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In 1957 Glenn T. Seaborg conceived and advocated for the construction of the High Flux Isotope Reactor (HFIR) and the Transuranium Processing Plant (since then renamed the Radiochemical Engineering Development Center, or REDC) at Oak Ridge National Laboratory. Heavily shielded hot cells, glove boxes, and laboratories allow recovery of transuranium elements produced in substantial quantities. Seaborg’s vision of HFIR and REDC producing milligram quantities of berkelium, californium, and einsteinium has been fulfilled beginning in 1966 through May 2019 with 78 production campaigns yielding a cumulative totals of 1.2 g of 249Bk, 10.2 g of 252Cf, 39 mg of 253Es, and 15 pg of 257Fm. Notably, 252Cf is a neutron source used in many industrial applications including oil exploration; process control systems for the cement industry, coal analysis, and power production; sources to start nuclear reactors and perform nondestructive materials analyses; homeland security and national defense detection devices; and medical research. Isotopes made available through transplutonium production at HFIR/REDC have enabled scientists to study the nuclear properties and reactions, chemical properties, optical properties, and solid-state properties of transplutonium elements. Long-lived isotopes have served as targets in heavy ion accelerators to produce heavier elements leading to the discovery of 104Rf, 105Db, 106Sg, 113Nh, 114Fl, 115Mc, 116Lv, 117Ts, and 118Og. This paper reviews the evolution of the processing flowsheets to produce, separate, and purify transplutonium isotopes, which have evolved over 50 years of operation at HFIR and REDC, and summarizes directions of future work to improve the efficiency of the production operations.

The US Department of Energy has presented a plan to use existing reactors at Oak Ridge National Laboratory (ORNL) and Idaho National Laboratory (INL) and processing facilities at ORNL, modified as needed, to produce Pu. The basic capabilities that need to be put into place to produce new Pu are (1) neptunium storage and transport, (2) target fabrication, (3) target irradiation, and (4) chemical processing of irradiated targets to recover Pu. Neptunium currently in storage at INL will be shipped to ORNL during CY 2015. The target design has progressed to a prototypic target design that is expected to be used for production. Initial chemical processing experiments have shown successful recovery of neptunium and plutonium, but overall product purity has not been as high as desired.

Selection of an aluminum alloy for target cladding affects post-irradiation target dissolution and separations. Recent tests with aluminum alloy 6061 yielded greater than expected precipitation in the caustic dissolution step, forming up to 10 wt.% solids of aluminum hydroxides and aluminosilicates. We present a study to maximize dissolution of aluminum metal alloy, along with silicon, magnesium, and copper impurities, through control of temperature, the rate of reagent addition, and incubation time. Aluminum phase transformations have been identified as a function of time and temperature, using X-ray diffraction. Solutions have been analyzed using wet chemical methods and X-ray fluorescence. These data have been compared with published calculations of aluminum phase diagrams. Temperature logging during the transients has been investigated as a means to generate kinetic and mass transport data on the dissolution process. Approaches are given to enhance the dissolution of aluminum and aluminosilicate phases in caustic solution.

The Radiochemical Engineering Development Center (REDC) at Oak Ridge National Laboratory (ORNL) processes highly irradiated targets for the Mark 42 program to separate Am, Cm, and Pu. The target feed material for each assembly was 3.3 kg of plutonium (78% 239Pu) that was irradiated at the Savannah River Site to yield approximately 100 g each of 243Am and 244Cm, and 100-g quantities of 242Pu for special DOE projects. The REDC has plans to process ten of these target assemblies over the next few years. The first assembly has been dissolved, and approximately 1/4 of this material has been used to test the processing flowsheet. Various aqueous processes developed at the REDC over the past years were utilized to dissolve the target segments, separate the bulk of the impurities from the transuranics, separate the plutonium from the transplutonium actinides, and separate the rare earth fission products from the Am-Cm. The separation of the Am-Cm products to the desired purity levels presented new proces...

The heaviest isotopes of elements Z = 117 to Z = 105, 294117, 293117, 290115, 289115, 286113, 285113, 282Rg, 281Rg, 278Mt, 274Bh, and 270Db, were identified by means of the Dubna gas-filled recoil separator among the products of the 249Bk + 48Ca reaction. The details of the observed six decay chains, indicating the production and decay of isotopes 293117 and 294117, are presented and discussed. The decay energies and resulting half-lives of these new nuclei show a strong rise of stability with increasing neutron number, validating the concept of the island of enhanced stability for superheavy nuclei.

The discovery of a new chemical element with atomic number Z=117 is reported. The isotopes {sup 293}117 and {sup 294}117 were produced in fusion reactions between {sup 48}Ca and {sup 249}Bk. Decay chains involving 11 new nuclei were identified by means of the Dubna gas-filled recoil separator. The measured decay properties show a strong rise of stability for heavier isotopes with Z{>=}111, validating the concept of the long sought island of enhanced stability for superheavy nuclei.

Selection of an aluminum alloy for target cladding affects post-irradiation target dissolution and separations. Recent tests with aluminum alloy 6061 yielded greater than expected precipitation in the dissolver, forming up to 10 wt.% solids of aluminum hydroxides and aluminosilicates. Aluminosilicate dissolution presents challenges in a number of different areas, including metals extraction from minerals, flyash treatment, and separations from aluminum alloys. We present experimental work that attempts to maximize dissolution of aluminum metal in caustic, along with silicon, magnesium, and copper impurities, through control of temperature, the rate of reagent addition, and incubation time. Aluminum phase transformations have been identified as a function of time and temperature, using X-ray diffraction. Solutions have been analyzed using wet chemical methods and X-ray fluorescence. These data have been compared with published calculations of aluminum phase diagrams. Approaches are given to enhance the dis...

The synthesis of the new chemical element with atomic number Z=117 is presented. The isotopes 293117 and 294117were produced in fusion reactions between 48Ca and 249Bk. The 249Bk was produced in the High Flux Isotope Reactor and chemically separated at Oak Ridge. Decay chains involving eleven new nuclei were identified by means of the Dubna Gas Filled Recoil Separator. The measured decay properties show a strong rise of stability for super-heavy nuclei toward N=184.