WO2019113842A1 - Quantum dot betavoltaic battery - Google Patents
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- 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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- G21H1/00—Arrangements for obtaining electrical energy from radioactive sources, e.g. from radioactive isotopes, nuclear or atomic batteries
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- 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.
Abstract
A quantum dot betavoltaic battery, comprising a semiconductor nanotube array film (4) between a bottom electrode (5) and a top electrode (1). The inner wall of each semiconductor nanotube is coated with a quantum dot layer (7). The quantum dot layer (7) is coated with a solid isotope radiation source layer (3), or the tubular space enclosed by the quantum dot layer (7) is filled with a gas or liquid isotope radiation source. The introduction of quantum dots to the semiconductor nanotube improves the short-circuit current and the open-circuit voltage as well as the energy conversion efficiency of the betavoltaic battery.
Description
本发明属于同位素电池领域，具体涉及一种量子点贝塔伏特电池。The invention belongs to the field of isotope batteries, and in particular relates to a quantum dot beta volt battery.
随着物联网技术的发展，能源供给装置的微型化、集成化成为微型传感***发展中迫切需要解决的问题。同时，越来越多的微传感***需要被置于特殊的环境下使用，如深海、深空、地下、极地、荒漠等。这些环境往往需要长寿命、免维护和高可靠的电源***。目前传统的能源由于各自的缺点很难满足使用要求。例如，化学电池能量密度低，高低温性能不稳定，需要频繁地充电。微型燃料电池效率较高，但电池体积大，需要定期向电池内输入燃料。太阳能电池输出功率强度依赖于外部光照和电池板面积。因此，传统的电池并不适用于特殊环境下的电子设备的使用。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. At the same time, 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. At present, traditional energy sources are difficult to meet the requirements of use due to their respective shortcomings. For example, 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.
同位素电池是利用放射性同位素衰变释放的能量转换成电能的自主发电装置，具有能量密度高、寿命长、工作可靠、环境适应性强、无需维护等特点，目前已成为核能源研究的重要方向，其在医学、军事、航空、民用领域等有广阔的应用前景。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.
将同位素辐射衰变能转换为电能主要有4种转换机制：热电转换式、直接充电式、直接能量转换式、间接能量转换式。热电转换式同位素电池使用高能辐射源，使用成本高、难于微型化。直接充电式同位素电池电流很小，驱动能力极弱。间接转换式同位素电池转换效率普遍偏低(<1％)。直接能量转换式同位素电池(又称贝塔伏特电池或β伏特电池)利用贝塔伏特效应，通过收集低能β辐射粒子在半导体材料中激发出的电子和空穴，从而实现电流倍增，可极大地提高了电流密度和转换效率。β伏特同位素电池的能量转换效率随半导体材料禁带宽度的增加而提高，其最高理论的量转换效率可达到32％。虽然贝塔伏特电池有较高的理论能量转换效率，但目前技术实现的转化效率仍低于5％，远未达到工程应用的程度。因此，如何提高贝塔伏特电池的能量转换效率是目前研究的当务之急。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) use the betavolta effect to maximize current doubling by collecting electrons and holes excited by low-energy beta radiation particles in the semiconductor material. Current density and conversion efficiency. The energy conversion efficiency of the β-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%. Although 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.
宽禁带半导体可增大贝塔伏特电池的开路电压，提高电池的输出功率。同
时，宽禁带半导体有高的辐射损伤阈值，具有抗辐射损伤能力强的特点。纳米管/孔材料具有高的比表面积，可极大地提高辐射源与半导体材料的接触面积，从而提高贝塔伏特电池能量转换效率和输出功率。厦门大学的San等人利用宽禁带半导体TiO2三维纳米多孔阵列结构制备了镍-63(Ni-63)贝塔伏特电池，最大有效转化效率达到7.3％(Qiang Zhang,Ranbin Chen,Haisheng San,Guohua Liu,Kaiying Wang,“Betavoltaic effect in titanium dioxide nanotube arrays under build-in potential difference”,Journal of Power Sources,Vol.282:529-533,2015)。但该能量转换效率仍然偏低，人们迫切希望进一步提高能量转换效率。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). Kaiying Wang, "Betavoltaic effect in titanium dioxide nanotube arrays under build-in potential difference", Journal of Power Sources, Vol. 282: 529-533, 2015). However, the energy conversion efficiency is still low, and people are eager to further improve the energy conversion efficiency.
发明内容Summary of the invention
本发明第一方面提供了一种量子点贝塔伏特电池，其包括置于底部电极5和顶部电极1之间的半导体纳米管阵列薄膜4，所述半导体纳米管的管内壁上涂有量子点层7，所述量子点层7上又涂有固态同位素辐射源层3，或者所述量子点层7所围成的管状空间填充有气态或液态同位素辐射源。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.
优选地，所述固态同位素辐射源层3也可以充满所述量子点层7所围成的管状空间。Preferably, the solid isotope radiation source layer 3 may also fill the tubular space enclosed by the quantum dot layer 7.
其中，所述半导体纳米管阵列薄膜4是由多个相互平行的纳米管并排排列而成。The semiconductor nanotube array film 4 is formed by arranging a plurality of mutually parallel nanotubes side by side.
其中，所述量子点层7和所述同位素辐射源层3为连续层或离散层或二者的组合。其可以是一层或多层。Wherein, 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.
优选地，所述半导体纳米管阵列薄膜4为禁带宽度大于2.3eV的晶态宽禁带半导体薄膜，其中半导体材料可以是半导体金属氧化物、半导体化合物和半导体单质中的至少一种。优选地，构成所述纳米管的材料包含二氧化钛、氧化锌、二氧化锆、氧化镉、五氧化二铌、氧化铈、三氧化二镓、二氧化锡、三氧化钨、碳化硅、氮化镓、铟镓氮、磷化镓、氮化铟、氮化铝、磷化铝、砷化铝等、二硫化钼、硫化镉、硫化锌、硫化镁、硒化锌、硒化镁、金刚石等。Preferably, 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. Preferably, 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. , indium gallium nitride, gallium phosphide, indium nitride, aluminum nitride, aluminum phosphide, aluminum arsenide, molybdenum disulfide, cadmium sulfide, zinc sulfide, magnesium sulfide, zinc selenide, magnesium selenide, diamond, etc.
优选地，所述半导体纳米管的管直径为10nm-1000nm，管长为200nm-100μm。
Preferably, the semiconducting nanotube has a tube diameter of 10 nm to 1000 nm and a tube length of 200 nm to 100 μm.
优选地，所述量子点层7为由半径不大于激子波尔半径的半导体材料纳米晶粒所组成的层。量子点是指半径小于或接近于激子玻尔半径的准零维纳米晶粒，其内部的电子在各个方向上的运动都受到限制，这赋予了它独特的性能。所述量子点的尺寸在1～100nm范围。通过适合的量子点材料的选择和调控量子点的尺寸可以改变量子点的能带结构以匹配宽禁带半导体纳米管/孔能带结构，实现贝塔辐射的多激子效，并通过量子点和纳米管/孔接触界面的异质结和量子点之间的量子隧道效应增强载流子的分离和传输。Preferably, 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.
构成所述量子点的所述半导体材料可以选自二氧化钛、氧化锌、二氧化锆、氧化镉、五氧化二铌、氧化铈、三氧化二镓、三氧化二铟、二氧化锡、三氧化钨、铟锡氧、镉铟氧、镉锡氧、碳化硅、氮化镓、铟镓氮、磷化镓、氮化铟、氮化铝、磷化铝、砷化铝、硫化镉、硫化锌、硫化镁、硒化锌、硒化镁、硫化镉、硒化镉、碲化镉、砷化铟、磷化铟、硫化锌、硫化铅、硒化铅、硫化铜、二硫化钼、铜铟硫、三硫化二锑、三硫化二铋、富勒烯、石墨烯或碳。所述的量子点材料的制备方法包括原位生长法和非原位生长法两种。原位生长法是在宽禁带半导体纳米管/孔上直接生长并沉积量子点的一种方法，包括化学浴沉淀法(chemical bath deposition，CBD)和连续离子层吸附与反应法(successive ionic layer absorption and reaction，SILAR)。非原位生长法是先合成量子点，再将量子点沉积宽禁带半导体纳米管/孔上，包括直接吸附和连接剂辅助吸附两种。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. , indium tin oxide, cadmium indium oxygen, cadmium tin oxide, silicon carbide, gallium nitride, indium gallium nitride, gallium phosphide, indium nitride, aluminum nitride, aluminum phosphide, aluminum arsenide, cadmium sulfide, zinc sulfide, Magnesium sulfide, zinc selenide, magnesium selenide, cadmium sulfide, cadmium selenide, cadmium telluride, indium arsenide, indium phosphide, zinc sulfide, lead sulfide, lead selenide, copper sulfide, molybdenum disulfide, copper indium sulfide , antimony trisulfide, antimony trisulfide, fullerene, graphene or carbon. 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). 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.
其中，所述同位素辐射源为在衰变时能够辐射贝塔粒子的辐射源，其半衰期不低于5年。为防止半导体材料的辐射损伤，贝塔粒子的平均能量不高于250KeV。所选的材料可包括氢-3(氚)、镍-63、碳-14、钴-60、钷-146、锶-90、铯-137中的至少一种。氢-3(氚)、镍-63、碳-14、钴-60、钷-146、锶-90、铯-137中的至少一种。可以选用单质或化合态的同位素。所述同位素辐射源材料可以是单一元素材料，也可是同位素与其他材料复合的材料。同位素辐射源的物理形态可以是固体、气体或液体。所述同位素辐射源材料沉积在量子点修饰的纳米管/孔里的方法包括原位生长法和非原位生长法两种。原位生长法是在宽禁带半导体纳米管/孔上直接生长并沉积同位素辐射源材料的一种方法，包括化学镀、电化学镀、原子层CVD沉积、高温高压扩散、等离子诱导注入、
磁控溅射、电子束/热蒸发等。非原位生长法是先合成同位素辐射源材料，再将同位素辐射源材料沉积到纳米管/孔里，包括直接吸附和连接剂辅助吸附两种。Wherein, 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. In order to prevent radiation damage of the semiconductor material, the average energy of the beta particles is not higher than 250 KeV. Selected materials may include at least one of hydrogen-3 (氚), nickel-63, carbon-14, cobalt-60, 钷-146, 锶-90, 铯-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.
其中，所述顶部电极1和底部电极5各自独立地选自金属、半导体、石墨、石墨烯、导电聚合物或导电浆料。顶部电极和底部电极可以是同种材料，也可以是不同种材料。当使用不同导电材料时，由于材料的功函数的不同，可以在宽禁带半导体纳米管/孔阵列薄膜上下两极板间形成接触电势差，强的极板电场有利于电子-空穴对的分离。Wherein, 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. When different conductive materials are used, due to the difference in work function of the 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.
本发明的有益效果：The beneficial effects of the invention:
通过向半导体纳米管内壁上引入量子点，利用量子点的限域效应和量子隧道效应使半导体带隙中产生中间能带，从而拓宽吸光范围，并通过碰撞电离效应，可以使吸收的一个高能粒子产生多个电子-空穴对即多激子效应；还通过量子隧道效应增强载流子的输运和分离，降低载流子复合几率。这些都大大提高了贝塔伏特电池的能量转换效率，其最高理论能量转换效率可达到66％，远远超过常规贝塔伏特电池32％的理论最高能量转换效率。By introducing quantum dots into the inner wall of the semiconductor nanotube, 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. These have greatly improved the energy conversion efficiency of the betavoltaic battery, and its highest theoretical energy conversion efficiency can reach 66%, far exceeding the theoretical maximum energy conversion efficiency of 32% of the conventional betavoltaic battery.
图1为本发明的量子点贝塔伏特电池的第一实施例的结构示意图；1 is a schematic structural view of a first embodiment of a quantum dot beta volt battery of the present invention;
图2为本发明的量子点贝塔伏特电池的第二实施例的结构示意图；2 is a schematic structural view of a second embodiment of a quantum dot beta volt battery of the present invention;
图3为本发明的多组量子点贝塔伏特电池的多单元串并联堆垛封装示意图。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.
其中各附图标记表示以下含义：Each of the reference numerals indicates the following meanings:
1-顶部电极；2-量子点；3-同位素辐射源层；4-半导体纳米管阵列薄膜；5-底部电极；6-纳米管；7-量子点层；8-外接负载；9-储电***；10-量子点贝塔伏特电池单元；11-导线。1-top electrode; 2-quantum dot; 3-isotopic radiation source layer; 4-semiconductor nanotube array film; 5- bottom electrode; 6-nanotube; 7-quantum dot layer; 8-external load; System; 10-quantum dot beta volt battery unit; 11-wire.
提供以下实施例旨在说明本发明的内容，而不是对本发明保护范围的进一
步限定。The following examples are provided to illustrate the contents of the present invention, rather than to further the scope of the present invention.
Step limit.
实施例1Example 1
图1为本发明所述的量子点贝塔伏特电池的第一实施例的结构示意图。如图1所示，所述的量子点贝塔伏特电池结构包括顶部电极1、量子点2、同位素辐射源3、纳米管阵列薄膜4、底部电极5。1 is a schematic view showing the structure of a first embodiment of a quantum dot beta volt battery according to the present invention. As shown in FIG. 1, 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.
本实施例所述纳米管阵列薄膜4是由多个平行的纳米管6与底部电极5垂直堆积而成。所述的纳米管阵列薄膜4的材料为宽禁带半导体二氧化钛；所述的量子点2附着在纳米管壁的内外表面形成量子点层7；所述的同位素辐射源3沉积在量子点层7的表面；所述顶部电极2的材料为金，底部电极为钛片；所述同位素辐射源为镍-63。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.
本实施例所述量子点贝塔伏特电池的制备方法，包含以下步骤：The method for preparing a quantum dot beta volt battery according to this embodiment comprises the following steps:
(1)纳米管阵列薄膜的制备：以金属钛片为阳极，铂金属片为阴极，以氟化胺和乙二醇的混合液为电解液，利用电化学阳极氧化工艺在金属钛片上制备二氧化钛纳米管阵列薄膜，纳米管直径为10nm～1000nm，，纳米管深度为200nm～100μm。然后把样品放在惰性气氛或氢气气氛中进行高温退火；纳米管的基底钛片作为电池的底部电极；(1) Preparation of 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 μm. 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;
(2)量子点修饰的纳米管阵列薄膜制备：将二氧化钛纳米管阵列薄膜在含有硝酸镉的阳离子反应物溶液中放置一段时间，取出后用去离子水冲洗，然后在含有硫化钠阴离子反应物溶液中放置一段时间，使吸附的镉离子与溶液中硫离子充分反应生成一定尺寸的硫化镉量子点，即完成一次沉积循环。如果需要，也可经过多次沉积循环后可形成多层沉积；(2) Preparation of quantum dot modified nanotube array film: The titanium dioxide nanotube array film is placed in a cationic reactant solution containing cadmium nitrate for a period of time, taken out, rinsed with deionized water, and then contained in a solution containing sodium sulfide anion reactant After being placed for a period of time, the adsorbed cadmium ions are fully reacted with the sulfur ions in the solution to form a certain size of cadmium sulfide quantum dots, that is, a deposition cycle is completed. If desired, multilayer deposition can also be formed after multiple deposition cycles;
(3)同位素辐射源在量子点表面的沉积：以含镍-63离子的溶液为电解液，利用电化学电镀技术，把镍-63金属电镀在量子点修饰的二氧化钛纳米管里；(3) Deposition of isotope radiation source on the surface of quantum dots: 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;
(4)顶部电极的制备：利用磁控溅射技术在纳米管阵列薄膜表面制备金电极层，电极材料在纳米管顶部与量子点层和镍-63层充分接触。金电极层的厚度为5nm～300nm。
(4) Preparation of top electrode: 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.
该实施例中的量子点贝塔伏特电池的能量转换效率为22％。The quantum dot beta volt battery in this example has an energy conversion efficiency of 22%.
实施例2Example 2
图2为本发明的量子点贝塔伏特电池的第二实施例的结构示意图；如图2所示，所述的量子点贝塔伏特电池结构包括顶部电极1、量子点2、同位素辐射源3、纳米管阵列薄膜4、底部电极5。2 is a schematic structural view of a second embodiment of a quantum dot beta volt battery according to the present invention; as shown in FIG. 2, 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.
本实施例所述纳米管阵列薄膜4是由多个平行的纳米管6与底部电极5垂直堆积而成。所述的纳米管阵列薄膜4的材料为宽禁带半导体碳化硅；所述的量子点2附着在纳米管壁的内表面形成量子点层7；所述的同位素辐射源3沉积在量子点修饰的碳化硅纳米管里；所述顶部电极1材料为金，底部电极5的材料为镍金复合层；所述同位素辐射源为氚化化合物。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.
本实施例所述的量子点贝塔伏特电池的制备方法，包含以下步骤：The method for preparing a quantum dot beta volt battery according to the embodiment includes the following steps:
(1)底部电极的制备：通过磁控溅射技术在碳化硅晶片表面沉积镍金复合金属层为电极。电极厚度在100nm～500nm；(1) Preparation of bottom electrode: 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;
(2)纳米管阵列薄膜的制备：以碳棒为阴极，碳化硅晶片为阳极，以氢氟酸、水和乙醇的混合液为电解质，利用电化学阳极氧化技术在碳化硅晶片上制备碳化硅纳米管阵列薄膜，纳米管直径为10nm～1000nm，薄膜厚度在200nm～100μm；(2) 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 μm;
(3)量子点修饰的纳米管阵列薄膜制备：把提前制备好的硫化铅量子点与甲苯溶液、全氟磺酸溶液和无水乙醇混合，经室温超声处理后，得到最终的混合溶液。将碳化硅纳米管阵列薄膜列置于真空旋涂仪上，将量子点混合溶液液滴滴在制备碳化硅纳米管阵列薄膜上，通过旋涂的作用，混合溶液就均匀覆盖在碳化硅纳米管阵列的表面。最后在室温下自然晾干；(3) Preparation of quantum dot modified nanotube array film: The lead sulfide quantum dots prepared in advance are mixed with a toluene solution, a perfluorosulfonic acid solution and absolute ethanol, and subjected to ultrasonication at room temperature to obtain a final mixed solution. The silicon carbide nanotube array film is placed on a vacuum spin coater, and the quantum dot mixed solution is dropped onto the prepared silicon carbide nanotube array film, and the mixed solution is evenly covered on the silicon carbide nanotube by spin coating. The surface of the array. Finally, dry naturally at room temperature;
(4)顶部电极的制备：利用磁控溅射技术在碳化硅纳米管阵列薄膜表面制备金电极层，电极材料在纳米管顶部与量子点层充分接触。金电极层的厚度为5nm～300nm，管口未被堵塞；(4) Preparation of 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;
(5)同位素辐射源在量子点表面的沉积：将含有氚化化合物的有机溶剂滴注到限定区域的金电极/量子点/碳化硅纳米管阵列结构薄膜的表面。经烘干
后，氚化化合物附着在量子点修饰的纳米管里。(5) Deposition of the isotope radiation source on the surface of the quantum dot: an organic solvent containing a deuterated compound is dropped onto the surface of the gold electrode/quantum dot/silicon carbide nanotube array structure film of the defined region. Dried
Thereafter, the deuterated compound is attached to the quantum dot modified nanotube.
该实施例中的量子点贝塔伏特电池的能量转换效率为20％。The quantum dot beta volt battery in this example has an energy conversion efficiency of 20%.
实施例3Example 3
图3为本发明的多单元量子点贝塔伏特电池的多单元串并联堆垛封装示意图。如图3所示，将多个实施例1或实施例2所述的量子点贝塔伏特电池单元通过串并联的方式多层堆垛集成封装，主要包括外接负载8、储电***9、量子点贝塔伏特电池单元10以及外接导线11。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. As shown in FIG. 3, 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. Betavolt battery unit 10 and external lead 11.
多组量子点贝塔伏特电池多单元的串并联多层堆垛集成封装的具体方法为：以实施例1或2所述量子点贝塔伏特电池单元依次堆垛串联，然后将多组堆垛串联的电池组进行并联形成串并联混合集成封装的具有高输出功率和高输出电压的电池。通过将集成封装的量子点贝塔伏特电池与储电***连接，实现贝塔辐射能量转换的电量收集、管理和应用。
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.
Claims (10)
- 一种量子点贝塔伏特电池，其特征在于，其包括置于底部电极(5)和顶部电极(1)之间的半导体纳米管阵列薄膜(4)，所述半导体纳米管的管内壁上涂有量子点层(7)，所述量子点层(7)上又涂有固态同位素辐射源层(3)，或者所述量子点层(7)所围成的管状空间填充有气态或液态同位素辐射源。A quantum dot beta voltaic cell comprising a semiconductor nanotube array film (4) disposed between a bottom electrode (5) and a top electrode (1), the inner wall of the tube of the semiconductor nanotube being coated a quantum dot layer (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 gaseous or liquid isotope radiation source.
- 根据权利要求1所述的量子点贝塔伏特电池，其特征在于，所述固态同位素辐射源层(3)充满所述量子点层(7)所围成的管状空间。The quantum dot beta volta cell according to claim 1, characterized in that the solid isotope radiation source layer (3) is filled with a tubular space surrounded by the quantum dot layer (7).
- 根据权利要求1所述的量子点贝塔伏特电池，其特征在于，所述半导体纳米管阵列薄膜(4)是由多个相互平行的纳米管并排排列而成。The quantum dot beta volt battery according to claim 1, wherein the semiconductor nanotube array film (4) is formed by arranging a plurality of mutually parallel nanotubes side by side.
- 根据权利要求1所述的量子点贝塔伏特电池，其特征在于，所述量子点层(7)和所述同位素辐射源层(3)为连续层或离散层或二者的组合。The quantum dot beta volta cell according to claim 1, wherein the quantum dot layer (7) and the isotope radiation source layer (3) are continuous layers or discrete layers or a combination of both.
- 根据权利要求1所述的量子点贝塔伏特电池，其特征在于，所述半导体纳米管阵列薄膜(4)为选自二氧化钛、氧化锌、二氧化锆、氧化镉、五氧化二铌、氧化铈、三氧化二镓、二氧化锡、三氧化钨、碳化硅、氮化镓、铟镓氮、磷化镓、氮化铟、氮化铝、磷化铝、砷化铝等、二硫化钼、硫化镉、硫化锌、硫化镁、硒化锌、硒化镁或金刚石的禁带宽度大于2.3eV的晶态宽禁带半导体材料薄膜。The quantum dot beta volt battery according to claim 1, wherein the semiconductor nanotube array film (4) is selected from the group consisting of titanium dioxide, zinc oxide, zirconium dioxide, cadmium oxide, antimony pentoxide, antimony oxide, Gallium trioxide, tin dioxide, tungsten trioxide, silicon carbide, gallium nitride, indium gallium nitride, gallium phosphide, indium nitride, aluminum nitride, aluminum phosphide, aluminum arsenide, molybdenum disulfide, vulcanization A film of a wide-bandgap semiconductor material having a forbidden band width of more than 2.3 eV of cadmium, zinc sulfide, magnesium sulfide, zinc selenide, magnesium selenide or diamond.
- 根据权利要求1所述的量子点贝塔伏特电池，其特征在于，所述半导体纳米管的管直径为10nm～1000nm，管长为200nm～100μm。The quantum dot beta volt battery according to claim 1, wherein the semiconductor nanotube has a tube diameter of 10 nm to 1000 nm and a tube length of 200 nm to 100 μm.
- 根据权利要求1所述的量子点贝塔伏特电池，其特征在于，所述量子点层(7)为由半径不大于激子波尔半径的半导体材料纳米晶粒所组成的层。The quantum dot beta volta cell according to claim 1, wherein the quantum dot layer (7) is a layer composed of nanocrystallites of semiconductor material having a radius not greater than the exciton Bohr radius.
- 根据权利要求7所述的量子点贝塔伏特电池，其特征在于，所述半导体材料选自二氧化钛、氧化锌、二氧化锆、氧化镉、五氧化二铌、氧化铈、三氧化二镓、三氧化二铟、二氧化锡、三氧化钨、铟锡氧、镉铟氧、镉锡氧、碳化硅、氮化镓、铟镓氮、磷化镓、氮化铟、氮化铝、磷化铝、砷化铝、硫化镉、硫化锌、硫化镁、硒化锌、硒化镁、硫化镉、硒化镉、碲化镉、砷化铟、磷化铟、硫化锌、硫化铅、硒化铅、硫化铜、二硫化钼、铜铟硫、三硫化二锑、三硫化二铋、富勒烯、石墨烯或碳。 The quantum dot beta volt battery according to claim 7, wherein the semiconductor material is selected from the group consisting of titanium dioxide, zinc oxide, zirconium dioxide, cadmium oxide, antimony pentoxide, antimony oxide, gallium trioxide, and trioxide. Di-indium, tin dioxide, tungsten trioxide, indium tin oxide, cadmium indium oxide, cadmium tin oxide, silicon carbide, gallium nitride, indium gallium nitride, gallium phosphide, indium nitride, aluminum nitride, aluminum phosphide, Aluminum arsenide, cadmium sulfide, zinc sulfide, magnesium sulfide, zinc selenide, magnesium selenide, cadmium sulfide, cadmium selenide, cadmium telluride, indium arsenide, indium phosphide, zinc sulfide, lead sulfide, lead selenide, Copper sulfide, molybdenum disulfide, copper indium sulfide, antimony trisulfide, antimony trisulfide, fullerene, graphene or carbon.
- 根据权利要求1所述的量子点贝塔伏特电池，其特征在于，所述同位素辐射源为氢-3(氚)、镍-63、碳-14、钴-60、钷-146、锶-90、铯-137中的至少一种，其放出的贝塔粒子的平均能量不高于250KeV。The quantum dot beta volt battery according to claim 1, wherein the isotope radiation source is hydrogen-3 (氚), nickel-63, carbon-14, cobalt-60, 钷-146, 锶-90, At least one of cesium-137, the average energy of the released beta particles is not higher than 250 KeV.
- 根据权利要求1所述的量子点贝塔伏特电池，其特征在于，所述顶部电极(1)和底部电极(2)各自独立地选自金属、半导体、石墨、石墨烯、导电聚合物或导电浆料。 The quantum dot beta volt battery according to claim 1, wherein the top electrode (1) and the bottom electrode (2) are each independently selected from the group consisting of metal, semiconductor, graphite, graphene, conductive polymer or conductive paste. material.
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