Collaborative Research: Crystal Chemistry of U,Th and Other Radionuclides in Apatite: Environmental and Geochemical Implications

合作研究:磷灰石中 U、Th 和其他放射性核素的晶体化学:环境和地球化学影响

基本信息

  • 批准号:
    0409422
  • 负责人:
  • 金额:
    --
  • 依托单位:
  • 依托单位国家:
    美国
  • 项目类别:
    Standard Grant
  • 财政年份:
    2004
  • 资助国家:
    美国
  • 起止时间:
    2004-07-01 至 2008-06-30
  • 项目状态:
    已结题

项目摘要

Apatite, Ca10(PO4)6(F,OH,Cl)2, can accommodate numerous substituents, including many radionuclides of environmental concern (90Sr, 90Y, REE, U and Th). Scores of studies have focused on the crystal chemistry of substituents in apatite; surprisingly, however, little is known about the mechanisms of incorporation and the structural response of apatite to U and Th, despite the fact that the presence of these elements in this mineral has been used in geochronologic and petrogenetic studies for decades. This two-part study focuses on fundamental mineralogical and geochemical aspects of U and Th incorporation in apatite and implications for apatite as a solid nuclear-waste form and a metal sequestration agent.Interest in apatite as a potential solid waste form for radionuclides is based on: 1) its high affinity for elements of environmental concern; 2) its thermal annealing properties; and 3) its relatively low solubility in most surface environments. Fundamental to our understanding of radionuclide retention and release are crystal chemical parameters such as site preference, oxidation state, and structural distortions/symmetry-breaking created by substituents such as U and Th; surprisingly, the crystal chemistry of their substitution in apatite is unknown. Part I of this study is to determine these structural parameters in a variety of natural and synthetic apatites with substituent U and Th. This will be accomplished through complementary use of crystal synthesis, single crystal X-ray diffraction, and X-ray absorption spectroscopy.Part II of this study focuses on the role of precursor calcium phosphate phases on the uptake of U, Th and other metals and the fate of these contaminants through structural transformations in these sequestered states. Use of apatite formation in contaminated sediments (sometimes called phosphate-induced metal stabilization, PIMS) is a new and promising method for metal sequestration (including radionuclides) and environmental remediation. Numerous experimental studies of apatite formation under the temperature and pH conditions found in sediments and soils indicate the formation of precursor phases such as OCP (octacalcium phosphate) and brushite is essential to the process. This fundamental aspect of apatite formation under surface conditions has not been addressed in the context of metal sequestration and fate. This has critical bearing on the effective use of apatite for metal immobilization and our understanding of the role of phosphate in the global geochemical cycling of heavy metals. Part II of the study will be accomplished through a combination of 1) low-temperature synthesis in the presence of U, Th and other metals with in situ (time-resolved synchrotron X-ray diffraction) and 2) ex situ chemical and structural analyses including Rietveld structure analysis and X-ray absorption spectroscopy.This work has broad environmental implications (heavy-metal and radionuclide sequestration) that are of immense importance to a society that generates radioactive waste. The research will include the participation and education of undergraduate and graduate students, as well as support the ongoing research of a Postdoctoral Fellow at Miami University.
磷灰石 Ca10(PO4)6(F,OH,Cl)2 可容纳多种取代基,包括许多环境问题的放射性核素(90Sr、90Y、REE、U 和 Th)。许多研究都集中在磷灰石取代基的晶体化学上。然而,令人惊讶的是,人们对磷灰石对 U 和 Th 的结合机制和结构响应知之甚少,尽管这种矿物中这些元素的存在已被用于地质年代学和岩石成因研究数十年。这项由两部分组成的研究重点关注磷灰石中 U 和 Th 掺入的基本矿物学和地球化学方面,以及磷灰石作为固体核废物形式和金属封存剂的影响。对磷灰石作为放射性核素的潜在固体废物形式的兴趣基于:1)其对环境关注元素的高亲和力; 2) 其热退火性能; 3) 在大多数表面环境中其溶解度相对较低。我们理解放射性核素保留和释放的基础是晶体化学参数,例如位点偏好、氧化态以及由 U 和 Th 等取代基产生的结构扭曲/对称性破坏;令人惊讶的是,它们在磷灰石中的取代的晶体化学性质尚不清楚。本研究的第一部分是确定各种带有 U 和 Th 取代基的天然和合成磷灰石的结构参数。这将通过晶体合成、单晶 X 射线衍射和 X 射线吸收光谱的互补使用来实现。本研究的第二部分重点关注前体磷酸钙相对 U、Th 和其他金属吸收的作用,以及这些污染物通过这些隔离状态的结构转变的命运。在受污染的沉积物中利用磷灰石形成(有时称为磷酸盐诱导金属稳定化,PIMS)是一种新的、有前景的金属封存(包括放射性核素)和环境修复方法。在沉积物和土壤中发现的温度和 pH 条件下磷灰石形成的大量实验研究表明,OCP(磷酸八钙)和透钙磷石等前体相的形成对于该过程至关重要。表面条件下磷灰石形成的这一基本方面尚未在金属封存和命运的背景下得到解决。这对于有效利用磷灰石进行金属固定以及我们对磷酸盐在全球重金属地球化学循环中的作用的理解具有至关重要的影响。该研究的第二部分将通过 1) 在 U、Th 和其他金属存在下的原位低温合成(时间分辨同步加速器 X 射线衍射)和 2)非原位化学和结构分析(包括 Rietveld 结构分析和 X 射线吸收光谱)来完成。这项工作具有广泛的环境影响(重金属和放射性核素封存),意义重大 对于产生放射性废物的社会具有重要意义。该研究将包括本科生和研究生的参与和教育,并支持迈阿密大学博士后研究员正在进行的研究。

项目成果

期刊论文数量(0)
专著数量(0)
科研奖励数量(0)
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Christopher Cahill其他文献

Resonant inelastic X-ray scattering tools to count 5 f electrons of actinides and probe bond covalency
用于计数锕系元素 5 f 电子并探测键共价性的共振非弹性 X 射线散射工具
  • DOI:
    10.1038/s41467-024-54574-7
  • 发表时间:
    2025-02-10
  • 期刊:
  • 影响因子:
    15.700
  • 作者:
    Bianca Schacherl;Michelangelo Tagliavini;Hanna Kaufmann-Heimeshoff;Jörg Göttlicher;Marinella Mazzanti;Karin Popa;Olaf Walter;Tim Pruessmann;Christian Vollmer;Aaron Beck;Ruwini S. K. Ekanayake;Jacob A. Branson;Thomas Neill;David Fellhauer;Cedric Reitz;Dieter Schild;Dominique Brager;Christopher Cahill;Cory Windorff;Thomas Sittel;Harry Ramanantoanina;Maurits W. Haverkort;Tonya Vitova
  • 通讯作者:
    Tonya Vitova

Christopher Cahill的其他文献

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{{ truncateString('Christopher Cahill', 18)}}的其他基金

CAREER: Design of Organic-Inorganic Hybrid Lanthanide and Actinide Materials
职业:有机-无机杂化镧系元素和锕系元素材料的设计
  • 批准号:
    0348982
  • 财政年份:
    2004
  • 资助金额:
    --
  • 项目类别:
    Continuing Grant
MRI: Acquisition of an Imaging Plate Based X-Ray Diffractometer for Use in a Materials Chemistry Research and Education Program
MRI:购买基于成像板的 X 射线衍射仪,用于材料化学研究和教育项目
  • 批准号:
    0419754
  • 财政年份:
    2004
  • 资助金额:
    --
  • 项目类别:
    Standard Grant

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