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XAFS investigation of polyamidoxime-bound uranyl contests the paradigm from small molecule studies

机译：XAFS研究与聚酰胺酰胺结合的铀酰竞争了小分子研究的范式

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摘要

Limited resource availability and population growth have motivated interest in harvesting valuable metals from unconventional reserves, but developing selective adsorbents for this task requires structural knowledge of metal binding environments. Amidoxime polymers have been identified as the most promising platform for large-scale extraction of uranium from seawater. However, despite more than 30 years of research, the uranyl coordination environment on these adsorbents has not been positively identified. We report the first XAFS investigation of polyamidoxime-bound uranyl, with EXAFS fits suggesting a cooperative chelating model, rather than the tridentate or eta(2) motifs proposed by small molecule and computational studies. Samples exposed to environmental seawater also display a feature consistent with a mu(2)-oxo-bridged transition metal in the uranyl coordination sphere, suggesting in situ formation of a specific binding site or mineralization of uranium on the polymer surface. These unexpected findings challenge several long-held assumptions and have significant implications for development of polymer adsorbents with high selectivity.
机译：有限的资源可用性和人口增长激发了人们从非常规储藏中收获有价值的金属的兴趣，但是为该任务开发选择性吸附剂需要金属结合环境的结构知识。 mid胺肟聚合物已被认为是从海水中大规模萃取铀的最有希望的平台。但是，尽管进行了30多年的研究，但尚未明确确定这些吸附剂上的铀酰配位环境。我们报告了首次XAFS调查的聚酰胺酰胺结合的铀酰，与EXAFS拟合表明合作的螯合模型，而不是由小分子和计算研究提出的三齿或eta（2）图案。暴露于环境海水中的样品还显示出与铀酰配位域中的mu（2）-氧代桥联过渡金属一致的特征，表明在聚合物表面上原位形成特定的结合位点或铀矿化。这些出乎意料的发现挑战了几个长期存在的假设，对开发具有高选择性的聚合物吸附剂具有重要意义。

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  • 来源
    《Energy & environmental science》 |2016年第2期|448-453|共6页
  • 作者

    Abney C. W.; Mayes R. T.; Piechowicz M.; Lin Z.; Bryantsev V. S.; Veith G. M.; Dai S.; Lin W.;

  • 作者单位

    Univ Chicago, 929 East 57th St, Chicago, IL 60637 USA|Oak Ridge Natl Lab, POB 2008, Oak Ridge, TN 37831 USA;

    Oak Ridge Natl Lab, POB 2008, Oak Ridge, TN 37831 USA;

    Univ Chicago, 929 East 57th St, Chicago, IL 60637 USA;

    Univ Chicago, 929 East 57th St, Chicago, IL 60637 USA;

    Oak Ridge Natl Lab, POB 2008, Oak Ridge, TN 37831 USA;

    Oak Ridge Natl Lab, POB 2008, Oak Ridge, TN 37831 USA;

    Oak Ridge Natl Lab, POB 2008, Oak Ridge, TN 37831 USA;

    Univ Chicago, 929 East 57th St, Chicago, IL 60637 USA;

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