Department of Chemistry, The University of North Carolina at Chapel Hill, Chapel Hill, NC 27599, USA.
Idaho National Laboratory, Aqueous Separations and Radiochemistry Department, Idaho Falls, ID, USA.
Science. 2015 Nov 6;350(6261):652-5. doi: 10.1126/science.aac9217.
Selective oxidation of trivalent americium (Am) could facilitate its separation from lanthanides in nuclear waste streams. Here, we report the application of a high-surface-area, tin-doped indium oxide electrode surface-derivatized with a terpyridine ligand to the oxidation of Am(III) to Am(V) and Am(VI) in nitric acid. Potentials as low as 1.8 volts (V) versus the saturated calomel electrode were applied, 0.7 V lower than the 2.6 V potential for one-electron oxidation of Am(III) to Am(IV) in 1 molar acid. This simple electrochemical procedure provides a method to access the higher oxidation states of Am in noncomplexing media for the study of the associated coordination chemistry and, more important, for more efficient separation protocols.
三价镅的选择性氧化可以促进其与核废料流中的镧系元素分离。在这里,我们报告了一种高表面积、锡掺杂氧化铟电极表面的应用,该电极表面用三吡啶配体衍生化,用于在硝酸中氧化 Am(III)为 Am(V)和 Am(VI)。与饱和甘汞电极相比,施加的电位低至 1.8 伏(V),比在 1 摩尔酸中 Am(III)单电子氧化为 Am(IV)的 2.6 V 电位低 0.7 V。这种简单的电化学方法提供了一种在非配位介质中获得 Am 更高氧化态的方法,用于研究相关的配位化学,更重要的是,用于更有效的分离方案。