Thallium isotope cycling between waters, particles, and sediments across a redox gradient
Thallium isotope cycling between waters, particles, and sediments across a redox gradient
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铊同位素在水、颗粒和沉积物之间通过氧化还原梯度循环
DOI：
10.1016/j.gca.2023.03.028
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发表时间：
2023
影响因子：
5
通讯作者：
Hansel, Colleen M.
中科院分区：
文献类型：
--
作者：
Ostrander, Chadlin M.;Nielsen, Sune G.;Gadol, Hayley J.;Villarroel, Luciana;Wankel, Scott D.;Horner, Tristan J.;Blusztajn, Jerzy;Hansel, Colleen M.
铊（Tl）同位素是追踪海水中分子氧历史的新兴工具。以这种方式使用铊同位素需要彻底了解现代铊同位素循环，特别是在代表地球过去海洋的缺氧环境中。为此，我们产生的Tl浓度和同位素数据的沃茨，颗粒和沉积物收集在三个春季，夏季，秋季现场季节在赛德斯池塘，盐分层和硫化物丰富（“euxinic”）的科德角（马萨诸塞州，美国）池塘。在较短的时间范围内（即，几天到几周），我们观察到池塘表面沃茨中溶解的Tl的丰度（Tldiss= 9 pM-42 pM）和同位素组成（ε 205 Tldiss = -3.9 ± 0.4; 2SD到-0.1 ± 0.7; 2SD）的很大程度的变化。铊下降是常见的，有利于去除较轻质量的铊同位素。我们推测生物学上的T1摄取在这种现象中起作用，但需要更多的工作来证实这一假设。在许多采样日，锰氧化物持续存在于池塘表面沃茨中，但对Tldiss没有明显影响，仅对锰氧化物最多积累日的颗粒ε 205 Tl值有轻微影响（使ε 205 Tl partas高达+0.9 ± 0.8; 2SD）。在富氧沃茨下的氧跃层，溶解的Tl的快速下降，观察到在所有采样日连同补充增加的颗粒Tl（高达Tlpart= 21 pM）。Tl和硫化物之间的强关联，和Tl和其他亲铜金属（钼和镉）之间，表明Tl可能是从euxinic沃茨中去除与颗粒硫化物，似乎没有可分辨的同位素分馏效应，尽管非定量Tl去除。沉积物数据跟踪池塘中的长期T1循环（即，多年来），并揭示有限的同位素变异性。从表层沉积物沥滤的铊同位素组成与同期沃茨的预测相匹配，或几乎如此，在池塘的所有深度（上面，里面，下面的氧跃层）。显然，只有一小部分的短期铊同位素变化中发现的好氧表面沃茨的赛德斯池塘得到转移到缺氧沃茨，基本上没有转移到沉积物。我们的研究结果重申了这一概念，铊同位素是唯一能够跟踪长期沉积锰氧化物埋藏-而不仅仅是锰氧化物的形成。我们的研究结果也验证了在还原条件下形成的沉积物捕获同期沃茨的铊同位素组成的能力。更广泛地说，我们的调查结果加强了我们对现代铊同位素循环的了解，从而允许对地球过去的这种循环进行更有信心的推断。
Thallium (Tl) isotopes are an emerging tool for tracking the history of molecular oxygen in seawater. Use of Tl isotopes in this manner requires a thorough understanding of the modern Tl isotope cycle, especially within the anoxic settings that typified Earth’s past oceans. To this end, we generated Tl concentration and isotope data for waters, particles, and sediments collected during three spring-summer-fall field seasons in Siders Pond, a salt-stratified and sulfide-rich (‘euxinic’) pond on Cape Cod (Massachusetts, USA). Over short timeframes (i.e., days to weeks), we observed a large degree of variability in the abundance (Tldiss= 9 pM–42 pM) and isotopic composition (ε205Tldiss= –3.9 ± 0.4; 2SD to –0.1 ± 0.7; 2SD) of dissolved Tl in pond surface waters. Thallium drawdown was common and favored removal of the lighter-mass Tl isotope. We surmise that biological Tl uptake plays a role in this phenomenon, but more work is warranted to confirm this hypothesis. Manganese oxides persisted in pond surface waters on many sampling days but had no obvious effect on Tldiss, only a slight effect on particulate ε205Tl values on the day of most prolific Mn oxide accumulation (driving ε205Tlpartas high as +0.9 ± 0.8; 2SD). In euxinic waters below the oxycline, rapid drawdown of dissolved Tl was observed on all sampling days together with a complimentary increase in particulate Tl (up to Tlpart= 21 pM). Strong associations between Tl and sulfide, and between Tl and other chalcophile metals (Mo and Cd), suggest that Tl is probably removed from euxinic waters in association with particulate sulfides, and seemingly with no resolvable isotopic fractionation effect despite non-quantitative Tl removal. The sediment data track the longer-term Tl cycle in the pond (i.e., across years) and reveal limited isotopic variability. Thallium isotope compositions leached from surface sediments match those predicted for contemporaneous waters, or nearly so, at all depths in the pond (above, within, and below the oxycline). Apparently, only a small fraction of the short-term Tl isotope variability found in the oxic surface waters of Siders Pond gets transferred to anoxic waters, and essentially none is transferred to sediments. Our results reaffirm the notion that Tl isotopes are uniquely capable of tracking long-term sedimentary Mn oxide burial – not mere Mn oxide formation. Our results also verify the ability of sediments formed under reducing conditions to capture the Tl isotope composition of contemporaneous waters. More broadly, the results of our investigation bolster our knowledge of the modern Tl isotope cycle and thereby permit more confident inferences of this cycle in Earth’s past.
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影响因子：
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DOI：
10.1007/bf00425919
发表时间：
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期刊：
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影响因子：
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作者：
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作者：
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