WO1999019881A1 - Low temperature electrolytic nuclear transmutation - Google Patents

Abstract

A method for producing low temperature nuclear transmutations by electrolysis in an aqueous media. New elements produced by transmutation are identified as having discrete peaks in occurrence by atomic number (Z) and by atomic mass (A). New complex nuclei produced by transmutation are idendified as having existed based upon the nature and occurrences of fission transmutation elements produced. 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 & 44) positioned therein. A plurality of cross-linked polymer non-metallic cores each having a uniform conductive exterior metallic surface formed of a high hydrogen absorbing 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 grids (38 & 44).

Description

LOW TEMPERATURE ELECTROLYTIC NUCLEAR TRANSMUTATION

BACKGROUND OF THE INVENTION

This is a continuation-in-part of U.S. provisional application No. 60/028,551 filed October 15, 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, characteristics of major groups of transmutation products, and isotopic distributions of heretofore unknown products. 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 (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 thereon 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 enhances 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 throughout. 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, where transmutations, in part, show the distinct characteristics of isotopes that have shifted in ratios of occurrence from those of natural abundance and of high temperature fission reactions. 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 conductive beads each having preferably cross linked polymer non-metallic cores and a uniform conductive exterior thin-film 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 a 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 a wide range of atomic masses lying both below and above that of the original metallic coating.

It is still another object of this invention to provide new elements produced by low temperature nuclear transmutation in an electrolytic cell which exhibit the double yield peaks in elemental product distribution which is characteristic of nuclear fission reactions. 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. Figures 3-A to 3-E are graphic presentations of the data shown in Table III of production rates vs. mass numbers taken from each of the individual test runs. Figure 4 is a graph presenting all of the data for all test runs shown in Table III.

Figures 5-A to 5-F are graphic presentations of the data shown in Table IV of production rates vs. atomic numbers (Z) taken from each of the individual test runs.

Figure 6 is a graph presenting all of the data shown in Table IV for all of the test runs. Figures 7-A to 7-F are graphs presenting the data shown in Table V of isotopic shifts vs. mass numbers from each of the test runs.

Figure 8 is a graph presenting all of the data shown in Table V for all of the test runs.

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 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 is 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. The various embodiments of these conductive beads 36 which are tested are described in detail below. About 1000 beads (-0.5 cm³ in volume) were used in each packed bead bed 35.

Still referring to Figure 2, a nonconducive 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 nonconductive mesh 40 is a plurality of nonconductive 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 nonconductive 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 nonconductive 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 nonconductive 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

( H₂0) the, preferable form being light water. 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 (Li₂S0 ) in a 1.0-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 six (6) cell operational test runs are reported and analyzed herebelow.

These test runs, numbered 5, 7A, 8, 11 , 13 and 18C, the physical and operational performance results of which are reported in Tables I and II herebelow. These beads utilize either a porous non-metallic and non-conductive styrene divinyl benzene (PS) core or a glass (GL) core having thin-film outer layers of nickel (N) and/or palladium (P) of uniform thickness formed thereon. Thus a PS/P/N microsphere has a plastic core with a first coating of palladium an a second coating of nickel. All coating were sputtered on, unless denoted as =E which used electroplating. Excess power measurements varied vary from run to run, but the PS/N run was typical for single coatings. It gave a temperature rise of the order of 0.5 °C throughout the run, representing an output of 0.5 ± 0.4 W. Multi-layers gave larger excess power, approaching 4 W. Calibration corrections due to heat losses and flow-pattern variations limited the measurement accuracy.

CELL OPERATION 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". Loading of hydrogen into the thin-films done at low (~25°C) temperatures. 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 and at an eventual equilibrium voltage level of ~2-3 V. 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 cell inlet temperature is also slowly raised over about 4-8 hours to a maximum allowed using the present cell construction (-60° to 70°C). 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 below 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. Likewise, the middle and lower layers of reacted beads were removed and treated similarly. A separate sample of the identical unreacted virgin beads was also washed with deionized water.

Equipment used for mass spectral analysis was a Cameca IMS 5F (SIMS) Secondary Ion Mass Spectrometer and a Nuclear Activation Analysis System (NAA) developed by the University of Illinois for use with the TRIGA research nuclear reactor. For Auger depth probing of samples, an auger electron spectroscope (AMS) by Perkin Elmer was utilized. A scanning electron microscope (SEM) by Hitachi was also used for detailed surface observations.

Each of the samples of reacted beads was 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.

By using a unique thin-film electrode configuration to produce and isolate the transmutation region, along with measurements based on neutron activation analysis, for the first time a quantitative measure of the yield of transmutations products has been achieved. Results from a thin-film (650A) nickel coating on 1-mm microspheres in a packed-bed type cell with 1 -molar LiS0₄-H₂0 electrolyte are now presented herebelow for thin-film Pd and Ni and for multiple Pd/Ni layers. The transmutation products in all cases characteristically divide into four major groups of elements with atomic number l≡ 6-18; 22-35; 38-55; 75-85. Yields of ~1 mg of key elements were obtained in a cell containing ~1000 microspheres (~1/2 cc). In several cases, over 40 atom % of the metal film consisted of these products after two weeks of operation.

Scattered observations of some nuclear transmutation products generated during electrolytic cell operation, typically employing Pd and heavy or light water with various electrolytes, have been reported by other researchers, e.g. see the proceedings of the First and Second International Conferences on Low Energy Nuclear Reactions (Bockris and Lin, 1996a; Bockris, Miley and Lin 1996b). However, these reports have typically dealt with impurity level quantities of elements, complicating the distinction from impurities and making quantitative evaluation impossible. In sharp contract, the thin (-600A) films used in present work result in transmutation of a significant percentage of the metal in the thin-film cathode. That result, combined with Neutron Activation Analysis (NAA) and Secondary Ion Mass Spectrometry (SIMS), provides a quantitative measure of the amounts of the various elements produced. Over a dozen experiments with various thin-film coatings have been carried out in different cells. Thin-film coatings on 1-mm-diameter plastic microspheres, ranging from 500-A-thick single layers of Pd or Ni to multiple Ni/Pd layers, were used in a flowing packed-bed-type electrolytic cell with a 1 -molar Li₂S0₄, light water electrolyte. Nuclear reaction products were obtained in all cases, with several runs resulting in concentrations of over 40 atomic % of the metallic film being Fe, Si, Mg, Cu, Cr, Zn and Ag. Six key runs, listed in Tables I and II are presented below.

Scanning electron microscope (SEM), photographs of the microspheres confirmed that a very smooth surface was achieved but with a small-scale, rough structure uniformly distributed over it. Some erosion of small particle and occasional ejection of larger "flakes" from the film occurs during operation as detected by debris collected by the loop filter. Concurrently, various fragile looking bead-like and fiber- like structures are typically visible on the film surface after electrolysis. REACTION PRODUCT ANALYSIS METHODS Reaction product measurements have utilized a combination of NAA, SIMS, energy dispersive x-ray (EDX) analysis, and Auger electron spectroscopy (AES). NAA can measure total quantities of elements in a sample containing multiple microspheres, while the other techniques are restricted to probing a local area on single microspheres. Due to variations among microspheres arising from location in the packed bed and other effects, this difference in technique is important for interpretation of results. NAA ANALYSIS

Both the microspheres and electrolytes were analyzed before and after the run. Sampling after a run was done by disassembling the cell and removing microspheres from different layers in the packed bed. (The approximate 1000 microspheres in the bed result in approximately 3-5 layers total). NAA of the microspheres was carried out at the University of Illinois' (Ul) TRIGA research reactor, typically using 10 microspheres. Techniques for short- and long-lived NAA were performed to determine the presence of Ag, Cu, Al, Fe, Cr, Zn, Ni, Co, and V, subsequently termed "NAA Elements". Typical detection limits were of the order of 2 ppm, with a precision of 2-10%. NAA was also employed to study key isotope ratios (e.g., Cu and Ag) for comparison to natural abundance. Calibration used certified liquid standards from the National Institute of Standards and Technology (NIST). Ores containing known quantities of these elements were analyzed simultaneously for quality control in all runs. SIMS ANALYSIS The SIMS analysis employed a Cameca IMS 5F unit operating with 8-keV oxygen primary beam in the positive ion mode (Wilson et al., 1989). Scans of key isotopes were made using single microspheres in a low-resolution (2,000 mass resolution) mode at several depths of interest. High-resolution (up to a maximum of 40,000 mass resolution) scans were then done to resolve any interferences involving important isotopes. Elements measured by SIMS, but not NAA, are termed "non- NAA elements". Calibration for the SIMS sensitivity was done using the measured concentration of the nine NAA elements (Table 3) to determine isotope ratios except for the Cu and Ag ratios that were determined explicitly by NAA. EDX ANALYSIS The EDX analysis used a Field Emission Electron Microscope (Hitachi S-800) operating in the energy dispersion analysis mode to detect elements with atomic concentrations above about 1%. This measurement largely served as added confirmation of NAA measurements. AES was used in a sputtering mode to perform semi-quantitative depth profiling for the major element species above 1 atom %. TRANSMUTATION TEST RESULTS

ELEMENT AND ISOTOPE CONCENTRATION

Results from NAA analyses of the net (final minus initial values) yields of high concentration elements in various runs are summarized in Table 3 showing mass number (A) and corresponding production rate or yield for beads taken from cells of each said test run. Element yields as high as several μg/microsphere are obtained, representing roughly a mg of these high yield elements per cell (1000 microspheres). The corresponding time average reaction rates are of order 10¹⁶ (atoms/cc film-sec). The data in Table III is presented graphically in Figs. 3A-3F. All of this data is combined in Fig. 4.

To evaluate the concentration of the non-NAA elements present and to obtain isotopic ratios, SIMS and NAA data were combined. Results for all elements observed in the six runs are shown in Fig. 6, which plots the data shown in Table IV of production rates vs. Z. NAA element values are thought to be quite accurate. The non-NAA element values are less certain due to uncertainties in the SIMS sensitivity calibration (i.e. "RSF" values) and the restricted location of the measurement on a single microsphere, but the results should still provide a good estimate of non-NAA isotopes. Further, note that the isotopic yields for NAA elements should be quite accurate, since the RSF values are constant for isotopes of a given element, while the total concentration of these elements are directly from NAA measurements. ELEMENT DEPTH PROFILES

Data from AES profile measurements show that most element profiles distinctly peak in the metal volume or near the metal-core interface, suggesting an internal source rather than diffusion in from the surface. However, the amount of peaking varies among elements and runs, complicating the interpretation of this measurement. Still, the results provide significant support for the conclusion that the elements observed did not diffuse in from the surface. NUCLEAR RADIATION EMISSION

In view of evidence shown in Table 3 and Fig. 4, that products are formed at a significant rate in an operating cell, measurable radiation emission would normally be expected. For example, assuming a rate of about (10¹⁶ reactions/cc film-sec.) x (10^"6 cc film) x (10³ microspheres) x (1 gamma/reaction) indicates ~10=¹³ gammas/sec. However, several attempts to date to measure nuclear radiation emission-neutrons, gammas, or x-rays-during cell operation have not detected any measurable quantities above background. Likewise, several attempts to measure gamma ray emission from microspheres removed from the cell after a run also failed to uncover signals above background. Thus, it must be concluded that to uncover signals above background. Thus, it must be concluded that transmutation products are created by a relatively slow process, leading to near stable products.

Recently, several sets of PS/N microspheres (run ~4 months earlier) were exposed to high-speed ASA 3000 film (Klema, 1996) for a four-day period with positive results. Unfortunately, these experiments are not very reproducible. A second positive exposure has been obtained, but three additional attempts failed. The technique is under study and, if verified, will demonstrate emission of low-energy beta rays or soft x-rays (estimated to be of the order of 20keV).

SYSTEMATICS The yields for both NAA and non-NAA elements have been converted to element production rates in Table IV and in Fig. 6 to remove differences arising from variations in the length of runs. The rates shown are average values over the run. As indicated in Fig. 6, the composite data of maximum production rates can be enclosed in an envelope (shown) with four distinct peaks at Z -13, 30, 47, and 82. The largest production rates (hence, yields) lie in bands around each peak. This striking result has a close resemblance to the well-known two-peak yield curve for neutron-induced fission of uranium (Katcoff, 1960). For that case, the peaks are associated with light and heavy fission products arising from the break-up

(fission) of the neutron-uranium compound nucleus. Thus, one interpretation for the present results is that the peaks of Fig. 6 also represent the fission of compound nuclei, created in this case by proton-metal reactions. The startling fact that elements in the higher Z peaks lie above the host metals (Ni or Pd) would then require multi-atom fusion to form a compound nucleus capable of fissioning into these high-Z products.

Comparison of the production rates vs. Z data shown in Figures 5A to 5F for the individual runs provides further important insight. Runs #8 and #18c, both of which used 650-A Ni film on a plastic core, are shown in Figs. 5C and F. However, they were done four months apart in different laboratories (U of Illinois and CETI, FL, respectively) with different cells. The most recent run (#18c shown in Figure 3F) used an ultra pure cell, the only metal parts being titanium electrodes, and highest purity electrolyte (99.996% LiSO₄) with an additional pre-run with "sacrificial-microspheres" for added purification. With these added precautions, impurity levels in the electrolyte in run #18c were reduced by a factor of 4-5 compared to the earlier run #8. But still more reaction products were observed in run #18c than in run #8 (62 element vs. 36 respectively), while the absolute rates for high yield elements and the four peak characteristic remains fairly similar. In that sense, the reproducibility of the experiment appears quite goods. In the sense that products with characteristic four-peak behavior have been obtained in the dozen plus experiments attempted to date, the reproducibility is excellent.

Run #13 (G/N) in Fig. 5-E employed Ni on a glass (vs. plastic) core. This resulted in a distinct decrease in products in the third and fourth groups (higher Z) and slightly reduced the yields in the first and second groups. This results suggests that the core material plays a role in the reaction mechanism.

The PS/P (palladium) core experiments shown in Figure 5-D also show a "four-peak" behavior, but, unlike the corresponding Ni runs, the amplitudes of the peaks decrease progressively in going to high-Z. Also, there appears to be a void of products between the third and fourth peaks.

The two multi-layer runs #5 and #7a shown in Figures 5A and 5B follow the same general trend as the single layer runs. Physically the beads used #7a differed from those of

#5 by having fewer layers (2 vs. 5), used much thicker (~1 μm vs. 300-500A) layers made by electroplating. Run #5 in particular shows a rich array of products (similar to the PS/N run #18c) whereas run #7a in Figure 5-B has few products in the region of the third and fourth yield peaks. Interestingly, the multiple layers also produced the most excess heat of all six runs (see Table 1).

The general view is that heavy elements generally involve low or negative Q-values

(endothermic reactions) whereas light elements involve positive Q-values (exothermic reactions). This explains why reacting products apparently can occur without a large heat production. Since the net balance involves differences in large numbers, small changes affect the ability to produce heat. These phenomena can be explained in terms of the formation of intermediate complex nuclei which are formed by the initial reaction, but which immediately decompose and fission. By complex nucleus, we mean a weakly bound nucleus composed of a coalescence of one or more metallic atoms from the thin-film material, plus protons from the electrolyte. The binding is due to a weak pairing of neutrons and protons in the nucleus, enabled by the unique conditions created by the electrolytic loading of protons in the solid-state lattice of the metallic coating. An example of such a complex, given later in Table VIII, is the reaction of twenty protons plus five Ni58's to create a complex nucleus of mass 310. As discussed later, this complex nucleus quickly decays to lower mass complexes (40, 76, 194 per Table VIII), which in turn, are unstable in fission to produce the observed transmutation products.

This behavior is further explained with reference to Figs. 3A to 3F, which show the spread of fission products for the various runs having different metal coatings on the beads. The "reference" runs with Ni coatings, shown in Figures 3D and 3F, gave transmutation products with high concentrations in all four of the ranges of mass A~30-40, 50-80, 110-130,

190-210. In sharp contrast, the run with a Pd coating resulted in transmutation products having high concentrations in the first two of these ranges, that is A~30-40, 50-80. As discussed in more detail later, this can be explained by the observation that the Ni-proton reaction favors formation of the complex at A=310, which decomposes and fissions into transmutation products with masses lying below A=310, i.e. covering all four of the mass ranges cited above (A-30-40, 50-80, 110-130, 190-210), as seen in Figures 3C and 3F. On the other hand, Pd reaction protons to predominantly recreate the complex nucleus 116, which decomposes and fissions to produce transmutation products with masses lying below

A=116, predominantly falling into the lower two mass ranges A~30-40, 50-80, as seen in

Figure 3D.

An important point is that the initial reaction between the metal and protons favors formation of the lowest mass complex nucleus, which can be created by a whole number of protons plus the metal. Thus, twenty protons plus five Ni-58 combine to give the complex of

A=310, while twelve protons plus one Pd-104 combine to give the nuclear complex A=116.

Consequently, it is possible to deliberately select base metals that will combine with protons to create more of the desired complex nuclei, and in turn favor production of desired ranges of transmutation products. Some examples of this are given in Table VIII. Coatings employing Ag-107, Bi-209 or Ti-48 predominantly create the nuclear complex at A=116, favoring lower mass range transmutation products. A coating of Th-232 predominantly creates a nuclear complex at A=234, which results in high concentrations of transmutation products at the intermediate mass ranges.

ISOTOPE SHIFTS The change in % abundance of the various isotopes as measured by SIMS relative to natural abundance is summarized in Fig. 8 (change<2% suppressed for clarity). From this result, it is seen that a majority of the isotopes observed have shifts. The larger values, marked with element symbols, are typically low-yield elements although some high-yield elements have significant shifts. Since Cu and Ag are key heavy elements, further confirmation for their shifts have been obtained from NAA. First results for Cu for run #8 with PS/N gave Cu-63; +3.6 ±1.6%;

Cu-65: -8.1 ±3.6% while corresponding SIMS value in (Fig. 5-D) are Cu-63: +0.8%, Cu-65: -

0.8%. While there are differences in absolute magnitude compared to SIMS, the positive and negative trends agree. The differences are attributed to the localized nature of the SIMS values compared to NAA results, which represent an average over the 10 microsphere samples employed.

In summary, despite variations in the individual runs, the data strongly supports the conclusion that significant deviations from natural abundance occurred. IMPURITY ISSUES

The use of thin-films introduces a potential impurity problem in reaction product studies due to the small volume occupied by the film vs. the large volume of the electrolyte.

Consequently, NAA measurements of the nine "NAA elements" were made on samples of microspheres, electrolytes and filter paper both before and after a run. (SIMS measurements were also done on microspheres before and after runs.) Quantities of these

NAA elements found prior to the run were consistently <10% of that found after the run

(except for Al which was initially higher in some cases). Analysis of other cell components, i.e. the anode and plastic did not uncover significant impurity concentrations of the NAA elements. Other tests included a "null" run with electrically conductivity sulfonated plastic beads used to simulate metal coated beads. Substitution of platinum for the titanium anode did not affect results. Various runs presented here used three entirely different cells. The first PS/Ni run employed some metal fittings in the loop which were thereafter substituted out in favor of plastic. Run #13 used an entirely new all plastic cell (the electrodes being the only metal components) with electrolyte that was first run with "sacrificial" PS/N microspheres for a week (to collect impurities on the miαospheres) before new microspheres were loaded and used for the actual run.

No impurity concentrations near the magnitude of the NAA elements in the film following the runs were identified with these exhaustive tests, strongly supporting the conclusion that these elements were produced by nuclear transmutations. In conclusion, the finding that the masses of the key isotopes following a run are large compared to possible sources of such isotopes from loop components. The negative results from simulation runs without Ni or Pd films, the observation of isotope shifts from natural abundance, and the observation that the isotopes vary with film material all combine to provide evidence that the reaction products reported are not caused by impurities. OVERVIEW

The key characteristic of the reaction products found in the thin-film measurements above described is a grouping of high-yield elements in roughly four "zones" of mass number. This pattern is clearly seen in Figure 8. Additional key experimental observations that appear to be characteristic of these reactions include a lack of high-energy radiation, the production of nearly stable elements, the observation of low-energy X-ray or beta radiation for beads following a run, and non-natural isotope occurrence ratios.

Further, since reaction products have been observed consistently in twenty runs using various metal films at the University of Illinois, the thin-film configuration appears to be an effective method to "initiate" reactions. Also, unlike solid electrode experiments that appear to have local active regions, sometimes giving volcanic-like spots on the electrode surface, the thin films appear to react more uniformly. While the film surface is roughened during a run, no significant local artifacts have been observed from SEM studies.

The yield pattern in Figure 8 resembles a fission spectrum with valleys of low yield lying at A = 20, 38, 97, and 155. This suggests that the corresponding compounding nuclei, lying at A = 40, 76, 194 and 310 fission to produce the pattern of light and heavy products on each side of the valleys. These compound nuclei, termed complexes, designated X* are theorized to be created through Bardeen-Cooper-Schrieffer (BCS) pairing of neutrons and protons. The corresponding liquid drop model predicts that the observed complexes are marginally unstable to fission. The initial complex immediately breaks up into several lower mass complexes, which then undergo fission into an array of products. The fission fragmentation for this pairing and the corresponding reduced energy is predicted to yield near-stable elements, in agreement with the experiment. The overall reactions involved are summarized in Table VII where reactions involving Ni and Pd corresponding to data from runs in Figure 8 are shown along with various possible reactants (thin-film materials). The reactants generally "funnel" into the lowest mass quasi-stable complex available, in these cases X* = 116, 232 and 310. This in turn determines the "breakup" states. Again, a consistency with the experiment is observed because Ni (runs 8 and 18c) gives high yields in all four mass number regions, whereas Pd has the highest yields at the two lower mass number regions.

As seen from Figure 8, this is consistent with the predicted breakup of the postulated complex nuclei. While these events proceed sequentially, the overall result is the combination of a large number of protons with the base metal nuclei as shown in brackets in

Table VII. It is interesting that predicted preference for reactions with Th, Ag, Bi and Ti to form lower mass number complexes is also in generally agreement with other unpublished results. TABLE I

TABLE II CATALYTIC BEAD DATA

A. PS/N/P/N/P/N (#59; used in Run #5)

B. PS/P/N-E (#C1 ; used in Run #7A)

C. PS/N (#60; used in Run #8)

D. PS/P (#63; used in Run #11 )

E. G/N (#61 ; used in Run #13)

F. PS/N (#76; used in Run #18c)

TABLE III

TABLE IV

TABLE V

ZSS8I/-.6Sn/lDd βz 18861/66 OΛV

ZSS8I/-.6Sf-ΛL3d ε 18861/66 OΛV

ZSS8I/-.6SflΛLDd Z£ 18861/66 OΛV

ZSS8VL6SIΛ/JLDd εε 18861/66 OΛV TABLE VI YIELD FOR NAA ELEMENTS

Yield (micro-grams / microsphere)

Element Z Run #5 Run #7A Run #8 Run #11 Run #13 Run #18C

TABLE VII Production Rate (atoms / s - cc of microsphere)

Element Z Run #5 Run #7A Run #8 Run #11 Run #13 Run #18C

TABLE VIII Illustrative Complex Nuclei Pathways

* [20p + 5Ni-58] = (X*)-310 = X*-194 + X*-76 + XMO

* [12p + Pd-104] = (X*)-116 = X*-76 + XMO

* [2p + Th-232] = (X*)-234 = X 94 + XMO

* [9p + Ag-107] = (X*)-116 = X^*-76 + XMO

* [33p + Bi-209] = (X*)-232 = 2X*-116 = 2X*-76 + 2XM0

* (20p + 2T 8 = (X*)-116 = X^*-76 + XMO

Claims

What is claimed is: 1. A method of producing product elements by low temperature nuclear transmutation during electrolysis in an aqueous media, said product elements produced being present only after operation of an electrolytic cell in accordance with said method having yields of transmutation products which demonstrate peaks in atomic numbers (Z) only in the ranges of 10 to 15, 25 to 30, 45 to 50 and 80 to 85, 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 readily combining with hydrogen or an isotope of hydrogen present in said aqueous media 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 said product elements.

2. A method as set forth in Claim 1 , wherein: said metallic hydride is taken from the group consisting of elements known for being capable of absorbing large quantities of hydrogen, namely palladium, lanthanum, praseodymium, cerium, titanium, zirconium, vanadium, tantalum, uranium, hafnium, and nickel.

3. A method of producing product elements by low temperature nuclear transmutation from initial elements present in a packed bed of conductive beads of an electrolytic cell during electrolysis in an aqueous media within said cell, said product elements being produced by said method characterized as clustering or peaking in nuclear atomic numbers (Z) primarily only at discrete atomic numbers, 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; said conductive beads each including: a non-conductive core; one or more thin-film outer layers of uniform thickness formed atop said non-conductive core, each said layer having a thickness in the range of 1000 angstroms (A) and high hydrogen adsorption capability;

B. circulating said aqueous media including lithium sulfate 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 said nuclear transmutations and said product elements, said product elements peaking at said discrete atomic numbers equal to about 13, 30, 47 and 82.

4. Product elements produced by low temperature nuclear transmutation and characterized as having peaks of atomic numbers (Z) at in the range of 6 to 18, 22 to 35, 38 to 55 and 75 to 85, said product elements 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; 5 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 l o 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. 15 D. operating said cell in accordance with steps B and C for a period sufficient to produce said nuclear transmutation.

5. A method of producing product elements by low temperature nuclear transmutation during electrolysis in an aqueous media, said product elements produced being present only after operation of an electrolytic cell in accordance with 20 said method having yields of transmutation products which demonstrate peak occurrences of product element having mass numbers (A) only in the ranges of 30 to 40, 50 to 80, 110 to 130 and 190 to 210, comprising the steps of: A. providing said electrolytic cell including: a non-conductive housing and an inlet and an outlet; 25 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: 30 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 readily combining with hydrogen or an isotope of hydrogen present in said aqueous media 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 o sufficient to produce said product elements.

6. A method as set forth in Claim 5, wherein: said metallic material is palladium and said product elements have mass numbers primarily in the range of 30 to 40 and 50 to 80.

7. A method as set forth in Claim 5, wherein: 5 said metallic material is nickel.

8. A method as set forth in Claim 5, wherein: said metallic material is palladium and nickel and said product elements have mass numbers primarily in the range of 50 to 80.

9. Product elements produced by low temperature nuclear transmutation and 0 characterized as having peaks of mass numbers (A) at in the range of 30 to 40, 50 to

80, 110 to 130 and 190 to 210, said product elements 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 5 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; 0 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 period sufficient to produce said product elements.

10. A method of producing complex nuclei by low temperature nuclear transmutation during electrolysis in an aqueous media, said complex nuclei produced being present during operation of an electrolytic cell in accordance with said method, 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 readily combining with hydrogen or an isotope of hydrogen present in said aqueous media 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 said complex nuclei, said complex nuclei having mass numbers of 40, 76, 116, 194, 232 and/or 310.