Microscale δ34S and δ18O variations of barite as an archive for fluid mixing and microbial sulphur metabolisms in igneous rock aquifers.

IF 1.1 4区 环境科学与生态学 Q4 CHEMISTRY, INORGANIC & NUCLEAR Isotopes in Environmental and Health Studies Pub Date : 2024-12-01 Epub Date: 2024-10-04 DOI:10.1080/10256016.2024.2410293
Vanessa Fichtner, Ferdinand Kirchner, Martin Kutzschbach, Harald Strauss, Mikael Tillberg, Martin Whitehouse, Henrik Drake
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Abstract

The stable isotope compositions of sulphur (δ34S) and oxygen (δ18O) in barite are frequently used as proxies for microbial sulphate reduction (MSR) in diverse environments, such as in relation to anaerobic oxidation of methane in marine cold seeps. There, isotopically heavy barite is used as a marker for MSR from a sulphate pool that has undergone semi-closed system conditions. Closed-system MSR is also a commonly observed feature in igneous rock hosted fracture aquifers, as shown by extremely 34S-enriched pyrite. What is less well-constrained is whether δ34S in barite can be used as a proxy for MSR in such systems. Here we explore the microscale heterogeneity of δ34S and δ18O via secondary ion mass spectrometry and the trace element Sr via LA-ICP-MS maps in barite precipitated in granite-hosted boreholes during a 17-year experiment, at Äspö, Sweden. We compare it with δ18Osulfate, δ34Ssulfate, and δ34Ssulfide of the fracture fluids and with paragenetic pyrite with δ34S values reflecting closed system MSR. The δ18O values in barite (+9.4 to +16.9 ‰) represent two generations of barite, one with low values and one with high values. The latter are likely impacted by sulphur disproportionating or -oxidizing bacteria. The barite reflects a much smaller span in δ34S (+14.5 to +28.6 ‰) than the pyrite (-47.2 to +53.3 ‰). This lack of extremely high δ34Sbarite values is proposed to be due to that barite saturation only occurred in the early parts of the Rayleigh cycle. Additionally, fluid migration has affected the δ34S values to lower values, accompanied by higher Sr concentrations. Taken together, barite δ34S values cannot be regarded as a reliable independent proxy for MSR in deep sulphate-poor igneous rock hosted aquifers. However, the relation between the δ34S values of coeval barite and pyrite is regarded as a useful proxy for MSR-related fractionation during early stages of MSR.

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重晶石的微尺度δ34S和δ18O变化作为火成岩含水层中流体混合和微生物硫代谢的档案。
重晶石中硫(δ34S)和氧(δ18O)的稳定同位素组成经常被用作不同环境中微生物硫酸盐还原(MSR)的替代物,例如与海洋冷渗漏中甲烷的厌氧氧化有关的替代物。在那里,同位素重晶石被用作经过半封闭系统条件的硫酸盐池中微生物硫酸盐还原的标记。封闭系统 MSR 也是在火成岩承压含水层中经常观察到的一个特征,34S 富集程度极高的黄铁矿就表明了这一点。重晶石中的δ34S是否可以作为此类系统中MSR的替代物,目前还不太清楚。在此,我们通过二次离子质谱法探究了重晶石中δ34S 和 δ18O的微观异质性,并通过LA-ICP-MS图谱探究了在瑞典Äspö进行的一项为期17年的实验中花岗岩寄生钻孔中沉淀的重晶石中痕量元素Sr的微观异质性。我们将其与裂缝流体中的δ18硫酸盐、δ34硫酸盐和δ34硫化物以及反映封闭系统 MSR 的δ34S 值的准成岩黄铁矿进行了比较。重晶石中的δ18O值(+9.4 至 +16.9‰)代表了两代重晶石,一代数值较低,一代数值较高。后者很可能受到硫歧化或氧化细菌的影响。与黄铁矿(-47.2 至 +53.3‰)相比,重晶石反映的 δ34S 跨度(+14.5 至 +28.6‰)要小得多。之所以没有极高的δ34S重晶石值,是因为重晶石饱和只发生在瑞利周期的早期。此外,流体迁移使δ34S值降低,同时锶浓度升高。综上所述,重晶石δ34S 值不能被视为贫硫酸盐火成岩深层含水层 MSR 的可靠独立替代值。然而,共生重晶石和黄铁矿的δ34S值之间的关系被认为是MSR早期阶段与MSR相关的分馏的有用替代值。
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来源期刊
CiteScore
2.80
自引率
7.70%
发文量
21
审稿时长
3.0 months
期刊介绍: Isotopes in Environmental and Health Studies provides a unique platform for stable isotope studies in geological and life sciences, with emphasis on ecology. The international journal publishes original research papers, review articles, short communications, and book reviews relating to the following topics: -variations in natural isotope abundance (isotope ecology, isotope biochemistry, isotope hydrology, isotope geology) -stable isotope tracer techniques to follow the fate of certain substances in soil, water, plants, animals and in the human body -isotope effects and tracer theory linked with mathematical modelling -isotope measurement methods and equipment with respect to environmental and health research -diagnostic stable isotope application in medicine and in health studies -environmental sources of ionizing radiation and its effects on all living matter
期刊最新文献
In memoriam: Dr. Keith Alan Hobson, a pioneer of stable isotope ecology. Stable-isotope variability in daily precipitation: insights from a low-cost collector in SE England. Copper and its isotopes: a brief overview of its implications in geology, environmental system, and human health. Estimation of radiological health risks due to 226Ra, 232Th, and 40K in foods consumed in Iraqi Kurdistan Region. Microscale δ34S and δ18O variations of barite as an archive for fluid mixing and microbial sulphur metabolisms in igneous rock aquifers.
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