The Effects of Radiation Chemistry on Solvent Extraction: 1. Conditions in Acidic Solution and a Review of TBP Radiolysis
Solvent extraction is the most commonly used process scale separation technique for nuclear applications and it benefits from more than 60 years of research and development and proven experience at the industrial scale. Advanced solvent extraction processes for the separation of actinides and fission products from dissolved nuclear fuel are now being investigated worldwide by numerous groups (US, Europe, Russia, Japan etc.) in order to decrease the radiotoxic inventories of nuclear waste. While none of the advanced processes have yet been implemented at the industrial scale their development studies have sometimes reached demonstration tests at the laboratory scale. Most of the partitioning strategies rely on the following four separations: 1. Partitioning of uranium and/or plutonium from spent fuel dissolution liquors. 2. Separation of the heat generating fission products such as strontium and cesium. 3. Coextraction of the trivalent actinides and lanthanides. 4. Separation of the trivalent actinides from the trivalent lanthanides. Tributylphosphate (TBP) in the first separation is the basis of the PUREX, UREX and COEX processes, developed in Europe and the US, whereas monoamides as alternatives for TBP are being developed in Japan and India. For the second separation, many processes were developed worldwide, including the use of crown-ether extractants, like the FPEX process developed in the USA, and the CCD-PEG process jointly developed in the USA and Russia for the partitioning of cesium and strontium. In the third separation, phosphine oxides (CMPOs), malonamides, and diglycolamides are used in the TRUEX, DIAMEX and the ARTIST processes, respectively developed in US, Europe and Japan. Trialkylphosphine oxide(TRPO) developed in China, or UNEX (a mixture of several extractants) jointly developed in Russia and the USA allow all actinides to be co-extracted from acidic radioactive liquid waste. For the final separation, soft donor atom-containing ligands such as the bistriazinylbipyridines (BTBPs) or dithiophosphinic acids have been developed in Europe and China to selectively extract the trivalent actinides. However, in the TALSPEAK process developed in the USA, the separation is based on the relatively high affinity of aminopolycarboxylic acid complexants such as DTPA for trivalent actinides over lanthanides. In the DIDPA, SETFICS and the GANEX processes, developed in Japan and France, the group separation is accomplished in a reverse TALSPEAK process. A typical scenario is shown in Figure 1 for the UREX1a (Uranium Extraction version 1a) process. The initial step is the TBP extraction for the separation of recyclable uranium. The second step partitions the short-lived, highly radioactive cesium and strontium to minimize heat loading in the high-level waste repository. The third step is a group separation of the trivalent actinides and lanthanides with the last step being partitioning of the trivalent lanthanides from the actinides.
- Research Organization:
- Idaho National Lab. (INL), Idaho Falls, ID (United States)
- Sponsoring Organization:
- DOE - NE
- DOE Contract Number:
- DE-AC07-99ID-13727
- OSTI ID:
- 950044
- Report Number(s):
- INL/JOU-08-14292; SEIEDB; TRN: US0901947
- Journal Information:
- Solvent Extraction and Ion Exchange, Vol. 27, Issue 1; ISSN 0736-6299
- Country of Publication:
- United States
- Language:
- English
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Related Subjects
ACTINIDES
AFFINITY
CESIUM
DISSOLUTION
FISSION PRODUCTS
INVENTORIES
LIQUID WASTES
MIXTURES
NUCLEAR FUELS
PHOSPHINE OXIDES
PLUTONIUM
RADIATION CHEMISTRY
RADIOACTIVE WASTES
RADIOLYSIS
RARE EARTHS
SOLVENT EXTRACTION
SPENT FUELS
STRONTIUM
TALSPEAK PROCESS
URANIUM
WASTES
actinides
fission products
separation
solvent extraction
spent nuclear fuel