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WO2019113842A1 - Pile bêtavoltaïque à points quantiques - Google Patents

Pile bêtavoltaïque à points quantiques Download PDF

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Publication number
WO2019113842A1
WO2019113842A1 PCT/CN2017/115954 CN2017115954W WO2019113842A1 WO 2019113842 A1 WO2019113842 A1 WO 2019113842A1 CN 2017115954 W CN2017115954 W CN 2017115954W WO 2019113842 A1 WO2019113842 A1 WO 2019113842A1
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WIPO (PCT)
Prior art keywords
quantum dot
beta
indium
sulfide
cadmium
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Ceased
Application number
PCT/CN2017/115954
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English (en)
Chinese (zh)
Inventor
陈继革
伞海生
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Shenzhen Betary Technologies Co Ltd
Shenzhen Research Institute of Xiamen University
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Shenzhen Betary Technologies Co Ltd
Shenzhen Research Institute of Xiamen University
Priority date (The priority date is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the date listed.)
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Application filed by Shenzhen Betary Technologies Co Ltd, Shenzhen Research Institute of Xiamen University filed Critical Shenzhen Betary Technologies Co Ltd
Priority to PCT/CN2017/115954 priority Critical patent/WO2019113842A1/fr
Publication of WO2019113842A1 publication Critical patent/WO2019113842A1/fr
Anticipated expiration legal-status Critical
Ceased legal-status Critical Current

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    • 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
    • G21H1/06—Cells wherein radiation is applied to the junction of different semiconductor materials

Definitions

  • the invention belongs to the field of isotope batteries, and in particular relates to a quantum dot beta volt battery.
  • micro-sensing systems With the development of the Internet of Things technology, the miniaturization and integration of energy supply devices have become an urgent problem to be solved in the development of micro-sensing systems.
  • more and more micro-sensing systems need to be used in special environments, such as deep sea, deep space, underground, polar, desert and so on. These environments often require long life, maintenance free, and highly reliable power systems.
  • traditional energy sources are difficult to meet the requirements of use due to their respective shortcomings.
  • chemical batteries have low energy density, unstable high and low temperature performance, and require frequent charging.
  • Micro fuel cells are more efficient, but they are bulky and require regular fuel input into the battery. The solar cell output power intensity is dependent on external illumination and panel area. Therefore, the conventional battery is not suitable for use in electronic devices in special environments.
  • Isotope battery is an autonomous power generation device that converts energy released by radioactive isotope decay into electrical energy. It has the characteristics of high energy density, long life, reliable operation, strong environmental adaptability and no maintenance. It has become an important direction of nuclear energy research. It has broad application prospects in the fields of medicine, military, aviation and civil.
  • thermoelectric conversion There are four main conversion mechanisms for converting isotope radiation decay energy into electrical energy: thermoelectric conversion, direct charge, direct energy conversion, and indirect energy conversion.
  • Thermoelectric conversion isotope batteries use high-energy radiation sources, which are expensive to use and difficult to miniaturize.
  • the direct-charged isotope battery has a small current and a very weak driving capability.
  • Indirect conversion isotope battery conversion efficiency is generally low ( ⁇ 1%).
  • Direct energy conversion isotope batteries also known as betavoltaic cells or beta volt cells
  • the energy conversion efficiency of the ⁇ -volt isotope battery increases with the increase of the forbidden band width of the semiconductor material, and the highest theoretical conversion efficiency can reach 32%.
  • the betavoltaic cell has a high theoretical energy conversion efficiency, the conversion efficiency achieved by the current technology is still less than 5%, far from the extent of engineering application. Therefore, how to improve the energy conversion efficiency of betavolta batteries is a top priority for current research.
  • the wide bandgap semiconductor can increase the open circuit voltage of the betavoltaic battery and increase the output power of the battery. Same At the time, the wide bandgap semiconductor has a high radiation damage threshold and is highly resistant to radiation damage.
  • the nanotube/porous material has a high specific surface area, which greatly increases the contact area between the radiation source and the semiconductor material, thereby improving the energy conversion efficiency and output power of the betavoltaic battery.
  • San et al. of Xiamen University used a wide-gap semiconductor TiO2 three-dimensional nanoporous array structure to prepare a nickel-63 (Ni-63) betavoltaic cell with a maximum effective conversion efficiency of 7.3% (Qiang Zhang, Ranbin Chen, Haisheng San, Guohua Liu).
  • a first aspect of the invention provides a quantum dot beta voltaic cell comprising a semiconductor nanotube array film 4 disposed between a bottom electrode 5 and a top electrode 1 having a quantum dot layer on the inner wall of the tube 7.
  • the quantum dot layer 7 is further coated with a solid isotope radiation source layer 3, or the tubular space surrounded by the quantum dot layer 7 is filled with a gaseous or liquid isotope radiation source.
  • the solid isotope radiation source layer 3 may also fill the tubular space enclosed by the quantum dot layer 7.
  • the semiconductor nanotube array film 4 is formed by arranging a plurality of mutually parallel nanotubes side by side.
  • the quantum dot layer 7 and the isotope radiation source layer 3 are continuous layers or discrete layers or a combination of the two. It can be one or more layers.
  • the semiconductor nanotube array film 4 is a crystalline wide band gap semiconductor film having a forbidden band width greater than 2.3 eV, wherein the semiconductor material may be at least one of a semiconductor metal oxide, a semiconductor compound, and a semiconductor element.
  • the material constituting the nanotube comprises titanium dioxide, zinc oxide, zirconium dioxide, cadmium oxide, antimony pentoxide, antimony oxide, gallium trioxide, tin dioxide, tungsten trioxide, silicon carbide, gallium nitride.
  • the semiconducting nanotube has a tube diameter of 10 nm to 1000 nm and a tube length of 200 nm to 100 ⁇ m.
  • the quantum dot layer 7 is a layer composed of nano-grains of semiconductor material having a radius not greater than the exciton Bohr radius.
  • Quantum dots are quasi-zero-dimensional nanocrystals with radii that are less than or close to the exciton's Bohr radius. The movement of electrons in all directions is limited, which gives it unique properties.
  • the size of the quantum dots ranges from 1 to 100 nm.
  • the choice of the appropriate quantum dot material and the size of the quantum dot can change the energy band structure of the quantum dot to match the wide band gap semiconductor nanotube/porous band structure, achieve the multi-exciton effect of beta radiation, and pass quantum dots and The quantum junction between the heterojunction at the nanotube/hole contact interface and the quantum dots enhances the separation and transport of carriers.
  • the semiconductor material constituting the quantum dot may be selected from the group consisting of titanium dioxide, zinc oxide, zirconium dioxide, cadmium oxide, antimony pentoxide, antimony oxide, gallium trioxide, indium trioxide, tin dioxide, tungsten trioxide.
  • the preparation method of the quantum dot material includes two methods of in situ growth and ex situ growth.
  • In-situ growth is a method of directly growing and depositing quantum dots on wide-bandgap semiconductor nanotubes/holes, including chemical bath deposition (CBD) and continuous ion layer adsorption and reaction (successive ionic layer). Absorption and reaction, SILAR).
  • CBD chemical bath deposition
  • SILAR continuous ion layer adsorption and reaction
  • the ex-situ growth method is to first synthesize quantum dots, and then deposit quantum dots on the wide band gap semiconductor nanotubes/holes, including direct adsorption and linker-assisted adsorption.
  • the isotope radiation source is a radiation source capable of radiating beta particles when decaying, and has a half-life of not less than 5 years.
  • the average energy of the beta particles is not higher than 250 KeV.
  • Selected materials may include at least one of hydrogen-3 ( ⁇ ), nickel-63, carbon-14, cobalt-60, ⁇ -146, ⁇ -90, ⁇ -137. At least one of hydrogen-3 (antimony), nickel-63, carbon-14, cobalt-60, cesium-146, strontium-90, and cesium-137. Simple or combined isotopes may be used.
  • the isotope radiation source material may be a single element material or a material in which an isotope is combined with other materials.
  • the physical form of the isotope radiation source can be a solid, a gas or a liquid.
  • the method for depositing the isotope radiation source material in quantum dot modified nanotubes/holes includes both in situ growth methods and ex situ growth methods.
  • the in-situ growth method is a method for directly growing and depositing an isotope radiation source material on a wide band gap semiconductor nanotube/hole, including electroless plating, electrochemical plating, atomic layer CVD deposition, high temperature and high pressure diffusion, plasma induced implantation, Magnetron sputtering, electron beam/thermal evaporation, and the like.
  • the ex-situ growth method is to first synthesize the isotope radiation source material, and then deposit the isotope radiation source material into the nanotube/hole, including direct adsorption and linker-assisted adsorption.
  • the top electrode 1 and the bottom electrode 5 are each independently selected from the group consisting of metal, semiconductor, graphite, graphene, conductive polymer or conductive paste.
  • the top electrode and the bottom electrode may be of the same material or different materials.
  • a contact potential difference can be formed between the upper and lower plates of the wide band gap semiconductor nanotube/hole array film, and the strong plate electric field facilitates the separation of electron-hole pairs.
  • the quantum band's confinement effect and quantum tunneling effect are used to generate an intermediate band in the semiconductor band gap, thereby widening the absorption range and by impact ionization effect, a high-energy particle can be absorbed.
  • a plurality of electron-hole pairs, that is, multiple exciton effects are generated; carrier transport and separation are also enhanced by quantum tunneling, and carrier recombination probability is reduced.
  • FIG. 1 is a schematic structural view of a first embodiment of a quantum dot beta volt battery of the present invention
  • FIG. 2 is a schematic structural view of a second embodiment of a quantum dot beta volt battery of the present invention.
  • FIG. 3 is a schematic diagram of a multi-cell series-parallel stacking package of a plurality of sets of quantum dot beta volt batteries according to the present invention.
  • the quantum dot beta volt battery structure comprises a top electrode 1, a quantum dot 2, an isotope radiation source 3, a nanotube array film 4, and a bottom electrode 5.
  • the nanotube array film 4 of the present embodiment is formed by vertically stacking a plurality of parallel nanotubes 6 and a bottom electrode 5.
  • the material of the nanotube array film 4 is a wide band gap semiconductor titanium dioxide; the quantum dots 2 are attached to the inner and outer surfaces of the nanotube wall to form a quantum dot layer 7; and the isotope radiation source 3 is deposited on the quantum dot layer 7
  • the surface of the top electrode 2 is gold, the bottom electrode is a titanium sheet; and the isotope radiation source is nickel-63.
  • nanotube array film using titanium metal sheet as anode and platinum metal sheet as cathode, using titanium oxide and ethylene glycol as electrolyte, preparing titanium dioxide on metal titanium sheet by electrochemical anodizing process
  • the nanotube array film has a nanotube diameter of 10 nm to 1000 nm and a nanotube depth of 200 nm to 100 ⁇ m.
  • the sample is then subjected to high temperature annealing in an inert atmosphere or a hydrogen atmosphere; the base titanium sheet of the nanotube serves as the bottom electrode of the battery;
  • nickel-63 metal is electroplated into quantum dot modified titanium dioxide nanotubes by electrochemical plating technology using a solution containing nickel-63 ions as electrolyte;
  • the gold electrode layer was prepared on the surface of the nanotube array film by magnetron sputtering technology, and the electrode material was in full contact with the quantum dot layer and the nickel-63 layer on the top of the nanotube.
  • the thickness of the gold electrode layer is 5 nm to 300 nm.
  • the quantum dot beta volt battery in this example has an energy conversion efficiency of 22%.
  • the quantum dot beta volt battery structure includes a top electrode 1, a quantum dot 2, an isotope radiation source 3, and a nanometer. Tube array film 4, bottom electrode 5.
  • the nanotube array film 4 of the present embodiment is formed by vertically stacking a plurality of parallel nanotubes 6 and a bottom electrode 5.
  • the material of the nanotube array film 4 is a wide band gap semiconductor silicon carbide; the quantum dots 2 are attached to the inner surface of the nanotube wall to form a quantum dot layer 7; the isotope radiation source 3 is deposited on the quantum dot modification In the silicon carbide nanotubes; the top electrode 1 material is gold, the bottom electrode 5 is made of a nickel-gold composite layer; and the isotope radiation source is a deuterated compound.
  • a nickel-gold composite metal layer was deposited on the surface of the silicon carbide wafer by an magnetron sputtering technique as an electrode.
  • the electrode thickness is between 100 nm and 500 nm;
  • nanotube array film Preparation of nanotube array film: using carbon rod as cathode, silicon carbide wafer as anode, using hydrofluoric acid, water and ethanol as electrolyte, using electrochemical anodization technology to prepare silicon carbide on silicon carbide wafer
  • the nanotube array film has a diameter of 10 nm to 1000 nm and a film thickness of 200 nm to 100 ⁇ m;
  • top electrode The gold electrode layer was prepared on the surface of the silicon carbide nanotube array film by magnetron sputtering technology, and the electrode material was in full contact with the quantum dot layer at the top of the nanotube.
  • the thickness of the gold electrode layer is 5 nm to 300 nm, and the nozzle is not blocked;
  • the quantum dot beta volt battery in this example has an energy conversion efficiency of 20%.
  • FIG. 3 is a schematic diagram of a multi-cell series-parallel stacking package of a multi-cell quantum dot betavoltaic cell of the present invention.
  • a plurality of quantum dot betavoltavolt cell units described in Embodiment 1 or Embodiment 2 are stacked in a multi-layer stack by serial-parallel connection, mainly including an external load 8, a power storage system 9, and quantum dots.
  • the specific method for multi-group quantum dot beta volt battery multi-unit series-parallel multi-layer stacking integrated package is as follows: the quantum dot beta volt battery cells described in Embodiment 1 or 2 are stacked in series, and then the plurality of stacks are connected in series. The battery pack is connected in parallel to form a battery with high output power and high output voltage in a series-parallel hybrid integrated package. The power collection, management and application of beta radiation energy conversion is realized by connecting the integrated packaged quantum dot beta volt battery to the power storage system.

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  • Physics & Mathematics (AREA)
  • Engineering & Computer Science (AREA)
  • General Engineering & Computer Science (AREA)
  • High Energy & Nuclear Physics (AREA)
  • Battery Electrode And Active Subsutance (AREA)

Abstract

La présente invention concerne une pile bêtavoltaïque à points quantique qui comprend un film de réseau de nanotubes semi-conducteurs (4) entre une électrode inférieure (5) et une électrode supérieure (1). La paroi interne de chaque nanotube semi-conducteur est revêtue d'une couche de points quantiques (7). La couche de points quantiques (7) est revêtue d'une couche de source de rayonnement d'isotope solide (3), ou l'espace tubulaire enfermé par la couche de points quantiques (7) est rempli d'une source de rayonnement d'isotope gazeux ou liquide. L'introduction de points quantiques dans le nanotube semi-conducteur améliore le courant de court-circuit et la tension de circuit ouvert ainsi que l'efficacité de conversion d'énergie de la pile bêtavoltaïque.
PCT/CN2017/115954 2017-12-13 2017-12-13 Pile bêtavoltaïque à points quantiques Ceased WO2019113842A1 (fr)

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Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN107945901A (zh) * 2017-12-13 2018-04-20 深圳贝塔能量技术有限公司 一种量子点贝塔伏特电池

Citations (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN102543239A (zh) * 2012-01-09 2012-07-04 北京大学 基于碳纳米管薄膜的三维异质结同位素电池及其制备方法
CN103325433A (zh) * 2013-06-20 2013-09-25 北京大学 一种单壁碳纳米管pn结同位素电池及其制备方法
US20140021827A1 (en) * 2012-07-18 2014-01-23 Seerstone Llc Primary voltaic sources including nanofiber schottky barrier arrays and methods of forming same
CN104200864A (zh) * 2014-08-25 2014-12-10 厦门大学 一种基于宽禁带半导体纳米管阵列薄膜结构的同位素电池

Patent Citations (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN102543239A (zh) * 2012-01-09 2012-07-04 北京大学 基于碳纳米管薄膜的三维异质结同位素电池及其制备方法
US20140021827A1 (en) * 2012-07-18 2014-01-23 Seerstone Llc Primary voltaic sources including nanofiber schottky barrier arrays and methods of forming same
CN103325433A (zh) * 2013-06-20 2013-09-25 北京大学 一种单壁碳纳米管pn结同位素电池及其制备方法
CN104200864A (zh) * 2014-08-25 2014-12-10 厦门大学 一种基于宽禁带半导体纳米管阵列薄膜结构的同位素电池

Cited By (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN107945901A (zh) * 2017-12-13 2018-04-20 深圳贝塔能量技术有限公司 一种量子点贝塔伏特电池
CN107945901B (zh) * 2017-12-13 2024-02-09 深圳贝塔能量技术有限公司 一种量子点贝塔伏特电池

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