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1.
In this study, the Cd isotopic composition of various geological reference materials and anthropogenic samples was investigated. The measurements were made by multicollector ICP-MS and instrumental mass fractionation was controlled using a "sample-standard bracketing" technique. Cadmium isotopic data are reported relative to an internal Cd solution (Cd Spex) and expressed as the 114 Cd/110Cd delta value. Two other Cd solutions (Prolabo and JMC) were analysed and yielded the same 0% delta value. A fractionated Cd metal sample (Münster Cd) was used as a secondary reference material for Cd isotopic measurements and we obtained a 114 Cd/110 Cd delta value of 4.48% relative to Cd Spex solution. As opposed to multi-stage Cd purification previously published in the literature, a new one step anionic exchange purification using dilute HCl for the analysis of Cd isotopes in geological samples was developed. This method enabled a high recovery (> 95%) and effective separation of the sample matrix to be achieved. The long-term external reproducibility was evaluated at 0.12% (2 standard deviations) for the 114 Cd/110Cd ratio, based on reference solutions and replicated measurements of samples over one year. The variation of Cd isotopic composition of natural terrestrial samples is restricted to a small range of 0.4%, which is similar to previously reported results. In contrast, large variations of Cd isotopic composition were found for anthropogenic samples with values as low as −0.64% for a dust sample issued from a lead smelter and values as high as +0.50% for NIST SRM 2711 (metal-rich soil). These variations are 10 times larger than the reproducibility and suggest that Cd isotopes can be useful as tracers of anthropogenic sources of Cd in the environment.  相似文献   

2.
高温下非传统稳定同位素分馏   总被引：5，自引：1，他引：4  
黄方 《岩石学报》2011,27(2):365-382
过去十几年来,非传统稳定同位素地球化学在高温地质过程的研究中取得了的重大进展。多接收诱导耦合等离子质谱(MC-ICP-MS)的应用引发了稳定同位素分析方法的重大突破,使得精确测定重元素的同位素比值成为可能。本文总结了以Li、Fe和Mg同位素为代表的非传统稳定同位素在岩石地球化学研究中的应用。Li同位素目前被广泛地用于地幔地球化学、俯冲带物质再循环和变质作用的研究中,可以用来示踪岩浆的源区性质和扩散等动力学过程。不同价态的Fe在矿物熔体相之间的分配可以产生Fe同位素分馏,可以发生在地幔交代、部分熔融、分离结晶等过程中。岩浆岩的Mg同位素则大致反映其源区的特征,地幔的Mg同位素组成比较均一,这为研究低温地球化学过程中Mg同位素的分馏提供一个均一的背景。此外,Cl,Si,Cu,Ca,U等等同位素体系也具有广阔的应用前景。对同位素分馏机制的实验研究和理论模拟为理解非传统稳定同位素数据提供了必要的指导。实验表明,高温下具有不同的迁移速度的轻、重同位素可以产生显著的动力学同位素分馏,这一分馏可以在化学扩散、蒸发和凝华等过程中发生;同位素在矿物和熔体以及流体相中化学环境的差异使得不同相之间可以发生平衡分馏。而最近的硅酸盐岩浆的热扩散和热迁移实验则揭示了一种"新"的岩浆分异和同位素分馏机制。沿着温度梯度,硅酸盐岩浆可以发生显著的元素和同位素分异,湿的安山岩可以通过这种方式演变成花岗质成分,因此这个过程可能对陆壳的产生和演化有重大影响。如果温度梯度在岩浆作用中能长期存在,热扩散就可以产生稳定同位素的分馏,这一机制有别于传统的平衡和动力学同位素分馏。 而多个稳定同位素体系的正相关关系是示踪热迁移过程的最有力证据。在热扩散过程中,流体承载的物质的浓度和它的索瑞系数有关。但是这个系数对体系的很多参数非常敏感,变化极大,因此对热扩散效应的研究产生极大的困难。对热扩散实验的镁、钙和铁同位素测量表明,同位素比值的变化与体系的化学组成以及总温度无关,只和温度变化的幅度有关,这意味着即使元素的索瑞系数变化多端,某一元素的同位素之间的索瑞系数的差别总为常数。这一发现有助于简化对热扩散和索瑞系数这一基础物理问题的研究 。  相似文献   

3.
Subduction zones involve many complex geological processes, including the release of slab-derived fluids, fluid/rock interactions, partial melting, isotopic fractionations, elemental transporting, and crust/mantle interactions. Lithium (Li) isotopes (6Li and 7Li) have relative mass difference up to 16%, being the largest among metal elements. Thus, Li isotopes have advantage to interprete trace various geological processes. Most importantly, during crust/mantle interactions in deep subduction zones, surface materials and mantle rocks usually have distinct Li isotopic compositions. Li isotopes can be potential tracer for subduction processes, from the onset of subduction to the release of Li from subducted slabs and interaction with mantle wedge, as well as the fate of Li in slab-derived fluids and residual slabs. Moreover, the Li isotopic composition of subducting output materials can provide useful information for understanding global Li circulation. With developments in measurement and expansion of Li isotopic database, Li isotopic geochemistry will provide more inference and be a powerful tracer for understanding subduction-related processes. This work retrospected the application of Li isotopes in tracing successive subduction processes, and made some prospects for further studies of Li isotopes.  相似文献   

4.
The CRPG (Nancy, France) has prepared secondary reference materials for Li isotope measurements by mixing 7Li or 6Li spikes and either L-SVEC or IRMM-016 certified reference materials to produce solutions having a known Li concentration and isotopic composition. The Li7-N and Li6-N solution samples (1.5 mol l−1 HNO3) have nominal δ7Li isotopic compositions of 30.1‰ and -9.7‰ respectively relative to L-SVEC and concentrations of 100 mg l−1. Repeated measurement of these samples using the QUAD-ICP-MS at the CRPG yielded δ7Li of 30.4 ± 1.1‰ (n = 13) and -8.9 ± 0.9‰ (n = 9) at the 2s level of confidence. An additional LiCl-N solution was measured and yielded a delta value of 9.5 ± 0.6‰ (n = 3). Identical results were obtained at the BRGM (Orléans, France) from determinations performed with a Neptune MC-ICP-MS (30.2 ± 0.3‰, n = 89 for the Li7-N, -8.0 ± 0.3‰, n = 38 for the Li6-N and 10.1 ± 0.2‰, n = 46 for LiCl-N at the 2s level of confidence). The deviation of measured composition relative to the nominal value for the Li6-N solution might be explained by either contamination during preparation or an error during sample weighing. These secondary reference materials, previously passed through ion exchange resin or directly analysed, may be used for checking the accuracy of Li isotopic measurements over a range of almost 40‰ and will be available to the scientific community upon request to J. Carignan or N. Vigier, CRPG.  相似文献   

5.
We have measured with an electron microprobe the Mg, Al, Si, Ca, Ti, Mn, and Fe contents of five strongly heated stony cosmic spherules (sCS) from the South Pole water well. We have also measured the isotopic compositions of Si, and when possible of Mg and of Fe in these objects by ion microprobe. Except for iron, the measured elemental compositions are chondritic within a factor of 2. In four samples, the ratio of 57Fe/56Fe exceeds the terrestrial value by 3.5‰ to 48‰. Mass-dependent fractionation of the isotopes of Si ranges from ∼2 to ∼8 ‰/AMU in three samples. Mg is clearly fractionated in only one sample, for which δ25Mg = ∼8 ‰. The extent of mass-dependent fractionation of the isotopes and, by implication, of evaporative loss generally follows a trend Mg < Si < Fe. The trend is similar to that found in laboratory heating experiments of charges with solar composition. Although the observed isotopic inhomogeneities within some samples call into question the strict validity of the Rayleigh equation for the sCS, its approximate application to our new and to previously published results for Mg suggests that evaporative losses of greater than 40 wt.% occur rarely from sCS, and that the precursor grains of the sCS had a CM-carbonaceous-chondrite-like complement of Mg, Si, Ca, and Al. Low Fe contents relative to CM abundances could reflect an unusual precursor composition, or, more probably, losses by processes that did not fractionate isotopes, i.e., ejection of immiscible FeS and FeNi beads from the melt or rapid, complete separation and decomposition of FeS at the surface.  相似文献   

6.
矿床的形成受制于多种复杂的地质作用,包括全球尺度的板块构造运动、岩浆活动、变质沉积改造等过程,并普遍伴随热液活动、流体迁移、水-岩相互作用、元素分异及同位素分馏等一系列局部区域地质和地球化学过程.在过去的矿床学研究中,地球化学方法主要围绕在主、微量元素和传统的稳定同位素等手段,解决了很多矿床成因问题.但仍存在不少的多解和难解问题,比如许多矿床在矿化类型、蚀变分带与金属矿物组合方面具有诸多相似之处,常规地球化学指标难以区分.随着测试精度的提高和自然储库组成的完善,Li同位素近些年来已成为新兴的稳定同位素体系.Li同位素在自然界过程中高达80‰的同位素分馏使其具有更好的辨识能力,同时兼有直接和间接指示作用,有潜力成为研究各种复杂成矿过程的良好示踪剂.本文总结了近年来有关矿床学中Li同位素的研究和应用进展,以俯冲带成矿为主,阐述了斑岩型-热液矿床、伟晶岩型矿床和沉积矿床等类型矿床的Li同位素地球化学特征,并探究新的Li同位素方法在矿床中的应用前景.基于Li同位素体系在各类矿床的应用实例,我们认为Li同位素体系将为矿床学研究提供更多的指示信息和依据.   相似文献   

7.
李东永  肖益林  王洋洋  沈骥  刘海洋 《地球科学》2019,44(12):4081-4085
金属稳定同位素体系是示踪板块俯冲对壳幔物质再循环影响的全新工具,因此其在俯冲带的地球化学行为备受关注.Mg同位素在俯冲过程中不发生显著分馏,但大陆玄武岩具有低于洋中脊玄武岩的Mg同位素,这可能是碳酸岩的俯冲再循环导致的.与角闪岩继承原岩的Li同位素组成不同,榴辉岩具有轻于原岩的Li同位素组成,可归因于俯冲折返过程中的动力学扩散、脱水反应或低Li同位素的流体交代.作为变价元素,Fe和Cr的同位素在榴辉岩的形成过程中均不发生显著分馏,但是蛇纹岩的Fe同位素和Cr同位素与氧逸度指标具有相关性,指示氧化还原条件变化时脱水过程或流体交代会导致同位素分馏.   相似文献   

8.
近年来,非传统稳定同位素地球化学得到了飞跃性的发展,其主要研究对象为海洋体系的演化。特别是氧化还原敏感元素(Se,Mo,Fe等)稳定同位素已经在古海洋环境的示踪研究中发挥重要的作用。相比分散元素(Ge,Cd,Tl)稳定同位素研究比较薄弱,但这些元素在海洋体系中有特殊的循环模式,这使得它们的同位素研究将可能存在很大地质潜力。海洋体系中它们的源汇简单,而且有机无机吸附过程都可能导致同位素分馏。Ge,Cd,Tl均属于挥发性元素,原始星云的形成过程可能存在较大的同位素分馏。我国南方大面积的低温成矿域,将为Ge,Cd,Tl稳定同位素的发展提供天然的平台。另外,Cd,Tl是环境污染的主要潜在元素,因此采用稳定同位素示踪还可能示踪表生环境中的污染来源。  相似文献   

9.
Chondritic Mg isotope composition of the Earth   总被引：2，自引：0，他引：2  
The processes of planetary accretion and differentiation have potentially been recorded as variations in the stable isotope ratios of the major elements between planetary objects. However, the magnitude of observed isotopic variations for several elements (Mg, Fe, Si) is at the limit of what current analytical precision and accuracy are able to resolve. Here, we present a comprehensive data set of Mg isotope ratios measured in ocean island and mid-ocean ridge basalts, peridotites and chondrites. The precision and accuracy were verified by isotopic standard addition for two samples, one carbonaceous chondrite (Murchison) and one continental flood basalt (BCR-1). In contrast with some previous studies, our data from terrestrial and chondritic materials have invariant Mg isotope ratios within the uncertainty of the method (0.1‰ for the 26Mg/24Mg ratio, 2SD). Although isotopic variations of less than about 0.1‰ could still be present, the data demonstrate that, at this level of uncertainty, the bulk silicate Earth and chondritic Mg reservoir have a homogeneous δ26Mg = −0.23‰ (26Mg/24Mg ratio of the sample relative to the DSM3 standard set to zero by definition). This implies that neither planetary accretion processes nor partial mantle melting and subsequent shallow-level differentiation have fractionated Mg isotope ratios. These observations imply in particular that the formation of the Earth cannot stem from preferential sorting of chondrite constituents that would have been fractionated in their Mg isotope composition. It also implies that unlike oxygen isotopes, there was no zonation in Mg isotopes in the inner solar system.  相似文献   

10.
Over 1400 electron probe and 700 ion probe microanalyses were performed on eleven mineral separates to evaluate their potential as reference materials for in situ Li isotopic determination. Our results suggest the homogenous distributions of major elements, Li and its isotopes for each sample. Hence, these samples are suitable to be used as reference materials for in situ measurements of Li abundance and Li isotopes by secondary ion mass spectrometry (SIMS) or laser ablation‐inductively coupled plasma‐mass spectrometry (LA‐ICP‐MS). These samples have the advantage of mitigating probable matrix effects during calibration owing to the wide range of compositions. The effect of composition on the δ7Li of olivine measured by SIMS is a linear function of composition, with δ7Li increasing by 1.0‰ for each mole per cent decrease in forsterite component.  相似文献   

11.
近年来,由于分析手段的不断改进,锂同位素的精确测试才得以实现。锂以其分馏大、中度不相容、易随流体迁移、地表环境与地幔锂同位素特征差异明显等优势,被认为是极具潜力的示踪元素。目前,锂同位素在壳幔物质循环、风化作用、岩浆作用、流体(热液)活动等方面研究中已得到广泛的应用,其中又以俯冲带锂同位素的研究程度最高。本文主要从锂同位素分馏机理、俯冲带锂的行为特征、岛弧岩浆的锂同位素研究以及深俯冲作用过程中锂的行为等方面总结了当前国内外锂同位素的研究进展。  相似文献   

12.
斜顽辉石、镁铝榴石和镁铝尖晶石作为辉石族、石榴石族以及尖晶石族中的重要端元,是地球上地幔主要组成矿物。Li同位素是重要的地幔地球化学示踪剂,其在橄榄石、辉石和石榴石等地幔矿物中的扩散分馏的性质对理解Li同位素作为地幔地球化学示踪剂非常重要。我们通过经典力场经验势方法,从原子尺度上计算研究了不同温压条件下Li同位素在斜顽辉石、镁铝榴石和镁铝尖晶石晶格中分别通过不同的填隙机制和取代空位机制迁移的活化能和其在不同晶格位上的分馏效应。我们发现Li同位素是通过取代空位机制在斜顽辉石、镁铝榴石和镁铝尖晶石中进行迁移扩散。Li同位素在不同晶格位上的分馏作用计算表明,在三种矿物中重同位素7Li会更多地进入晶格填隙位中,而6Li则相对更多进入Mg位。温度是影响这种分馏作用的一个关键因素,相应的结果可用来解释地幔Li同位素组成特征及冷却条件下的同位素分馏等科学问题。  相似文献   

13.
This paper contains the results of an extensive isotopic study of United States Geological Survey GSD‐1G and MPI‐DING reference glasses. Thirteen different laboratories were involved using high‐precision bulk (TIMS, MC‐ICP‐MS) and microanalytical (LA‐MC‐ICP‐MS, LA‐ICP‐MS) techniques. Detailed studies were performed to demonstrate the large‐scale and small‐scale homogeneity of the reference glasses. Together with previously published isotopic data from ten other laboratories, preliminary reference and information values as well as their uncertainties at the 95% confidence level were determined for H, O, Li, B, Si, Ca, Sr, Nd, Hf, Pb, Th and U isotopes using the recommendations of the International Association of Geoanalysts for certification of reference materials. Our results indicate that GSD‐1G and the MPI‐DING glasses are suitable reference materials for microanalytical and bulk analytical purposes.  相似文献   

14.
Silicon isotope analysis traditionally uses a standard-sample bracketing (SSB) method that relies upon greater instrument stability than can be consistently expected. The following proposed method reduces the level of instrumental stability required for the analysis process and provides a valid solution for high-precision and accurate studies of Si isotopic compositions. Rock samples were dissolved by using alkali fusion and acidification. Silicon isotopes were purified with an ion exchange resin. Interfering peaks for isotopes were separated by using a Nu Plasma 1700 multi-collector inductively coupled plasma mass spectrometry (MS) system in high-resolution mode (M/ΔM > 8000 RP). Two magnesium isotopes (25Mg and 26Mg) and three silicon isotopes (28Si, 29Si, and 30Si) were analyzed in the same data collection cycle. Mg isotopes were used as an internal standard to calibrate the mass discrimination effects in MS analysis of Si isotopes in combination with the SSB method in order to reduce the effects of MS interference and instrumental mass discrimination on the accuracy of measurements. The conventional SSB method without the Mg internal standard and the proposed SSB method with Mg calibration delivered consistent results within two standard deviations. When Mg was used as an internal standard for calibration, the analysis precision was better than 0.05 ‰ amu.  相似文献   

15.
锂同位素分馏机制讨论   总被引：7，自引：0，他引：7  
作为一种新兴的稳定同位素示踪工具, 锂同位素地球化学的研究近年来受到了国际地学界日益广泛的关注.其应用领域涵盖了从地表到地幔的流体与矿物之间的相互作用.在地表风化作用过程中, 轻锂同位素(6Li) 优先进入固体相, 而7Li则进入流体相, 因而地表风化作用淋滤出了岩石中的重锂, 致使河水具有重的锂同位素组成, 河水又将重锂同位素组分补给海洋, 洋壳的低温蚀变作用使得海水的锂同位素组成进一步变重.在俯冲带, 由于俯冲板片释放的流体具有重锂同位素组成的特征, 它们上升并交代上覆的地幔楔和相邻的地幔, 使得地幔楔的锂同位素组成变重.同时, 深俯冲的板片由于脱水而具有较轻的锂同位素组成, 它们在地幔中可能形成一个局部轻锂的地幔储源.影响地幔橄榄岩锂同位素分馏的因素主要有3个方面: 温度、扩散机制以及外来熔体的反应.由于高温下地幔矿物之间的锂同位素分馏很小, 而单纯的扩散分馏机制不能够很好的解释我国华北汉诺坝地区地幔橄榄岩中矿物之间的锂同位素分馏.因此, 具有轻锂同位素组成的熔体与橄榄岩之间的反应是上述现象的一个合理解释.需要指出的是, 在橄榄岩-熔体反应的过程中, 锂同位素的扩散作用也对地幔矿物之间的同位素分馏有一定的贡献.   相似文献   

16.
Experiments specifically designed to measure the ratio of the diffusivities of ions dissolved in water were used to determine . The measured ratio of the diffusion coefficients for Li and K in water (DLi/DK = 0.6) is in good agreement with published data, providing evidence that the experimental design being used resolves the relative mobility of ions with adequate precision to also be used for determining the fractionation of isotopes by diffusion in water. In the case of Li, we found measurable isotopic fractionation associated with the diffusion of dissolved LiCl (D7Li/D6Li=0.99772±0.00026). This difference in the diffusion coefficient of 7Li compared to 6Li is significantly less than that reported in an earlier study, a difference we attribute to the fact that in the earlier study Li diffused through a membrane separating the water reservoirs. Our experiments involving Mg diffusing in water found no measurable isotopic fractionation (D25Mg/D24Mg=1.00003±0.00006). Cl isotopes were fractionated during diffusion in water (D37Cl/D35Cl=0.99857±0.00080) whether or not the co-diffuser (Li or Mg) was isotopically fractionated. The isotopic fractionation associated with the diffusion of ions in water is much smaller than values we found previously for the isotopic fractionation of Li and Ca isotopes by diffusion in molten silicate liquids. A major distinction between water and silicate liquids is that water surrounds dissolved ions with hydration shells, which very likely play an important but still poorly understood role in limiting the isotopic fractionation associated with diffusion.  相似文献   

17.
非传统同位素体系(如Hf、Os、Li、Fe、Ti、Mg、He、Ar等)是相对于传统同位素体系(如Sr、Nd、Pb、O等)而言的,即新近发展起来的同位素体系。随着同位素测试技术的进步和多接收电感耦合等离子体质谱仪(MC-ICP-MS)、二次离子质谱仪(SIMS)以及激光剥蚀技术配合MC-ICP-MS(LA-MC-ICP-MS)等测试手段的开发应用,多种同位素体系(包括放射性同位素和稳定同位素体系)的示踪作用在地学研究中得到了日益广泛的应用。在简要介绍传统同位素体系的基础上,旨在总结报道近年来国际上有关非传统同位素体系在地幔地球化学研究中取得的重要成果,展示这些同位素体系在地幔地球化学研究中的重要性及其可能的应用前景,以加速我国在非传统同位素地球化学方面的应用研究。  相似文献   

18.
The terrestrial biogenic Si (BSi) pool in the soil-plant system is ubiquitous and substantial, likely impacting the land-ocean transfer of dissolved Si (DSi). Here, we consider the mechanisms controlling DSi in forest soil in a temperate granitic ecosystem that would differ from previous works mostly focused on tropical environments. This study aims at tracing the source of DSi in forest floor leachates and in soil solutions under various tree species at homogeneous soil and climate conditions, using stable Si isotopes and Ge/Si ratios. Relative to granitic bedrock, clays minerals were enriched in 28Si and had high Ge/Si ratios, while BSi from phytoliths was also enriched in 28Si, but had a low Ge/Si ratio. Such a contrast is useful to infer the relative contribution of silicate weathering and BSi dissolution in the shallow soil on the release of DSi in forest floor leachate solutions. The δ30Si values in forest floor leachates (−1.38‰ to −2.05‰) are the lightest ever found in natural waters, and Ge/Si ratios are higher in forest floor leachates relative to soil solution. These results suggest dissolution of 28Si and Ge-enriched secondary clay minerals incorporated by bioturbation in organic-rich horizons in combination with an isotopic fractionation releasing preferentially light Si isotopes during this dissolution process. Ge/Si ratios in soil solutions are governed by incongruent weathering of primary minerals and neoformation of secondary clays minerals. Tree species influence Si-isotopic compositions and Ge/Si ratios in forest floor leachates through differing incorporation of minerals in organic horizons by bioturbation and, to a lesser extent, through differing Si recycling.  相似文献   

19.
We present the first measurements of vanadium (V) stable isotopes for six reference materials – USGS PCC‐1, BHVO‐2, BCR‐2, BIR‐1a, GSP‐2 and AGV‐2 – plus the widely available carbonaceous chondrite Allende. We present standard addition and matrix spiking tests to assess the robustness and reproducibility of our data. Standard addition utilised an enriched 50V solution designated VISSOX (Vanadium Isotope Standard Solution OXford). We further assessed the veracity of the method by spiking collected sample matrices with the same amount of a V standard solution, whose isotopic composition was defined as 0‰. Standard addition and matrix spiking tests recorded no appreciable artificial isotope fractionation. We estimate that the best currently attainable long‐term reproducibility of stable 51V/50V isotope measurements in complex matrices is 0.15‰, which is in the same order as the reproducibility achievable with standard solutions. Finally, a large range of ～ 1.2‰ in stable V isotopic composition was documented, with ～ 0.5‰ of that variation in high temperature igneous materials alone. The range and resolving power of V stable isotopes, with respect to igneous material, compared favourably with the magnitude of fractionation reported for other non‐traditional stable isotope systems, which bodes well for the utility of this new system.  相似文献   

20.
This study presents lithium (Li) and magnesium (Mg) isotope data from experiments designed to assess the effects of dissolution of primary phases and the formation of secondary minerals during the weathering of basalt. Basalt glass and olivine dissolution experiments were performed in mixed through-flow reactors under controlled equilibrium conditions, at low pH (2-4) in order to keep solutions undersaturated (i.e. far-from equilibrium) and inhibit the formation of secondary minerals. Combined dissolution-precipitation experiments were performed at high pH (10 and 11) increasing the saturation state of the solutions (moving the system closer to equilibrium) and thereby promoting the formation of secondary minerals.At conditions far from equilibrium saturation state modelling and solution stoichiometry suggest that little secondary mineral formation has occurred. This is supported by the similarity of the dissolution rates of basalt glass and olivine obtained here compared to those of previous experiments. The δ7Li isotope composition of the experimental solution is indistinguishable from that of the initial basalt glass or olivine indicating that little fractionation has occurred. In contrast, the same experimental solutions have light Mg isotope compositions relative to the primary phases, and the solution becomes progressively lighter with time. In the absence of any evidence for secondary mineral formation the most likely explanation for these light Mg isotope compositions is that there has been preferential loss of light Mg during primary phase dissolution.For the experiments undertaken at close to equilibrium conditions the results of saturation state modelling and changes in solution chemistry suggest that secondary mineral formation has occurred. X-ray diffraction (XRD) measurements of the reacted mineral products from these experiments confirm that the principal secondary phase that has formed is chrysotile. Lithium isotope ratios of the experimental fluid become increasingly heavy with time, consistent with previous experimental work and natural data indicating that 6Li is preferentially incorporated into secondary minerals, leaving the solution enriched in 7Li. The behaviour of Mg isotopes is different from that anticipated or observed in natural systems. Similar to the far from equilibrium experiments initially light Mg is lost during olivine dissolution, but with time the δ26Mg value of the solution becomes increasingly heavy. This suggests either preferential loss of light, and then heavy Mg from olivine, or that the secondary phase preferentially incorporates light Mg from solution. Assuming that the secondary phase is chrysotile, a Mg-silicate, the sense of Mg fractionation is opposite to that previously associated with silicate soils and implies that the fractionation of Mg isotopes during silicate precipitation may be mineral specific. If secondary silicates do preferentially remove light Mg from solution then this could be a possible mechanism for the relatively heavy δ26Mg value of seawater. This study highlights the utility of experimental studies to quantify the effects of natural weathering reactions on the Li and Mg geochemical cycles.  相似文献   

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