CN102543239A - 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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- CN102543239A CN102543239A CN2012100047738A CN201210004773A CN102543239A CN 102543239 A CN102543239 A CN 102543239A CN 2012100047738 A CN2012100047738 A CN 2012100047738A CN 201210004773 A CN201210004773 A CN 201210004773A CN 102543239 A CN102543239 A CN 102543239A
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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 miniature isotope battery, particularly a kind of three-dimensional based on isotope battery of carbon nanotube heterojunction and preparation method thereof, belong to the little energy field in the micromechanics electronic system.
Background technology
Micro electro mechanical system (MEMS) technology (be called for short MEMS) is with the design of micro-/ nano magnitude and is fabricated to the basis, the microsystem that circuit such as microsensor, microactrator and control, interface and power supply are integrated.The past few decades MEMS is just in develop rapidly, and the micro-energy resource system that along with the size of electronic system reduces, the development volume is little, in light weight, energy density is high, the high life also can continue energy supply has great importance to MEMS.At present, micro-energy resource system is just becoming one of domestic and international research focus, like 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, and these energy use all has certain limitation in the MEMS system.Isotope battery is called nuclear battery again, is the device that radioisotopic decay can directly or indirectly be converted into electric energy.Radioisotopic energy density is up to 1-100MJ/cc (the traditional fuel energy density is 1-20kJ/cc), and the life-span reaches 1-100, receives environmental influence little.Therefore, the research of isotope battery has caused domestic and international researcher's extensive concern.
Isotope battery comprises by the classification of energy conversion mechanism: direct charge type isotope battery, contact gesture type isotope battery, p-n junction isotope battery, heat power type isotope battery, thermoelectric conversion isotope battery, thermionic emission isotope battery, piezoelectricity conversion hysteria isotope battery etc.In above-mentioned these isotope batteries, thermoelectric conversion isotope battery is used the most extensive, and the theoretical efficiency of p-n junction isotope battery is to be used in one of optimal energy conversion mode in the MEMS up to 40%.
The 1950's, discover that the β particle that the isotope decay produces can produce electron hole pair in semiconductor, this phenomenon is called as β radiation volta effect.β radiation volta effect is very similar with photovoltaic effect on principle, and difference is that β radiation volta effect is to transform energy with the β particle, and what photovoltaic effect used then is photon.The β particle hits semiconductor material that has certain energy produces electron hole pair through the power electrical effect near the depletion region of pn knot, under the built in field effect of pn knot, realize the separation to electron hole pair simultaneously, forms electric current at the device terminal.In recent years, domestic and international researcher or improve the open-circuit voltage and the short-circuit current of battery through the structure that changes silica-based pn knot, perhaps through using anti-irradiation material such as GaN, SiC to wait to improve the anti-radiation property of device, but effect is not very remarkable.
Compare with traditional semiconductor material, CNT has unique nanometer one-dimentional structure and excellent electrical properties.The one-dimensional nano structure of CNT makes its electronics and have quantum effect along the transmission of tubular axis shear wave, makes CNT have high carrier mobility and ballistic transport characteristics simultaneously.The caliber of CNT and helicity have determined its band structure, and its energy gap width can change to silicon from zero and equate.Simultaneously, the porous structure of carbon nano-tube film makes it have very big specific surface area.These characteristics make the heterojunction based on CNT 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 the transducing structure, utilize the three-dimensional structure of ins and outs and the substrate of carbon nanotube material to improve the performance of battery based on carbon nano-tube film.This isotope battery volume is little, and conversion efficiency is high, and structure is simple with technology, is easy to realization, can work long hours, and can work in various complex environments.
Technical scheme of the present invention is following:
A kind of 3-D heterojunction isotope battery based on carbon nano-tube film; Comprise transducing structure and source structure two parts; Wherein: the transducing structure comprises first substrate; Be positioned at the back electrode of first substrate back, and be positioned at the patterned insulation course of first substrate face and the front electrode on the insulation course; The front of said first substrate has the cubical array structure, and surface deposition has carbon nano-tube film; The contact portion of this carbon nano-tube film and first substrate forms heterojunction, forms Ohmic contact with front electrode; Source structure comprises second substrate and the radioactive isotope film that is positioned at second substrate surface; Source structure and transducing structure are aimed at and are sealed, electric isolation between the two contacted position, and the heterojunction of the radioactive isotope film of source structure and transducing structure is relative, is positioned at the cavity that sealing-in forms.
Said first substrate is the substrate of transducing structure; It also is the semiconductor that forms 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 the said insulation course need form Ohmic contact with carbon nanocapsule thin film, can be selected from one or more of following metal: Au, Pd and Pt etc.
Said insulation course and front electrode are through the certain pattern of graphical formation, and first substrate face goes out groove at the partial etching that does not cover insulation course and front electrode, forms the cubical array structure.Said groove can be inverted pyramid shape or rectangle etc.
The back electrode material of said first substrate back can be selected a kind of of following multiple metal: Au, Al, Pt etc.
Said second substrate is the substrate of source structure, and it can be a metal substrate, and for example nickel sheet and copper sheet etc. also can be non-metal substrate, for example silicon chip and glass sheet etc.
Above-mentioned 3-D heterojunction isotope battery based on carbon nano-tube film can prepare through following method:
1) prepare the transducing structure according to following step a-d:
A, form patterned insulation course and front electrode in the front of first substrate;
B, form the cubical array structure in the front of first substrate;
C, make back electrode at the back side of first substrate;
D, carbon nano-tube film is deposited on first substrate face, makes the carbon nano-tube film and first substrate form heterojunction, and form Ohmic contact with front electrode;
2) preparation source structure: deposit radioactive isotope film on second substrate;
3) make the heterojunction of the radioactive isotope face of source structure, source structure and transducing structure aligning are sealed, and realize electric isolation at the two contacted position to the transducing structure.
Above-mentioned steps 1) a forms earlier insulation course in first substrate face, on insulation course, adopts methods such as sputter, evaporation or plating to prepare the front metal electrode then, and through the lithographic definition electrode pattern, method realizes metal patternization to adopt corrosion or peel off etc.; Through photoetching and front electrode pattern alignment, realize that through dry etching or wet etching insulation course is graphical again.
Above-mentioned steps 1) the said cubical array of b can prepare through the mode that wet etching or dry etching do not cover first substrate part of insulation course and front electrode.
Above-mentioned steps 1) the said back electrode of c is a metal electrode, can adopt methods such as sputter, evaporation or plating to prepare.
Above-mentioned steps 1) the said carbon nano-tube film of d can wait through direct evaporation method, chemical vapour deposition technique, print process, electrophoresis and filter membrane method and prepare.
Above-mentioned steps 2) preparation of radioactive isotope film can be adopted plating or methods such as molecular plating or electroless plating in.
Above-mentioned steps 3) method for sealing of transducing structure and source structure can bond the two with cementing agent in, also can the two be fixed together with the external reinforcement fixed structure.
Above-mentioned steps 3) insulation at position of contacting between transducing structure and the source structure in is isolated and can be utilized the insulating washer between the two or directly be made in source structure or the structural insulation system of transducing is realized, also can source structure and transducing construction bonds be realized together through using all kinds of insulating adhesives such as silica gel or epoxy resin.
The present invention is based on the 3-D heterojunction isotope battery of carbon nano-tube film, and it is simple in structure, stable performance, and volume is little; Three-dimensional structure can effectively increase the device active area, improves device performance; Adopt carbon nano-tube film to contact the heterojunction that forms 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 technology of standard mostly, and technology is simple, can make in batches, cost is low, yield rate is high, reliability is high; The preparation process in carbon nano-tube film and source also is easier to compatible mutually with MEMS technology.
Description of drawings
Fig. 1 is the vertical view of the transducing structure of embodiment of the invention preparation, has shown the three-dimensional structure of first substrate, the carbon nano-tube film and the heterojunction of first substrate formation and drawing of front electrode;
Fig. 2 is the sectional view of the isotope battery device of embodiment of the invention preparation;
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 invention preparation;
Wherein, 1-transducing structured substrate, 2-transducing structure insulation course, 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, the present invention is described in further detail through embodiment:
As depicted in figs. 1 and 2, the prepared isotope battery of present embodiment comprises transducing structure and source structure two parts, and the two is sealed, and the contact position is through separation layer 8 electric isolation.Said transducing structure comprises first substrate (transducing structured substrate) 1, on first substrate, 1 upper surface (front), has stacked gradually through patterned insulation course 2 and front electrode 3; First substrate 1 is positive to have the cubical array structure through after graphical and the corrosion, at the surface deposition of cubical array structure or whole first substrate carbon nano-tube film 5 is arranged; The back side of first substrate 1 is metal back electrode 4.Said source structure then comprises second substrate (source structure substrate) 6 and the radioactive isotope film 7 that is positioned at its lower surface.
Above-mentioned isotope battery prepares 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 (first substrate) 1, at first thermal oxide forms the thick silicon dioxide of 300nm on first substrate, 1 surface; Remove the silicon dioxide at the back side then, the silicon dioxide that keeps upper surface is as insulation course 2, then first sputter adhesion layer Metal Cr on the silicon dioxide of upper surface; Thickness 15nm, splash-proofing sputtering metal Au again, thickness 150nm; As front electrode 3, see Fig. 3 (a).
B, frontal electrode 3 and insulation course 2 photoetching corrosions go out figure, at first substrate, the 1 positive rectangular array that forms 80 μ m * 80 μ m, referring to Fig. 3 (b).
C, through the KOH anisotropic etch; At first substrate, the 1 positive cubical array that forms the inverted pyramid groove; And do back electrode 4 at first substrate, 1 back spatter Metal Cr/Au 15nm/150nm, alloy makes the back electrode 4 and 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 following:
CNT is dissolved in the dimethyl formamide organic solvent processes the carbon nano tube suspension that concentration is 5 μ g/ml; With the ultrasonic 2h that surpasses of solution; First substrate 1 that forms inverted pyramid cubical array structure is placed on is heated to 100 ℃ on the heating plate; Carbon nano tube suspension is dropped on the silicon substrate 1, and solvent evaporates forms carbon nano-tube film 5, shown in Fig. 3 (d).
2) making of source structure
Get the nickel sheet as source structure substrate (second substrate) 6,, form source structure, see Fig. 3 (e) at its positive radioactive isotope film Ni-63 that electroplates 2mCi.
3) source structure and transducing structure are aimed at, and utilize insulation silica gel the two to be bonded together, form three-dimensionally, see Fig. 3 (f) based on carbon nano-tube film-silicon heterogenous isotope battery as separation layer 8.
Present embodiment provides a kind of structure and preparation method based on the isotope battery of carbon nano-tube film-silicon heterogenous of three-dimensional, and the present invention not only is 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 like silicon nitride, thickness is scalable also.
Front electrode Cr/Au in the present embodiment can be other metals, like Au, Pd and Pt.
Back electrode Cr/Au in the present embodiment can be other metals, like Al, Pt etc.
Front and back metal in the present embodiment adopts the sputtering method preparation, also can adopt methods such as evaporation, plating.
The carbon nano-tube film preparation method is direct evaporation method in the present embodiment, and it also can utilize method preparation, for example chemical vapour deposition technique, print process, electrophoresis and filter membrane method etc.
The solvent of carbon nano tube suspension, concentration are all adjustable in the present embodiment, and the temperature when directly evaporating is also adjustable.
Source structure can use metal as the source structure substrate in the present embodiment, like sheet metals such as nickel sheet or copper sheets, also can do substrate with nonmetal semiconductor or insulator, like glass etc.If as substrate, need between the two, insert insulation course when so transducing structure and source structure being fitted together with metal or semiconductor.
Radioactive isotope can use plating in the present embodiment, and the mode of molecular plating or electroless plating obtains, and radioisotopic radioactive intensity is adjustable.
The transducing structure separation layer that contacts with source structure can be an insulating washer in the present embodiment, or the tack coat that forms of all kinds of insulating adhesives such as silica gel or epoxy resin, or directly is made in source structure or the structural insulation system layer of transducing.
The method for sealing of transducing structure and source structure can be to utilize cementing agent that the two is bondd in the present embodiment, also can the two be fixed together with the external reinforcement fixed structure.
More than describe the isotope battery based on carbon nanotube heterojunction provided by the present invention in detail through embodiment, it will be understood by those of skill in the art that in the scope that does not break away from essence of the present invention, can make certain deformation or modification to the present invention; Its preparation method also is not limited to disclosed content among the embodiment.
Claims (10)
1. 3-D heterojunction isotope battery; Comprise transducing structure and source structure two parts; Wherein: the transducing structure comprises first substrate, is positioned at the back electrode of first substrate back, and is positioned at the patterned insulation course of first substrate face and the front electrode on the insulation course; The front of said first substrate has the cubical array structure, and surface deposition has carbon nano-tube film; The contact portion of this carbon nano-tube film and first substrate forms heterojunction, forms Ohmic contact with front electrode; Source structure comprises second substrate and the radioactive isotope film that is positioned at second substrate surface; Source structure and transducing structure are aimed at and are sealed, electric isolation between the two contacted position, and the heterojunction of the radioactive isotope film of source structure and transducing structure is relative, is positioned at the cavity that sealing-in forms.
2. 3-D heterojunction isotope battery as claimed in claim 1 is characterized in that, said first substrate is silicon chip, gallium arsenide film, silicon carbide plate or gallium nitride sheet; Said insulating layer material is silicon dioxide or silicon nitride; Said front electrode material is selected from one or more of following metal: Au, Pd and Pt; Said 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, said first substrate face goes out groove at the partial etching that does not cover insulation course and front electrode, forms the cubical array structure.
4. 3-D heterojunction isotope battery as claimed in claim 1 is characterized in that, said groove is inverted pyramid shape or rectangle.
5. the preparation method of the arbitrary said 3-D heterojunction isotope battery of claim 1～4 may further comprise the steps:
1) prepare the transducing structure according to following step a-d:
A, form patterned insulation course and front electrode in the front of first substrate;
B, form the cubical array structure in the front of first substrate;
C, make back electrode at the back side of first substrate;
D, carbon nano-tube film is deposited on first substrate face, makes the carbon nano-tube film and first substrate form heterojunction, and form Ohmic contact with front electrode;
2) preparation source structure: deposit radioactive isotope film on second substrate;
3) make the heterojunction of the radioactive isotope face of source structure, source structure and transducing structure aligning are sealed, and realize electric isolation at the two contacted position to the transducing structure.
6. preparation method as claimed in claim 5 is characterized in that, step 1) a forms insulation course earlier in first substrate face, on insulation course, adopts sputter, evaporation or electric plating method to prepare the front metal electrode then; Through the lithographic definition electrode pattern, adopt corrosion or stripping means to realize metal patternization; Through photoetching and front electrode pattern alignment, realize that through dry etching or wet etching insulation course is graphical again.
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 the cubical array structure.
8. the described preparation method of claim 5 is characterized in that, step 1) c adopts sputter, evaporation or electric plating method to make metal back electrode.
9. the described preparation method of claim 5 is characterized in that, step 1) d prepares carbon nano-tube film through direct evaporation method, chemical vapour deposition technique, print process, electrophoresis or filter membrane method; Step 2) makes the radioactive isotope film in the method for employing plating or molecular plating or electroless plating.
10. the described preparation method of claim 5; It is characterized in that; Step 3) transducing structure and source structure contact the electric isolation at position through following method I) or II) realize: insulating washer I) is set between the two or directly is made in source structure or the structural insulation system of transducing, again the two is sealed; II) use insulating adhesive that source structure and transducing construction bonds are in the same place.
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| CN104200864A (en) * | 2014-08-25 | 2014-12-10 | 厦门大学 | Isotope battery based on wide bandgap semiconductor nano-tube array film structure |
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| WO2019113842A1 (en) * | 2017-12-13 | 2019-06-20 | 深圳贝塔能量技术有限公司 | Quantum dot betavoltaic battery |
| CN113290760A (en) * | 2020-04-10 | 2021-08-24 | 广州市香港科大霍英东研究院 | Conductive elastomer based on three-pump folding structure and application thereof |
| 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 |
| CN111968772A (en) * | 2020-08-25 | 2020-11-20 | 中国科学院合肥物质科学研究院 | Heterojunction isotope battery based on graphene |
| 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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