Pacific Northwest National Laboratory, 902 Battelle Blvd, Richland, WA, USA.
Pacific Northwest National Laboratory, 902 Battelle Blvd, Richland, WA, USA.
J Hazard Mater. 2018 Jan 5;341:238-247. doi: 10.1016/j.jhazmat.2017.07.055. Epub 2017 Jul 26.
A cementitious waste form, Cast Stone, is a possible candidate technology for the immobilization of low activity nuclear waste (LAW) at the Hanford site. This work focuses on the addition of getter materials to Cast Stone that can sequester Tc from the LAW, and in turn, lower Tc release from the Cast Stone. Two getters which produce different products upon sequestering Tc from LAW were tested: Sn(II) apatite (Sn-A) that removes Tc as a Tc(IV)-oxide and potassium metal sulfide (KMS-2) that removes Tc as a Tc(IV)-sulfide species, allowing for a comparison of stability of the form of Tc upon entering the waste form. The Cast Stone with KMS-2 getter had the best performance with addition equivalent to ∼0.08wt% of the total waste form mass. The observed diffusion (D) of Tc decreased from 4.6±0.2×10cm/s for Cast Stone that did not contain a getter to 5.4±0.4×10cm/s for KMS-2 containing Cast Stone. It was found that Tc-sulfide species are more stable against re-oxidation within getter containing Cast Stone compared with Tc-oxide and is the origin of the decrease in Tc D when using the KMS-2.
一种水硬胶凝废物形式,铸石,是一种可能的候选技术,用于在汉福德现场固定低活度核废物(LAW)。这项工作专注于向铸石中添加吸附加料,这些吸附加料可以将 Tc 从 LAW 中隔离出来,从而降低铸石中 Tc 的释放。测试了两种从 LAW 中隔离 Tc 时会产生不同产物的吸附加料:将 Tc 作为 Tc(IV)-氧化物去除的 Sn(II)磷灰石(Sn-A)和将 Tc 作为 Tc(IV)-硫化物物种去除的钾金属硫化物(KMS-2),从而可以比较进入废物形式时 Tc 的形态稳定性。具有 KMS-2 吸附加料的铸石的性能最佳,添加量相当于总废物形式质量的约 0.08wt%。在没有吸附加料的铸石中,Tc 的扩散(D)为 4.6±0.2×10cm/s,而含有 KMS-2 的铸石中,Tc 的扩散(D)为 5.4±0.4×10cm/s。结果发现,与 Tc-氧化物相比,Tc-硫化物物种在含有吸附加料的铸石中更不易被重新氧化,这是使用 KMS-2 时 Tc D 降低的原因。