Np(Ⅴ)吸附于纤铁矿/水界面的扩展X射线吸收精细结构(EXAFS)分析

    Neptunium(Ⅴ) Adsorption to γ-FeOOH/Water Interface: EXAFS Analysis

    • 摘要: 本工作采用原位扩展X射线吸收精细结构(EXAFS)能谱首次揭示了Np(Ⅴ)吸附于合成纤铁矿(γ-FeOOH)表面的化学形态。Np L边EXAFS分析结果显示Np(Ⅴ)以五价镎酰离子吸附于γ-FeOOH,未发现多核络合物与表面沉淀。傅里叶转化结果在约3 Å(1Å=0.1 nm )附近的能峰可归于Np-Fe配位层,证明了Np(Ⅴ)γ-FeOOH形成了内层吸附的单一形态表面络合物。所得分析结果与Np(Ⅴ)在相似构成的含铁矿物上的吸附形态结果进行了比较,进一步确认了Np-Fe、Np-O等关键配位层的存在。然而,还需要更多设计良好的EXAFS实验来确认是否存在Np-C配位层,以确认纤铁矿界面是否存在Np碳酸根表面络合物。

       

      Abstract: This work apply in situ extended X-ray absorption fine structure(EXAFS) to reveal sorption speciation of Np(Ⅴ) on synthetic lepidocrocite(γ-FeOOH). Np L-edge EXAFS analysis shows that Np(Ⅴ) is absorbed on γ-FeOOH as neptunyl ion, with no observations of multinuclear surface complexes or surface precipitates. The Fourier transform(FT) magnitude of the EXAFS also shows an obvious peak feature at about 3 Å (1 Å =0.1 nm), that can be attributed to a Np-Fe scattering path, consistent with the formation of an inner sphere Np(Ⅴ)-lepidocrocite surface complex. The EXAFS FT results were compared between Np(Ⅴ) speciation on difference iron mineral phases with similar compositions. However, it remains a question whether or not a Np-C coordination exists, indicating the possible presence of Np(Ⅴ)/carbonate species on the lepidocrocite surface. Additional studies are needed, particularly well-designed EXAFS studies, to answer this question and verify the identity of the surface complex.

       

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