Selective separation of rare earth, Sr, Mo, and Zr from simulated raffinate of uranium/plutonium co-purification process

Abstract

Spent fuel contains many elements including those that are radioactive. Separation and recovery of these substances have been challenging. This paper presents an efficient strategy for stepwise separation of the rare earth, strontium, molybdenum, and zirconium from the simulated raffinate of a uranium/plutonium co-purification process. This strategy employed three extractants with different metal ion selectivity, and cyclohexanediamine tetraacetic acid (CDTA) was introduced as a complexing agent to inhibit the extraction of Zr(IV) and precious metals. The recovery efficiency of all the rare earth elements was more than 97 % through the three-stage extraction, with N,N,N′,N′-tetranoctyl-diglycolamide (TODGA) as the extractant and N,N-dibutyloctanamide (DBOA) as the phase modifiers. Sr(II) was selectively recovered using N,N,N′,N′-tetracyclohexyl-diglycolamide (TCHDGA). A bisphosphonic acid extractant, N,N-hexadecylamine bis (methylene phenylphosphonic acid) (HADMPPA), was designed and synthesized for the selective separation of Zr(IV) and Mo(VI). The separation conditions of the recovered elements from other elements in each step were systematically examined. Moreover, the mechanism of the extraction reaction was investigated using FTIR spectroscopy, the slope method, and the equimolar series method. To our knowledge, this is the first time that four groups of major elements have been sequencially separated from the simulated high-level waste liquid in one process. This work could contribute to nuclear fuel reprocessing as well as the sustainable development of nuclear energy.