CN103325433B - A kind of Single Walled Carbon Nanotube PN junction isotope battery and preparation method thereof - Google Patents
A kind of Single Walled Carbon Nanotube PN junction isotope battery and preparation method thereof Download PDFInfo
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- CN103325433B CN103325433B CN201310247435.1A CN201310247435A CN103325433B CN 103325433 B CN103325433 B CN 103325433B CN 201310247435 A CN201310247435 A CN 201310247435A CN 103325433 B CN103325433 B CN 103325433B
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Abstract
The invention discloses a kind of Single Walled Carbon Nanotube PN junction isotope battery and preparation method thereof.The metal electrode pair that the transducing unit of this isotope battery comprises substrate I, back electrode, patterned insulation course and is positioned on insulation course, and align the semi-conductive single-walled carbon nanotubes contacted with substrate I between metal electrode pair; The two ends of described Single Walled Carbon Nanotube form Ohmic contact with two metal electrodes respectively, and center section contacts with substrate I and forms PN junction; Radiation source comprises substrate II and radioactive isotope film; Described radiation source and transducing elemental area opposite are aimed at and are sealed, electric isolation between the position of the two contact, described radioactive isotope film and Single Walled Carbon Nanotube are positioned at the cavity that sealing-in is formed, and a metal electrode in described substrate I upper surface and back electrode form battery electrode.This isotope battery has that volume is little, structure is simple, be easy to the feature realized, and conversion efficiency is higher, can work long hours in various complex environment.
Description
Technical field
The present invention relates to isotope battery, particularly a kind of Single Walled Carbon Nanotube PN junction isotope battery and preparation method thereof, belong to the micro-energy field in MEMS.
Background technology
Along with the development of MEMS (MicroelectroMechanicalSystem) rapid technological improvement, and the feature of its application terminal " light, thin, short, little ", the application of MEMS is increasingly extensive, and the figure of MEMS product has also appearred in the field such as consumer electronics, medical treatment in a large number.MEMS technology is that functional integrated in micro volume provides possibility, but same yardstick just becomes difficulty for Power supply unit.Traditional energy meets with bottleneck when providing the energy for MEMS, as low in very small chemical battery (lithium battery) energy density, the life-span is short, and micro solar battery is again by restrictions such as illumination conditions.
Therefore, many researchers give very large concern for micro-energy resource supply, and research finds that isotope battery has the advantages such as energy density high (1-100MJ/cc), life-span long (1-100), non-maintaining, strong interference immunity.Isotope battery is the supply unit of emitted particle when utilizing radioisotope decays (as α particle, β particle and gamma-rays) institute kinetic energy generating.Isotope battery can be divided into by changing the mechanism generally directly changes the mechanism (as direct charging modes and radiation volta effect etc.) and indirect conversion mechanism (causing fluorescence volta effect and thermionic emission etc. as ray).In above-mentioned isotope battery, had a good application prospect by the radiation voltaic element of PN junction as transducing unit, PN junction radiation voltaic element energy conversion efficiency in theory maximum possible reaches 40%.
Rappaport seminar found in nineteen fifty-three, and 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 particle-irradiation, on semiconductor material, produces electron-hole pair by ionisation effect.When electron-hole pair diffuses to depletion region (restraining barrier) of semiconductor PN, under the effect of PN junction built in field, realize the separation to electron-hole pair, generation current exports.In recent years, domestic and international researcher or improve the conversion efficiency of battery by the structure such as porous silicon, the three-dimensional structure etc. that change PN junction, or by using new material such as SiC etc. to improve the Flouride-resistani acid phesphatase of device, but the conversion efficiency of β radiation battery is all low than expected results.
Because carbon nano-tube has unique nanometer one-dimentional structure and unusual electrical properties, and the energy gap width of carbon nano-tube can change to equal with silicon from zero, show as semiconductive.The β radiation battery material that these features make carbon nano-tube become desirable.At present, the micro isotope battery based on carbon nano-tube mainly contains two classes, and a class is film-type, forms primarily of carbon nano-tube film and semiconductor substrate materials; Another kind of is haplotype, forms primarily of single or multiple semi-conductive single-walled carbon nanotubes and low workfunction metal.Although film-type structure is simple, handling ease, its performance can not show a candle to haplotype.In existing haplotype structure, the contact area of Single Walled Carbon Nanotube and low workfunction metal is very limited, only has end about tens nanometer range, makes the heterojunction area for energy conversion very little.On the other hand, because the energy gap of Single Walled Carbon Nanotube is less, the space charge sector width formed with Metal Contact is also relatively little.These 2 greatly limit haplotype energy conversion effect volume, also make performance be difficult to further raising.
Summary of the invention
For above problem, the present invention proposes a kind of Single Walled Carbon Nanotube PN junction isotope battery.It utilizes P-type semiconductor Single Walled Carbon Nanotube and N-type semiconductor substrate contact to form the transducing structure of PN junction as isotope battery.
Technical scheme of the present invention is as follows:
A kind of Single Walled Carbon Nanotube PN junction isotope battery, comprises transducing unit and radiation source two parts.Transducing unit comprises substrate I, is positioned at the back electrode at the substrate I back side, is positioned at the patterned insulation course of substrate I upper surface and is positioned at metal electrode pair on insulation course, and aligns the Single Walled Carbon Nanotube contacted with substrate I between metal electrode pair.Described metal electrode is to the metal adopting work function higher than Single Walled Carbon Nanotube Fermi level.The two ends of described Single Walled Carbon Nanotube form Ohmic contact with two metal electrodes respectively, and center section contacts with substrate I and forms PN junction.Radiation source comprises substrate II and is deposited on the radioactive isotope film on substrate II.Radiation source and transducing elemental area opposite are aimed at and are sealed, electric isolation between the position of the two contact, described radioactive isotope film and Single Walled Carbon Nanotube are positioned at the cavity that sealing-in is formed, and a metal electrode in described substrate I upper surface and back electrode form battery electrode.
Described substrate I is the N-type semiconductor substrate of transducing unit, and it can be silicon chip, gallium arsenide film, silicon carbide plate or gallium nitride sheet etc., and the material of the insulation course on surface can be silicon dioxide, silicon nitride or hafnia etc.
Described Single Walled Carbon Nanotube is P-type semiconductor Single Walled Carbon Nanotube, and its two ends form Ohmic contact with two metal electrodes respectively, and center section contacts with N-type semiconductor substrate I and forms PN junction, forms the transducing structure of this isotope battery.
Described metal electrode to can be comb electrodes to, interdigital electrode to or the electrode of other simple structures.
Described work function can be selected from one or more in following metal higher than the metal of Single Walled Carbon Nanotube Fermi level: Au, Pd and Pt etc.
Described substrate II is the substrate of radiation source structure, and it can be metal substrate, such as nickel sheet and copper sheet etc., also can be nonmetallic substrate, such as silicon chip and glass sheet etc.
The above-mentioned PN junction isotope battery preparation method based on Single Walled Carbon Nanotube is as follows:
1) transducing unit is prepared according to following step a-e:
A, form insulation course at substrate I upper surface, and make patterned metal electrode pair on the insulating layer, the electrode of this electrode pair is the metal of work function higher than Single Walled Carbon Nanotube Fermi level;
B, the back side of substrate I make back electrode;
C, Single Walled Carbon Nanotube is assembled in described metal electrode between, the two ends of Single Walled Carbon Nanotube are contacted with two metal electrodes respectively;
D, removal metallic single-wall carbon nano-tube, retain semi-conductive single-walled carbon nanotubes;
Insulation course on e, wet etching substrate I, utilizes solution surface tension effect that semi-conductive single-walled carbon nanotubes is formed with substrate I in good condition and contacts.
2) radiation source is prepared: deposit radioactive isotope film on substrate II;
3) there are by radiation source the face of radioactive isotope film and transducing unit to have relative aligning the in the face of Single Walled Carbon Nanotube to seal, and realize electric isolation at the position of the two contact.
Above-mentioned steps 1) methods such as sputtering, evaporation, plating can be adopted to prepare metal electrode pair in a, by lithographic definition electrode pattern, adopt the methods such as corrosion or stripping to realize metal patternization.
Above-mentioned steps 1) back electrode described in b is metal electrode, and the methods such as sputtering, evaporation or plating can be adopted to prepare.
Above-mentioned steps 1) method that Single Walled Carbon Nanotube is assembled between metal electrode pair of c mainly contains chemical vapor deposition, dielectrophoresis and arc discharge method etc.;
Above-mentioned steps 1) d by applying larger voltage or electric current burns metallic single-wall carbon nano-tube between two metal electrodes, retain semi-conductive single-walled carbon nanotubes.
Above-mentioned steps 1) e wet etching insulation course makes semi-conductive single-walled carbon nanotubes contact with substrate I to form PN junction.
Above-mentioned steps 2) in the preparation of radioactive isotope film can adopt plating or the method such as molecular plating or electroless plating.
Above-mentioned steps 3) in the method for sealing of radiation source structure and transducing unit with cementing agent, the two can be bondd, also with external reinforcement fixed structure, the two can be fixed together.
Above-mentioned steps 3) in electric isolation between transducing unit and radiation source contact site insulating washer can be set between or realize by directly this insulation system being produced on radiation source structure or transducing unit, also can realize by using all kinds of insulating adhesive such as silica gel or epoxy resin radiation source structure and transducing unit to be sticked together.
The present invention proposes a kind of Single Walled Carbon Nanotube PN junction isotope battery.It utilizes P-type semiconductor Single Walled Carbon Nanotube and N-type semiconductor substrate contact to form the transducing structure of PN junction as isotope battery, is a kind of New Type of Carbon nanotube haplotype micro isotope battery.This battery adopts single wall semiconductive carbon nano tube structure, its structural integrity, compared with carbon nano-tube film, greatly can reduce the recombination rate of electron hole pair in interface that radiation produces, improve the conversion efficiency of isotope battery.On the other hand, except the region that metal electrode contact end portion is very little, Single Walled Carbon Nanotube major part region can contact completely with N-type semiconductor substrate, not only greatly increase the junction area of PN junction, and there is larger energy gap due to N-type semiconductor substrate, make also significantly being increased of space charge sector width, thus improve electron hole pair separation rate.Process aspect owing to only needing a kind of metal as electrode, the preparation technology of this Single Walled Carbon Nanotube PN junction isotope battery also comparatively before simple.Therefore this isotope battery has that volume is little, structure is simple, be easy to the feature realized, and conversion efficiency is higher, can work long hours in various complex environment.
Accompanying drawing explanation
Fig. 1 is the vertical view of PN junction transducing unit prepared by the embodiment of the present invention, shows single-root carbon nano-tube and the right symmetric contact of metal electrode, with the contact of N-type semiconductor substrate;
Fig. 2 is the sectional view of isotope battery device prepared by the embodiment of the present invention;
Fig. 3 (a)-Fig. 3 (g) is for embodiment of the present invention preparation is based on the process chart of the isotope battery of Single Walled Carbon Nanotube;
Wherein, 1-transducing unit substrate, 2-transducing unit insulation course, 3-high-work-function metal electrode, 4-Single Walled Carbon Nanotube, 5-metal back electrode, 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 isotope battery prepared by the present embodiment comprises transducing unit and radiation source two parts, and the two seals, and is contacted and electric isolation by separation layer 8.This transducing structure comprises substrate I(transducing structured substrate) 1, surface is insulation course 2 on substrate 1, insulation course 2 has the metal electrode pair that two comb-like electrodes are formed, it is all high-work-function metal electrode 3, metal electrode between oriented alignment have single wall semiconductive carbon nano tube 4, and contact with substrate 1 and form PN junction, the back side of substrate 1 is metal back electrode 5.Radiation source structure then comprises substrate II(source structure substrate) 6 and be positioned at the radioactive isotope film 7 on its surface.
Above-mentioned isotope battery is prepared according to following method:
1) preparation of transducing unit
A, get the substrate I of monocrystalline silicon piece a slice (two throwing silicon chip, 400 μm) as transducing structure, thermal oxide forms the silicon dioxide of 100nm, then removes the silicon dioxide at the back side, and the silicon dioxide retaining upper surface, as insulation course 2, is shown in Fig. 3 (a).
B, photoetching sputter adhesion layer Metal Cr 20nm on insulation course 2, sputter high-work-function metal Au150nm again, use lift-off technology to obtain the figure of high-work-function metal electrode 3, the width of each comb of this electrode is 3 μm, length is 30 μm, and each comb tooth spacing is 5 μm.
To the structure after preparing as shown in Figure 3 (b), the high-work-function metal electrode 3 of comb teeth-shaped forms 30 electrode pairs (showing 5 electrode pairs in Fig. 1) to metal electrode altogether, and the spacing between each electrode pair is 3 μm.
C, do back electrode 5 at transducing unit substrate 1 back spatter Metal Cr/Au20nm/150nm, and alloy, form Ohmic contact with silicon substrate 1, see Fig. 3 (c).
D, utilize dielectrophoresis method to carry out Single Walled Carbon Nanotube assembling, concrete grammar is as follows:
Single Walled Carbon Nanotube is dissolved in dimethyl formamide and makes Single Walled Carbon Nanotube suspending liquid, by ultrasonic for solution 2h, the peak-to-peak value that two metal electrodes 3 apply 5MHz is the alternating voltage of 5V, then by made Single Walled Carbon Nanotube hanging drop on two electrodes, Single Walled Carbon Nanotube is assembled into the Single Walled Carbon Nanotube aligned under the effect of dielectrophoresis power, the suspending liquid nitrogen gun on electrode is blown away after 30s.
E, overleaf electrode apply 10V voltage makes the semi-conductive single-walled carbon nanotubes in front be in cut-off state, a metal electrode adds malleation, another metal electrode ground connection, apply 15V voltage, burn metallic Single Walled Carbon Nanotube, obtain the semi-conductive single-walled carbon nanotubes 4 aligned between electrode pair, as shown in Fig. 3 (d).
Insulation course on f, wet etching substrate I, utilizes the surface tension of solution that Single Walled Carbon Nanotube is formed with substrate I and contacts, and forms PN junction, as Fig. 3 (e).
2) making of radiation source structure
Get nickel sheet as source structure substrate 6, at front plating 3.3mCi/cm
2radioactive isotope film Ni-63, formed source structure, see Fig. 3 (f).
3) radiation source is had the face of radioactive isotope film and transducing unit have Single Walled Carbon Nanotube in the face of accurate, and utilize insulation silica gel the two to be bonded together as separation layer 8, form the isotope battery based on Single Walled Carbon Nanotube, see Fig. 3 (g).
Present embodiments provide a kind of structure and preparation method of the isotope battery based on P-type semiconductor Single Walled Carbon Nanotube, the present invention is not only confined to this embodiment, can make corresponding amendment according to actual needs with designing requirement.
In the present embodiment, the thickness of substrate I, doping content are realize higher conversion efficiency all can regulate.
Can be other insulators as the silicon dioxide of insulation course 2 in the present embodiment, as silicon nitride or hafnia, thickness be also adjustable.
In the present embodiment, high-work-function metal Au can be other metals, as Pd, Pt etc., and structure, size, logarithm (showing 5 electrode pairs in Fig. 1) and the equal adjustable of spacing that metal electrode is right.
In the present embodiment, the concentration of Single Walled Carbon Nanotube suspending liquid is adjustable, magnitude of voltage during assembling and frequency-adjustable, and built-up time is also adjustable.
In the present embodiment, radioactive isotope can be other radioelement, as tritium etc.
In the present embodiment, radiation source with metal as source structure substrate, as the sheet metal such as nickel sheet or copper sheet, also can do substrate, as glass etc. with non-metal semiconductive or insulator.If with metal or semiconductor as substrate, need when so transducing unit and radiation source being fitted together to insert insulation course between.
In the present embodiment, radioactive isotope can use plating, and the mode of molecular plating or electroless plating obtains, and radioisotopic radioactive intensity is adjustable.
In the present embodiment, the transducing unit separation layer that contacts with radiation source structure can be insulating washer, or the tack coat that all kinds of insulating adhesive such as silica gel or epoxy resin is formed, or is directly produced in source structure or transducing structure by insulation system layer.
In the present embodiment, the method for sealing of transducing structure and source structure can be utilize cementing agent the two to be bondd, and also the two can be fixed together with external reinforcement fixed structure.
Describe Single Walled Carbon Nanotube PN junction isotope battery provided by the present invention in detail by embodiment above, it will be understood by those of skill in the art that in the scope not departing from essence of the present invention, certain distortion or amendment can be made to the present invention; Its preparation method is also not limited to content disclosed in embodiment.
Claims (10)
1. a Single Walled Carbon Nanotube PN junction isotope battery, comprise transducing unit and radiation source two parts, wherein: transducing unit comprises N-type semiconductor substrate I, be positioned at the back electrode at the N-type semiconductor substrate I back side, be positioned at the patterned insulation course of N-type semiconductor substrate I upper surface and be positioned at metal electrode pair on insulation course, and align the P-type semiconductor Single Walled Carbon Nanotube contacted with N-type semiconductor substrate I between metal electrode pair; Described metal electrode is to the metal adopting work function higher than P-type semiconductor Single Walled Carbon Nanotube Fermi level; The two ends of described P-type semiconductor Single Walled Carbon Nanotube form Ohmic contact with two metal electrodes respectively, and center section contacts with N-type semiconductor substrate I and forms PN junction; Radiation source comprises substrate II and is deposited on the radioactive isotope film on substrate II; Described radiation source and transducing elemental area opposite are aimed at and are sealed, electric isolation between the position of the two contact, described radioactive isotope film and P-type semiconductor Single Walled Carbon Nanotube are positioned at the cavity that sealing-in is formed, and a metal electrode in described N-type semiconductor substrate I upper surface and back electrode form battery electrode.
2. Single Walled Carbon Nanotube PN junction isotope battery as claimed in claim 1, it is characterized in that, described N-type semiconductor substrate I comprises silicon chip, gallium arsenide film, silicon carbide plate or gallium nitride sheet; The material of described insulation course is silicon dioxide, silicon nitride or hafnia; Described work function is selected from one or more in following metal higher than the metal of P-type semiconductor Single Walled Carbon Nanotube Fermi level: Au, Pd and Pt.
3. Single Walled Carbon Nanotube PN junction isotope battery as claimed in claim 1, is characterized in that, described metal electrode to be comb electrodes to or interdigital electrode pair.
4. Single Walled Carbon Nanotube PN junction isotope battery as claimed in claim 1, it is characterized in that, described substrate II is metal substrate or nonmetallic substrate.
5. the preparation method of the arbitrary described Single Walled Carbon Nanotube PN junction isotope battery of Claims 1 to 4, comprises the following steps:
1) transducing unit is prepared according to following step a-e:
A, form insulation course at N-type semiconductor substrate I upper surface, and make patterned metal electrode pair on the insulating layer, the right electrode of this metal electrode is the metal of work function higher than Single Walled Carbon Nanotube Fermi level;
B, the back side of N-type semiconductor substrate I make back electrode;
C, Single Walled Carbon Nanotube is assembled in described metal electrode between, the two ends of Single Walled Carbon Nanotube are contacted with two metal electrodes respectively;
D, removal metallic single-wall carbon nano-tube, retain P-type semiconductor Single Walled Carbon Nanotube;
Insulation course on e, wet etching N-type semiconductor substrate I, utilizes solution surface tension effect that P-type semiconductor Single Walled Carbon Nanotube is formed with N-type semiconductor substrate I in good condition and contacts;
2) radiation source is prepared: deposit radioactive isotope film on substrate II;
3) there are by radiation source the face of radioactive isotope film and transducing unit to have relative aligning the in the face of P-type semiconductor Single Walled Carbon Nanotube to seal, and realize electric isolation at the position of the two contact.
6. preparation method as claimed in claim 5, is characterized in that, step 1) adopt sputtering, evaporation or electric plating method to prepare metal electrode pair in a, by lithographic definition electrode pattern, adopt corrosion or the method peeled off to realize metal patternization.
7. preparation method as claimed in claim 5, is characterized in that, step 1) back electrode described in b is metal electrode, sputtering can be adopted, to evaporate or prepared by electric plating method.
8. preparation method as claimed in claim 5, is characterized in that, step 1) method that Single Walled Carbon Nanotube is assembled between metal electrode pair of c comprises chemical vapor deposition, dielectrophoresis and arc discharge method; Step 1) d by applying larger voltage or electric current burns metallic carbon nanotubes between two metal electrodes, retain P-type semiconductor Single Walled Carbon Nanotube; Step 1) e wet etching insulation course makes P-type semiconductor Single Walled Carbon Nanotube contact with N-type semiconductor substrate I to form PN junction.
9. preparation method as claimed in claim 5, is characterized in that, step 2) middle employing is electroplated or the method for molecular plating or electroless plating prepares radioactive isotope film.
10. preparation method as claimed in claim 5, it is characterized in that, step 3) in electric isolation between transducing unit and radiation source contact site by following method I) or II) realization: insulating washer is set I) between or directly this insulation system is produced on radiation source or transducing unit; II) insulating adhesive is used radiation source and transducing unit to be sticked together.
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| CN103886913B (en) * | 2014-03-31 | 2016-09-14 | 西安紫光国芯半导体有限公司 | SRAM reads time self testing circuit and method of testing |
| CN104200864B (en) * | 2014-08-25 | 2017-05-03 | 厦门大学 | Isotope battery based on wide bandgap semiconductor nano-tube array film structure |
| CN106586952A (en) * | 2016-12-14 | 2017-04-26 | 南开大学 | Carbon nanotube single molecular junction preparation method with high success rate |
| WO2019113842A1 (en) * | 2017-12-13 | 2019-06-20 | 深圳贝塔能量技术有限公司 | Quantum dot betavoltaic battery |
| CN110556192B (en) * | 2018-02-08 | 2021-04-13 | 长安大学 | Pm-147 silicon carbide slow-change PN type isotope battery and manufacturing method thereof |
| CN112086217B (en) * | 2020-08-21 | 2022-12-06 | 中国科学院合肥物质科学研究院 | SiC three-dimensional PIN structure radiation volt type 3 H source isotope battery |
| 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 |
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