WO2023171524A1 - Dispositif de production d'énergie et système de production d'énergie - Google Patents

Dispositif de production d'énergie et système de production d'énergie Download PDF

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WO2023171524A1
WO2023171524A1 PCT/JP2023/007790 JP2023007790W WO2023171524A1 WO 2023171524 A1 WO2023171524 A1 WO 2023171524A1 JP 2023007790 W JP2023007790 W JP 2023007790W WO 2023171524 A1 WO2023171524 A1 WO 2023171524A1
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power generation
oxide particles
water
metal oxide
radiation
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PCT/JP2023/007790
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English (en)
Japanese (ja)
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要 堤内
真一 橋本
桃子 島岡
左京 上野
裕佐 室屋
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学校法人中部大学
国立大学法人大阪大学
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Application filed by 学校法人中部大学, 国立大学法人大阪大学 filed Critical 学校法人中部大学
Publication of WO2023171524A1 publication Critical patent/WO2023171524A1/fr

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    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J19/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
    • B01J19/08—Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor
    • G—PHYSICS
    • G21—NUCLEAR PHYSICS; NUCLEAR ENGINEERING
    • G21H—OBTAINING ENERGY FROM RADIOACTIVE SOURCES; APPLICATIONS OF RADIATION FROM RADIOACTIVE SOURCES, NOT OTHERWISE PROVIDED FOR; UTILISING COSMIC RADIATION
    • G21H1/00—Arrangements for obtaining electrical energy from radioactive sources, e.g. from radioactive isotopes, nuclear or atomic batteries

Definitions

  • the present invention relates to a power generation method and power generation system using radiolysis of water.
  • Patent Document 1 Previous research to improve hydrogen generation efficiency includes a technique in which metals are present in water and irradiated with radiation (Patent Document 1), and an experiment in which fine alumina particles are dispersed in water and irradiated with 60 Co gamma rays (Non-patent Document 1). Reference 1). It has been confirmed that alumina promotes hydrogen production through radiolysis of water.
  • the present inventors thought that similar effects could be expected by using iron oxide particles, and conducted experiments. As a result, almost no hydrogen generation was observed in the iron oxide particles, and the reduction reaction of trivalent iron was progressing.
  • the present inventors focused on this phenomenon and, as a result of conducting extensive research, discovered that it is possible to generate electricity by utilizing the above-mentioned phenomenon.
  • an object of the present invention is to provide a power generation method and power generation system using water radiolysis.
  • the invention according to claim 1 provides a power generation method by radiolysis of water, in which a power generation tank capable of containing water and provided with a pair of electrodes is prepared, and the water is supplied with oxygen at a non-stoichiometric ratio. a step of dispersing metal oxide particles having properties and conductivity; a step of irradiating the water in which the metal oxide particles are dispersed with radiation from a radiation source; and after irradiating the radiation, the metal oxide particles are dispersed near one electrode.
  • a technical means is used that includes a step of unevenly distributing oxide particles and a step of extracting electricity from the electrode.
  • oxygen nonstoichiometricity indicates that disorder occurs in the lattice points occupied by oxygen ions, resulting in a nonstoichiometric composition in which the composition of the material deviates from the stoichiometric ratio.
  • oxygen nonstoichiometricity indicates that disorder occurs in the lattice points occupied by oxygen ions, resulting in a nonstoichiometric composition in which the composition of the material deviates from the stoichiometric ratio.
  • divalent and trivalent iron coexists and their ratio changes due to redox
  • large oxygen nonstoichiometry occurs.
  • the metal oxide particles are unevenly distributed near one electrode means that the metal oxide particles move toward the electrode and approach to a distance where they can transfer electric charge. This concept involves particles coming into contact with an electrode.
  • the metal oxide particles are magnetite or maghemite.
  • the radiation includes at least one of ⁇ rays and ⁇ rays. .
  • the technical feature is that the radiation source is a long-lived fission product. use means.
  • the invention according to claim 6 is a power generation system that generates power by radiolysis of water, wherein the power generation system generates power by radiolysis of water, wherein metal oxide having oxygen nonstoichiometry and conductivity is present in water.
  • a technical means is used that includes a means for unevenly distributing the information.
  • the power generation method and power generation system of the present invention it is possible to generate power in a simple process using a radiation source such as spent nuclear fuel that can no longer be used in nuclear power generation.
  • the present invention directly converts the chemical species (solvated electrons, radicals, etc.) generated by radiolysis of water molecules into electrical energy, so the system is very simple and can be used to control nuclear reactions such as nuclear power generation. It does not require complex and large-scale equipment such as systems or heat transfer flow systems.
  • radioactive sources such as radioactive waste, which have not been used until now, can be used as energy sources. In principle, this system is activated when radiolysis of water occurs, and the type of radiation incident on the water does not matter when it is operated.
  • the aquarium can be irradiated from the outside, so gamma and beta rays, which have a longer range, are used rather than alpha rays, which have a short range. It is preferable.
  • the power generation system can operate stably.
  • FIG. 1 is a schematic diagram showing the configuration of a power generation system.
  • 1 is a schematic diagram of a power generation system in a state of generating power. It is an explanatory view showing steps of a power generation method. It is an explanatory diagram showing a power generation mechanism.
  • FIG. 3 is a schematic diagram showing an example of a modification of the power generation system. It is a figure showing a time change of electromotive force.
  • FIG. 3 is a diagram showing a current-voltage curve.
  • FIG. 1 An example of a power generation system is schematically shown in Figure 1.
  • the power generation system S includes a dispersion means 1, an irradiation means 2, a power extraction means 3, an uneven distribution means 4, a power generation tank 5, and a control device (not shown).
  • iron oxide particles are used as metal oxide particles having non-stoichiometric oxygen properties and conductivity.
  • the dispersion means 1 is a means for dispersing iron oxide particles in water, and includes a stirrer that stirs water stored in the power generation tank, a rotation device that rotates the power generation tank, a circulation device that circulates water in the power generation tank, Various methods such as these can be adopted.
  • the irradiation means 2 is a means for irradiating water in which iron oxide particles are dispersed with radiation.
  • various means can be employed, such as exposing water in which iron oxide particles are dispersed to a radiation source, or inserting a radiation source into a power generation tank.
  • the irradiation means 2 is, for example, an irradiation member 20 formed by enclosing a long-life nuclear fission product shaped into a pellet in a metal container.
  • the irradiation member 20 is placed underwater in the power generation tank 5 .
  • radiation refers to particles ( ⁇ rays, ⁇ rays, neutron beams), electromagnetic waves ( ⁇ rays, X rays), electron beams, and particle beams emitted from radioactive substances.
  • the initial yield of radiolysis is expressed by the G value (the number of chemical species produced per 100 eV of absorbed energy).
  • the initial G value during radiolysis of water when irradiated with low LET rays ( ⁇ rays and ⁇ rays) is as follows (Yosuke Katsumura et al., Nuclear Engineering Radiochemistry, Maruzen Publishing (2020)). It can be seen that among the chemical species produced by radiolysis of water, many hydrated electrons (e - aq ) and .OH are produced.
  • Gamma rays have a longer range than alpha and beta rays, and even in a sealed radiation source, it is easy to extract energy outside the container.
  • the yield of hydrated electrons (e - ) and .OH produced by irradiating water with gamma rays is higher than that with alpha ray irradiation. , gamma rays are most preferred.
  • the power extraction means 3 is a system for extracting electric power, and corresponds to a pair of extraction electrodes 30, 31, an extraction device 32, etc. arranged in the power generating tank 5.
  • the extraction electrodes 30 and 31 are made of a noble metal that has a low ionization tendency, such as gold. The following description will be made assuming that the extraction electrode 31 is an extraction electrode in which oxide particles are unevenly distributed.
  • the power extraction means 3 can adopt various configurations as long as it can extract electric power from the power generation tank 5. For example, it is also possible to adopt a configuration in which an electrode layer is formed on the inner surface of the power generating tank 5. Moreover, in order to increase the probability of contact with oxide particles, the shape of the extraction electrode 31 can be made into a shape with a large surface area, such as a mesh shape or a honeycomb shape.
  • the uneven distribution means 4 is a means for unevenly distributing the iron oxide particles P near one electrode.
  • a magnetic force generating means capable of switching between a state in which magnetic force is generated and a state in which magnetic force is not generated can be arranged near one of the electrodes.
  • gravity segregation may be performed by arranging the extraction electrode 30 above and the extraction electrode 31 below without using magnetic force. At this time, in order to make it easier for the iron oxide particles P to gather near the extraction electrode 31 in the power generation tank 5, a configuration such as providing an inclination toward the extraction electrode 31 on the inner surface of the power generation tank 5 may be adopted as the uneven distribution means 4. Can be done.
  • Iron oxides include wustite (Fe 2+ O) consisting of divalent iron oxide, magnetite (Fe 2+ Fe 3+ 2 O 4 ) consisting of divalent and trivalent iron, and ⁇ type consisting of trivalent iron. Examples include hematite ( ⁇ -Fe 3+ 2 O 3 ) and ⁇ -type maghemite ( ⁇ -Fe 3+ 2 O 3 ). Iron oxide has three stable phases: wustite, magnetite, and hematite at room temperature and pressure, but hematite is the most stable under atmospheric oxygen partial pressure.
  • iron oxide containing trivalent iron is used.
  • Magnetite Fe 2+ Fe 3+ 2 O 4
  • ⁇ -type hematite ⁇ -Fe 3+ 2 O 3
  • ⁇ -type maghemite ⁇ -Fe 3+ 2 O 3
  • magnetite and maghemite are used.
  • nanoparticles for example, they can be produced by further performing ultrasonic crushing with a ceramic ball and fractionating the nanoparticles from the supernatant after centrifugation.
  • step S1 iron oxide particles P containing trivalent iron are dispersed in water W.
  • this corresponds to the step of activating the dispersion means 1 to disperse iron oxide particles in water.
  • the particle size of the iron oxide particles P is preferably about 1 to 100 ⁇ m.
  • the particle size becomes nano-order it is possible to scatter radiation and improve water decomposition efficiency, but it becomes difficult to make it unevenly distributed near one electrode.
  • step S2 the water in which the iron oxide particles were dispersed in step S1 is irradiated with radiation from a radiation source.
  • this corresponds to a step in which the irradiation means 2 irradiates water W in which iron oxide particles P are dispersed with radiation.
  • gamma rays are used as radiation.
  • the oxide particles P be added in an amount sufficient to receive hydrated electrons ejected from water molecules by radiation.
  • the amount added can be determined as appropriate, taking into consideration the particle size, ease of uneven distribution, and the like.
  • OH radicals cause the reaction shown in FIG. 4B.
  • water molecules are regenerated or converted into hydrogen molecules (H 2 ) and hydrogen peroxide (HOOH) through reactions between radical chemical species (hydrated electrons, .H , .OH).
  • radical chemical species hydrated electrons, .H , .OH.
  • the reaction path changes, and hydrated electrons are captured by the iron oxide particles in step S2.
  • the radical reaction e - aq + ⁇ OH ⁇ OH -
  • the yield of hydroxyl radicals ⁇ OH
  • the yield of hydrogen peroxide (HOOH) produced by the reaction ⁇ OH + ⁇ OH ⁇ HOOH will also increase.
  • step S3 the iron oxide particles P that have been irradiated with radiation in step S2 are unevenly distributed in the vicinity of the extraction electrode 31 by the uneven distribution means 4.
  • this corresponds to a step in which the irradiation means 2 operates the electromagnet 40, which is the uneven distribution means 4, and causes the iron oxide particles P to be unevenly distributed near the extraction electrode 31 by magnetic force.
  • the electrons ejected from the water molecules are taken into the iron oxide particles P, so that the reduced iron oxide fine particles P rich in electrons can be unevenly distributed in the vicinity of the extraction electrode 31.
  • the extraction electrodes 30 and 31 are electrically connected by the power extraction means 3, and electric power is extracted by reaction C shown in FIG.
  • the extraction electrode 30 receives electrons from the extraction electrode 32, and hydrogen peroxide (HOOH) is reduced and converted into stable hydroxide ions (-OH).
  • HOOH hydrogen peroxide
  • -OH stable hydroxide ions
  • Cathode reaction proceeds. This reaction is a spontaneous favorable reaction with an energy change of -1.76 eV, so this reaction is the source of the electromotive force. If electrons can be received from the electrode, the reaction that produces two hydroxide ions (-OH) will proceed spontaneously (HOOH + 2e- ⁇ HO- + -OH).
  • anode reaction proceeds in which some of the divalent iron constituting the particles becomes trivalent iron (Fe II ⁇ Fe III ).
  • Fe II ⁇ Fe III trivalent iron
  • the change from Fe II ⁇ Fe III is an involuntary unfavorable change with an energy change of +0.771 eV.
  • the reduction reaction of hydrogen peroxide that proceeds on the opposite side of the electrode has greater energy and proceeds in a more stable direction, so the reduction reaction of hydrogen peroxide takes priority and electrons are released from the reduced iron oxide particles. The oxidation reaction begins to progress.
  • the electromagnet 40 After extracting the electric power, the electromagnet 40 is stopped, the state is switched to a state in which no magnetic force is generated in the vicinity of the extracting electrode 31, and then steps S1 to S4 are performed again to repeatedly generate electricity.
  • aggregates of unevenly distributed iron oxide particles have a higher electrical resistance than gold electrodes, and iron oxide particles located at the outermost part of the aggregate are oxidized relatively quickly, so they react with hydrogen peroxide. It is thought that it becomes less likely to cause this and provides a function similar to that of a separator. Due to these factors, this power generation system is able to supply electricity without a separator.
  • the hydrogen peroxide aqueous solution on the anode side has many opportunities to physically come into contact with the iron oxide particles on the cathode side due to convection, and hydrogen peroxide and iron oxide particles directly react, causing a reduction in power generation efficiency. There is. Therefore, by introducing a separator, it is possible to generate electricity more efficiently.
  • CoFe 2 O 4 is a candidate for other metal oxide particles that can be applied to the power generation system of the present invention.
  • the requirements to be met are that it has oxygen nonstoichiometry, conductivity, and magnetism, and that it has a smaller redox potential than hydrogen peroxide.
  • composite oxides can also be included as metal oxides.
  • an LLFP irradiation member 20
  • a circulating water pipe 22 that can irradiate radiation emitted from the LLFP inside the storage 21 is provided, and a power generation tank 5
  • the water inside is circulated by a liquid feeding pump 23. Thereby, radiation can be irradiated with the iron oxide fine particles P dispersed in the water.
  • the power generation method and power generation system of the present invention it is possible to generate power in a simple process using a radiation source such as spent nuclear fuel that can no longer be used in nuclear power generation.
  • a radiation source such as spent nuclear fuel that can no longer be used in nuclear power generation.
  • the chemical species hydrated electrons, OH, etc.
  • the system is very simple and can be used in nuclear reaction control systems and heat transfer systems, such as in nuclear power generation.
  • a complex and large-scale system such as a flow system is not required.
  • radioactive sources such as radioactive waste, which have not been used until now, can be used as energy sources. In principle, this system is activated when radiolysis of water occurs, and the type of radiation incident on the water does not matter when it is operated.
  • the power generation system can operate stably.
  • the fluid used in these systems is water, which is chemically safe and acts as a radiation shield, so the safety equipment for power generation systems will be relatively lighter than the current radioactive waste management system. be able to.
  • a radioactive substance such as LLFP is used as a radiation source, electricity can be extracted as long as it emits radiation. Additionally, electricity can be extracted safely on a small scale without bringing radioactive materials into a critical state.
  • the obtained particles were subjected to measurement of iron concentration using o -phenanthroline coloring method, measurement of divalent iron content, measurement of particle size using SEM, and analysis of crystal structure using XRD. It was confirmed that flake-like particles with a size of 100 to 150 ⁇ m and having a magnetite crystal structure and a divalent iron content of over 20% were obtained. These particles have magnetic properties, and it was thought that they could be separated from water using a magnet.
  • a gold electrode was prepared using gold, which has a low ionization tendency.
  • a gold plate with a diameter of 1 cm and a thickness of 0.2 mm was thermally bonded to a gold wire with a diameter of 0.4 mm and a length of 10 cm, and the gold wire was coated with two acrylic plates to avoid contact with the solution.
  • the gold plate was fixed at 90° to the coated acrylic plate.
  • An electrode was created by bonding the exposed gold wire with a copper wire with a diameter of 0.4 mm and a length of 30 cm using solder. The two gold plates were placed so that the distance between them was 2.0 cm.
  • Dispersion means 2 ... Irradiation means 20. Irradiation member 21... Storage 22... Circulating water piping 23... Liquid sending pump 23 3... Power extraction means 30, 31... Extraction electrode 32. Extraction device 4... Uneven distribution means 40... Electromagnet 5... Power generation tank S... Power generation system P... Oxide particles W... Water

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Abstract

Le problème à résoudre par la présente invention est de fournir un procédé de production d'énergie et un système de production d'énergie qui font appel à la radiolyse de l'eau. La solution selon l'invention porte sur un procédé de production d'énergie pour produire de l'énergie par radiolyse de l'eau, le procédé de production d'énergie comprenant : une étape consistant à préparer un réservoir de production d'énergie qui peut contenir de l'eau et dans lequel est disposée une paire d'électrodes, et à disperser dans l'eau des particules d'oxyde métallique ayant une non-stœchiométrie en oxygène et une conductivité ; une étape consistant à irradier l'eau contenant les particules d'oxyde métallique dispersées avec un rayonnement provenant d'une source de rayonnement ; une étape consistant à déposer localement les particules d'oxyde métallique à proximité de l'une des électrodes après l'irradiation ; et une étape consistant à extraire de l'électricité des électrodes.
PCT/JP2023/007790 2022-03-07 2023-03-02 Dispositif de production d'énergie et système de production d'énergie WO2023171524A1 (fr)

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Citations (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JP2002034233A (ja) * 2000-07-12 2002-01-31 Ts Heatronics Co Ltd 発電システム
CN112750548A (zh) * 2021-01-29 2021-05-04 厦门大学 一种放射性的三维纳米结构辐伏电化学电池

Patent Citations (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JP2002034233A (ja) * 2000-07-12 2002-01-31 Ts Heatronics Co Ltd 発電システム
CN112750548A (zh) * 2021-01-29 2021-05-04 厦门大学 一种放射性的三维纳米结构辐伏电化学电池

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