Uranium "Stable" Isotope Fractionation and Its Applications in Earth Science
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摘要: 铀“稳定”同位素（238U/235U，通常记为δ238U）目前已经成为非传统稳定同位素领域的研究热点.20世纪人们曾经认为铀同位素不存在分馏，因而铀同位素研究发展缓慢.然而随着分析技术的发展，人们发现自然界中铀同位素238U和235U存在显著的分馏，可以作为良好的示踪工具.迄今为止，已经有大量铀同位素作为古氧化还原指标的研究发表，比如用铀同位素示踪地球近地表环境氧含量随时间的演化以及生物大灭绝与海洋氧化还原状态之间的潜在关系.尽管铀同位素在水圈和生物圈协同演化领域取得了丰硕的研究成果，但仍有不少问题亟待深入解决.例如，生物和非生物还原高价铀的微观反应过程对铀同位素分馏的影响，以及铀同位素如何示踪铀矿物质来源等.系统总结了铀同位素地球化学最近十年的研究进展，希望将来铀同位素在铀多金属矿床成因和高温地球化学领域能有所突破.Abstract: Uranium isotope (238U/235U, usually expressed as δ238U) has been the research hotspot in the field of non-traditional stable isotopes. In the last century, it was thought that uranium isotope fractionation did not exist, so the development of uranium isotope research was very slow. However, with the development of the analytical technology, it has been found that there exists significant fractionation between238U and 235U in nature, which makes uranium isotopes an ideal tracer in Earth science. Indeed, overwhelming amounts of studies of uranium isotopes as a paleo-redox proxy have been published so far, most of which use uranium isotope to track the evolution of oxygen levels of Earth's subaerial environments through time and, furthermore, the potential relationship between the several big mass extinctions and the redox conditions of the oceans. Although researches on uranium isotope have achieved progresses in the co-evolution of the hydrosphere and biosphere, some problems still remain some unsolved. For example, the effects of microcosmic pathways of biological and abiotic reduction reactions on uranium isotope fractionation, and how the 238U/235U can trace the source of uranium ore deposits. Here, in this paper, it provides an overview of the uranium and its isotope geochemistry over the last decades, aiming at promoting applications of uranium isotopes in the genesis of uranium polymetallic deposits and high-temperature geochemistry in the future.
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Key words:
- uranium isotopes /
- fractionation mechanism /
- tracer /
- oxygen level /
- mass extinction /
- redox condition /
- U ore deposit /
- geochemistry
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图 1 Th和U元素在铀特效树脂U-TEVA的分配系数(Kd)随酸硝酸和盐酸浓度的变化(数据引自Tissot and Dauphas, 2015)
Fig. 1. The distribution coefficients of Th and U on U-TEVA resin in the concentration of HNO3 and HCl (data sources are from Tissot and Dauphas, 2015)
图 2 用双稀释剂和只用样品标样间插法(SSB)法得到的铀同位素结果对比(数据来源于Tissot and Dauphas, 2015)
Fig. 2. Comparison of uranium isotope compositions obtained from double spike and just sample-standard bracketing(data sources are from Tissot and Dauphas, 2015)
图 3 自然界主要的铀同位素储库
数据来源：Stirling et al.（2007）；Weyer et al.（2008）；Romaniello et al.（2013）；Montoya-Pino et al.（2010）；Noordmann et al.(2012, 2016)；Telus et al.（2012）；Andersen et al.(2014, 2015, 2017)；Goto et al.（2014）；Goldmann et al.（2015）；Tissot and Dauphas（2015）；Wang et al.（2016）；Rolison et al.（2017）；图修改自Tissot and Dauphas（2015）
Fig. 3. Uranium isotope compositions of main reservoirs in narure
图 4 海洋系统铀同位素储库与质量平衡示意
铀同位素平衡关系为：δ238U河流=δ238U强还原×f强还原+δ238U弱还原×f弱还原+δ238U原生碳酸盐×f原生碳酸盐+ δ238U铁锰结壳×f铁锰结壳+ δ238U热液蚀变物质×f热液蚀变物质，f为各个储库所占比例.数据来源于Stirling et al.（2007）；Weyer et al.（2008）；Romaniello et al.（2009）；Montoya-Pino et al.（2010）；Noordmann et al.(2012, 2016)；Andersen et al.(2014, 2015, 2017)；Goto et al.（2014）；Tissot and Dauphas（2015）；Wang et al.（2016）；Rolison et al.（2017）；图修改自Tissot and Dauphas（2015）和Andersen et al.（2017）；三角形符号代表不同储库与海水之间的分馏程度
Fig. 4. Uranium isotope compositions of main reservoirs or sinks in ocean
图 5 全球铀循环卡通示意
其中AOC代表蚀变洋壳；MORB代表洋中脊玄武岩；OIB代表洋岛玄武岩；ARC代表大洋岛弧.图修改自Andersen et al.（2015）
Fig. 5. Cartoon of the terrestrial U isotope cycle over the history of Earth
图 6 反应进程中溶液中剩余的U6+的同位素组成
K为反应速率常数，K越大，反应速率越快.如图a所示，化学反应速率越快，分馏的程度就越小；反之就越大.图b为不同方法消耗原始溶液中U的反应进程（用lnT0.5来表征）与分馏因子α的相关性.数据引自Rademacher et al.（2006）；Stirling et al.（2007）；Stylo et al.（2015）；Wang et al.（2015a）；Brown et al.（2018）
Fig. 6. δ238U of dissolved uranium in the solution for each reaction rate as a function of remaining aqueous U fraction (a); Relationship between the half-life of aqueous U (representing the extent of U removal from solution) and the isotopic fractionation factor (α) in different experiments of previous studies (b)
图 7 吸附过程中溶解铀和被吸附的铀之间的同位素分馏.尽管实验所用吸附剂不同，铀同位素分馏程度基本在0.17‰~0.23‰
橘黄色圆圈代表实际观测到的海洋铁锰结核、海洋浮游植物与海水之间的偏差；数据来源Weyer et al.（2008）；Brennecka et al.（2011a）；Goto et al.（2014）；Jemison et al.（2016）；Wang et al.（2016）；Chen et al.（2020）
Fig. 7. δ238U offset between dissolved and adsorbed uranium. Different adsorbents show basically close offset between -0.17‰ and -0.23‰
图 8 溶解态的铀被吸附到铁锰氧化物表面的吸附机理(修改自Dang et al., 2016).碳酸铀酰在吸附前后U-O键键长发生了改变(Dang et al., 2016)
Fig. 8. Postulated models of U adsorption on Fe and Mn oxides(modified from Dang et al., 2016). Ball-and-stick representation of the dissolved uranyl carbonate complex. Note that the length of U-O band changes after adsorption(Dang et al., 2016)
图 9 不同时代碳酸盐岩(灰色符号)、古土壤(紫色符号)、富铁沉积物(橙色符号)和页岩(蓝色符号)铀同位素组成
数据来源：Weyer et al.（2008）；Montoya-Pino et al.（2010）；Brennecka et al.（2011a）；Asael et al.（2013）；Kendall et al.(2013, 2015)；Andersen et al.（2014）；Dahl et al.（2014）；Goto et al.（2014）；Holmden et al.（2015）；Noordmann et al.（2015）；Elrick et al.（2017）；Hinojosa et al.（2016）；Lau et al.(2016, 2017)；Wang et al.(2016, 2018)；Rolison et al.（2017）
Fig. 9. Variation of uranium isotope compositions for shales (blue circles), carbonate (gray circles), iron-rich (orange circles) and paleosol (purple circles) through time
图 10 现今海洋富氧(a)和地质历史时期缺氧(b)状态下海水的铀同位素质量平衡(修改自Brennecka et al., 2011a)
Fig. 10. Schematic illustration of the isotopic U mass balance of the modern oxygenated ocean (a) and anoxic ocean in ancient times (b) (modified from Brennecka et al., 2011a)
图 11 两种不同类型的铀矿: 低温砂岩型铀矿和高温岩浆型铀矿的235U含量(a)(Cowan and Adler, 1976; Bopp et al., 2009)和铀同位素238U/235U组成(b)(修改自Bopp et al., 2009；Brennecka et al., 2010).这些数据表明，高温型铀矿较为富集235U，而低温型铀矿铀238U含量相对较高
Fig. 11. Histogram of 235U contents for sandstone U ores and magmatic U ores (a) studied by Cowan and Adler (1976) and Bopp et al.(2009); uranium isotope compositions for low-temperature and high-temperature deposits (b) (modified from Bopp et al., 2009; Brennecka et al., 2010). Colored bars are the 2 standard error confidence intervals for each style of U ores
表 1 利用U-TEVA树脂分离铀步骤
Table 1. Separation protocol of U on U/TEVA
步骤 加酸介质 体积 目的 清洗柱 0.05 M HCl 20 mL 清洗柱 平衡柱 3 M HNO3 6 mL 上样 3 M HNO3 10 mL 淋洗 3 M HNO3 40 mL 仅保留Th、U和Np 盐酸介质 11 M HCl 6 mL 接Th，Np 5 M HCl+0.1 M oxalic 20 mL 洗掉Th、Np 去草酸 5 M HCl 10 mL 接U 0.05 M HCl 25 mL 回收U 注：引自 Weyer et al.(2008) ；Tissot and Dauphas(2015).
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