华南早寒武世沉积岩容矿型重晶石矿的成矿作用与研究展望
doi: 10.19762/j.cnki.dizhixuebao.2024014
袁彭1 ， 徐林刚2,3 ， 闫浩2 ， 付雪瑞2 ， 孙凯2 ， 周天霁2
1. 中国地质科学院，北京， 100037
2. 中国地质大学(北京)地球科学与资源学院，北京， 100083
3. 自然资源部成矿作用与资源评价重点实验室，北京， 100083
基金项目: 本文为国家自然科学基金项目(编号42172080，41972072) ； 中国地质科学院基本科研业务费(编号JKY202215)联合资助的成果
作者简介
袁彭，男，1992年生。博士研究生，助理研究员，矿物学、岩石学、矿床学专业，从事沉积成矿方向的研究。E-mail: gscypeng@outlook.com。
通讯作者
徐林刚，男，1981年生。博士，教授，主要从事沉积与成矿作用及地球表生环境演化方向的研究。E-mail: xulingang@cugb.edu.cn。
Metallogenesis of Early Cambrian massive barite deposits in southern China: An overview and prospects
YUAN Peng1 ， XU Lingang2,3 ， YAN Hao2 ， FU Xuerui2 ， SUN Kai2 ， ZHOU Tianji2
1. Chinese Academy of Geological Sciences, Beijing 100037 , China
2. School of Earth Science and Resources, China University of Geosciences, Beijing 100083 , China
3. MNR Key Laboratory for Exploration Theory and Technology of Critical Mineral Resources, China University of Geosciences, Beijing 100083 , China
摘要
华南早寒武世沉积岩容矿型重晶石矿储量居世界首位，在空间上分布于扬子地台北缘的秦岭-大巴山成矿带和东南缘的江南成矿带。本文在简述现代海洋钡的生物化学循环过程基础上，总结了华南早寒武世重晶石矿的地质特征，并对比分析了两条成矿带在含矿建造、矿石组构、化学组成等方面的相似性和差异性，认为两条成矿带的重晶石矿具有相同的物质来源，并沉积于相似的古海洋环境中。寒武纪早期扬子地台周缘海水中较高的生产力，导致了Ba的富集，进而为重晶石的大规模矿化提供充足的物质来源。盆地中缺氧的海水限制了重晶石的沉积，SO2-4来源和浓度是制约华南重晶石沉积和空间分布的重要因素。成岩作用不仅导致了Ba的迁移、富集和再结晶，也可能是秦岭-大巴山成矿带重晶石和毒重石的矿化分带重要控制因素；相对重晶石矿，毒重石矿中有机质降解程度高，CO2-3可能来自于甲烷厌氧的氧化作用。但华南早寒武世重晶石矿在物质来源、沉积环境、成岩作用等方面还需进一步探讨，比如热液喷流和冷泉活动对重晶石和毒重石矿形成的贡献、海洋生产力的水平、SO2-4的来源和空间分布特征等。针对华南早寒武世重晶石矿的研究现状和存在问题，本文认为可通过秦岭-大巴山成矿带和江南成矿带的精细对比研究工作，利用微区原位Sr-S-O-C同位素以及显微矿物学研究，可以更好地约束Ba的物质来源，精细刻画重晶石的沉积-成岩过程。结合Ba同位素，可进一步探讨Ba的富集机制与早寒武世海洋环境之间的关系。
Abstract
The Early Cambrian stratiform massive barite in southern China is one of the largest barite metallogenic provinces in the world. It includes two major metallogenic belts-the Qinling-Daba and the Jiangnan metallogenic belt-spatially distributed along the northern and eastern margins of the Yangtze platform, respectively. Based on the biogeochemical cycle of barium in the modern ocean, this paper described the geological characteristics of typical barite deposits in the Qingling-Daba and the Jiangnan belts. In particular, the similarities and differences in the mineralogical and geochemical composition of barite deposits from the two metallogenic belts are discussed. Similar geochemical and stable isotope composition suggest that barite deposits of the two metallogenic belts may have the same barium sources and deposited in a similarpaleoceanographic environment. During the Early Cambrian, the high primary productivity in the ocean around the Yangtze platform enhanced the barium accumulation in the seawater, providing the prerequisite for massive barite deposition. The sulfate concentration and spatial distribution in the ocean are the significant factors controlling the precipitation of the barite. The diagenetic process not only caused the dissolution, migration and recrystallization of deposited barite, but also responsible for the mineralization zonation of barite and witherite in the Qinling-Daba metallogenic belt. Compared to the barite deposits, the deposition of witherite may involve methanogenesis contributed by the organic matter degradation and production of carbonates from the anaerobic oxidation of methane. Although intensively studies, as yet, the barium sources, paleoceanographic environment, and diagenetic processes of the Early Cambrian massive barite deposits in south China need to be further discussed, such as the contribution of hydrothermal overprinting and cold seep activities to the formation of barite and witherite deposits, the primary productivity and sulfate concentration of the seawater during the Early Cambrian. Prospectively, the barium sources, paleoceanographic environment, and diagenetic processes could be better constrained and characterized by the detailed comparison of the Qinling-Daba and the Jiangnan metallogenic belt through in-situ Sr-S-C-O isotopic and microscopic analysis. Particularly, combined with the Ba isotope, the relationship between voluminous Ba accumulation and the paleoceanographic environment of the Early Cambrian would be better constrained.
重晶石（BaSO4）矿在国民经济建设中具有重要的经济价值，重晶石因具有密度高、较柔软、耐化学腐蚀等特点被广泛应用于石油钻探、医疗、辐射防护等领域。因此，重晶石矿不但被美国、欧盟等经济体列入关键矿产目录（Schulz，2017），在我国也是重要的战略性非金属矿产资源之一（陈正国等，2021）。据美国地质调查局统计，全球重晶石矿储量为3.9亿t，其中，伊朗、哈萨克斯坦、印度、巴基斯坦和中国是世界上最主要的重晶石资源国和生产国（图1）（USGS，2023）。按照产出形式和成矿过程，重晶石矿床类型包括：沉积岩容矿型、火山岩容矿型、脉状变质型和风化残积型（Clark et al.，1990）。沉积岩容矿型重晶石矿可进一步划分为生物—化学沉积作用形成的层状重晶石矿和海底热液喷流形成的层状、透镜状重晶石矿等亚类型。从构造背景来看，沉积岩容矿型重晶石矿可发育在大陆边缘和克拉通裂谷等不同大地构造背景（Maynard et al.，1991）。从成矿时代来看，沉积岩容矿型重晶石矿自太古宙（3.5 Ga）至今均有发育，其中古生代为最主要的成矿爆发期，形成包括中国华南、加拿大Selwyn盆地以及美国内华达、阿肯色、阿拉斯加等多个成矿省（图2）（Jewell，2000；潘忠飞等，2023）。在寒武纪早期，我国华南地区爆发式发育了世界上规模最大、空间分布最广的重晶石矿集区。华南地区重晶石矿不但规模巨大，在矿化特点上也颇具特色，矿石矿物除了重晶石以外，还发育毒重石（BaCO3）和钡方解石（BaCa（CO3）2）等碳酸盐矿物，形成沿扬子地台周缘分布的秦岭-大巴山重晶石-毒重石成矿带和江南重晶石成矿带（Wang Zhongcheng et al.，1991）。目前，我国学者针对这两个成矿带的重晶石和毒重石矿床展开大量矿物学、岩石学、地球化学等方面的研究，提出Ba可能来源于海底热液喷流、海底冷泉、大陆风化补给、海洋自生沉积等，并提出基于成矿物质来源的成矿模型（褚有龙，1989；吕志成等，2004；Han Shanchu et al.，2015；Xu Lingang et al.，2016; Zhou Xiqiang et al.，2022）。这些研究为我们进一步理解Ba在海洋中的地球化学行为以及重晶石和毒重石矿的成矿过程提供了重要的研究基础。然而，前人研究主要针对单个矿床，缺少从成矿带的尺度针对秦岭-大巴山成矿带和江南成矿带的对比分析以及成矿规律总结。近年来研究表明，Ba的大规模富集成矿与海洋环境密切相关，海水的物质组成、氧化还原状态、微生物作用等条件控制着重晶石的成矿过程以及重晶石-毒重石的矿化分异过程（Jewell，2000; Pi Daohui et al.，2014; Xu Lingang et al.，2016; 王富良等，2020；Han Tao et al.，2022）。前人已经在矿床地质特征、成矿作用、成因类型和成矿模型等方面对重晶石矿进行了系统阐述（周锡强等，2016；潘忠飞等，2023）。本文在前人研究的基础上，以海洋中的Ba循环过程角度出发，对华南早寒武世重晶石矿床研究成果进行系统梳理，通过对比分析秦岭-大巴成矿带和江南成矿带之间的相似性和差异性，从成矿物质来源、古海洋沉积环境、沉积-成岩作用过程三个方面探讨华南早寒武世重晶石矿的成矿规律以及重晶石和毒重石的矿化分带机制。在此基础上，基于实验室分析技术现状及目前存在的科学问题，提出研究展望。本研究将进一步深化对华南早寒武世沉积岩容矿型重晶石矿的成矿规律认识，对深入理解寒武纪早期的古海洋环境与Ba富集成矿过程之间的耦合关系具有重要意义。
1 现代海洋中钡的地球化学循环
Ba在海洋中的循环主要受控于陆源、热液、冷泉等的输入以及通过结晶作用和有机质、铁锰氢氧化物等吸附的形式以重晶石、含Ba碳酸盐矿物在海底发生沉积的输出过程（图3）。据估算，海洋中Ba的总输入通量为7~22 Gmol/a，其中陆源输入通量为7~10 Gmol/a，是海洋中Ba的最主要来源（Mayfield et al.，2021）。陆源输入的Ba来自大陆岩石风化，以离子态、吸附态、悬浮物等形式随地表径流和地下水发生迁移并输入海洋。受陆源输入的影响，区域海岸带和河流入海口的钡浓度一般比海洋中Ba的平均值高（Coffey et al.，1997），但不同地区的河流和地下水中Ba的浓度变化较大，进而导致靠近海岸的海水中Ba浓度存在空间差异，其浓度范围在47.8~1466.6 nmol/kg之间（Cao Zhimian et al.，2016）。海底热液和冷泉流体也是海洋中Ba的重要物质来源。海底热液是海水在浅部岩浆或构造活动加热下，萃取围岩中的金属化合物形成的地质流体，广泛发育在洋中脊、岛弧、弧后盆地等火山活动活跃地带（Hannington et al.，2005）。冷泉流体富含甲烷，与沉积后的有机质降解和微生物活动密切相关（Suess et al，1989）。富Ba的冷泉流体一般发育在全球范围的大陆边缘，如秘鲁、加利福尼亚、阿拉斯加等汇聚型大陆边缘，以及日本海、墨西哥湾、鄂霍次克海等大陆斜坡环境（Aquilina et al.，1997; Naehr et al.，2000; Greinert et al.，2002; Hein et al.，2007; Feng Dong et al.，2011; Treude et al.，2014）。据统计，热液和冷泉流体中Ba的浓度范围在10~40 μmol/kg（Von Damm et al.，1985; Torres et al.，2002; McQuay et al.，2008）。热液和冷泉流体中的Ba以重晶石烟囱、岩丘等形式堆积在热液或冷泉喷口周围（Torres et al.，2003; Aloisi et al.，2004）。也可以是Ba2+的形式被释放进入海水，从而促进海水中的钡离子的浓度升高（Hsieh et al.，2017）。
图1世界主要国家重晶石储量分布（据美国地质调查局，2023）
Fig.1Proportion of barite reserves of major countries over the word (after United States Geological Survey, 2023)
图2全球主要沉积岩容矿型重晶石矿时空分布图（据Han Tao et al.，2022；潘忠飞等，2023）
Fig.2Spatial and temporal distribution of significant barite deposits over the word (after Han Tao et al., 2022; Pan Zhongfei et al., 2023)
图3现代海洋中钡的地球化学循环过程示意图（a，据Horner et al.，2021 修改）及冷泉和热液活动产出地质背景图（b，据周锡强等，2016修改）
Fig.3Simplified diagram showing geochemical cycle of Ba in modern ocean (a, modified from Horner et al., 2021) and simplified diagram showing geological background of cold seep and hydrothermal activities (b, modified from Zhou Xiqiang et al., 2016)
重晶石的结晶和溶解是海洋中Ba循环过程中的重要环节。重晶石在水中的溶解度很低（20℃时，溶解度为2.448×10-3 mg/mL），当海水中的Ba2+和SO2-4浓度积超过1.0842×10-10（25℃）时，重晶石便通过结晶作用析出。类似的，当水体中SO2-4浓度不足，但CO2-3浓度较高时，钡离子便与CO2-3结合并以碳酸盐岩的形式结晶析出（图4）。现代海洋中重晶石是不饱和的，其结晶过程与有机质降解形成的重晶石过饱和微环境有关（Dehairs et al.，1980; Bishop，1988）。生物过程参与重晶石沉淀过程表现为两个方面：首先，在海洋生物最活跃的透光带中，Ba被吸附或络合进入浮游生物体内（Fisher et al.，1991; Sternberg et al.，2008），携带大量不稳定态Ba的浮游生物死后沉降至弱光带中，随着沉积环境的改变，有机体发生分解，并释放Ba进入海水，这一过程导致局部海水中Ba的浓度升高，促使重晶石微颗粒由于过饱和而结晶析出（Ganeshram et al.，2003）。其次，实验研究证明重晶石的结晶过程与海洋微生物和有机质密切相关，某些细菌的胞外聚合物是重晶石形成的重要场所（Gonzalez-Munoz et al.，2012），有机质聚合体的内部可以形成重晶石过饱和的微环境（Martinez-Ruiz et al.，2019）。重晶石微颗粒的形成过程伴随着微生物呼吸作用对氧气的大量消耗，因此，在重晶石微颗粒富集的水体中，微生物活跃度较高但氧气含量相对较低（Dehairs et al.，1992，2008; Jacquet et al.，2011; Planchon et al.，2013）。由于重晶石微颗粒的形成与生物活动密切相关，海洋自生重晶石的富集与海洋生产力呈正相关关系，因此海洋自生重晶石可以作为重建海洋生产力的重要指标（Schmitz，1987; Dymond et al.，1992; Paytan et al.，2007; Schoepfer et al.，2015）。重晶石形成与沉淀是受到海水氧化还原环境、化学组成、微生物作用、温度、压力等多种因素影响的动态平衡过程。在特殊环境下，已经形成的重晶石颗粒还会发生不同程度的溶解和重结晶。在重晶石不饱和的水体中，已结晶的重晶石微颗粒在沉降过程中会发生不同程度的溶解，导致Ba在深层海水中的浓度大大超过表层海水（McManus et al.，1998; Monnin et al.，1999; Bridgestock et al.，2018）。在缺氧的受限制盆地中，还原作用促使重晶石大量溶解，从而释放大量的Ba进入海水，导致Ba在海水的氧化还原界面附近高度富集。例如，海水中的重晶石再溶解，死海中Ba浓度最高可达460 nmol/kg（Falkner et al.，1993）。此外，在大洋环流的作用下，深层海水中的Ba又可被携带至表层海水，造成表层海水中Ba的局部富集（Cao Zhimian et al.，2016）。
图4重晶石、毒重石、方解石和硬石膏在25℃和0.101325 MPa 水溶液中的相图（据Maynard et al.，1991修改）
Fig.4Phase diagram illustrating stability fields for Ba-Ca sulfates and carbonates in aqueous solution at 25℃ and 0.101325 MPa (modified from Maynard et al., 1991)
在海水中结晶的重晶石沉降并保存在海底沉积物中。重晶石的富集与海洋生产力密切相关，在高海洋生产力的区域，海底沉积物中富集较高含量的重晶石（Paytan et al.，2007）。除重晶石以外，Ba也可以吸附或以类质同象的形式存在于铁锰氧化物、铝硅酸盐矿物等沉积物中。与铁锰氧化物有关的Ba主要发育在氧化的沉积物中，而与铝硅酸盐矿物有关的Ba主要受控于大陆风化来源，二者在现代海洋沉积物中占比较小（Schenau et al.，2001）。沉积埋藏后重晶石受孔隙水中SO2-4的浓度影响，发生溶解、迁移和重结晶。微生物硫酸盐还原作用是孔隙水中SO2-4消耗的主要方式（Jørgensen，1982; Kasten et al.，2000; Boetius et al.，2013）。在微生物硫酸盐还原作用下，孔隙水中SO2-4被大量消耗，导致重晶石由于不饱和发生溶解，释放Ba2+进入孔隙水，进而形成富Ba2+的地质流体。当重晶石埋藏较深时，富Ba2+的地质流体主要以扩散的形式在沉积物的孔隙或裂隙中迁移，与富含SO2-4的流体混合后，结晶形成成岩重晶石（Riedinger et al.，2006; Hendy，2010）。当重晶石埋藏较浅时，富含Ba2+的地质流体沿孔隙、裂隙流出水岩界面进入海水（Torres et al.，2003）。
2 华南早寒武世重晶石矿床特征
在华南地区，在扬子地台北缘和东南缘的大陆边缘相沉积环境中，发育众多大型—超大型沉积岩容矿重晶石矿床。这些矿床虽然空间上不连续，但层位稳定，形成具有世界级储量规模的扬子地台北缘秦岭-大巴山成矿带和东南缘的江南成矿带（图5）（Wang Zhongcheng et al.，1991）。秦岭-大巴山成矿带中矿石矿物除了重晶石以外，还发育毒重石、钡方解石等碳酸盐矿物，形成了世界罕见的毒重石成矿带，尤其是重晶石矿和毒重石矿在空间上呈现出从东北向西南由重晶石逐渐过渡到毒重石的矿化分带特征（涂怀奎，1999）。该成矿带的典型矿床包括陕西安康石梯重晶石矿、湖北柳林重晶石矿、湖北竹山文峪河毒重石-重晶石矿、陕西黄柏树湾毒重石矿等。江南成矿带的矿石矿物主要为重晶石，代表性矿床包括贵州大河边重晶石矿、湖南贡溪重晶石矿、广西板必重晶石矿等。早寒武世重晶石、毒重石矿在两条成矿带均呈块状、结核状、纹层状赋存在黑色页岩和硅质岩中（图6），除了重晶石、毒重石矿外，该层位还发育镍钼多金属矿、钒矿、磷矿、石煤等多种矿产。
2.1 秦岭-大巴山重晶石-毒重石成矿带
秦岭-大巴山重晶石-毒重石成矿带在空间上西起陕西西乡富水河，东至湖北竹山、竹溪一带，延伸超过300 km，跨越陕西、重庆、四川和湖北等多个省市。目前，已发现70多个不同规模的重晶石、毒重石矿床，并在区域上形成明显的矿化分带特征（图7）。根据矿石类型，可进一步分为以重晶石矿床为主的北矿带和以毒重石矿床为主的南矿带，中间为重晶石-毒重石共生的矿床（涂怀奎，1999）。矿体呈层状、似层状或透镜体状赋存在下寒武统鲁家坪组的富硅质和碳质黑色岩系中下部，与围岩呈整合接触，具同生沉积特征。该围岩自下而上依次发育有块状硅质岩、碳质硅质岩与碳质页岩互层、碳质页岩和千枚状板岩。其中，硅质岩中普遍含有放射虫化石，而碳质页岩缺少生物化石和生物扰动构造，除了重晶石和毒重石矿以外，局部地区还发育磷矿和钒矿（孙兴文，1990；吕志成，2004；唐用洋等，2020）。围岩中碳酸盐岩夹层较为常见，且呈现向上增多的趋势，局部地区发育有凝灰岩夹层（高怀忠，1998）。单个矿体的厚度从几米到几十米不等，最长可延伸几千米。重晶石矿主要赋存在富碳质硅质岩中，与围岩呈整合渐变关系（方旭等，2013）。矿石矿物主要为重晶石，伴生有石英、水云母、绢云母、白云母、褐铁矿、白云石、方解石等矿物，具有粒状结构，呈块状、条带状、纹层状等构造。毒重石矿主要发育在厚层硅质岩与黑色页岩的过渡带（吕志成等，2005），与钡方解石和重晶石紧密共生，自下而上依次发育有钡方解石矿层、毒重石矿层和毒重石-重晶石混合矿层，矿层之间以薄层硅质岩相隔。矿石矿物包括毒重石、重晶石以及少量钡方解石，伴生有石英、绢云母、白云母、黄铁矿、闪锌矿、方解石、菱镁矿、胶磷矿、钡钒云母、铝硅钡石等矿物。矿石发育粒状、玫瑰花状、脉状、变晶等结构，呈块状、条带状和纹层状构造（图8）。秦岭-大巴山成矿带典型沉积岩容矿型重晶石-毒重石矿床地质特征见表1。
图5华南寒武纪早期古地理环境及主要沉积岩容矿型矿产分布图（据Lehmann et al.，2016修改）
Fig.5Reconstruction of Early Cambrian paleogeographic environment and distribution of major sedimentary rock-hosted deposits of South China (modified from Lehmann et al., 2016)
图6秦岭-大巴山成矿带和江南成矿带典型重晶石矿和毒重石矿地层柱状图（据吕志成等，2005；方旭等，2013；王富良等，2020；夏瑞等，2021修改）
Fig.6Stratigraphy sequences of typical barite and witherite deposits from the Jiangnan and Qinling-Dabashan metallogenic belts (modified after Lü Zhicheng et al., 2005; Fang Xu et al., 2013; Wang Fuliang et al., 2020; Xia Rui et al., 2021)
2.2 江南重晶石成矿带
江南重晶石成矿带空间上西起广西北部，经贵州、湖南、江西延伸到安徽，超1100 km，呈NEE-SWW向展布，发育有多个大型-超大型重晶石矿床。矿体呈层状、似层状或透镜体状赋存在下寒武统牛蹄塘组的含碳质硅质岩和黑色页岩中。矿体下伏围岩与埃迪卡拉纪灯影组白云岩整合接触，向上依次发育有块状含铀磷硅质岩和含钒碳质页岩，局部夹有碳质粉砂岩和碳质黏土岩薄层，顶部渐变为泥质灰岩（夏瑞等，2021）。其中，下寒武统的黑色页岩局部发育多孔动物、节肢动物以及软体动物化石（Li Guoxiang et al.，2007; Weber et al.，2007），以及超常富集Ni、Mo、V、U等金属元素（Lehmann et al.，2007；Xu Lingang et al.，2021，2023）。重晶石矿体与围岩呈整合渐变接触关系，矿体厚度与围岩的厚度成反比，即硅质岩厚的区域，重晶石矿体相对较薄。局部地区，重晶石矿体可与下伏白云岩直接整合接触。矿石矿物主要为重晶石，伴生矿物包括方解石、白云石、石英、钡冰长石、胶磷矿、黄铁矿等，局部可见少量方铅矿和闪锌矿（Han Tao et al.，2022; Zhou Xiqiang et al.，2022），发育有菌藻类、海绵骨针、管状生物等生物化石（杨瑞东等，2007；夏瑞等，2021）。重晶石的颗粒直径一般在10~200 um，呈他形、半自形、自形等结构，局部可见放射状和树枝状结构。矿石发育有结核状、块状、花斑状和纹层状构造，并在垂向上呈现一定的规律性分带（夏瑞等，2021）。结核状重晶石主要分布在矿体的顶部或底部围岩中，大小不均一，具有同心环状构造。块状重晶石发育在矿体的下部，品位最高，常见网脉状重晶石穿插其中（图9）。块状重晶石向上渐变为花斑状重晶石，包含数量不等的方解石和硫化物状，矿体的上部为纹层状重晶石，是由重晶石和有机质纹层互层形成。总体上呈现向上碎屑含量增多而重晶石含量减少的趋势。江南成矿带典型沉积岩容矿矿型重晶石矿床地质特征见表2。
图7秦岭-大巴山重晶石—毒重石成矿带区域地质图（据Xu Lingang et al.，2016修改）
Fig.7Reginal geological map shows representative barite and witherite deposits in the Qinling-Dabashan metallogenic belt (modified from Xu Lingang et al., 2016)
图8秦岭-大巴成矿带不同结构、构造类型重晶石和毒重石矿石显微照片
Fig.8Microscopic images show various textures and structures of barite and witherite ores in the Qinling-Dabashan metallogenic belt
（a）—砂糖状重晶石（样品采自安康柳树河重晶石矿床）；（b）—块状重晶石（样品采自平利清水河重晶石-毒重石矿）；（c）—纹层状重晶石（样品采自平利清水河重晶石-毒重石矿）；（d）—纹层状毒重石（样品采自紫阳黄柏树湾毒重石矿床）
(a) —equigranular barite (sample from Liushuhe barite deposit) ; (b) —massive barite (sample from Qingshuihe barite-witherite deposit) ; (c) —laminated barite (sample from Qingshuihe barite-witherite deposit) ; (d) —laminated witherite (sample from Huangbaishuwan witherite deposit)
表1秦岭-大巴山成矿带典型重晶石和毒重石矿床地质特征
Table1Geological characteristics of typical barite and witherite deposits in the Qinling-Dabashan metallogenic belt
3 秦岭-大巴成矿带和江南成矿带矿物学、地球化学特征
华南早寒武世重晶石、毒重石矿床在空间上沿秦岭-大巴成矿带和江南成矿带分布，均形成与边缘海或大陆斜坡地区，两个成矿带在矿体的空间形态、结构构造、含矿岩性组合等方面存在高度的相似性（表3）。矿体均呈结核状、块状、纹层状赋存在下寒武统的黑色页岩和硅质岩中，具有强烈的层控特点，产状与围岩一致；在地层层序上，赋存地层均由富硅质的化学沉积向碎屑沉积转变，钡的含量向上逐渐降低；在物质组成上，矿石都发育有石英、方解石、白云石、胶磷矿、黄铁矿等伴生矿物，陆源碎屑含量较少。与围岩相比，矿石的有机碳含量相对较低。其中，秦岭-大巴成矿带重晶石-毒重石矿的有机碳含量在0.41%~4.3%之间（刘家军等，2007）；赋矿围岩的有机碳含量最高可达17%（吕志成等，2005）；江南成矿带重晶石矿的有机碳含量在0.24%~2.46%之间（韩善楚等，2014）；上覆围岩的有机碳含量在6.4%~35.5%之间（Cheng Meng et al.，2020）。不同的是，江南成矿带重晶石矿床的下伏陡山沱组白云岩中发育有Pb-Zn矿床（Zhou Zhengbing et al.，2018），而秦岭-大巴成矿带的矿石矿物除重晶石以外，还发育有毒重石、钡方解石等碳酸岩矿物，但尚未有Pb-Zn矿化的报道。
Sr、S、C、O同位素是研究重晶石和毒重石成矿物质来源和形成环境最主要的地球化学指标，两条成矿带的重晶石、毒重石以及自生碳酸盐矿物具有整体上相似的Sr、S、C、O同位素组成特征，但范围存在一定的差异。重晶石和毒重石的87Sr/86Sr比值结果范围较大，秦岭-大巴成矿带重晶石、毒重石的87Sr/86Sr比值范围在0.7076~0.7089（吕志成等，2005； 罗莉，2011；刘家军等，2014；Xu Lingang et al.，2016），江南成矿带重晶石的87Sr/86Sr比值范围在0.7082~0.7279（夏菲，2004；Zhou Xiqiang et al.，2022; Han Tao et al.，2022）；重晶石δ34S的组成普遍偏重，秦岭-大巴山成矿带中的重晶石δ34S值的范围在22.1‰~76.1‰（刘家军等，2008；Xu Lingang et al.，2016），江南成矿带中重晶石的δ34S值的范围在32.3‰~61.1‰（王富良等，2020；Zhou Xiqiang et al.，2022）；碳酸盐矿物的δ13C均为负值且组成范围较大，秦岭-大巴山成矿带毒重石、钡方解石的δ13C值范围在-24.78‰~-6.3‰（吕志成等；2003；罗莉等，2012；Xu Lingang et al.，2016; 彭不同等，2023），江南成矿带自生白云石的δ13C值范围在-18.3‰~-7.2‰（Zhou Xiqiang et al.，2022）；硫酸盐矿物和碳酸盐矿物具有不同范围的δ18OV-SMOW值，秦岭-大巴山成矿带重晶石的δ18OV-SMOW值范围为18.7‰~24.8‰，毒重石的δ18OV-SMOW值范围为9.9‰~22.4‰（吕志成等，2003； 罗莉等，2012；Xu Lingang et al.，2016; 彭不同等，2023），江南成矿带重晶石的δ18OV-SMOW值范围为18.1‰~20.7‰，自生白云石的δ18OV-SMOW值范围为19.2‰~23.2‰（Zhou Xiqiang et al.，2022）。
图9江南成矿带不同构造类型重晶石矿石照片
Fig.9Images show various structures of barite ore in the Jiangnan metallogenic belt
（a，b）—脉状重晶石；（c，d）—块状重晶石；（e，f）—花斑状重晶石；（g，h）—纹层状重晶石（样品均采自大河边重晶石矿床）
(a, b) —vein barite; (c, d) —massive barite; (e, f) —granophyric barite; (g, h) —laminated barite (all samples are from Dahebian barite deposit)
4 华南早寒武世重晶石矿成矿过程
如前所述，秦岭-大巴山重晶石-毒重石成矿带和江南重晶石成矿带不但在成矿时代上具有一致性，在矿物类型、地球化学组成等方面也具有高度的相似性，反映了两条成矿带可能具有相同的成矿物质来源和相似的古海洋沉积环境。然而，秦岭-大巴山成矿带的矿石矿物除重晶石以外，还发育有毒重石、钡方解石等碳酸盐矿物，但不发育Pb-Zn矿化，而江南重晶石成矿带发育有Pb-Zn矿，但含钡矿物仅发育重晶石，极少发育毒重石、钡方解石等碳酸盐矿物。此外，两条成矿带在Sr、S、C、O同位素组成上也具有差异性，可能反映在相似的成矿背景下，局部古地理环境、微生物作用、海底热液、冷泉活动等对不同成矿带的成矿过程及矿化分带具有一定影响。本文将在前人研究的基础上，结合现代海洋中钡的化学循环过程，分别从钡的物质来源、沉积环境、成岩作用等方面探讨华南早寒武世重晶石矿床的成矿过程。
4.1 钡的物质来源
丰富的成矿物质供给是形成大型、超大型重晶石和毒重石矿床的基础。华南重晶石矿床中Ba的物质来源存在大陆风化、热液喷流和冷泉流体等不同认识（褚有龙，1989; Han Shanchu et al.，2015； Xu Lingang et al.，2016; Zhou Xiqiang et al.，2022）。大陆风化来源的观点认为早寒武世富氧大气加速了陆源物质的氧化与风化（Zhang Gongjing et al.，2021; Bayon et al.，2022），大量Ba以真溶液或者胶体溶液的形式通过地下水或地表径流进入海洋，与海水中的SO2-4结合后沉淀形成重晶石矿床（褚有龙，1989）。华南早寒武世重晶石矿纯度高，且Al、Ti等反映陆源物质的元素含量极低，说明重晶石是通过海水化学沉积作用形成，而不是以陆源碎屑物的形式富集。
热液喷流来源的观点认为寒武纪早期扬子地台周缘广泛发育的热液活动可为重晶石和毒重石成矿提供大量的物质来源（王忠诚等，1992；唐菊兴等， 1998；杨瑞东等，2007；Han Shanchu et al.，2015; 夏瑞等，2021）。在埃迪卡拉纪至寒武纪早期，扬子地台周缘发育受同生断裂控制的断陷盆地，海水沿断裂或裂隙进入洋壳，在浅部岩浆活动的加热下发生对流循环，萃取围岩内的多种金属化合物，形成含有Ba2+以及多种金属元素的还原性热液流体（Hannington et al.，2005）。热液流体沿构造破碎带喷流出海底，与海水混合后形成硅质岩、重晶石和Pb-Zn硫化物组合的喷流沉积型成矿系统（Chen Daizhao et al.，2009；Zhou Zhengbing et al.，2018）。江南成矿带和秦岭-大巴山成矿带的重晶石矿内均发现钡冰长石矿物，以及稀土元素配分模式中具有Eu正异常特征，被认为是热液喷流来源的证据（彭军等，1999；韩善楚等，2013；陶银龙等，2016）。但富钡流体在成岩阶段对长石矿物的交代，也可在重晶石矿体中形成钡冰长石（Fernandes et al.，2017）。而Eu的正异常也可能是由于沉积物中的火山碎屑物质与孔隙水相互作用而释放Eu进入孔隙水，并迁移至海水所致（吕志成等，2004）。Pb-Zn矿化与重晶石矿的空间密切共生关系被认为是热液成因重晶石的最重要证据之一。现有研究表明，江南成矿带中Pb-Zn矿主要赋存在下伏陡山沱组白云岩中（温汉捷等，2017；Zhou Zhengbing et al.，2018），在成矿时代上与重晶石矿并不完全一致。此外，赋矿硅质岩的地球化学数据显示负Ce异常以及类似海水的稀土元素分布模式，指示了硅质岩的形成可能与生物作用有关（Guo Qingjun et al.，2007）。因此，江南成矿带重晶石矿的热液喷流来源还需更多证据的支持，如精确的陡山沱组赋存的Pb-Zn矿以及重晶石矿的成矿年龄，两种矿化类型在空间上的递变关系等。
表2江南成矿带典型重晶石矿床地质特征
Table2Geological characteristics of typical barite deposits in the Jiangnan metallogenic belt
表3秦岭-大巴山成矿带与江南成矿带矿物学和地球化学特征对比
Table3Comparison of mineralogical and geochemical composition between the Qinling-Dabashan and Jiangnan metallogenic belts
冷泉流体来源的观点认为华南早寒武世重晶石矿和毒重石矿的形成可能受控于大陆边缘富钡的冷泉流体（Zhou Xiqiang et al.，2022）。富含重晶石的海底沉积物在埋藏后，同沉积的有机质发生降解并产生甲烷（Suess et al.，1989），在甲烷的厌氧氧化和硫酸盐的还原硫化作用下（Boetius et al.，2000），沉积物孔隙水中的碳酸盐碱度升高，而SO2-4被大量消耗，从而促使沉积物中的重晶石由于不饱和而发生溶解，释放Ba2+进入孔隙水中。在构造活动的控制下，富含Ba2+以及CH4、HCO-3、HS-等离子的流体沿着孔隙或裂隙渗流而出，与海水混合结晶形成冷泉重晶石（Torres et al.，2003）。华南重晶石矿中伴生的方解石、白云石等矿物，以及发育的簇状、树枝状、放射状重晶石被认为是冷泉重晶石的证据（Greinert et al.，2002; Feng Dong et al.，2011; Zhou Xiqiang et al.，2022）。此外，冷泉流体也为秦岭-大巴山成矿带的毒重石、钡方解石等碳酸盐矿物的形成提供CO2-3离子（Xu Lingang et al.，2016）。现代海洋学研究表明，冷泉重晶石一般发育在海底沉积物富集重晶石的高海洋生产力区域，冷泉重晶石的形成与海洋环境密切相关（Aloisi et al.，2004）。此外，冷泉流体是成岩作用的产物，即冷泉流体是在沉积物早期埋藏阶段，有机质降解释放甲烷并喷流出海底形成（Whiticar，1999; Suess，2010）。成岩作用过程对华南寒武纪早期扬子地台周缘重晶石和毒重石的成矿过程影响将在本文4.3章节进一步探讨。
Sr和Ba元素具有相似的化合价和离子半径，因此Sr能以类质同象的形式替代Ba进入到重晶石和毒重石中。Sr同位素是示踪成矿物质来源的有效手段，进而可以约束Ba的物质来源（Paytan et al.，2002）。海洋自生重晶石可以保留同期海水的信息，具有和同期海水较为一致的87Sr/86Sr组成特征（Paytan et al.，1993）。热液重晶石和冷泉重晶石的87Sr/86Sr比值变化范围较大，主要与流体在运移过程中，所反应的围岩或沉积物的组成有关（Paytan et al.，2002; Feng Dong et al.，2011）。若沉积物中含有较多的火山物质，则流体中的87Sr/86Sr比值偏小，而如果沉积物中包含较多的陆源碎屑物质，则流体中的87Sr/86Sr比值偏大。寒武纪早期海水的87Sr/86Sr比值范围在0.7081~0.7090（Maloof et al.，2010; Li Da et al.，2013; Bowyer et al.，2022）。华南重晶石矿和毒重石矿的87Sr/86Sr比值整体上与同期海水基本一致（图10），反映了江南成矿带和秦岭-大巴山成矿带的Ba具有相似的物质来源，且物质来源可能主要为海水（Paytan et al.，1993; Xu Lingang et al.，2016）。此外，少部分华南重晶石矿和毒重石矿的87Sr/86Sr比值偏离同期海水，指了两条成矿带中Ba的物质来源也可能局部受到陆源碎屑或热液流体叠加的影响。其中江南成矿带的部分87Sr/86Sr比值偏大，尤其是低品位重晶石矿石的87Sr/86Sr比值可达0.7279（Zhou Xiqiang et al.，2022），可能与陆源碎屑的混入有关。而秦岭-大巴山成矿带的部分的87Sr/86Sr比值偏小，特别是在与青白口系耀岭河群中基性火山岩接触的重晶石-毒重石矿床中呈现了相对较低的87Sr/86Sr比值（吕志成等，2005），说明在成岩过程中，富Ba2+流体与火山岩发生交代作用，置换出火山岩中贫放射性的Sr进入富Ba2+流体中，进而可能导致部分重结晶的重晶石或毒重石的87Sr/86Sr比值低于同期海水。总之，重晶石矿石的结构和品位对Sr同位素组成均产生影响。识别重晶石的不同结构和构造类型，利用自生重晶石判断其沉积环境和成岩过程，结合原位Sr同位素分析，可以更好地约束Ba的物质来源（Paytan et al.，2002；周锡强等，2016），并精细刻画重晶石的形成过程（Jamieson et al.，2016）。综上，扬子地台周缘重晶石矿和毒重石矿的物质来源可能主要为海水，虽然江南成矿带尚不能排除可能有部分成矿物质来自热液系统，但还需要更多地质、地球化学数据的支持。但不论Ba是哪种来源，均需以离子形式溶解在海水中，导致海洋中的Ba2+浓度升高，进而为大规模重晶石和毒重石矿化提供物质基础。此外，大规模重晶石矿化都与海水或孔隙水中的Ba2+和SO2-4过饱和有关，受控于古海洋的沉积环境和成岩作用过程。
4.2 沉积环境
海洋沉积环境对重晶石的大规模沉淀具有重要意义（Falkner et al.，1993; Monnin et al.，1999; Cao Zhimian et al.，2016; Bridgestock et al.，2018）。海洋沉积环境涵盖了海水酸碱度、氧化还原程度以及与之相关的沉积盆地形貌、物质循环过程等多种因素。华南重晶石矿在寒武纪早期这一关键地质历史时期爆发式发育，反映了特殊的古海洋环境对重晶石矿的形成具有控制作用。本文聚焦于关键地质历史时期重大地质事件对海洋氧化还原沉积环境，以及伴生的海洋生产力变化对重晶石成矿的影响。地球的表生环境演化过程呈现阶梯性增氧（Lyons et al.，2014; Alcott et al.，2019），到寒武纪早期，大气圈的含氧量可能已经达到现代大气水平（Chen Xi et al.，2015）。大量氧气溶解在表层海洋中，从而促使海洋透光带中生物的大规模发育，进而导致扬子地台周缘的表层海水呈现较高的生产力（Jin Chengsheng et al.，2016; Cheng Meng et al.，2020）。一方面，华南重晶石矿和毒重石矿的赋矿围岩有机碳含量相对较高，江南成矿带和秦岭-大巴山成矿带中有机碳含量最高分别达8.3%和17%（吕志成等，2005；韩善楚等，2014）。其主要来源为海相低等菌藻类浮游生物（侯东壮等，2014；韩善楚等，2014）。此外，矿石中还发育胶磷矿、菌藻类生物化石等成分（杨瑞东等，2022），同样反映了扬子地台周缘寒武纪早期海水具有较高的生物原始产率。在海洋高生物原始产率背景下，大量有机碳在透光带中产生，并吸附或络合大量的Ba（Fisher et al.，1991; Sternberg et al.，2008）。另一方面，与赋矿围岩相比，华南重晶石矿和毒重石矿矿石的有机碳含量相对较低，秦岭-大巴山成矿带矿石的有机碳含量在0.41%~4.3%之间，江南成矿带矿石的有机碳含量在0.24%~2.46%之间（刘家军等，2007；韩善楚等，2014）。可能反映了有机碳在沉积过程中被大量降解，导致有机碳在沉积物中埋藏较少。在有机碳降解过程中，Ba被重新释放进入海水，从而导致Ba在海水中的富集（Paytan et al.，2007），进而为华南重晶石的大规模矿化提供充足的物质来源（Jewell，2000; 吕志成等，2005）。
图10秦岭-大巴山成矿带与江南成矿带重晶石和毒重石87Sr/86Sr同位素组成对比
Fig.10Comparison of 87Sr/86Sr values of barite and witherite between the Qinling-Dabashan and Jiangnan metallogenic belt
数据来源：夏菲，2004；吕志成等，2005；罗莉，2011；刘家军等，2014；Xu Lingang et al.，2016; Zhou Xiqiang et al.，2022; Han Tao et al.，2022
Data sources: Xia Fei, 2004; Lü Zhicheng et al., 2005; Luo Li, 2011; Liu Jiajun et al., 2014; Xu Lingang et al., 2016; Zhou Xiqiang et al., 2022; Han Tao et al., 2022
重晶石的结晶、沉淀与海水中的SO2-4浓度密切相关，即受控于海洋的氧化还原状态影响（Falkner et al.，1993; Wei Guangyi et al.，2021a）。虽然寒武纪早期的大气和海洋的含氧量已升至较高水平（Chen Xi et al.，2015），但在扬子地台周缘大陆斜坡环境，局部仍发育有表层氧化而深部缺氧硫化的局限盆地（Li Chao et al.，2015; Jin Chengsheng et al.，2016）。局限盆地相对稳定、低能的环境有利于纹层状、条带状重晶石和毒重石的沉积。此外，局限盆地缺氧硫化的水体可溶解大量Ba2+，从而有利于大规模的重晶石和毒重石的沉淀（Falkner et al.，1993; Jewell，1994）。海洋沉积物中U、V、Mo等微量元素含量是指示海洋氧化还原环境的重要指标（Tribovillard et al.，2006）。在富H2S的还原环境中，海水中溶解的Mo被吸附于富硫有机物质或者铁硫化物中，并在沉积物中超常富集（Zheng Yan et al.，2000）。此外，当海水缺氧时，U、V也在沉积物中呈现异常高含量特征（Piper et al.，2009; Bennett et al.，2020）。王富良等（2020）针对江南成矿带中大河边和云洞重晶石矿床的微量元素分析，认为矿石中超常富集U、V、Mo等微量元素指示了重晶石形成时的古海洋为缺氧环境。类似的，秦岭-大巴山成矿带的重晶石-毒重石矿床的微量元素研究也指示了毒重石形成于相对缺氧的水体环境（Pi Daohui et al.，2014）。重晶石中记录的δ34S信息可以反映海水的SO2-4来源以及氧化还原状态（Paytan et al.，2002）。寒武纪早期海水δ34S值的范围在29‰~32‰（Claypool et al.，1980; He Tianchen et al.，2019），华南早寒武世重晶石的δ34S值普遍偏重（图11），指示了强烈的微生物还原作用（刘家军等，2008；Han Shanchu et al.，2015; Xu Lingang et al.，2016; 王富良等，2020）。在相对局限的盆地中，强烈的微生物还原作用限制了海水中SO2-4的浓度。因此，在SO2-4浓度有限的缺氧的环境中，Ba将在海水中呈溶解的离子态存在（Falkner et al.，1993），导致寒武纪早期的海洋中可能形成一个巨大的Ba2+储库（Crockford et al.，2019; Han Tao et al.，2022）。研究表明，寒武纪早期扬子地台周缘的局限盆地在海进海退的过程中可能与开阔大洋是间歇性相通的（Wei Guangyi et al.，2021b）。在这种情况下，大陆风化以及远洋氧化性的海水在洋流的作用下，为局限盆地输入大量的SO2-4，并与溶解的Ba2+混合形成重晶石。另一方面，华南早寒武世重晶石的δ34S值范围较大，可能反映了微生物的还原作用在区域上存在差异，导致SO2-4的浓度在空间上呈不均匀分布，从而造成重晶石矿和毒重石矿在空间上不连续分布和差异性成矿。王富良等（2020）通过对比江南成矿带大河边和云洞重晶石矿床的δ34S值，发现成矿规模较小、品位较差的云洞重晶石矿床的δ34S值相对偏高；而成矿规模较大、品位较高的大河边重晶石矿床的δ34S值相对较低，反映了两个矿床沉积时海水中的SO2-4浓度存在差异，从而导致两个矿床的成矿规模和矿石品位的不同。Xu Lingang et al.（2016）通过研究秦岭-大巴山成矿带的重晶石矿和毒重石矿，认为强烈的微生物还原作用导致局限盆地内的SO2-4被消耗殆尽，从而促使毒重石的大规模沉积。目前，寒武纪早期扬子地台周缘海水的氧化还原环境与重晶石沉积之间的关系还需进一步探讨，尤其是海水中SO2-4的来源和浓度，不仅控制着重晶石的大规模沉积与空间分布，也对我们理解寒武纪早期这一特殊地质历史时期的硫循环具有重要意义。
4.3 成岩作用
沉积埋藏后的重晶石在成岩作用下可发生溶解、迁移和再结晶，成岩作用被认为是沉积岩容矿型重晶石矿床形成的重要机制（Zhou Xiqiang et al.，2015; Fernandes et al.，2017）。在海水中结晶形成的重晶石，经过沉积埋藏后，进入早期成岩阶段，同沉积的有机质发生降解，在水界面以下的沉积物中依次形成硫酸盐带、硫酸盐-甲烷转换带和甲烷带（Claypool et al.，1974; Knittel et al.，2009）。甲烷带中的原生重晶石会被溶解并在孔隙水中形成富Ba2+流体，这种流体在迁移至硫酸盐-甲烷转换带后，重结晶形成成岩重晶石（图12）（Riedinger et al.，2006; Hendy，2010）。此外，当重晶石埋藏较浅，或者受到构造活动影响，富Ba2+流体将向上渗流出水岩界面，与海水中的SO2-4结合结晶形成重晶石，并以冷泉成因烟囱、结壳等形式分布在海底（Torres et al.，1996，2003）。
图11秦岭-大巴山成矿带与江南成矿带重晶石δ34S值对比
Fig.11Comparison of δ34S values of barite between the Qinling-Dabashan and Jiangnan metallogenic belt
数据来源：刘家军等，2008；王富良等，2020；Xu Lingang et al.，2016; Zhou Xiqiang et al.，2022
Data sources: LiuJiajun et al., 2008; Wang Fuliang et al., 2020; Xu Lingang et al., 2016; Zhou Xinqiang et al., 2022
在早期成岩阶段，沉积物中的有机质在氧化作用、微生物作用或热化学作用下发生降解，释放并溶解形成CO2-3、 HCO-3、 HS-等离子进入孔隙水，可为碳酸盐矿物的结晶提供碳源（Emerson，1985; Whiticar，1999; Suess 2010; LaRowe et al.，2020）。碳酸盐矿物中记录的碳同位素可示踪碳的物质来源。研究表明，海水碳酸盐的δ13C均值约为0‰，有机碳的δ13C均值约为-25‰（Hoefs，2009）。秦岭-大巴山成矿带中毒重石、钡方解石，以及江南成矿带中自生白云石的δ13C值均偏负，且数值范围均介于-25‰~0‰之间（表3），指示两条成矿带中毒重石、钡方解石、自生白云石等碳酸盐矿物的碳为海水碳酸盐和有机碳的混合来源，反映了在早期成岩过程中有机质发生降解，并为毒重石、钡方解石、自生白云石等碳酸盐矿物的形成提供了部分碳源（吕志成等；2003；罗莉等，2012； Xu Lingang et al.，2016; Zhou Xiqiang et al.，2022）。另一方面，早期成岩过程中的微生物还原硫化作用可以降低孔隙水中SO2-4离子浓度，从而使重晶石由于不饱和溶解，释放Ba2+进入孔隙水，在与富含SO2-4的流体混合后，在孔隙或裂隙中重结晶形成板状、玫瑰花状、孔隙充填状等重晶石结构（图13）。微生物硫酸盐还原作用包括两种驱动机制：甲烷厌氧氧化作用（AOM：SO2-4 + CH4 → HCO-3+ HS- + H2O）和有机质碎屑硫酸盐还原作用（OSR：SO2-4 + 2CH2O → 2HCO-3+ HS- + H+）。研究表明，重晶石中记录的δ18O/δ34S值可以有效示踪微生物硫酸盐还原作用的驱动方式，其中δ18O/δ34S ＜ 0.5指示了AOM主导的硫酸盐还原作用，而δ18O/δ34S ＞ 0.7则指示了OSR主导的硫酸盐还原作用（Antler et al.，2015; Feng Dong et al.，2016）。华南早寒武世重晶石具有较低的δ18O/δ34S值，其中秦岭-大巴成矿带的δ18O/δ34S值约为0.1（彭不同等，2023），江南成矿带的δ18O/δ34S值最低为0.04（Zhou Xiqiang et al.，2022），均指示了两条成矿带在成岩过程中存在AOM主导的硫酸盐还原作用。但是甲烷的浓度、运移方式（渗流或喷流）的差异均会导致δ18O/δ34S值无法有效示踪生物硫酸盐还原作用的驱动方式（Antler et al.，2017; Pellerin et al.，2018; Gong Shanggui et al.，2021）。例如，Xu Ligang et al.（2016）认为秦岭-大巴山成矿带毒重石偏低的δ18O值，指示了有机质降解可能在热化学作用下进入甲烷生成阶段，富含甲烷和CO2的冷泉流体喷流出海底后，与海水中的Ba2+混合沉积形成毒重石。吕志成等（2005）认为秦岭-大巴山成矿带重晶石中的有机质是通过氧化作用降解，并没有进入甲烷生成阶段，而毒重石的CO2-3来自甲烷厌氧氧化，重晶石和毒重石是在孔隙水中由Ba2+与SO2-4或 CO2-3结合形成，并不发育喷流出海底的冷泉活动。因此，华南早寒武世重晶石矿和毒重石矿在早期成岩过程，甲烷的来源和浓度可能在区域上存在差异。秦岭-大巴山成矿带在寒武纪早期的海底沉积物中可能发育有富含甲烷的流体，在AOM主导的硫酸盐还原作用下，导致水体中CO2-3浓度升高，SO2-4浓度降低，进而结晶沉淀毒重石。而江南成矿带重晶石矿在早期成岩过程中是否发育富含甲烷流体还需更多证据支持。综上所述，成岩作用不仅导致了钡的迁移、富集和再结晶，也可能是秦岭-大巴山成矿带重晶石和毒重石的矿化分带重要控制因素。但成岩作用对华南早寒武世重晶石矿和毒重石矿的控制机制还需深入探讨，尤其是甲烷产生的机制以及是否发育大规模冷泉活动还需深入研究。比如利用微区原位C同位素的技术手段进一步约束有机碳的来源（Himmler et al.，2015）；探讨毒重石矿体中的碳酸盐岩夹层是否为冷泉活动的产物等。
图12现代海洋成岩重晶石成因模式图（a）和冷泉重晶石成因模式图（b）（据周锡强等，2016修改）
Fig.12Formation of diagenetic barite (a) and formation of cold seep barite (b) in modern ocean (modified after Zhou Xiqiang et al., 2016)
4.4 矿床成因
根据钡的物质来源、沉积环境和成岩过程，沉积岩容矿型重晶石可以分为海洋自生重晶石、热液重晶石、冷泉重晶石和成岩重晶石四种不同成因类型（Griffith et al.，2012；周锡强等，2016）。Sr-S-O同位素是判断重晶石成因类型的重要手段（Griffith et al.，2018）。其中Sr同位素是示踪重晶石中钡来源的有效手段，S-O同位素组成可以反映海水中SO2-4来源以及微生物作用机制。海洋自生重晶石可以保留同期海水的信息，具有和同期海水较为一致的87Sr/86Sr、δ34S和δ18O组成特征（Paytan et al.，1993; Paytan et al.，1998）。热液、冷泉和成岩重晶石的87Sr/86Sr值变化范围较大，主要与流体在运移过程中，所反映的围岩或沉积物的组成有关（Paytan et al.，2002; Feng Dong et al.，2011）。冷泉和成岩重晶石的结晶过程伴随着微生物的还原作用，从而具有高于同期海水的δ34S和δ18O值（Greinert et al.，2002）。热液重晶石的形成受控于热液流体中HS-氧化形成的SO2-4与海水中SO2-4的混合，从而导致热液重晶石具有低于同期海水δ34S值的特征（Hannington et al.，1988; Seal et al.，2006）。
图13江南成矿带成岩重晶石的不同结构类型
Fig.13Microscopic images show various textures of diagenetic barite in the Jiangnan metallogenic belt
（a）—棱柱状重晶石；（b）—粒状重晶石；（c）—孔隙充填状重晶石；（d）—放射状重晶石（样品均采自大河边重晶石矿床）
(a) —prismatic barite; (b) —granular barite; (c) —barite filled in the interparticle pore spaces; (d) —acicular barite (all samples are from Dahebian barite deposit)
华南早寒武世重晶石矿的Sr-S-O同位素数据表明，华南重晶石矿与海洋自生、冷泉、热液和成岩重晶石的87Sr/86Sr、δ34S和δ18O组成均存在差别。华南早寒武世重晶石、毒重石矿的87Sr/86Sr比值整体上与同期海水基本一致，反映了钡可能主要来源于海水。海水中钡的富集过程与海洋生产力以及海洋氧化还原沉积环境密切相关。寒武纪早期扬子地台周缘表层海水中较高的生物原始生产率以及局部缺氧的受限盆地，促进了钡在海水中的大规模富集，从而为重晶石、毒重石沉淀提供物质基础。华南早寒武世重晶石、毒重石矿的δ34S和δ18O值普遍偏重，指示了强烈的微生物还原作用。一方面微生物还原作用强度在区域上的差异导致SO2-4的浓度在空间上不均匀分布，从而造成重晶石、毒重石矿在空间上的不连续分布。另一方面，微生物还原作用的驱动机制在区域上也存在差异，强烈的甲烷厌氧氧化作用可能是毒重石成矿的主要因素。
5 总结与展望
钡在海洋中的化学循环过程与海洋环境密切相关，海洋的生产力、氧化还原状态、化学组成、微生物作用、洋流作用等条件控制着钡的迁移富集以及重晶石的结晶沉淀。全球范围内大规模重晶石矿在早寒武世爆发式发育，反映了特殊的古海洋环境对重晶石的超常富集成矿具有控制作用。华南早寒武世沉积岩容矿型重晶石矿储量居世界首位，在空间上分布于扬子地台北缘的秦岭-大巴山成矿带和东南缘的江南成矿带。本文通过对比分析，认为两条成矿带在赋存围岩、矿物组成、结构构造、地球化学特征等方面具有高度相似性，反映了两条成矿带的重晶石矿总体上具有相同的物质来源，并形成于相似的古海洋环境中。两条成矿带的成矿物质主要为海水，但江南成矿带中的成矿物质并不能排出热液流体的参与。寒武纪早期扬子地台周缘海洋高生产力，以及SO2-4有限的缺氧盆地导致了Ba2+在海水中大规模富集，当富含SO2-4的海水输入后，与富含Ba2+的海水混合结晶并沉积重晶石。微生物的还原作用在区域上存在差异，导致SO42-的浓度在空间上呈不均匀分布，从而造成重晶石矿在空间上不连续分布。沉积后的重晶石在成岩作用下发生部溶解和重结晶，重晶石矿和毒重石矿在成岩过程中的有机质降解的程度以及硫酸盐还原作用存在差异，相对重晶石矿，秦岭-大巴山成矿带中毒重石矿中有机质降解程度高，可能进入甲烷生成阶段，CO2-3离子可能来自于甲烷厌氧氧化作用。
虽然有证据表明寒武纪早期在秦岭-大巴山成矿带和江南成矿带可能分别发育有热液喷流和冷泉活动，但是热液喷流和冷泉活动对重晶石和毒重石矿形成的贡献还需要进一步厘定。江南成矿带陡山沱组Pb-Zn矿与重晶石矿的时空关系，以及秦岭-大巴山成矿带中甲烷产生的机制以及运移方式，均需要地球化学数据的支持。此外，古海洋环境对华南早寒武世重晶石大规模富集成矿的控制作用还需深入探讨，包括古海洋生产力水平、SO2-4的来源和空间分布等，不仅制约了钡的大规模富集成矿，也对我们理解寒武纪早期这一特殊地质历史时期的海洋环境演化具有重要意义。
针对华南早寒武世重晶石矿的研究现状和存在问题，本文认为可通过秦岭-大巴山成矿带和江南成矿带的精细对比研究工作，利用微区原位分析测试技术，开展重晶石的原位Sr-S-O-C同位素以及微观组成结构研究，结合“将今论古”的方法，可以更好地约束钡的物质来源，并精细刻画重晶石的沉积-成岩过程。此外，寒武纪早期扬子地台周缘海水中较高的生产力与钡的大规模富集之间的关系还缺少有力证据支持。随着测试技术的提高，获得高精度Ba同位素成分成为可能，而Ba同位素的分馏过程被认为是示踪古海洋生产力的有力手段，可以预见，利用Ba同位素研究寒武纪早期扬子地台周缘海水中生产力水平，并进一步探讨钡的大规模富集成矿与寒武纪早期这一特殊地质历史时期的海洋环境之间的关系，将对深入认识Ba的物质循环以及早寒武世地球表生环境演化过程具有良好的前景。
图1世界主要国家重晶石储量分布（据美国地质调查局，2023）
Fig.1Proportion of barite reserves of major countries over the word (after United States Geological Survey, 2023)
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图2全球主要沉积岩容矿型重晶石矿时空分布图（据Han Tao et al.，2022；潘忠飞等，2023）
Fig.2Spatial and temporal distribution of significant barite deposits over the word (after Han Tao et al., 2022; Pan Zhongfei et al., 2023)
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图3现代海洋中钡的地球化学循环过程示意图（a，据Horner et al.，2021 修改）及冷泉和热液活动产出地质背景图（b，据周锡强等，2016修改）
Fig.3Simplified diagram showing geochemical cycle of Ba in modern ocean (a, modified from Horner et al., 2021) and simplified diagram showing geological background of cold seep and hydrothermal activities (b, modified from Zhou Xiqiang et al., 2016)
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图4重晶石、毒重石、方解石和硬石膏在25℃和0.101325 MPa 水溶液中的相图（据Maynard et al.，1991修改）
Fig.4Phase diagram illustrating stability fields for Ba-Ca sulfates and carbonates in aqueous solution at 25℃ and 0.101325 MPa (modified from Maynard et al., 1991)
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图5华南寒武纪早期古地理环境及主要沉积岩容矿型矿产分布图（据Lehmann et al.，2016修改）
Fig.5Reconstruction of Early Cambrian paleogeographic environment and distribution of major sedimentary rock-hosted deposits of South China (modified from Lehmann et al., 2016)
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图6秦岭-大巴山成矿带和江南成矿带典型重晶石矿和毒重石矿地层柱状图（据吕志成等，2005；方旭等，2013；王富良等，2020；夏瑞等，2021修改）
Fig.6Stratigraphy sequences of typical barite and witherite deposits from the Jiangnan and Qinling-Dabashan metallogenic belts (modified after Lü Zhicheng et al., 2005; Fang Xu et al., 2013; Wang Fuliang et al., 2020; Xia Rui et al., 2021)
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图7秦岭-大巴山重晶石—毒重石成矿带区域地质图（据Xu Lingang et al.，2016修改）
Fig.7Reginal geological map shows representative barite and witherite deposits in the Qinling-Dabashan metallogenic belt (modified from Xu Lingang et al., 2016)
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图8秦岭-大巴成矿带不同结构、构造类型重晶石和毒重石矿石显微照片
Fig.8Microscopic images show various textures and structures of barite and witherite ores in the Qinling-Dabashan metallogenic belt
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图9江南成矿带不同构造类型重晶石矿石照片
Fig.9Images show various structures of barite ore in the Jiangnan metallogenic belt
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图10秦岭-大巴山成矿带与江南成矿带重晶石和毒重石87Sr/86Sr同位素组成对比
Fig.10Comparison of 87Sr/86Sr values of barite and witherite between the Qinling-Dabashan and Jiangnan metallogenic belt
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图11秦岭-大巴山成矿带与江南成矿带重晶石δ34S值对比
Fig.11Comparison of δ34S values of barite between the Qinling-Dabashan and Jiangnan metallogenic belt
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图12现代海洋成岩重晶石成因模式图（a）和冷泉重晶石成因模式图（b）（据周锡强等，2016修改）
Fig.12Formation of diagenetic barite (a) and formation of cold seep barite (b) in modern ocean (modified after Zhou Xiqiang et al., 2016)
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图13江南成矿带成岩重晶石的不同结构类型
Fig.13Microscopic images show various textures of diagenetic barite in the Jiangnan metallogenic belt
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表1秦岭-大巴山成矿带典型重晶石和毒重石矿床地质特征
Table1Geological characteristics of typical barite and witherite deposits in the Qinling-Dabashan metallogenic belt
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表2江南成矿带典型重晶石矿床地质特征
Table2Geological characteristics of typical barite deposits in the Jiangnan metallogenic belt
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表3秦岭-大巴山成矿带与江南成矿带矿物学和地球化学特征对比
Table3Comparison of mineralogical and geochemical composition between the Qinling-Dabashan and Jiangnan metallogenic belts
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袁彭，徐林刚，闫浩，付雪瑞，孙凯，周天霁.2025.华南早寒武世沉积岩容矿型重晶石矿的成矿作用与研究展望[J].地质学报,99(3):1005-1026.
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YUAN Peng, XU Lingang, YAN Hao, FU Xuerui, SUN Kai, ZHOU Tianji.2025.Metallogenesis of Early Cambrian massive barite deposits in southern China: An overview and prospects[J].Acta Geologica Sinica,99(3):1005-1026.
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图1世界主要国家重晶石储量分布（据美国地质调查局，2023）
Fig.1Proportion of barite reserves of major countries over the word (after United States Geological Survey, 2023)
图2全球主要沉积岩容矿型重晶石矿时空分布图（据Han Tao et al.，2022；潘忠飞等，2023）
Fig.2Spatial and temporal distribution of significant barite deposits over the word (after Han Tao et al., 2022; Pan Zhongfei et al., 2023)
图3现代海洋中钡的地球化学循环过程示意图（a，据Horner et al.，2021 修改）及冷泉和热液活动产出地质背景图（b，据周锡强等，2016修改）
Fig.3Simplified diagram showing geochemical cycle of Ba in modern ocean (a, modified from Horner et al., 2021) and simplified diagram showing geological background of cold seep and hydrothermal activities (b, modified from Zhou Xiqiang et al., 2016)
图4重晶石、毒重石、方解石和硬石膏在25℃和0.101325 MPa 水溶液中的相图（据Maynard et al.，1991修改）
Fig.4Phase diagram illustrating stability fields for Ba-Ca sulfates and carbonates in aqueous solution at 25℃ and 0.101325 MPa (modified from Maynard et al., 1991)
图5华南寒武纪早期古地理环境及主要沉积岩容矿型矿产分布图（据Lehmann et al.，2016修改）
Fig.5Reconstruction of Early Cambrian paleogeographic environment and distribution of major sedimentary rock-hosted deposits of South China (modified from Lehmann et al., 2016)
图6秦岭-大巴山成矿带和江南成矿带典型重晶石矿和毒重石矿地层柱状图（据吕志成等，2005；方旭等，2013；王富良等，2020；夏瑞等，2021修改）
Fig.6Stratigraphy sequences of typical barite and witherite deposits from the Jiangnan and Qinling-Dabashan metallogenic belts (modified after Lü Zhicheng et al., 2005; Fang Xu et al., 2013; Wang Fuliang et al., 2020; Xia Rui et al., 2021)
图7秦岭-大巴山重晶石—毒重石成矿带区域地质图（据Xu Lingang et al.，2016修改）
Fig.7Reginal geological map shows representative barite and witherite deposits in the Qinling-Dabashan metallogenic belt (modified from Xu Lingang et al., 2016)
图8秦岭-大巴成矿带不同结构、构造类型重晶石和毒重石矿石显微照片
Fig.8Microscopic images show various textures and structures of barite and witherite ores in the Qinling-Dabashan metallogenic belt
图9江南成矿带不同构造类型重晶石矿石照片
Fig.9Images show various structures of barite ore in the Jiangnan metallogenic belt
图10秦岭-大巴山成矿带与江南成矿带重晶石和毒重石87Sr/86Sr同位素组成对比
Fig.10Comparison of 87Sr/86Sr values of barite and witherite between the Qinling-Dabashan and Jiangnan metallogenic belt
图11秦岭-大巴山成矿带与江南成矿带重晶石δ34S值对比
Fig.11Comparison of δ34S values of barite between the Qinling-Dabashan and Jiangnan metallogenic belt
图12现代海洋成岩重晶石成因模式图（a）和冷泉重晶石成因模式图（b）（据周锡强等，2016修改）
Fig.12Formation of diagenetic barite (a) and formation of cold seep barite (b) in modern ocean (modified after Zhou Xiqiang et al., 2016)
图13江南成矿带成岩重晶石的不同结构类型
Fig.13Microscopic images show various textures of diagenetic barite in the Jiangnan metallogenic belt
表1秦岭-大巴山成矿带典型重晶石和毒重石矿床地质特征
Table1Geological characteristics of typical barite and witherite deposits in the Qinling-Dabashan metallogenic belt
表2江南成矿带典型重晶石矿床地质特征
Table2Geological characteristics of typical barite deposits in the Jiangnan metallogenic belt
表3秦岭-大巴山成矿带与江南成矿带矿物学和地球化学特征对比
Table3Comparison of mineralogical and geochemical composition between the Qinling-Dabashan and Jiangnan metallogenic belts
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