Savannah River National Laboratory, Aiken, SC, 29808, United States.
Savannah River National Laboratory, Aiken, SC, 29808, United States.
J Environ Radioact. 2019 Nov;208-209:106017. doi: 10.1016/j.jenvrad.2019.106017. Epub 2019 Jul 17.
Silver (Ag)-based technologies are amongst the most common approaches to removing radioiodine from aqueous waste streams. As a result, a large worldwide inventory of radioactive AgI waste presently exits, which must be stabilized for final disposition. In this work, the efficacy of silver-impregnated granular activated carbon (Ag-GAC) to remove iodide (I), iodate (IO) and organo-iodine (org-I) from cementitious leachate was examined. In addition, cementitious materials containing I, IO, or org-I loaded Ag-GAC were characterized by iodine K-edge XANES and EXAFS to provide insight into iodine stability and speciation in these waste forms. The Ag-GAC was very effective at removing I and org-I, but ineffective at removing IO from slag-free grout leachate under oxic conditions. I or org-I removal was due to the formation of insoluble AgI or Ag-org-I on the Ag-GAC. When I-loaded Ag-GAC material was cured with slag-free and slag grouts, I was released from AgI to form a hydrated I species. Conversely, when org-I loaded Ag-GAC material was cured in the two grout formulations, no change was observed in the iodine speciation, indicating the org-I species remained bound to the Ag. Because little IO was bound to the Ag-GAC, it was not detectable in the grout. Thus, grout formulation and I speciation in the waste stream can significantly influence the effectiveness of the long-term disposal of radioiodine associated with Ag-GAC in grout waste forms.
银(Ag)基技术是从水中废物流中去除放射性碘的最常见方法之一。因此,目前全世界都有大量的放射性碘化银废物库存,必须对其进行稳定化处理,以进行最终处置。在这项工作中,研究了载银颗粒活性炭(Ag-GAC)从水泥浸出液中去除碘化物(I)、碘酸盐(IO)和有机碘(org-I)的效果。此外,还通过碘 K 边 XANES 和 EXAFS 对含有 I、IO 或 org-I 的载银活性炭的水泥材料进行了表征,以深入了解这些废物形式中碘的稳定性和形态。Ag-GAC 非常有效地去除 I 和 org-I,但在有氧条件下对无渣灌浆浸出液中的 IO 无效。I 或 org-I 的去除是由于在 Ag-GAC 上形成了不溶性 AgI 或 Ag-org-I。当 I 负载的 Ag-GAC 材料与无渣和渣灌浆固化时,I 从 AgI 中释放出来形成水合 I 物种。相反,当 org-I 负载的 Ag-GAC 材料在两种灌浆配方中固化时,碘的形态没有观察到变化,表明 org-I 物种仍然与 Ag 结合。由于很少有 IO 与 Ag-GAC 结合,因此在灌浆中无法检测到。因此,灌浆配方和废物流中的 I 形态会显著影响与 Ag-GAC 相关的放射性碘在灌浆废物形式中的长期处置的有效性。