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Iron Isotopes reveal volcanogenic input during Oceanic Anoxic Event 2 (OAE 2 ∼ 94 Ma) 铁同位素揭示了大洋缺氧事件 2(OAE 2 ∼ 94 Ma)期间的火山生成输入量
IF 4.5 1区 地球科学 Q1 GEOCHEMISTRY & GEOPHYSICS Pub Date : 2025-01-15 DOI: 10.1016/j.gca.2024.10.023
Lucien Nana Yobo , Helen M. Williams , Alan D. Brandon , Chris Holmden , Kimberly V. Lau , Steven C. Bergman , James S. Eldrett , Daniel Minisini
Anomalously high metal concentrations including iron enrichments are recorded in marine carbonates deposited during Ocean Anoxic Event 2 (OAE 2). These metal enrichments have been attributed to massive submarine eruptions during the formation of one or more large igneous provinces, the proposed trigger for OAE 2 (hydrothermal hypothesis), or to the release of metals from the reoxidation of formerly anoxic marine sediment during a period of temporary cooling during OAE 2 (sediment release hypothesis). Here we use iron stable isotopes to help distinguish between the two hypotheses for a trace metal enriched interval during OAE 2 in the Iona-1 core in the Western Interior Seaway, Texas. Our results show a two-step negative excursion during OAE 2 that is coincident with osmium isotope volcanic proxies measured in the same core, with peak negative values centered on a trace metal-enriched interval. After corrections for detrital and locally supplied iron to the study setting, the δ56Fe value of the remotely supplied iron is –0.28 ± 0.05 ‰, falling in the range of iron δ56Fe values observed in modern hydrothermal plumes (–0.1 to –0.5 ‰), thus supporting the hydrothermal hypothesis as the source of iron and other associated trace metals enriched in the study core during OAE 2. By contrast, the sediment release hypothesis predicts much lower δ56Fe values, between –1.0 ‰ to –3.3 ‰ predicted for benthic supplies of iron from anoxic marine sediment overlying re-oxygenated bottom waters. This study shows that combining iron with other proxies for environmental change, particularly submarine volcanism, can distinguish hydrothermally supplied iron from dust, rivers, and shelf sediment supplies of iron despite iron’s reputation for complicated cycling.
在大洋缺氧事件 2(OAE 2)期间沉积的海洋碳酸盐中记录了异常高的金属浓度,包括铁富集。这些金属富集被归因于一个或多个大型火成岩带形成过程中的大规模海底喷发(热液假说),或归因于 OAE 2 期间暂时冷却期间以前缺氧的海洋沉积物重新氧化释放出的金属(沉积物释放假说)。在这里,我们利用铁稳定同位素来帮助区分这两种假说,即德克萨斯州西内海道 Iona-1 岩芯中 OAE 2 期间的痕量金属富集区间。我们的结果显示,在 OAE 2 期间出现了两级负偏移,这与在同一岩芯中测量到的锇同位素火山代用指标相吻合,负值峰值集中在痕量金属富集区间。在对研究环境中的碎屑铁和本地提供的铁进行校正后,远程提供的铁δ56Fe值为-0.28 ± 0.05 ‰,处于现代热液羽流中观察到的铁δ56Fe值范围(-0.1 至 -0.5‰)内,因此支持热液假说,即研究岩心在 OAE 2 期间富集的铁和其他相关痕量金属的来源。相比之下,沉积物释放假说预测的δ56Fe值要低得多,在-1.0‰至-3.3‰之间,预测底栖供应的铁来自缺氧海洋沉积物上覆的复氧底层水。这项研究表明,将铁与环境变化的其他代用指标(尤其是海底火山活动)结合起来,可以将热液提供的铁与尘埃、河流和陆架沉积物提供的铁区分开来,尽管铁的循环很复杂。
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引用次数: 0
Deciphering multiple episodes of partial melting, metasomatic and remelting processes in the Eastern Pyrenean orogenic mantle massif 解读东比利牛斯山造山带地块的多期部分熔融、交代和重熔过程
IF 4.5 1区 地球科学 Q1 GEOCHEMISTRY & GEOPHYSICS Pub Date : 2025-01-15 DOI: 10.1016/j.gca.2024.11.033
Yujian Wang, Jingao Liu
Secular variations in the composition of the subcontinental lithospheric mantle (SCLM) are intimately controlled by multiple geological processes, including diverse melting mechanisms and complex metasomatic processes. We present comprehensive analyses of whole rock and mineral chemistry, along with Re-Os isotopic system of the Eastern Pyrenean orogenic mantle massifs, supported by quantitative modeling through alphaMELTS thermodynamic software. The Eastern Pyrenean lherzolites display consistent negative correlations of TiO2/Al2O3, TiO2 versus MgO and relatively high and unfractionated heavy rare earth elements. These chemical features shed light on the diverse melting mechanisms responsible for these rocks, encompassing passive continuous melting in regions of lithospheric extension and decompression melting linked to the upwelling asthenospheric mantle. Some refractory harzburgites exhibit elevated TiO2/Al2O3, TiO2 contents and moderate light rare earth element enrichment. This suggests chromatographic metasomatism due to the reactive porous flow of evolved melts/fluids in the upper part of the lithosphere during their ascent to the surface. An isochron analogy between 187Os/188Os and Al2O3 yields an age of ∼ 1.5 Ga, constraining the timing of partial melting responsible for the formation of SCLM beneath the Eastern Pyrenean region. We then expand the scope of our study to encompass on– and off-cratonic SCLM on a global scale. This expanded analysis explores the variations in melting mechanisms across different tectonic settings and geological epochs and scrutinizes the role of diverse metasomatic processes in shaping the characteristics of the lithospheric mantle and its longevity on a broad scale. Silicate metasomatism typically produces fertile peridotites at the asthenosphere-lithosphere boundary, making them vulnerable to thermomechanical erosion, whereas cryptic metasomatism, commonly observed in refractory mantle rocks induced by evolved melts at decreasing melt-rock ratios (e.g., hydrocarbon-bearing silicate melt, carbonatite melt etc.), generally forms enrichment of highly incompatible elements but less significant influence on the mineral assemblages and major element geochemistry of the on-cratonic refractory SCLM, making them remain stable for extended periods.
次大陆岩石圈地幔成分的长期变化受到多种地质作用的密切控制,包括多种熔融机制和复杂的交代作用。本文采用alphamelt热力学软件进行定量建模,对东比利牛斯山造山地幔块体的岩石和矿物化学以及Re-Os同位素系统进行了综合分析。东比利牛斯山橄榄岩中TiO2/Al2O3、TiO2与MgO、相对高且未分选的重稀土元素呈负相关。这些化学特征揭示了形成这些岩石的多种熔融机制,包括岩石圈伸展区的被动持续熔融和与软流圈地幔上涌有关的减压熔融。部分难熔硬土表现出TiO2/Al2O3、TiO2含量升高和轻稀土元素富集。这表明在岩石圈上部演化的熔体/流体上升到地表的过程中,由于反应性多孔流动导致了色谱交代作用。187Os/188Os和Al2O3之间的等时线类比得出了~ 1.5 Ga的年龄,限制了东比利牛斯地区下造成SCLM形成的部分熔化的时间。然后我们扩展我们的研究范围,以涵盖全球范围内的克拉通和非克拉通SCLM。这一扩展分析探讨了在不同构造环境和地质时代中熔融机制的变化,并在大范围内审视了不同交代过程在形成岩石圈地幔特征及其寿命方面的作用。硅酸盐交代作用通常在软流圈-岩石圈边界产生肥沃的橄榄岩,使它们容易受到热机械侵蚀,而隐交代作用,通常在由熔体-岩石比逐渐减少的熔体演化引起的难熔地幔岩石中观察到(例如,含烃硅酸盐熔体,碳酸盐岩熔体等),一般形成高不相容元素的富集,但对非克拉通性难熔SCLM的矿物组合和主元素地球化学影响不显著,使其长期保持稳定。
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引用次数: 0
Mineralogic control on the calcium and magnesium stable isotopic compositions of modern microbial carbonates 现代微生物碳酸盐钙镁稳定同位素组成的矿物学控制
IF 4.5 1区 地球科学 Q1 GEOCHEMISTRY & GEOPHYSICS Pub Date : 2025-01-15 DOI: 10.1016/j.gca.2025.01.005
Elizabeth M. Griffith , Matthew S. Fantle , Brittan V. Wogsland , Zijian Li , Majie Fan , David J. Wronkiewicz
Modern microbialites grow in a variety of environments including the hypersaline, turbid, low alkalinity, high magnesium (Mg) and calcium (Ca) concentrations (and Mg/Ca ∼ 4.5 mol/mol), shallow (less than 2 m deep) Storr’s Lake on San Salvador Island, The Bahamas. Rather than growing via the trapping and binding of sediments, these largely micritic microbialites form via microbial processes creating crusts and mounds with laminated to clotted structures comprised of both high-Mg calcite and aragonite. The primary objective of this study was to determine whether the mineralogy of representative microbialite mounds dictates their pre-burial metal isotopic compositions. The Mg and Ca isotopic compositions (δ26Mg, δ44/40Ca) of two mounds collected from 0.6 to 1.1 m water depth range considerably, from −3.04 to −2.33 ‰ (relative to DSM3) and 0.38 to 0.94 ‰ (relative to SRM 915a), respectively. Along with Sr/Ca and Mg/Ca molar ratios, δ26Mg and δ44/40Ca are unambiguously related to mineralogy. This stands in contrast to the carbon and oxygen isotopic compositions of the microbial carbonates, which do not correlate solely with mineralogy. A simple bimineralic mixture of aragonite and high-Mg calcite can explain the observations; such a mixture could be a consequence of both phases forming independently or as one phase recrystallizes from another prior to burial. To evaluate the latter hypothesis, we used a time-dependent advection-recrystallization model. We found that recrystallization of high-Mg calcite to aragonite would require an unreasonable Sr partition coefficient, while recrystallization of aragonite to high-Mg calcite could explain the observed geochemical variations in the two mounds. No microbial isotopic effect is apparent for Mg or Ca, however a difference is seen in the carbon isotopic composition of inorganic carbon where or when aragonite and high-Mg calcite form suggesting they form in two different (micro)environments. Consequently, investigations of ancient microbialites (and carbonates in general) need to consider whether mixtures of primary (original) carbonate minerals and/or recrystallization and transformation pre-burial could impact δ26Mg, δ44/40Ca, δ13C and their interpretation using a combination of isotopic, elemental, petrographic, and modeling methods. This is especially important for Mg, whose elemental and isotopic composition can be dominated by even small amounts of calcite or dolomite.
现代微生物岩生长在各种环境中,包括巴哈马圣萨尔瓦多岛上的高盐、浑浊、低碱度、高镁(Mg)和高钙(Ca)浓度(Mg /Ca ~ 4.5 mol/mol)、浅(不到2米深)的斯托尔湖。这些微晶微生物岩不是通过沉积物的捕获和结合而生长的,而是通过微生物过程形成的,形成了由高镁方解石和文石组成的层压到凝块结构的地壳和土丘。本研究的主要目的是确定具有代表性的微生物岩丘的矿物学是否决定了它们埋前的金属同位素组成。在水深0.6 ~ 1.1 m处采集的两个土丘的Mg和Ca同位素组成(δ26Mg, δ44/40Ca)变化幅度较大,分别为- 3.04 ~ - 2.33‰(相对于DSM3)和0.38 ~ 0.94‰(相对于SRM 915a)。δ26Mg和δ44/40Ca与Sr/Ca和Mg/Ca的摩尔比具有明确的矿物学关系。这与微生物碳酸盐的碳和氧同位素组成形成对比,后者不仅仅与矿物学有关。文石和高镁方解石的简单双矿物混合物可以解释这些观察结果;这种混合物可能是两相独立形成的结果,也可能是一相在埋藏之前从另一相再结晶的结果。为了评估后一种假设,我们使用了一个随时间变化的平流-再结晶模型。高镁方解石重结晶为文石需要不合理的Sr分配系数,而文石重结晶为高镁方解石可以解释两个土丘的地球化学变化。Mg或Ca没有明显的微生物同位素效应,但无机碳的碳同位素组成在文石和高Mg方解石形成的地点或时间上存在差异,表明它们形成于两种不同的(微)环境。因此,对古代微生物岩(以及一般的碳酸盐)的研究需要考虑原生(原始)碳酸盐矿物和/或重结晶转化前埋藏的混合物是否会影响δ26Mg、δ44/40Ca和δ13C,以及使用同位素、元素、岩石学和建模方法的组合解释。这对镁尤其重要,因为镁的元素和同位素组成可以由少量方解石或白云石主导。
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引用次数: 0
One-pot synthesis of non-canonical ribonucleosides and their precursors from aldehydes and ammonia under prebiotic Earth conditions 在地球前生物条件下利用醛和氨一步合成非典核糖核苷及其前体
IF 4.5 1区 地球科学 Q1 GEOCHEMISTRY & GEOPHYSICS Pub Date : 2025-01-15 DOI: 10.1016/j.gca.2024.11.006
Yuta Hirakawa , Hidenori Okamura , Fumi Nagatsugi , Takeshi Kakegawa , Yoshihiro Furukawa
The formation of polymers that can hold gene information and work as catalysts is a crucial step for the origin of life. The discovery of catalytic RNA (i.e., ribozyme) supports the hypothesis that RNA might have served these functions at the early stage of life on the Earth. Given this, the spontaneous formation of RNA monomers (i.e., ribonucleotides) and their polymerization on Hadean Earth are essential steps for the origin of life. Previous experiments have investigated the chemical reactions that allow the formation of ribonucleotides and their components. These works have revealed the required molecules to form biological ribonucleotides (i.e., canonical ribonucleotides). Based on geochemical perspectives, abundantly available reactive molecules spontaneously react with each other to provide abundant products. Aldehydes and ammonia are reactive molecules assumed to have been present in considerable amounts on Hadean Earth. However, little is understood about whether or not nucleotides and their components were formed from these molecules under prebiotic conditions. We investigated the incubation products of alkaline aqueous solutions of aldehydes and ammonia. The product solution contained sugars (including ribose), various imidazole derivatives, and ribosyl imidazole (i.e., imidazole ribonucleoside). Ribosyl imidazole is formed via ribosyl amine, which reveals a new reaction pathway for prebiotic ribonucleoside synthesis. The imidazole ribonucleoside was then phosphorylated to imidazole ribonucleotide via a simple dry-down reaction with phosphate. Borate ion improved the reaction yields of these nucleosides and nucleotides. Because all the reactants were available on prebiotic Earth and the reactions progressed spontaneously, imidazole ribonucleotides could have accumulated in prebiotic environments. The experimental simplicity of the present reaction suggests that imidazoles were more abundant than canonical nucleobases on the prebiotic Earth. This further implies that prebiotic oligonucleotides contained imidazole bases in addition to the canonical nucleobases. The improvement of the reaction yields by borate indicates that borate-rich environments were conducive places for the formation and accumulation of non-canonical nucleosides and nucleotides. Such environments could have facilitated the formation of primordial ribonucleic acids on Hadean Earth.
形成可保存基因信息并可作为催化剂的聚合物是生命起源的关键一步。催化 RNA(即核糖核酸酶)的发现支持了一种假设,即在地球生命的早期阶段,RNA 可能就具有这些功能。有鉴于此,RNA 单体(即核糖核苷酸)的自发形成及其在哈代地球上的聚合是生命起源的必要步骤。以前的实验研究了核糖核苷酸及其成分形成的化学反应。这些工作揭示了形成生物核糖核苷酸(即典型核糖核苷酸)所需的分子。从地球化学的角度来看,大量存在的活性分子会自发地相互反应,提供丰富的产物。据推测,醛和氨这两种活性分子在哈代地球上的存在量相当大。然而,人们对核苷酸及其成分是否在前生物条件下由这些分子形成知之甚少。我们研究了醛和氨的碱性水溶液的孵育产物。产物溶液中含有糖(包括核糖)、各种咪唑衍生物和核糖基咪唑(即咪唑核糖核苷)。核糖基咪唑是通过核糖基胺形成的,这揭示了前生物核糖核苷合成的新反应途径。然后,咪唑核糖核苷通过与磷酸盐的简单干化反应被磷酸化成咪唑核糖核苷酸。硼酸根离子提高了这些核苷和核苷酸的反应产率。由于在前生物地球上可以获得所有反应物,而且反应是自发进行的,因此咪唑核糖核苷酸可能在前生物环境中积累。本反应的实验简易性表明,在前生物地球上,咪唑类比典型核碱基更为丰富。这进一步意味着,前生物寡核苷酸除了含有典型的核碱基外,还含有咪唑碱基。硼酸盐提高了反应产率,这表明富含硼酸盐的环境有利于非经典核苷酸和核苷酸的形成和积累。这种环境可能促进了哈代地球上原始核糖核酸的形成。
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引用次数: 0
Rhenium residency in molybdenite, compressional textures and relationship to polytypism 辉钼矿中的铼驻留、挤压结构及其与多型关系
IF 4.5 1区 地球科学 Q1 GEOCHEMISTRY & GEOPHYSICS Pub Date : 2025-01-15 DOI: 10.1016/j.gca.2024.12.012
Mao Tan , Yiping Yang , Xiao-Wen Huang , Jiaxin Xi , Nuo Li , Yu-Miao Meng , Liang Qi
Molybdenite has been established as a robust mineral for Re-Os isotope dating. However, higher-precision Re-Os molybdenite dating is necessary to accurately determine the absolute timing of metal mineralization and duration of ore-forming hydrothermal systems. To improve the precision and accuracy of molybdenite Re-Os dating, molybdenite from the Longmendian deposit—with its old age, heterogeneous distribution of Re, compression deformation, and complex polytypes—serves as a reference for enhancing the precision of in-situ Re-Os dating or grain-scale sampling during solution Re-Os isotope dating of molybdenite. High-resolution scanning transmission electron microscopy (TEM) analysis demonstrates that Re, Os, Pb, Bi, Cu, and Fe are incorporated into the molybdenite crystal through isomorphic substitution for Mo. Electron probe analysis shows that a single molybdenite grain exhibits heterogeneous textures consisting of Re-rich (∼0.29–0.82 wt%) and Re-poor (<0.29 wt%) domains. Some molybdenite grains have undergone compression deformation. Rhenium can be enriched in either the deformed or the undeformed domains of molybdenite grains. Compression deformation in some grains induces delamination cracks in Re-rich domains, facilitating ore-forming fluid infiltration and leading to an inhomogeneous distribution of Re and other elements in molybdenite grains. Re-rich domain in molybdenite is enriched in other metals, including Fe, Co, Zn, Pb, and Bi, due to the overprint of the hydrothermal fluids with a lower temperature and a relatively high oxygen fugacity, leading to the formation of heterogeneous molybdenite. Micro-X-ray diffraction (μXRD) and TEM analyses have revealed that both the Re-rich and Re-poor domains belong to the 2H1 polytype, indicating that Re concentration and distribution are not directly related to the polytype of molybdenite. The Re-poor and deformed domain of molybdenite shows the coexistence of 2H1 and 3R polytypes (in a ratio of 9:1), suggesting that compression deformation led to polytype transformation. Therefore, the diverse characteristics of molybdenite in the Longmendian deposit present challenges for obtaining primary Re-Os age information. Nondestructive pre-characterization of molybdenite is essential before dating to ensure age homogeneity. Molybdenite samples with an undeformed and uniform distribution of elements (Re) within molybdenite grains are suitable candidates for analysis. Our findings collectively offer strategies to enhance precision while advancing the understanding of elemental and isotopic geochemical behavior in the contexts of metamorphism, deformation, and fluid flow environments.
辉钼矿已被确定为 Re-Os 同位素测年的可靠矿物。然而,要准确确定金属成矿的绝对时间和成矿热液系统的持续时间,就需要更高精度的辉钼矿Re-Os年代测定。为了提高辉钼矿Re-Os定年的精度和准确性,龙门甸矿床的辉钼矿--其年代久远、Re分布不均、压缩变形和复杂的多型性--可作为提高辉钼矿原位Re-Os定年或溶液Re-Os同位素定年过程中晶粒尺度取样精度的参考。高分辨率扫描透射电子显微镜(TEM)分析表明,Re、Os、Pb、Bi、Cu 和 Fe 是通过同构取代 Mo 的方式融入辉钼矿晶体的。电子探针分析表明,单个辉钼矿晶粒呈现出由富Re(0.29-0.82 wt%)和贫Re(0.29 wt%)域组成的异质纹理。一些辉钼矿晶粒经历了压缩变形。铼可在辉钼矿晶粒的变形或未变形域中富集。某些晶粒的压缩变形会在富铼域诱发分层裂纹,促进成矿流体的渗入,导致钼矿晶粒中的铼和其他元素分布不均。由于热液温度较低,氧富集度相对较高,导致形成异质辉钼矿,因此辉钼矿中的富集域富含其他金属,包括铁、钴、锌、铅和铋。显微 X 射线衍射(μXRD)和 TEM 分析表明,富 Re 域和贫 Re 域都属于 2H1 多晶型,表明 Re 的浓度和分布与辉钼矿的多晶型没有直接关系。辉钼矿的再贫域和变形域显示出 2H1 和 3R 多型共存(比例为 9:1),表明压缩变形导致了多型转化。因此,龙门甸矿床中辉钼矿的多样化特征为获取原始Re-Os年龄信息带来了挑战。在测年之前,必须对辉钼矿进行非破坏性预表征,以确保年龄的均一性。辉钼矿样品中的元素(Re)在辉钼矿晶粒内未变形且分布均匀,适合进行分析。我们的研究结果共同为提高精确度提供了策略,同时也推进了对变质、变形和流体流动环境下元素和同位素地球化学行为的理解。
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引用次数: 0
Stable and radiogenic strontium isotopes trace the composition and diagenetic alteration of remnant glacial seawater 稳定锶同位素和放射性锶同位素追踪残余冰川海水的组成和成岩蚀变过程
IF 4.5 1区 地球科学 Q1 GEOCHEMISTRY & GEOPHYSICS Pub Date : 2025-01-15 DOI: 10.1016/j.gca.2024.10.028
Madison M. Wood , Clara L. Blättler , Ana Kolevica , Anton Eisenhauer , Adina Paytan
A remnant of glacial seawater preserved in the pore fluids of sediment cores from the Maldives Inner Sea provided an opportunity to investigate the stable strontium isotopic composition (δ88/86Sr) of the ocean during the Last Glacial Maximum and explore the usefulness of δ88/86Sr as a tracer of early marine diagenesis. We used paired measurements of δ88/86Sr and radiogenic Sr isotope ratios (87Sr/86Sr) in pore fluids and surrounding carbonate sediments to constrain the diagenetic history of the preserved glacial water mass at IODP Sites U1466 and U1468. These pore fluid profiles document variability in δ88/86Sr in a shallow marine setting, revealing distinct diagenetic processes dominating within different depth intervals. We find evidence for isotope fractionation during secondary calcite precipitation at intermediate depths and observe that in aragonite-dominated settings, fractionation during recrystallization may be obscured by the dissolution of aragonite in the uppermost sediments. Correcting for the effect of carbonate recrystallization on pore fluid Sr concentration ([Sr]) and isotopic composition, we estimate that glacial seawater [Sr] was higher (98μM) and δ88/86Sr lower (0.32‰) compared to the modern ocean, consistent with hypotheses attributing the present-day disequilibrium of the ocean Sr budget to glacial/interglacial changes in shelf carbonate weathering and burial. Our results provide evidence that the ocean [Sr] and δ88/86Sr are sensitive to carbon cycle changes on timescales much shorter than its residence time (2 Myr) and demonstrate that pore fluid δ88/86Sr measurements are a useful addition to multi-tracer studies of diagenesis in complex marine systems.
马尔代夫内海沉积岩芯孔隙流体中保存的冰川海水残余为研究末次冰川极盛时期海洋的稳定锶同位素组成(δ88/86Sr)提供了机会,并探索了δ88/86Sr作为早期海洋成岩作用示踪剂的作用。我们利用孔隙流体和周围碳酸盐沉积物中的δ88/86Sr和放射性Sr同位素比值(87Sr/86Sr)的成对测量来制约IODP U1466和U1468站点保存的冰川水团的成岩历史。这些孔隙流体剖面记录了浅海环境中δ88/86Sr的变化,揭示了不同深度区间内占主导地位的不同成岩过程。我们发现了中等深度次生方解石沉淀过程中同位素分馏的证据,并观察到在以霰石为主的环境中,重结晶过程中的分馏可能会被最上层沉积物中霰石的溶解所掩盖。在校正碳酸盐重结晶对孔隙流体锶浓度([Sr])和同位素组成的影响后,我们估计冰期海水[Sr]比现代海洋高(∼98μM),δ88/86Sr比现代海洋低(∼0.32‰),这与冰期/间冰期陆架碳酸盐风化和埋藏变化导致当今海洋锶预算失衡的假设是一致的。我们的研究结果提供了证据,表明海洋[Sr]和δ88/86Sr对碳循环变化的敏感性在时间尺度上远远短于其停留时间(2 Myr),并证明孔隙流体δ88/86Sr测量是对复杂海洋系统成因多示踪研究的有益补充。
{"title":"Stable and radiogenic strontium isotopes trace the composition and diagenetic alteration of remnant glacial seawater","authors":"Madison M. Wood ,&nbsp;Clara L. Blättler ,&nbsp;Ana Kolevica ,&nbsp;Anton Eisenhauer ,&nbsp;Adina Paytan","doi":"10.1016/j.gca.2024.10.028","DOIUrl":"10.1016/j.gca.2024.10.028","url":null,"abstract":"<div><div>A remnant of glacial seawater preserved in the pore fluids of sediment cores from the Maldives Inner Sea provided an opportunity to investigate the stable strontium isotopic composition (<span><math><msup><mrow><mi>δ</mi></mrow><mrow><mn>88</mn><mo>/</mo><mn>86</mn></mrow></msup></math></span>Sr) of the ocean during the Last Glacial Maximum and explore the usefulness of <span><math><msup><mrow><mi>δ</mi></mrow><mrow><mn>88</mn><mo>/</mo><mn>86</mn></mrow></msup></math></span>Sr as a tracer of early marine diagenesis. We used paired measurements of <span><math><msup><mrow><mi>δ</mi></mrow><mrow><mn>88</mn><mo>/</mo><mn>86</mn></mrow></msup></math></span>Sr and radiogenic Sr isotope ratios (<sup>87</sup>Sr/<sup>86</sup>Sr) in pore fluids and surrounding carbonate sediments to constrain the diagenetic history of the preserved glacial water mass at IODP Sites U1466 and U1468. These pore fluid profiles document variability in <span><math><msup><mrow><mi>δ</mi></mrow><mrow><mn>88</mn><mo>/</mo><mn>86</mn></mrow></msup></math></span>Sr in a shallow marine setting, revealing distinct diagenetic processes dominating within different depth intervals. We find evidence for isotope fractionation during secondary calcite precipitation at intermediate depths and observe that in aragonite-dominated settings, fractionation during recrystallization may be obscured by the dissolution of aragonite in the uppermost sediments. Correcting for the effect of carbonate recrystallization on pore fluid Sr concentration ([Sr]) and isotopic composition, we estimate that glacial seawater [Sr] was higher (<span><math><mrow><mo>∼</mo><mn>98</mn><mspace></mspace><mi>μ</mi></mrow></math></span>M) and <span><math><msup><mrow><mi>δ</mi></mrow><mrow><mn>88</mn><mo>/</mo><mn>86</mn></mrow></msup></math></span>Sr lower (<span><math><mo>∼</mo></math></span>0.32‰) compared to the modern ocean, consistent with hypotheses attributing the present-day disequilibrium of the ocean Sr budget to glacial/interglacial changes in shelf carbonate weathering and burial. Our results provide evidence that the ocean [Sr] and <span><math><msup><mrow><mi>δ</mi></mrow><mrow><mn>88</mn><mo>/</mo><mn>86</mn></mrow></msup></math></span>Sr are sensitive to carbon cycle changes on timescales much shorter than its residence time (<span><math><mo>∼</mo></math></span>2 Myr) and demonstrate that pore fluid <span><math><msup><mrow><mi>δ</mi></mrow><mrow><mn>88</mn><mo>/</mo><mn>86</mn></mrow></msup></math></span>Sr measurements are a useful addition to multi-tracer studies of diagenesis in complex marine systems.</div></div>","PeriodicalId":327,"journal":{"name":"Geochimica et Cosmochimica Acta","volume":"389 ","pages":"Pages 211-223"},"PeriodicalIF":4.5,"publicationDate":"2025-01-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142673701","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"地球科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Influence of the Amazon River on the composition of particulate organic carbon in the western tropical Atlantic Ocean
IF 4.5 1区 地球科学 Q1 GEOCHEMISTRY & GEOPHYSICS Pub Date : 2025-01-15 DOI: 10.1016/j.gca.2024.09.011
Giovanna S.A. Utsumi , Ding He , William M. Berelson , Renato M. Castelao , Patricia L. Yager , Patricia M. Medeiros
The Amazon River exports ∼13.7 Tg yr−1 of particulate organic carbon (POC) to the ocean, a portion of which is transported vertically through the water column. Here, we investigated in detail the composition of POC using a multi-tracer approach, including POC concentration, stable carbon isotopes (δ13C) and a wide range of molecular biomarkers to assess the contribution of POC export from the Amazon River to the western tropical Atlantic Ocean (WTAO). For this purpose, suspended and sediment trap POC were collected at multiple depths along the Amazon River plume under high and low river discharge conditions. Concentrations of POC detected in the plume were ∼2 to 3-fold higher than those below the plume. Overall, δ13C signatures of suspended and sediment trap POC samples were enriched, averaging −19.9 ‰ and –22.8 ‰, respectively. At the surface, POC composition was mainly characterized by low molecular weight n-alkanoic acids (<C20), mono- and disaccharides (e.g., glucose, scyllo-inositol and melibiose) and triglyceride derivatives (e.g., glycerol and 2-O-glycerol-α-D-galactopyranoside), indicating fresh inputs of organic matter (OM) presumably derived from algal blooms. These biomarkers were observed in lower concentrations in sediment traps. Trap samples were marked by zooplankton- (e.g., cholesterol, occelasterol) and bacteria-derived (e.g., C15 and C17 branched n-alkanoic acids) biomarkers, indicating metabolic alteration of OM at those depths. Solvent-extractable terrestrial biomarkers (e.g., dehydroabietic acid and levoglucosan) were only found in minor concentrations in most samples, which contrasts with the dissolved fraction which has been previously shown to have a primary signature of terrigenous inputs. Our results clarify the Amazon River plume’s impact on the biological pump of the WTAO, consistent with a river plume fueling primary production, and with increased zooplankton and bacteria contributions to POC composition at depth and in the POC that is vertically exported.
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引用次数: 0
Polycrystalline diamond aggregates and their role in Earth’s deep carbon cycle 多晶金刚石聚集体及其在地球深层碳循环中的作用
IF 4.5 1区 地球科学 Q1 GEOCHEMISTRY & GEOPHYSICS Pub Date : 2025-01-15 DOI: 10.1016/j.gca.2024.10.021
Dorrit E. Jacob , Richard A. Stern , Janina Czas , Magnus Reutter , Sandra Piazolo , Thomas Stachel
Polycrystalline diamond aggregates (PDAs) are small rocks composed mostly of diamond grains, but often containing also peridotitic, eclogitic and/or websteritic minerals as accessory phases. PDAs are formed rapidly in Earth’s mantle, and the diamonds preserve heterogeneity not often seen in monocrystalline diamond. Here, diamond grains from forty-three PDAs from the Venetia diamond mine (RSA) with grain-sizes < 1 mm are presented. They have heterogeneous and complex cathodoluminescence signatures that are best explained by multiple, separate diamond growth episodes from compositionally distinct COH fluids/melts. The diamonds show a large range of nitrogen concentrations (0.5 to 2,891 at. ppm), δ15N (−4.3 to + 16.8 ‰) and δ13C values (−27.8 to −7.6 ‰). The positive δ15N median of + 6.4 ‰ and negative δ13C median of −21.2 ‰ indicate derivation of the diamond-forming fluid from organic materials in subducted oceanic crust and lithosphere. Two PDAs have δ13C and δ15N values typical for Earth’s mantle. Thirty-three PDAs contain websteritic garnets, or peridotitic garnets and clinopyroxenes and/or micas. Unradiogenic εNdi values in the garnets (−15.9 to −29.7) and clinopyroxene (−8.3) and δ18O values of 6.49 to 8.09 ‰ in websteritic garnets are consistent with an origin from subducted altered oceanic crust and support the findings from N and C systematics in the diamonds. Nitrogen aggregation data for the diamonds range from 25 % to 100 %B and vary by as much as 60 % within some individual PDAs. We explain the geochemical and isotopic heterogeneity of diamonds and silicates as well as the complex cathodoluminescence features with a model of episodic melt/fluid −rock interaction involving a reducing asthenospheric melt in the cratonic roots or the thermal boundary layer. We suggest that large volumes of PDA are formed in the cratonic roots and thermal boundary layer by this mechanism, making them an important reservoir for carbon storage, which is corroborated with their locally high abundance (ca. 20 %) in some kimberlites.
多晶金刚石集合体(PDAs)是一种小型岩石,主要由金刚石颗粒组成,但通常也含有橄榄石、夕闪石和/或网状石矿物作为附属相。PDAs 在地幔中迅速形成,其金刚石保留了单晶金刚石中不常见的异质性。这里展示的是来自 Venetia 钻石矿(RSA)的 43 个 PDA 的钻石晶粒,晶粒大小为 1 毫米。这些金刚石具有异质和复杂的阴极荧光特征,最好的解释是来自成分不同的 COH 流体/熔体的多个独立的金刚石生长过程。这些钻石的氮浓度(0.5 至 2,891 at. ppm)、δ15N 值(-4.3 至 + 16.8 ‰)和δ13C 值(-27.8 至 -7.6‰)范围很大。δ15N中值为+ 6.4‰,δ13C中值为-21.2‰,这表明金刚石形成流体来自俯冲洋壳和岩石圈中的有机物质。两个 PDA 的 δ13C 和 δ15N 值是地幔的典型值。33个PDA含有网状石榴石,或橄榄石榴石和霰石和/或云母。石榴石(-15.9 至 -29.7)和霞石(-8.3)中的非辐射εNdi 值,以及蹼星状石榴石中 6.49 至 8.09 ‰ 的 δ18O 值,都与来源于俯冲蚀变的大洋地壳相一致,并支持钻石中 N 和 C 系统学的发现。金刚石的氮聚集数据从 25 % 到 100 %B 不等,在某些单个 PDA 中,差异高达 60 %。我们用一个涉及板块根部或热边界层中还原性天体层熔体的偶发性熔体/流体-岩石相互作用模型来解释金刚石和硅酸盐的地球化学和同位素异质性以及复杂的阴极发光特征。我们认为,在这种机制下,大量的PDA在板根和热边界层中形成,使其成为碳储存的重要储藏库,这与某些金伯利岩中PDA的局部高丰度(约20%)相印证。
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引用次数: 0
Climate controls on speleothem initial 234U/238U ratios in midlatitude settings over two glacial cycles 在两个冰期旋回中纬度环境下,气候对洞穴初始234U/238U比值的控制
IF 4.5 1区 地球科学 Q1 GEOCHEMISTRY & GEOPHYSICS Pub Date : 2025-01-15 DOI: 10.1016/j.gca.2024.11.016
Carlos Pérez-Mejías , Jian Wang , Youfeng Ning , Ana Moreno , Antonio Delgado-Huertas , R. Lawrence Edwards , Hai Cheng , Heather M. Stoll
<div><div>Despite early hydrological studies of <sup>234</sup>U/<sup>238</sup>U in groundwaters, their utilization as a paleoclimatic proxy in stalagmites has remained sporadic. This study explores uranium isotope ratios in 235 datings (<sup>230</sup>Th) from six stalagmites in Ejulve cave, northeastern Iberia, covering the last 260 ka. The observed <sup>234</sup>U enrichment is attributed to selective leaching of <sup>234</sup>U from damaged lattice sites, linked to the number of microfractures in the drip route and wetness frequency, which under certain conditions, may result in the accumulation of <sup>234</sup>U recoils. This selective leaching process diminishes with enhanced bedrock dissolution, leading to low δ<sup>234</sup>U. Temperature variations significantly influence bedrock dissolution intensity. During stadial periods and glacial maxima, lower temperatures likely reduced vegetation and respiration rates, thereby decreasing soil CO<sub>2</sub> and overall rock dissolution rates. This reduction could enhance the preferential leaching of <sup>234</sup>U from bedrock surfaces due to lower bulk rock dissolution. Additionally, the temperature regime during cold periods may have facilitated more frequent freeze–thaw cycles, resulting in microfracturing and exposure of fresh surfaces. Conversely, warmer temperatures increased soil respiration rates and soil CO<sub>2</sub>, accelerating rock dissolution rates during interstadials and interglacials, when low δ<sup>234</sup>U is consistent with high bedrock dissolution rates. The contribution of a number of variables sensitive to bedrock dissolution and wetness frequency processes successfully explains 57% and 74% of the variability observed in the δ<sup>234</sup>U in <em>Andromeda</em> stalagmite during MIS 3–4 and MIS 5b-5e, respectively. Among these variables, the growth rate has emerged as crucial to explain δ<sup>234</sup>U variability, highlighting the fundamental role of soil respiration and soil CO<sub>2</sub> in δ<sup>234</sup>U through bedrock dissolution. I-STAL simulations provides the potential for a combination of Prior Calcite Precipitation (PCP) indicators like Mg/Ca with PCP-insensitive indicators of bedrock dissolution such as δ<sup>234</sup>U, along with growth rate data, may be useful to diagnose when PCP variations reflect predominantly changes in drip intervals and when changes in bedrock dissolution intensity contribute. The relationship between stalagmite δ<sup>234</sup>U, bedrock dissolution, and initial dripwater oversaturation suggests two significant advancements in paleoclimate proxies. First, δ<sup>234</sup>U could serve as a valuable complement to δ<sup>13</sup>C since it is significantly influenced by soil respiration and soil CO<sub>2</sub>, thereby reflecting soil and vegetation productivity sensitive to both humidity and temperature. Secondly, since PCP does not fractionate uranium isotopes, δ<sup>234</sup>U could be used in combination with Mg/Ca or δ<sup>4
尽管很早就对地下水中的 234U/238U 进行了水文研究,但将其用作石笋中的古气候替代物的研究仍是零星的。本研究探讨了伊比利亚东北部埃居尔韦洞六根石笋中 235 定量(230Th)的铀同位素比率,时间跨度为过去 260 ka。观察到的 234U 富集现象归因于 234U 从受损晶格部位的选择性沥滤,这与滴水路径中的微裂缝数量和湿润频率有关,在某些条件下,可能会导致 234U 反冲的积累。这种选择性沥滤过程会随着基岩溶解度的提高而减弱,从而导致 234U δ 值降低。温度变化对基岩溶解强度有很大影响。在恒星期和冰川最大值期间,较低的温度可能会降低植被和呼吸速率,从而减少土壤中的二氧化碳和整体岩石溶解速率。由于岩石的整体溶解度降低,这种降低可能会加强 234U 从基岩表面的优先沥滤。此外,寒冷时期的温度机制可能会促进更频繁的冻融循环,导致微裂缝和新鲜表面的暴露。相反,在间冰期和间冰期,较高的温度增加了土壤呼吸速率和土壤二氧化碳含量,从而加快了岩石溶解速率,此时低δ234U与高基岩溶解速率相一致。在 MIS 3-4 和 MIS 5b-5e 期间,对基岩溶解和湿润频率过程敏感的一些变量分别成功地解释了在仙女座石笋中观察到的δ234U 变化的 57% 和 74%。在这些变量中,生长率是解释δ234U变化的关键,突出了土壤呼吸和土壤二氧化碳通过基岩溶解在δ234U中的基本作用。I-STAL 模拟提供了将镁/钙等方解石降水(PCP)指标与δ234U 等对 PCP 不敏感的基岩溶解指标结合起来的可能性,再加上生长率数据,可能有助于诊断 PCP 变化主要反映的是滴水间隔的变化,而基岩溶解强度的变化则是主要原因。石笋δ234U、基岩溶解和初始滴水过饱和之间的关系表明了古气候代用指标的两个重大进展。首先,δ234U 可以作为δ13C 的重要补充,因为它受到土壤呼吸作用和土壤二氧化碳的显著影响,从而反映了对湿度和温度敏感的土壤和植被生产力。其次,由于五氯苯酚不对铀同位素进行分馏,δ234U 可与 Mg/Ca 或 δ44Ca 结合使用,以将滴水速率变化引起的五氯苯酚变化与初始饱和状态变化引起的五氯苯酚变化区分开来。这项研究强调了气候对δ234U的压倒性控制作用,而不考虑样本间234U/238U活性的绝对比值及其与世俗平衡的远近。
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引用次数: 0
Chemical characteristics of the Yamato-type (CY) carbonaceous chondrites 大和型(CY)碳质软玉的化学特征
IF 4.5 1区 地球科学 Q1 GEOCHEMISTRY & GEOPHYSICS Pub Date : 2025-01-15 DOI: 10.1016/j.gca.2024.10.026
Mitsuru Ebihara , Naoki Shirai , Takahito Osawa , Akira Yamaguchi
Fifteen elements, including most of the major elements, were quantified using neutron-induced prompt gamma-ray analysis for five Antarctic carbonaceous chondrites with CI affinities and seven with CM affinities. Common among the twelve meteorites is the depletion of volatile elements H and chlorine, showing a positive correlation and being depleted compared to non-Antarctic CI levels. This depletion is not thought to have occurred after the fall on Antarctica, but to have been caused by thermal metamorphism on the parent body. Among the meteorites analyzed in this study, six meteorites (Y-86029, Y 980115 and Y-82162 (with CI affinities), and Y-86720, Y-86789 and B-7904 (with CM affinities)) have previously been proposed to constitute a new meteorite group, the Yamato-type (CY), based on their oxygen isotopic compositions and petrological features. The elemental compositional characteristics of the remaining six meteorites analyzed in this study, Y-86737 and Y 980134 (with CI affinities), and Y-86770, Y-86771, Y-86772 and Y-86773 (with CM affinities), suggest that these meteorites are all classified into the same chemical group CY. Based on the abundance of moderately volatile elements Mn and S, the twelve meteorites can be divided into two groups: one with levels similar to non-Antarctic CI and the other with intermediate levels between CI and CM. These results suggest that CY chondrites originate from two distinct parent bodies. To facilitate further discussions on CY chondrites, we propose naming the groups with compositions close to CI and CM as CYi and CYm, respectively.
利用中子诱导瞬时伽马射线分析,对五块具有 CI 亲缘关系的南极碳质陨石和七块具有 CM 亲缘关系的南极碳质陨石的十五种元素(包括大多数主要元素)进行了定量分析。这十二块陨石的共同点是挥发性元素 H 和氯的消耗,与非南极 CI 水平相比,这两种元素的消耗呈正相关。这种损耗被认为不是在陨落到南极洲之后发生的,而是由母体的热变质作用引起的。在这项研究分析的陨石中,有六块陨石(Y-86029、Y 980115 和 Y-82162(具有 CI 亲缘关系),以及 Y-86720、Y-86789 和 B-7904(具有 CM 亲缘关系))曾被根据它们的氧同位素组成和岩石学特征而提议构成一个新的陨石群--大和类型(CY)。本研究分析的其余六块陨石,即 Y-86737 和 Y 980134(具有 CI 亲缘关系),以及 Y-86770、Y-86771、Y-86772 和 Y-86773(具有 CM 亲缘关系)的元素组成特征表明,这些陨石都被归入同一化学组 CY。根据中等挥发性元素 Mn 和 S 的丰度,这 12 块陨石可分为两组:一组的含量与非南极 CI 相似,另一组的含量介于 CI 和 CM 之间。这些结果表明,CY 陨石起源于两个不同的母体。为了便于进一步讨论CY软玉,我们建议将成分接近CI和CM的组别分别命名为CYi和CYm。
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Geochimica et Cosmochimica Acta
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