WO1998054380A2

WO1998054380A2 - Electrolytic heat production and deactivation of radioactive substance

Info

Publication number: WO1998054380A2
Application number: PCT/US1998/011046
Authority: WO
Inventors: James A. Patterson
Original assignee: Patterson James A
Priority date: 1997-05-28
Filing date: 1998-05-28
Publication date: 1998-12-03
Also published as: WO1998054380A3; AU7605498A

Abstract

An electrolytic system (10) for producing heat and for deactivation of a radioactive substance such as radioactive waste material by electrolysis in an aqueous media (54) which carries the radioactive substance in solution. The electrolytic cell (12) includes a non-conductive housing (34) having an inlet (18) and an oulet (20) and spaced-apart first and second carbon electrodes (36/38) positioned within the housing (34). The electrodes (36/38) are preferably coaxially arranged within the housing (34) so that the proximal ends (50/52) of the electrodes (36/38) face one another and are separated by a gap (48) in the range of 1-5 mm. The electrolyte (54) is water-based and carries the radioactive material in solution as a salt. The carbon electrodes (36/38) preferably include a central passageway (44/46) formed longitudinally for electrolyte (54) flow therethrough. An alternating current (a.c.) electric power source (22) in the system (10) is operably connected across the first and second proximal ends (50/52) whereby electrical current flows across the gap (48) within the aqueous media (54) flowing through the cell (12).

Description

SYSTEM FOR PRODUCING HEAT AND DEACTIVATING A RADIOACTIVE SUBSTANCE BY ELECTROLYSIS

This invention relates generally to electrolytic cells and more particularly to an electrolytic cell and system for producing heat and for deactivating radioactive metals by electrolysis.

The utilization of palladium coated microspheres or beads as a catalytic agent for the absorption of hydrogen is taught in prior U.S. patents 4,943,355 ('355) and 5,036,031 (O31). In these patents, the utilization of cross linked polymer microspheres forming an inner core and having a coating of palladium and other halide forming metals thereatop exhibit significant improvements in the level of hydrogen absorption and the absorption of isotopes of hydrogen.

Utilizing these catalytic microspheres led to the invention disclosed in U.S. patents 5,318,675 ('675) and 5,372,688 ("688) which teach an electrolytic cell, system and method for, inter alia, producing excess heat within a liquid electrolyte.

More recently, U.S. patent 5,494,559 ('559) discloses an improvement in the layer structure of the catalytic microspheres or beads within an electrolytic cell. The combination of nickel/palladium layers enhance the production of excess heat within the liquid electrolyte.

In each of these prior '675, '688 and '559 U.S. patents, the electrolytic cell described therein included an inlet and an outlet facilitating the flow of the liquid electrolyte therethrough. Thus, as the liquid electrolyte is passed through the electrolytic cell, it is acted upon catalytically by the particular bed of catalytic particles contained within the housing of the electrolytic cell to produce excess heat for use.

The following additional issued U.S. patents related to electrolytic cells for heat production and of which James A. Patterson is either a sole inventor or co-inventor are as follows: U.S. Patent No. 5,580,838 U.S. Patent No. 5,607,563 U.S. Patent No. 5,616,219 U.S. Patent No. 5,618,394

U.S. Patent No. 5,628,886 U.S. Patent No. 5,628,887

These prior art patents are also directed to catalytic particles with high hydrogen absorption characteristics and to electrolytic cells using such catalytic particles for electrolysis of water contained in the liquid electrolyte and the production of heat in the liquid electrolyte.

Applicant is co-inventor and co-author of an article related to transmutation of the thin metallic layers applied atop the above-described catalytic particles. This article is entitled Nuclear Transmutations in Thin- Film Nickel Coatings Undergoing Electrolysis by George H. Miley and James A. Patterson, presented at the 2nd International Conference on Low Energy Nuclear Reactions at Texas A & M, College Station Texas on September 13- 14, 1996 in which is presented scientific evidence as to the underlying mechanism which produces heat within one or more of the above-referenced electrolytic cells. That mechanism has been shown to be in the form of low temperature nuclear transmutations of non-radioactive elements.

The present invention broadens the utility of a unique electrolytic cell by not only providing heat, but by also deactivating radioactive material such as nuclear reactive waste byproducts and does this on a more commercially viable basis. The radioactive byproducts are combined into the electrolyte, preferably in salt form, and directed to circulate through the cell during operation of the system.

This invention is directed to an electrolytic cell, system and method for producing heat for use and for deactivation of radioactive material by electrolysis in an aqueous media. The electrolytic cell includes a non- conductive housing having an inlet and an outlet and spaced apart first and second carbon electrodes positioned within the housing. The electrodes are spaced apart at their facing proximal ends a controlled distance defining a gap of about 1 to 5 mm. The electrolyte tested is formed of radioactive uranium oxynitrate in combination with deionized water. The electrolyte flows through central longitudinal passageways formed through each electrode for enhanced deactivation and heat production. An electric power source in the system is operably connected across the first and second electrodes whereby electrical current flows between the proximal spaced ends of the electrodes which are submerged within the aqueous media flowing through the cell.

It is therefore an object of this invention to provide an improved electrolytic cell and system for producing heat.

It is yet another object of this invention to provide an improved electrolytic cell, system and method for producing heat for use and for deactivating radioactive materials by electrolysis in an aqueous media.

It is still another object of this invention to provide a system for deactivation of radioactive waste on a continuous process.

In accordance with these and other objects which will become apparent hereinafter, the instant invention will now be described with reference to the accompanying drawings.

Figure 1 is a schematic view of a system and electrolytic cell embodying the present invention.

Figure 2 is a simplified section view of the electrolytic cell shown in Figure 1.

Figure 3 is a calibration curve for radioactive uranium salt in deionized water used as an electrolyte.

Referring now to the drawings and particularly to Figures 1 and 2, a system embodying concepts of the invention utilized during testing procedures is shown generally at numeral 10. This system 10 includes an electrolytic cell shown generally at numeral 12 interconnected at each end 18 and 20 with a closed loop electrolyte circulation system at 14 and 16, respectively. The circulation system includes a constant volume pump 28 which draws a liquid electrolyte 54 (shown only in Fig. 2) from a reservoir 24 and forces the electrolyte 54 in the direction of arrow A into an inlet 18 of electrolytic cell 12. After the electrolytic cell 12 is completely filled with the electrolyte 54, the electrolyte 54 then exits an outlet 20 and, thereafter, returning to reservoir 24. A separate piece of equipment 56 capable of either directly utilizing heated liquid or one which is capable of converting heat energy into other forms of energy such as electrical energy may be connected to the heated electrolyte flow downstream of the cell 12.

A geiger counter 26 is operably positioned adjacent reservoir 24 to monitor the radioactivity level in counts per minute (c.p.m.) of the electrolyte 54 during system operation. A rate meter from Technical Associates, Inc., along with a 1" diameter cell #P6-LB was used for testing. A conventional heat exchanger 30 may also be provided to dissipate heat output from the cell 12 by submerging a coil 32 of the electrolyte conduit into a volume of liquid as shown. Inlet and outlet temperature of the electrolyte 54 were monitored at T1 and T2, respectively, by thermometers operably placed in the flow of electrolyte.

In Figure 2, the details of the electrolytic cell 12 are there shown. A cylindrical glass non-conductive housing 34 includes electrodes 36 and 38 sealably engaged by clamps 40 and 42 in each end of housing 34. These electrodes 36 and 38 are formed of carbon having an o.d. of 1/4" and central passageways 44 and 46, respectively, of 1/16" diameter. The facing proximal ends 50 and 52 are radiused as shown.

Referring now to Figure 3, the geiger counter 26 was calibrated with respect to a standard electrolyte used in the test reported herebelow having x grams of radioactive uranium oxynitrate purchased from Alza Chemical in combination with 100 ml of deionized water forming the electrolyte for system 10. A thin window was utilized in the geiger counter 26, along with the previously described narrow window. The curve in Figure 3, an essentially straight line function, correlates the grams of the uranium salt (uranium oxynitrate) to the geiger counter response in counts per minute. For example, using an electrolyte having 0.9 grams of the uranium salt in solution with 100 ml of deionized water would produce a geiger counter count of just under 1,000 counts per minute, this data point being marked at numeral 60 in Figure 3.

ELECTRODES 5 The electrodes are preferably formed of pure carbon rods having an outside diameter (o.d.) of 1/4" and a longitudinally extending central aperture therethrough having an inside diameter of 1/16". The length of these rods used in experiments reported herebelow was 3.5 cm.

To insure that the carbon electrodes 36 and 38 are impurity free, they o are leached with AQUA REGA, a solution containing hydrochloric and nitric acid before cell assembly. For enhanced current flow across the gap 48 between the proximal ends 50 and 52 of the electrodes 36 and 38, respectively, a uniform radius is formed thereon as seen in Figure 2. The preferred gap 48 is in the range of 1.5-3.0 mm. 5 ELECTROLYTE

The electrolyte preferred and used in experiments reported herebelow, sometimes referred to as a media, was comprised of the following formula:

0 These initial ingredients were added in the amounts of 12J grams of uranium oxynitrate with 100 ml of deionized water, resulting in a pH of 0.8- 1.0.

Following each successive run of the same test set-up, an appropriate amount of uranium oxynitrate was added to the electrolyte, along 5 with sufficient deionized water to raise the volume level within the reservoir

24 back to the original preestablished level at the onset of testing.

A.C. ELECTRICAL CURRENT It has been found that conventional alternating current at the voltage and current level reported herebelow was best suited for the dual purposes 0 of the present invention. A conventional variable output power supply 22 was interconnected to electrical conduits 62 and 64 shown in Figures 1 and 2 into the corresponding electrodes 36 and 38, respectively. Voltage and current levels were then slowly increased to the point where minimal boiling or bubbling of the electrolyte 54 was viewable through the transparent housing 34. Periodic adjustment was required to maintain this minimal current in voltage level on this basis.

EXPERIMENTAL RESULTS The experimental system 10 as described hereinabove was test run in two separate experiments reported herebelow. The first experimental test comprised a series of five (5) separate test runs which were run in seriatim fashion. That is to say, the initial set-up as shown under Run #1 in Table 1 reported herebelow was based upon an initial electrolyte composition of 12.1 grams of uranium oxynitrate in 100 ml of deionized water. Electrode gap was preset at 3.0 mm. Prior to beginning this experiment, an initial geiger counter count

(c.p.m.) was taken and is shown as 7300 c.p.m. The electrolytic cell 12 and system 10 were operated for 180 minutes of run time, at which time the final geiger counter count had dropped to 2800 c.p.m. This represented a count reduction (reduction in radioactivity or deactivation) of approximately 62%. This deactivation percentage was carried over into the "% uranium reacted" column and then applied against the known initial quantity of uranium salt, i.e. 12.1 gms, leaving a calculated remaining amount of unreacted uranium salt of 4.6 grams remaining in the electrolyte 54. Consequently, during Run #1 , a total of 7.5 grams of uranium salt was reacted or deactivated. In Run #2 as set forth in Table 1 , an arbitrary amount of 7.1 grams of the uranium salt was added to the electrolyte solution and, again, a sufficient amount of deionized water was also added to bring the electrolyte level back to that of the original mark placed on the reservoir. An initial geiger counter count of 7300 c.p.m. was taken before Run #2 was begun. At the end of 180 minutes of run time, the counts per minute had dropped to 4000 c.p.m. for a reduction of 45%. Again, the same percentage of 45% was applied to calculate the grams of uranium salt remaining in the electrolyte at 6.4 gms, with a reacted quantity of salt being calculated at 5.3 grams.

This test was continued through run #5 utilizing the procedures of the addition of radioactive uranium salt in the quantities indicated of 7J grams at the beginning of each test, along with sufficient deionized water to restore electrolyte level. During the four runs, a total of 40.5 grams of radioactive uranium salt had been added into the electrolyte and a total of 28.4 grams of the radioactive uranium salt were reacted, reflecting a percentage of reacted (deactivated) uranium salt of 71 %.

During all of the runs, it is noted that there was a substantially constant positive temperature differential of the electrolyte flowing through the cell of 19°C, clearly representing useful heat production during these test runs. After the fourth test run, all of the tubing and pump 28 were disassembled and checked for radioactive losses by the use of geiger counter 26. None were found during the experiment. The average wattage input in the form of electric power was 12.4 watts, while the wattage output in terms of heated electrolyte based upon the flow rate indicated of 45 ml per minute and a ΔT of 19°C produced heat output of 213 watts. This shows a yield of approximately 201.4 watts of useable heat energy within the electrolyte as it left the cell 12.

TABLE 1

Seriatim Experiments

Run Gms. Initial Final % Net

Time ΔT U Salt Count Count Count Volts Amps Flow Initial % U Gms U Gms U

Run (min) (°C) Added (c.p.m.) (c.p.m.) Reduc. (a.c.) (rms) ml/min Gms U Reacted Remain Reacted

#1 180 19 12.1 7300 2800 62 13.3 2.3 45 12.1 62 4.6 7.5

#2 180 19 7.1 7300 4000 45 14.0 1.0 45 11.7 45 6.4 5.3

#3 150 19 7.1 6400 2600 59 14.5 2.7 45 13.5 59 5.5 8.0 oo

#4 195 19 7.1 5200 3000 42 13.6 1.3 45 12.6 42 7.3 5.3

#5 135 66 7.1 4400 3700 16 23.3 1.7 45 14.4 16 12.1 2.3

TOTAL 40.5 70 12.1 28.4

RERUN

The same basic experimental set-up was rerun after all electrolyte conduit and pump 28 had been either cleaned or replaced. Ten (10) grams of uranium oxynitrate (radioactive) was mixed with 85 ml of deionized water. A gap between the proximal ends of the electrodes was measured at 4.5 mm which had increased about 1.5 mm as a result of the first experimental runs described above. The electrolyte flow rate was set at 60 ml/min. This test run data is reported herebelow in Table 2.

TABLE II New Setup Rerun

Flow Rate = 60 ml/min.

Time Count ΔT Amps Volts Watts Watts Yield

(min) (c.p.m.) (°C) (rms) (a.c.) _ln Out Wo-Win

Start 6836

20 4917 46 1.7 15.5 18.4 193.2 174.8 30 3518

40 2910

90 1968 60 1.8 30.0 37.8 252. 214.2

The experiment was run for a total of 90 minutes. The geiger counter count prior to the beginning of this experiment at 6836 c.p.m. which was reduced to 1968 c.p.m. at the end of the 90 minute experiment reflecting a 71 % reduction in radioactivity or deactivation. Two data points with respect to ΔT across the cell are shown at 20 minutes at 46°C and, at the end of the experiment, a ΔT was recorded to be in excess of 60°C. Input and output wattages were calculated at the same two data points reflecting yields (watts out-watts in) in the amounts of 174.8 and 214.2 watts yield, respectively.

Although the embodiment of the carbon electrodes with the central aperture is preferred at this time, other embodiments of these electrodes wherein electrolyte flows around the exterior surface of through intentionally formed porosity within the carbon itself are envisioned within the scope of this invention. Likewise, any of the radioactive actinide in salt compound form are also envisioned within the scope of this invention.

While the instant invention has been shown and described herein in what are conceived to be the most practical and preferred embodiments, it is recognized that departures may be made therefrom within the scope of the invention, which is therefore not to be limited to the details disclosed herein, but is to be afforded the full scope of the claims so as to embrace any and all equivalent apparatus and articles.

Claims

CLAIMSWhat is claimed is:

1. A system for producing heat and for deactivation of a radioactive material by electrolysis comprising: an electrolytic cell including a non-conductive housing and an inlet and an outlet; first and second conductive carbon-containing electrodes each having a proximal end and a distal end and connected within a non-conductive housing with said proximal ends generally aligned and spaced apart a distance defining a gap therebetween; each said electrode having a central passageway formed therethrough, a distal end of said passageway of said first electrode defining said inlet to said cell, a distal end of said passageway of said second electrode defining said outlet of said cell; an electrolyte flowing through said system whereby at least said central passageway and said proximal end of each said electrode are immersed in said electrolyte during operation of said system; said electrolyte including a radioactive material within water; means for pumping said electrolyte into said electrolytic cell through said inlet whereby said proximal ends of said first and second electrodes are immersed in said electrolyte, said electrolyte exiting from said electrolytic cell through said outlet; means for applying an alternating electric current between said first and second electrodes whereby electric current flows across said gap and through a portion of said electrolyte flowing in close proximity to said proximal ends of said first and second electrodes.

2. A system as set forth in Claim 1 , wherein: said radioactive material is in the form of a conductive salt.

3. A system as set forth in Claim 1 , wherein: said radioactive material is taken from the group of metallic actinides consisting of actinium, thorium, protactinium, uranium, neptunium, plutonium, americium, curium, berkelium, californium, einsteinium, fermium, mendelevium, and lawrencium.

4. A system as set forth in Claim 1 , wherein: each said proximal end is radiused for enhanced electrical current flow therebetween.

5. A system as set forth in Claim 1 , wherein: said radioactive material is taken from the actinide series and daughter elements thereof.

6. A system as set forth in Claim 2, wherein: said conductive salt is uranium or thorium oxynitrate.

7. A system for deactivating a radioactive material by electrolysis in a liquid electrolyte, comprising: an electrolytic cell including a non-conductive housing and an inlet and an outlet; first and second conductive carbon-containing electrodes each having a proximal end and a distal end and connected within a non-conductive housing with said proximal ends generally aligned and spaced apart a distance defining a gap therebetween; each said electrode having a central passageway formed therethrough, a distal end of said passageway of said first electrode defining said inlet to said cell, a distal end of said passageway of said second electrode defining said outlet of said cell; said electrolyte which will flow through said system during operation thereof whereby at least said central passageway and said proximal end of each said electrode are immersed in said electrolyte during operation of said system; said electrolyte including a radioactive material within water; means for pumping said electrolyte into said electrolytic cell through said inlet whereby said proximal ends of said first and second electrodes are immersed in said electrolyte, said electrolyte exiting from said electrolytic cell through said outlet; means for applying an alternating electric current between said first and second electrodes whereby electric current flows across said gap and through a portion of said electrolyte flowing in close proximity to said proximal ends of said first and second electrodes.

8. A system as set forth in Claim 7, wherein: said radioactive material is in the form of a conductive salt.

9. A system as set forth in Claim 7, wherein: said radioactive material is taken from the group of metallic actinides consisting of actinium, thorium, protactinium, uranium, neptunium, plutonium, americium, curium, berkelium, californium, einsteinium, fermium, mendelevium, and lawrencium.

10. A system as set forth in Claim 7, wherein: each said proximal end is radiused for enhanced electrical current flow therebetween.

11. A system as set forth in Claim 7, wherein: said radioactive material is taken from the actinide series and daughter elements thereof.

12. A system as set forth in Claim 7, wherein: said conductive salt is uranium or thorium oxynitrate.