CN104465980B - Thermoelectric material based on aluminium/nano-crystal silicon/Copper thin film and preparation method thereof - Google Patents
Thermoelectric material based on aluminium/nano-crystal silicon/Copper thin film and preparation method thereof Download PDFInfo
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Abstract
The invention discloses a kind of thermoelectric material based on aluminium/nano-crystal silicon/Copper thin film and preparation method thereof, the thermoelectric material is the first aluminium film for being sequentially depositing 60~140nm from the bottom up on a glass substrate, 150~350nm hydrogenation non crystal silicon film, 35~90nm Copper thin film, is then annealed in nitrogen atmosphere.Thermoelectric material material requested rich reserves of the present invention, cheap, without toxic element, preparation technology is simple, overcome conventional thermoelectric material material requested reserves it is few, containing toxic element, preparation technology it is complicated the problems such as, and relative to typical thermoelectric material (such as：Bi2Te3、Ca3Co4O9Deng) low temperature when (less than 100 DEG C) short circuit current flow, open-circuit voltage it is larger.
Description
Technical field
The invention belongs to field of material technology, and in particular to a kind of thin film thermoelectric materials, more particularly to based on aluminium/nano-crystal
Thermoelectric material of silicon/Copper thin film and preparation method thereof.
Background technology
Environment in recent years pollution, the requirement of energy crisis and some device miniaturizations (such as refrigerator and generator it is small-sized
Change etc.) the problems such as increasingly highlight, in the urgent need to new energy conversion technology solves these problems.Heat to electricity conversion is great potential
One of energy conversion technology.
Thermoelectric material be it is a kind of can by heat energy and the functional material of the mutual phase transformation of electric energy, with it is pollution-free, without machine driving
The advantages of, its micro element prepared can be utilized to be used to prepare micro power, microcell cooling, optical communication laser diode and infrared
The thermoregulating system of line sensor.Current existing thermoelectric material has semiconducting alloy thermoelectric material (such as Bi2Te3、PbTe、SiGe
Deng), Cobaltite Oxide Thermoelectric Materials (such as NaCo2O4、Ca3Co2O9Deng), metal alloy solid solution thermoelectric material (such as
AgTiTe, ZrNiSn, TiNiSn etc.), metal silicide type thermoelectric material (such as FeSi2、MnSi2Deng), Skutterudite thermoelectricity
(its formula is AB to material3, A is metallic element, and such as Ir, Co, Rh, Fe, B are V group elements, such as As, Sb, p, such as CoSb3)。
In above-mentioned thermoelectric material, some materials contain toxic element (such as Bi, Pb, As, Sb, P), and some contain on earth
Amount is few, and some preparation technologies are complicated.Therefore, it is necessary to explore cheap, aboundresources, prepare simple and environment-friendly thermoelectricity material
Material.
The content of the invention
The technical problems to be solved by the invention be overcome the problem of above-mentioned thermoelectric material is present there is provided one kind based on aluminium/
Thermoelectric material of nano-crystal silicon/Copper thin film and preparation method thereof.
Solving the technical scheme that is used of above-mentioned technical problem is：The above-mentioned thermoelectric material based on aluminium/nano-crystal silicon/Copper thin film
Prepared by following methods：
1st, the aluminium film that a layer thickness is 60~140nm is deposited on a glass substrate using thermal evaporation.
2nd, the hydrogen that a layer thickness is 150~350nm is deposited in aluminium film using plasma reinforced chemical vapour deposition method
Change amorphous silicon membrane.
3rd, the Copper thin film that a layer thickness is 35~90nm is deposited on hydrogenation non crystal silicon film using thermal evaporation, is obtained
Aluminium/amorphous silicon hydride/copper film material.
4th, aluminium/amorphous silicon hydride/copper film material is annealed 40~60 minutes for 500~600 DEG C in nitrogen atmosphere, obtained
Thermoelectric material based on aluminium/nano-crystal silicon/Copper thin film.
In above-mentioned step 1, the aluminium film that a layer thickness is 80nm is deposited on a glass substrate preferably by thermal evaporation,
The system base vacuum of thermal evaporation is 3 × 10-4Pa。
In above-mentioned step 2, a layer thickness is deposited in aluminium film preferably by plasma reinforced chemical vapour deposition method
For 200nm hydrogenation non crystal silicon film, the system base vacuum of plasma reinforced chemical vapour deposition method is 2 × 10-4Pa, deposition
When electrode spacing be 1.9cm, underlayer temperature be 160 DEG C, operating pressure is 60Pa, and power is 8W, SiH4Flow is 9sccm, H2Stream
Measure as 60sccm.
In above-mentioned step 3, it is 50nm's to deposit a layer thickness on hydrogenation non crystal silicon film preferably by thermal evaporation
Copper thin film, Copper thin film area is less than hydrogenation non crystal silicon film area, and the system base vacuum of thermal evaporation is 3 × 10-4Pa, is obtained
Aluminium/amorphous silicon hydride/copper film material.
The invention has the advantages that：The thermoelectric material material requested rich reserves of the present invention, it is cheap, be free of
Toxic element, preparation technology is simple, and relative to typical thermoelectric material (such as：Bi2Te3、Ca3Co4O9Deng) low temperature when (100 DEG C
Short circuit current flow, open-circuit voltage are larger below).
Brief description of the drawings
Fig. 1 is the structural representation of aluminium/amorphous silicon hydride/copper film material.In figure, 1 is glass substrate, and 2 be aluminium film,
3 be hydrogenation non crystal silicon film, and 4 be Copper thin film.
Fig. 2 is the open-circuit voltage and short circuit current flow variation with temperature graph of a relation of thermoelectric material prepared by embodiment 1.
Fig. 3 is the open-circuit voltage and short circuit current flow variation with temperature graph of a relation of thermoelectric material prepared by embodiment 2.
Fig. 4 is the open-circuit voltage and short circuit current flow variation with temperature graph of a relation of thermoelectric material prepared by embodiment 3.
Fig. 5 is the open-circuit voltage and short circuit current flow variation with temperature graph of a relation of thermoelectric material prepared by embodiment 4.
Embodiment
The present invention is described in more detail with reference to the accompanying drawings and examples, but protection scope of the present invention is not limited only to
These embodiments.
Embodiment 1
1st, by sheet glass substrate successively in acetone, ethanol be cleaned by ultrasonic 10 minutes, then successively with 70 DEG C of RCA1,
RCA2 solution soaks 20 minutes, then is cleaned up with deionized water, is finally dried up with nitrogen.As shown in figure 1, utilizing thermal evaporation
The aluminium film that deposition a layer thickness is 80nm on a glass substrate, thermal evaporation system base vacuum is 3 × 10-4Pa。
2nd, it is the hydrogenated amorphous of 200nm to deposit a layer thickness in aluminium film using plasma reinforced chemical vapour deposition method
Silicon thin film, the system base vacuum of plasma reinforced chemical vapour deposition method is 2 × 10-4Pa, electrode spacing is during deposition
1.9cm, underlayer temperature is 160 DEG C, and operating pressure is 60Pa, and power is 8W, SiH4Flow is 9sccm, H2Flow is 60sccm.
3rd, the Copper thin film that a layer thickness is 50nm, thermal evaporation system are deposited on hydrogenation non crystal silicon film using thermal evaporation
Base vacuum is 3 × 10-4Pa, Copper thin film area is less than hydrogenation non crystal silicon film area, obtains aluminium/amorphous silicon hydride/Copper thin film
Material.
4th, aluminium/amorphous silicon hydride/copper film material is annealed 50 minutes for 550 DEG C in nitrogen atmosphere, obtained based on aluminium/receive
The thermoelectric material of crystal silicon/Copper thin film.
After tested, there is transverse current between the Copper thin film of the thermoelectric material and nano-crystal silicon thin film, the short circuit of the thermoelectric material
Electric current and open-circuit voltage are as shown in Figure 2 with the variation relation of environment temperature.As seen from the figure, in absolute temperature 293K, its short circuit
Electric current and open-circuit voltage are 0.05 μ A, 0.222mV respectively；In 311K, its short circuit current flow and open-circuit voltage be respectively 0.30 μ A,
3.75mV；In 328K, its short circuit current flow and open-circuit voltage are 0.68 μ A, 9.2mV respectively；In 342K, its short circuit current flow with
Open-circuit voltage is 0.87 μ A, 12.8mV respectively；In 358K, its short circuit current flow and open-circuit voltage are 1.14 μ A, 17.9mV respectively；
In 370K, its short circuit current flow and open-circuit voltage are 1.48 μ A, 23.0mV respectively.
Embodiment 2
In the present embodiment, the deposit thickness of aluminium film is that 60nm, the deposit thickness of hydrogenation non crystal silicon film are 150nm, copper
The deposit thickness of film is 90nm, and other steps are same as Example 1, obtain the thermoelectricity material based on aluminium/nano-crystal silicon/Copper thin film
Material.After tested, have transverse current between the Copper thin film of the thermoelectric material and nano-crystal silicon thin film, the short circuit current flow of the thermoelectric material and
Open-circuit voltage is as shown in Figure 3 with the variation relation of environment temperature.As seen from the figure, in absolute temperature 293K, its short circuit current flow with
Open-circuit voltage is 0.006 μ A, 0.41mV respectively；In 311K, its short circuit current flow and open-circuit voltage be respectively 0.019 μ A,
1.31mv；In 328K, its short circuit current flow and open-circuit voltage are 0.047 μ A, 6.94mV respectively；In 342K, its short circuit current flow
It is 0.075 μ A, 15.56mV respectively with open-circuit voltage；In 358K, its short circuit current flow and open-circuit voltage be respectively 0.111 μ A,
18.14mV；In 370K, its short circuit current flow and open-circuit voltage are 0.157 μ A, 39mV respectively.
Embodiment 3
In the present embodiment, the deposit thickness of aluminium film is that 100nm, the deposit thickness of hydrogenation non crystal silicon film are 150nm, copper
The deposit thickness of film is 35nm, and other steps are same as Example 1, obtain the thermoelectricity material based on aluminium/nano-crystal silicon/Copper thin film
Material.After tested, have transverse current between the Copper thin film of the thermoelectric material and nano-crystal silicon thin film, the short circuit current flow of the thermoelectric material and
Open-circuit voltage is as shown in Figure 4 with the variation relation of environment temperature.As seen from the figure, in absolute temperature 293K, its short circuit current flow with
Open-circuit voltage is 0.001 μ A, 1.30mV respectively；In 311K, its short circuit current flow and open-circuit voltage be respectively 0.005 μ A,
3.44mV；In 328K, its short circuit current flow and open-circuit voltage are 0.013 μ A, 6.82mV respectively；In 342K, its short circuit current flow
It is 0.019 μ A, 11.32mV respectively with open-circuit voltage；In 358K, its short circuit current flow and open-circuit voltage be respectively 0.029 μ A,
20.86mV；In 370K, its short circuit current flow and open-circuit voltage are 0.039 μ A, 26.36mV respectively.
Embodiment 4
In the present embodiment, the deposit thickness of aluminium film is that 140nm, the deposit thickness of hydrogenation non crystal silicon film are 350nm, copper
The deposit thickness of film is 50nm, and other steps are same as Example 1, obtain the thermoelectricity material based on aluminium/nano-crystal silicon/Copper thin film
Material.After tested, have transverse current between the Copper thin film of the thermoelectric material and nano-crystal silicon thin film, the short circuit current flow of the thermoelectric material and
Open-circuit voltage is as shown in Figure 5 with the variation relation of environment temperature.As seen from the figure, in absolute temperature 293K, its short circuit current flow with
Open-circuit voltage is 0.002 μ A, 0.42mV respectively；In 311K, its short circuit current flow and open-circuit voltage be respectively 0.014 μ A,
1.24mV；In 328K, its short circuit current flow and open-circuit voltage are 0.032 μ A, 3.13mV respectively；In 342K, its short circuit current flow
It is 0.046 μ A, 4.76mV respectively with open-circuit voltage；In 358K, its short circuit current flow and open-circuit voltage be respectively 0.063 μ A,
12.74mV；In 370K, its short circuit current flow and open-circuit voltage are 0.080 μ A, 13.21mV respectively.
Embodiment 5
In the step 4 of embodiment 1~4,500 DEG C of annealing in nitrogen atmosphere by aluminium/amorphous silicon hydride/copper film material
60 minutes, other steps were identical with corresponding embodiment, obtained the thermoelectric material based on aluminium/nano-crystal silicon/Copper thin film.
Embodiment 6
In the step 4 of embodiment 1~4,600 DEG C of annealing in nitrogen atmosphere by aluminium/amorphous silicon hydride/copper film material
40 minutes, other steps were identical with corresponding embodiment, obtained the thermoelectric material based on aluminium/nano-crystal silicon/Copper thin film.
Claims (5)
1. a kind of thermoelectric material based on aluminium/nano-crystal silicon/Copper thin film, it is characterised in that it is prepared by following methods：
(1) aluminium film that a layer thickness is 60~140nm is deposited on a glass substrate using thermal evaporation；
(2) plasma reinforced chemical vapour deposition method is utilized to deposit the hydrogenation that a layer thickness is 150~350nm in aluminium film non-
Polycrystal silicon film；
(3) Copper thin film that a layer thickness is 35~90nm is deposited on hydrogenation non crystal silicon film using thermal evaporation, obtains aluminium/hydrogen
Change non-crystalline silicon/copper film material；
(4) aluminium/amorphous silicon hydride/copper film material is annealed 40~60 minutes for 500~600 DEG C in nitrogen atmosphere, obtains base
In the thermoelectric material of aluminium/nano-crystal silicon/Copper thin film.
2. the thermoelectric material according to claim 1 based on aluminium/nano-crystal silicon/Copper thin film, it is characterised in that：Described step
(1) in, the aluminium film that a layer thickness is 80nm is deposited on a glass substrate using thermal evaporation, the system background of thermal evaporation is true
Sky is 3 × 10-4Pa。
3. the thermoelectric material according to claim 2 based on aluminium/nano-crystal silicon/Copper thin film, it is characterised in that：Described step
(2) in, the amorphous silicon hydride that a layer thickness is 200nm is deposited in aluminium film using plasma reinforced chemical vapour deposition method thin
Film, the system base vacuum of plasma reinforced chemical vapour deposition method is 2 × 10-4Pa, electrode spacing is 1.9cm, lining during deposition
Bottom temperature is 160 DEG C, and operating pressure is 60Pa, and power is 8W, SiH4Flow is 9sccm, H2Flow is 60sccm.
4. the thermoelectric material according to claim 3 based on aluminium/nano-crystal silicon/Copper thin film, it is characterised in that：Described step
(3) in, the Copper thin film that a layer thickness is 50nm, the system of thermal evaporation are deposited on hydrogenation non crystal silicon film using thermal evaporation
Base vacuum is 3 × 10-4Pa, obtains aluminium/amorphous silicon hydride/copper film material.
5. the thermoelectric material according to claim 1 based on aluminium/nano-crystal silicon/Copper thin film, it is characterised in that：Described copper is thin
Membrane area is less than hydrogenation non crystal silicon film area.
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| CN1870302A (en) * | 2006-06-14 | 2006-11-29 | 秦友刚 | Photoelectric/thermoelectric conversion battery |
| CN102002673A (en) * | 2010-09-17 | 2011-04-06 | 陕西师范大学 | Preparation method of nanocrystalline silicon-aluminum oxide/silicon oxide thermoelectric film material |
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| WO2011148686A1 (en) * | 2010-05-28 | 2011-12-01 | 学校法人東京理科大学 | Method for production of thermoelectric conversion module, and thermoelectric conversion module |
| WO2012021872A2 (en) * | 2010-08-12 | 2012-02-16 | Sager Brian M | Thermoelectric stack coating for improves solar panel function |
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| CN1870302A (en) * | 2006-06-14 | 2006-11-29 | 秦友刚 | Photoelectric/thermoelectric conversion battery |
| CN102002673A (en) * | 2010-09-17 | 2011-04-06 | 陕西师范大学 | Preparation method of nanocrystalline silicon-aluminum oxide/silicon oxide thermoelectric film material |
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| 铝诱导晶化法制备多晶硅薄膜;刘伟等;《现代显示》;20080229(第84期);"铝诱导晶化法制备多晶硅薄膜的一般过程"部分 * |
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