WO1998003699A2

WO1998003699A2 - Electrolytic nuclear transmuted elements having unnatural isotopic distributions

Info

Publication number: WO1998003699A2
Application number: PCT/US1997/012309
Authority: WO
Inventors: James A. Patterson; George H. Miley
Original assignee: Patterson James A; Miley George H
Priority date: 1996-07-09
Filing date: 1997-07-09
Publication date: 1998-01-29
Also published as: WO1998003699A3; AU4644097A

Abstract

A method for producing low temperature nuclear transmutations which occur during electrolysis in an aqueous medium within a cell (12). New elements produced by transmutation during operation of the cell are both higher and lower in atomic mass than the original element undergoing transmutation. Many of the new elements also exhibit isotopic shifts from natural isotope abundance. The electrolytic cell (12) includes a non-conductive housing (14) having an inlet (54) and an outlet (56) and spaced apart first and second conductive grids (38 and 44) positioned within the housing (14). A plurality of preferably cross-linked polymer non-metallic cores each having a uniform conductive exterior metallic surface formed of a high hydrogen absorbing material, such as a metallic hydride forming material, form a bed (35) of conductive beads (36) closely packed within the housing (14) in electrical contact with the first grid (38) adjacent the inlet (54). An electric power source (15, 16) in the system (10) is operably connected across the first and second grid (38 and 44) whereby electrical current flows between the grids (38 and 44) and within the aqueous medium (59) flowing through the cell (12) during cell operation.

Description

NUCLEAR TRANSMUTED ELEMENTS HAVING

UNNATURAL ISOTOPIC DISTRIBUTIONS

BY ELECTROLYSIS AND METHOD OF PRODUCTION

BACKGROUND OF THE INVENTION

This is a continuation-in-part of PCT application No. PCT/US97/05946 filed April 10, 1997 claiming priority from U.S. provisional application No. 60/015,229 filed April 10, 1996 and U.S. provisional application No. 60/021,439 filed July 9, 1996. SCOPE OF INVENTION This invention relates generally to electrolytic cells and TO transmutation of elements and compounds and more particularly to a method of producing low temperature endothermic and exothermic nuclear transmutations in the presence of an aqueous media which demonstrate the occurrence of isotopic shifts from natural abundance. PRIOR ART

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 ('031 ). 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.

BRIEF SUMMARY OF THE INVENTION This invention is directed to a method for producing new elements by low temperature nuclear transmutations during electrolysis in an aqueous media within an electrolytic cell, which transmutations, in part, show the distinct characteristics of isotopes which have shifted in ratios of occurrence from those natural abundance. The electrolytic cell includes a non-conductive housing having an inlet and an outlet and spaced apart first and second conductive grids positioned within the housing. A plurality of preferably cross linked polymer non-metallic cores each having a uniform conductive exterior metallic surface formed of a high hydrogen absorbing material, such as a metallic hydride forming material, form a bed of conductive beads closely packed within the housing in electrical contact with the first grid adjacent the inlet. An electric power source in the system is operably connected across the first and second grid whereby electrical current flows between the grids and within the aqueous media flowing through the cell.

It is therefore an object of this invention to provide a method of operating an electrolytic cell and system for producing low temperature nuclear transmutations of elements by electrolysis which demonstrate isotopic shifts from natural abundance. It is yet another object of this invention to provide an improved method for producing low temperature nuclear transmutations by electrolysis in an aqueous media which are strongly characterized as including isotopes having an unnatural atomic mass distribution.

It is still another object of this invention to provide new elements produced by low temperature nuclear transmutation in an electrolytic cell which exhibit isotopic shifts from natural abundance.

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. BRIEF DESCRIPTION OF THE DRAWINGS

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

Figure 2 is a section view of the electrolytic cell shown in Figure 1. Figure 3 is processed data from a secondary ion mass spectrometer (SIMS) analysis of the outer bead material of beads utilized in Test Number 3 before test run.

Figure 4 is processed data from a SIMS analysis of the outer bead material of beads utilized in Test Number 3 after test run. Figure 5 is a graph depicting binding energy per nucleon versus atomic mass number.

Figures 6a and 6b are graphic depictions of the data presented in Table VIII.

Figures 7a and 7b are graphic depictions of total increases elemental masses per microsphere and in the thin outer film, respectively, and corresponding to data presented in Figures 6a and 6b.

Figure 8 is a graphic depiction of differences between isotopic percentage concentrations observed after cell operation and those for natural abundance for the reaction product elements shown in Table III.

DETAILED DESCRIPTION OF THE INVENTION Referring now to the drawings, a system embodying concepts of the invention utilized during testing procedures is shown generally at numeral 10 in Figure 1. This system 10 includes an electrolytic cell shown generally at numeral 12 interconnected at each end with a closed loop electrolyte circulation system. The circulation system includes a constant volume pump 18 which draws a liquid electrolyte 59 from a reservoir 32 and forces the electrolyte 59 in the direction of the arrow into inlet 54 of electrolytic cell 12. After the electrolytic cell 12 is completely filled with the electrolyte 59, the electrolyte then exits an outlet 56, thereafter flows into a gas separator 26 which is provided to separate and recombine hydrogen and oxygen gas from the electrolyte 59. An in-line filter 22 capable of filtering down to 0.8 microns of particle size is provided for filtration of debris within the system. The system 10 also includes a digital flow meter 19 to accurately measure electrolyte flow through the system 10.

Still referring to Figure 1 is an in-line heater 21 disposed between the filter 22 and the cell 12. This heater 21 is provided to heat the electrolyte liquid 59 as it flows through the system 10 and the cell 12. Note importantly that the heater 21 may be positioned anywhere in the closed system electrolyte flow path as the heating applied is of a steady state nature rather than only a pre-heating condition of the electrolyte, although positioning of the heater 21 is preferred to be adjacent the inlet

54 of the cell 12 for better liquid electrolyte temperature control. The heating of the electrolyte external to the cell 12 is one means for triggering and enhancing the catalytic reaction within the cell 12 to produce a positive temperature differential (ΔT) of the electrolyte as it flows through the cell 12. Shown in Figure 2 is another means preferred for triggering this heat production reaction between the electrolyte 59 and a bed 35 of conductive particles 36 within the cell 12 is by the application of sufficient electric d.c. current across electrodes 15 and 16 as described herebelow.

In Figure 2, the details of the electrolytic cell 12 utilized during testing procedures is there shown. A cylindrical glass or nylon non-conductive housing 14, open at each end, includes a moveable non-conductive end member 46 and 48 at each end thereof. These end members 46 and 48 are sealed within the housing 14 by O-rings 62 and 64. The relative spacing between these end members 46 and 48 is controlled by the movement of end plates 50 and 52 thereagainst.

Each of the end members 46 and 48 includes an inlet stopper 54 and an outlet stopper 56, respectively. Each of these stoppers 54 and 56 define an inlet and an outlet passage, respectively into and out of the interior volume, respectively, of the electrolytic cell 12. These end members 46 and 48 also include a fluid chamber 58 and 60, respectively within which are mounted electrodes 15 and 16, respectively, which extend from these chambers 58 and 60 to the exterior of the electrolytic cell 12 for interconnection to a constant current-type d.c. power supply (not shown) having its negative and positive terminals connected as shown. Also positioned within the chambers 58 and 60 are thermocouples 70 and 72 for monitoring the electrolyte temperature at these points of inlet and outlet of the electrolytic cell 12. However, in the experiments reported herebelow, the inlet temperature of the liquid electrolyte was measured just outside of the cell 12 immediately upstream of stopper 54 to more accurately reflect true temperature differential (ΔT) of the liquid electrolyte 59 while passing through the cell 12. Thus, all exposed surfaces to the liquid media are non- metallic except for the conductive beads and the conductive grid.

A plurality of separate, packed conductive beads or particles 36 are positioned to define a bead bed 35 within housing 14 immediately adjacent and against a conductive foraminous or porous grid 38 formed of titanium and positioned transversely across the housing 14 as shown. These conductive beads 36 are described in detail herebelow.

Still referring to Figure 2, a non-conducive foraminous or porous nylon mesh 40 is positioned against the other end of these conductive particles 36 so as to retain them in the position shown. Adjacent the opposite surface of this non-conductive mesh 40 is a plurality of non-conductive spherical beads, or more generally particles, 42 formed of cross-linked polystyrene and having a nominal diameter of about 1.0 mm. Against the other surface of this layer of non-conductive beads 42 is a conductive foraminous or porous grid 44 formed of titanium and positioned transversely across the housing 14 as shown. Should the liquid electrolyte in the system 10 boil off or otherwise inadvertently be lost, a means of preventing system damage is preferred which replaces the non- conductive beads 42 with non-metallic spherical cation ion exchange polymer conductive beads preferably made of cross-linked styrene divinyl benzene having fully pre-sulfonated surfaces which have been ion exchanged with a lithium salt. This preferred non-metallic conductive microbead structure will thus form a "salt bridge" between the anode 44 and the conductive particles 36, the non-conductive mesh 40 having apertures sufficiently large to permit contact between the conductive particles 36 and the conductive non-metallic microbeads. The mesh size of mesh 40 is in the range of 200-500 micrometers. This preferred embodiment thus prevents melting of the sulfonated non-conductive beads 42 while reducing cell resistance during high loading and normal operation.

The end of the electrode 15 is in electrical contact at 66 with conductive grid 38, while electrode 16 is in electrical contact at 68 with conductive grid 44 as shown. By this arrangement, when there is no electrolyte within the electrolytic cell 12, no current will flow between the electrodes 15 and 16.

ELECTROLYTE

When the electrolytic cell 12 is filled with a liquid electrolyte 59, electric current will flow between the electrodes 15 and 16. The preferred formulation for this electrolyte 59 is generally that of a conductive salt in solution with water. The preferred embodiment of water is that of either light water (¹H₂0) or heavy water and, preferably deuterium (²H₂0). The purity of all of the electrolyte components is of utmost importance. The water (¹H₂0) and the deuterium (²H₂0) must have a minimum resistance of one megohm with a turbidity of less than 0.2 N.T.U. This turbidity is controlled by the ultra membrane filtration. The preferred salt solution is lithium sulfate (Li₂S0₄) in a 0.5-molar mixture with deionized water and is of chemically pure quality having a resistance of 2 X 10⁶ ohms or greater. In general, although a lithium sulfate is preferred, other conductive salts chosen from the group containing boron, aluminum, sodium, gallium, and thallium, as well as lithium, may be utilized. The preferred pH or acidity of the electrolyte is 9.0.

CELL RESISTANCE In preparing the electrolytic cells for testing, the cell resistance utilizing a Whetstone Bridge or ohm meter was utilized prior to the introduction of the electrolyte into the electrolytic cell. This cell resistance, when dry, should be infinitely high. Otherwise, a short between the anode screen and the cathode beads exists and the unit would have to be repacked. When testing with electrolyte present at 0.02 amps, the resistance should be in the range of 100 to 200 ohms per sq. cm of cross section area as measured transverse to the direction of current flow.

CATALYTIC BEAD CONSTRUCTION A total of eight cell operational test runs are reported herebelow in Tables I and

II. The first test runs, 1 , 2, 3 and 8 reported in Table I herebelow included beads designated as Ni-Pd-Ni beads which utilized a porous non-metallic and non- conductive styrene divinyl benzene core, the only beads used in Run No. 1 having a nickel layer of uniform 1 μ thickness, a palladium layer of uniform 1 μ thickness and a second or outer nickel layer of uniform 1 μ thickness. The beads used in Runs 1 , 2 and 3 also have a copper flash coating formed directly atop the cores. Run 7A used a bead construction having a plated layer of palladium on a sulfonated core built up to 1.0μ to 1.4μ, followed by a 0.6μ plated nickel layer. These layers were deposited by electroless plating, the details of which are fully described in U.S. Patent No. 5,580,838 issued December 3, 1996. Catalytic beads utilized in the remaining test runs 4, 5, 6 and 8 were made using the technique of sputtering for the application of very thin, uniform layers atop the same styrene divinyl benzene core. For beads in these later test runs, nickel was sputtered directly atop the styrene core in preparation for direct adhesion of the first layer of sputtered nickel. Sputtering is preferred because coatings are very uniform, thin, and nearer to full density (about 80%). Moreover, sputtered layers load much faster, typically in as little as about ten minutes as opposed to 1 to 3 hours for plated layers.

A sputtering technique that utilizes a vibrator method to suspend beads during sputtering application of surface thin film coatings has been developed and is the subject of a separate U.S. patent application 08/748,682 filed November 13, 1996 and co-pending with this application. This invention was developed and employed to produce the sputtering samples reported in Test Runs 4 through 8 and facilitated the multiple thin films in Test Runs 6 and 7. The advantage of the sputtering technique as facilitated by this improved application apparatus include the ability to achieve thinner layers with better control of uniformity, the ability to achieve a large number of multiple layers, and the capacity to employ a variety of materials.

The catalytic beads utilized in Test Run #4 had a combination of nickel atop the styrene core, followed by palladium, followed by an outer nickel layer. Catalytic beads utilized in Test Run #5 had two additional layers, first of palladium, then nickel thereatop as did the catalytic beads utilized in Test Run #6. In Test Run #7, the catalytic beads only had a single sputtered layer of nickel formed directly atop the styrene non-conductive core. Catalytic particles utilized in Test Run #8 reported in Table II herebelow utilized a palladium layer sputtered directly atop the styrene core, followed by a sputtered layer of nickel. This test electrolytic cell was specially prepared as a "clean cell" sample to insure that virtually no foreign contamination of any sort would interfere with test results. In general, all of the clean cells have high purity aqueous media circulated in contact with only plastic surfaces to eliminate contact with metal, and thus, no metal contamination is possible.

O 98/03699

RELATIVE SURFACE AREAS

The range in diameters of the conductive particles as above described is relatively broad, limited primarily by the ability to plate the cores and the economic factors involved therein. As a guideline however, it has been determined that there exists a preferred range in the ratio between the total surface area of all of the conductive particles collectively within the electrolytic cell and the inner surface area of the non-conductive housing which surrounds the bed of conductive particles.

A minimum preferred ratio of the total bead surface area to the inner housing surface area is in the range of 5 to 1 (5:1). However, an ideal area ratio is 10 to 1 (10:1) and is typically utilized in the experiments reported herebelow. This ratio is thus affected primarily by the size of the conductive particles, the smaller the diameter, the higher the ratio becomes. CELL OPERATION RESULTS

The testing procedures for cell operation incorporated two stages. The first stage may be viewed as a loading stage during which a relatively low level current

(approx. .05 amps) is introduced across the conductive members, that current facilitated by the presence of the electrolyte 59 as previously described.

LOADING

During the initial loading, electrolysis of the aqueous media within the liquid electrolyte occurs so that the hydrogen active surface of the conductive particles fully absorbs and combines with hydrogen, i.e. becomes "loaded". This loading takes about two hours under a current flow through the cell of about 0.05 amps per two (2) cm³ of particle volume. As the particles load with hydrogen, the resistance of the cell will be seen to increase. The cell's resistance measured at constant temperature should be seen to raise about 10%. It is recommended that the loading should proceed at least until the resistance is no longer increasing. As loading proceeds further, a decrease in resistance will appear.

TEST RUN

After hydrogen and/or hydrogen isotope loading of the hydrogen active material into the conductive beads, the current level between conductive members is then incrementally increased, during which time the electrolyte temperature differential is monitored. The temperature of the electrolyte 59 circulating through the electrolytic cell 12 and system 10 was fully monitored, along with temperature differential between thermocouples 70 and 72 and flow rate of the liquid electrolyte 59.

Preferably, and more accurately, in lieu of placing the thermocouple 70 as shown in

Figure 2, the electrolyte inlet temperature was monitored immediately upstream of stopper 54 to more accurately reflect temperature differential (ΔT).

In general, all tabular results herebelow represent data taken on a steady state basis, input and output temperatures of the liquid electrolyte 59 being taken upstream of stopper 54 and at 72, respectively, voltage (v) and current flow (a) across the electrolytic cell 12 measured between terminals or conductors 15 and 16. The flow rate of the liquid electrolyte 59 (ml/min) and calculated wattage input and wattage output and percent yield are also shown. Wattage input to the cell 12 is calculated as the product of voltage (v) X amps (a), while wattage output is calculated based upon a formula for converting calorific heat to power and watts according to a formula -

Watts Out = Flow Rate (liters per minute) x ΔT x 70. As can be seen from these test results, in all cases, after initial loading of the catalytic particles within the cell, excess energy in the form of heated liquid media was found to be present in very significant quantities. Moreover, each of the test runs reported in Tables I and II produced excess heat over a very extended period of time. INITIAL BEAD ANALYSIS

After each of these test runs, the reacted beads were removed from each cell for thorough testing which included gamma scanning, electron microscopy and mass spectrometry. The top layer of reacted beads next to the anode of each test cell was taken and washed with deionized water. A separate sample of the identical unreacted virgin beads was also washed with deionized water.

Equipment used for mass spectral analysis was a Camica 5F (SIMS)

Secondary Ion Mass Spectrograph and a Nuclear Activation Analysis System (NAA) developed by the University of Illinois for use with the TRIGA research nuclear reactor. For Auger probing of samples, an auger electro spectroscope (AMS) by Perkin Elmer was utilized. A scanning electron microscope (SEM) by Hatachi was also used for surface observations.

Each of the samples of reacted beads were tested with a Geiger-Mueller scanning for gamma rays with negative results, as was the check for tritium in the liquid medium. A portion of each of the reacted beads was also placed on an x-ray sensitive film for a period of five days with no significant flogging detected.

TEMPERATURE ENDOTHERMIC AND EXOTHERMIC TRANSMUTATIONS IN BEADS

Results of the mass spectrograph analysis on one sample of unreacted beads sample from Test Run #2 are shown in Figure 3. A corresponding mass spectral analysis of the reacted beads from the same cell from Test Run #2 are shown in

Figure 4. Each of these sets of mass spectral analysis process data was taken at the University of Illinois and, as reported in more detail in the paper entitled Nuclear

Transmutations in Thin-Film Nickel Coatings Undergoing Electrolysis, by George H.

Mi ley and James A. Patterson presented at the 2nd International Conference on Low

Energy Nuclear Reactions, Texas A & M, College Station, Texas, published in the Journal of New Energy, Vol. 1 , #3, page 5.

RUN NO. 8

An example of a more thorough analysis of this processed data is shown in

Table III herebelow. These results were taken with respect to the palladium/nickel catalytic beads used in the test cell in Run #8 reported hereinabove. Table III shows the isotopic shifts with error bars, while Table IV shows the isotopic shifts overlapping with other elements. The fact that such a large number of elements have a non-natural isotopic distribution indicates that they cannot be attributed to impurities entering the coating. These exact amounts of select elements before and after running were determined by NM while the isotope shifts are from SIMS measurements.

Run No. 8 lasted for 310 hours and employed an entering electrolyte temperature of approximately 60°C. Termination of the run was made prior to any noticeable deterioration of thermal performance. A temperature rise across the cell of less than 0.5°C was obtained throughout the run, representing an output of 0.5± 0.4 watts. Calibration corrections due to heat losses and flow-pattern variations prevented a more accurate measurement, but the output always indicated a positive excess heat.

The cell employed for the run used all plastic fittings with the exception of the pressure and flow meters and the pump. (To further decrease possible impurity sources, a loop with all plastic components except for the electrodes was developed for subsequent runs. As noted later, this modification did not cause a noticeable change in film products.) Titanium electrodes were used. A filter fitted with 0.8-μm pore size filter paper was inserted in the loop to collect any fine particles entering the electrolyte, either from film surfaces or from other parts of the system. Table III

Characteristics of the 650-A Ni film microspheres used in run #8 are summarized in Table IV. A 650-A-thick Ni film was laid down by sputtering the Ni on to a 1-mm plastic core. The thickness of the layer was determined by weighing a calibration sample coated under the same conditions as the microspheres in the sputtering unit. Some coating variations, estimated to be ±30%, can occur among the 1000 microspheres used in the cell, however. Measurements with an Auger electron probe on selected microspheres confirmed the film thickness to be reasonable uniform (±20%).

TABLE IV DATA FOR NICKEL COATED MICROSPHERES (#60)

Total Mass of a microsphere (g) 6.11 E-04

Total Mass of metal on a microsphere (g) 2.04E-06 Total Atoms of metal 2.09E+16

ELEMENT DEPTH PROFILES

Data from an Auger Electron Scan (AES) profile measurement on a typical microsphere are presented in Table V herebelow for the higher concentration elements. While the isotopes' profile behaviors are hard to interpret quantitatively, several observations can be made. Most profiles peak in the nickel volume or near the film-plastic interface, suggesting an internal source rather than diffusion in from the surface. For example, the key elements Ag and Fe peak near the Ni-plastic interface, (at '650 A corresponding to about 12 min. sputtering time). Cu peaks further out in the film. While this data strongly infers an internal source, amplitude of the peaks is too small to draw quantitative conclusions about an internal source versus diffusion inward from the electrolyte. This depth profile data, however, shows that contamination from the surface was impossible. TABLE V Tabulated atomic % vs. Depth from AES Scan

ENERGETICS OF TRANSMUTATIONS The energetics of the cell operation can be explained as follows. The array of elements observed in the metal film after a run are attributed to nuclear transformations induced by light ion (e.g. H, D, ...) absorbed in the metal film (e.g. Ni in run # 8). For the metals selected, the ratio of absorbed ions to metal ions can approach unity. According to other studies using flat plate electrodes, a high loading of this type is necessary and this requirement seems reasonable for the present thin film case. Indeed, the loading is observed qualitatively in the experiment by following the voltage change during the initial hour of the run.

After the run, a large number of new elements attributed to the transmutation reactions are observed. Knowing the yields of these elements, it is possible to calculate the energy released by the reactions without specifying the detailed reaction channels. This calculation can be illustrated from run # 8 that used Ni films.

The basis concept comes from the well known binding energy curve (Larmash) shown in Fig 5 which was derived (2nd ed.) from Introduction to Nuclear Engineering, by John R. Larmash, at pg. 29. If a light or heavier element with a lower binding energy per nucleon (BE/N) split into elements with a higher binding energy, the e in binding energy is released as excess energy from the reaction (the Q-value for the reaction). A positive Q-value represents, then, an exothermic (+Q) reaction, while a negative Q-value is associated with an endothermic (-Q) reaction. Well known examples of this are fission, i.e. splitting of heavy elements into lighter ones, giving a positive, Q value and fusion, i.e. fusing together of lighter elements to give heavier ones, again with a positive Q value. Thus, fission on Fig 5 proceeds from high mass numbers on the right of the curve to the middle, giving higher BE/N products, while fusion goes from low mass numbers on the left to the center region of the curve, again increasing the BE/N. The case of Run #8 used as an example of the various test runs, where the starting point is Ni (mass no. = 58), is more difficult to analyze since Ni lies near to, but not quite at, the top of the BE/N curve. Thus when the array of products observed occur, some have slightly higher BE/N (giving a positive contribution to the Q-value) while others result in a lower BE/N (negative contribution). Thus a careful accounting of the BE/N for the various products is necessary. Such an accounting is shown in Table VI herebelow.

Delta BE/atm = sum BE/atm products - Sum BE/atm reactants = 25201 V/atm reacted Total watts per cell = Delta BE/atm x atms reacted/sec in Run #8 = 0.302 watts

Note: all binding energies are from Brockhaven National Laboratory's Nuclear Data Center

In Table VI, the eight large yield product elements from N.AA analysis are used. The added elements from SIMS will change the analysis, but the trends will remain and that is the point of this example. Their respective BE/atom are multiplied by the observed atom fraction in the film after the run; the result is then summed and the Ni BE subtracted to obtain the net energy released (overall Q- value) per atom reacting. Note from the "contributions" column that various of the elements have BE/atm lying both above and below Ni. As seen, four elements have a (+) contribution to the BE/atom (i.e. to the Q-value) while four give (-) contributions. The energy released is then converted to an average power output for Run #8 using the run time of 311 hours and the number of atoms in the Ni film (see Texas AM Paper). A positive output of 0.3 watts is found, in good agreement with the 0.5 watt + 0.5 watt observed in the experiment. This calculation then demonstrates that the observed excess power can be accounted for in a straightforward manner by summing the (+) and (-) Q- values for the various nuclear transmutation reactions involved. The fact that both (+) and (-) Q-value reactions occur in such cells had not been realized prior to this discovery.

Clearly, as seen from Table VI, the output power depends on differences between two large numbers, making it very sensitive to the transmutations occurring, i.e. to the starting material and the reaction conditions (e.g. loading, temperature, electrolyte, etc.). These factors affect the reaction channels and the balance of + versus - Q-values that result. The channels are also strongly dependent on the bead design and metals, plus the cell operating conditions. For example, in Run #2 of Table I, a multiple 2-layer coating of nickel and palladium was used to increase the excess power up to 4.5 watts vs. the 0.5 watt for Run #8, using a single film of nickel. Two important additional conclusions can be drawn from this example.

First, other experimenters have had difficulty with reproducibility of excess power (heat) experiments using a variety of "other" cell configurations, typically with flat plate type electrodes. In view of the example above, this is understandable. Just small differences in set up can throw the positive vs. negative Q balance off, causing this non-reproducibility. On the other hand, even when non-measurable excess power is observed, transmutations can occur, allowing the detection of products possible without excess heat. In this sense, transmutation experiments are not so sensitive to conditions and this is viewed as the reason the present experiments (e.g. Run #8) are reasonable reproducible. A second point is that, recognizing the delicate Q-value balance involved in production of excess power, and knowing the various products obtained from different starting materials as obtained in the present experiments, it becomes possible to tailor bead designs/operating conditions to maximize heat production or to emphasize certain transmutation products. The multi-layer run cited earlier is only one example of applying this knowledge. This energy balance model (termed RIFEX in the reference paper in the Journal of New Energy by George Miley), combined with the isotope production rate ("yield") versus A plot in Figures 7a and 7b, have a number of important implications. The energetics shown in Table VI are consistent with a reaction initiated by a proton plus the base metal element (Ni in the example used for Run #8). In order to create elements with mass numbers lying both above and below the base element A number, this reaction (presumed to be a fusion reaction), must lead to a heavier element of mass A' (A'>A for the base element) which then breaks up or "fissions" into fragments yielding the elements observed, i.e. representing the process by which transmutation occurs. The heavier element undergoing fission will be termed the "compound nucleus". This breakup can be understood by analogy to the well- known process for neutron-induced fission. In that case, the compound neutron- uranium nucleus undergoes a binary breakup into two fragments, one light and one heavy mass element. The sum of the mass numbers for the two fragments add up to the mass of the uranium plus neutron (less a small conversion to energy released by ΔMC², Einstein's famous relation). The present compound nucleus can be viewed as playing the role of uranium, and the fission breakup viewed in a similar fashion.

In the uranium fission case, the output energy can be calculated from the mass difference between the compound nucleus and the fission products. In the present case, however, the creation of the compound nucleus from the proton plus base element consumes energy, so the net release is the mass difference between the initial reactants (e.g. proton plus Ni in Run #8) and all of the products. Indeed, that is the basis for the previous energetics calculations in Table VI.

It is possible to roughly identify the compound nuclei involved from the production rate versus the data of element A in Figures 7a and 7b. From that figure, it is observed that the minimum yield points lie between peaks in yield as summarized in Table Vl-A below. Compound Nucleus 2 (Min A)

80

160

320

640

The peak yield regions on the "sides" of each minimum point are viewed as the fission fragments that result from the breakup of the compound nucleus. For mass conservation then, the compound nucleus must lie at an A value of ~ 80, 160,

320, 640, .

This result, in addition to explaining the basic process involved in the transmutation studies, has a number of very important implications. By selection of the base element, the mix of products can be varied. For example, if a base element of mass A" with A" > 160 is used, the compound nucleus mass will lie above 160, i.e.

320, 640, . Then the fission of the compound nucleus will lead to an array of product elements with light-heavy pairs having mass sums equaling 320, 640, .

This then predicts not only a number of standard elements as products, but some new stable heavy elements not yet identified.

Another consequence is that it becomes feasible to select base elements such that the transmutation process, in addition to element production, can produce excess energy in the form of heat. Indeed, as both the experiment and energy balance calculations show, excess heat production (in addition to transmutated elements) occurred for the Ni coating in Run #8. Excess heat was also obtained in other runs shown in Table I.

ELEMENT AND ISOTOPE CONCENTRATIONS

Results from NAA and EDX analysis of high concentration elements (Mg.

Al, Si, Ag, Cr, Fe, Zn and Cu) in the Ni run are summarized and compared in Table VII. (Two NAA runs on the microspheres yielded values within 10% of those shown for NAA in the table.) The variation in concentrations observed is attributed to the fact that each analysis used a different sampling of micro- spheres taken from various locations in the packed bed at the end of the run. Some differences are expected from microsphere to microsphere due to variations in location and coating. Further, the NAA results provide total concentrations for a sample of 10 microspheres, while EDX examined only a small volume of an individual microsphere. Still, the important point is that these independent measurements confirm that following a run, over 40 atom % of the film consists of these elements, the reminder being the host Ni plus trace elements.

TABLE VII Comparison of NAA and EDX Analysis for Several Microspheres ANALYSIS COMPARISON (Atomic %)*

* Microspheres taken from same location in the packed bed.

** Ni % (from NAA) adjusted for a total of 100%

NA: Not included in analysis

NL: Percentage below detection limit To evaluate the other major non-NAA elements present and to obtain isotopic concentrations, SIMS and NAA data have been combined in Table III (above). NAA elements are listed in bold. (Light elements, still under study, and other isotopes not observed are omitted from Table III.) This table shows the yield, i.e., the difference between the final and initial weight for each isotope (fourth column). NAA only measured the elemental concentrations; therefore the NAA values for a given element have been pro-rated between isotopes according to the SIMS isotopic analysis to obtain isotopic concentrations. Corresponding values for the number of atoms of each isotope before ("fresh MS") and after ("reacted MS") a run follow in the fifth and sixth columns. Non- NAA elements used the SIMS data directly for both the element yield and the isotope values, based on the instrument sensitivity (RSF) interpretation discussed in the referenced Journal of New Energy paper. REACTION PRODUCT SYSTEMATICS

PRODUCTION RATES

Based on the yield data presented earlier in Table III, time-averaged element production rates are computed in Table VIII and plotted in Figs 6a and 6b in terms of weight fraction of the metal film/s-cm³ of film and atoms/s-cm³ of film, respectively. These figures assume that the production rate was constant over the 310 hour run. There is some preliminary indication that the rate is higher at the start, and the time dependence, along with the effect of microsphere location, is now under study.

Table vin Production rate data

later, due to the formation of heavy elements like Cu, Ag and Cd, some endothermic reactions "absorb" energy. Thus the 0.5 W excess must be viewed as "net" energy release from these various reactions.

The corresponding total increase in element masses, or in element atoms, are presented in Figs 7a and 7b, respectively. Consistent with the production rate graphs, these figures show total yields per microsphere approaching 0.1-0.2 μg for high yield elements, or 3-6 atomic % per element in the metallic film.

ISOTOPE SHIFTS FROM NATURAL ABUNDANCE

Differences between the isotopic percentage concentrations observed with the SIMS vs. those for natural abundance for the reaction product elements, listed earlier in Table 111, right hand column (Δa/o) are summarized in Figure 8. The accuracy of these measurements is estimated to be of order of ±3% in the difference when high resolution is employed. High resolution was used to eliminate possible line overlap in all important cases, but with the large number of elements found, this was not possible for all of the lower yield isotopes. Thus, those results must be viewed as less certain. Of the higher concentration elements, Fe and Zn show significant deviations. Cr and Ag are in the ±3-5% range, while Cu is the ±1% range. Many low-concentration elements show quite large differences, e.g. Ti-50, +77.7%, Ge-72, +21%, Se-82, +32%, Zr-96, +97%; etc. There are no obvious patterns, however.

To further study the deviation from natural abundance for the vital isotopes of Cu (Cu-63 and -65) and Ag (Ag-107 and -109) special NAA isotope measurements (described in the referenced Journal of New Energy paper) were carried out. Illustrative results for the Ni run, #8, based on a sample of 10 microspheres, indicates a deviation from natural % abundance of +3.6 ± 1.6% for Cu-63 and -8.1 ± 3.6% for Cu-65. (Since the two results are from different lines, unlike SIMS, slightly different values can occur in the + and - values for pairs.) These results are to be compared to a deviation of +0.8% for Cu-63 and -0.8% for Cu-65 from the SIMS data. The reason for larger percent difference from the NAA analysis than from SIMS is not clear. A possible explanation is that as stressed earlier, the SIMS results are localized on a spot on a single bead film whereas the NAA value represents the ratio of total amounts of each isotope contained in the films on the 10 microsphere sample. In any case, both methods show a deviation from natural abundance.

The trend in the Cu shifts found here is similar, but smaller, than reported by Mizuno et al. (1996) who cite Cu-63, +25% and Cu-65 -25%. Shifts for Fe have been reported in articles by Mizuno, T, T. Ohmori, and M. Enyo, 1996,

"Changes of Isotope Distribution Deposited on Palladium Induced by

Electrochemical Reaction" and Ohmori, T, and M. Enyo, 1996, "iron Formation in

Gold and Palladium Cathodes", Journal of New Energy, 1, 1, 15-22 and are compared to results in Table IX. While differences are observed, two isotopes,

56 and 57, do show the same trend for all cases.

TABLE IX

Isotope Shifts Reported in Fe in Various Systems

*Electrode Material (a) Not Reported

In summary, a large number of elements produced in these various runs (e.g. > 30 in Run #8) showed a measurable deviation from the isotope ratios found in natural elements. This appears to be conclusive proof that nuclear transmutation reactions are occurring and is entirely consistent with the increased concentration of these elements found in the metallic coatings after a run. It is concluded, then, that the electrolytic cell described in this disclosure is capable of carrying out nuclear transmutation reactions for the production of a variety of elements, i.e. elements absent or in low concentration in the original metallic coating. Further, an inspection of the data shows that the production of desired elements can be enhanced by judicious selection of the element(s) used for the metallic coating.

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 method of producing product elements by low temperature nuclear transmutation during electrolysis in an aqueous media, at least one said product element produced being present only after operation of an electrolytic cell in accordance with said method in an unnatural isotopic ratio which is shifted from an isotopic ratio of natural abundance, comprising the steps of:

A. providing said electrolytic cell including: a non-conductive housing and an inlet and an outlet; a first conductive porous grid positioned within said housing adjacent to said inlet; a second conductive porous grid positioned within said housing spaced from said first conductive grid and adjacent to said outlet; a plurality of conductive beads each including: a non-conductive core; a uniform thin conductive layer of a metallic material forming a conductive surface over said non-conductive core, said metallic material being a metallic hydride which combines with hydrogen or an isotope of hydrogen during operation of said cell;

B. circulating said aqueous media through said electrolytic cell;

C. passing an electrical current between said first and second grids when said aqueous media is circulating within said electrolytic cell.

D. operating said cell in accordance with steps B and C for a time period sufficient to produce a desired quantity of product elements.

2. A method as set forth in Claim 1 , wherein: said metallic hydride is taken from the group consisting of palladium, lanthanum, praseodymium, cerium, titanium, zirconium, vanadium, tantalum, uranium, hafnium, and nickel.

3. A method as set forth in Claim 1 , wherein: said conductive layer is relatively high in density and is formed by sputtering.

4. A method as set forth in Claim 1 , wherein: said conductive layer has a uniform thickness in the range of about 500 to

1000 angstroms.

5. A method as set forth in Claim 1 , wherein said product elements include: elements lying in nuclear mass number bands in a range of between about

25 to 35, 50 to 66, 74 to 85, 105 to 120, and 204 to 208.

6. A method as set forth in Claim 5, wherein said elements include:

Si, Al, Cr, Mn, Fe, Cu, Ti, Se, Zn, Ag, Cd, Hg and Pb.

7. A method as set forth in Claim 1 , wherein: said product elements have mass numbers which are both higher and lower than a mass number of a corresponding said metallic hydride.

8. A method of producing product elements from initial elements present in an electrolytic cell prior to its operation by low temperature nuclear transmutation during electrolysis in an aqueous media within said cell, at least one of said product elements being produced by said method exhibiting an unnatural isotopic ratio which is shifted from an isotopic ratio of natural abundance, comprising the steps of: A. providing said electrolytic cell including: a non-conductive housing and an inlet and an outlet; a first conductive porous grid positioned within said housing adjacent to said inlet; a second conductive porous grid positioned within said housing spaced from said first conductive grid and adjacent to said outlet; a plurality of conductive beads each including: a non-conductive core; said initial elements including a first nickel layer of uniform thickness formed atop a non-conductive core, a palladium layer of uniform thickness formed atop said first nickel layer and having high hydrogen adsorption capabilities, and a second nickel layer of uniform thickness formed atop said palladium layer;

B. circulating said aqueous media through said electrolytic cell;

D. operating said cell in accordance with steps B and C for a time period sufficient to produce said nuclear transmutation and said product elements, said product elements having both higher and lower atomic number than an atomic number of a corresponding said initial element from which said product elements are produced.

9. A method as set forth in Claim 8, wherein each said conductive bead further comprises: a second palladium layer of uniform thickness formed atop said second nickel layer; a third nickel layer of uniform thickness formed atop said second palladium layer.

10. A method as set forth in Claim 9, wherein: said palladium layers and said nickel layers are formed by sputtering and are of high density and highly uniform.

11. Product elements exhibiting isotopic shifts which differ from those corresponding isotopes of natural abundance formed by the process of: A. providing said electrolytic cell including: a non-conductive housing and an inlet and an outlet; a first conductive porous grid positioned within said housing adjacent to said inlet; a second conductive porous grid positioned within said housing spaced from said first conductive grid and adjacent to said outlet; a plurality of conductive beads each including: a non-conductive core; a uniform thin conductive layer of a metallic material forming a conductive surface over said non-conductive core, said metallic material being a metallic hydride which combines with hydrogen or an isotope of hydrogen during operation of said cell;

B. circulating said aqueous media through said electrolytic cell;

5 C. passing an electrical current between said first and second grids when said aqueous media is circulating within said electrolytic cell.

D. operating said cell in accordance with steps B and C for a period sufficient to produce said nuclear transmutation.

12. Product elements as set forth in Claim 11 , wherein: l o said product elements have mass numbers which are higher and lower than a mass number of a corresponding said metallic hydride.

13. Product elements as set forth in Claim 12, wherein: said product elements are produced during Step D as a result of low temperature nuclear reaction forming a compound nucleus which 15 then fissions to produce said product elements.