CN102543239B - Three-dimensional heterojunction isotope battery based on carbon nanotube film and preparation method of three-dimensional heterojunction isotope battery - Google Patents
Three-dimensional heterojunction isotope battery based on carbon nanotube film and preparation method of three-dimensional heterojunction isotope battery Download PDFInfo
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- CN102543239B CN102543239B CN201210004773.8A CN201210004773A CN102543239B CN 102543239 B CN102543239 B CN 102543239B CN 201210004773 A CN201210004773 A CN 201210004773A CN 102543239 B CN102543239 B CN 102543239B
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Abstract
The invention discloses a three-dimensional heterojunction isotope battery based on a carbon nanotube film and a preparation method of the three-dimensional heterojunction isotope battery. A transduction structure of the isotope battery comprises a substrate, a back electrode, a patterned insulating layer, and a positive electrode on the insulating layer; the front side of the substrate of the transduction structure is provided with a three-dimensional array structure, and the carbon nanotube film is deposited on the surface of the front side of the first substrate; a heterojunction is formed on a contact part of the carbon nanotube film and the substrate so as to form ohmic contact with the positive electrode; a source structure comprises a substrate and a radioactive isotope film on the surface of the substrate; the source structure and the transduction structure are aligned and sealed together, contact parts of the source structure and the transduction structure are electrically isolated, and the radioactive isotope film of the source structure and the heterojunction of the transduction structure are opposite to each other and are positioned in a cavity formed by sealing. By the three-dimensional structure in the isotope battery, an action area of a device is effectively enlarged, and the performance of the device is improved. Moreover, due to the heterojunction formed by contacting the carbon nanotube film with other semiconductor materials, the conversion efficiency of the isotope battery is improved.
Description
Technical field
The present invention relates to micro isotope battery, particularly isotope battery based on carbon nanotube heterojunction of a kind of three-dimensional and preparation method thereof, belongs to the micro-energy field in MEMS.
Background technology
Micro electro mechanical system (MEMS) technology (be called for short MEMS) is that to take the Design and manufacture of micro-/ nano magnitude be basis, the microsystem that the circuit such as microsensor, microactrator and control, interface and power supply are integrated.In the past few decades MEMS (micro electro mechanical system) is just in develop rapidly, and along with the size reduction of electronic system, development volume is little, lightweight, energy density is high, high life the micro-energy resource system that can continue energy supply have great importance to MEMS (micro electro mechanical system).At present, micro-energy resource system is just becoming one of study hotspot both domestic and external, as micro fuel cell, environmental energy pick-up, micro solar battery etc.But fuel cell needs postcombustion in the course of the work, and micro solar battery needs illumination, and the energy conversion rate of environmental energy pick-up is too low, these energy are used all has certain limitation in MEMS system.Isotope battery is called again nuclear battery, is radioisotopic decay can be directly or indirectly converted to the device of electric energy.Radioisotopic energy density is up to 1-100MJ/cc (traditional fuel energy density is 1-20kJ/cc), and the life-span reaches 1-100, is subject to environmental influence little.Therefore, the research of isotope battery has caused domestic and international researcher's extensive concern.
Isotope battery, by the classification of energy conversion mechanism, comprising: direct charge type isotope battery, contact gesture type isotope battery, p-n junction isotope battery, heat power type isotope battery, thermoelectricity conversion isotope battery, thermionic emission isotope battery, piezoelectricity conversion hysteria isotope battery etc.In above-mentioned these isotope batteries, thermoelectricity conversion isotope battery is most widely used, and the theoretical efficiency of p-n junction isotope battery is up to 40%, is to be used in one of optimal energy conversion mode in MEMS (micro electro mechanical system).
The 1950's, research finds that the β particle that isotope decay produces can produce electron hole pair in semiconductor, and this phenomenon is called as β radiation volta effect.β radiation volta effect is very similar with photovoltaic effect in principle, and difference is that β radiation volta effect is that what photovoltaic effect was used is photon with β particle conversion of energy.With the β particle hits semiconductor material of certain energy, by power electrical effect, near the depletion region of pn knot, produce electron hole pair, under the built in field effect of pn knot, realize the separation to electron hole pair simultaneously, in device terminal, form electric current.In recent years, domestic and international researcher or improve open-circuit voltage and the short-circuit current of battery by changing the structure of silica-based pn knot, or by improving the anti-radiation property of device with irradiation resistant material as GaN, SiC etc., but effect is not very remarkable.
With traditional semiconductor material, compare, carbon nano-tube has unique nanometer one-dimentional structure and excellent electrical properties.The one-dimensional nano structure of carbon nano-tube makes its electronics and have quantum effect along the transmission of tubular axis shear wave, makes carbon nano-tube have high carrier mobility and ballistic transport feature simultaneously.The caliber of carbon nano-tube and helicity have determined its band structure, and its energy gap width can change to silicon and equate from zero.Meanwhile, the porous structure of carbon nano-tube film makes it have very large specific surface area.These features make the heterojunction based on carbon nano-tube become desirable β radiation electric pool structure.
Summary of the invention
The object of the present invention is to provide a kind of heterogeneous three-dimensional isotope battery of becoming transducing structure based on carbon nano-tube film, utilize the ins and outs of carbon nanotube material and the three-dimensional structure of substrate to improve the performance of battery.This isotope battery volume is little, and conversion efficiency is high, and structure and technique simple, be easy to realize, can work long hours, and can work in various complex environments.
Technical scheme of the present invention is as follows:
A kind of 3-D heterojunction isotope battery based on carbon nano-tube film, comprise transducing structure and source structure two parts, wherein: transducing structure comprises the first substrate, be positioned at the back electrode of the first substrate back, and be positioned at the patterned insulation course of the first substrate face and the front electrode on insulation course; The front of described the first substrate has cubical array structure, and surface deposition has carbon nano-tube film; The contact portion of this carbon nano-tube film and the first substrate forms heterojunction, forms Ohmic contact with front electrode; Source structure comprises the second substrate and is positioned at the radioactive isotope film of the second substrate surface; Source structure and transducing structure are aimed at and are sealed, electric isolation between the two position contacting, and the radioactive isotope film of source structure is relative with the heterojunction of transducing structure, is positioned at the cavity that sealing-in forms.
Described the first substrate is the substrate of transducing structure, also be to form the semiconductor of heterojunction with carbon nano-tube film, it can be silicon chip, gallium arsenide film, silicon carbide plate or gallium nitride sheet etc., and the material of the insulation course of its front face surface can be silicon dioxide or silicon nitride etc.Insulation course is in order to prevent that front electrode from directly contacting with substrate.
Front electrode on described insulation course need to form Ohmic contact with carbon nanocapsule thin film, can be selected from one or more of following metal: Au, Pd and Pt etc.
Described insulation course and front electrode are through the certain pattern of graphical formation, and the first substrate face goes out groove at the partial etching that does not cover insulation course and front electrode, forms cubical array structure.Described groove can be reverse pyramid or rectangle etc.
The back electrode material of described the first substrate back can be selected a kind of of following various metals: Au, Al, Pt etc.
Described the second substrate is the substrate of source structure, and it can be metal substrate, and such as nickel sheet and copper sheet etc. can be also non-metal substrate, such as silicon chip and glass sheet etc.
The above-mentioned 3-D heterojunction isotope battery based on carbon nano-tube film can be prepared by following method:
1) according to following step a-d, prepare transducing structure:
A, in the front of the first substrate, form patterned insulation course and front electrode;
B, in the front of the first substrate, form cubical array structure;
C, at the back side of the first substrate, make back electrode;
D, carbon nano-tube film is deposited on to the first substrate face, makes carbon nano-tube film and the first substrate form heterojunction, and form Ohmic contact with front electrode;
2) prepare source structure: deposit radioactive isotope film on the second substrate;
3) heterojunction of the radioactive isotope face that makes source structure to transducing structure, source structure and transducing structure is aimed at and sealed, and electric isolation is realized at the position contacting at the two.
Above-mentioned steps 1) a first forms insulation course in the first substrate face, then on insulation course, adopts the methods such as sputter, evaporation or plating to prepare front metal electrode, and by lithographic definition electrode pattern, method realizes metal patternization to adopt corrosion or peel off etc.; Again by photoetching and front electrode pattern alignment, through dry etching or wet etching, realize insulation course graphical.
Prepared by the mode that above-mentioned steps 1) described in b, cubical array can not cover the first substrate part of insulation course and front electrode by wet etching or dry etching.
Above-mentioned steps 1) described in c, back electrode is metal electrode, can adopt the methods such as sputter, evaporation or plating to prepare.
Above-mentioned steps 1) described in d, carbon nano-tube film can be prepared by direct evaporation method, chemical vapour deposition technique, print process, electrophoresis and filter membrane method etc.
Above-mentioned steps 2) in, the preparation of radioactive isotope film can adopt the methods such as plating or molecular plating or electroless plating.
Above-mentioned steps 3) in, the method for sealing of transducing structure and source structure can bond the two with cementing agent, also can the two be fixed together with external reinforcement fixed structure.
Above-mentioned steps 3) the insulation isolation at position of contacting between transducing structure and source structure in can utilize the insulating washer between the two or directly be made in source structure or the structural insulation system of transducing is realized, also can be by source structure being realized together with transducing construction bonds with all kinds of insulating adhesives such as silica gel or epoxy resin.
The present invention is the 3-D heterojunction isotope battery based on carbon nano-tube film, and it is simple in structure, stable performance, and volume is little; Three-dimensional structure can effectively increase device active area, improves device performance; Adopt carbon nano-tube film to contact the heterojunction forming with other semiconductor materials, can produce high output voltage, output current and current amplification factor, improved the conversion efficiency of isotope battery.Its manufacture process adopts the MEMS technique of standard mostly, and technique is simple, can manufacture in batches, cost is low, yield rate is high, reliability is high; The preparation process in carbon nano-tube film and source is also easier to MEMS technique compatible mutually.
Accompanying drawing explanation
Fig. 1 is the vertical view of the transducing structure prepared of the embodiment of the present invention, has shown the three-dimensional structure of the first substrate, the drawing of the heterojunction that carbon nano-tube film and the first substrate form and front electrode;
Fig. 2 is the sectional view of the isotope battery device prepared of the embodiment of the present invention;
Fig. 3 (a)-Fig. 3 (f) is the three-dimensional process chart based on carbon nano-tube film-silicon heterogenous isotope battery of embodiment of the present invention preparation;
Wherein, 1-transducing structured substrate, 2-transducing structural insulation layer, 3-front electrode, 4-back electrode, 5-carbon nano-tube film, 6-source structure substrate, 7-radioactive isotope film, 8-separation layer.
Embodiment
Below in conjunction with accompanying drawing, by embodiment, the present invention is described in further detail:
As depicted in figs. 1 and 2, the prepared isotope battery of the present embodiment comprises transducing structure and source structure two parts, and the two seals, and contact position is by separation layer 8 electric isolation.Described transducing structure comprises the first substrate (transducing structured substrate) 1, on the first substrate 1 upper surface (front), has stacked gradually through patterned insulation course 2 and front electrode 3; The first substrate 1 front has cubical array structure after graphical and corrosion, at the surface deposition of cubical array structure or whole the first substrate, has carbon nano-tube film 5; The back side of the first substrate 1 is metal back electrode 4.Described source structure comprises the second substrate (source structure substrate) 6 and is positioned at the radioactive isotope film 7 of its lower surface.
Above-mentioned isotope battery is prepared according to following method:
1) preparation of transducing structure
A, get monocrystalline silicon piece a slice (two throwing silicon chips, thickness 400 μ m) as transducing structured substrate (the first substrate) 1, first thermal oxide forms the thick silicon dioxide of 300nm on the first substrate 1 surface, then removes the silicon dioxide at the back side, retains the silicon dioxide of upper surface as insulation course 2, then first sputter adhesion layer Metal Cr on the silicon dioxide of upper surface, thickness 15nm, then splash-proofing sputtering metal Au, thickness 150nm, as front electrode 3, see Fig. 3 (a).
B, front electrode 3 and insulation course 2 photoetching corrosions are gone out to figure, at the positive rectangular array that forms 80 μ m * 80 μ m of the first substrate 1, referring to Fig. 3 (b).
C, by KOH anisotropic etch, at the positive cubical array that forms inverted pyramid groove of the first substrate 1, and do back electrode 4 at first substrate 1 back spatter Metal Cr/Au 15nm/150nm, alloy makes back electrode 4 and the first substrate 1 form Ohmic contact, sees Fig. 3 (c).
D, utilize direct evaporation method at the positive carbon nano-tube film that forms of silicon substrate 1, concrete grammar is as follows:
Carbon nano-tube is dissolved in to dimethyl formamide organic solvent and makes the carbon nano tube suspension that concentration is 5 μ g/ml, by the ultrasonic 2h that surpasses of solution, the first substrate 1 that forms inverted pyramid cubical array structure is placed on heating plate and is heated to 100 ℃, carbon nano tube suspension is dropped on silicon substrate 1, solvent evaporates forms carbon nano-tube film 5, as shown in Fig. 3 (d).
2) making of source structure
Get nickel sheet as source structure substrate (the second substrate) 6, at its positive radioactive isotope film Ni-63 that electroplates 2mCi, form source structure, see Fig. 3 (e).
3) source structure and transducing structure are aimed at, and utilize insulation silica gel as separation layer 8, the two to be bonded together, form three-dimensionally based on carbon nano-tube film-silicon heterogenous isotope battery, see Fig. 3 (f).
The present embodiment provides a kind of structure and preparation method of the isotope battery based on carbon nano-tube film-silicon heterogenous of three-dimensional, and the present invention is not only confined to this embodiment, can make corresponding modification with designing requirement according to actual needs.
Silicon dioxide as insulation course 2 in the present embodiment can be other insulators, and as silicon nitride, thickness is also adjustable.
Front electrode Cr/Au in the present embodiment can be other metals, as Au, Pd and Pt.
Back electrode Cr/Au in the present embodiment can be other metals, as Al, Pt etc.
Front and back metal in the present embodiment adopts sputtering method preparation, also can adopt the methods such as evaporation, plating.
In the present embodiment, carbon nano-tube film preparation method is direct evaporation method, and it also can utilize method preparation, such as chemical vapour deposition technique, print process, electrophoresis and filter membrane method etc.
In the present embodiment, the solvent of carbon nano tube suspension, concentration are all adjustable, and the temperature while directly evaporating is also adjustable.
In the present embodiment, source structure can, with metal as source structure substrate, as sheet metals such as nickel sheet or copper sheets, also can be done substrate with nonmetal semiconductor or insulator, as glass etc.If as substrate, need to the two between insert insulation course when so transducing structure and source structure are fitted together with metal or semiconductor.
In the present embodiment, radioactive isotope can be used plating, and the mode of molecular plating or electroless plating obtains, and radioisotopic radioactive intensity is adjustable.
In the present embodiment, the transducing structure separation layer that contacts with source structure can be insulating washer, or the tack coat that forms of all kinds of insulating adhesives such as silica gel or epoxy resin, or is directly made in source structure or the structural insulation system layer of transducing.
In the present embodiment, the method for sealing of transducing structure and source structure can be to utilize cementing agent that the two is bondd, and also can the two be fixed together with external reinforcement fixed structure.
By embodiment, describe the isotope battery based on carbon nanotube heterojunction provided by the present invention in detail above, it will be understood by those of skill in the art that within not departing from the scope of essence of the present invention, can make certain distortion or modification to the present invention; Its preparation method is also not limited to disclosed content in embodiment.
Claims (10)
1. a 3-D heterojunction isotope battery, comprise transducing structure and source structure two parts, wherein: transducing structure comprises the first substrate, be positioned at the back electrode of the first substrate back, and be positioned at the patterned insulation course of the first substrate face and the front electrode on insulation course; Described the first substrate adopts semiconductor material, and the front of described the first substrate has cubical array structure, and surface deposition has carbon nano-tube film; Thereby this carbon nano-tube film covers the cubical array structure of described the first substrate and the contact portion of the first substrate forms heterojunction, form Ohmic contact with front electrode; Source structure comprises the second substrate and is positioned at the radioactive isotope film that can radiate β particle of the second substrate surface; Source structure and transducing structure are aimed at and are sealed, electric isolation between the two position contacting, and the radioactive isotope film of source structure is relative with the heterojunction of transducing structure, is positioned at the cavity that sealing-in forms.
2. 3-D heterojunction isotope battery as claimed in claim 1, is characterized in that, described the first substrate is silicon chip, gallium arsenide film, silicon carbide plate or gallium nitride sheet; Described insulating layer material is silicon dioxide or silicon nitride; Described front electrode material is selected from one or more of following metal: Au, Pd and Pt; Described back electrode material is selected from one or more of following metal: Au, Al and Pt.
3. 3-D heterojunction isotope battery as claimed in claim 1, is characterized in that, described the first substrate face goes out groove at the partial etching that does not cover insulation course and front electrode, forms cubical array structure.
4. 3-D heterojunction isotope battery as claimed in claim 3, is characterized in that, described groove is reverse pyramid or rectangle.
5. the preparation method of the arbitrary described 3-D heterojunction isotope battery of claim 1～4, comprises the following steps:
1) according to following step a-d, prepare transducing structure:
A, in the front of the first substrate, form patterned insulation course and front electrode;
B, in the front of the first substrate, form cubical array structure;
C, at the back side of the first substrate, make back electrode;
D, carbon nano-tube film is deposited on to the first substrate face, makes carbon nano-tube film and the first substrate form heterojunction, and form Ohmic contact with front electrode;
2) prepare source structure: deposit radioactive isotope film on the second substrate;
3) heterojunction of the radioactive isotope face that makes source structure to transducing structure, source structure and transducing structure is aimed at and sealed, and electric isolation is realized at the position contacting at the two.
6. preparation method as claimed in claim 5, is characterized in that, step 1) a first forms insulation course in the first substrate face, then on insulation course, adopts sputter, evaporation or electric plating method to prepare front metal electrode; By lithographic definition electrode pattern, adopt corrosion or stripping means to realize metal patternization; Again by photoetching and front electrode pattern alignment, through dry etching or wet etching, realize insulation course graphical.
7. preparation method as claimed in claim 5, is characterized in that, step 1) b does not cover the part of insulation course and front electrode at the first substrate face wet etching or dry etching, forms cubical array structure.
8. preparation method claimed in claim 5, is characterized in that, step 1) c adopts sputter, evaporation or electric plating method to make metal back electrode.
9. preparation method claimed in claim 5, is characterized in that, step 1) d prepares carbon nano-tube film by direct evaporation method, chemical vapour deposition technique, print process, electrophoresis or filter membrane method; Step 2) in the method for employing plating or molecular plating or electroless plating, make radioactive isotope film.
10. preparation method claimed in claim 5, it is characterized in that, step 3) transducing structure and source structure contact the electric isolation at position by following method I) or II) realize: I) insulating washer be set between the two or be directly made in source structure or the structural insulation system of transducing, then the two is sealed; II) use insulating adhesive by source structure together with transducing construction bonds.
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| CN103325433B (en) * | 2013-06-20 | 2016-04-20 | 北京大学 | A kind of Single Walled Carbon Nanotube PN junction isotope battery and preparation method thereof |
| CN104658628A (en) * | 2013-11-18 | 2015-05-27 | 胡寻伟 | Thermonuclear electric cell |
| WO2015153187A1 (en) * | 2014-03-31 | 2015-10-08 | Medtronic, Inc. | Nuclear radiation particle power converter |
| CN104200864B (en) * | 2014-08-25 | 2017-05-03 | 厦门大学 | Isotope battery based on wide bandgap semiconductor nano-tube array film structure |
| WO2019113842A1 (en) * | 2017-12-13 | 2019-06-20 | 深圳贝塔能量技术有限公司 | Quantum dot betavoltaic battery |
| CN113290760B (en) * | 2020-04-10 | 2023-06-13 | 广州市香港科大霍英东研究院 | Conductive elastomer based on three-pump folding structure and application thereof |
| CN111968772B (en) * | 2020-08-25 | 2022-12-02 | 中国科学院合肥物质科学研究院 | Heterojunction isotope battery based on graphite alkene |
| CN112750547A (en) * | 2021-01-29 | 2021-05-04 | 厦门大学 | Photovoltaic electrochemical radioisotope battery |
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