Hanford, recovery

An overview is given of plutonium process chemistry used at the U. S. Department of Energy Hanford, Los Alamos National Laboratory, Rocky Flats, and Savannah River sites, with particular emphasis on solution chemistry involved in recovery, purification, and waste treatment operations. By extrapolating from the present system of processes, this paper also attempts to chart the future direction of plutonium process development and operation. Areas where a better understanding of basic plutonium chemistry will contribute to development of improved processing are indicated. 

Large-scale plutonium recovery/processing facilities originated at Los Alamos and Hanford as part of the Manhattan Project in 1943. Hanford Operations separated plutonium from irradiated reactor fuel, whereas Los Alamos purified plutonium, as well as recovered the plutonium from scrap and residues. In the 1950 s, similar processing facilities were constructed at Rocky Flats and Savannah River. 

In 1942, the Mallinckrodt Chemical Company adapted a diethylether extraction process to purify tons of uranium for the U.S. Manhattan Project [2] later, after an explosion, the process was switched to less volatile extractants. For simultaneous large-scale recovery of the plutonium in the spent fuel elements from the production reactors at Hanford, United States, methyl isobutyl ketone (MIBK) was originally chosen as extractant/solvent in the so-called Redox solvent extraction process. In the British Windscale plant, now Sellafield, another extractant/solvent, dibutylcarbitol (DBC or Butex), was preferred for reprocessing spent nuclear reactor fuels. These early extractants have now been replaced by tributylphosphate [TBP], diluted in an aliphatic hydrocarbon or mixture of such hydrocarbons, following the discovery of Warf [9] in 1945 that TBP separates tetravalent cerium from... 

Moore, R. L., Progress in Fission Products Recovery at Hanford, HW 83609, 1954-64, Richland, Wash. 

High-level radioactive defense waste solutions, originating from plutonium recovery and waste processing operations at the U.S. Department of Energy s Hanford Site, currently are stored in mild steel-lined concrete tanks located in thick sedimentary beds of sand and gravel. Statistically designed experiments were used to identify the effects of 12 major chemical components of Hanford waste solution on radionuclide solubility and sorption. 

Solvent Extraction Process for Recovery of Americium-241 at Hanford... 

In the early years of plutonium scrap processing operations, the CAW stream was routed to trenches(1 ) specially excavated in Hanford soil. Batch recovery of americium was started in 1965. Later (1970-1976), a continuous countercurrent solvent extraction process employing DBBP (dibutylbutyl phosphonate) as the extractant was operated to recover, at least partially, plutonium and americium values from the CAW stream. Aqueous waste from the DBBP extraction process, still containing some plutonium and americium, was blended with other Plutonium Reclamation Facility (PRF) wastes, made alkaline, and routed to underground tanks for storage. 

Purex [Plutonium and uranium recovery by extraction] A process for the solvent extraction of plutonium from solutions of uranium and fission products, obtained by dissolving spent nuclear fuel elements in nitric acid. The solvent is tri- -butyl phosphate (TBP) in kerosene. First operated by the U.S. Atomic Energy Commission at its Savannah River plant, SC, in 1954 and at Hanford, WA, in 1956. Now in operation, with modifications, in several countries. Sites include Savannah River (SC), Cap de la Hague (France), Marcoule (France), Sellafield (England), Karlsruhe (Germany), and Trombay (India). See also Recuplex. 

U adioactive wastes have accumulated at Hanford since 1944 when the first reactor fuel was processed for plutonium recovery. High-level liquid wastes generated by the Purex, Redox, and BiP04 processes have been stored as neutralized slurries in 151 underground storage tanks. 

Seaborg and associates [LI] had found that tetravalent plutonium [Pu(IV)] could be coprecipitated from aqueous solution in good yield with insoluble bismuth phosphate BiP04, made by adding bismuth nitrate and sodium phosphate to an aqueous solution of plutonium nitrate. The bismuth phosphate process was developed at the Metallurgical Laboratory, demonstrated at the X-10 pilot plant at Oak Ridge National Laboratory in 1944, and put into operation for large-scale recovery of plutonium from irradiated fuel at Hanford in early 1945. 

U.S. plants. The principal U.S. reprocessing plants are listed in Table 10.3, together with their main process features. All use some form of the Purex process. In 1979, the only ones operating were the Savannah River and Idaho plants of the U.S. Department of Energy (DOE). The Hanford plant had been used primarily for recovery of plutonium and uranium from irradiated natural uranium, but was versatile and had been used, for example, for Thorex... 

Special campaigns for recovering neptunium from Purex solutions have been run at Oak Ridge [F4], Hanford [D3], Savannah River [P7], Windscale [Nl], and Marcoule [C6]. None of these sought complete recovery. A brief description will be given of the first three. 

Figure 11.22 presents a scheme of typical plutonium recovery operations. The Plutonium Reclamation Facility (PRF) [Rl] at Hanford incorporates many of these options. Geometrically favorable process equipment and storage tanks are used to ensure criticality safety. 

Figure 11.22 Typical plutonium-recovery operations (Hanford Engineering Development Laboratory). (From Richardson (RlJ.)...

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