烃源岩作为铀源岩的可能性:研究现状与展望

doi:10.13745/j.esf.sf.2023.5.33

地学前缘 ›› 2024, Vol. 31 ›› Issue (2): 284-298.DOI: 10.13745/j.esf.sf.2023.5.33

烃源岩作为铀源岩的可能性:研究现状与展望

刘超¹^,²^,³(), 付晓飞¹^,³^,^*(), 李扬成⁴, 王海学¹^,³, 孙冰¹, 郝炎¹, 胡慧婷¹, 杨子成¹^,³, 李依霖¹^,³, 谷社峰⁴, 周爱红⁴, 马成龙⁵

1.东北石油大学非常规油气研究院, 黑龙江大庆 163318
2.东北石油大学应用技术研究院, 黑龙江大庆 163318
3.东北石油大学 “陆相页岩油气成藏及高效开发”教育部重点实验室, 黑龙江大庆 163318
4.大庆油田有限责任公司, 黑龙江大庆 163712
5.中国石油辽河油田分公司勘探开发研究院, 辽宁盘锦 124010

收稿日期:2023-01-26 修回日期:2023-04-27 出版日期:2024-03-25 发布日期:2024-04-18
通讯作者: *付晓飞(1973—),男,教授,博士生导师,主要从事断层封闭性及与流体运移研究工作。E-mail: fuxiaofei2008@sohu.com
作者简介:刘超(1985—),男,副教授,主要从事油气地球化学、油气成藏、油铀共存机理研究工作。E-mail: lcyxdz@163.com
基金资助:
黑龙江省自然科学基金资助项目(LH2022D014);东北地质科技创新中心区创基金项目(QCJJ2022-31);东北石油大学国家自然科学基金培育项目(2022GPL-05)

Can hydrocarbon source rock be uranium source rock?—a review and prospectives

LIU Chao¹^,²^,³(), FU Xiaofei¹^,³^,^*(), LI Yangcheng⁴, WANG Haixue¹^,³, SUN Bing¹, HAO Yan¹, HU Huiting¹, YANG Zicheng¹^,³, LI Yilin¹^,³, GU Shefeng⁴, ZHOU Aihong⁴, MA Chenglong⁵

1. Institute of Unconventional Oil and Gas, Northeast Petroleum University, Daqing 163318, China
2. Institute of Applied Technology, Northeast Petroleum University, Daqing 163318, China
3. Ministry of Education Key Laboratory of Continental Shale Hydrocarbon Accumulation and Efficient Development, Northeast Petroleum University, Daqing 163318, China
4. Daqing Oilfield Company Ltd., Daqing 163712, China
5. Liaohe Oilfield Company Research Institute of Petroleum Exploration & Development, Panjin 124010, China

Received:2023-01-26 Revised:2023-04-27 Online:2024-03-25 Published:2024-04-18

摘要/Abstract

摘要：

烃源岩与砂岩型铀矿通常同盆共生,除了提供矿化剂之外,烃源岩能否成为铀源岩对砂岩型铀矿的勘探范围向盆地纵深部位拓展具有重要意义。研究针对烃源岩能否成为铀源岩所涉及的三个关键问题,即“铀从烃源岩中迁出的比例、如何随地层流体运移、在何种条件下沉淀和聚集”,梳理了国内外相关研究进展,指出了有必要加强研究的薄弱环节。结果表明:热模拟实验证实烃源岩中的铀能够迁出,迁出的铀很可能以U(IV)/U(VI)混合的形式随含烃地层水和石油运移,温度、压力的降低以及pH、Eh变化会导致铀溶解度的下降和铀运移载体的分解而发生铀沉淀,沉淀物也可能重新被含氧的地层水溶解。问题与建议包括:(1)铀从烃源岩中迁出的比例存在不确定性,迁出的机制以及地质规律尚不清楚,需要开展进一步的生烃-排铀模拟实验及排铀动力学表征研究;(2)铀在低温、含烃、还原性热液中的赋存状态是研究其迁移机制的基础,目前对与铀结合的优势配体的类型、产物热力学性质、铀在含烃地下水与石油中的分布比例所知甚少,有必要开展基于热模拟实验的原位测试研究;(3)携铀流体向浅部运移的过程中温度、压力、pH、Eh、有机-无机组分的变化控制铀的迁移/沉淀,不同组合条件下铀赋存形式的转化规律、主控因素尚不清楚,有待开展多因素、多变量的烃-铀运移模拟实验进行揭示。

关键词: 烃源岩, 铀源, 油气, 砂岩型铀矿, 迁移, 成矿机制

Abstract:

The coexistence of hydrocarbon source rocks and sandstone-hosted uranium (U) deposits in the same basin has been widely reported. Hydrocarbon source rock contributes to uranium precipitation and enrichment by providing oil and gas; whereas, whether it can be a source of uranium supply is of great relevance as to weather uranium prospecting should expand deep into the basin. This study reviews relevant domestic and international studies and offers perspectives on this topic, focusing on three key issues: migration potential of uranium in source rock, possible ways of uranium transport by formation fluids, and mechanisms of uranium precipitation and accumulation. Hydrothermal modeling results show that uranium migration can occur during hydrocarbon generation and expulsion, and the migrated-uranium, probably a mix of U(IV) and U(VI), is likely transported by both hydrocarbon-bearing formation water and oils. The transported-uranium precipitates due to a decrease of uranium solubility and decomposition of the transport fluids caused by a decrease of temperature and pressure and change of pH and Eh; the uranium precipitates can also redissolve in oxygen-rich formation water. The main perspectives are: (1) the amount of migrated-uranium is uncertain, and the mechanism and laws of U migration are still unclear, thus further modeling experiments on source rock-uranium system is recommended to understand the kinetics of uranium migration. (2) Up to now, little is known about the dominant U mobile forms and their thermodynamic properties and distribution between hydrocarbon-bearing formation water and oil, thus, in-situ thermal testing via thermal simulation experiments is recommended to address this issue. (3) During uranium upward transport, changes in temperature, pressure, Eh, and organic/inorganic components of the transport fluids control uranium geochemistry, thereby, in order to understand uranium geochemistry and its controlling factors under different conditions, multi-variable simulation experiments on hydrocarbon-uranium transport is suggested.

Key words: hydrocarbon source rocks, source of uranium, oil and gas, sandstone-hosted uranium deposit, mobile, metallogenetic mechanism

中图分类号:

刘超, 付晓飞, 李扬成, 王海学, 孙冰, 郝炎, 胡慧婷, 杨子成, 李依霖, 谷社峰, 周爱红, 马成龙. 烃源岩作为铀源岩的可能性:研究现状与展望[J]. 地学前缘, 2024, 31(2): 284-298.

LIU Chao, FU Xiaofei, LI Yangcheng, WANG Haixue, SUN Bing, HAO Yan, HU Huiting, YANG Zicheng, LI Yilin, GU Shefeng, ZHOU Aihong, MA Chenglong. Can hydrocarbon source rock be uranium source rock?—a review and prospectives[J]. Earth Science Frontiers, 2024, 31(2): 284-298.

图/表 9

图1 砂岩铀矿“渗入+渗出”双重铀源成矿模式图

Fig.1 Metallogenic model of sandstone-hosted uranium deposit characterized by dual uranium sources consisting of supergene altered rocks and uranium-bearing hydrocarbon source rocks

表1 烃源岩层含铀量统计表

Table 1 A summary of uranium content in source rocks

盆地/地区	烃源岩层	铀含量/10^-6	文献来源
鄂尔多斯盆地铜川地区	长7段暗色泥岩	5.40~140.00/(51.10)	[19]
鄂尔多斯盆地东胜-准格尔旗	直罗组含泥煤岩	15.33~30.99/(21.49)	[20]
江西省修水地区	观音堂组、王音铺组黑色页岩	9.37~202.00/(47.47)	[21]
中国华南地区	牛蹄塘组黑色页岩	0.84~97.9/(13.10)	[22]
塔里木盆地北部	玉尔吐斯组黑色页岩	21.10~194.90/(61.90)	[23]
修武盆地	下寒武统黑色页岩	0.57~48.60/(11.89)	[24]
中国湘西地区	上震旦—下寒武统黑色页岩	2.29~138.07/38.09)	[25]
松辽盆地钱家店地区	姚家组灰色泥岩	4.75~5.00/(4.88)	[11]
中国赣北地区	震旦系和寒武系碳硅泥岩	8.11~61.56/(30.05)	[26]
瑞典	Upper Alum	100.00~300.00/(118.00)	[27]
伊利诺斯盆地	New Albany	6.79~63.88/(24.20)	[28]
阿巴拉契亚盆地	Woodford (George)	8.10~61.80/(29.36)	[29]
阿巴拉契亚盆地	Cleveland	1.00~22.60/(9.10)	[29]
威利斯顿盆地	Upper Bakken	21.40~70.60/(42.50)	[29]
威利斯顿盆地	Lower Bakken	22.20~176.30/(77.50)	[29]
摩洛哥	Timahdit	(41.00)	[30]
英国谢菲尔德地区	Parkhouse	5.00~199.00/(35.75)	[31]
阿巴拉契亚盆地	Marcellus	1.90~470/(14.07)	[32]
爱尔兰西部	石炭系页岩	5.86~158.00/9.52	[33]

表2 烃源岩排铀热模拟实验

Table 2 A summary of simulation experiments of uranium emitted from source rocks

体系	样品类型	TOC 含量/%	有机质类型	铀含量/ 10^-6	实验条件 (T为温度,p为压力,t为加热时间)	EasyR_o/ %	活化铀比例或迁出率/%	文献来源
高压釜封闭体系,搅拌	泥岩粉末	16.38	II₂	180	T=200 ℃,p=2、3、4、5 MPa,t=72 h	0.35	59.5~77.8	[12]
	泥岩粉末	16.38	II₂	180	p=2 MPa,T=30、100、150、200 ℃,t=72 h	0.2~0.35	12.5~59.5
	煤岩粉末		III	60	T=260 ℃,p=2、3、4、5 MPa,t=72 h	0.57	79.1~95.5
	煤岩粉末		III	60	p=3 MPa,T=220、260、300、340 ℃,t=72 h	0.4~1.10	90.3~97.7
高压釜+黄金管封闭体系	页岩粉末	18.48	II	124.5	T=350 ℃,p=70 MPa,t=24 h	0.92	0	[27]
高压釜半封闭体系	人工样品		III	50	T=120 ℃,p=7 MPa,t=144 h	0.21		[41]
					T=200 ℃,p=7 MPa,t=144 h	0.34
					T=200 ℃,p=28 MPa,t=48 h	0.31
					T=200 ℃,p=28 MPa,t=144 h	0.34
					T=300 ℃,p=28 MPa,t=144 h	0.68

图2 泥岩、煤岩样品在不同实验条件下的排铀率(据文献[12])

Fig.2 Uranium expulsion rate of shale and coal samples under different experimental conditions. Adapted from [12].

图3 含铀煤岩样品在不同条件下的排烃-排铀曲线(据文献[41]) a—实验装置及取样位置示意图;b—各测试点有机碳丰度曲线;c—各测试点含铀量;d—各测试点铀与有机碳含量的关系。A:120 ℃, 7 MPa, 144 h; B:200 ℃, 7 MPa, 144 h; C:200 ℃, 28 MPa, 48 h; D:200 ℃, 28 MPa, 144 h; E:300 ℃, 28 MPa, 144 h。

Fig.3 Simulation experiment of hydrocarbon generation and uranium expulsion of uranium-bearing coal under different temperature and pressure. Adapted from [41].

图4 哈达图铀矿床渗出铀成矿模式图(据文献[17]) E—古近系;K2e—二连组;K1s2—赛汉组上段;K1t—腾格尔组。

Fig.4 Exudative metallogenic model of Hadatu uranium deposit. Adapted from [17].

图5 Witwatersrand盆地沥青中铀矿物的微观图像(据文献[4]) a—碎屑铀矿物被有机质部分溶蚀和置换:b—沥青中次棱角状铀矿物聚合体;c—具有“海绵状”结构的次生铀矿物集合体;d—沥青脉中原位形成的自形铀矿物。

Fig.5 Uraninite grains with variable morphology in Carbon Leader Reef, Witwatersrand Supergroup, South Africa. Adapted from [4].

图6 排铀率与生烃量、EasyRo关系(数据据文献[12])

Fig.6 The relationship between uranium-expulsion rate and hydrocarbon-generation content and EasyRo. Data adapted from [12].

图7 含烃还原性热液中富赋存状态与运移模式图

Fig.7 Occurrence of uranium in hydrocarbon bearing and reducing hydrothermal fluid

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烃源岩作为铀源岩的可能性:研究现状与展望

Can hydrocarbon source rock be uranium source rock?—a review and prospectives

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