Authors:
Meng Wei Institute of Nuclear and New Energy Technology, Tsinghua University, Beijing, 100084 China

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Qian’ge He Institute of Nuclear and New Energy Technology, Tsinghua University, Beijing, 100084 China

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Xiaogui Feng Institute of Nuclear and New Energy Technology, Tsinghua University, Beijing, 100084 China

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Jing Chen Institute of Nuclear and New Energy Technology, Tsinghua University, Beijing, 100084 China

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Abstract  

The crystal structure, melting range, decomposition temperature, solubilities in aqueous and organic phase, and distribution ratio in biphase system of N,N,N′,N′-tetramethyl diglycolamide (TMDGA) have been studied in the present work. Water-soluble TMDGA with very low solubility in kerosene or 30 % trialkyl phosphine (TRPO)/kerosene meets the primary requirement to act as the stripping agent in TRPO process which has been developed for actinides partitioning from high level waste. Slope analysis, electrospray ionization mass spectrometry (ESI–MS) and spectrophotometric titration indicate that in weak and moderate acidic aqueous solution, up to three TMDGA molecules form complexes with Zr4+, trivalent lanthanides (Ln3+), trivalent actinides (An3+) or tetravalent actinides (An4+). Their complex formation constants determined by liquid–liquid extraction method follow the order predicted by the electrostatic model of 4f and 5f elements and the covalent model of 4d transition elements: Ln3+ ~ An3+ < An4+ ≪ Zr4+. Hydrolysis of actinide cations, especially An4+, in the media of low acidity, reduces the complexation stability. In addition, the effect of aqueous acidity and temperature has been investigated. No obvious influence of temperature on Np4+ complexes has been found. However, the influence on Am3+ and Pu4+, especially on their 1:1 or 1:2 complex species with TMDGA, is relatively considerable. Strong affinity of TMDGA to An3+ and An4+ implies that TMDGA has potential to strip An3+ and An4+ from TRPO.

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Journal of Radionalytical and Nuclear Chemistry
Language English
Size A4
Year of
Foundation
1968
Volumes
per Year
1
Issues
per Year
12
Founder Akadémiai Kiadó
Founder's
Address
H-1117 Budapest, Hungary 1516 Budapest, PO Box 245.
Publisher Akadémiai Kiadó
Springer Nature Switzerland AG
Publisher's
Address
H-1117 Budapest, Hungary 1516 Budapest, PO Box 245.
CH-6330 Cham, Switzerland Gewerbestrasse 11.
Responsible
Publisher
Chief Executive Officer, Akadémiai Kiadó
ISSN 0236-5731 (Print)
ISSN 1588-2780 (Online)