三氟乙酸锂-15-冠醚-5体系电迁移法分离锂同位素

锂同位素(6 Li和7 Li)在核工业中有着重要作用.锂汞齐法是目前唯一实现锂同位素工业化生产的方法,然而由于汞的使用,该方法具有较大的环境风险.开发绿色高效的锂同位素分离方法对国家能源安全具有重要意义.在本论文中,制备了溶解锂盐的冠醚溶液,并以其作为阳极液,施加电场驱动锂离子向阴极液迁移;与溶有15-冠醚-5的锂盐水...     

Nb–Ta fractionation induced by fluid‐rock interaction in subduction‐zones: constraints from UHP eclogite‐ and vein‐hosted rutile from the Dabie orogen,Central‐Eastern China

Niobium and Ta concentrations in ultrahigh‐pressure (UHP) eclogites and rutile from these eclogites and associated high pressure (HP) veins were used to study the behaviour of Nb–Ta during dehydration and fluid‐rock interaction. Samples were collected through a ～2 km profile at the Bixiling complex in the Dabie orogenic belt, Central‐Eastern China. All but one eclogite away from veins (EAVs) display nearly constant Nb/Ta ratios ranging from 16.1 to 19.2, with an average of 16.9 ± 0.8 (2 SE), similar to that of their gabbroic protolith from the Yangtze Block. Nb/Ta ratios of rutile from the EAVs range from 12.7 to 25.3 among different individual grains, with the average values close to those of the corresponding bulk rocks. These observations show that Nb and Ta were not significantly fractionated by prograde metamorphism up to eclogite facies when no significant fluid‐rock interaction occurs. In contrast, Nb/Ta ratios of rutile from eclogites close to veins (ECVs) are highly variable from 17.8 to 49.8, which are systematically higher (by up to 17) than those of rutile from the veins. These observations demonstrate that Nb and Ta were mobilized and fractionated during localized fluid flow and intensive fluid‐rock interaction. This is strongly supported by Nb/Ta zoning patterns in single rutile grains revealed by in situ LA‐ICP‐MS analysis. Ratios of Nb/Ta in the ECV‐hosted rutile decrease gradually from cores towards rims, whereas those in the EAV‐hosted rutile are nearly invariable. Furthermore, the vein rutile shows Nb/Ta zoning patterns that are complementary to those in rutile from their immediate hosts (ECVs), suggesting an internal origin for the vein‐forming fluids. The Nb/Ta ratios of such fluids evolved from low values at the early stage of subduction to higher values at later supercritical conditions with increased temperature and pressure. Quantitative modelling was conducted to constrain the compositional evolution of metamorphic fluids during dehydration and fluid‐rock interaction focusing on Nb–Ta distribution. The modelling results based on our proposed multistage fluid phase evolution path can essentially reproduce the natural observations reported in the present study.     

湖泊沉积有机碳同位素与环境变化的研究进展

湖泊沉积有机质稳定碳同位素（δ^13Corg)在区域气候与环境变化方面的应用近年来发展迅速,成果令人瞩目,保存在各类湖泊岩芯中的δ^13Corg记录揭示了晚更新世以来大气CO2浓度的变化、湖泊水位波动、湖区生态与植被的变迁以及气温变化等重要环境信息,由于造成δ^13Corg值变化的影响因素较多,确定个湖与环境变化有关的主导因素时常有赖于其它证据的帮助,诸如地球化学、古湖沼学、孢粉学、分子同位素地层学等等,前人通过研究来自不同类型湖泊、具不同曲线形态特征的δ^13Corg记录,提出了多种环境解释模型,本文对此作了归纳和评述。鉴别和澄清湖泊沉积有机质的源物质以及有机物源随环境变化而发生过的变化,是研究δ^13Corg记录环境意义至关重要的基础性工作,由于有机质含量、碳氮比值、氢指数、生物残留物鉴别等常能提供有关有关湖泊有机质来源、产率、成岩作用等方面的有用信息,这方面的研究结果应该尽可能一并提供,以利于恰当地应用现有的环境解释模型,或者建立个湖新模型,单体生物标志化合物鉴别通常也能为区分湖积有机质中陆生、水生、细菌生等不同碳的来源提供有用信息,特定化合物同位素分析技术近年来成功地应用于建立单体生物标志化合物碳同位素地层学,为湖积有机碳同位素在生态环境演变研究方面的应用提供了思路,我国许多湖泊的湖底沉积岩芯尚未钻取,那些对过去全球变化研究有价值的δ^13Corg记录有待我们去获取和研究。     

Spatio‐temporal variability of the isotopic input signal in a partly forested catchment: Implications for hydrograph separation

The isotopic composition of precipitation (D and ¹⁸O) has been widely used as an input signal in water tracer studies. Whereas much recent effort has been put into developing methodologies to improve our understanding and modelling of hydrological processes (e.g., transit‐time distributions or young water fractions), less attention has been paid to the spatio‐temporal variability of the isotopic composition of precipitation, used as input signal in these studies. Here, we investigated the uncertainty in isotope‐based hydrograph separation due to the spatio‐temporal variability of the isotopic composition of precipitation. The study was carried out in a Mediterranean headwater catchment (0.56 km²). Rainfall and throughfall samples were collected at three locations across this relatively small catchment, and stream water samples were collected at the outlet. Results showed that throughout an event, the spatial variability of the input signal had a higher impact on hydrograph separation results than its temporal variability. However, differences in isotope‐based hydrograph separation determined preevent water due to the spatio‐temporal variability were different between events and ranged between 1 and 14%. Based on catchment‐scale isoscapes, the most representative sampling location could also be identified. This study confirms that even in small headwater catchments, spatio‐temporal variability can be significant. Therefore, it is important to characterize this variability and identify the best sampling strategy to reduce the uncertainty in our understanding of catchment hydrological processes.     

Combined Sr isotope and trace element analysis of melt inclusions at sub-ng levels using micro-milling, TIMS and ICPMS

This paper describes a technique, which allows precise and accurate Sr isotope measurement combined with trace element analysis of individual melt inclusions, of sample sizes  1 ng of Sr. The technique involves sampling by micro-milling, chemical dissolution, micro Sr column chemistry, TIMS, and ICPMS analyses. A 10% aliquot of each sample solution is used for trace element analysis by double focusing magnetic sector field ICPMS, while Sr is chemically separated from the remaining 90% and used for ⁸⁷Sr/⁸⁶Sr determinations by TIMS.During the development of the technique outlined above, we documented in detail the potential sources of blank contributions and their magnitude. The average size and Sr isotope composition of our laboratory total procedural blank during this study was 5.4 pg ± 0.3 pg Sr (n = 21) with an ⁸⁷Sr/⁸⁶Sr of 0.7111 ± 0.0002 (2SE, n = 3). The total procedural Rb blank was 1.9 ± 0.7 pg (n = 21). The total procedural blank was found to have minimal effect (< 150 ppm shift) on the ⁸⁷Sr/⁸⁶Sr of sample material containing down to  250 pg Sr. Applying a blank correction allows ‘in house’ standards of this size to be corrected back to within 175 ppm of their accepted values. By applying blank corrections we can confidently measure the Sr isotope composition on sample sizes down to  25 pg Sr to an accuracy better than 400 ppm.The utility of the technique is illustrated by application to a suite of melt inclusions from NW Iceland and their host olivines. It is shown that the effect of a small amount of entrainment of the host olivine during sampling of 50 μm melt inclusions has a negligible effect on the measured Sr isotope and trace element composition. Furthermore, where melt inclusions are < 50 μm it is possible to obtain Sr isotope and trace element data on multiple melt inclusions hosted in a single olivine. This provides similar information to that of the single melt inclusions.     

Geochronological Study of Caledonian Granulite and High-Pressure Gneiss in the Dabie Mountains

Using the single-zircon evaporation technique and U-Pb method, the authors have conducted an isotope geochonological study of the Huilanshan granulite and Shima garnet-bearing plagioclase gneiss (" country rocks" of the Shima eclogite) in the Dabie Mountains. The study shows that these rocks have peak metamorphic ages of 443-455 Ma, which are essentially consistent with that of the Caledonian high-ultrahigh pressure eclogites. This indicates the existence of the Caledonian collisional orogeny in the Dabie Mountains.     

黑河流域中上游地区降水中氢氧同位素研究

根据黑河流域中上游地区取得的降水水样和气象资料,分析了该区域地区降水线和降水中氘盈余分布特征,为同位素技术在黑河流域水循环研究中的应用提供科学依据.结果表明:受降水再次强烈蒸发同位素动力分馏效应影响,地区大气降水线(LMWL)δD=4.1447δ18O-20.6852(‰)的斜率很低,符合干旱区降水线斜率很低的规律.冬秋两个季节降水线的斜率明显高于春夏季节,氢氧同位素的相关性也远高于春夏季节.降水中氘盈余(d)变化幅度较大,呈现山区高平原低和冬季高夏季低的时空分布规律.     

新疆彩霞山铅锌矿床硫、碳、氢、氧同位素地球化学

文章通过对彩霞山铅锌矿床硫、碳、氢、氧同位素的研究,探讨了矿床成矿流体来源及演化,揭示了成矿作用过程中的某些重要信息.初步认为矿石中的硫主要来自同化了海水硫酸盐的岩浆硫,同时有少量生物还原硫参与;碳、氧同位素组成指示碳来源于壳幔混合.成矿流体以建造水为主,早期有岩浆水参与.     

重庆地区岩溶地下河水溶解无机碳及其稳定同位素特征

稳定碳同位素是指示岩溶动力系统碳来源及转化的重要指标。为揭示重庆地区岩溶地下水中溶解无机碳基本特征和碳来源,本文对该地区63条岩溶地下河水样进行了水化学和碳同位素分析。研究结果表明,重庆地区地下河水溶解无机碳主要表现形式为HCO3-,雨季由于稀释作用其浓度低于旱季。重庆岩溶地下河水δ13C-DIC（V-PDB）旱季变化范围为-15.34 ‰～-5.89 ‰,雨季变化范围为-17.40 ‰～-4.23 ‰。根据δ13C同位素质量平衡方法,计算得到重庆地下河旱季碳酸盐岩溶蚀对DIC贡献为45.1 % ～79.7 %,雨季平均为34.6 %～82.1 % 。计算结果表明,在人类活动不断增强的情况下,岩溶水体DIC通量中碳酸盐岩溶解来源的DIC和其参与岩溶地下水δ13C值的形成并不一定是岩溶作用理论方程中所计算的50 %,而是有一定的变化范围。因此在计算岩溶作用碳汇时,建议通过δ13C值扣除碳酸盐岩溶蚀形成DIC的通量后再来推算岩溶作用形成的碳汇量。     

新疆阿尔泰花岗岩类源区物质的定量模拟

对产出于阿尔泰、额尔齐斯、乌化古三条构造-岩浆带上的六个典型岩体进行了源区岩石化学组成和初始熔体部分熔融程度的定量模拟。模拟结果表明:六个岩体的ε_(Sr)~t值多介于0-120之间,源区岩石多为地幔物质与陆壳物质的混合源,地壳柱中成熟陆壳所占比例较少,反映了中亚型地洼区在地壳化学结构上的一个重要特征.从北往南,ε_(Sr)~t值与壳源锶所占百分率逐渐减小,反映了从地槽造山带核心部位往边缘部位往边缘部位,地壳柱中成熟陆壳所占比例逐渐减小。初始熔浆部分熔融程度温度、压力呈正消长关系。