Lukens Wayne W, Shuh David K, Schroeder Norman C, Ashley Kenneth R
Chemical Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720, USA.
Environ Sci Technol. 2004 Jan 1;38(1):229-33. doi: 10.1021/es034318d.
Immobilization of the high-level nuclear waste stored at the Hanford Reservation has been complicated by the presence of soluble, lower-valent technetium species. Previous work by Schroeder and Blanchard has shown that these species cannot be removed by ion-exchange and are difficult to oxidize. The Tc K-edge XANES spectra of the species in Tanks SY-101 and SY-103 were reported by Blanchard, but they could not be assigned to any known technetium complex. We report that the XANES spectra are most likely those of Tc(I)-carbonyl species, especially fac-Tc(CO)3(gluconate)(2-). This is further supported by EXAFS and 99Tc-NMR studies in nonradioactive simulants of these tank wastes.
存储在汉福德保留地的高放核废料的固化因可溶性低价锝物种的存在而变得复杂。施罗德和布兰查德之前的研究表明，这些物种无法通过离子交换去除，且难以氧化。布兰查德报告了SY - 101和SY - 103号罐中这些物种的锝K边X射线吸收近边结构（XANES）光谱，但无法将它们归属于任何已知的锝配合物。我们报告这些XANES光谱很可能是Tc(I)-羰基物种的光谱，尤其是面式-Tc(CO)3(葡萄糖酸盐)(2-)的光谱。这些罐式废料的非放射性模拟物的扩展X射线吸收精细结构（EXAFS）和99Tc-核磁共振（NMR）研究进一步支持了这一结论。
