# US 12,002,596 B2 · Targetry coupled separations

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- Number: US 12,002,596 B2
- Document ID: US12002596B2
- Status: Granted
- Kind: B2
- Application number: 17/533,264
- Filed: 2021-11-23
- Published: 2022-09-29
- Granted: 2024-06-04
- Earliest claimed: 2014-12-29
- Assignees: TerraPower, LLC
- Applicants: TerraPower, LLC
- Inventors: Ken Czerwinski; Joshua C. Walter; Christopher P. Dunckley
- Web page: https://patentgrep.com/patent/US12002596B2

## CPC

- G21G 1/02: in nuclear reactors (by thermonuclear reactions G21B; conversion of nuclear fuel G21C)
- B01D 11/0203: {with a supercritical fluid}
- B01D 11/0403: {with a supercritical fluid}
- B01D 15/40: using supercritical fluid as mobile phase or eluent
- G21C 19/42: Reprocessing of irradiated fuel
- G21G 1/08: accompanied by nuclear fission
- G01N 35/02: using a plurality of sample containers moved by a conveyor system past one or more treatment or analysis stations {(G01N35/0098 and G01N35/0099 take precedence)}
- G21G 2001/0036: {Molybdenum}
- G21G 2001/0089: {Actinium}
- G21G 2001/0094: {Other isotopes not provided for in the groups listed above}
- Y02A 50/30: Against vector-borne diseases, e.g. mosquito-borne, fly-borne, tick-borne or waterborne diseases whose impact is exacerbated by climate change
- Y02E 30/30: Nuclear fission reactors
- Y02P 20/54: using solvents, e.g. supercritical solvents or ionic liquids
- G21G: CONVERSION OF CHEMICAL ELEMENTS; RADIOACTIVE SOURCES (applications of radiation in general G21H5/00; handling particles, e.g. neutrons, or electromagnetic radiation not otherwise provided for G21K)
- B01D: SEPARATION (separating solids from solids by wet methods B03B, B03D; by pneumatic jigs or tables B03B; by other dry methods B07; magnetic or electrostatic separation of solid materials from solid materials or fluids, separation by high-voltage electric fields B03C; centrifuges, vortex apparatus B04; presses per se for squeezing-out liquid from liquid-containing material B30B9/02; treatment of water C02F, e.g. softening by ion-exchange C02F1/42; {arrangements of air intake cleaners in gas turbine plants F02C7/05} ; arrangements or mounting of filters in air-conditioning, air-humidification or ventilation F24F13/28)
- G21C: NUCLEAR REACTORS (fusion reactors, hybrid fission-fusion reactors G21B; nuclear explosives G21J)
- G01N: INVESTIGATING OR ANALYSING MATERIALS BY DETERMINING THEIR CHEMICAL OR PHYSICAL PROPERTIES (measuring or testing apparatus or processes other than immunoassay, involving enzymes or microorganisms C12M, C12Q)
- Y02A: TECHNOLOGIES FOR ADAPTATION TO CLIMATE CHANGE
- Y02E: REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02P: CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS

## Abstract

Targetry coupled separation refers to enhancing the production of a predetermined radiation product through the selection of a target (including selection of the target material and the material's physical structure) and separation chemistry in order to optimize the recovery of the predetermined radiation product. This disclosure describes systems and methods for creating (through irradiation) and removing one or more desired radioisotopes from a target and further describes systems and methods that allow the same target to undergo multiple irradiations and separation operations without damage to the target. In contrast with the prior art that requires complete dissolution or destruction of a target before recovery of any irradiation products, the repeated reuse of the same physical target allowed by targetry coupled separation represents a significant increase in efficiency and decrease in cost over the prior art.

## Claims

### Claim 1

A method of manufacturing a radionuclide metal that is a fission product of the fissioning of uranium, the method comprising:
fissioning a molten fuel salt containing uranium, thereby generating an irradiated fuel salt mixture containing molten uranium salt and fission products, wherein the fission products include the radionuclide metal;
contacting at least some of the irradiated fuel salt mixture with supercritical carbon dioxide containing a ligand that forms a metal complex with the radionuclide metal but does not form a metal complex with the uranium in the fuel salt, thereby forming a combined fuel salt and supercritical carbon dioxide mixture containing an amount of radionuclide metal complexes;
separating at least some of the radionuclide metal complexes from the combined fuel salt and supercritical carbon dioxide mixture; and
decomposing the radionuclide metal complexes to obtain the radionuclide metal.

### Claim 2 (depends on 1)

The method of claim 1, wherein the contacting further comprises:
removing the irradiated fuel salt mixture from a molten fuel salt nuclear reactor;
placing the irradiated fuel salt mixture in an extraction vessel; and
injecting the supercritical carbon dioxide containing the ligand into the extraction vessel.

### Claim 3 (depends on 2)

The method of claim 2, wherein the contacting further comprises:
placing the irradiated fuel salt mixture into the extraction vessel containing supercritical carbon dioxide containing the ligand.

### Claim 4 (depends on 1)

The method of claim 1, wherein the separating further comprises:
adjusting at least one of a temperature or a pressure of the combined fuel salt and supercritical carbon dioxide mixture in an extraction vessel.

### Claim 5 (depends on 4)

The method of claim 4, wherein the adjusting further comprises:
increasing the temperature, the pressure, or both to volatilize the radionuclide metal complexes out of the combined fuel salt and supercritical carbon dioxide mixture as a separate gas phase.

### Claim 6 (depends on 5)

The method of claim 5, wherein the separating further comprises:
removing the separate gas phase from the extraction vessel.

### Claim 7 (depends on 6)

The method of claim 6, wherein the decomposing further comprises:
heating the separate gas phase, thereby decomposing the radionuclide metal complexes.

### Claim 8 (depends on 4)

The method of claim 4, wherein the adjusting further comprises:
decreasing the temperature, the pressure, or both to obtain a liquid phase separate from the combined fuel salt and supercritical carbon dioxide mixture, the liquid phase containing the radionuclide metal complexes.

### Claim 9 (depends on 8)

The method of claim 8, wherein the separating further comprises:
removing the liquid phase from the extraction vessel.

### Claim 10 (depends on 9)

The method of claim 9, wherein the decomposing further comprises:
heating the liquid phase, thereby decomposing the radionuclide metal complexes.

### Claim 11 (depends on 1)

The method of claim 1, wherein the radionuclide metal is selected from 227Ac, 213Bi, 131Cs, 133Cs, 11C, 51Cr, 57Co, 60Co, 64Cu, 67Cu, 165Dy, 169Er, 18F, 67Ga, 68Ga, 68Ge, 198Au, 166Ho, 111In, 123I, 124I, 125I, 131I, 192I, 59Fe, 212Pb, 177Lu, 99Mo, 13N, 15O, 103Pd, 32P, 238Pu, 42K, 227Ra, 223Ra, 186Re, 188Re, 81Rb, 82Rb, 101Ru, 103Ru, 153Sm, 75Se, 24Na, 82Sr, 89Sr, 99 mTc, and 201Tl.

### Claim 12 (depends on 1)

The method of claim 1, wherein the molten fuel salt contains a chloride salt of uranium.

### Claim 13 (depends on 1)

The method of claim 1, wherein the contacting is performed with the irradiated fuel salt mixture in a liquid form.

### Claim 14 (depends on 1)

The method of claim 1, wherein the contacting is performed with the irradiated fuel salt mixture in a solid form.

### Claim 15 (depends on 1)

The method of claim 1, wherein the contacting is performed on the irradiated fuel salt mixture while the irradiated fuel salt mixture is in a molten fuel salt nuclear reactor.

### Claim 16

A method of manufacturing 177Lu radioisotope comprised of:
preparing an enriched dry 176Yb oxide source material within a pressurized containment vessel;
irradiating the 176Yb oxide containing source with neutrons at suitable neutron flux density to achieve reaction of 176Yb to 177Yb via the reaction 176Yb(n,γ)177Yb will decay to 177Lu by the reaction 177Yb→177Lu+β− with half-life of 1.91 h;
injecting the pressurized containment vessel containing the irradiated 176Yb oxide source with supercritical carbon dioxide containing a ligand that selectively forms a metal complex with the lutetium but does not form a metal complex with the ytterbium, thereby forming a supercritical carbon dioxide mixture containing an amount of lutetium metal complexes;
removing the supercritical carbon dioxide mixture containing an amount of lutetium metal complexes; and
separating at least some of the radionuclide lutetium complexes from the supercritical carbon dioxide mixture to provide a 177Lu rich separation fraction.

### Claim 17

A method of manufacturing 67Cu radioisotope comprised of:
packing an enriched 70Zn oxide source material in an appropriate a cavity within an irradiation target box;
irradiating the 70Zn source with 15-20 MeV of deuterons), yielding 67Cu via the reaction 70Zn(p,α)67Cu with estimated cross-sections of 67Cu formation of 15-27 mb;
contacting the 70Zn oxide target with supercritical carbon dioxide containing a ligand that selectively forms a metal complex with the copper but does not form a metal complex with the zinc oxide, thereby forming a supercritical carbon dioxide mixture containing an amount of radionuclide metal complexes;
separating at least some of the radionuclide metal complexes from the combined radionuclide and supercritical carbon dioxide mixture;
separating the radionuclide from the combined radionuclide and supercritical carbon dioxide mixture; and
purifying the 67Cu radionuclide.