出, 次生成因主要强调蒸发作用所导致的元素过饱和。Kim 等(2023)通过数值模拟以及透射电子显微镜实验验证后, 提出溶液在过饱和与欠饱和状态之间频繁循环可促进白云石晶体快速生长, 从而为白云石在地表频繁改变的蒸发— 非蒸发环境中的形成提供了理论依据。进一步解释了为什么在实验中1000倍的过饱和条件下仍未能析出白云石(Land, 1998)。而埋藏模式与热液改造模式则是受到深部热液流体影响所致。

表 1 次生白云岩成因模式 Table1 Genetic models of secondary dolostone
表 2 原生白云岩成因模式 Table2 Genetic models of primary dolostone

原生白云岩成因目前主要包括微生物成因及热液沉积成因。 微生物可以通过自身新陈代谢机制促进白云石形成, 按照微生物代谢方式, 与白云石形成有关的微生物自身新陈代谢机制可分为硫酸盐还原反应(Vasconcelos and McKenzie, 1997; Mazzullo, 2000; Warthmann et al., 2000; Wright and Wacey, 2005)、甲烷生成作用(Mazzullo, 2000; Moore et al., 2004; Roberts et al., 2004; Kenward et al., 2009)、硫化物氧化(Moreira et al., 2004)和需氧异养模式(Sá nchez-Romá n et al., 2008; Petrash et al., 2017; 表 2)。

热液成因白云岩在地质学界中更为常见的是热液改造成因白云岩, 是指热液能够改变碳酸盐岩矿物的物理化学性质、结构构造和化学成分并形成白云岩(Smith, 2006)。但是近10余年诸多学者在许多含油气湖相盆地的重要页岩油型烃源岩中发现了与火山-热液活动相关的泥晶白云岩。其明显缺乏热液改造常见的重结晶特征(如“ 鞍状白云石” 等; 郑荣才等, 2003; 柳益群等, 2010; 钟大康等, 2015)。该类白云石具有明显的“ 原生” 特征, 且由于其成分较纯且分布较广而明显区别于微生物成因白云石。学者将富含这类白云石的白云岩称为火山-热液沉积型白云岩(郑荣才等, 2006; 柳益群等, 2010, 2011; 钟大康等, 2015; Jiao et al., 2023)。该类白云岩是来自深部的热液流体通过断裂或裂缝上涌后进入湖盆与湖水混合, 热液流体压力和温度降低导致白云石和伴生矿物连续沉淀后所形成(Yang et al., 2020)。这类白云岩的形成往往伴随着拉张构造运动。火山活动及深大断裂为热液上涌提供通道, 不仅带来了Ca、Si、Fe、Mg等白云石发育的物质基础(郑荣才等, 2006; 文华国等, 2009; Hollise et al., 2017), 而且热液可以提供较高的温度, 使湖底水温局部升高, 促进了白云石的成核与发育(Jiao et al., 2023)。

2 现代湖相白云石全球分布及形成环境特征

现代湖相白云石在全球主要大陆均有分布。目前有文献记录发育白云石的湖泊有近40个, 主要集中在北美、澳大利亚、欧洲、亚洲及非洲。将这些湖泊位置放于全球气候带分布图(图 1)中可发现, 它们主要分布于温带大陆性气候地区, 部分在热带草原气候地区和热带沙漠气候地区。在地中海、热带季风和热带雨林气候地区也有少量分布, 表明白云石多形成于温暖环境。进一步将这些湖泊位置放于全球干旱带分布图(图 2)中可发现, 它们主要围绕着干旱带分布, 表明一定的蒸发作用对白云石形成十分重要。

图 1 全球气候带及白云石发育湖泊分布
底图为全球卫星云图, 引自http://lpolaac.usgs.gov/products/astgtmv003/Fig.1 Global distribution of climate zone and dolomite precipitated lakes

图 2 全球火山、干旱带及白云石发育湖泊分布
底图引自“ 标准地图服务” , 网址http://bzdt.ch.mnr.gov.cn/Fig.2 Global distribution of volcanos, arid zone, and dolomite precipitated lakes

详细研究发现, 这些湖泊多数为封闭的浅水、蒸发咸水湖, 且呈碱性。但是位于美国加利福尼亚州东部的Deep Springs Lake(Meister et al., 2011)和位于北达科塔州的冰川湖Lake Agassiz(Liu et al., 2014)、位于奥地利的Lake Neusiedl(Zá molyi et al., 2017; Tolotti et al., 2021)和位于非洲加纳Lake Bosumtwi(Giresse and Makaya-Mvoubou, 2010)等均为开放湖泊, 同样发育有白云石。而位于非洲肯尼亚的开放湖泊Lake Bogoria(Cort et al., 2013, 2019; Renaut et al., 2017; Mccall, 2020)火山活动频繁, 湖泊中发育有典型的火山-热液矿物蒙脱石, 表明在白云石形成过程中可能受到了火山作用的影响。

然而, 上述湖相中发育的白云石含量普遍较低, 甚至仅为痕量。但位于意大利的开放湖Lake Specchio di Venere(Aiuppa et al., 2007; Cangemi et al., 2016, 2018)则沉积含量较高的白云石(Last, 1990)。该湖泊位于一个火山口内, 为非蒸发环境。湖泊沉积物除少量陆源碎屑外还含有火山物质, 在湖泊周围可见相当强烈的热液喷出活动, 表明其中大量生成的白云石与湖泊中火山热液作用密切相关。

目前相较于蒸发环境的浅水湖相白云石, 深水环境中形成的现代白云石报道非常少。这可能与目前深水湖盆沉积物、尤其是白云石研究采样较难和关注度较低有关。但富存于中国拉张盆地背景中的富有机质黑色页岩中的泥晶白云岩则具有半深湖— 深湖相沉积特征, 明显区别于目前主流的浅水原生白云岩成因。

3 火山-热液沉积型白云岩特征

火山-热液沉积型白云岩目前主要发现在新疆三塘湖盆地和准噶尔盆地、甘肃酒西盆地及内蒙古二连盆地(郑荣才等, 2003; 柳益群等, 2010, 2013; 钟大康等, 2015)。上述盆地中的白云岩具有如下几点明显的相似特征。

3.1 地质学特征

1)构造背景: 所处盆地在白云岩形成时期均与拉张构造背景有关, 均为经受伸展作用后形成的裂陷盆地(文华国等, 2014; 焦鑫等, 2017; Yang et al., 2020; 张帅等, 2020)。

2)地层组合: 白云岩均以层状或透镜状发育于富含有机质的细粒沉积岩中, 构成盆内重要的烃源岩。近年来富含有机质的细粒沉积岩被视为黑色页岩, 并作为页岩油或致密油油气藏生油岩及储集层进行生产与研究(周雪, 2022)。除三塘湖盆地芦草沟组是被夹于2套重要的陆相火山沉积地层以外, 其余白云岩发育层位均被夹于以砂岩— 粉砂岩为主的陆相沉积地层中(表 4)。

3.2 岩石矿物学特征

1)岩石学特征: 白云岩均以纹层状产出为主(图 3-A, 3-B, 3-C), 局部可见同沉积软变形构造(图 3-D), 表明白云石形成时期水体整体较为平静, 局部存在动荡。

图 3 火山-热液沉积型白云岩沉积学特征
A— 三塘湖盆地芦草沟组纹层状白云岩与深棕色富有机质纹层互层(Jiao et al., 2023), 单偏光; B— 酒西盆地下沟组纹层状泥晶白云岩(郑荣才等, 2018), 正交偏光; C— 二连盆地腾格尔组纹层状微晶白云岩(郭强等, 2012), 单偏光; D— 二连盆地腾格尔组纹层状微晶白云岩软变形沉积(郭强等, 2012), 单偏光Fig.3 Sedimentary characteristics of the volcanic-hydrothermal sedimentary dolostones

2)白云石矿物学特征: 白云石均以泥晶为主, 粒径多小于3 μ m, 有序度较低(0.17~0.60; 表 4), 但其自形程度总体较好, 多为半自形— 自形晶(图 4-A, 4-B, 4-C, 4-D), 甚至可见纳米级自形菱形晶体(图 4-A)。此外, 局部层位的白云石发生了明显的次生变化。例如, 三塘湖盆地中1口钻井集中出现了蒙脱石富集层位, 其中的白云石重结晶后粒度介于10~40 μ m之间, 并且边部发生的蛇纹石化(图 5-A), 代表了火山及相关热液活动对白云石的局部改造作用(Jiao et al., 2023)。准噶尔盆地芦草沟组中的白云石与硅质沉积共存时, 重结晶为10~50 μ m的球粒, 并显示含铁量不同的生长环带(图 5-B), 代表了热液流体的多期次交代沉积(张帅等, 2020)。二连盆地腾格尔组中的白云石也出现了典型的热液蚀变成因鞍形白云石(图 5-C; Yang et al., 2020)。

图 4 火山-热液沉积型白云岩中泥晶白云石矿物学特征
A— 三塘湖盆地芦草沟组火山-热液沉积型白云岩中白云石呈约1 μ m的自形晶体(Jiao et al., 2023), SEM; B— 准噶尔盆地芦草沟组他形微粉晶白云石(张帅等, 2020), SEM; C— 酒西盆地下沟组火山-热液沉积型白云岩中粒径为5~10 μ m的菱形铁白云石(红色箭头)(文华国等, 2014), SEM; D— 二连盆地腾格尔组火山-热液沉积型白云岩中白云石晶体呈大小约3 μ m半自形— 自形晶体(魏巍等, 2017), SEM。SEM— 扫描电镜Fig.4 Mineralogical characteristics of micro-crystalline dolomite in the volcanic-hydrothermal sedimentary dolostones

图 5 火山-热液沉积型白云岩中重结晶白云石特征
A— 三塘湖盆地芦草沟组火山-热液沉积型白云岩中白云石重结晶后边部被蛇纹石(红色箭头)交代(Jiao et al., 2023), XL; B— 准噶尔盆地芦草沟组硅质白云岩, 白云石呈球粒状, 自内向外由于含铁量不同而呈环带(张帅等, 2020), BS; C— 二连盆地腾格尔组火山— 热液沉积型白云岩中鞍状粗晶白云石, 边部呈弯曲弧形(郭强等, 2012), XL。XL— 正交偏光; BS— 电子探针背散射Fig.5 Mineralogical characteristics of recrystallized dolomite in the volcanic-hydrothermal sedimentary dolostones

3)伴生矿物: 总体上4个研究区火山-热液沉积型白云岩中白云石较纯, 但均含有少量的伴生矿物。除了包含常见的陆源碎屑颗粒(石英、斜长石、钾长石)外, 还含有不同比例典型的火山-热液成因矿物(图 6-A至6-F; 郑荣才等, 2006; 柳益群等, 2011; Yang et al., 2020; 张帅等, 2020; Jiao et al., 2023)。例如普遍存在的方沸石为碱性热液流体直接沉淀的产物或火山灰被湖水早期蚀变的产物(Li et al., 2021)。蒙脱石作为三塘湖盆地芦草沟白云岩中主要的黏土类型(图 6-A), 其成因也是由碱性火山岩被酸性流体蚀变或由湖水中的火山灰蚀变而形成(Jiao et al., 2023)。同时, 具有明显鸡骨状结构的火山玻屑也出现在白云岩中(图 6-B)。此外, 准噶尔盆地芦草沟组白云岩中所含有的钠长石和水铵长石(图 6-C), 也同样为火山-热液作用的产物(张帅等, 2020)。酒西盆地下沟组白云岩中存在的钠长石、重晶石及透闪石(图 6-E, 6-F), 也说明了火山热液对白云岩形成与成岩环境的影响(文华国等, 2014)。

图 6 火山-热液沉积型白云岩伴生特殊矿物特征
A— 三塘湖盆地芦草沟组火山-热液沉积型白云岩, 浅灰色碱性长石(黄色箭头)和蒙脱石以不同比例填充于白云石晶间孔中(Jiao et al., 2023), BS; B— 三塘湖盆地芦草沟组火山-热液沉积型白云岩中富含鸡骨状玻屑与棱角状晶屑(Jiao et al., 2023), PL; C— 准噶尔盆地芦草沟组火山-热液沉积型白云岩中白云石(Dol)呈~5 μ m的半自形晶体, 与水铵长石(Kf+Bdt)、方沸石(Ana)和钠长石(Ab)共生(张帅等, 2020), BS; D— 准噶尔盆地芦草沟组火山-热液沉积型白云岩, 白云石(Dol)与方沸石(Ana)、钠长石等矿物共存(张帅等, 2020), XL; E— 酒西盆地下沟组火山-热液沉积型白云岩中呈斑晶产出透闪石(文华国等, 2014), XL; F— 二连盆地腾格尔组火山-热液沉积型白云岩中的方沸石(Ana)与钠沸石(N)(钟大康等, 2018), SEM。BS-电子探针背散射; PL— 单偏光; XL— 正交偏光; SEM— 扫描电镜Fig.6 Mineralogical characteristics of associated minerals in the volcanic-hydrothermal sedimentary dolostones

4)有机物分布: 4个研究区白云岩中可见丰富的有机质纹层, 其中可见微生物藻类沉积(图 7), 并与火山-热液物质的分布呈较强的耦合关系(Jiao et al., 2020)。

图 7 火山-热液沉积型白云岩中有机碎屑及富藻有机质纹层
A— 三塘湖盆地芦草沟组火山-热液沉积型白云岩中纹层状富含有机物的微生物沉积(红色箭头)(Jiao et al., 2023), XL; B— 三塘湖盆地芦草沟组火山-热液沉积型白云岩富有机质层中海藻酸盐(红色箭头), 入射蓝光下的荧光图像(Jiao et al., 2023); C— 酒西盆地下沟组火山-热液沉积型白云岩中纹层状藻类沉积(郑荣才等, 2018), XL; D— 二连盆地腾格尔组火山-热液沉积型白云岩藻类纹层(郭强等, 2012), XL。XL— 正交偏光Fig.7 Organic particles and algal-rich organic lamination in the volcanic-hydrothermal sedimentary dolostones

3.3 地球化学特征

除上述相似岩石学特征外, 4个研究区的火山-热液沉积型白云岩在碳、氧同位素、稀土元素及锶同位素地球化学方面也具有相似的特征和少数差异性。

1)碳、氧同位素: 4个研究区白云岩的碳、氧同位素具有明显的一致性(图 8), 即明显的δ 13C正异常(介于1.79‰ ~10.16‰ 之间, 平均4.69‰)和 δ 18O 负异常(介于-22.70‰ ~-2.32‰ 之间, 平均-10.51‰)。这与其他常见类型白云岩的碳、氧同位素值有明显的不同。例如: (1)塔里木盆地下奥陶统蓬莱坝组埋藏成因白云岩均为负异常的δ 13C值(介于-2.91‰ ~0.01‰ 之间, 平均-1.41‰)和 δ 18O 值(介于-12.81‰ ~-5.52‰ 之间, 平均-8.30‰ ; Qiao et al., 2021)。(2)形成于潮间带的硫酸盐还原菌型白云岩δ 13C值(介于-10.30‰ ~0.87‰ 之间)主要呈负异常特征, δ 18O值(介于-3.2‰ ~4.3‰ 之间)没有明显正、负异常特征(Mazzullo, 2000)。(3)具有明显δ 13C正异常的形成于浅海潮下带的产甲烷菌型微生物白云岩(Mazzullo, 2000)。(4)加拿大不列颠哥伦比亚省中泥盆统Slave Point组热液蚀变白云岩δ 13C值(介于-2.51‰ ~-0.31‰ 之间, 平均-1.04‰)和 δ 18O 值(介于-16.73‰ ~-13.00‰ 之间, 平均-14.43‰)均为负异常(Lonnee and Mache, 2006)。此外, 4个研究区内白云岩碳、氧同位素值没有明显的相关性关系(R2=0.1682, n=54), 也表明该类白云岩未受到明显的成岩作用改变(文华国等, 2014), 这与其整体以泥晶白云石为主的矿物学特征一致。

图 8 火山-热液沉积型白云岩与次生白云岩及微生物白云岩的碳、氧同位素特征Fig.8 Carbon and oxygen isotopic characteristics of the volcanic-hydrothermal sedimentary dolostones, secondary dolostones, and microbial mediated dolostones

一般而言, 白云岩碳同位素正异常往往是受到了微生物产甲烷菌活动的影响(Mazzullo, 2000); 而氧同位素负异常则常与热液活动或淡水注入有关(Boni et al., 2000; Davies and Smith, 2006; Hollis et al., 2017)。4个研究区火山-热液沉积型白云岩碳同位素分布范围较为集中, 其中三塘湖盆地芦草沟组白云岩δ 13C值介于3.70‰ ~9.90‰ 之间, 平均5.60‰ ; 准噶尔盆地芦草沟组白云岩的δ 13C值介于4.16‰ ~10.20‰ 之间, 平均7.30‰ ; 酒西盆地下沟组白云岩δ 13C值介于1.79‰ ~5.82‰ 之间, 平均4.04‰ ; 二连盆地腾格尔组白云岩δ 13C值介于1.40‰ ~8.60‰ 之间, 平均3.65‰ 。Jiao 等(2023)认为三塘湖盆地芦草沟组白云岩δ 13C值正偏可能是白云岩形成过程中受到了来自幔源流体及微生物产甲烷菌活动的共同影响; 张帅等(2020)认为在准噶尔盆地芦草沟组中有机质埋藏量较高, 其生物生产量高导致同期湖水贫12C(张晓宝等, 2000; 张帅等, 2018), 湖水参与白云岩成矿流体导致δ 13C正异常; 文华国等(2014)和Yang 等(2020, 2021)均认为来自深部的热液流体上涌进入湖盆内后释放富12C的CO2导致白云岩δ 13C值正偏。综上, 微生物和深部流体活动可能作为导致4个研究区火山-热液沉积型白云岩碳同位素正异常的主要原因。

氧同位素整体分布范围较大, 三塘湖盆地芦草沟组白云岩 δ 18O 值介于-22.70‰ ~-3.10‰ 之间, 平均-14.00‰ ; 准噶尔盆地芦草沟组白云岩介于-9.81‰ ~-2.32‰ 之间, 平均-6.01‰ ; 酒西盆地下沟组白云岩 δ 18O 值介于-14.15‰ ~-5.89‰ 之间, 平均-10.24‰ ; 二连盆地腾格尔组白云岩介于-18.40‰ ~-4.30‰ 之间, 平均-12.60‰ 。结合矿物学特征发现, 粗晶白云石往往比微晶白云石更具负异常特征(图 8)。Jiao等(2023)认为三塘湖盆地芦草沟组白云岩 δ 18O 值负偏与热液流体的影响有关, 同时强烈的热液活动将导致氧同位素值更负。加之三塘湖盆地芦草沟组白云岩呈现出火山碎屑含量与白云石自形程度及有序度呈正相关的特点, 进一步说明白云石形成和生长过程中受到了强烈的火山-热液作用影响。张帅等(2020)、文华国等(2014)和Yang 等(2021)同样认为 δ 18O 值负异常与深部热液的局部高温作用相关。

2)稀土元素: 将4个研究区火山-热液沉积型白云岩的稀土元素数据进行PAAS标准化处理后分析显示: 这些白云岩的稀土元素蛛网图特征较为一致, 整体表现为Eu正异常较为明显的略平坦曲线(图 9)。该特征与埋藏模式重结晶白云岩(Qiao et al., 2021)较为类似, 而与湖相微生物碳酸盐岩具有轻微的Eu负异常特征(Chagas et al., 2016)明显不同。但由于4个研究区白云岩中白云石均以泥晶为主, 而非明显重结晶的白云石(图 6; 表 3), 因此两者在岩石学和矿物学特征缺乏相似性。其中三塘湖盆地芦草沟组白云岩δ Eu(介于1.09~1.62之间, 平均1.25; 焦鑫等, 2017)整体均表现为正异常。酒西盆地下沟组白云岩δ Eu(介于1.00~1.24之间, 平均1.16; 文华国等, 2014)整体为表现为正异常, 但是部分白云岩δ Eu介于1.05~0.95之间没有异常特征; 二连盆地腾格尔组白云岩δ Eu(介于1.01~1.41之间, 平均1.13; Yang et al., 2020)为4个研究区内白云岩δ Eu最低但仍表现为正异常。经过详细矿物学特征划分后发现, 以泥晶为主的白云岩δ Eu小于1.05, 而粗晶白云岩则大于1.05, 火山-热液沉积型白云岩δ Eu大小可能与白云石结晶程度呈正相关, 可能代表了热液高温的影响作用。

图 9 火山-热液沉积型白云岩、次生白云岩和微生物白云岩REE+Y模式Fig.9 REE+Y distribution patterns of the volcanic-hydrothermal sedimentary dolostones, secondary dolostones, and microbial mediated dolostones

表 3 全球发育白云石的湖泊特征统计 Table3 Characteristics of global dolomite precipitated lakes

3)锶同位素: 4个研究区火山-热液沉积型白云岩的全岩锶同位素值特征可分为2种类型(图 10)。第1类型为三塘湖盆地和准噶尔盆地芦草沟组白云岩。它们的 87Sr/86Sr 数值分布较为集中, 且整体与全球幔源岩Sr同位素值(0.703 50)较为接近(图 10; Palmer and Elderfield, 1985), 而远离壳源岩石。其中三塘湖盆地芦草沟组白云岩 87Sr/86Sr 介于0.704 829~0.704 963之间, 平均0.704 910(焦鑫等, 2017); 准噶尔盆地芦草沟组白云岩 87Sr/86Sr 介于0.705 474~0.706 177之间, 平均0.705 489(张帅等, 2020)。2个盆地中火山-热液沉积型白云岩中均可见火山-热液矿物, 表明其形成流体主要来源于幔源(柳益群等, 2011; 张帅等, 2020)。第2类型为酒西盆地下沟组与二连盆地腾格尔组白云岩。它们的白云岩 87Sr/86Sr值数据较为分散, 且整体上与壳源锶同位素平均值(图 10; 0.720± 0.005; Faure, 1986)较为接近。其中酒西盆地下沟组白云岩 87Sr/86Sr 介于0.713 829~0.714 650之间, 平均0.714 718(文华国等, 2014)。二连盆地腾格尔组白云岩 87Sr/86Sr 介于0.171 585~0.719 273之间, 平均0.179 225(Yang et al., 2021)。因此酒西盆地下沟组与二连盆地腾格尔组形成白云岩的流体应主要来自于壳源物质, 且由于物质相对复杂, 从而导致锶同位素分异较为明显。综合上述数据, 4个研究区火山-热液沉积型白云岩的Sr同位素特征整体区别于同时期全球Sr同位素, 而显示出湖水与幔源或壳源流体相混合的特征, 这可能与不同盆地的裂谷类型不同有关。

图 10 火山-热液沉积型白云岩锶同位素特征Fig.10 Strontium isotopic characteristics of the volcanic-hydrothermal sedimentary dolostones

4 火山-热液沉积型白云岩未来研究展望
4.1 火山-热液沉积型白云岩成因争议

经过多位学者10余年的研究, 火山-热液沉积型白云岩作为中国在陆相细粒沉积岩研究领域中的特色亮点发现, 目前已产出大量学术成果, 但依然存在争议(Jiao et al., 2023)。究其原因主要与现代缺乏实例、国外缺少同类报道以及地质时期样品中缺少火山-热液喷口等直接证据有关。作者分析可能原因如下: (1)目前中国所报道的该类白云岩均发育在各个研究盆地重要的深湖相烃源岩中, 因而得到了重视并被详细研究; 而国外重点研究的类似烃源岩则以海相为主, 并未发育这类白云岩。(2)关于原生白云岩的研究, 受到“ 将今论古” 思路的影响, 使得地质时期白云岩的出现往往被定义成与浅水蒸发环境和微生物作用有关。由于现代深湖沉积物研究和采样相对有一定难度且经济效益较低, 因此, 报道较少(Jiao et al., 2023)。然而, 报道较少并不能说明不存在该类白云石。文中所详述的该类白云岩特征明显区别于常见的次生白云石化成因白云岩, 又与浅水蒸发相微生物成因白云岩不同。作者团队希望能引起国内外同行的关注, 从而研究并找到更多该类白云岩, 为“ 白云石问题” 这一古老议题提供一种新的研究思路。

4.2 火山-热液沉积型白云岩代表的构造背景示踪

4个研究区火山-热液沉积型白云岩岩石学、矿物学特征经研究后发现, 三塘湖盆地和准噶尔盆地芦草沟组白云岩中均可见大量的火山碎屑及与白云岩交互呈纹层的凝灰岩和凝灰质泥岩。而酒西盆地下沟组和二连盆地腾格尔组中的白云岩中并未发现明显的火山物质(表 4)。说明火山作用影响了三塘湖盆地和准噶尔盆地白云岩沉积过程。同时, 地球化学特征中Sr同位素分析结果表明, 三塘湖盆地和准噶尔盆地芦草沟组白云岩的成岩流体来源以幔源为主, 而酒西盆地下沟组和二连盆地腾格尔组则更多为壳源影响。白云岩沉积时期的构造背景不同可能是导致上述差异的主要原因。

表 4 中国火山-热液沉积型白云岩盆地构造背景、岩石学及矿物学特征 Table4 Characteristics of basin tectonic background, petrology and mineralogy of the volcanic-hydrothermal sedimentary dolostone in China

虽然4个盆地在火山-热液沉积型白云岩形成时期均为拉张背景(文华国等, 2014; 焦鑫等, 2017; Yang et al., 2020; 张帅等, 2020), 但前人通过大量岩石学、地球化学与构造特征研究表明, 三塘湖盆地和准噶尔盆地在晚石炭世— 中二叠世经历了碰撞后的裂谷拉伸环境(Feng et al., 1989; Zhao et al., 2003; Choulet et al., 2012), 导致了伸展构造和下地壳的剥离(Karsli et al., 2010), 形成大量的火山作用和相关的火山灰。这种盆地的典型特征是因为存在壳源性火山灰和幔源性物质(Zhang et al., 2023), 这与三塘湖盆地和准噶尔盆地芦草沟组白云岩中可见火山物质及强烈的幔源Sr同位素特征一致。因此, 火山作用所带来的深源物质以火山灰的形式进入湖盆, 为白云石的形成提供了Mg和Fe离子的物质基础; 同时, 火山活动带来的热量也有助于白云石成核与进一步生长(Jiao et al., 2023)。而酒西盆地和二连盆地则可能代表了弧后裂谷盆地。该类盆地主要以幕式断裂、岩浆活动和热构造沉降为主要特征(Zhang et al., 2023)。其中酒西盆地是受到伸展断陷作用后发育而成的陆相断陷盆地。盆地中白云岩形成时期早白垩世为全球性大规模火山活动时期(文华国等, 2014)。二连盆地是一个中生代陆相裂谷盆地, 晚侏罗世和早白垩世期间, 该地区经历了太平洋板块在欧亚板块下的俯冲, 构造活动为热液流体上涌提供了通道(Yang et al., 2020)。酒西盆地下沟组和二连盆地腾格尔组火山-热液沉积型白云岩分布多与区内深大断裂发育较为一致。因此, 该类白云岩在沉积过程中受到了更加强烈的热液活动影响。热液流体沿着裂缝上涌并携带深部物质, 为白云岩形成提供了条件。依据该类白云岩所蕴含的地球化学信息, 可为所处盆地沉积时期的构造背景探讨提供新的研究思路与证据。

4.3 火山-热液沉积型白云岩与油气生成、聚集的关系

白云岩在以往都被视作良好的油气储集层, 如四川盆地龙王庙组(邹才能等, 2014)、 塔里木盆地寒武系和奥陶系等白云岩储集层(Jiang et al., 2018)。 但是4个研究区火山-热液沉积型白云岩不仅可以作为良好的储集层, 还具有一定的生油潜力(高阳等, 2016, 2020; 靳军等, 2018; 张记刚等, 2022)。 4 个研究区内白云岩夹层中可见黑色页岩, 在白云岩中也存在富藻类有机质纹层和有机碎屑(图 7), 说明在白云岩沉积时期伴随着生物活动。 三塘湖盆地和准噶尔盆地芦草沟组白云岩在形成过程存在大量火山活动形成的火山灰。 火山灰是大陆碰撞时岩浆活动的典型产物, 对碳氢化合物的初级生产力有重要影响(Huff et al., 1992; Lee et al., 2018)。 其中富含的营养物质可以使得浮游植物尤其是藻类的大量繁殖, 从而提高初级生产力, 进而提高页岩层系中有机质富集。 同时, 热液流体上涌的同时会携带大量的热能, 可以显著加速盆地烃源岩的演化, 促进油气生成(Liu et al., 2019)。 因此, 这类纹层状泥晶白云岩同样具有较高的生油潜力, 可作为一类生油岩进行研究与勘探。

5 小结

1)全球发育白云石的湖泊主要分布于受到蒸发作用影响的干旱带周围, 但仍有部分分布在非蒸发环境地区并与火山活动有关, 表明火山及相关热液活动同样可以影响白云岩形成。地质时期, 在中国的富有机质页岩中广泛存在的泥晶白云岩, 则代表了火山-热液活动影响下的半深湖— 深湖相沉积环境。这些白云岩保留了原始纹层, 均以层状或透镜状发育于富含有机质的细粒沉积岩中。其中的白云石均以泥晶为主, 有序度较低。伴生矿物主要包括常见的陆源碎屑矿物(石英、斜长石、钾长石)等, 还包含有明显的火山-热液成因矿物。

2)该类白云岩地球化学特征显示, 碳、氧同位素具有明显的碳正、氧负特征, 且分布范围非常接近; 稀土元素趋势图显示整体较为平缓, 并具有明显的Eu正异常, 与微生物白云岩和次生白云岩有非常明显的差异。Sr同位素结果显示三塘湖盆地和准噶尔盆地芦草沟组白云岩热液主要为幔源物质; 而酒西盆地下沟组和二连盆地腾格尔组白云岩热液来源为壳源且成分相对复杂, 并具有明显的湖水与幔源或壳源物质混合特征。

3)该类白云岩均形成于拉张构造背景, 受到火山-热液活动不同程度的影响。三塘湖盆地和准噶尔盆地为碰撞后形成的裂谷盆地, 酒西盆地和二连盆地则可能为弧后裂谷背景下的盆地。丰富的火山灰可以使浮游植物尤其是藻类大量繁殖, 从而提高初级生产力, 为页岩油生成与聚集提供物质基础。来自深源的热液流体上涌携带大量的热能可以加速烃源岩演化, 促进油气生成。因此, 该类白云岩可作为有效的烃源岩做进一步研究。

致谢 感谢成都理工大学郑荣才教授、文华国教授和中国石油大学(北京)钟大康教授、杨喆博士在热液沉积学研究领域常年给予本研究团队的指导与帮助。感谢3位匿名评审专家富有建设性的修改意见。

(责任编辑 郑秀娟)

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