CN110277292A - A kind of middle cryogenic vacuum thermoelectric conversion element and preparation method thereof - Google Patents
A kind of middle cryogenic vacuum thermoelectric conversion element and preparation method thereof Download PDFInfo
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- CN110277292A CN110277292A CN201910381775.0A CN201910381775A CN110277292A CN 110277292 A CN110277292 A CN 110277292A CN 201910381775 A CN201910381775 A CN 201910381775A CN 110277292 A CN110277292 A CN 110277292A
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01J—ELECTRIC DISCHARGE TUBES OR DISCHARGE LAMPS
- H01J19/00—Details of vacuum tubes of the types covered by group H01J21/00
- H01J19/02—Electron-emitting electrodes; Cathodes
- H01J19/04—Thermionic cathodes
- H01J19/06—Thermionic cathodes characterised by the material
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01J—ELECTRIC DISCHARGE TUBES OR DISCHARGE LAMPS
- H01J19/00—Details of vacuum tubes of the types covered by group H01J21/00
- H01J19/02—Electron-emitting electrodes; Cathodes
- H01J19/04—Thermionic cathodes
- H01J19/14—Cathodes heated indirectly by an electric current; Cathodes heated by electron or ion bombardment
- H01J19/18—Insulating layer or body located between heater and emissive material
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01J—ELECTRIC DISCHARGE TUBES OR DISCHARGE LAMPS
- H01J9/00—Apparatus or processes specially adapted for the manufacture, installation, removal, maintenance of electric discharge tubes, discharge lamps, or parts thereof; Recovery of material from discharge tubes or lamps
- H01J9/02—Manufacture of electrodes or electrode systems
- H01J9/04—Manufacture of electrodes or electrode systems of thermionic cathodes
- H01J9/042—Manufacture, activation of the emissive part
Abstract
The invention discloses a kind of middle cryogenic vacuum thermoelectric conversion element and preparation method thereof, the middle cryogenic vacuum thermoelectric conversion element includes cathode construction and anode construction；The cathode construction includes the cathode base being cascading, bottom gate thin film, dielectric film and cathode electrode, the dielectric film with a thickness of 0.5~10nm, apply grid voltage between the bottom gate thin film and cathode electrode；The anode construction includes the anode electrode being stacked and anode grid substrate.The cathode construction of middle cryogenic vacuum thermoelectric conversion element provided by the invention is based on metal-insulator-metal type (MIM) structure, additional light source is not needed, bigger heat emission electric current can be obtained under middle low temperature, realize the vacuum thermoelectric conversion of high-output power, and structure is simple, is easy preparation.In addition, the tunelling electrons in the MIM cathode based on two-dimensional atomic crystal are direct tunnellings, electronics has higher electronic transmitting efficiency because the energy of scattering loss is less.
Description
Technical field
The present invention relates to thermoelectric conversion element technical fields, more particularly, to a kind of middle cryogenic vacuum thermoelectric converter
Part and preparation method thereof.
Background technique
Energy crisis is the important issue that 21st century human social development faces.Waste Heat Reuse is to solve to be somebody's turn to do
A kind of important channel of problem.Thermoelectric conversion element can be produced electricl energy using waste heat, be conducive to alleviating energy crisis.With it is solid
State thermo-electric device is compared, and vacuum thermoelectric device has a clear superiority on conversion efficiency of thermoelectric since there is no heat transfer.
However, since traditional vacuum thermoelectric device is the thermionic emission based on cathode come work, and thermoelectron is sent out
It is higher to penetrate the commonly required temperature wanted, therefore, which is only capable of forming effective output power under high temperature environment.Expand
The application range of vacuum thermoelectric device needs to reduce its operating temperature.In general, pass through the surface work function of reduction cathode
It can reduce heat emission temperature.But the low-work-function cathode material being currently known is not able to satisfy condition still that (lanthanum hexaboride is
The stable low-work-function material being currently known, heat emission temperature are still greater than 1000K).Another method is increased using light
Heat-flash electron emission increases cathode heat emission electric current at low temperature.However, this method needs additional light source, it is not suitable for
There is no the application of light source.
It is lower and do not need the vacuum thermoelectric switching device of additional light source therefore, it is necessary to develop operating temperature.
Summary of the invention
The present invention is to overcome operating temperature described in the above-mentioned prior art higher or need additional light source to increase cathode
The defect of emission current at low temperature provides a kind of middle cryogenic vacuum thermoelectric conversion element, and the middle cryogenic vacuum thermoelectricity provided turns
The cathode construction of parallel operation part is based on MIM structure, does not need additional light source, can obtain under middle low temperature
Bigger heat emission electric current realizes the vacuum thermoelectric conversion of high-output power, and structure is simple, is easy preparation.
Another object of the present invention is to provide the preparation methods of cryogenic vacuum thermoelectric conversion element among the above.
In order to solve the above technical problems, the technical solution adopted by the present invention is that:
A kind of middle cryogenic vacuum thermoelectric conversion element, including cathode construction and anode construction；
The cathode construction includes the cathode base being cascading, bottom gate thin film, dielectric film and cathode electrode,
The dielectric film with a thickness of 0.5~10nm, apply grid voltage between the bottom gate thin film and cathode electrode；
The anode construction includes the anode electrode being stacked and anode grid substrate；
The anode construction is located at the cathode electrode side of the cathode construction；The cathode construction is located at the anode
The anode electrode side of structure.
The bottom gate thin film, dielectric film and cathode electrode form MIM structure, referred to as MIM knot
Structure.
Working principle: when middle cryogenic vacuum thermoelectric conversion element of the invention works, being placed in hot end for cathode construction, will
Anode construction is placed in cold end, and applies certain negative voltage as grid between the bottom gate thin film and cathode electrode of cathode construction
Pole tension.Mim structure is used in thermoelectric conversion element by the present invention for the first time.Middle cryogenic vacuum thermoelectric converter of the invention
Part generates the field pyrogenicity electronics of high-energy using the mim structure on cathode base, to obtain the heat of enhancing under middle low temperature
Emission current improves thermoelectricity output power.More thermal electrons can absorb more energy from heat source, so that the device
Part structure can realize the vacuum thermoelectric conversion of high-output power under middle low temperature.
To sum up, the cathode construction of cryogenic vacuum thermoelectric conversion element is based on MIM structure among the above, no
Additional light source is needed, bigger heat emission electric current can be obtained under middle low temperature, realizes that the vacuum thermoelectric of high-output power turns
It changes, and structure is simple, is easy preparation.
Preferably, the dielectric film is by one of boron nitride, silicon nitride, silica, aluminium oxide or hafnium oxide
Or two or more compositions.
It is highly preferred that the dielectric film is made of hexagonal boron nitride.
Preferably, the dielectric film with a thickness of 5nm.
Preferably, the cathode base is insulating substrate.
Preferably, the cathode base is coated in silicon wafer, metal molybdenum or the tungsten of insulating layer by glass, ceramics, surface
One or more kinds of constitute.
Preferably, the bottom gate thin film is made of graphene and/or the first metal material；First metal material is
The combination of one or more of chromium, copper, tungsten or molybdenum.
Preferably, the bottom gate thin film is with a thickness of 100nm or less.
Preferably, the cathode electrode is made of graphene and/or the second metal material；Second metal material is
The combination of one or more of gold, copper, tungsten or chromium.
It is highly preferred that the cathode electrode is made of graphene.
Preferably, the cathode electrode with a thickness of 10nm or less.
It is highly preferred that the cathode electrode with a thickness of monoatomic layer thickness.
The above-mentioned cathode using mim structure is properly termed as MIM cathode.
Realize the sustainable use of cryogenic vacuum thermoelectric conversion element among the above, thermoelectricity output power needs are greater than
The driving power of MIM cathode.Therefore, the tunelling electrons needs in MIM cathode directly tunnel through dielectric film and cathode electrode.
In view of electronics can in two-dimensional atomic crystal ballistic transport, to realize the MIM cathode of above-mentioned direct tunnelling, dielectric film can
It is preferably constituted using two-dimensional atomic crystals such as hexagonal boron nitrides, cathode electrode preferably uses the two dimension such as graphene former
Sub- crystal is constituted.
Tunelling electrons in MIM cathode based on two-dimensional atomic crystal are direct tunnelling, energy of the electronics because of scattering loss
Measure it is less, therefore have higher electronic transmitting efficiency.
It is therefore preferred that the dielectric film is made of hexagonal boron nitride, the cathode electrode is made of graphene.
Preferably, the anode grid substrate is made of one or more of glass, ceramics, silicon wafer or metal plate.
Preferably, the metal plate is the combination of one or more of copper, stainless steel or tungsten.
The anode electrode can be low-work-function material.Preferably, the anode electrode is graphene and/or six boron
Change lanthanum.
The present invention protects the preparation method of cryogenic vacuum thermoelectric conversion element among the above simultaneously, and the preparation method includes
Following steps:
S1. prepare cathode base and anode grid substrate；
S2. bottom gate thin film is prepared on the cathode base；
S3. dielectric film is prepared in the bottom gate thin film；
S4. cathode electrode is prepared on the dielectric film；
S5. anode electrode is prepared in the anode grid substrate.
Specific preparation method is the prior art, can carry out conventional selection according to the prior art by those skilled in the art
It obtains.
Preferably, step S1. includes the steps that cleaning cathode base and anode grid substrate.
Compared with prior art, the beneficial effects of the present invention are:
The cathode construction of middle cryogenic vacuum thermoelectric conversion element provided by the invention is based on metal-insulator-metal type knot
Structure does not need additional light source, and bigger heat emission electric current can be obtained under middle low temperature, realizes the vacuum of high-output power
Heat to electricity conversion, and structure is simple, is easy preparation.
In addition, being obtained former based on two dimension when dielectric film is made of hexagonal boron nitride, cathode electrode is made of graphene
The MIM cathode of sub- crystal, the tunelling electrons in the MIM cathode based on two-dimensional atomic crystal are direct tunnellings, and electronics is because of scattering
The energy of loss is less, has higher electronic transmitting efficiency.
Detailed description of the invention
Fig. 1 is the structural schematic diagram of middle cryogenic vacuum thermoelectric conversion element of the invention.Wherein, Fig. 1 (a) is cathode knot
The main view of structure and anode construction, Fig. 1 (b) are the left view of cathode construction and anode construction.It " is rotated by 90 ° " and refers in figure,
After device is rotated by 90 ° in the horizontal direction, view is changed into Fig. 1 (b) by Fig. 1 (a).
Fig. 2 is traditional vacuum thermoelectric conversion element schematic diagram.Fig. 2 foundation existing technical literature (Khalid K AA,
Leong T J,Mohamed K.Review on Thermionic Energy Converters[J].IEEE
Transactions on Electron Devices, 2016,63 (6): 2231-2241.) it obtains.
Fig. 3 is the schematic diagram of the preparation method of the middle cryogenic vacuum thermoelectric conversion element of the embodiment of the present invention 2.Wherein, scheme
3 (b) and Fig. 3 (c) indicates that the different views of same structure, Fig. 3 (b) are main view, and Fig. 3 (c) is left view." rotation 90 in figure
Degree " refers to that after device is rotated by 90 ° in the horizontal direction, view is changed into Fig. 3 (c) by Fig. 3 (b).
Fig. 4 be middle cryogenic vacuum thermo-electric device of the invention from traditional vacuum thermo-electric device under different cathode temperatures
The simulation calculated result of maximum conversion efficiency of thermoelectric and peak power output density.Wherein, solid line and dotted line respectively represent this hair
Bright and traditional devices results.
Fig. 5 is the maximum heat to electricity conversion of middle cryogenic vacuum thermo-electric device of the invention under different MIM cathode band structures
The simulation calculated result of efficiency and output power density.Wherein, Fig. 5 (a) is maximum conversion efficiency of thermoelectric；Fig. 5 (b) is maximum
Output power density.
In Fig. 1~3,1 is cathode base, and 2 be bottom gate thin film, and 3 be dielectric film, and 4 be cathode electrode, and 5 be anode base
Plate, 6 be anode electrode.
Specific embodiment
The present invention is further illustrated With reference to embodiment.
The same or similar label correspond to the same or similar components in the attached drawing of the embodiment of the present invention；Of the invention
In description, it is to be understood that if there is the instructions such as term " on ", "lower", "left", "right", "top", "bottom", "inner", "outside"
Orientation or positional relationship is to be based on the orientation or positional relationship shown in the drawings, and is merely for convenience of the description present invention and simplification is retouched
It states, rather than the device or element of indication or suggestion meaning must have a particular orientation, constructed and grasped with specific orientation
Make, therefore the terms describing the positional relationship in the drawings are only for illustration, should not be understood as the limitation to this patent.
In addition, if there is the terms such as " first ", " second " to be used for description purposes only, be mainly used for distinguishing different devices,
Element or component (specific type and construction may identical may also be different), be not intended to show or imply indicated by
The relative importance and quantity of device, element or component, and should not be understood as indicating or implying relative importance.
Raw material in embodiment can be by being commercially available；
Unless stated otherwise, the present invention uses reagent, method and apparatus for the art conventional reagent, method and
Equipment.
Embodiment 1
A kind of middle cryogenic vacuum thermoelectric conversion element, as shown in Figure 1, including cathode construction and anode construction.Cathode construction
Including cathode base 1, bottom gate thin film 2, dielectric film 3 and the cathode electrode 4 being cascading.Bottom gate thin film 2 and cathode electricity
Apply grid voltage between pole 4.Anode construction includes the anode electrode 6 being stacked and anode grid substrate 5.Anode construction is located at
4 side of cathode electrode of cathode construction；Cathode construction is located at 6 side of anode electrode of anode construction.
Fig. 2 gives the structural schematic diagram of traditional vacuum thermoelectric conversion element.Its basic structure includes cathode base 1, yin
Pole electrode 4, anode grid substrate 5 and anode electrode 6.
When two kinds of proper device operations of Fig. 1 and Fig. 2, cathode base and anode grid substrate need to be respectively placed in hot end and cold end,
Output power between cathode and anode.Different from traditional vacuum thermo-electric device, middle cryogenic vacuum thermoelectric conversion element of the invention
Need to apply between bottom gate thin film and cathode electrode certain negative voltage to generate high energy field pyrogenicity electronics.
(1) maximum of the traditional vacuum thermoelectric conversion element of middle cryogenic vacuum thermoelectric conversion element and Fig. 2 based on Fig. 1
The simulation comparison of computational results of conversion efficiency of thermoelectric and peak power output density.
Simulation is calculated and is carried out in MATLAB.In calculation procedure, traditional vacuum conversion efficiency of thermoelectric η0And output power
Density P0It is obtained by following formula,
P0=(Jc-Ja)(Φc-Φa)/e
Wherein, JcAnd JaFor the heat emission current density of cathode and anode, TcAnd TaFor cathode and temperature of anode, ΦcAnd Φa
For the surface work function of cathode and anode, e is electron charge, and k is Boltzmann constant.
Since the vacuum thermoelectric device of the invention based on MIM cathode needs additional input electric energy to drive MIM cathode,
Therefore its conversion efficiency of thermoelectric ηFTECWith output power density PFTECIt is obtained by following formula,
PFTEC=(JFTE-Ja)(Φc-Φa)/e-JTFNV0
Wherein, JFTEFor the heat emission current density of MIM cathode, V0For the driving voltage of MIM cathode, JTFNTo drive MIM
The tunneling current density of cathode, JTFNV0For the driving power density of MIM cathode.
In view of JTFNWith the dielectric film thickness t in MIM cathode, the contact berrier Φ of grid and dielectric film0And
Driving voltage V0Related, calculation formula is represented by,
Wherein, F=V0/εrT is the electric field strength in dielectric film, εrFor the relative dielectric constant of dielectric film, m is electricity
Sub- effective mass, h are Planck's constant.
On the other hand, current density, J could only be generated when the electron energy in cathode is greater than its surface potential barrierFTE,
Therefore,
Wherein, it is Energy distribution of the electronics in cathode that vacuum level, which is set as zero, N (E),.Consider the electronics energy in MIM cathode
It is direct tunneling to vacuum, N (E)=jTFN(E-eV0-Φ0+Φc), and jTFNFor JTFNElectron energy distribution.
The dielectric film in Fig. 1 device is set as the hexagonal boron nitride of 5nm thickness, contact of the bottom gate thin film with silica
Potential barrier Φ0For 1.5eV, the temperature of cold end locating for anode is 300K, and numerical value calculates grid voltage, cathode and anode work function number
Respectively in the range of 0 to -10V, 2.5 to 5.5eV and 0 to 5.5eV, the conversion efficiency of thermoelectric and output power of the device are close
The maximum extreme value of degree with cathode temperature (600 arrive 1200K) situation of change.It is to be noted that conversion efficiency of thermoelectric and output
The maximum extreme point of power density can obtain simultaneously under the same conditions.Solid line and dotted line in Fig. 4 respectively represent the present invention
The analog result of device and the traditional devices maximum conversion efficiency of thermoelectric under different cathode work function numbers and output power density.
It can be seen that compared with traditional vacuum thermoelectric conversion element, though middle cryogenic vacuum thermo-electric device of the invention is in transfer efficiency
The decline of more than half is so had more than, but the device can generate the output power density of higher than ten orders of magnitude or more.It should
Humidification is more significant at low temperature.Therefore, the vacuum thermoelectric proposed by the present invention based on direct tunnelling type MIM cathode turns
Parallel operation part can realize effective vacuum thermoelectric conversion under middle low temperature.
(2) the maximum conversion efficiency of thermoelectric of the middle cryogenic vacuum thermoelectric conversion element based on Fig. 1 and output power density with
The simulation calculated result of the band structure relationship of MIM cathode.
Using calculation procedure identical with Fig. 4, cathode temperature is fixed as 700K, temperature of anode is fixed as 300 K, numerical value
Different-thickness hexagonal boron nitride film and difference MIM cathode contacts potential barrier are calculated to device maximum conversion efficiency of thermoelectric and defeated
The relationship of power density out.Fig. 5 a and Fig. 5 b respectively correspond the result of transfer efficiency and output power density.It can be seen that with
Hexagonal boron nitride thickness and its increase with bottom gate contact berrier, maximum conversion efficiency of thermoelectric increases, and output power density is then
Decline.By taking the Waste Heat Reuse in a four cylinder automobiles as an example, the output power of 1kW or more is obtained, the defeated of thermo-electric device is needed
Power density is greater than 12500W/m out2.By carrying out suitable energy band design to MIM cathode, when hexagonal boron nitride with a thickness of
9nm, contact berrier 1.25eV, cathode work function number 2.5eV, anode work function number is 0.5eV, when grid voltage is -1.5V,
The device can be 14000W/m in output power density2In the case where, obtain 17% conversion efficiency of thermoelectric (cathode temperature
Degree: 700K；Temperature of anode: 300K).
Embodiment 2
A kind of preparation method of middle cryogenic vacuum thermoelectric conversion element, as shown in figure 3, preparing surface growth first has
The silicon wafer of silica is as cathode base 1 (Fig. 3 a)；Then molybdenum film is deposited on it as bottom gate thin film 2 (Fig. 3 b and figure
3c)；Then the hexagonal boron nitride dielectric film 3 (Fig. 3 d) of 5nm thickness is prepared in bottom gate thin film；Finally made on dielectric film
Standby graphene cathode electrode 4 (Fig. 3 e).It needs to guarantee that in vertical direction, Graphene electrodes exist and bottom gate in cathode preparation
The unfolded region of electrode is to be used for lead.
The production of MIM cathode based on other novel low-dimension nano materials in the present invention can be according to the basic step of embodiment 2
It is rapid to carry out.
It is important to note that the middle cryogenic vacuum thermoelectric conversion element structure in Fig. 1 is not limited only in figure
Shown in single structure, can also connect between multiple structures using to improve output voltage.
Obviously, the above embodiment of the present invention be only to clearly illustrate example of the present invention, and not be pair
The restriction of embodiments of the present invention.For those of ordinary skill in the art, may be used also on the basis of the above description
To make other variations or changes in different ways.There is no necessity and possibility to exhaust all the enbodiments.It is all this
Made any modifications, equivalent replacements, and improvements etc., should be included in the claims in the present invention within the spirit and principle of invention
Protection scope within.
Claims (10)
1. a kind of middle cryogenic vacuum thermoelectric conversion element, which is characterized in that including cathode construction and anode construction；
The cathode construction includes the cathode base (1) being cascading, bottom gate thin film (2), dielectric film (3) and cathode electricity
Pole (4), the dielectric film (3) with a thickness of 0.5~10nm, apply grid between the bottom gate thin film (2) and cathode electrode (4)
Pole tension；
The anode construction includes the anode electrode (6) being stacked and anode grid substrate (5)；
The anode construction is located at cathode electrode (4) side of the cathode construction；The cathode construction is located at the anode knot
Anode electrode (6) side of structure.
2. middle cryogenic vacuum thermoelectric conversion element according to claim 1, which is characterized in that the dielectric film (3) by
One or more of boron nitride, silicon nitride, silica, aluminium oxide or hafnium oxide are constituted.
3. middle cryogenic vacuum thermoelectric conversion element according to claim 2, which is characterized in that the dielectric film (3) by
Hexagonal boron nitride is constituted.
4. described in any item middle cryogenic vacuum thermoelectric conversion elements according to claim 1~3, which is characterized in that the dielectric
Film (3) with a thickness of 5nm.
5. middle cryogenic vacuum thermoelectric conversion element according to claim 1, which is characterized in that the cathode base (1) by
Glass, ceramics or surface are coated with one or more of the silicon wafer of insulating layer, metal molybdenum, tungsten and constitute.
6. middle cryogenic vacuum thermoelectric conversion element according to claim 1, which is characterized in that the bottom gate thin film (2) by
Graphene and/or the first metal material are constituted；First metal material is one or more of chromium, copper, tungsten or molybdenum
Combination.
7. middle cryogenic vacuum thermoelectric conversion element according to claim 1, which is characterized in that the cathode electrode (4) by
Graphene and/or the second metal material are constituted；Second metal material is one or more of gold, copper, tungsten or chromium
Combination.
8. middle cryogenic vacuum thermoelectric conversion element according to claim 1, which is characterized in that the anode grid substrate (5) by
One or more of glass, ceramics, silicon wafer or metal plate are constituted.
9. middle cryogenic vacuum thermoelectric conversion element according to claim 1, which is characterized in that the anode electrode (6) is
Graphene and/or lanthanum hexaboride.
10. the preparation method of any one of the claim 1~9 middle cryogenic vacuum thermoelectric conversion element, which is characterized in that including
Following steps:
S1. prepare cathode base and anode grid substrate；
S2. bottom gate thin film is prepared on the cathode base；
S3. dielectric film is prepared in the bottom gate thin film；
S4. cathode electrode is prepared on the dielectric film；
S5. anode electrode is prepared in the anode grid substrate.
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| GB961004A (en) * | 1962-03-22 | 1964-06-17 | Siemens Ag | A thermionic converter |
| US4281280A (en) * | 1978-12-18 | 1981-07-28 | Richards John A | Thermal electric converter |
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