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Interstitial Incorporation of Plutonium into a Low-Dimensional Potassium Borate

机译：sti向低维硼酸钾中的间隙掺入

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摘要

The molten boric acid flux reaction of PuBr3 with KBO2 at 200 °C results , in the formation of large light-yellow crystals of K[BsO7(OH)2]-H2O:Pu4*. Single-crystal X-ray diffraction experiments on the Pu-doped K[B5O7(OH)2] • H2O demonstrate two features: (1) K[B5O7(OH)2]-H2O:Pu adopts a one-dimensional borate chain structure with void spaces between the chains. (2) The doping plutonium atoms do not reside on the potassium sites. The latter are not fully occupied. Both laser-ablation inductively coupled plasma mass spectrometry (LA-1CP-MS) and energy-dispersive spectrometry analyses indicate that plutonium atoms are uniformly distributed in crystals of K[BSO7(OH)2] • H2O with an atomic K:Pu ratio of approximately 65:1 measured by LA-ICP-MS. UV-vis-NIR spectra taken from both freshly made and one day old crystals show that the plutonium present within the crystals is predominantly characterized by Pu(IV). A small amount of Pu(HI) is also present initially, but slowly oxidized to Pu(IV) via interaction with oxygen in the air. X-ray absorption near-edge structure and extended X-ray absorption fine structure spectroscopic measurements confirm that plutonium is mainly present as a form similar to that of a PuO2 cluster. The combined results suggest that the clusters containing Pu(IV) ions are uniformly distributed in the void spaces between the borate chains.
机译：PuBr3与KBO2在200°C时发生熔融硼酸助熔剂反应，形成K [BsO7（OH）2] -H2O：Pu4 *的浅黄色大晶体。 Pu掺杂的K [B5O7（OH）2]•H2O的单晶X射线衍射实验显示两个特征：（1）K [B5O7（OH）2] -H2O：Pu采用一维硼酸盐链结构链之间有空隙。 （2）p原子不存在于钾原子上。后者没有完全占据。激光烧蚀电感耦合等离子体质谱（LA-1CP-MS）和能量色散质谱分析均表明，atoms原子均匀分布在K [BSO7（OH）2]•H2O晶体中，其K：Pu原子比为通过LA-ICP-MS测得约为65：1。从新鲜晶体和一天后的晶体中获得的UV-vis-NIR光谱表明，晶体中存在的p主要由Pu（IV）表征。最初还存在少量的Pu（HI），但通过与空气中的氧气相互作用而缓慢氧化为Pu（IV）。 X射线吸收近边缘结构和扩展的X射线吸收精细结构光谱测量结果证实，mainly主要以与PuO2团簇相似的形式存在。综合结果表明，含Pu（IV）离子的团簇均匀分布在硼酸盐链之间的空隙中。

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  • 来源
    《Environmental Science & Technology》 |2011年第21期|p.9457-9463|共7页
  • 作者

    Shuao Wang; Juan Diwu; Antonio Simonetti; Corwin H. Booth; Thomas E. Albrecht-Schmitt;

  • 作者单位

    Departments of Civil Engineering and Geological Sciences and of Chemistry and Biochemistry, University of Notre Dame,Notre Dame, Indiana 46556, United States;

    Departments of Civil Engineering and Geological Sciences and of Chemistry and Biochemistry, University of Notre Dame,Notre Dame, Indiana 46556, United States;

    Departments of Civil Engineering and Geological Sciences and of Chemistry and Biochemistry, University of Notre Dame,Notre Dame, Indiana 46556, United States;

    Chemical Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States;

    Departments of Civil Engineering and Geological Sciences and of Chemistry and Biochemistry, University of Notre Dame,Notre Dame, Indiana 46556, 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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