Environmental Earth System Science, Stanford Univ., Stanford, CA 94305, USA.
J Environ Qual. 2011 Jan-Feb;40(1):90-7. doi: 10.2134/jeq2010.0304.
Uranium is a pollutant of concern to both human and ecosystem health. Uranium's redox state often dictates whether it will reside in the aqueous or solid phase and thus plays an integral role in the mobility of uranium within the environment. In anaerobic environments, the more oxidized and mobile form of uranium (UO2(2+) and associated species) may be reduced, directly or indirectly, by microorganisms to U(IV) with subsequent precipitation of UO. However, various factors within soils and sediments, such as U(VI) speciation and the presence of competitive electron acceptors, may limit biological reduction of U(VI). Here we examine simultaneous dissimilatory reduction of Fe(III) and U(VI) in batch systems containing dissolved uranyl acetate and ferrihydrite-coated sand. Varying amounts of calcium were added to induce changes in aqueous U(VI) speciation. The amount of uranium removed from solution during 100 h of incubation with S. putrefaciens was 77% in absence of Ca or ferrihydrite, but only 24% (with ferrihydrite) and 14% (without ferrihydrite) were removed for systems with 0.8 mM Ca. Dissimilatory reduction of Fe(III) and U(VI) proceed through different enzyme pathways within one type of organism. We quantified the rate coefficients for simultaneous dissimilatory reduction of Fe(III) and U(VI) in systems varying in Ca concecentration (0-0.8 mM). The mathematical construct, implemented with the reactive transport code MIN3P, reveals predominant factors controlling rates and extent of uranium reduction in complex geochemical systems.
铀是人类和生态系统健康的关注污染物。铀的氧化还原状态通常决定了它将存在于水相还是固相中,因此在铀在环境中的迁移性中起着不可或缺的作用。在厌氧环境中,更氧化和更易移动的铀形式(UO2(2+)和相关物种)可能被微生物直接或间接地还原为 U(IV),随后沉淀为 UO。然而,土壤和沉积物中的各种因素,如 U(VI)形态和存在的竞争电子受体,可能会限制 U(VI)的生物还原。在这里,我们研究了含有溶解的乙酸铀酰和水铁矿涂层砂的批处理系统中同时进行的 Fe(III)和 U(VI)异化还原。添加不同量的钙来诱导水溶液中 U(VI)形态的变化。在与 S. putrefaciens 孵育 100 小时期间,从溶液中去除的铀量在没有 Ca 或水铁矿的情况下为 77%,但在有 0.8 mM Ca 的系统中,仅去除了 24%(有水铁矿)和 14%(没有水铁矿)。Fe(III)和 U(VI)的异化还原通过一种生物体内的不同酶途径进行。我们量化了 Ca 浓度(0-0.8 mM)变化的系统中同时异化还原 Fe(III)和 U(VI)的速率系数。该数学结构,使用反应传输代码 MIN3P 实现,揭示了控制复杂地球化学系统中铀还原速率和程度的主要因素。