CN104934526B - A kind of heterogeneous flexible thermoelectric conversion element of flexible folding - Google Patents
A kind of heterogeneous flexible thermoelectric conversion element of flexible folding Download PDFInfo
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Abstract
The present invention relates to a kind of heterogeneous flexible thermoelectric conversion element of flexible folding, the heterogeneous flexible thermoelectric conversion element includes flexible substrate, grows dielectric layer and heterojunction structure on flexible substrates successively, the heterojunction structure includes overlapping the graphene layer and two-dimensional semiconductor crystal layer set from bottom to top, the metal electrode of graphene layer one end growth regulation one, the metal electrode of two-dimensional semiconductor crystal layer one end growth regulation two, and it is mutually isolated between the first metal electrode and the second metal electrode；During work, under the radiation of external heat source, the overlapping region of graphene layer and two-dimensional semiconductor crystal layer produces thermograde, causes Seebeck effect, produces open-circuit voltage, and carry out heat to electricity conversion.Compared with prior art, overall structure of the present invention is simple, compact, flexible to fold, Seebeck coefficient and thermoelectricity value with superelevation, wearable device and other flexible electronic application fields is can apply to, with wide application prospect.
Description
Technical field
The invention belongs to flexible electronic technical field, it is related to a kind of heterogeneous flexible thermoelectric conversion element of flexible folding,
More particularly to a kind of heterogeneous flexible thermoelectric converter of the two-dimensional semiconductor crystalline material-graphene grown on flexible substrates
Part.
Background technology
Due to the growing miniaturization trend of portable type electronic product, the research and development of compact power supply has been promoted.
Thermoelectric generator is as a kind of self-centered energy, and heat energy is converted directly into electric energy by it by Seebeck effect, as one
Plant the new and high technology of energy field.On the other hand, due to the growing miniaturization trend of portable type electronic product, miniaturization electricity
The research and development in source turns into focus.
Because graphene is different from the Seebeck coefficient of two-dimensional semiconductor crystalline material, both can be combined altogether
With heterojunction structure is constituted, thermoelectric conversion element is formed.When contacting infrared source, graphene and two-dimensional semiconductor crystal in device
Material is different because of its Seebeck coefficient, and both overlapping regions produce thermograde, causes Seebeck effect, and produce open circuit electricity
Pressure, while open-circuit voltage is linearly proportional to temperature difference：Δ V=α (αTwo-dimensional semiconductor-αGraphene) Δ T, wherein, αsFor Seebeck coefficient,
Also referred to as thermoelectric (al) power.As described above, in the presence of external heat source, Seebeck between graphene and two-dimensional semiconductor crystalline material
Heat energy conversion then has wide application prospect caused by the difference of coefficient.
Simultaneously as graphene has unique two-dimension plane structure with two-dimensional semiconductor crystalline material, can be with the modern times
Micro-nano technology technology is connected, and the High Density Integration of thermo-electric device can be realized well.On the other hand, two kinds of materials all have can
On stretching, extension, flexible feature, the heterostructure growth that both are formed to any flexible material substrate, it can be achieved curved therewith
Characteristic that is bent, folding.Application to two kinds of material flexibility features, can obtain the thermoelectric conversion element of random bending fold, can be full
The application demand of some special circumstances of foot, can more meet technical need of the portable type electronic product to compact power supply.
However, graphene is used in combination with two-dimensional semiconductor crystalline material at present, it is provided commonly for preparing flexible thermoelectricity turn
The technology of parallel operation part is rarely reported.
The content of the invention
It is an object of the present invention to overcome the above-mentioned drawbacks of the prior art and provide one kind is partly led based on two dimension
The flexible thermoelectric conversion element of body material-graphene heterojunction structure, to improve conversion efficiency of thermoelectric, and improves device integration
And portability.
The purpose of the present invention can be achieved through the following technical solutions：
A kind of heterogeneous flexible thermoelectric conversion element of flexible folding, the heterogeneous flexible thermoelectric conversion element includes flexible liner
Bottom, dielectric layer and heterojunction structure on flexible substrates are grown successively, described heterojunction structure, which includes overlapping from bottom to top, to be set
Graphene layer and two-dimensional semiconductor crystal layer, the described metal electrode of graphene layer one end growth regulation one, described two dimension half
The metal electrode of conductor crystal layer one end growth regulation two, and between the first described metal electrode and the second metal electrode mutually every
From；
During work, under the radiation of external heat source, described graphene layer and the overlapping region of two-dimensional semiconductor crystal layer
Thermograde is produced, causes Seebeck effect, open-circuit voltage is produced, and carry out heat to electricity conversion.
The material of described flexible substrate is one kind in ultra-thin glass, high molecular polymer or tinsel.
The thickness of described ultra-thin glass is within 10um.
Described high molecular polymer is polyimides, PEN or polyethylene terephthalate
In one kind.
Described dielectric layer is silica dioxide medium layer, and the thickness of silica dioxide medium layer is 10-100nm.
The overlapping setting vertical with two-dimensional semiconductor crystal layer of described graphene layer.
The thickness of described graphene layer is 10-20nm, and the thickness of described two-dimensional semiconductor crystal layer is 1-
50nm
The material of described two-dimensional semiconductor crystal layer is the chalcogen compound of transition metal two, and the transition metal two is chalcogenide
Compound includes MoS2、MoSe2、WS2、WSe2、TiS2Or VSe2In one kind.
The thickness of the first described metal electrode is 10-200nm, and the material of the first described metal electrode includes
One kind in gold, silver, aluminium or titanium.
The thickness of the second described metal electrode is 10-200nm, and the material of the second described metal electrode includes
One kind in gold, silver, aluminium or titanium.
Thermoelectric conversion element of the present invention grows titanium dioxide successively on flexible substrates using flexible material formation flexible substrate
Silicon dielectric layer, graphene layer and two-dimensional semiconductor crystal layer, wherein, graphene layer is overlapped with two-dimensional semiconductor crystal layer and set
Put, collectively form heterojunction structure, meanwhile, the metal electrode of growth regulation one in graphene layer one end, in two-dimensional semiconductor crystal layer one
The metal electrode of growth regulation two is held, and without any overlapping between the first metal electrode and the second metal electrode.Due to graphene with
The Seebeck coefficient of two-dimensional semiconductor crystal is different, when contacting infrared source, graphene layer and two dimension in thermoelectric conversion element
The overlapping region of crystal semiconductor layer produces thermograde, causes Seebeck effect, produces open-circuit voltage, and carry out thermoelectricity turn
Change.
In actual fabrication process, layer of silicon dioxide dielectric layer is first deposited in flexible substrate, with increase graphene with it is soft
Adhesiveness between property substrate；Then, by vapour deposition process (CVD) direct growth or standard mechanical stripping technology can be passed through
Graphene is obtained, is transferred on silica dioxide medium layer, graphene can be individual layer or number layer graphene；On graphene layer
When preparing two-dimensional semiconductor crystal layer, two dimension half can be prepared using mechanical stripping method, chemical liquid phase synthesis or vapour deposition process
Conductor crystal layer, is then transferred on graphene layer by transfer techniques, or directly using vapour deposition on graphene layer
Method grows one layer of two-dimensional semiconductor crystal layer；Finally, by magnetically controlled sputter method, electron-beam vapor deposition method or thermal evaporation method, point
Layer of metal barrier film is not deposited in one end of one end of graphene layer, two-dimensional semiconductor crystal layer, then by stripping technology, system
Into the first metal electrode and the second metal electrode.
Compared with prior art, the invention has the characteristics that：
1) in the presence of external heat source, Seebeck coefficient is different between graphene and two-dimensional semiconductor crystal, produces thermal voltage,
Device architecture has the Seebeck coefficient and thermoelectricity value of superelevation, and caused heat energy conversion has wide application prospect；
2) graphene and two-dimensional semiconductor crystal used is respectively provided with the two-dimension plane structure of uniqueness, can be with modern high-tech
The micro-nano technology technology of skill is mutually connected, and the High Density Integration of thermo-electric device can be realized well；
3) overall structure is simple, compact, uses flexible substrate, and graphene and two-dimensional semiconductor crystal all have and can stretched
Exhibition, flexible feature, the thermoelectric conversion element being made have can arbitrarily bending fold the characteristics of, after bending, the electricity of device
Learn property retention constant, meet the application demand of some special circumstances, can more meet portable type electronic product to compact power supply
Technical need, with good application prospect.
Brief description of the drawings
Fig. 1 is dimensional structure diagram of the present invention；
Description of symbols in figure：
1-flexible substrate, 2-dielectric layer, 3-graphene layer, 4-two-dimensional semiconductor crystal layer, the 5-the first metal electricity
Pole, the 6-the second metal electrode.
Embodiment
The embodiment illustrated below in conjunction with particular instance, embodiment and various features and relevant details herein will be referred to
The non-limiting example that is described in detail in accompanying drawing in diagram and following description and be explained more fully.Omit well-known
The description of part and treatment technology, in order to avoid the unnecessary embodiment indigestion made herein., can be with when making the structure
Use well-known traditional handicraft in semiconductor technology.Example used herein understands implementation herein just for the sake of help
The mode that example can be carried out, and further such that those skilled in the art can implement embodiment herein.Thus, should not
Example herein is interpreted as limiting to the scope of embodiment herein.
It should be noted that the diagram provided in the present embodiment only illustrates the basic conception of the present invention in a schematic way,
Then schema only shows with relevant component in the present invention rather than drawn according to component count, shape and the size during actual implement,
Kenel, quantity and the ratio of each component can be a kind of random change during its actual implementation, and its assembly layout kenel may also
It is increasingly complex.
Embodiment 1：
As shown in figure 1, a kind of heterogeneous flexible thermoelectric conversion element of flexible folding, the heterogeneous flexible thermoelectric conversion element
Including flexible substrate 1, the dielectric layer being grown in successively in flexible substrate 12 and heterojunction structure, heterojunction structure includes handing over from bottom to top
The folded graphene layer 3 and two-dimensional semiconductor crystal layer 4 set, the metal electrode 5 of 3 one end growth regulation of graphene layer one, two dimension is partly led
The metal electrode 6 of 4 one end growth regulation of body crystal layer two, and it is mutually isolated between the first metal electrode 5 and the second metal electrode 6；
During work, under the radiation of external heat source, the overlapping region of graphene layer 3 and two-dimensional semiconductor crystal layer 4 produces thermograde,
Cause Seebeck effect, produce open-circuit voltage, and carry out heat to electricity conversion.
Wherein, the material of flexible substrate 1 is polyethylene terephthalate, and dielectric layer 2 is silica dioxide medium layer, should
The thickness of silica dioxide medium layer is 100nm.
In heterojunction structure, the overlapping setting vertical with two-dimensional semiconductor crystal layer 4 of graphene layer 3, the thickness of graphene layer 3
It is 10nm for 20nm, and two-dimensional semiconductor crystal layer 4 thickness, the material of two-dimensional semiconductor crystal layer 4 is MoS2。
In actual fabrication process, layer of silicon dioxide dielectric layer is first deposited in flexible substrate 1, with increase graphene with it is soft
Adhesiveness between property substrate 1；Graphene layer 3 by vapour deposition process (CVD) direct growth silica dioxide medium layer, its
In, the graphene in graphene layer 3 is single-layer graphene；Then, directly using vapour deposition process growth one on graphene layer 3
Layer two-dimensional semiconductor crystal layer 4；Finally, by magnetically controlled sputter method respectively in one end of graphene layer 3, two-dimensional semiconductor crystal
One end deposit layer of metal barrier film of layer 4, then by stripping technology, is made the first metal electrode 5 and the second metal electrode 6.
In the present embodiment, the thickness of the first metal electrode 5 and the second metal electrode 6 is 200nm, and material is titanium.
Embodiment 2：
In the present embodiment, the material of flexible substrate 1 is PEN, and dielectric layer 2 is silica dioxide medium
Layer, the thickness of silica dioxide medium layer is 80nm；The thickness of graphene layer 3 is 15nm, and two-dimensional semiconductor crystal layer 4
Thickness is 50nm, and the material of two-dimensional semiconductor crystal layer 4 is MoSe2。
During preparation, graphene layer 3 is obtained by standard mechanical stripping technology, transferred on silica dioxide medium layer, stone
Graphene in black alkene layer 3 is multi-layer graphene, then, two-dimensional semiconductor crystal layer 4 is prepared using mechanical stripping method, by turning
Move on technique transfers to graphene layer 3, finally, by electron-beam vapor deposition method respectively in one end of graphene layer 3, two-dimensional semiconductor
One end deposit layer of metal barrier film of crystal layer 4, then by stripping technology, is made the first metal electrode 5 and the second metal electricity
Pole 6.
In the present embodiment, the thickness of the first metal electrode 5 and the second metal electrode 6 is 100nm, and material is aluminium.Its
Remaining be the same as Example 1.
Embodiment 3：
In the present embodiment, the material of flexible substrate 1 is polyimides, and dielectric layer 2 is silica dioxide medium layer, the titanium dioxide
The thickness of silicon dielectric layer is 60nm；The thickness of graphene layer 3 is 16nm, and the thickness of two-dimensional semiconductor crystal layer 4 is 32nm,
The material of two-dimensional semiconductor crystal layer 4 is WS2。
During preparation, graphene layer 3 is obtained by standard mechanical stripping technology, transferred on silica dioxide medium layer, stone
Graphene in black alkene layer 3 is multi-layer graphene, then, two-dimensional semiconductor crystal layer 4 is prepared using chemical liquid phase synthetic method, led to
Cross transfer techniques to be transferred on graphene layer 3, finally, partly led in one end of graphene layer 3, two dimension respectively by thermal evaporation method
One end deposit layer of metal barrier film of body crystal layer 4, then by stripping technology, is made the first metal electrode 5 and the second metal
Electrode 6.
In the present embodiment, the thickness of the first metal electrode 5 and the second metal electrode 6 is 80nm, and material is silver.Remaining
Be the same as Example 1.
Embodiment 4：
In the present embodiment, the material of flexible substrate 1 is tinsel, and dielectric layer 2 is silica dioxide medium layer, the titanium dioxide
The thickness of silicon dielectric layer is 30nm；The thickness of graphene layer 3 is 12nm, and the thickness of two-dimensional semiconductor crystal layer 4 is 6nm,
The material of two-dimensional semiconductor crystal layer 4 is WSe2。
During preparation, graphene layer 3 is obtained by standard mechanical stripping technology, transferred on silica dioxide medium layer, stone
Graphene in black alkene layer 3 is multi-layer graphene, then, two-dimensional semiconductor crystal layer 4 is prepared using vapour deposition process, by turning
Move on technique transfers to graphene layer 3, finally, by magnetically controlled sputter method respectively in one end of graphene layer 3, two-dimensional semiconductor
One end deposit layer of metal barrier film of crystal layer 4, then by stripping technology, is made the first metal electrode 5 and the second metal electricity
Pole 6.
In the present embodiment, the thickness of the first metal electrode 5 and the second metal electrode 6 is 50nm, and material is aluminium.Remaining
Be the same as Example 1.
Embodiment 5：
In the present embodiment, the material of flexible substrate 1 is ultra-thin glass, and the thickness of the ultra-thin glass is 10 μm, and dielectric layer 2 is
Silica dioxide medium layer, the thickness of silica dioxide medium layer is 10nm；The thickness of graphene layer 3 is 10nm, and two dimension is partly
The thickness of conductor crystal layer 4 is 1nm, and the material of two-dimensional semiconductor crystal layer 4 is TiS2。
In the present embodiment, the thickness of the first metal electrode 5 and the second metal electrode 6 is 10nm, and material is gold.Remaining
Be the same as Example 1.
Embodiment 6：
In the present embodiment, the material of flexible substrate 1 is ultra-thin glass, and the thickness of the ultra-thin glass is 6 μm, and dielectric layer 2 is
Silica dioxide medium layer, the thickness of silica dioxide medium layer is 15nm；The thickness of graphene layer 3 is 15nm, and two dimension is partly
The thickness of conductor crystal layer 4 is 10nm, and the material of two-dimensional semiconductor crystal layer 4 is VSe2。
In the present embodiment, the thickness of the first metal electrode 5 and the second metal electrode 6 is 20nm, and material is gold.Remaining
Be the same as Example 1.
Described above is only presently preferred embodiments of the present invention, and any type of limitation is not done to the present invention.Although
The present invention is disclosed above with preferred embodiments, but is not limited to the present invention.Any those skilled in the art,
Do not depart from the range of technical solution of the present invention, when making a little change using method and technology contents described above or repair
The equivalent embodiment for equivalent variations is adornd, as long as being the content without departing from the technology of the present invention incidence of criminal offenses, the technology according to the present invention is real
Any simple modification, equivalent variations and modification that confrontation above example is made, in the range of still falling within technical solution of the present invention.
Claims (7)
1. a kind of heterogeneous flexible thermoelectric conversion element of flexible folding, it is characterised in that the heterogeneous flexible thermoelectric conversion element
Including flexible substrate, grow dielectric layer and heterojunction structure on flexible substrates successively, described heterojunction structure include from it is lower to
The upper overlapping graphene layer and two-dimensional semiconductor crystal layer set, the described metal electrode of graphene layer one end growth regulation one, institute
The metal electrode of two-dimensional semiconductor crystal layer one end growth regulation two stated, and described the first metal electrode and the second metal electrode
Between it is mutually isolated；
Described dielectric layer is silica dioxide medium layer, and the thickness of silica dioxide medium layer is 10-100nm；
The overlapping setting vertical with two-dimensional semiconductor crystal layer of described graphene layer；
The thickness of described graphene layer is 10-20nm, and the thickness of described two-dimensional semiconductor crystal layer is 1-50nm；
During work, under the radiation of external heat source, the overlapping region of described graphene layer and two-dimensional semiconductor crystal layer is produced
Thermograde, causes Seebeck effect, produces open-circuit voltage, and carry out heat to electricity conversion.
2. the heterogeneous flexible thermoelectric conversion element of a kind of flexible folding according to claim 1, it is characterised in that described
Flexible substrate material be ultra-thin glass, high molecular polymer or tinsel in one kind.
3. the heterogeneous flexible thermoelectric conversion element of a kind of flexible folding according to claim 2, it is characterised in that described
Ultra-thin glass thickness be 10um within.
4. the heterogeneous flexible thermoelectric conversion element of a kind of flexible folding according to claim 2, it is characterised in that described
High molecular polymer be polyimides, PEN or polyethylene terephthalate in one kind.
5. the heterogeneous flexible thermoelectric conversion element of a kind of flexible folding according to claim 1, it is characterised in that described
The material of two-dimensional semiconductor crystal layer be the chalcogen compound of transition metal two, the chalcogen compound of transition metal two includes
MoS2、MoSe2、WS2、WSe2、TiS2Or VSe2In one kind.
6. the heterogeneous flexible thermoelectric conversion element of a kind of flexible folding according to claim 1, it is characterised in that described
The thickness of the first metal electrode be 10-200nm, and the material of described the first metal electrode is included in gold, silver, aluminium or titanium
One kind.
7. the heterogeneous flexible thermoelectric conversion element of a kind of flexible folding according to claim 1, it is characterised in that described
The thickness of the second metal electrode be 10-200nm, and the material of described the second metal electrode is included in gold, silver, aluminium or titanium
One kind.
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| CN105789323A (en) * | 2016-04-06 | 2016-07-20 | 清华大学 | Field effect transistor and preparation method thereof |
| CN105870314B (en) * | 2016-04-26 | 2018-08-07 | 桂林电子科技大学 | A kind of flexible silicon based nano film thermo-electric device |
| CN107293634A (en) * | 2017-06-14 | 2017-10-24 | 上海萃励电子科技有限公司 | A kind of preparation method of novel flexible thermoelectric element |
| CN108878636A (en) * | 2018-06-26 | 2018-11-23 | 上海电力学院 | A method of two-dimentional thermo-electric device is prepared based on two telluride molybdenums |
| CN113782665B (en) * | 2021-09-16 | 2023-06-16 | 河北工业大学 | WSe (Wireless sensor package) 2 /MoS 2 Preparation method of composite thermoelectric material |
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