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Superparamagnetic bi-functional composite bead for the thermal ionization mass spectrometry of plutonium(IV) ions

机译：用于钚（IV）离子的热电电离质谱法的超顺磁性双官能复合珠

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Single resin bead-based thermal ionization mass spectrometry (TIMS) offers numerous advantages for Pu(IV) determinations in complex aqueous samples. These include removal of the matrix and interfering ions by a one-step process, selective preconcentration of Pu(IV) ions with a high chemical recovery, transportation without heavy shielding, avoiding the possibility of cross-contamination, and acting as a point source. The single-bead TIMS method reported in literature is based on an anion-exchange resin that lacks sorption-selectivity toward Pu(IV) ions, and where the beads are not easily retrievable from a large volume sample. Therefore, silica-coated superparamagnetic Fe3O4 embedded functionalized porous poly(ethersulfone) (PES) beads were developed for Pu(IV) preconcentration and analysis by TIMS. The beads were functionalized with a phosphate bearing monomer along with or without a quaternary ammonium bearing monomer by UV-induced surface grafting. Since the beads were used in a highly acidic solution, the Fe3O4 nanoparticles were protected with a silica coating formed by the hydrolysis and condensation of tetraethoxysilane. The PES porous beads were prepared by a phase inversion method. The monomers used for UV-grafting were 2-hydroxyethyl methacrylate ester and (3-acrylamidopropyl) trimethylammonium chloride. The functionalized beads were characterized by scanning electron microscopy, energy dispersive analysis, and vibrating sample magnetometry. The sorption studies indicated that the bi-functionalized PES beads consisting of phosphate and quaternary ammonium groups not only have a higher distribution coefficient (K-d) for Pu(IV) but also high selectivity toward Pu(IV) ions in the presence of a large excess of U(VI) ions (K-d(Pu(VI))/K-d(U(IV)) = 11.5). The phosphate-functionalized PES beads showed comparable selectivity (K-d(Pu(VI))/K-d(U(IV)) = 9.1), but a lower K-d value for Pu(IV). The quaternary ammonium-functionalized PES beads were found to have lower selectivity and Kd values toward Pu(IV) ions. The analytical performance of single bi-functionalized bead-based TIMS for the determination of Pu(IV) using isotope dilution was compared with the solution-based TIMS, validated using the Pu isotopic standard reference material NIST SRM-947 and applied to real samples such as dissolver solutions and soil leach liquors.
机译：单基于珠树脂热电离质谱（TIMS）提供了许多优势，为复杂的含水样品中的普（IV）测定。这些包括具有高化学回收去除矩阵的和干扰的离子通过一步法，选择性富集浦（IV）离子的，运输而不重屏蔽，避免了交叉污染的可能性，并作为一个点光源。单珠TIMS方法在文献中报道是基于缺少朝向莆吸附选择性（IV）离子的阴离子交换树脂，并且其中所述珠子是不容易从大体积样品检索。因此，嵌入的二氧化硅涂布的超顺磁性的Fe3O4官能多孔聚（醚砜）（PES）珠浦开发（IV）富集和分析由TIMS。珠用沿着具有或不具有通过UV诱导的表面接枝的季铵轴承单体磷酸酯轴承单体官能化。由于珠粒在强酸性溶液中使用的，四氧化三铁纳米颗粒与由水解和四乙氧基硅烷的缩合形成的二氧化硅涂层保护。的PES多孔珠通过相转化方法制备。用于UV-接枝的单体是2-羟乙基甲基丙烯酸酯和（3-丙烯酰胺丙基）三甲基氯化铵。通过扫描电子显微镜，能量色散分析，和振动样品磁强计的官能化珠进行了表征。吸附研究表明，该双官能化PES珠自由磷酸和季铵基团的不仅有浦（IV），但也高的选择性更高的分配系数（KD）朝向浦（IV）离子在大量过量的存在下铀（VI）离子（KD（浦（VI））/ KD（U（IV））= 11.5）。磷酸官能PES珠显示出相当的选择性（K-d（浦（VI））/ K-d（U（IV））= 9.1），但对于浦较低K-d值（IV）。被发现的季铵官能化的PES颗粒具有较低选择性和朝向浦（IV）离子的Kd值。单个双官能的基于珠的TIMS的用于使用同位素稀释浦（IV）的测定的分析性能与基于溶液的TIMS进行比较，使用普同位素标准参考物质NIST SRM-947验证并应用于这种实际样品作为溶解溶液和土壤浸出液。

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  • 来源
    《RSC Advances》 |2016年第4期|共9页
  • 作者

    Paul Sumana; Pandey Ashok K.; Shah Raju V.; Alamelu D.; Aggarwal Suresh K.;

  • 作者单位

    Bhabha Atom Res Ctr Div Fuel Chem Bombay 400085 Maharashtra India;

    Bhabha Atom Res Ctr Div Radiochem Bombay 400085 Maharashtra India;

    Bhabha Atom Res Ctr Div Fuel Chem Bombay 400085 Maharashtra India;

    Bhabha Atom Res Ctr Div Fuel Chem Bombay 400085 Maharashtra India;

    Bhabha Atom Res Ctr Div Fuel Chem Bombay 400085 Maharashtra India;

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  • 正文语种 eng
  • 中图分类 化学;
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