CN103325433A - Single-walled carbon nanotube PN junction isotope battery and preparation method thereof - Google Patents
Single-walled carbon nanotube PN junction isotope battery and preparation method thereof Download PDFInfo
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- CN103325433A CN103325433A CN2013102474351A CN201310247435A CN103325433A CN 103325433 A CN103325433 A CN 103325433A CN 2013102474351 A CN2013102474351 A CN 2013102474351A CN 201310247435 A CN201310247435 A CN 201310247435A CN 103325433 A CN103325433 A CN 103325433A
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Abstract
The invention discloses a single-walled carbon nanotube PN junction isotope battery and a preparation method of the single-walled carbon nanotube PN junction isotope battery. An energy conversion unit of the isotope battery comprises a substrate I, a back electrode, a graphical insulating layer, a metal electrode couple located on the insulating layer and semiconductor type single-walled carbon nanotubes which are arranged between the metal electrode couple in an oriented mode and make contact with the substrate I. The two ends of each single-walled carbon nanotube are in ohmic contact with the two metal electrodes respectively, and the middle portion of each single-walled carbon nanotube makes contact with the substrate I to form a PN junction. A radiation source comprises a substrate II and a radioactive isotope film. The radiation source and the energy conversion unit can be aligned face to face and connected together in a packed mode, and the contacted part of the radiation source and the contacted part of the energy conversion unit are electrically isolated. The radioactive isotope film and the single-walled carbon nanotubes are located in a cavity formed through packed connection. One metal electrode on the upper surface of the substrate I and the back electrode form battery electrodes. The single-walled carbon nanotube PN junction isotope battery has the advantages of being small in size, simple in structure, easy to realize, high in conversion efficiency, and capable of working for a long time in various complex environments.
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 belongs to the little energy field in the MEMS.
Background technology
Development along with MEMS (Microelectro Mechanical System) rapid technological improvement, with and the characteristics of application terminal " light, thin, short, little ", the application of MEMS device is increasingly extensive, and the figure of MEMS product has also appearred in the fields such as consumer electronics, medical treatment in a large number.The MEMS technology for functional integrated in micro volume provide may, but same yardstick for the Power supply unit with regard to difficult.Traditional energy meets with bottleneck when providing the energy for the MEMS device, low such as very small chemical battery (lithium battery) energy density, the life-span is short, and micro solar battery is subjected to again the restrictions such as illumination condition.
Therefore, many researchers give very large concern for little 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 (such as α particle, β particle and gamma-rays) institute kinetic energy generating when utilizing the radioactive isotope decay.Isotope battery can be divided into directly by changing the mechanism generally changes the mechanism (such as direct charging modes and radiation volta effect etc.) and indirect conversion mechanism (causing fluorescence volta effect and thermionic emission etc. such as ray).In the above-mentioned isotope battery, the radiation voltaic element of PN junction as the transducing unit had a good application prospect, PN junction radiation voltaic element energy conversion efficiency in theory maximum possible reaches 40%.
Rappaport seminar finds in nineteen fifty-three, and the β particle that the isotope decay produces can produce electron hole pair in semiconductor, and this phenomenon is called as β radiation volta effect.The β particle-irradiation produces electron-hole pair by ionisation effect to semiconductor material.When electron-hole pair diffuses to the 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 output.In recent years, domestic and international researcher or by the structure that changes PN junction such as the conversion efficiency that porous silicon, three-dimensional structure etc. improve battery, perhaps by improving the anti-radiation property of device with new material such as SiC etc., 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 silicon from zero and equate, shows as semiconductive.These characteristics make carbon nano-tube become desirable β radiation battery material.At present, mainly contain two classes based on the micro isotope battery of carbon nano-tube, a class is film-type, mainly is comprised of carbon nano-tube film and semiconductor substrate materials; Another kind of is haplotype, mainly is comprised of single or a plurality of semi-conductive single-walled carbon nanotubes and low workfunction metal.Although film-type is simple in structure, handling ease, its performance can not show a candle to haplotype.In the existing haplotype structure, the contact area of Single Walled Carbon Nanotube and low workfunction metal is very limited, only has approximately tens nanometer range of end, so that it is very little to be used for the heterojunction area of energy conversion.On the other hand, because the energy gap of Single Walled Carbon Nanotube is less, the space charge sector width that forms with Metal Contact is less also.These 2 have greatly been limited haplotype energy conversion effect volume, have also made 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 conductive single-walled carbon nanotubes and N-type semiconductor substrate contact to form PN junction as the transducing structure of 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.The 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 the insulation course, and align at metal electrode a Single Walled Carbon Nanotube that contacts with substrate I.Described metal electrode is to adopting work function to be higher than the metal of 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 the radioactive isotope film that is deposited on the 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 forms, and metal electrode and back electrode in the described substrate I upper surface consist of battery electrode.
The N-type semiconductor substrate that described substrate I is the transducing unit, it can be silicon chip, gallium arsenide film, silicon carbide plate or gallium nitride sheet etc., the material of the insulation course on surface can be silicon dioxide, silicon nitride or hafnia etc.
Described Single Walled Carbon Nanotube is the P-type semiconductor conductive single-walled carbon nanotubes, 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, consists of 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.
The metal that described work function is higher than the Single Walled Carbon Nanotube Fermi level can be selected from one or more in the following metal: Au, Pd and Pt etc.
Described substrate II is the substrate of radiation source structure, and it can be metal substrate, and such as nickel sheet and copper sheet etc. also can be non-metal substrate, such as silicon chip and glass sheet etc.
Above-mentioned PN junction isotope battery preparation method based on Single Walled Carbon Nanotube is as follows:
1) prepare the transducing unit according to following step a-e:
A, form insulation course at substrate I upper surface, and make patterned metal electrode pair at insulation course, the electrode of this electrode pair is the metal that work function is higher than the Single Walled Carbon Nanotube Fermi level;
B, make back electrode at the back side of substrate I;
C, with Single Walled Carbon Nanotube be 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 keep semi-conductive single-walled carbon nanotubes;
Insulation course on e, the wet etching substrate I utilizes the solution surface tension effect that semi-conductive single-walled carbon nanotubes is formed with substrate I in good condition and contacts.
2) preparation radiation source: deposit radioactive isotope film on substrate II;
3) radiation source there is the face of radioactive isotope film have the relative aligning of face of Single Walled Carbon Nanotube to seal with the transducing unit, and realizes electric isolation at the position of the two contact.
Above-mentioned steps 1) can adopt the methods such as sputter, evaporation, plating to prepare metal electrode pair among a, by the lithographic definition electrode pattern, method realizes metal patternization to adopt corrosion or peel off etc.
Above-mentioned steps 1) the described back electrode of b is metal electrode, can adopt the methods such as sputter, evaporation or plating to prepare.
Above-mentioned steps 1) c with Single Walled Carbon Nanotube be assembled in metal electrode to method mainly contain chemical vapor deposition, dielectrophoresis and arc discharge method etc.;
Above-mentioned steps 1) d can by applying larger voltage or electric current is burnt metallic single-wall carbon nano-tube between two metal electrodes, keep 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 and forms PN junction.
Above-mentioned steps 2) preparation of radioactive isotope film can be adopted plating or the methods such as molecular plating or electroless plating in.
Above-mentioned steps 3) method for sealing of radiation source structure and transducing unit 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) electric isolation between transducing unit and radiation source contact site can arrange insulating washer or realize by directly this insulation system being produced on radiation source structure or the transducing unit between the two, also can be by with all kinds of insulating adhesives such as silica gel or epoxy resin radiation source structure and transducing unit being sticked together to realize.
The present invention proposes a kind of Single Walled Carbon Nanotube PN junction isotope battery.It utilizes P-type semiconductor conductive single-walled carbon nanotubes and N-type semiconductor substrate contact to form PN junction as the transducing structure of 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, and its structural integrity is compared with carbon nano-tube film, can greatly reduce electron hole pair that radiation produces at the interface recombination rate, improves the conversion efficiency of isotope battery.On the other hand, except very little zone, metal electrode contact end, the most of zone of Single Walled Carbon Nanotube can both contact fully with the N-type semiconductor substrate, not only greatly increased the junction area of PN junction, and because the N-type semiconductor substrate has larger energy gap, make also significantly being increased of space charge sector width, thereby improve the electron hole pair separation rate.Process aspect is owing to only needing a kind of metal as electrode, and the preparation technology of this Single Walled Carbon Nanotube PN junction isotope battery is simple before also.Therefore to have a volume little, simple in structure for this isotope battery, the characteristics that are easy to realize, and conversion efficiency is higher, can work long hours in various complex environments.
Description of drawings
Fig. 1 is the vertical view of the PN junction transducing unit of embodiment of the invention preparation, and right symmetry contacts to have shown single-root carbon nano-tube and metal electrode, with contacting of N-type semiconductor substrate;
Fig. 2 is the sectional view of the isotope battery device of embodiment of the invention preparation;
Fig. 3 (a)-Fig. 3 (g) is the process chart of embodiment of the invention preparation based on 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 prepared isotope battery of the present embodiment comprises transducing unit and radiation source two parts, and the two seals, by separation layer 8 contact and electric isolation.This transducing structure comprises substrate I(transducing structured substrate) 1, insulation course 2 at substrate 1 upper surface, has metal electrode that two comb-like electrodes consist of pair at insulation course 2, it all is high-work-function metal electrode 3, metal electrode between oriented alignment single wall semiconductive carbon nano tube 4 is arranged, and contact with substrate 1 and to form PN junction, the back side of substrate 1 is metal back electrode 5.The radiation source structure then comprises substrate II(source structure substrate) 6 and be positioned at its surperficial radioactive isotope film 7.
Above-mentioned isotope battery prepares according to following method:
1) preparation of transducing unit
A, get monocrystalline silicon piece a slice (two throwing silicon chips, 400 μ m) as the substrate I of transducing structure, thermal oxide forms the silicon dioxide of 100nm, then removes the silicon dioxide at the back side, keeps the silicon dioxide of upper surface as insulation course 2, sees Fig. 3 (a).
B, on insulation course 2 photoetching and sputter adhesion layer Metal Cr 20nm, sputter high-work-function metal Au150nm uses lift-off technology to obtain the figure of high-work-function metal electrode 3 again, and the width of this each broach of electrode is 3 μ m, length is 30 μ m, and each comb tooth spacing is 5 μ m.
Shown in Fig. 3 (b), the high-work-function metal electrode 3 of comb teeth-shaped forms 30 electrode pairs (having shown 5 electrode pairs among Fig. 1) to metal electrode altogether to the structure after preparing, and the spacing between each electrode pair is 3 μ m.
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 the dielectrophoresis method to carry out Single Walled Carbon Nanotube assembling, concrete grammar is as follows:
Single Walled Carbon Nanotube is dissolved in dimethyl formamide makes Single Walled Carbon Nanotube suspending liquid, with the ultrasonic 2h of solution, the peak-to-peak value that applies 5MHz at two metal electrodes 3 is the alternating voltage of 5V, then with on made Single Walled Carbon Nanotube hanging drop to two electrode, Single Walled Carbon Nanotube is assembled into the Single Walled Carbon Nanotube that aligns under the effect of dielectrophoresis power, after the 30s suspending liquid on the electrode is blown away with nitrogen gun.
E, electrode applies 10V voltage and makes positive semi-conductive single-walled carbon nanotubes be in cut-off state overleaf, add malleation on the metal electrode, another metal electrode ground connection, apply 15V voltage, burn metallic Single Walled Carbon Nanotube, obtain aligning the semi-conductive single-walled carbon nanotubes 4 between electrode pair, shown in Fig. 3 (d).
Insulation course on f, the wet etching substrate I utilizes the surface tension of solution that Single Walled Carbon Nanotube is contacted with substrate I formation, consists of PN junction, such as Fig. 3 (e).
2) making of radiation source structure
Get the nickel sheet as source structure substrate 6, electroplate 3.3mCi/cm in the front
2Radioactive isotope film Ni-63, form 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 as separation layer 8 the two to be bonded together, form the isotope battery based on Single Walled Carbon Nanotube, see Fig. 3 (g).
The present embodiment provides a kind of structure and preparation method of the isotope battery based on the P-type semiconductor conductive single-walled carbon nanotubes, and the present invention not only is confined to this embodiment, can make corresponding modification with designing requirement according to actual needs.
The thickness of substrate I, doping content all can be regulated for realizing higher conversion efficiency in the present embodiment.
Silicon dioxide as insulation course 2 in the present embodiment can be other insulators, and such as silicon nitride or hafnia, thickness also can be regulated.
High-work-function metal Au can be for other metals in the present embodiment, such as Pd, and Pt etc., and right structure, size, logarithm (having shown 5 electrode pairs among Fig. 1) and the equal capable of regulating of spacing of metal electrode.
The concentration of Single Walled Carbon Nanotube suspending liquid is adjustable in the present embodiment, and magnitude of voltage and frequency during assembling are adjustable, and built-up time is also adjustable.
Radioactive isotope can be other radioelement in the present embodiment, such as tritium etc.
Radiation source can with metal as the source structure substrate, such as sheet metals such as nickel sheet or copper sheets, also can be done substrate with nonmetal semiconductor or insulator, such as glass etc. in the present embodiment.If as substrate, need to the two between insert insulation course when so transducing unit and radiation source 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 unit separation layer that contacts with the radiation source structure can be 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 the insulation system layer directly is produced on source structure or the transducing structure.
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.
Abovely describe Single Walled Carbon Nanotube PN junction isotope battery provided by the present invention in detail by 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 distortion or modification to the present invention; Its preparation method also is not limited to disclosed content among the embodiment.
Claims (10)
1. Single Walled Carbon Nanotube PN junction isotope battery, comprise transducing unit and radiation source two parts, wherein: the transducing unit comprises substrate I, be positioned at the back electrode at the substrate I back side, be positioned at the patterned insulation course of substrate I upper surface and be positioned at metal electrode pair on the insulation course, and align at metal electrode a semi-conductive single-walled carbon nanotubes that contacts with substrate I; Described metal electrode is to adopting work function to be higher than the metal of 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 the radioactive isotope film that is deposited on the 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 Single Walled Carbon Nanotube are positioned at the cavity that sealing-in forms, and metal electrode and back electrode in the described substrate I upper surface consist of battery electrode.
2. Single Walled Carbon Nanotube PN junction isotope battery as claimed in claim 1 is characterized in that, described substrate I is the N-type semiconductor substrate, 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; The metal that described work function is higher than the Single Walled Carbon Nanotube Fermi level is selected from one or more in the following metal: 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 is characterized in that, described substrate II is metal substrate or nonmetal substrate.
5. the preparation method of the arbitrary described Single Walled Carbon Nanotube PN junction isotope battery of claim 1～4 may further comprise the steps:
1) prepare the transducing unit according to following step a-e:
A, form insulation course at substrate I upper surface, and make patterned metal electrode pair at insulation course, the right electrode of this metal electrode is the metal that work function is higher than the Single Walled Carbon Nanotube Fermi level;
B, make back electrode at the back side of substrate I;
C, with Single Walled Carbon Nanotube be 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 keep semi-conductive single-walled carbon nanotubes;
Insulation course on e, the wet etching substrate I utilizes the solution surface tension effect that semi-conductive single-walled carbon nanotubes is formed with substrate I in good condition and contacts.
2) preparation radiation source: deposit radioactive isotope film on substrate II;
3) radiation source there is the face of radioactive isotope film have the relative aligning of face of semi-conductive single-walled carbon nanotubes to seal with the transducing unit, and realizes electric isolation at the position of the two contact.
6. preparation method as claimed in claim 5 is characterized in that, adopts sputter, evaporation or electric plating method to prepare metal electrode pair among the step 1) a, by the lithographic definition electrode pattern, adopts corrosion or the method peeled off realizes metal patternization.
7. preparation method as claimed in claim 5 is characterized in that, the described back electrode of step 1) b is metal electrode, can adopt sputter, evaporation or electric plating method to prepare.
8. preparation method as claimed in claim 5 is characterized in that, step 1) c with Single Walled Carbon Nanotube be assembled in metal electrode to method comprise chemical vapor deposition, dielectrophoresis and arc discharge method; Step 1) d keeps semi-conductive single-walled carbon nanotubes by applying larger voltage or electric current is burnt metallic carbon nanotubes between two metal electrodes; Step 1) e wet etching insulation course makes semi-conductive single-walled carbon nanotubes contact with substrate I and forms PN junction.
9. preparation method as claimed in claim 5 is characterized in that step 2) in adopt the method for plating or molecular plating or electroless plating to prepare the radioactive isotope film.
10. preparation method as claimed in claim 5, it is characterized in that, the electric isolation in the step 3) between transducing unit and radiation source contact site is by following method I) or II) realize: insulating washer I) is set between the two or directly this insulation system is produced on radiation source or the transducing unit; II) use insulating adhesive that radiation source and transducing unit are sticked together.
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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 |
| CN110556192A (en) * | 2018-02-08 | 2019-12-10 | 长安大学 | Pm-147 silicon carbide slow-change PN type isotope battery and manufacturing method thereof |
| CN112086217A (en) * | 2020-08-21 | 2020-12-15 | 中国科学院合肥物质科学研究院 | SiC three-dimensional PIN structure radiation volt type3H source isotope battery |
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