Surface Modified, Collapsible Controlled Pore Glass Materials for Sequestration and Immobilization of Trivalent Metal Ions

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• 作者：Ilya A. Shkrob ; Angela R. Tisch ; Timothy W. Marin ; John V. Muntean ; Michael D. Kaminski ; A. Jeremy Kropf
• 刊名：Industrial & Engineering Chemistry Research
• 出版年：2011
• 出版时间：April 20, 2011
• 年：2011
• 卷：50
• 期：8
• 页码：4686-4696
• 全文大小：1043K
• 年卷期：v.50,no.8(April 20, 2011)
• ISSN：1520-5045

文摘

We report a one-pot method for sequestration, containment, and immobilization of lanthanide (Ln) ions from dilute aqueous waste streams. The approach is based on the use of collapsible, surface modified controlled pore glass (CPG) nanomaterials. We present several approaches for a single-step chemical modification of 3-propylaminated CPGs that yield highly efficient Ln-extracting materials with distribution coefficients exceeding 10000 mL/g. The resulting Ln complexes were studied using X-ray absorption, magnetic resonance, and time-resolved luminescence spectroscopies. One of these CPG materials involving an imidodi(methanediphosphate) moiety demonstrated high extraction efficacy, significant ionic radius sensitivity, and exceptional tolerance to masking agents, which is conducive to its use for removal of traces of radionuclide ions from aqueous TALSPEAK raffinate (trivalent actinide鈭抣anthanide separation by phosphorus reagent extraction from aqueous complexes process used in processing of spent nuclear fuel). The glass loaded with the extracted metal ions can be calcined and sintered at 1100 掳C, yielding fused material that buries Ln ions in the vitreous matrix. This processing temperature is significantly lower than 1700 掳C that is required for direct vitrification of lanthanide oxides in high-silica glass. X-ray absorption spectroscopy and acid leaching tests indicate that the immobilized ions are isolated and dispersed in the fused glass matrix. Thus, the method integrates Ln ions into the glass network. The resulting glass can be used for temporary storage or as the source of silica for production of borosilicate waste forms that are used for long-term disposal of high level radioactive waste.