CN106653897A - Copper, zinc, tin, sulfur and selenium thin film solar cell and preparation method therefor - Google Patents
Copper, zinc, tin, sulfur and selenium thin film solar cell and preparation method therefor Download PDFInfo
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- CN106653897A CN106653897A CN201510742016.4A CN201510742016A CN106653897A CN 106653897 A CN106653897 A CN 106653897A CN 201510742016 A CN201510742016 A CN 201510742016A CN 106653897 A CN106653897 A CN 106653897A
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- sulfur selenium
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- 239000010409 thin film Substances 0.000 title claims abstract description 64
- 239000011701 zinc Substances 0.000 title claims abstract description 42
- 238000002360 preparation method Methods 0.000 title claims abstract description 34
- 239000011669 selenium Substances 0.000 title claims abstract description 12
- 229910052711 selenium Inorganic materials 0.000 title claims abstract description 10
- BUGBHKTXTAQXES-UHFFFAOYSA-N Selenium Chemical compound [Se] BUGBHKTXTAQXES-UHFFFAOYSA-N 0.000 title claims abstract 8
- 239000010949 copper Substances 0.000 title abstract description 12
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 title abstract description 9
- 229910052802 copper Inorganic materials 0.000 title abstract description 9
- 229910052717 sulfur Inorganic materials 0.000 title abstract description 9
- 229910052718 tin Inorganic materials 0.000 title abstract description 8
- 239000011135 tin Substances 0.000 title abstract description 8
- 229910052725 zinc Inorganic materials 0.000 title abstract description 8
- NINIDFKCEFEMDL-UHFFFAOYSA-N Sulfur Chemical compound [S] NINIDFKCEFEMDL-UHFFFAOYSA-N 0.000 title abstract 7
- ATJFFYVFTNAWJD-UHFFFAOYSA-N Tin Chemical compound [Sn] ATJFFYVFTNAWJD-UHFFFAOYSA-N 0.000 title abstract 7
- HCHKCACWOHOZIP-UHFFFAOYSA-N Zinc Chemical compound [Zn] HCHKCACWOHOZIP-UHFFFAOYSA-N 0.000 title abstract 7
- 239000011593 sulfur Substances 0.000 title abstract 7
- 238000001755 magnetron sputter deposition Methods 0.000 claims abstract description 32
- 239000000758 substrate Substances 0.000 claims abstract description 31
- SEUJAMVVGAETFN-UHFFFAOYSA-N [Cu].[Zn].S=[Sn]=[Se] Chemical compound [Cu].[Zn].S=[Sn]=[Se] SEUJAMVVGAETFN-UHFFFAOYSA-N 0.000 claims description 79
- 238000004544 sputter deposition Methods 0.000 claims description 37
- 238000000034 method Methods 0.000 claims description 21
- 239000002243 precursor Substances 0.000 claims description 21
- 210000001142 back Anatomy 0.000 claims description 18
- 238000010438 heat treatment Methods 0.000 claims description 16
- 239000013077 target material Substances 0.000 claims description 16
- 239000005361 soda-lime glass Substances 0.000 claims description 9
- WILFBXOGIULNAF-UHFFFAOYSA-N copper sulfanylidenetin zinc Chemical compound [Sn]=S.[Zn].[Cu] WILFBXOGIULNAF-UHFFFAOYSA-N 0.000 claims description 5
- 238000005987 sulfurization reaction Methods 0.000 claims description 4
- TVZPLCNGKSPOJA-UHFFFAOYSA-N copper zinc Chemical compound [Cu].[Zn] TVZPLCNGKSPOJA-UHFFFAOYSA-N 0.000 claims description 2
- JPUIEYBUBJBWQJ-UHFFFAOYSA-N selanylidene(sulfanylidene)tin Chemical compound S=[Sn]=[Se] JPUIEYBUBJBWQJ-UHFFFAOYSA-N 0.000 claims description 2
- ZOKXTWBITQBERF-UHFFFAOYSA-N Molybdenum Chemical compound [Mo] ZOKXTWBITQBERF-UHFFFAOYSA-N 0.000 claims 1
- 229910052750 molybdenum Inorganic materials 0.000 claims 1
- 239000011733 molybdenum Substances 0.000 claims 1
- 238000005516 engineering process Methods 0.000 abstract description 9
- 238000010521 absorption reaction Methods 0.000 abstract 1
- 231100000701 toxic element Toxicity 0.000 abstract 1
- 239000007789 gas Substances 0.000 description 29
- 239000011777 magnesium Substances 0.000 description 21
- 238000005477 sputtering target Methods 0.000 description 15
- 239000010408 film Substances 0.000 description 13
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 description 12
- XLOMVQKBTHCTTD-UHFFFAOYSA-N Zinc monoxide Chemical compound [Zn]=O XLOMVQKBTHCTTD-UHFFFAOYSA-N 0.000 description 12
- 239000010453 quartz Substances 0.000 description 12
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N silicon dioxide Inorganic materials O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 description 12
- JYMITAMFTJDTAE-UHFFFAOYSA-N aluminum zinc oxygen(2-) Chemical group [O-2].[Al+3].[Zn+2] JYMITAMFTJDTAE-UHFFFAOYSA-N 0.000 description 10
- 239000000463 material Substances 0.000 description 8
- CSCPPACGZOOCGX-UHFFFAOYSA-N Acetone Chemical compound CC(C)=O CSCPPACGZOOCGX-UHFFFAOYSA-N 0.000 description 6
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 6
- 229910003310 Ni-Al Inorganic materials 0.000 description 6
- 239000011787 zinc oxide Substances 0.000 description 6
- 238000000151 deposition Methods 0.000 description 5
- 231100000252 nontoxic Toxicity 0.000 description 4
- 230000003000 nontoxic effect Effects 0.000 description 4
- FBWUJLFVLPYHMZ-UHFFFAOYSA-N [O-2].[Al+3].[Zn+2].[O-2].[Al+3].[Zn+2] Chemical compound [O-2].[Al+3].[Zn+2].[O-2].[Al+3].[Zn+2] FBWUJLFVLPYHMZ-UHFFFAOYSA-N 0.000 description 3
- 239000003708 ampul Substances 0.000 description 3
- 230000003139 buffering effect Effects 0.000 description 3
- 239000012159 carrier gas Substances 0.000 description 3
- 238000004140 cleaning Methods 0.000 description 3
- 238000001816 cooling Methods 0.000 description 3
- 239000008367 deionised water Substances 0.000 description 3
- 229910021641 deionized water Inorganic materials 0.000 description 3
- 235000019441 ethanol Nutrition 0.000 description 3
- 229910052757 nitrogen Inorganic materials 0.000 description 3
- 239000000843 powder Substances 0.000 description 3
- 230000002000 scavenging effect Effects 0.000 description 3
- 238000000427 thin-film deposition Methods 0.000 description 3
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Chemical compound O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 3
- 150000001450 anions Chemical class 0.000 description 2
- 238000010924 continuous production Methods 0.000 description 2
- 230000008021 deposition Effects 0.000 description 2
- 230000000694 effects Effects 0.000 description 2
- 229910052733 gallium Inorganic materials 0.000 description 2
- 229910052738 indium Inorganic materials 0.000 description 2
- 238000004519 manufacturing process Methods 0.000 description 2
- 238000005457 optimization Methods 0.000 description 2
- 230000003647 oxidation Effects 0.000 description 2
- 238000007254 oxidation reaction Methods 0.000 description 2
- 230000006798 recombination Effects 0.000 description 2
- 238000005215 recombination Methods 0.000 description 2
- 230000009466 transformation Effects 0.000 description 2
- 229910000611 Zinc aluminium Inorganic materials 0.000 description 1
- PDYXSJSAMVACOH-UHFFFAOYSA-N [Cu].[Zn].[Sn] Chemical compound [Cu].[Zn].[Sn] PDYXSJSAMVACOH-UHFFFAOYSA-N 0.000 description 1
- PGTXKIZLOWULDJ-UHFFFAOYSA-N [Mg].[Zn] Chemical compound [Mg].[Zn] PGTXKIZLOWULDJ-UHFFFAOYSA-N 0.000 description 1
- ZQRRBZZVXPVWRB-UHFFFAOYSA-N [S].[Se] Chemical compound [S].[Se] ZQRRBZZVXPVWRB-UHFFFAOYSA-N 0.000 description 1
- HXFVOUUOTHJFPX-UHFFFAOYSA-N alumane;zinc Chemical compound [AlH3].[Zn] HXFVOUUOTHJFPX-UHFFFAOYSA-N 0.000 description 1
- 229910052782 aluminium Inorganic materials 0.000 description 1
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 description 1
- 150000001875 compounds Chemical class 0.000 description 1
- 238000002347 injection Methods 0.000 description 1
- 239000007924 injection Substances 0.000 description 1
- 238000013082 photovoltaic technology Methods 0.000 description 1
- 231100000614 poison Toxicity 0.000 description 1
- 230000007096 poisonous effect Effects 0.000 description 1
- 238000005036 potential barrier Methods 0.000 description 1
- 239000010970 precious metal Substances 0.000 description 1
- 239000012495 reaction gas Substances 0.000 description 1
- 239000007787 solid Substances 0.000 description 1
- 239000000243 solution Substances 0.000 description 1
Classifications
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
- H01L31/00—Semiconductor devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation and specially adapted either for the conversion of the energy of such radiation into electrical energy or for the control of electrical energy by such radiation; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof
- H01L31/0248—Semiconductor devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation and specially adapted either for the conversion of the energy of such radiation into electrical energy or for the control of electrical energy by such radiation; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof characterised by their semiconductor bodies
- H01L31/0256—Semiconductor devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation and specially adapted either for the conversion of the energy of such radiation into electrical energy or for the control of electrical energy by such radiation; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof characterised by their semiconductor bodies characterised by the material
- H01L31/0264—Inorganic materials
- H01L31/032—Inorganic materials including, apart from doping materials or other impurities, only compounds not provided for in groups H01L31/0272 - H01L31/0312
- H01L31/0322—Inorganic materials including, apart from doping materials or other impurities, only compounds not provided for in groups H01L31/0272 - H01L31/0312 comprising only AIBIIICVI chalcopyrite compounds, e.g. Cu In Se2, Cu Ga Se2, Cu In Ga Se2
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
- H01L31/00—Semiconductor devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation and specially adapted either for the conversion of the energy of such radiation into electrical energy or for the control of electrical energy by such radiation; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof
- H01L31/0248—Semiconductor devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation and specially adapted either for the conversion of the energy of such radiation into electrical energy or for the control of electrical energy by such radiation; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof characterised by their semiconductor bodies
- H01L31/0256—Semiconductor devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation and specially adapted either for the conversion of the energy of such radiation into electrical energy or for the control of electrical energy by such radiation; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof characterised by their semiconductor bodies characterised by the material
- H01L31/0264—Inorganic materials
- H01L31/032—Inorganic materials including, apart from doping materials or other impurities, only compounds not provided for in groups H01L31/0272 - H01L31/0312
- H01L31/0322—Inorganic materials including, apart from doping materials or other impurities, only compounds not provided for in groups H01L31/0272 - H01L31/0312 comprising only AIBIIICVI chalcopyrite compounds, e.g. Cu In Se2, Cu Ga Se2, Cu In Ga Se2
- H01L31/0323—Inorganic materials including, apart from doping materials or other impurities, only compounds not provided for in groups H01L31/0272 - H01L31/0312 comprising only AIBIIICVI chalcopyrite compounds, e.g. Cu In Se2, Cu Ga Se2, Cu In Ga Se2 characterised by the doping material
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
- H01L31/00—Semiconductor devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation and specially adapted either for the conversion of the energy of such radiation into electrical energy or for the control of electrical energy by such radiation; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof
- H01L31/0248—Semiconductor devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation and specially adapted either for the conversion of the energy of such radiation into electrical energy or for the control of electrical energy by such radiation; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof characterised by their semiconductor bodies
- H01L31/0352—Semiconductor devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation and specially adapted either for the conversion of the energy of such radiation into electrical energy or for the control of electrical energy by such radiation; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof characterised by their semiconductor bodies characterised by their shape or by the shapes, relative sizes or disposition of the semiconductor regions
-
- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E10/00—Energy generation through renewable energy sources
- Y02E10/50—Photovoltaic [PV] energy
- Y02E10/541—CuInSe2 material PV cells
-
- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
- Y02P70/00—Climate change mitigation technologies in the production process for final industrial or consumer products
- Y02P70/50—Manufacturing or production processes characterised by the final manufactured product
Abstract
The invention discloses a copper, zinc, tin, sulfur and selenium thin film solar cell and a preparation method therefor. The solar cell comprises a substrate, a back electrode layer, a copper, zinc, tin, sulfur and selenium absorption layer, a buffer layer, a transparent conductive oxide layer and a top electrode that are orderly stacked; the buffer layer is made of (Zn1-xMgx)O; x is greater than or equal to 0.1 while being smaller than or equal to 0.25, and the buffer layer ranges from 50 nm and 80 nm in thickness. All layers in the solar cell are prepared via magnetron sputtering technologies. According to the copper, zinc, tin, sulfur and selenium thin film solar cell and the preparation method therefor, the (Zn1-xMgx)O buffer layer is used for replacing a CdS buffer layer and an intrinsic ZnO layer that are commonly adopted in a conventional copper, zinc, tin, sulfur and selenium thin film solar cell; the copper, zinc, tin, sulfur and selenium thin film solar cell disclosed in the invention is advantageous in that 1) via adjustment of Zn/Mg in (Zn1-xMgx)O, conduction band edge imbalance value of an interface of the copper, zinc, tin, sulfur and selenium/buffer layer can be optimized, and open-circuit voltage of the cell can be improved; 2) a toxic element Cd in CdS can be prevented, and large scale application of the cell can be facilitated; 3) cell preparation technologies are simplified.
Description
Technical field
The present invention relates to a kind of copper zinc tin sulfur selenium thin-film solar cells and preparation method thereof, belongs to photovoltaic technology
Field.
Background technology
As Cu (In, Ga) (S, Se)2(CIGSSe) substitute of thin-film solar cells, copper zinc tin sulfur selenium
CuZnSn (S, Se)4(CZTSSe) Zn and Sn of rich content replace in the thin-film solar cells earth's crust
Rare precious metals In and Ga in CIGSSe, greatly reduces the preparation cost of solar cell, therefore,
CZTSSe hull cells are considered to be a kind of solar cell of sustainable development.At present, CZTSSe films
The laboratory peak efficiency of battery up to 12.6% [Wang W.et al., Adv.Energy Mater., 4 (2014),
1301465], but Distance Theory efficiency still has larger gap.
It is to limit for CZTSSe absorbs layer material, dephasign and poor heterogeneous microstructure in material etc.
The main cause that this kind of thin-film solar cells efficiency is improved, but, except CZTSSe absorbs layer material
Oneself factor, the electrology characteristic of interface contacts equally can be very big between CZTSSe absorbed layers and cushion
Impact solar cell performance [Haight R.et al., Appl.Phys.Lett., 98 (2011), 253502].
Because CZTSSe hull cells are the substitutes of CIGSSe hull cells, for the ease of studying, at present
CZTSSe hull cells generally adopt the structure of CIGSSe batteries, wherein, using CdS as the buffering of battery
Layer material.For CIGS batteries, CIGS/CdS interfaces conduction band side imbalance value (CBO) is in 0.2~0.3eV models
In enclosing, little positive CBO is conducive to improving the open-circuit voltage (V of solar cellOC)[Gloeckler M.et
Al., Thin Solid Fims, 241 (2005), 480-481].And for CZTSSe hull cells,
The CBO of CZTSSe/CdS interfaces is usually negative value [Yan C.et al., Appl.Phys.Lett., 104
(2014), 173901;Li J.et al., Electron.Mater.Lett., 8 (2012), 365;Bar M.et al., Appl.
Phys.Lett., 99 (2011), 222105;Santoni A.et al., J.Phys.D:Appl.Phys., 46 (2013),
175101], negative CBO causes CZTSSe/CdS interfaces to form the potential barrier of electron injection, increases interface
The probability of recombination of majority carrier, and reduce the V of batteryoc.At present, CZTSSe hull cells are relatively low
VOCIt is to limit the principal element that battery efficiency is improved, and this and not optimized CZTSSe/CdS interfaces
The band arrangement at place has direct relation, additionally, the Cd elements in CdS cushions are poisonous, this also can be certain
The popularization and application of CZTSSe hull cells are hindered in degree.
Therefore, it is necessary to seek a kind of nontoxic New Buffering layer material to substitute CdS cushions, optimize
The CBO of CZTSSe/ buffer layer interfaces, improves the V of CZTSSe hull cellsOC, and then improve battery
Photoelectric transformation efficiency.
The content of the invention
It is an object of the invention to provide a kind of copper zinc tin sulfur selenium thin-film solar cells, using nontoxic new
Cushioning layer material optimizes CZTSSe/ buffer layer interfaces substituting CdS cushions and intrinsic zno layer
CBO, improves the V of CZTSSe hull cellsOC, and then improve the photoelectric transformation efficiency of battery.
Another object of the present invention is to provide the preparation method of the copper zinc tin sulfur selenium thin-film solar cells.
For achieving the above object, the present invention is employed the following technical solutions:
A kind of copper zinc tin sulfur selenium thin-film solar cells, including the substrate, dorsum electrode layer, copper zinc that stack gradually
Tin sulphur selenium absorbed layer, cushion, including transparent conducting oxide layer and top electrode, the cushion is by (Zn1-xMgx)O
Make, wherein 0.1≤x≤0.25.
Wherein, the including transparent conducting oxide layer is zinc oxide aluminum transparent conductive oxide layer.The cushion
Thickness be 50nm-80nm.
In the copper zinc tin sulfur selenium thin-film solar cells of the present invention, for (Zn1-xMgx) O, x is in [0.1,0.25]
In the range of.As x < 0.1, Mg contents are to (Zn1-xMgx) O band structures adjustment effect it is unobvious,
(Zn1-xMgx) O band structures are with the difference of ZnO band structures less, it is impossible to play optimization copper zinc tin sulfur selenium
/(Zn1-xMgx) effect of conduction band side imbalance value at O interface;As x > 0.25, (Zn1-xMgx) O occurs phase
Separate, generate the excessive MgO of energy gap, be unfavorable for copper zinc tin sulfur selenium/(Zn1-xMgx) conduction band at O interface
The optimization of side imbalance value.
And for (Zn1-xMgx) thickness of O cushions must be controlled in the range of [50nm, 80nm].Due to copper zinc
Tin-sulfur-selenium thin film itself has certain roughness, as (Zn1-xMgx) O buffer layer thicknesses be less than 50nm when,
(Zn1-xMgx) O cushions may not be completely covered copper zinc tin sulfur selenium film, so as to cause copper zinc tin sulfur selenium
Film portion surface directly contacts with the zinc oxide aluminum transparent conductive oxide layer of subsequent deposition, and copper-zinc-tin-sulfur
Selenium/zinc oxide aluminum interface has larger negative conduction band side imbalance value, therefore, the open-circuit voltage of battery can be deteriorated,
Al elements in simultaneous oxidation zinc-aluminium may diffuse into copper zinc tin sulfur selenium film, cause entering for battery efficiency
One step is reduced.As (Zn1-xMgx) O buffer layer thicknesses be more than 80nm when, the series electrical of hull cell can be increased
Resistance, reduces the short circuit current of battery.Therefore, (Zn1-xMgx) O buffer layer thicknesses are in the range of [50nm, 80nm]
It is more suitable.
A kind of preparation method of the copper zinc tin sulfur selenium thin-film solar cells, comprises the following steps:
1) with soda-lime glass as substrate, substrate is cleaned;
2) magnetron sputtering is adopted, copper dorsum electrode layer is prepared on substrate;
3) magnetron sputtering is adopted, copper zinc tin sulfur selenium precursor thin-film is prepared on dorsum electrode layer;
4) precursor thin-film is heat-treated, obtains copper zinc tin sulfur selenium absorbed layer;
5) magnetron sputtering is adopted, (Zn is prepared on copper zinc tin sulfur selenium absorbed layer1-xMgx) O cushions;
6) magnetron sputtering is adopted, in (Zn1-xMgx) including transparent conducting oxide layer is prepared on O cushions;
7) magnetron sputtering is adopted, top electrode is prepared on including transparent conducting oxide layer, obtain copper zinc tin sulfur selenium thin
Film solar cell.
In the present invention, described (Zn1-xMgx) preparation method of O cushions has various, wherein, it is described
(Zn1-xMgx) the first preparation methods of O cushions is:Using ZnO and MgO as target, with O2With
The mixed gas of Ar, using double target co-sputtering mode, are made as sputter gas on copper zinc tin sulfur selenium absorbed layer
Standby (Zn1-xMgx) O cushions.By the sputtering of regulation ZnO and MgO target in cushion preparation process
Power is adjusting (Zn1-xMgx) Zn/Mg ratios in O cushions, O in sputter gas2Effect be to keep away
Exempt from occur anion vacancy in the cushioning layer material for preparing, reduce the probability of recombination of photo-generated carrier.
(the Zn1-xMgx) second preparation method of O cushions be:Using Zn and MgO as target, with
O2With the mixed gas of Ar as sputter gas, using double target co-sputtering mode, in copper zinc tin sulfur selenium absorbed layer
Upper preparation (Zn1-xMgx) O cushions.In cushion preparation process, by adjusting Zn and MgO target
Sputtering power is adjusting (Zn1-xMgx) Zn/Mg ratios in O cushions, O in sputter gas2As reaction gas
Body, realizes the complete oxidation of buffer layer thin film.
(the Zn1-xMgx) the third preparation methods of O cushions is:With (Zn1-xMgx) O as target, with
O2With the mixed gas of Ar as sputter gas, mode is sputtered using single target, on copper zinc tin sulfur selenium absorbed layer
Prepare (Zn1-xMgx) O cushions.In cushion preparation process, by from Zn/Mg than different
(Zn1-xMgx) O targets to be adjusting (Zn1-xMgx) Zn/Mg ratios in O cushions, O in sputter gas2Work
With being anion vacancy occur in cushioning layer material in order to avoid preparing, the compound general of photo-generated carrier is reduced
Rate.
In above-mentioned preparation method, copper zinc tin sulfur selenium forerunner is prepared using the sputtering of single target or More target sputtering together mode
Body thin film, in copper zinc tin sulfur selenium presoma heat treatment process, using sulfuration or selenizing heat treatment mode, obtains
Obtain copper zinc tin sulfur selenium absorbed layer finally.
It is an advantage of the current invention that:
The present invention is with nontoxic (Zn1-xMgx) O cushions replace copper zinc tin sulfur selenium hull cell in commonly use CdS
Cushion and intrinsic zno layer, by adjusting (Zn1-xMgx) Zn/Mg ratios in O, optimize copper zinc tin sulfur selenium
/(Zn1-xMgx) conduction band side imbalance value at O interface, improve the open-circuit voltage of copper zinc tin sulfur selenium hull cell with
And photoelectric efficiency, and adopt (Zn1-xMgx) O cushions replace CdS cushions and intrinsic zno layer, moreover it is possible to
Enough simplify the preparation technology of copper zinc tin sulfur selenium thin-film solar cells.Additionally, in the copper zinc tin sulfur selenium of the present invention
In the preparation method of thin-film solar cells, each layer deposition adopts magnetron sputtering technique in battery, is conducive to
The exploitation of copper zinc tin sulfur selenium hull cell on-line continuous production technology, improve production efficiency.
Description of the drawings
Fig. 1 is the structural representation of the copper zinc tin sulfur selenium thin-film solar cells of the present invention.
Fig. 2 is the preparation technology flow chart of the copper zinc tin sulfur selenium thin-film solar cells of the present invention.
Specific embodiment
With reference to the accompanying drawings and examples the present invention will be further described, but embodiments of the present invention are not limited
In this.
As shown in figure 1, the structural representation of the copper zinc tin sulfur selenium thin-film solar cells of the present invention, including according to
It is the substrate 100 of secondary stacking, dorsum electrode layer 110, copper zinc tin sulfur selenium absorbed layer 120, cushion 130, transparent
Conductive oxide layer 140 and top electrode 150, the cushion is by (Zn1-xMgx) O makes, wherein
0.1≤x≤0.25, thickness is in the range of [50nm, 80nm].
As shown in Fig. 2 the preparation technology flow chart of the copper zinc tin sulfur selenium thin-film solar cells of the present invention, according to
It is secondary to comprise the following steps:
With soda-lime glass as substrate, substrate is cleaned;
Using magnetron sputtering, copper dorsum electrode layer is prepared on substrate;
Using magnetron sputtering, copper zinc tin sulfur selenium precursor thin-film is prepared on dorsum electrode layer;
Precursor thin-film is heat-treated, copper zinc tin sulfur selenium absorbed layer is obtained;
Using magnetron sputtering, (Zn is prepared on copper zinc tin sulfur selenium absorbed layer1-xMgx) O cushions, wherein
0.1≤x≤0.25, thickness is in the range of [50nm, 80nm];
Using magnetron sputtering, in (Zn1-xMgx) zinc oxide aluminum transparent conductive oxide layer is prepared on O cushions;
Using magnetron sputtering, top electrode is prepared in zinc oxide aluminum transparent conductive oxide layer, obtain copper zinc-tin
Sulfur-selenium thin film solar cell.
The present invention is with nontoxic (Zn1-xMgx) O cushions replace copper zinc tin sulfur selenium hull cell in commonly use CdS
Cushion and intrinsic zno layer, by adjusting (Zn1-xMgx) Zn/Mg ratios in O, optimize copper zinc tin sulfur selenium
/(Zn1-xMgx) conduction band side imbalance value at O interface, improve copper zinc tin sulfur selenium hull cell open-circuit voltage and
Photoelectric efficiency, and the preparation technology of copper zinc tin sulfur selenium thin-film solar cells can be simplified, be conducive to copper zinc-tin
The exploitation of sulfur-selenium thin film battery on-line continuous production technology, improve production efficiency.
Embodiment 1
All thin film depositions in the copper zinc tin sulfur selenium thin-film solar cells of the present embodiment adopt magnetron sputtering skill
Art, the copper zinc tin sulfur selenium thin-film solar cells finally prepared include stack gradually substrate, dorsum electrode layer,
Copper zinc tin sulfur selenium absorbed layer, cushion, including transparent conducting oxide layer and top electrode, the cushion by
(Zn0.85Mg0.15) O makes, buffer layer thickness is 60nm.Concrete preparation flow is as follows:
Step 1:Substrate is cleaned
With soda-lime glass as substrate, sequentially using deionized water, acetone and absolute ethyl alcohol substrate is carried out respectively
It is cleaned by ultrasonic, scavenging period is 10min, with nitrogen gun the ethanol of substrate surface remaining is blown off.
Step 2:It is prepared by Mo dorsum electrode layers
With Mo as sputtering target material, mode is sputtered using single target and is deposited on the soda-lime glass substrate that cleaning is finished
The Mo dorsum electrode layers of 1 μ m-thick.
Step 3:It is prepared by precursor thin-film
Using magnetron sputtering technique, with Cu2S, ZnS and SnS2For sputtering target material, three target co-sputterings prepare copper
Zinc-tin sulphur precursor thin-film, sputter gas be Ar gas, sputtering pressure 0.25Pa, Cu2S, ZnS and SnS2
Target as sputter power is followed successively by 65W, 87W and 27W, sputtering time 20min.
Step 4:Precursor thin-film is heat-treated
Selenizing heat treatment is carried out to copper-zinc-tin-sulfur precursor thin-film.Precursor thin-film is placed in tube furnace, together
When, the quartz boat equipped with Se powder is put in quartz ampoule, film is heated respectively with quartz boat, with N2As
Selenizing carrier gas.Quartz boat heating-up temperature is 400 DEG C, and film heat treatment temperature is 550 DEG C, heat treatment time
30min.After heating terminates, room temperature is naturally cooled to, in cooling procedure, N2Flow is constant, steady air current,
The final copper zinc tin sulfur selenium absorbed layer for preparing productization.
Step 5:(Zn1-xMgx) preparation of O cushions
Using magnetron sputtering technique, by sputtering target material double target co-sputtering of ZnO and MgO (Zn is prepared1-xMgx)O
Cushion.Sputter gas are O2With Ar mixed gas, O2It is 1: 50 with the gas flow ratio of Ar, sputters gas
Press as 0.3Pa, ZnO and MgO target sputtering power are respectively 80W and 17W, and sputtering time is 5min,
Finally prepare (Zn0.85Mg0.15) O cushions, buffer layer thickness is 60nm.
Step 6:It is prepared by zinc oxide aluminum transparent conductive oxide layer
Using magnetron sputtering technique, by sputtering target material of zinc oxide aluminum zinc oxide aluminum transparent conductive oxide is prepared
Layer.Al in target2O3Doping 3at%, sputter gas are Ar, and sputtering pressure is 0.3Pa, and sputtering power is
75W, sputtering time is 20min, finally prepares the zinc oxide aluminum transparent conductive oxide that thickness is 0.8 μm
Layer.
Step 7:It is prepared by top electrode
Ni-Al top electrodes are prepared using magnetron sputtering on including transparent conducting oxide layer.With Ni in sputter procedure
It is sputtering target material with Al, first deposits depositing Al layer after Ni layers, in the final Ni-Al top electrodes for preparing, Ni
0.05 μm of thickness degree, 1.95 μm of Al thickness degree.
According to copper zinc tin sulfur selenium thin-film solar cells prepared by above-mentioned technique, copper zinc tin sulfur selenium film
/(Zn0.85Mg0.15) the conduction band side imbalance value of O buffer layer interfaces is 0.15eV, battery open circuit voltage is
404mV, battery efficiency is 5.71%.
Embodiment 2
All thin film depositions in the copper zinc tin sulfur selenium thin-film solar cells of the present embodiment adopt magnetron sputtering skill
Art, the copper zinc tin sulfur selenium thin-film solar cells finally prepared include stack gradually substrate, dorsum electrode layer,
Copper zinc tin sulfur selenium absorbed layer, cushion, including transparent conducting oxide layer and top electrode, the cushion by
(Zn0.9Mg0.1) O makes, buffer layer thickness is 80nm.Concrete preparation flow is as follows:
Step 1:Substrate is cleaned
With soda-lime glass as substrate, sequentially using deionized water, acetone and absolute ethyl alcohol substrate is carried out respectively
It is cleaned by ultrasonic, scavenging period is 10min, with nitrogen gun the ethanol of substrate surface remaining is blown off.
Step 2:It is prepared by Mo dorsum electrode layers
With Mo as sputtering target material, mode is sputtered using single target and is deposited on the soda-lime glass substrate that cleaning is finished
The Mo dorsum electrode layers of 1 μ m-thick.
Step 3:It is prepared by precursor thin-film
Using magnetron sputtering technique, with copper zinc tin sulfur selenium as sputtering target material, single target sputtering is prepared before copper-zinc-tin-sulfur
Body thin film is driven, sputter gas are Ar gas, and sputtering pressure 0.25Pa, target as sputter power is followed successively by 90W, splashes
Penetrate time 25min.
Step 4:Precursor thin-film is heat-treated
Sulfuration heat treatment is carried out to copper zinc tin sulfur selenium precursor thin-film.Precursor thin-film is placed in tube furnace,
Meanwhile, the quartz boat equipped with S powder is put in quartz ampoule, film is heated respectively with quartz boat, with N2As
Sulfuration carrier gas.Quartz boat heating-up temperature is 130 DEG C, and film heat treatment temperature is 550 DEG C, heat treatment time
30min.After heating terminates, room temperature is naturally cooled to, in cooling procedure, N2Flow is constant, steady air current,
The final copper zinc tin sulfur selenium absorbed layer for preparing productization.
Step 5:(Zn1-xMgx) preparation of O cushions
Using magnetron sputtering technique, by sputtering target material double target co-sputtering of Zn and MgO (Zn is prepared1-xMgx)O
Cushion.Sputter gas are O2With Ar mixed gas, O2It is 1: 5 with the gas flow ratio of Ar, sputters gas
Press as 0.3Pa, Zn and MgO target sputtering power are followed successively by 90W and 20W, and sputtering time is 5min,
Finally prepare (Zn0.9Mg0.1) O cushions, buffer layer thickness is 80nm.
Step 6:It is prepared by zinc oxide aluminum transparent conductive oxide layer
Using magnetron sputtering technique, by sputtering target material of zinc oxide aluminum zinc oxide aluminum transparent conductive oxide is prepared
Layer.Al in target2O3Doping 3at%, sputter gas are Ar, and sputtering pressure is 0.3Pa, and sputtering power is
75W, sputtering time is 20min, finally prepares the zinc oxide aluminum transparent conductive oxide that thickness is 0.8 μm
Layer.
Step 7:It is prepared by top electrode
Ni-Al top electrodes are prepared using magnetron sputtering on including transparent conducting oxide layer.With Ni in sputter procedure
It is sputtering target material with Al, first deposits depositing Al layer after Ni layers, in the final Ni-Al top electrodes for preparing, Ni
0.05 μm of thickness degree, 1.95 μm of Al thickness degree.
According to copper zinc tin sulfur selenium thin-film solar cells prepared by above-mentioned technique, copper zinc tin sulfur selenium film
/(Zn0.85Mg0.15) O buffer layer interfaces conduction band side imbalance value be 0.1eV, battery open circuit voltage is 383mV,
Battery efficiency is 5.62%.
Embodiment 3
All thin film depositions in the copper zinc tin sulfur selenium thin-film solar cells of the present embodiment adopt magnetron sputtering skill
Art, the copper zinc tin sulfur selenium thin-film solar cells finally prepared include stack gradually substrate, dorsum electrode layer,
Copper zinc tin sulfur selenium absorbed layer, cushion, including transparent conducting oxide layer and top electrode, the cushion by
(Zn0.75Mg0.25) O makes, buffer layer thickness is 50nm.Concrete preparation flow is as follows:
Step 1:Substrate is cleaned
With soda-lime glass as substrate, sequentially using deionized water, acetone and absolute ethyl alcohol substrate is carried out respectively
It is cleaned by ultrasonic, scavenging period is 10min, with nitrogen gun the ethanol of substrate surface remaining is blown off.
Step 2:It is prepared by Mo dorsum electrode layers
With Mo as sputtering target material, mode is sputtered using single target and is deposited on the soda-lime glass substrate that cleaning is finished
The Mo dorsum electrode layers of 1 μ m-thick.
Step 3:It is prepared by precursor thin-film
Using magnetron sputtering technique, with copper zinc tin sulfur selenium as sputtering target material, single target sputtering prepares copper zinc tin sulfur selenium
Precursor thin-film, sputter gas are Ar gas, and sputtering pressure 0.25Pa, target as sputter power is 95W, is sputtered
Time 23min.
Step 4:Precursor thin-film is heat-treated
Selenizing heat treatment is carried out to copper-zinc-tin-sulfur precursor thin-film.Precursor thin-film is placed in tube furnace, together
When, the quartz boat equipped with Se powder is put in quartz ampoule, film is heated respectively with quartz boat, with N2As
Selenizing carrier gas.Quartz boat heating-up temperature is 350 DEG C, and film heat treatment temperature is 550 DEG C, heat treatment time
30min.After heating terminates, room temperature is naturally cooled to, in cooling procedure, N2Flow is constant, steady air current,
The final copper zinc tin sulfur selenium absorbed layer for preparing productization.
Step 5:(Zn1-xMgx) preparation of O cushions
Using magnetron sputtering technique, by sputtering target material list target sputtering of magnesium zinc (Zn is prepared1-xMgx) O bufferings
Layer.Sputter gas are O2With Ar mixed gas, O2Gas flow ratio with Ar is 1: 50, and sputtering pressure is
0.3Pa, target as sputter power is 60W, and sputtering time is 5min, finally prepares (Zn0.75Mg0.25) O delay
Layer is rushed, buffer layer thickness is 50nm.
Step 6:It is prepared by zinc oxide aluminum transparent conductive oxide layer
Using magnetron sputtering technique, by sputtering target material of zinc oxide aluminum zinc oxide aluminum transparent conductive oxide is prepared
Layer.Al in target2O3Doping 3at%, sputter gas are Ar, and sputtering pressure is 0.3Pa, and sputtering power is
75W, sputtering time is 20min, finally prepares the zinc oxide aluminum transparent conductive oxide that thickness is 0.8 μm
Layer.
Step 7:It is prepared by top electrode
Ni-Al top electrodes are prepared using magnetron sputtering on including transparent conducting oxide layer.With Ni in sputter procedure
It is sputtering target material with Al, first deposits depositing Al layer after Ni layers, in the final Ni-Al top electrodes for preparing, Ni
0.05 μm of thickness degree, 1.95 μm of Al thickness degree.
According to copper zinc tin sulfur selenium thin-film solar cells prepared by above-mentioned technique, copper zinc tin sulfur selenium film
/(Zn0.85Mg0.15) the conduction band side imbalance value of O buffer layer interfaces is 0.21eV, battery open circuit voltage is
422mV, battery efficiency is 5.79%.
Claims (7)
1. a kind of copper zinc tin sulfur selenium thin-film solar cells, it is characterised in that including the substrate for stacking gradually,
Dorsum electrode layer, copper zinc tin sulfur selenium absorbed layer, cushion, including transparent conducting oxide layer and top electrode, it is described slow
Layer is rushed by (Zn1-xMgx) O makes, wherein 0.1≤x≤0.25.
2. copper zinc tin sulfur selenium thin-film solar cells according to claim 1, it is characterised in that described
The thickness of cushion is 50nm-80nm.
3. the preparation method of copper zinc tin sulfur selenium thin-film solar cells described in a kind of claim 1 or 2, it is special
Levy and be, comprise the following steps:
1) with soda-lime glass as substrate, substrate is cleaned;
2) magnetron sputtering is adopted, molybdenum dorsum electrode layer is prepared on substrate;
3) magnetron sputtering is adopted, copper zinc tin sulfur selenium precursor thin-film is prepared on dorsum electrode layer;
4) precursor thin-film is heat-treated, obtains copper zinc tin sulfur selenium absorbed layer;
5) magnetron sputtering is adopted, (Zn is prepared on copper zinc tin sulfur selenium absorbed layer1-xMgx) O cushions;
6) magnetron sputtering is adopted, in (Zn1-xMgx) including transparent conducting oxide layer is prepared on O cushions;
7) magnetron sputtering is adopted, top electrode is prepared on including transparent conducting oxide layer, obtain copper zinc tin sulfur selenium thin
Film solar cell.
4. preparation method according to claim 3, it is characterised in that:Using ZnO and MgO as target
Material, with O2With the mixed gas of Ar as sputter gas, using double target co-sputtering mode, in copper-zinc-tin-sulfur
(Zn is prepared on selenium absorbed layer1-xMgx) O cushions, by adjust the sputtering power of ZnO and MgO target come
Adjust (Zn1-xMgx) Zn/Mg ratios in O cushions.
5. preparation method according to claim 3, it is characterised in that:Using Zn and MgO as target,
With O2With the mixed gas of Ar as sputter gas, using double target co-sputtering mode, inhale in copper zinc tin sulfur selenium
Receive and prepare on layer (Zn1-xMgx) O cushions, adjusted by adjusting the sputtering power of Zn and MgO target
(Zn1-xMgx) Zn/Mg ratios in O cushions.
6. preparation method according to claim 3, it is characterised in that:With (Zn1-xMgx) O as target,
With O2With the mixed gas of Ar as sputter gas, mode is sputtered using single target, absorbed in copper zinc tin sulfur selenium
(Zn is prepared on layer1-xMgx) O cushions, by from Zn/Mg than different (Zn1-xMgx) O targets to be adjusting
(Zn1-xMgx) Zn/Mg ratios in O cushions.
7. the preparation method according to any one of claim 3-6, it is characterised in that:Preparing copper zinc
During tin sulphur selenium precursor thin-film, prepared before copper zinc tin sulfur selenium using the sputtering of single target or More target sputtering together mode
Drive body thin film;In copper zinc tin sulfur selenium presoma heat treatment process, using sulfuration or selenizing heat treatment mode,
Obtain final copper zinc tin sulfur selenium absorbed layer.
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CN108336180A (en) * | 2017-12-30 | 2018-07-27 | 凯盛光伏材料有限公司 | The XRF detection methods of preformed layer in a kind of CIGS solar cells |
CN108461556A (en) * | 2018-01-26 | 2018-08-28 | 南京邮电大学 | Prepare precursor solution and its battery preparation and application of efficient CZTS solar cells |
CN108551312A (en) * | 2018-05-09 | 2018-09-18 | 常州大学 | A kind of Sb with stretchable structure2Se3Thin-film solar cells and preparation method |
CN114005903A (en) * | 2021-11-01 | 2022-02-01 | 中国科学院物理研究所 | Copper zinc tin sulfur selenium solar cell with back interface electric field and preparation method thereof |
CN114171636A (en) * | 2021-11-24 | 2022-03-11 | 湖北工业大学 | Preparation method of Cd-free tunneling buffer layer for CZTS thin-film solar cell |
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