β-radiation voltage effect device

Abstract

This disclosure relates to apparatus for generating electrical energy, methods for generating electrical energy, products used in apparatus for generating electrical energy, and methods for manufacturing apparatus for generating electrical energy. In some embodiments, this disclosure provides an electrical energy generating apparatus. The apparatus includes at least one battery comprising: a spaced-apart first electrode and a second electrode, the first electrode comprising a low work function material and the second electrode comprising a high work function material; and a semiconductor material and a radioactive nuclide emitting beta particles disposed between the first electrode and the second electrode, the semiconductor material being capable of generating electron-hole pairs in response to beta particle emission from the radioactive nuclide.

Description

[0001] Priority Statement

[0002] This application claims priority to Australian Provisional Patent Application No. 2019901722, filed on 21 May 2019, and Australian Provisional Patent Application No. 201990172322, filed on 21 May 2019, the contents of which are incorporated herein by reference. Technical Field

[0003] This disclosure relates to apparatus for generating electrical energy, methods for generating electrical energy, products used in apparatus for generating electrical energy, and methods for producing apparatus for generating electrical energy. Background Technology

[0004] Electrochemical devices are widely used to generate electricity. These devices rely on conventional chemical reactions to provide power, but their lifespan is limited in themselves without recharging or refueling. Rechargeable electrochemical devices can extend the lifespan of electrochemical energy devices, but they are also subject to many of their own limitations, especially as the devices lose their rechargeability over time.

[0005] Devices that convert ionizing radiation into electrical energy have also been developed. For example, devices that generate electricity using beta radiation have been developed and are commonly referred to as "beta radiation voltaic effect" devices. Such devices have attracted great interest in fields requiring long-term power output or where power supply replacement or maintenance is impractical.

[0006] Given the vast amounts of waste radionuclides generated historically and in the future by various processes, it would be advantageous to power such devices with the unique high-energy particle emission capabilities of these waste radionuclides. This would provide economic and / or environmental benefits associated with utilizing the aforementioned waste radionuclides.

[0007] However, although beta-radiation photovoltaic devices have been developed, they typically have many limitations, such as low conversion efficiency, low power output, and / or shortened lifetime due to radiation damage.

[0008] This disclosure relates to a beta-radiation photovoltaic effect device capable of generating electricity using a variety of different radionuclides that emit beta particles, and as discussed herein, it overcomes one or more disadvantages of the prior art and / or provides one or more advantages. Summary of the Invention

[0009] This disclosure relates to apparatus for generating electrical energy, methods for generating electrical energy, products used in apparatus for generating electrical energy, and methods for producing apparatus for generating electrical energy.

[0010] Some embodiments of this disclosure provide an energy generating device, the device including at least one battery, the battery comprising:

[0011] A first electrode and a second electrode are spaced apart, the first electrode comprising a low work function material and the second electrode comprising a high work function material; and

[0012] A semiconductor material and a radioactive nuclide that emits beta particles are disposed between a first electrode and a second electrode, wherein the semiconductor material is capable of generating electron-hole pairs in response to beta particle emission from the radioactive nuclide.

[0013] Some embodiments of this disclosure provide a method for generating electricity, the method comprising generating electricity using an energy generating apparatus as described herein.

[0014] Some embodiments of this disclosure provide a method for generating electrical energy, the method comprising:

[0015] A potential difference is generated between a closely spaced first electrode and a second electrode, wherein the first electrode comprises a low work function material and the second electrode comprises a high work function material.

[0016] High-energy beta particles emitted from a radioactive nuclide generate electron-hole pairs, which are in close proximity to a semiconductor material disposed between the first and second electrodes. These electron-hole pairs are movable under the influence of an electric field.

[0017] The electron-hole pairs are captured into an external circuit by utilizing the electric field existing between the electrodes;

[0018] This generates electrical energy.

[0019] Some embodiments of this disclosure provide a method for generating electrical energy, the method comprising:

[0020] An electric field is generated between a first electrode and a second electrode spaced apart, the first electrode comprising a low work function material and the second electrode comprising a high work function material, and the electric field is generated due to different Schottky junctions at the two different electrodes;

[0021] High-energy beta particles emitted from a radioactive nuclide generate electron-hole pairs, which are in close proximity to a semiconductor material disposed between the first and second electrodes. These electron-hole pairs are movable under the influence of an electric field.

[0022] The electron-hole pairs are captured into an external circuit by utilizing the electric field existing between the electrodes;

[0023] This generates electrical energy.

[0024] Some embodiments of this disclosure provide an apparatus for generating electrical energy using the methods described herein.

[0025] Some embodiments of this disclosure provide a product comprising a first material having a low work function, a second material having a high work function, a semiconductor material disposed between the first material and the second material, and a radionuclide emitting beta particles, the semiconductor material being capable of generating electron-hole pairs in response to beta particle emission from the radionuclide.

[0026] Some embodiments of this disclosure provide an electrical power generation apparatus including products as described herein.

[0027] Some embodiments of this disclosure provide a method for generating electrical energy, the method including using a product as described herein.

[0028] Some embodiments of this disclosure provide a method for producing an electrical energy generating device, the method comprising incorporating one or more batteries into the electrical energy generating device, the one or more batteries comprising a spaced first electrode and a second electrode, the first electrode comprising a low work function material and the second electrode comprising a high work function material, and a semiconductor material disposed between the first electrode and the second electrode and a radionuclide emitting beta particles, the semiconductor material being capable of generating electron-hole pairs in response to beta particle emission from the radionuclide.

[0029] Some embodiments of this disclosure provide an electrical energy generating apparatus produced by the methods described herein.

[0030] Other embodiments are disclosed herein. Attached Figure Description

[0031] To better understand this disclosure, and to more clearly illustrate how this disclosure may be implemented according to one or more embodiments thereof, reference will be made to the accompanying drawings by way of example.

[0032] Figure 1 The diagram shows that semiconductor materials for beta-radiation photovoltaic devices can occupy any position within a space defined by three end members: (i) a pure semiconductor polymer with suitable electronic properties; (ii) a semiconductor single-phase composite material, including an inorganic compound chemically compounded with a polymer (typically containing nitrogen and / or sulfur heteroatoms); and (iii) a crystalline semiconductor with a defined chemical composition and stoichiometry. Semiconductor materials can include mixtures or blends (at the nanoscale) between any two end members or between all three end members. Detailed Implementation

[0033] This disclosure relates to apparatus for generating electrical energy, methods for generating electrical energy, products used in apparatus for generating electrical energy, and methods for producing apparatus for generating electrical energy.

[0034] This disclosure is based on the understanding that electrical energy can be generated using a device that utilizes a semiconductor material disposed between electrodes having different work functions and exposes the semiconductor material to a radionuclide that emits beta particles. In response to the emission of beta particles from the radionuclide, electron-hole pairs are generated in the semiconductor material, which, combined with the potential difference between the electrodes, generate electrical energy.

[0035] Without being bound by theory, this disclosure is based on the potential difference generated between a first and second electrode spaced apart by forming different Schottky junctions at two different electrodes. Upon excitation by high-energy β particles emitted by a radioactive nuclide doped in the semiconductor material, electron-hole pairs are generated within the semiconductor material. These electron-hole pairs generated within the material are mobile under the influence of an electric field. Utilizing the potential difference existing between the two different electrodes, the electron-hole pairs are swept into an external circuit, thereby generating electrical energy.

[0036] Certain embodiments of this disclosure relate to products and methods having a combination of one or more advantages. For example, some advantages of some embodiments disclosed herein include one or more of the following: new and / or improved apparatus for generating electrical energy; new methods for converting beta emissions from radionuclides into electrical energy; generating electrical energy using radioactive materials previously considered waste; producing apparatus capable of powering specialized long-distance power needs; producing beta-volt effect electrical energy generating apparatus with improved resistance to radiation-induced damage; beta-volt effect apparatus that allows selection of radioactive isotopes with different half-lives to power the apparatus, thereby achieving different overall lifetimes required for specific applications; compliance of the materials used in producing the battery to allow for scalable automated manufacturing methods; solving one or more problems and / or providing one or more advantages, or providing a commercial alternative. Other advantages of certain embodiments of this disclosure are also disclosed herein.

[0037] Some embodiments of this disclosure provide an electrical energy generating device.

[0038] Some embodiments of this disclosure provide an energy generating device, the device including at least one battery, the battery comprising:

[0039] A first electrode and a second electrode spaced apart, the first electrode comprising a low work function material and the second electrode comprising a high work function material; and

[0040] A semiconductor material and a radioactive nuclide that emits beta particles are disposed between a first electrode and a second electrode, wherein the semiconductor material is capable of generating electron-hole pairs in response to beta particle emission from the radioactive nuclide.

[0041] As used in this article, the term "battery" refers to a functional unit used to generate electrical energy.

[0042] In some embodiments, the device includes more than one battery. In other embodiments, the device includes multiple batteries. An appropriate number of batteries can be selected based on the desired characteristics of the device. Methods of electrically connecting a single battery to achieve current flow are known in the art.

[0043] The dimensions of the first and second electrodes can be selected based on the properties of the materials used in the electrodes and the desired characteristics of the power generation device.

[0044] In some embodiments, the first and second electrodes are separated by a distance ranging from 0.3 to 100 micrometers. In some embodiments, the first and second electrodes are separated by a distance ranging from 0.5 to 30 micrometers. Other distances are taken into consideration.

[0045] In this embodiment, an inter-electrode electric field is generated between the closely spaced first and second electrodes using the different Schottky junctions at each electrode. The Schottky junction formed between the semiconductor and the first electrode comprising a low work function material will have a different barrier height, depletion width, and energy distribution than the Schottky junction formed at the second electrode comprising a high work function material. In summary, the electric fields associated with the two different Schottky junctions can reinforce each other to provide a considerable macroscopic field for collecting charge carriers into external circuitry.

[0046] Methods for determining the work function of a material are known in the art and include methods that utilize electron emission from the sample induced by photon absorption (optical emission), high temperature (thermal electron emission), electric field (field electron emission), or measurement using a Kelvin probe. Related methods leverage the difference in work function between the sample and a reference metal.

[0047] In some embodiments, the first and / or second electrodes comprise a metal. In some embodiments, the first and / or second electrodes comprise a non-metal. In some embodiments, the first and / or second electrodes comprise a composite material (e.g., a cermet). In some embodiments, the first and / or second electrodes comprise a material that has been treated (e.g., coated) to alter the work function of the electrode.

[0048] Low work function materials and high work function materials are commercially available and / or can be produced by methods known in the art.

[0049] In some embodiments, the low work function material includes materials having a work function of less than 3.0 eV.

[0050] In some embodiments, the low work function material includes materials having a work function of 2.5 eV or less. In some embodiments, the low work function material includes materials with a work function in the range of 2.7 to 3.5 eV.

[0051] In some embodiments, the low work function material comprises metals and / or intermetallic compounds.

[0052] As used in this article, the term "metal" refers to one or more metals, or a material containing a significant proportion of metals.

[0053] In some embodiments, the low work function material is essentially a pure elemental metal. In some embodiments, the low work function material comprises two or more metals. In some embodiments, the low work function material comprises one or more metals and other materials. In some embodiments, the low work function material is an alloy.

[0054] As used herein, the term "intermetallic compound" refers to a material composed of two or more metals with defined stoichiometry, and may also contain other nonmetallic elements, such as Mg₂Ca, Al₂Ca, Mg 17 Al 12 Materials.

[0055] In some embodiments, the low work function material comprises a metal and / or a metal-containing compound, the metal-containing compound comprising one or more of the following: europium, strontium, barium, samarium, calcium, magnesium, cerium, sodium, lithium, potassium, rubidium, cesium, dysprosium, neodymium, gadolinium, terbium, holmium, erbium, thulium, lanthanum, scandium, thorium, yttrium, and ytterbium. These low work function materials are commercially available and / or can be produced by methods known in the art.

[0056] In some embodiments, the low work function material includes samarium metal. Samarium metal is commercially available.

[0057] Other examples of low work function materials include Ag-O-Cs, WO-Ba, Sc2O3, and LaB6, all of which are commercially available or can be produced by methods known in the art.

[0058] In some embodiments, the low work function material comprises a metal. In some embodiments, the low work function material comprises a mixture of metals. In some embodiments, the low work function material comprises a metal treated (e.g., coated) with another material to alter the work function of the electrode.

[0059] In some embodiments, the low work function includes nonmetals.

[0060] In some embodiments, the low work function material includes composite materials. In some embodiments, the low work function material includes materials that have been treated to alter the work function of the material.

[0061] In some embodiments, the high work function material includes materials with a work function greater than 4.0 eV. In some embodiments, the high work function material includes chemical elements with a work function greater than 4.0 eV.

[0062] In some embodiments, the high work function material comprises metals and / or intermetallic compounds.

[0063] In some embodiments, the high work function material is essentially a pure elemental metal. In some embodiments, the high work function material comprises two or more metals. In some embodiments, the high work function material comprises one or more metals and other materials. In some embodiments, the high work function material is an alloy.

[0064] In some embodiments, the high work function material comprises one or more metals selected from nickel, platinum, silver, gold, aluminum, cadmium, cobalt, chromium, copper, beryllium, bismuth, cadmium, iron, gallium, mercury, indium, iridium, manganese, molybdenum, niobium, osmium, lead, palladium, rhenium, rhodium, ruthenium, antimony, silicon, tin, tantalum, technetium, titanium, vanadium, tungsten, zinc, and zirconium. These high work function materials are commercially available and / or can be produced by methods known in the art.

[0065] In some embodiments, the high work function material includes nickel metal.

[0066] In some embodiments, the high work function material comprises a metal. In some embodiments, the high work function material comprises a mixture of metals. In some embodiments, the high work function material comprises a metal treated with another material to alter the work function of the electrode.

[0067] In some embodiments, the high work function material includes nonmetals.

[0068] In some embodiments, the second electrode comprises a ceramic-metal composite material (i.e., a cermet material).

[0069] In some embodiments, the high work function material includes composite materials. In some embodiments, the high work function material includes materials that have been treated (e.g., coated) to alter the work function of the material.

[0070] The radionuclides that emit beta particles are known in the art and commercially available, and can also be obtained from sources derived from discarded radioactive products, byproducts of fission reactors, and legacy radionuclides produced for industrial, medical, or research purposes.

[0071] In some embodiments, the radionuclide that emits beta particles is derived from discarded radioactive material.

[0072] Examples of radionuclides that emit beta particles include 90 Sr, 99 Tc, 3 H, 14 C, 63 Ni, 137 Cs, 147 Pm, 151 Sm, 121m Sn, 155 Eu, 93 Zr, 126 Sn, 60 Co, 210 Pb, 90 Y, 129 I, 188 W, 35 S, 121m Sn, 123 Sn, 45 Ca, 106 Ru, 170 Tm, 171 Tm, 134 Cs, 32 Si, 113 Cd and 79 One or more of Se. The radionuclides may be provided in a suitable chemical form for use in various embodiments of this disclosure.

[0073] In some embodiments, the radionuclide includes 90 Sr, 99 Tc, 3 H, 14 C, 63 Ni, 137 Cs, 147 Pm, 151 Sm, 121m Sn, 155 Eu, 93 Zr, 126 Sn, 60 Co and 210 One or more of Pb.

[0074] In some embodiments, the radionuclide comprises a single type of radionuclide. In some embodiments, the radionuclide comprises two or more different types of radionuclide.

[0075] In some embodiments, the radionuclide includes an isotope that eventually decays into a stable isotope / nucleus, for example... 90 Sr and 126 When Sn is present, the isotope emits multiple β-particles through its decay daughter radionuclide chain.

[0076] It should also be understood that a single radioactive beta decay event leads to a cascade of secondary electrons extending from the original decaying atom to tens of micrometers (μm), and each of these secondary electrons can potentially result in multiple excited electronic states within the semiconductor. Furthermore, it should be understood that the radionuclide may undergo multimode emission.

[0077] In some embodiments, the radionuclide has one or more of the following preferred characteristics: (i) the radionuclide emits β-particles with energies in the range of 1-100 keV; (ii) the radionuclide emits β-particles at a rate depending on its half-life, which is in the range of 1-40 years, for example about 5 years (to minimize replacement intervals); (iii) the radionuclide is an isotope of an element with readily processable chemistry; and (iv) the radionuclide emits β-particles with little or no associated gamma (γ) radiation emission.

[0078] In some embodiments, the radionuclide is dispersed in the semiconductor material.

[0079] In some embodiments, the radionuclide is incorporated into the chemical structure and / or structural framework of the semiconductor material.

[0080] In some embodiments, the radionuclide is at 10 -1 GBq / mm 3 Up to 10 4 GBq / mm 3 The specific activity within a certain range is incorporated into the semiconductor material. A suitable specific activity can be selected based on the desired characteristics of the power generation device.

[0081] In some embodiments, the semiconductor material includes a composite semiconductor material.

[0082] In some embodiments, an adhesive material is used to deposit, coat, or fuse the semiconductor material to at least one of the electrodes. Methods for depositing, coating, or fusing materials are known in the art.

[0083] In some embodiments, the semiconductor material includes a single-phase composite semiconductor material.

[0084] In some embodiments, the single-phase composite semiconductor material comprises an inorganic semiconductor chemically composited with a polymer.

[0085] In some embodiments, the inorganic semiconductor includes a band gap of at least 1.1 eV.

[0086] Examples of inorganic semiconductors include one or more of halides and chalcogenides, which are commercially available or can be produced by methods known in the art.

[0087] In some embodiments, the inorganic semiconductor includes one or more of the following: cesium halide, rubidium halide, potassium halide, lead halide, bismuth halide, antimony halide, arsenic halide, tellurium halide, tin halide; tellurides of zinc, cadmium, mercury, gallium, indium, thallium, germanium, tin, lead, arsenic, antimony, bismuth, and selenium; selenides of zinc, cadmium, mercury, gallium, indium, thallium, germanium, tin, lead, arsenic, antimony, bismuth, and tellurium; and sulfides of zinc, cadmium, mercury, gallium, indium, thallium, germanium, tin, lead, arsenic, antimony, bismuth, and selenium.

[0088] In some embodiments, the single-phase composite semiconductor material comprises a halide chemically composited with a polymer. For example, the halide can undergo supramolecular composite formation with nitrogen or sulfur atoms in the polymer.

[0089] In some embodiments, the inorganic semiconductor includes one or more of BiI3, PbI2, CsPbBr3, CsPbI3, CsPbCl3, CsSnI3, CsSnBr3, and CsSnCl3.

[0090] Other inorganic semiconductors include, for example, ZnS and / or CdSe, both of which are commercially available and / or can be produced by methods known in the art.

[0091] In some embodiments, the polymer includes nylon, polyimide, polythiophene, polypyrrole, polyacrylonitrile, polyurethane, polycarbazole, polyaniline, polysulfide, polysulfone, polysulfide, polythiocarbonate, polysulfate, polyurethane, polysulfoximine, and polysulfonium salt, or a mixture of one or more of the above polymers.

[0092] In some embodiments, the single-phase composite semiconductor material comprises a polymer and a high concentration of the inorganic semiconductor. For example, the single-phase composite semiconductor material may have a concentration of at least 50% (w / w) or in the range of 50% to 95% (w / w) of the inorganic semiconductor.

[0093] In some embodiments, the inorganic semiconductor and the radionuclide are different types.

[0094] In some embodiments, the inorganic semiconductor includes the radioactive nuclide. For example, the inorganic semiconductor may be... 210 PbI2 and / or Bi 129 I3. These compounds are commercially available or can be produced by methods known in the art.

[0095] In some embodiments, the radionuclide is mixed with the polymer. In some embodiments, the radionuclide is dispersed together with the polymer. In some embodiments, the radionuclide is located near the polymer. In some embodiments, both the polymer and the semiconductor are present in particulate form, and the particulates are present in a mixture with the semiconductor.

[0096] In some embodiments, the radionuclide is incorporated into the chemical structure of the polymer. Methods for incorporating a radionuclide into a polymer are known in the art and include, for example, using a suitable radionuclide (e.g., 3 H or 14 C) Labeled monomers, or the use of a gaseous form of a radionuclide (e.g., tritium) incorporated into the polymer through exchange.

[0097] In some embodiments, the radionuclide is mixed with the polymer. In some embodiments, the radionuclide is dispersed in the polymer. In some embodiments, the radionuclide is located near the polymer. In some embodiments, both the polymer and the radionuclide are present in particulate form, and the particulates are present in a mixture with the semiconductor.

[0098] In some embodiments, the radionuclide is incorporated into the chemical structure of the polymer, and the inorganic semiconductor is mixed with the polymer.

[0099] In some embodiments, the radionuclide forms part of the inorganic semiconductor, and the inorganic semiconductor is mixed with the polymer.

[0100] In some embodiments, the radionuclide, the inorganic semiconductor, and the polymer are all in particulate form, and the particulates exist in a mixture.

[0101] In some embodiments, the radionuclide is incorporated into a higher-order structure present in a material comprising the inorganic semiconductor, for example, into voids in an irregular structure present in the inorganic semiconductor.

[0102] In some embodiments, the semiconductor material comprises a semiconductor polymer. The semiconductor polymer (and / or its monomeric components) is commercially available or can be produced by methods known in the art.

[0103] In some embodiments, the semiconductor polymer includes one or more of polythiophene, polyacetylene, polyphenylene oxide, polypyrrole polyphenylene sulfide, polyaniline, polyvinylacetylene, polypyrrole, polyindole, polyethylene, polyazine, and organoboron polymers. Examples include P3HT and PEDOT polymers. Other types of polymers are considered.

[0104] In some embodiments, the radionuclide is mixed with the semiconductor polymer. In some embodiments, the radionuclide is dispersed with the semiconductor polymer. In some embodiments, the radionuclide is located near the semiconductor polymer. In some embodiments, both the semiconductor polymer and the radionuclide are present in particulate form, and the particulates are present in a mixture with the semiconductor.

[0105] In some embodiments, the radionuclide is incorporated into the chemical structure of the semiconductor polymer. Methods for incorporating a radionuclide into a polymer are known in the art and include, for example, using a suitable radionuclide (e.g., 3 H or 14 C) Labeled monomers, or the use of gaseous radionuclides (e.g., tritium) incorporated into the semiconductor polymer through exchange.

[0106] In some embodiments, the semiconductor material includes semiconductor polymers and additional semiconductors.

[0107] Other examples of semiconductors include one or more of halides, chalcogenides, oxides, nitrides, carbides, perovskites, borides, tellurides, selenides, antimonides, germanides, arsenides, sulfides, silicides, phosphides, aluminides, carbon allotropes, and intermetallic compounds, all of which are commercially available and can be produced by methods known in the art.

[0108] In some embodiments, the additional semiconductor includes one or more BiI3, PbI2, CsPbBr3, CsPbI3, CsPbCl3, CsSnI3, CsSnBr3, and CsSnCl3. Other inorganic semiconductors include one or more of, for example, PbZrO3, PbTiO3, SrTiO3, SrZnO3, and (K,Cs)TaO3, all of which are commercially available.

[0109] In some embodiments, the semiconductor material comprises the semiconductor polymer and a low concentration of the additional semiconductor. For example, the semiconductor material may have a concentration of at least 5% (w / w) or in the range of 5% to 50% (w / w) of the additional semiconductor in the semiconductor polymer.

[0110] In some embodiments, the semiconductor material comprises the semiconductor polymer and an additional semiconductor, and the radionuclide forms part of the additional semiconductor.

[0111] In some embodiments, the semiconductor material comprises the semiconductor polymer and the additional semiconductor, and the radionuclide, the additional semiconductor, and the semiconductor polymer are all in particulate form, and the particulates are present in a mixture.

[0112] In some embodiments, the semiconductor material comprises the semiconductor polymer and the additional semiconductor, and the radionuclide and / or the additional semiconductor are dispersed in the matrix of the semiconductor polymer.

[0113] In some embodiments, the semiconductor material includes a crystalline semiconductor.

[0114] In some embodiments, the crystalline semiconductor comprises one or more of nitrides, carbides, halides, mixed chalcogenides, tellurides, selenides, antimonides, germanides, arsenides, silicides, phosphides, aluminides, carbon allotropes, perovskites or other complex oxygen-containing anionic crystalline phase materials, simple oxides, doped oxides, sulfides, borides, and intermetallic compounds, all of which are commercially available or can be produced by methods known in the art. In some embodiments, the crystalline semiconductor comprises one or more of titanates, zirconates, molybdates, vanadates, technetates, pertechnetates, tungstates, niobates, tantalates, doped tin oxide, doped zinc oxide, hafnium oxide, germanium oxide, cobaltates, ferrates, and manganates, all of which are commercially available or can be produced by methods known in the art. Other crystalline semiconductors are considered.

[0115] In some embodiments, the crystalline semiconductor comprises titanate and / or zirconate.

[0116] In some embodiments, the crystalline semiconductor includes one or more of strontium zirconate (SrZrO3), strontium titanate (SrTiO3), and titanium oxide.

[0117] In some embodiments, the crystalline semiconductor has one or more of the following preferred properties: low electron-hole recombination rate; high electron and hole mobility under the influence of an electric field; melting point of at least 250°C; oxidation resistance; hardness; strength; resistance to impact fracture, corrosion, and / or wear. Methods for evaluating the above properties are known in the art.

[0118] In some embodiments, the crystalline semiconductor includes a band gap of at least 2.0 eV. In some embodiments, the crystalline semiconductor has a band gap of at least 2.6 eV. In some embodiments, the crystalline semiconductor has a band gap of at least 3.1 eV. In some embodiments, the crystalline semiconductor has a band gap of at least 3.2 eV. In some embodiments, the crystalline semiconductor has a band gap of at least 3.4 eV. In some embodiments, the crystalline semiconductor has a band gap of 2.6 to 5.4 eV, 3.1 to 5.4 eV, 3.2 to 5.4 eV, or 3.4 to 5.4 eV. Methods for determining the semiconductor band gap are known in the art and are generally expressed relative to a standard hydrogen electrode.

[0119] In some embodiments, the crystalline semiconductor has the characteristic of high charge carrier mobility.

[0120] In some embodiments, the semiconductor material comprises a crystalline semiconductor and the radionuclide comprises... 90 Sr、 99 Tc, 3 H, 14 C 63 Ni、 137 Cs、 147 Pm, 151 Sm、 121m Sn、 155 Eu、 93 Zr、 210 Pb, 60 Co and 126 One or more of Sn. Other radionuclides that emit beta particles are also considered.

[0121] In some embodiments, the radionuclide is incorporated into the chemical or structural framework of the crystalline semiconductor.

[0122] In this respect, the radioactive nuclide can be, for example, an atom that can enter the lattice of the crystalline semiconductor to make a substitution, for example... 90 Sr replaces a portion of the strontium (Sr) in the lattice of strontium titanate (SrTiO3). In another embodiment, the radionuclide may be an atomic or ionic compound that can occupy vacancies or other structural defects in the lattice.

[0123] In some embodiments, the radionuclide is at 10 -1 GBq / mm 3 Up to 10 4 GBq / mm 3 A specific activity within a certain range is incorporated into the crystalline semiconductor. A suitable specific activity can be selected based on the desired characteristics of the power generation device.

[0124] Methods for incorporating radioactive nuclides into crystalline semiconductors are known in the art.

[0125] In some embodiments, the radionuclide is incorporated into the chemical or structural framework of the crystalline semiconductor. Methods for incorporating a radionuclide that emits beta particles into the chemical or structural framework of a crystal are known in the art and include, for example, isotope exchange using an isotope concentration gradient.

[0126] In some embodiments, the radionuclide is incorporated into the chemical or structural framework of the crystal semiconductor by replacing one or more suitable atoms in the lattice of the crystal semiconductor with the radionuclide (substitution doping), by incorporating the radionuclide interstitial material into the framework of the crystal semiconductor, or by incorporating the radionuclide into vacancies or voids in the structural framework.

[0127] In some embodiments, the radionuclide is incorporated into a less ordered structure present in the crystalline semiconductor, for example, into voids present in an irregular structure in the semiconductor.

[0128] In some embodiments, the semiconductor material comprises the crystalline semiconductor and a binder. In some embodiments, the semiconductor material comprises the crystalline semiconductor and a polymer binder.

[0129] In some embodiments, the binder material is used to deposit, coat, or fuse the semiconductor material to at least one of the electrodes. Methods for depositing, coating, or fusing materials are known in the art.

[0130] In some embodiments, the semiconductor material is deposited, coated, or fused onto the first and / or second electrodes. In some embodiments, the material is deposited, coated, or fused onto the first electrode. In some embodiments, the material is deposited onto the second electrode. In some embodiments, the material is deposited onto both electrodes.

[0131] In some embodiments, the material is deposited on, coated on, and / or fused to one of the electrodes. Methods for depositing, coating, or fusing materials are known in the art.

[0132] In some embodiments, the semiconductor material is in a form suitable for being applied to the electrode by a wet coating process.

[0133] In some embodiments, the device includes a plurality of batteries, each battery comprising an insulating layer between the batteries. The insulating material is known in the art. In some embodiments, the insulating layer is a thin film.

[0134] In some embodiments, the batteries are connected in series. In some embodiments, the batteries are connected in parallel. Methods for connecting the batteries are known in the art.

[0135] The methods for producing electrical energy generating devices as described herein are known in the art.

[0136] In some embodiments, the power generation device described herein can be used in applications requiring long-term power supply, such as military, telecommunications, mining, space, and medical applications. Other applications are also considered.

[0137] The electrical energy generating device described herein may also be referred to herein as a “β-radiation voltaic effect device”, which is a current generator that uses energy from a radioactive source that emits β particles (electrons).

[0138] Some embodiments of this disclosure provide a beta-radiation voltage effect device.

[0139] In some embodiments, this disclosure provides a beta-radiation photovoltaic effect device, the device comprising at least one battery, the battery comprising:

[0140] A first electrode and a second electrode are spaced apart, the first electrode comprising a low work function material and the second electrode comprising a high work function material; and

[0141] A semiconductor material and a radioactive nuclide that emits beta particles are disposed between the first and second electrodes, wherein the semiconductor material is capable of generating electron-hole pairs in response to beta particle emission from the radioactive nuclide.

[0142] This article describes a beta-radiation photovoltaic effect device and its manufacturing method.

[0143] Some embodiments of this disclosure provide a method for generating electrical energy.

[0144] The methods for generating electrical energy are described in this article.

[0145] In some embodiments, this disclosure provides a method for generating electrical energy, the method comprising:

[0146] A potential difference is generated between a closely spaced first electrode and a second electrode, wherein the first electrode comprises a low work function material and the second electrode comprises a high work function material.

[0147] High-energy beta particles emitted from a radioactive nuclide generate electron-hole pairs, which are in close proximity to a semiconductor material disposed between the first and second electrodes. These electron-hole pairs are movable under the influence of an electric field.

[0148] The electric field existing between the electrodes is used to capture electron-hole pairs into an external circuit.

[0149] This generates electrical energy.

[0150] In some embodiments, this disclosure provides a method for generating electrical energy, the method comprising:

[0151] An electric field is generated between a first electrode and a second electrode spaced apart, the first electrode comprising a low work function material and the second electrode comprising a high work function material, and the electric field is generated due to the different Schottky junctions at the two different electrodes;

[0152] High-energy beta particles emitted from a radioactive nuclide generate electron-hole pairs, which are in close proximity to a semiconductor material disposed between the first and second electrodes. These electron-hole pairs are movable under the influence of an electric field.

[0153] The electron-hole pairs are captured into an external circuit by utilizing the electric field existing between the electrodes;

[0154] This generates electrical energy.

[0155] In some embodiments, the potential difference is generated by using materials with different work functions. In some embodiments, the first electrode comprises a low work function material and the second electrode comprises a high work function material.

[0156] This paper describes suitable first and second electrodes, as well as low work function and high work function materials.

[0157] This article describes radionuclides and semiconductor materials. Examples of semiconductor materials are described in this article.

[0158] Certain embodiments of this disclosure provide an apparatus for generating electrical energy using the methods described herein. The method for generating electrical energy using the described method is as described herein.

[0159] Some embodiments of this disclosure provide a product.

[0160] In some embodiments, the product is suitable for use in beta-radiation photovoltaic effect devices.

[0161] In some embodiments, this disclosure provides a product comprising a first material having a low work function, a second material having a high work function, a semiconductor material disposed between the first material and the second material, and a radionuclide emitting beta particles, the semiconductor material being capable of generating electron-hole pairs in response to beta particle emission from the radionuclide.

[0162] The methods for producing the products are as described herein. This document describes low work function materials and high work function materials. This document also describes radionuclides and semiconductor materials.

[0163] In some embodiments, the product is used in the manufacture of batteries. In some embodiments, the product is used in an energy-generating device. Other uses are considered.

[0164] Certain embodiments of this disclosure provide an electrical energy generating apparatus including products as described herein.

[0165] The method of using the product in an electrical energy generating device is as described herein.

[0166] Some embodiments of this disclosure provide a method for generating electrical energy, the method comprising using a product as described herein in an apparatus to generate the electrical energy.

[0167] Some embodiments of this disclosure provide a method for producing an electrical energy generating device.

[0168] In some embodiments, this disclosure provides a method for producing an electrical energy generating device, the method comprising incorporating one or more batteries into the electrical energy generating device, the one or more batteries comprising a spaced first electrode and a second electrode, the first electrode comprising a low work function material and the second electrode comprising a high work function material, and a semiconductor material disposed between the first electrode and the second electrode and a radionuclide emitting beta particles, the semiconductor material being capable of generating electron-hole pairs in response to beta particle emission from the radionuclide.

[0169] This paper describes suitable first and second electrodes, as well as low work function and high work function materials.

[0170] This article describes radionuclides and semiconductor materials. Examples of semiconductor materials are described in this article.

[0171] Some embodiments of this disclosure provide an electrical energy generating apparatus produced by the methods described herein.

[0172] Certain embodiments of this disclosure provide a method for producing batteries for use in an electrical energy generation device, as described herein.

[0173] The present disclosure is further described through the following examples. It should be understood that the following description is for the purpose of describing particular embodiments only and is not intended to limit the scope of the description.

[0174] Example 1 – Using single-phase composite semiconductor materials to produce a beta-radiation photovoltaic effect device.

[0175] Non-radioactive, layered, asymmetric metal-semiconductor-metal structures were created to serve as prototype beta-radiation photovoltaic devices for testing at ultraviolet (UV) photon fluxes. UV photons were used to simulate the electron excitation effect provided by beta radiation, thus avoiding the use of radioactive materials. The UV source provided photons with energies of 4–5 eV.

[0176] The first metal layer used is a lightly polished pure nickel strip approximately 150 μm thick, which serves as both an electrode and a substrate for the semiconductor composite layer. The pure nickel was obtained from Mid-North Coast Components, Port Macquarie, NSW, Australia.

[0177] Two different semiconductor composite materials were prepared as different examples of semiconductor components for novel β-radiation-voltaic AMSM structures. The semiconductor layer is where charge carriers are generated in response to radiative excitation, and layers with a thickness of 2–5 μm are sought.

[0178] The first semiconductor composite material is a cesium-modified polyaniline-nylon composite material, prepared by the following method: (a) Nylon-6 (0.24 g; Duromer Products, Australia) and 0.009 g of cesium bromide (Sigma Aldrich, 99.999%; product number 203017) were dissolved together in 2 mL of 95% formic acid in a glass vial, and the mixture was stirred at 50 °C until completely clear (approximately 30 minutes); (b) a finely ground polyaniline (0.053 g - emeraldine - from Aldrich; product number 428329) dispersion in formic acid (1.5 mL) was prepared by stirring the components together at 50 °C for approximately 20 minutes; (c) the cesium-modified nylon solution and the polyaniline dispersion were mixed together. (d) Stir the resulting blend for at least 20 minutes and heat to remove some formic acid, thereby increasing viscosity; (e) Transfer the mixed formic acid dispersion / cesium bromide polyaniline-nylon solution to a small syringe fitted with a 0.45 μm syringe filter; (f) Drop a few drops of cesium bromide polyaniline-nylon onto a nickel metal substrate by pushing the dispersion / solution through the syringe filter; (g) Allow the deposited fluid to slowly diffuse onto the substrate by gently rotating a glass slide until almost all the formic acid has evaporated; (h) Once solidified, dry the film on a hot plate at approximately 110 °C. The concentration of cesium bromide in the film is approximately 3 wt%.

[0179] The second semiconductor material prepared was a single-phase, fully composite bismuth triiodide (BiI3)-nylon composite containing high-quality loaded BiI3. It was prepared by: (a) tightly mixing fine Nylon-12 powder (0.5 g; Duromer Products, Australia) with fine BiI3 powder (0.5 g; >98%, Tokyo Chemical Industry (TCI) product number B5787); (b) placing the powder mixture in a vial and heating the mixture to approximately 150°C to allow the BiI3 to be absorbed into the nylon; (c) placing the Nylon-BiI3 powder on a nickel metal substrate and heating the nickel from below at approximately 250°C until the material was completely solidified, as evidenced by the clear deep orange color of the resulting mixed polymer melt (approximately 5 minutes), further demonstrating the complexation of the iodide with the amide groups of the nylon; and (d) allowing the melt to diffuse onto the substrate by maintaining the heat and allowing it to form the desired thickness.

[0180] The third semiconductor composite material prepared is a composite material of a single-phase, fully composite BiI3-nylon mixture containing high-quality loaded bismuth triiodide (BiI3) and polyaniline. It was prepared by the following method: (a) tightly mixing 0.5 g of fine Nylon-12 powder with 0.5 g of fine BiI3 powder; (b) placing the powder mixture in a vial and heating the mixture to about 150°C to allow BiI3 to be absorbed into the nylon; (c) mixing the Nylon-BiI3 powder with finely ground polyaniline (0.053 g - emeraldine - salt form); (d) placing the Nylon-BiI3-polyaniline powder on a nickel metal substrate and heating the nickel from below at about 250°C until the material was completely solidified, as evidenced by the clear deep orange-green color of the resulting blend polymer-polyaniline melt (about 5 minutes); (e) allowing the melt to diffuse on the substrate and pressing a polished samarium metal electrode into the melt while melting.

[0181] Each example of a semiconductor composite material occupies a different position on a triaxial composition diagram, which illustrates the different types of semiconductor materials described herein (see [link to triaxial composition diagram]). Figure 1 The figure depicts a space defined by three end members: (i) a pure semiconductor polymer with suitable electronic properties; (ii) a semiconductor single-phase composite material comprising an inorganic compound chemically complexed with the polymer (typically containing nitrogen and / or sulfur heteroatoms); and (iii) a crystalline semiconductor with a defined chemical composition and stoichiometry. The semiconductor material may comprise a mixture or blend between any two end members or between all three end members (e.g., at the nanoscale).

[0182] For the first and second semiconductor composite materials described above, the second (low work function) metal layer includes 10 -6 A 150 nm thick layer of samarium metal was vacuum-deposited in a standard vacuum deposition chamber operating at mbar. The samarium metal crucible (Treibacher Industrie AG; Austria) was bombarded with an electron beam focused at its center. Subsequently, a stable stream of samarium metal atoms was deposited onto a substrate located approximately 20 cm directly above the crucible. At the end of the samarium metal deposition, a 150 nm layer of copper metal was applied on top of the samarium as a protective coating. The conditions for intermittent electron beam physical vapor deposition in a vacuum chamber equipped with an ion gun are as follows:

[0183]

[0184] Before evaluating the sample, a small area on the copper-faced samarium electrode was lightly sanded off with 3000-grit sandpaper until the dark color of the central semiconductor was just visible, to allow a reasonable flux of UV photons to penetrate into the semiconductor layer.

[0185] By connecting the completed device in series to Keysight 6 1 A 2-digit multimeter (model 34465A) was used to perform simulated beta-radiation voltage effect current measurements in DC ammeter mode with a resolution of 500 picoamperes (picoAmps) over a 1 μm range. Flat connector clips ensured good electrical contact with both high and low work function electrodes. Baseline thermocurrents were detected in most samples, indicating no short circuits and thus suitability for further inspection. A UV photon beam (500 mW power) was aimed at a worn portion of the electrode surface. The current reading on the ammeter jumped immediately and continued to climb. The recorded values ​​were obtained immediately (approximately 1 second) after the UV beam encountered the sample. The results are shown in Table 1.

[0186] Table 1

[0187]

[0188] As shown in Table 1, considerable instantaneous UV-induced currents were measured in each prototype β-radiation-volt effect structure tested in the experiment. The induced currents generated immediately after the start of UV irradiation are relevant in the β-radiation-volt effect response because they are entirely due to charge carriers generated by electronic excitation, while later current levels may include a thermally induced current component as heat gradually accumulates in the sample. Although the generation of thermal currents could not be measured in this experiment, the currents reported in the second column of Table 1 may underestimate the amount of charge carriers generated and collected by the type of electronic excitation, which is similar to that generated by β-radiation, as a large portion of the total current may be electronic current, even one second after the start of UV irradiation.

[0189] A key inference that can be drawn from these experiments is that the electric field collecting charge carriers must be considerable enough for them to be swept into the external circuit before recombination. This implies, in turn, that different metal-semiconductor junctions on samarium (low work function) and nickel / copper (high work function) electrodes are sufficient in terms of strength, polarity, and spatial range to achieve this.

[0190] Example 2 - Production of a beta-volt effect device by incorporating radionuclides into a polymer through exchange

[0191] The first electrode, made of samarium metal (e.g., 99.9%), can be produced using samarium foil / plates of suitable thickness, for example, in the range of 0.01 to 0.4 mm, commercially available, for example, from Sigma-Aldrich (catalog #693731). The foil / plate can be used in suitable dimensions, for example, 20 to 40 mm long × 20 to 40 mm high. An example of a produced samarium metal electrode is described in Example 1.

[0192] The second electrode, made of nickel metal (e.g., 99.6%), can be produced using foil / plate of suitable thickness, for example, in the range of 0.01 to 0.4 mm, commercially available, for example, from Baoji TST Nonferrous Metal Co., Ltd. The metal foil / plate can be used in suitable dimensions, for example, 20 to 40 mm long × 20 to 40 mm high. An example of the produced nickel metal electrode is described in Example 1.

[0193] tritium( 3Tritium (H) is a radioactive isotope that emits beta radiation. It is produced in large quantities as a byproduct of some nuclear power reactors and as waste from other nuclear processing operations. Tritium can be provided in high-pressure gaseous form (T2) at quantities of 100 gigabecquerels in many tritium treatment facilities (e.g., Canadian Nuclear Laboratories, Chalk River, Ontario), or in other chemical forms (e.g., T2O).

[0194] Inorganic semiconductors, such as BiI3, are commercially available, for example from Alfa, Ward Hill, Massachusetts (99.999% purity, recrystallized from tetrahydrofuran under nitrogen (N2)).

[0195] Matrix polymers, such as nylon-11[NH-CO-(CH2)] 10 -] n These are commercially available. The presence of the polyamide moiety in the polymer can lead to strong interactions with iodine atoms, which may be part of an inorganic semiconductor (e.g., BiI3), and these interactions can help dissolve the inorganic components in the polymer, as shown in Example 1.

[0196] BiI3-nylon-11 composites can be produced as described in Example 1 or by using a melt of nylon-11 (pre-dried under vacuum at 150°C to remove moisture) under nitrogen at 200°C to 240°C for 5 to 15 minutes to obtain a deep orange solution, for example containing about 65%-75% (by weight) BiI3.

[0197] This can be achieved by using a special tritium chamber that operates under elevated temperatures and pressures. 3 The H radionuclide is incorporated into the polymer to promote hydrogen-tritium exchange in the polymer matrix. The composite material can then be deposited onto a heated first and / or second electrode using methods such as drop casting to produce a coating of approximately 1 to 30 micrometers upon cooling.

[0198] The first and second electrodes are then brought very close together (e.g., 1 to 30 micrometers) and made to be largely parallel.

[0199] A β-radiation volt-effect power generation device using a single cell is then produced by completing the circuit (with a small resistive load) between the first and second electrodes. To manufacture a multi-cell power generation device, multiple cells using a first electrode, a second electrode, and a coating applied to either electrode can then be produced. In this case, a thin insulating layer is located between the individual cells and between the first and second electrodes of each cell connected in series or parallel.

[0200] The aforementioned power generation device is considered to have many advantages. For example, the device will generate electrical energy over a relatively long period, reflecting the usable lifetime of the radionuclide used to power the device. The device will also be resistant to radiation damage and the heat generated by the decay of the radionuclide.

[0201] Example 3 - Production of β-volt effect devices by using labeled monomers to bind radionuclides to polymers Place,

[0202] A first electrode made of samarium metal (e.g., 99.9%) can be produced using samarium foil / plates with a suitable thickness (e.g., in the range of 0.01 to 0.4 mm), which are commercially available, for example, from Sigma-Aldrich (catalog #693731). The metal foil / plate can be used in suitable dimensions, for example, 20 to 40 mm long × 20 to 40 mm high. An example of a manufactured samarium metal electrode is described in Example 1.

[0203] The second electrode, made of nickel metal (e.g., 99.6%), can be produced using a foil / plate having a suitable thickness (e.g., in the range of 0.02 to 0.4 mm), which is commercially available, for example, from Baoji TST Nonferrous Metal Co., Ltd. The metal foil / plate can be used in suitable dimensions, e.g., 20 to 40 mm long × 20 to 40 mm high. An example of the produced nickel metal electrode is described in Example 1.

[0204] Inorganic semiconductors, such as PbI2, are commercially available, for example from Sigma-Aldrich (99.999% purity).

[0205] It is possible to obtain substances such as nylon-11[NH-CO-(CH2)] 10 -] n Insulating polymers, which have been used 3 H or 14 C radionuclide labeling. For example, for nylon-11, the polymer can be labeled using a monomer incorporated into 11-aminoundecanoic acid. 3 H and 14 C is labeled, and polymers are produced by polymerizing the labeled monomers using standard synthesis conditions.

[0206] PbI2-nylon-11 composites can be produced by incubating a marked nylon-11 melt (pre-dried under vacuum at 150°C to remove moisture) under nitrogen atmosphere at 220°C to 290°C to obtain a thick, transparent, orange solution, for example, containing approximately 65% ​​(by weight) PbI2. This produces PbI2- 3 H or 14 C nylon-11 composite material. The solution can then be deposited onto the heated first and / or second electrodes using polymer film application processes (such as sheet extrusion) to produce a coating of approximately 1 to 30 micrometers upon cooling.

[0207] Then the first and second electrodes are brought very close together (e.g., 1 to 50 micrometers) and made to be largely parallel.

[0208] A β-radiation volt-effect power generation device using a single cell is then produced by completing the circuit (with a small resistive load) between the first and second electrodes. To produce a multi-cell power generation device, multiple cells using a first electrode, a second electrode, and a coating applied to either of the electrodes can then be manufactured. In this case, a thin insulating layer is located between the individual cells and between the first and second electrodes of each cell connected in series or parallel.

[0209] The aforementioned power generation device is considered to have many advantages. For example, the device will generate electrical energy over a period of time, reflecting the available lifetime of the radionuclide used to power the device. The material will be resistant to radiation damage and also provides resistance to the heat generated by the decay of the radionuclide.

[0210] Example 4 - Using crystalline semiconductors to produce beta-volt effect devices

[0211] The first electrode, made of samarium metal (99.9%), can be produced using a samarium foil / plate with a suitable thickness (e.g., in the range of 0.02 to 0.4 mm), which is commercially available, for example, from Sigma-Aldrich (catalog #693731). This metal foil / plate can be used in suitable dimensions, such as 20 to 40 mm long × 20 to 40 mm high.

[0212] The second electrode, made of nickel metal (99.6%), can be produced using nickel foil / plates of suitable thickness (e.g., in the range of 0.02 to 0.4 mm), which are commercially available, for example, from Baoji TST Nonferrous Metal Co., Ltd. The foil / plate can be used in suitable dimensions, such as 20 to 40 mm long × 20 to 40 mm high.

[0213] Semiconductor charge carrier collector materials in thin-plate form can be used. For example, strontium titanate (SrTiO3) can be used with suitable... 90 Sr source (e.g., ( 90 Sr, nat SrCO3 (with a specific activity of 500 GBq / g) is doped with powdered, inactive SrCO3 and powdered TiO2. The mixture can be ball-milled for 24 hours in an ethanol medium using yttrium-stabilized zirconia balls in a plastic container. The slurry can then be dried, ground, sieved (100 mesh), and calcined at a suitable temperature for a suitable time, for example, 2 hours in the range of 1000°C to 1200°C. The calcined powder can then be ball-milled, dried, and ground into a fine powder again, and then a 3 wt% solution of polyvinyl alcohol 1799 (PVA) (alcoholic 99.8-100% (mol / mol), Aladdin Industrial Co.) is added dropwise to the dried powder as a binder. The mixture can then be coated onto the first or second electrode using a wet coating process, such as spin coating, and dried to produce a coating of approximately 1 to 50 micrometers.

[0214] Strontium-90 ( 90 Sr), a radioactive nuclide that emits beta particles, can be used as... 90 Radioactive waste in the form of SrCO3 was obtained.

[0215] SrCO3 is commercially available, for example, in powder form from Sinopharm Chemical Reagent Co. Ltd.

[0216] TiO2 is commercially available, for example, in powder form from Sinopharm Chemical Reagent Co. Ltd.

[0217] The first and second electrodes (one of which is coated) are then brought close together (e.g., 1 to 50 micrometers) and made to be largely parallel.

[0218] A β-radiation voltaic effect energy-generating cell is then produced by completing a circuit (with a small resistive load) between the first and second electrodes. To manufacture a multi-cell energy-generating device, multiple cells can then be manufactured using a first electrode, a second electrode, and a coating applied to either of the electrodes. In this case, a thin insulating layer is located between the individual cells and between the first and second electrodes of each cell connected in series or parallel.

[0219] The aforementioned power generation device is considered to have many advantages. For example, the device will generate electrical energy over a relatively long period, reflecting the usable lifetime of the radionuclide used to power the device. The materials used in the device will resist radiation damage and also provide resistance to the heat generated by the decay of the radionuclide.

[0220] Example 5 – Preparation of Tritium Semiconductor Polymers

[0221] Tritium-modified polyaniline polymers with desired semiconductor properties can be prepared by two methods. Methods for preparing polyaniline are known in the art, for example, as described in Boeva ​​and Sergeyev (2014) “Polyaniline: Synthesis, Properties and Application” Polymer Science, Ser. C 56:144-153.

[0222] In one instance, polyaniline can be prepared by chemical polymerization of aniline using ammonium persulfate, as described, for example, in J. Stejskal and RG Gilbert, Pure Appl. Chem. 74, 857 (2002). 3 H radionuclides can be incorporated into polymers using a special tritium chamber operated at elevated temperatures to promote hydrogen-tritium exchange within the polymer matrix.

[0223] In another example, polyaniline with the desired conductivity can be labeled with aniline. 3 H or 14 It is prepared by chemical polymerization of C radionuclides and ammonium persulfate, as described, for example, in J. Stejskal and RG Gilbert, Pure Appl. Chem.

[0224] Although this disclosure has been described with reference to specific examples, those skilled in the art will understand that this disclosure may be embodied in many other forms.

[0225] It should be understood that various changes, additions and / or modifications may be made to the previously described portions without departing from the scope of this disclosure, and that this disclosure may be implemented in software, firmware and / or hardware in various ways that will be understood by those skilled in the art, based on the foregoing teachings.

[0226] As used in this article, the singular forms “a kind of,” “one,” and “the” can refer to plural articles unless otherwise specified.

[0227] Throughout this specification, unless the context otherwise requires, the word “comprising” or variations such as “including” or “containing” will be understood to imply inclusion of the stated element or integer or group of elements or integers but not to exclude any other element or integer or group of elements or integers.

[0228] All methods described herein may be performed in any suitable order unless otherwise stated herein or clearly contradicted by the context. Unless otherwise stated, the use of any and all instances or exemplary language (e.g., “such as”) provided herein is intended only to better illustrate exemplary embodiments and does not constitute a limitation on the scope of the claimed invention. No language in the specification should be construed as indicating that any unclaimed element is essential.

[0229] The description provided herein relates to several embodiments that may share common characteristics and features. It should be understood that one or more features of one embodiment may be combined with one or more features of other embodiments. Furthermore, individual features or combinations of features of embodiments may constitute additional embodiments.

[0230] The headings used herein are included for convenience of the reader only and should not be used to limit the subject matter found throughout the disclosure or claims. These headings should not be used to interpret the scope or limitation of the claims.

[0231] Future patent applications may be filed based on this application, for example, by claiming priority to this application or by claiming divisional status. It should be understood that the following claims are provided by way of example only and are not intended to limit the scope of protection that may be claimed in any such future application. Nor should the claims be construed as limiting the understanding of this disclosure (or excluding any other understanding of this disclosure). Features may be added or omitted later in the example claims.

Claims

1. An electrical energy generating device, the device comprising at least one battery, the battery comprising: A first electrode and a second electrode spaced apart, the first electrode comprising a low work function material and the second electrode comprising a high work function material; and A semiconductor material comprising a semiconductor polymer or a semiconductor polymer composite and a radionuclide emitting beta particles is disposed between a first electrode and a second electrode, wherein the semiconductor material is capable of generating electron-hole pairs in response to beta particle emission from the radionuclide.

2. The power generation device according to claim 1, wherein, The radionuclides include 90 Sr、 99 Tc, 3 H, 14 C 63 Ni、 137 Cs、 147 Pm, 151 Sm、 155 Eu、 93 Zr、 126 Sn、 60 Co、 210 Pb, 90 Y、 129 I, 188 W, 35 S, 123 Sn、 45 Ca, 106 Ru、 170 Tm、 171 Tm、 134 Cs、 32 Si、 113 Cd and 79 One or more of Se.

3. The power generation device according to claim 1 or 2, wherein, The low work function material includes metals or metal-containing compounds.

4. The power generation device according to claim 1 or 2, wherein, The low work function materials include intermetallic compounds.

5. The power generation device according to claim 3, wherein, The metal or metal-containing compound includes one or more of europium, strontium, barium, samarium, dysprosium, neodymium, gadolinium, terbium, holmium, erbium, thulium, lanthanum, scandium, thorium, calcium, magnesium, cerium, yttrium, ytterbium, sodium, lithium, potassium, rubidium, and cesium.

6. The power generation device according to claim 4, wherein, The intermetallic compounds include one or more of europium, strontium, barium, samarium, dysprosium, neodymium, gadolinium, terbium, holmium, erbium, thulium, lanthanum, scandium, thorium, calcium, magnesium, cerium, yttrium, ytterbium, sodium, lithium, potassium, rubidium, and cesium.

7. The power generation device according to claim 1 or 2, wherein, The low work function material includes samarium metal.

8. The power generation device according to claim 1 or 2, wherein, The high work function materials include metals and / or intermetallic compounds.

9. The power generation device according to claim 1 or 2, wherein, The high work function material includes one or more metals selected from nickel, platinum, silver, gold, aluminum, cobalt, chromium, copper, beryllium, bismuth, cadmium, iron, gallium, germanium, mercury, indium, iridium, manganese, molybdenum, niobium, osmium, lead, palladium, rhenium, rhodium, ruthenium, antimony, silicon, tin, tantalum, technetium, titanium, vanadium, tungsten, zinc, and zirconium.

10. The power generation device according to claim 1 or 2, wherein, The high work function material includes nickel metal.

11. The power generation device according to claim 1 or 2, wherein, The radionuclides are dispersed in the semiconductor material.

12. The power generation device according to claim 1 or 2, wherein, The radioactive nuclide is incorporated into the chemical structure of the semiconductor material.

13. The power generation device according to claim 1 or 2, wherein, The semiconductor material includes single-phase composite semiconductor material.

14. The power generation device according to claim 13, wherein, The single-phase composite semiconductor material includes inorganic semiconductors chemically composited with polymers.

15. The power generation device according to claim 1 or 2, wherein, The semiconductor material includes crystalline semiconductors.

16. The power generation device according to claim 1 or 2, wherein, The first electrode and the second electrode are separated by a distance ranging from 0.3 to 100 micrometers.

17. The power generation device according to claim 1 or 2, wherein, The device includes multiple batteries.

18. A method for generating electricity, the method comprising using an electrical energy generating device according to any one of claims 1 to 17.

19. A method for generating electrical energy, the method comprising: A potential difference is generated between a closely spaced first electrode and a second electrode, wherein the first electrode comprises a low work function material and the second electrode comprises a high work function material. High-energy beta particles emitted from a radioactive nuclide generate electron-hole pairs, the radioactive nuclide being in close proximity to a semiconductor material comprising a semiconductor polymer or a semiconductor polymer composite disposed between a first electrode and a second electrode, the electron-hole pairs being movable under the influence of an electric field between the electrodes; and The electric field existing between the electrodes is used to capture electron-hole pairs into an external circuit. This generates electrical energy.

20. A method for generating electrical energy, the method comprising: An electric field is generated between a first electrode and a second electrode spaced apart, the first electrode comprising a low work function material and the second electrode comprising a high work function material, and the electric field is generated due to different Schottky junctions at the two different electrodes; High-energy beta particles emitted from a radioactive nuclide generate electron-hole pairs, the radioactive nuclide being in close proximity to a semiconductor material comprising a semiconductor polymer or a semiconductor polymer composite disposed between a first electrode and a second electrode, the electron-hole pairs being movable under the influence of an electric field; and The electron-hole pairs are captured into an external circuit by utilizing the electric field existing between the electrodes; This generates electrical energy.

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