Pacific Northwest National Laboratory, Richland, Washington, USA.
Environ Sci Technol. 2012 Nov 6;46(21):11610-7. doi: 10.1021/es3028956. Epub 2012 Oct 24.
Time-dependent reduction of PuO(2)(am) was studied over a range of pH values in the presence of aqueous Fe(II) and magnetite (Fe(3)O(4)) nanoparticles. At early time frames (up to 56 days) very little aqueous Pu was mobilized from PuO(2)(am), even though measured pH and redox potentials, coupled to equilibrium thermodynamic modeling, indicated the potential for significant reduction of PuO(2)(am) to relatively soluble Pu(III). Introduction of Eu(III) or Nd(III) to the suspensions as competitive cations to displace possible sorbed Pu(III) resulted in the release of significant concentrations of aqueous Pu. However, the similarity of aqueous Pu concentrations that resulted from the introduction of Eu(III)/Nd(III) to suspensions with and without magnetite indicated that the Pu was solubilized from PuO(2)(am), not from magnetite.
研究了在水相 Fe(II)和磁铁矿(Fe3O4)纳米粒子存在下,不同 pH 值条件下 PuO2(am) 的时间依赖性还原。在早期时间范围内(长达 56 天),从 PuO2(am)中很少有 Pu 被水相释放,尽管测量的 pH 值和氧化还原电位,结合平衡热力学模型,表明 PuO2(am)有很大的可能被还原为相对可溶性的 Pu(III)。将 Eu(III)或 Nd(III)引入悬浮液中作为竞争阳离子以取代可能被吸附的 Pu(III),导致大量的 Pu 被水相释放。然而,引入 Eu(III)/Nd(III)后悬浮液中 Pu 的水相浓度与不含磁铁矿的悬浮液相似,这表明 Pu 是从 PuO2(am)中而不是从磁铁矿中被溶解出来的。