Various exemplary embodiments disclosed herein relate generally to systems for storing toxic radioactive salt solutions.
Acid deficient uranyl nitrate solutions are used in a sol-gel process for fuel fabrication. However, such solutions are toxic, and a system for safely storing unused or waste uranyl nitrate solutions, as well as other radioactive salt solutions, is required. Additionally, acid deficient uranyl nitrate solutions have a uranium concentration of from 0.5 M to 3.5 M, and a pH of 0.5 to 2.8. The system for storing uranyl nitrate solutions must therefore be able to withstand exposure to highly acidic conditions.
Other radioactive salt solutions may be used in a sol-gel process for fuel fabrication, including various nitrate salts of radioactive metals. Ceramic fuel elements based on uranium, thorium, and plutonium are made from acidic solutions of UO2(NO3)2 (uranyl nitrate), U(NO3)6 (uranium nitrate), K2UO2(SO4)2 (potassium uranyl sulfate), UO2(SO4) (uranyl sulfate), U(SO4)2 (uranium sulfate), uranium phosphates, Th(NO3)4, or Pu(NO3)4. Thus, a system for safely storing unused or waste radioactive salt solution should be suitable for storing various radioactive metal salts.
In view of the foregoing, it would be desirable to develop improved methods and systems for storing toxic radioactive salt solutions.
In light of the present need for storing toxic, radioactive, or otherwise dangerous liquid materials, a brief summary of various embodiments is presented. Some simplifications and omissions may be made in the following summary, which is intended to highlight and introduce some aspects of the embodiments disclosed herein, but not to limit the scope of the invention. Detailed descriptions of embodiments adequate to allow those of ordinary skill in the art to make and use the inventive concepts will follow in later sections.
Various embodiments disclosed herein relate to a system for receiving and storing a radioactive salt solution, including:
In various embodiments, the cap includes a lateral wye fitting having:
The system for receiving and storing a radioactive salt solution may also include a pickup for the ventilation system configured to receive the gases from the tank, and a second air gap between the pickup and the vertical pipe configured to prevent flow of the radioactive salt solution into the pickup.
In various embodiments, the system includes a control system having:
The system for receiving and storing a radioactive salt solution may also include a solution outlet at the bottom of the tank, and a valve configured to allow the radioactive salt solution in the tank to flow through the solution outlet, thereby emptying the tank.
The system for receiving and storing a radioactive salt solution may include an input pump configured to pump the radioactive salt solution to the solution inlet, wherein the input pump stops pumping the radioactive salt solution upon receipt of a signal from the level switch, thereby preventing overfilling of the tank.
In various embodiments, the overflow bottle in the system for receiving and storing a radioactive salt solution includes a container having a mouth; and a cap including a breather vent configured to trap harmful vapors, an opening welded to the overflow line; and a means for removably securing the cap to the mouth of the container. The means for removably securing the cap to the mouth of the container may include:
In order to better understand various exemplary embodiments, reference is made to the accompanying drawings, wherein:
Scrap or waste acid-deficient uranyl nitrate (ADUN) solutions need to be stored safely. Safe ADUN storage requires a tank which is geometrically safe to prevent possibility of a criticality accident, i.e., a tank having an outer diameter of about 5 inches or less, 4.5 inches or less, or 4 inches or less. The tank must be chemically resistant to concentrated nitric acid.
While ADUN solution storage is of particular interest herein, other radioactive salt solutions which may be used as precursors for formation radioactive ceramic nuclear fuels by sol-gel processes may be stored with the systems disclosed herein. Suitable radioactive salt solutions include acidic solutions of UO2(NO3)2 (uranyl nitrate), Th(NO3)4, Pu(NO3)4, and mixtures thereof. Radioactive salt solutions based on uranium, thorium, and plutonium may be acidic solutions of UO2(NO3)2 (uranyl nitrate), U(NO3)6 (uranium nitrate), K2UO2(SO4)2 (potassium uranyl sulfate), UO2(SO4) (uranyl sulfate), U(SO4)2 (uranium sulfate), uranium phosphates, Th(NO3)4, or Pu(NO3)4.
A solution of acid deficient uranyl nitrate, may be prepared by dissolving a uranium oxide in aqueous nitric acid to produce a uranium solution, placing the uranium solution under a pressure of 5 to 40 atmospheres in a sealed reaction chamber, and heating the uranium solution to a desired holding temperature of between 150° C. and 250° C. The uranium solution is maintained at the desired holding temperature in the sealed vessel for a desired hold time, and then the pressure and temperature of the uranium solution are reduced to obtain an acid deficient uranyl nitrate solution.
Once the acid deficient uranyl nitrate solution is prepared, it is converted into a ceramic nuclear fuel particle by sol-gel processes known in the art. Such conversion may be carried out immediately, or acid deficient uranyl nitrate solution may be stored for later use in an acid-resistant tank.
Storage of scrap acid-deficient uranyl nitrate (ADUN) requires a tank which is geometrically safe, to prevent possibility of a criticality accident. Generally, the tank may have any desired height, but must have a narrow width to avoid excessive buildup of nuclear material at any point along the height of the tank. Since acid-deficient uranyl nitrate is formed in a nitric acid solution, the tank must be chemically resistant to concentrated nitric acid. The tank must be designed to preclude the possibility of solution backflow into a solution inlet, which may be done through the inclusion of air gaps. The tank should be capable of sealing to simultaneously limit both gas emissions and overflow of ADUN solution from the tank.
The tank should include a pickup for ventilation to remove off gases from the tank during filling and emptying operations, where ventilation from the tank cannot blocked unless all flow into or out of the tank is ceased. Additional features of the system include:
The system for receiving and storing a radioactive salt solution disclosed herein contains the following improved design features:
The system disclosed herein is suitable for receiving and storing any fissile-bearing solution inside a fuel manufacturing facility. Any soluble salt of uranium, thorium, plutonium, or an oxidized form thereof may be used. The only limitation is material compatibility between the tank 1 and the solution. A solution of a salt of uranium, thorium, or plutonium in an aqueous sulfuric, nitric, or phosphoric acid medium is compatible with stainless steel tank 1. A solution of a salt of uranium, thorium, or plutonium in aqueous HCl would not be compatible with stainless steel, as HCl corrodes stainless steel. Should storage of a salt of uranium, thorium, or plutonium in aqueous HCl be desired, tank 1 may be constructed from a glass pipe.
The upper end of tank 1 is sealed with the backflow-safe inlet flange, which includes cap 2 having a flange. The cap 2 includes a lateral wye fitting 5 with a vertical pipe and a lateral pipe 4. The lateral pipe 4 is configured to direct radioactive salt solution from a solution inlet to the interior of tank 1. The vertical pipe in the lateral wye fitting 5 is configured to vent gases in tank 1 to a ventilation system. Tank 1 may include a demister 17, to enhance the removal of radioactive salt solution droplets from gases vented from tank 1. Demister 17 may be a mesh-type coalescer to cause droplets to coalesce into larger drops. Demister 17 may be a knitted wire mesh pad mist eliminator, a woven mesh mist eliminator, a nonwoven mesh mist eliminator, or a mist eliminator formed from a plate or a series of plates with fine perforations. Demister 17 is positioned in tank 1, immediately under cap 2.
To prevent spilling radioactive salt solution in the event that tank 1 overflows during filling, an overflow line 13 carries excess radioactive salt solution from the lateral wye fitting 5 to criticality-safe tank overflow bottle 12, shown in more detail in
Between cap 2 and lateral wye fitting 5, valve 3 may be positioned. When valve 3 is open while filling tank 1, radioactive salt solution may pass from lateral pipe 4 to the interior of tank 1, and gases in tank 1 may be vented through the vertical pipe in fitting 5 to the ventilation system. When valve 3 is closed, radioactive salt solution may be stored in tank 1 without allowing spillage of the solution or venting of gases. Valve 3 may be controlled by control 3a.
Tank 1 may include a solution outlet 14 at the bottom of the tank, allowing the contents of tank 1 to be emptied and recovered. Valve 7 may be used to open or close solution outlet 14. A sidestream 15 opened or closed by valve 6 may be used to sample the radioactive salt solution in tank 1.
Overflow line 13 may be fitted with a sight glass 16. The interior of overflow line 13 may be monitored with a camera or optical sensor 10 to detect radioactive salt solution in the overflow line. If radioactive salt solution is detected in the overflow line 13, sensor 10 may send a signal to CPU 11.
In various embodiments, tank 1 is manufactured from a stainless steel pipe with a nominal pipe size (NPS) of 4 to 5, and cap 2 at the top of tank 1 is a flange cap for an NPS 4 pipe or an NPS 5 pipe, as needed. Two ports are machined into the flange cap: a ¾″ port for a level switch, and a 2″ port for connection to the lateral wye fitting through valve 3. In various embodiments, the inlet assembly includes the following components:
When level switch 31 detects that tank 1 is full, a signal from level switch 31 is sent to CPU 22, which may be the same as, or different from, CPU 11 in
Valve 21 is set to a Normally Closed condition so that, should valve 21 fail, it will fail in a closed position to prevent overfilling of the tank. Valve 21 is meant to cut off flow from the solution input. While filling the tank, CPU 22 sends a signal to valve 21 to open to allow flow of the radioactive salt solution into the tank 1.
Valve 3 is set to a Normally Open condition so that, should valve 3 fail, it will fail in an open position to prevent spilling of the radioactive salt solution when the tank is being filled. When the tank is not being filled or emptied, valve 3 is closed to seal radioactive salt solution and vapors within tank 1, so as to limit emissions that may be radioactive or dangerous. During normal operation, valves 3 and 21 work together to allow flow only under conditions which prevent backflow.
In various embodiments, valves 3 and 21 are remote-actuated valves. Suitable remote-actuated valves include air actuated pneumatic valves, motor-driven valves, and solenoid valves.
An overflow pipe 32 extends from the vertical pipe of lateral wye fitting 5. If tank 1 is overfilled during a filling operation, the excess solution may back up into the lateral wye fitting. This solution is drained through overflow pipe 32 to an overflow bottle (shown in
As seen in
Lateral wye fitting 5 provides a solution input through the lateral pipe 4, an independent ventilation pathway through the vertical pipe, and an independent overflow pathway through overflow pipe 32. Positioning the wye fitting 5 above valve 36 allows for the sealing of tank 1 without providing the avenue for a blocked ventilation pathway. The ventilation pathway through the vertical pipe of fitting 5 must passively be open during operation. If the ventilation pathway and the solution input were separate ports in cap 2, a valve on the ventilation pathway would allow for the valve to fail in an open position, and thus would not be passively safe. Since the ventilation pickup 33 and the solution inlet 34 are each above valve 36, if valve 36 is closed, the tank is not in operation and gases cannot escape from the tank. Thus, the ventilation pickup and inlet filling are linked by this component.
The system of
A second air gap may be introduced between the ventilation pickup 33 and the opening in the vertical pipe of lateral wye fitting 5. This air gap prevents radioactive salt solution in the lateral wye fitting 5 from being sucked into ventilation pickup 33.
Referring to
In various embodiments, an NPS 4 pipe flange or an NPS 5 pipe flange is used as flange 37, and is bolted to plate 44. Flange 37 is also secured to an outer surface of tank 1, in much the same way that cap 2 is fixed to the upper end of tank 1. Plate 44 is secured to the support skids 56. This provides a robust support for tank 1.
Although the various exemplary embodiments have been described in detail with particular reference to certain exemplary aspects thereof, it should be understood that the invention is capable of other embodiments and its details are capable of modifications in various obvious respects. As is readily apparent to those skilled in the art, variations and modifications can be affected while remaining within the spirit and scope of the invention. Accordingly, the foregoing disclosure, description, and figures are for illustrative purposes only and do not in any way limit the invention, which is defined only by the claims.