Pu Coexists in Three Oxidation States in a Borosilicate Glass: Implications for Pu Solubility

被引：18

作者：

Bahl, Sebastian ^{[1
]}

Peuge, Sylvain ^{[2
]}

Pidchenko, Ivan ^{[1
]}

Pruessmarm, Tim ^{[1
,3
,4
]}

Rothe, Joerg ^{[1
]}

Dardenne, Kathy ^{[1
]}

Delrieu, Julien ^{[2
]}

Fellhauer, David ^{[1
]}

Jegou, Christophe ^{[2
]}

Geckeis, Horst ^{[1
]}

Vitova, Tonya ^{[1
]}

机构：

[1] Karlsruhe Inst Technol, Inst Nucl Waste Disposal, POB 3640, D-76021 Karlsruhe, Germany

[2] CEA Valrho Marcoule, Inst Chim Separat Marcoule, UMR 5257, BP 17171, F-30207 Bagnols Sur Ceze, France

[3] Karlsruhe Inst Technol, Inst Catalysis Res & Technol IKFT, POB 3640, D-76021 Karlsruhe, Germany

[4] Karlsruhe Inst Technol, Inst Chem Technol & Polymer Chem ITCP, Engesserstr 20, D-76131 Karlsruhe, Germany

来源：

INORGANIC CHEMISTRY | 2017年 / 56卷 / 22期

关键词：

X-RAY-ABSORPTION; CERAMIC WASTE FORMS; PLUTONIUM SOLUBILITY; NEUTRON-DIFFRACTION; NUCLEAR-WASTE; HR-XANES; SPECTROSCOPY; URANIUM; SYSTEMS; SPECIATION;

D O I：

10.1021/acs.inorgchem.7b02118

中图分类号：

O61 [无机化学];

学科分类号：

070301 ; 081704 ;

摘要：

Pu(III), Pu(IV), and a higher oxidation state of Pu, likely Pu(VI), are for the first time characterized simultaneously present in a borosilicate glass using Pu M-5 edge high energy resolution X-ray absorption near edge structure (HR-XANES) technique. We illustrate that the method can be very efficiently used to determine Pu oxidation states, which control the solubility limit of Pu in a glass matrix. HR-XANES results show that the addition of excess Si3N4 is not,1 sufficient for complete reduction of Pu to Pu(III), which has a relatively high solubility limit (9-22 wt % Pu) due to its network-modifying behavior in glasses. We provide evidence that the initially added Pu(VI) might be partly preserved during vitrification at 1200/1400 degrees C in Ar atmosphere. Pu(VI) could be very advantageous for vitrification of Pu-rich wastes, since it might reach solubility limits of 40 wt % comparable to U(VI).

引用

页码：13982 / 13990

页数：9

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