铀在海相烃源岩中富集的条件及主控因素

doi:10.11867/j.issn.1001-8166.2017.02.0199

地球科学进展 ›› 2017, Vol. 32 ›› Issue (2): 199 -208. doi: 10.11867/j.issn.1001-8166.2017.02.0199

铀在海相烃源岩中富集的条件及主控因素

蔡郁文 ^1, ^2, ³(

), 王华建 ^2, ³, 王晓梅 ^2, ³, 何坤 ^2, ³, 张水昌 ^2, ³, 吴朝东 ¹

1.北京大学地球科学与空间科学学院,北京 100871
2.中国石油天然气股份有限公司油气地球化学重点实验室,北京 100083
3.中国石油勘探开发研究院,北京 100083

收稿日期:2016-10-20 修回日期:2017-01-02 出版日期:2017-02-20
基金资助:
国家自然科学基金重点项目“中国元古代海相烃源岩形成的生物、海洋和地质因素及耦合关系研究”(编号:41530317);国家自然科学基金青年科学基金项目“铀的放射性作用对有机质成熟和生烃的影响”(编号:41602144)资助

Formation Conditions and Main Controlling Factors of Uranium in Marine Source Rocks

Yuwen Cai ^1, ^2, ³( ), Huajian Wang ^2, ³, Xiaomei Wang ^2, ³, Kun He ^2, ³, Shuichang Zhang ^2, ³, Chaodong Wu ¹

1.School of Earth and Space Sciences, Peking University,Beijing 100083,China
2.Key Laboratory of Petroleum Geochemistry, China National Petroleum Corporation,Beijing 100083,China
3.Research Institute of Petroleum Exploration and Development,Beijing 100083,China

Received:2016-10-20 Revised:2017-01-02 Online:2017-02-20 Published:2017-02-20
About author:
First author:Cai Yuwen(1989-), female, Daqing City, Heilongjiang Province, Ph. D student. Research areas include petroleum geochemistry.E-mail:caiyuwen1@aliyun.com
Supported by:
Project supported by the National Natural Science Foundation of China “Influences of biology, ocean and geology in the formation of marine source rocks and their coupling relationships”(No.41530317);The Young Scientists Fund of the National Natural Science Foundation of China “Effects of radioactivity of uranium on organic matter maturation and hydrocarbon generation”(No.41602144)

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国内外沉积盆地中铀的富集不同程度地伴随烃源岩的形成。铀作为一种兼具催化、氧化和放射性的特殊元素, 其对有机矿产的形成及演化可能具有重要的促进作用,通过调查并统计国内外烃源岩中铀含量,在分析铀与各类矿物、有机质及微生物等相互作用的基础上, 讨论了铀在海相烃源岩中的富集条件及主控因素, 提出古大气和古海洋的氧化程度是烃源岩中铀富集的主要控制因素, 陆地含氧风化和海底热液可能是海相沉积铀的2个主要来源,含铁矿物组成、有机质、磷酸盐矿物、黏土矿物及一些微生物等均可导致铀价态转化, 并作为载体, 通过吸附或络合作用使铀在沉积物中富集。因此, 铀富集可能是烃源岩形成的一个伴随结果。

关键词: 铀, 烃源岩, 铁, 有机质, 古海洋

The research of petroleum exploration demonstrates that source rocks, developed in petroleum-bearing sedimentary basins worldwide, are accompanied by uranium to different degrees.As a special element with catalytic, oxidative and radioactive features, uranium may play important roles in the source rock formation and hydrocarbon generation. In this paper, we systematically discussed the formation conditions and main controlling factors of uranium in marine source rocks based on the comprehensive analysis of uranium contents in the worldwide source rocks and the interactions of uranium with minerals, organic materials and microbes. The results indicated that oxidative degrees of ancient atmosphere and palaeo-ocean were governing factors of uranium enrichment in source rocks. Oxidative weathering and hydrothermal solution might be the two main sources of marine sedimentary uranium. In addition, iron-bearing minerals, phosphate minerals, clay minerals, organic materials, and microbes were of great significance in promoting the transformation of the uranium valence states. They could also act as carriers to absorb or combine uranium, resulting in the enrichment of uranium in sediments. Therefore, the enrichment of uranium might be an inevitable result of source rocks formation.

Key words: Uranium, Source rocks, Iron, Organic materials, Palaeo-ocean.

中图分类号:

P619.14

图1 地史时期沉积物中的铀和有机质含量及大气氧化进程(修改并补充自参考文献[13,17~22])
图中阴影为碳酸盐岩中碳同位素的变化 ^{[

23
]}

Fig.1 U and TOC contents in organic-rich shales, and the atmospheric oxidation process through geological time(modified and supplemented after references[13,17~22])
Gray-band: Inorganic carbon isotope composition of carbonates ^{[

23
]}

表1 国内不同时期烃源岩中的TOC,U,Fe,Al,P含量及比值

Table 1 TOC, U, Fe, Al, P content and ratios in organic shales through time

层位	地区	沉积环境	TOC /wt%	U /(μg/g)	Fe /wt%	Al /wt%	P /wt%	U/TOC /×10^-4	U/Fe /×10^-4	U/Al /×10^-4	U/P /×10^-4	样品 /个
串岭沟组(Pt₁)	华北克拉通	潮下—泻湖	1.48	2.13	3.76	9.23	0.04	1.43	0.57	0.23	53.25	31^*
下马岭组(Pt₂)	华北克拉通	浅海	4.94	5.61	2.89	5.99	0.19	1.14	1.94	0.82	26.0	146^*
大塘坡组(Pt₃)	扬子地台	浅海—斜坡	2.47	1.45	3.68	5.95	0.17	0.59	0.39	0.24	8.53	58^*
陡山沱组(Pt₃)	扬子地台	深水陆棚	8.49	16.19	2.46	3.22	0.17	2.86	6.57	5.03	95.03	15^*
牛蹄塘组(∈₁)	扬子地台	深水盆地	3.79	40.70	2.25	4.59	0.22	10.74	18.09	8.87	185.0	45^*
五峰—龙马溪组(O₃-S₁)	四川盆地	深水陆棚	4.12	11.27	2.41	5.36	0.04	2.73	4.67	2.10	281.75	24^{[ 37 ]}
延长组(T₃)	鄂尔多斯盆地	半深—深湖	13.73	45.93	6.73	7.17	0.18	2.98	5.32	12.04	251.38	22^{[ 38 ]}

表1 国内不同时期烃源岩中的TOC,U,Fe,Al,P含量及比值

Table 1 TOC, U, Fe, Al, P content and ratios in organic shales through time

层位	地区	沉积环境	TOC /wt%	U /(μg/g)	Fe /wt%	Al /wt%	P /wt%	U/TOC /×10^-4	U/Fe /×10^-4	U/Al /×10^-4	U/P /×10^-4	样品 /个
串岭沟组(Pt₁)	华北克拉通	潮下—泻湖	1.48	2.13	3.76	9.23	0.04	1.43	0.57	0.23	53.25	31^*
下马岭组(Pt₂)	华北克拉通	浅海	4.94	5.61	2.89	5.99	0.19	1.14	1.94	0.82	26.0	146^*
大塘坡组(Pt₃)	扬子地台	浅海—斜坡	2.47	1.45	3.68	5.95	0.17	0.59	0.39	0.24	8.53	58^*
陡山沱组(Pt₃)	扬子地台	深水陆棚	8.49	16.19	2.46	3.22	0.17	2.86	6.57	5.03	95.03	15^*
牛蹄塘组(∈₁)	扬子地台	深水盆地	3.79	40.70	2.25	4.59	0.22	10.74	18.09	8.87	185.0	45^*
五峰—龙马溪组(O₃-S₁)	四川盆地	深水陆棚	4.12	11.27	2.41	5.36	0.04	2.73	4.67	2.10	281.75	24^{[ 37 ]}
延长组(T₃)	鄂尔多斯盆地	半深—深湖	13.73	45.93	6.73	7.17	0.18	2.98	5.32	12.04	251.38	22^{[ 38 ]}

图2 铀在磁铁矿表面的还原沉淀 ^{[

39
]}

Fig.2 Model illustrating remediation of uranium at magnetite surfaces by reductive precipitation ^{[

39
]}

表2 沉积物中铀富集条件及赋存状态

Table 2 Enrichment and occurrence of uranium in sediments

反应方式		反应物	赋存状态	水体环境
化学	氧化还原、络合作用	H₂S,CH₄	U(IV)固体颗粒	缺氧硫化
化学	氧化还原、络合作用	Fe(II),有机质	与含铁矿物,有机质, 磷酸结合的U(VI)金属络合物	缺氧—亚氧化
物理	吸附作用	腐殖酸,含磷矿物,含铁矿物,黏土矿物	有机质,或(和)U(IV) 固体颗粒	任何环境
生物	吸附作用	微生物	U(IV)固体颗粒	任何环境

表2 沉积物中铀富集条件及赋存状态

Table 2 Enrichment and occurrence of uranium in sediments

反应方式		反应物	赋存状态	水体环境
化学	氧化还原、络合作用	H₂S,CH₄	U(IV)固体颗粒	缺氧硫化
化学	氧化还原、络合作用	Fe(II),有机质	与含铁矿物,有机质, 磷酸结合的U(VI)金属络合物	缺氧—亚氧化
物理	吸附作用	腐殖酸,含磷矿物,含铁矿物,黏土矿物	有机质,或(和)U(IV) 固体颗粒	任何环境
生物	吸附作用	微生物	U(IV)固体颗粒	任何环境

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