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Plutonium oxidation and subsequent reduction by Mn(IV) minerals in Yucca Mountain tuff

机译：丝兰山凝灰岩中的氧化及随后的Mn（IV）矿物的还原

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摘要

Plutonium oxidation state distribution on Yucca Mountain tuff and synthetic pyrolusite (beta-MnO2) suspensions was measured using synchrotron X-ray micro-spectroscopy and microimaging techniques as well as ultrafiltration/solvent-extraction techniques. Plutonium sorbed to the tuff was preferentially associated with manganese oxides. For both Yucca Mountain tuff and synthetic pyrolusite, Pu(IV) or Pu(V) was initially oxidized to more mobile Pu(V/VI), but over time, the less mobile Pu(IV) became the predominant oxidation state of the sorbed Pu. The observed stability of Pu(IV) on oxidizing surfaces (e.g., pyrolusite), is proposed to be due to the formation of a stable hydrolyzed Pu(IV) surface species. These findings have important implications in estimating the risk associated with the geological burial of radiological waste in areas containing Mn-bearing minerals, such as at the Yucca Mountain or the Hanford Sites, because plutonium will be predominantly in a much less mobile oxidation state (i.e., Pu(IV)) than previously suggested (i.e., Pu(V/VI)).
机译：使用同步加速器X射线显微光谱和显微成像技术以及超滤/溶剂萃取技术，对丝兰山凝灰岩和合成软锰矿（β-MnO2）悬浮液上的氧化态分布进行了测量。吸附在凝灰岩上的优先与氧化锰结合。对于丝兰山凝灰岩和合成软锰矿，Pu（IV）或Pu（V）最初被氧化成更多可移动的Pu（V / VI），但随着时间的流逝，更少移动的Pu（IV）成为吸附剂的主要氧化态。建议在氧化表面（如软锰矿）上观察到Pu（IV）的稳定性，是由于形成了稳定的水解Pu（IV）表面物质。这些发现对于估算含含锰矿物的地区（如尤卡山或汉福德遗址）与放射性废物地质掩埋有关的风险具有重要意义，因为p将主要处于活动性较低的氧化态（即，Pu（IV））比以前建议的值（即Pu（V / VI））高。

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