Ultra-Efficient Americium/Lanthanide Separation through Oxidation State Control

Wang，Zhipeng1; Lu，Jun Bo2; Dong，Xue1; Yan，Qiang1; Feng，Xiaogui1; Hu，Han Shi3; Wang，Shuao4; Chen，Jing1; Li，Jun2,3; Xu，Chao1

2022

10.1021/jacs.2c00594

Journal of the American Chemical Society   影响因子和分区

0002-7863

1520-5126

Lanthanide/actinide separation is a worldwide challenge for atomic energy and nuclear waste treatment. Separation of americium (Am), a critical actinide element in the nuclear fuel cycle, from lanthanides (Ln) is highly desirable for minimizing the long-term radiotoxicity of nuclear waste, yet it is extremely challenging given the chemical similarity between trivalent Am(III) and Ln(III). Selective oxidation of Am(III) to a higher oxidation state (OS) could facilitate this separation, but so far, it is far from satisfactory for practical application as a result of the unstable nature of Am in a high OS. Herein, we find a novel strategy to generate stable pentavalent Am (Am(V)) through coordination of Am(III) with a diglycolamide ligand and oxidation with Bi(V) species in the presence of an organic solvent. This strategy leads to efficient stabilization of Am(V) and an extraordinarily high separation factor (>104) of Am from Ln through one single contact in solvent extraction, thereby opening a new avenue to study the high-OS chemistry of Am and fulfill the crucial task of Ln/Am separation in the nuclear fuel cycle. The synergistic coordination and oxidation process is found to occur in the organic solvent, and the mechanism has been well elucidated by quantum-theoretical modeling.

SCI ; EI

英语

NI论文

通讯

National Natural Science Foundation of China[21790372,21822606,22033005] ; Beijing Natural Science Foundation[JQ20041] ; Science Challenge Project[TZ2016004] ; Guangdong Provincial Key Laboratory of Catalysis[2020B121201002]

Chemistry

Chemistry, Multidisciplinary

WOS:000790698300030

AMER CHEMICAL SOC

20221511960821

Americium ; Bismuth compounds ; Organic solvents ; Oxidation ; Radioactive wastes ; Rare earth elements ; Solvent extraction ; Waste treatment

Industrial Wastes Treatment and Disposal:452.4 ; Rare Earth Metals:547.2 ; Radioactive Materials, General:622.1 ; Radioactive Wastes:622.5 ; Chemical Reactions:802.2 ; Chemical Operations:802.3 ; Chemical Agents and Basic Industrial Chemicals:803 ; Organic Compounds:804.1

2-s2.0-85127879318

Scopus

1.Institute of Nuclear and New Energy Technology,Tsinghua University,Beijing,100084,China
2.Department of Chemistry,Southern University of Science and Technology,Shenzhen,518055,China
3.Department of Chemistry,Key Laboratory of Organic Optoelectronics and Molecular Engineering,The Ministry of Education,Tsinghua University,Beijing,100084,China
4.State Key Laboratory of Radiation Medicine and Protection,School for Radiological and Interdisciplinary Sciences,Soochow University,Suzhou,215123,China

Wang，Zhipeng,Lu，Jun Bo,Dong，Xue,et al. Ultra-Efficient Americium/Lanthanide Separation through Oxidation State Control[J]. Journal of the American Chemical Society,2022,144(14):6383-6389.

Wang，Zhipeng.,Lu，Jun Bo.,Dong，Xue.,Yan，Qiang.,Feng，Xiaogui.,...&Xu，Chao.(2022).Ultra-Efficient Americium/Lanthanide Separation through Oxidation State Control.Journal of the American Chemical Society,144(14),6383-6389.

Wang，Zhipeng,et al."Ultra-Efficient Americium/Lanthanide Separation through Oxidation State Control".Journal of the American Chemical Society 144.14(2022):6383-6389.