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细菌和零价铁还原六价铀过程中实验测定的铀同位素分馏

Experimentally determined uranium isotope fractionation during reduction of hexavalent U by bacteria and zero valent iron.

作者信息

Rademacher Laura K, Lundstrom Craig C, Johnson Thomas M, Sanford Robert A, Zhao Juanzho, Zhang Zhaofeng

机构信息

Department of Geosciences, University of the Pacific, USA.

出版信息

Environ Sci Technol. 2006 Nov 15;40(22):6943-8. doi: 10.1021/es0604360.

Abstract

Variations in stable isotope ratios of redox sensitive elements are often used to understand redox processes occurring near the Earth's surface. Presented here are measurements of mass-dependent U isotope fractionation induced by U(VI) reduction by zerovalent iron (Fe0) and bacteria under controlled pH and HCO3- conditions. In abiotic experiments, Fe0 reduced U(VI), but the reaction failed to induce an analytically significant isotopic fractionation. Bacterial reduction experiments using Geobacter sulfurreducens and Anaeromyxobacter dehalogenans reduced dissolved U(VI) and caused enrichment of 238U relative to 235U in the remaining U(VI). Enrichmentfactors (epsilon) calculated using a Rayleigh distillation model are -0.31% per hundred and -0.34% per hundred for G. sulfurreducens and A. dehalogenans, respectively, under identical experimental conditions. Further studies are required to determine the range of possible values for 238U/235U fractionation factors under a variety of experimental conditions before broad application of these results is possible. However, the measurable variations in delta(5238)U show promise as indicators of reduction for future studies of groundwater contamination, geochronology, U ore deposit formation, and U biogeochemical cycling.

摘要

氧化还原敏感元素稳定同位素比值的变化常被用于理解地球表面附近发生的氧化还原过程。本文展示了在受控的pH值和HCO₃⁻条件下,零价铁(Fe⁰)和细菌对U(VI)的还原作用所导致的质量依赖型U同位素分馏的测量结果。在非生物实验中,Fe⁰还原了U(VI),但该反应未能诱导出具有分析意义的同位素分馏。使用硫还原地杆菌(Geobacter sulfurreducens)和脱卤厌氧粘细菌(Anaeromyxobacter dehalogenans)进行的细菌还原实验降低了溶解态的U(VI),并导致剩余U(VI)中²³⁸U相对于²³⁵U的富集。在相同实验条件下,使用瑞利蒸馏模型计算得出的硫还原地杆菌和脱卤厌氧粘细菌的富集因子(ε)分别为每千-0.31%和每千-0.34%。在广泛应用这些结果之前,需要进一步研究以确定在各种实验条件下²³⁸U/²³⁵U分馏因子的可能值范围。然而,δ(⁵²³⁸)U中可测量的变化有望作为未来地下水污染、地质年代学、铀矿床形成和铀生物地球化学循环研究中还原作用的指标。

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