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首页> 外文期刊>Environmental Science & Technology >Heterogeneous Reduction of PuO_2 with Fe(II): Importance of the Fe(III) Reaction Product
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Heterogeneous Reduction of PuO_2 with Fe(II): Importance of the Fe(III) Reaction Product

机译：Fe（II）异质还原PuO_2：Fe（III）反应产物的重要性

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摘要

Heterogeneous reduction of actinides in higher, more soluble oxidation states to lower, more insoluble oxidation states by reductants such as Fe(II) has been the subject of intensive study for more than two decades. However, Fe(II)-induced reduction of sparingly soluble Pu(IV) to the more soluble lower oxidation state Pu(III) has been much less studied, even though such reactions can potentially increase the mobility of Pu in the subsurface. Thermodynamic calculations are presented that show how differences in the free energy of various possible solid-phase Fe(III) reaction products can greatly influence aqueous Pu(III) concentrations resulting from reduction of PuO_2(am) by Fe(II). We present the first experimental evidence that reduction of PuO_2(am) to Pu(III) by Fe(II) was enhanced when the Fe(III) mineral goethite was spiked into the reaction. The effect of goethite on reduction of Pu(IV) was demonstrated by measuring the time dependence of total aqueous Pu concentration, its oxidation state, and system pe/pH. We also re-evaluated established protocols for determining Pu(III) {[Pu(III) + Pu(IV)] - Pu(IV)} by using thenoyltrifluoroacetone (TTA) in toluene extractions; the study showed that it is important to eliminate dissolved oxygen from the TTA solutions for accurate determinations. More broadly, this study highlights the importance of the Fe(III) reaction product in actinide reduction rate and extent by Fe(II).
机译：二十多年来，诸如Fe（II）之类的还原剂将higher系元素以更高，更易溶的氧化态异质还原为更低，更不溶的氧化态一直是深入研究的主题。然而，对Fe（II）诱导的难溶Pu（IV）还原为更易溶的较低氧化态Pu（III）的研究很少，尽管此类反应可能会增加Pu在地下的迁移率。提出的热力学计算表明，各种可能的固相Fe（III）反应产物的自由能差异如何极大地影响由于Fe（II）还原PuO_2（am）而导致的Pu（III）水溶液浓度。我们提供的第一个实验证据表明，当将Fe（III）矿物针铁矿掺入反应中时，Fe（II）将PuO_2（am）还原为Pu（III）的反应得到增强。通过测量总含水Pu浓度，其氧化态和系统pe / pH的时间依赖性证明了针铁矿对Pu（IV）还原的影响。我们还重新评估了在甲苯萃取中使用壬基三氟丙酮（TTA）确定Pu（III）{[Pu（III）+ Pu（IV）]-Pu（IV）}的既定方案；研究表明，从TTA溶液中消除溶解氧对于准确测定非常重要。更广泛地说，这项研究突出了Fe（III）反应产物在act离子还原速率和Fe（II）还原程度方面的重要性。

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  • 来源
    《Environmental Science & Technology》 |2011年第9期|p.3952-3958|共7页
  • 作者

    Andrew R. Felmy; Dean A. Moore; Kevin M. Rosso; Odeta Qafoku; Dhanpat Rai; Edgar C. Buck; Eugene S. Ilton;

  • 作者单位

    Pacific Northwest National Laboratory, Richland, Washington, United States;

    Pacific Northwest National Laboratory, Richland, Washington, United States;

    Pacific Northwest National Laboratory, Richland, Washington, United States;

    Pacific Northwest National Laboratory, Richland, Washington, United States;

    Rai Enviro-Chem, LLC, Yachats, Oregon, United States;

    Pacific Northwest National Laboratory, Richland, Washington, United States;

    Pacific Northwest National Laboratory, Richland, Washington, United States;

  • 收录信息 美国《科学引文索引》(SCI);美国《工程索引》(EI);美国《生物学医学文摘》(MEDLINE);美国《化学文摘》(CA);
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