CN103855307A - Perovskite solar battery and preparing method thereof - Google Patents
Perovskite solar battery and preparing method thereof Download PDFInfo
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- CN103855307A CN103855307A CN201410095058.9A CN201410095058A CN103855307A CN 103855307 A CN103855307 A CN 103855307A CN 201410095058 A CN201410095058 A CN 201410095058A CN 103855307 A CN103855307 A CN 103855307A
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- H10K85/00—Organic materials used in the body or electrodes of devices covered by this subclass
- H10K85/20—Carbon compounds, e.g. carbon nanotubes or fullerenes
- H10K85/211—Fullerenes, e.g. C60
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Abstract
The invention relates to a perovskite solar battery and a preparing method thereof. The perovskite solar battery comprises a transparent electrode, a hole transmission layer, a perovskite light absorption layer, an electronic transmission layer and a metal electrode. The hole transmission layer comprises at least one of PEDOT: PSS, P3HT, PTAA, PThTPTI, metallic oxide and graphene oxide. The electronic transmission layer comprises at least one of 58 pi-electronic fullerene PCBM, 56 pi-electronic fullerene OQMF, 54 pi-electronic fullerene OQBMF, PFN, PEIE, ZnO, TiO2, doped or modified ZnO or TiO2. The perovskite solar battery is high in energy exchange efficiency and low in cost and can be produced on a large scale, and the preparing method is simple in technology.
Description
Technical field
The present invention relates to solar cell field, relate in particular to a kind of efficient calcium titanium ore solar cell and preparation method thereof.
Background technology
Along with the mankind are to the increasing substantially and the serious environmental pollution that causes of fossil energy of energy demand, and the continuous exhaustion of fossil energy, energy problem has become the major issue that the whole mankind faces.The Spring Festival in 2014 shortly past, there is the serious haze being caused by vehicle exhaust and industrial discharge in many ground, the whole nation, greatly damaged people ' s health and national image day after day, caused the concern of the whole society to the energy and environmental pollution, fast-developing clear energy sources is imperative.Solar energy is a kind of clean, safe and inexhaustible energy, effectively utilizes solar energy to alleviating energy crisis and protection of the environment, promotes economic development significant.
1954, the single crystal silicon solar cell that U.S.'s Bell Laboratory reported first efficiency is 6%.Afterwards, the research in solar cell field sustainable development always.Solar cell mainly comprises monocrystalline/polycrystalline silicon solar cell, inorganic semiconductor (GaAs, cadmium telluride and Copper Indium Gallium Selenide) thin film solar cell, and three generations's solar cell such as dye sensitization, quantum dot, organic photovoltaic cell.Although these a few class batteries are all obtaining further investigation aspect basic science and practical application, because once making solar cell development, the problems such as production cost is high or toxicity is large or energy conversion efficiency is low were absorbed in the bottleneck phase.
2009, Miyasaka etc. were first by perovskite CH
3nH
3pbI
3and CH
3nH
3pbBr
3obtain 3.8% energy conversion efficiency for dye-sensitized cell as sensitising agent.Afterwards, perovskite (CH
3nH
3pbI
3-xb
x, B=I, Cl, Br) because it is synthetic simple, cost is low, solution-processible, absorptivity be high, possess the advantage such as transporting holes and electronic capability simultaneously obtains fast development in photovoltaic field.2012, the people such as the Snaith of Oxford University were by perovskite CH
3nH
3pbI
2cl is used for the fine and close TiO of FTO/ as light-absorption layer
2layer/mesoporous TiO
2or Al
2o
3in/calcium titanium ore bed/Spiro-OMeTAD hole transmission layer/Ag solar cell, battery open circuit voltage V
ocup to 1.1V, energy conversion efficiency PCE, up to 10.9%, starts the upsurge of research perovskite solar cell in the world.2014, Snaith etc. were by improving fine and close TiO
2layer refreshes battery efficiency to 15.9%, and this is the peak efficiency of current perovskite solar cell.But there are some problems in this battery, as fine and close TiO
2electron transfer layer and mesoporous TiO
2shelf layer all needs 500 DEG C of high-temperature process, hole transmission layer Spiro-OMeTAD expensive etc.Therefore, explore new calcium titanium ore solar battery structure and preparation method, to obtain higher-energy transformation efficiency and to there is lower cost, be significant.
Summary of the invention
For the deficiencies in the prior art, the invention provides a kind of perovskite solar cell and preparation method thereof, described perovskite solar cell has higher energy conversion efficiency, and has lower cost; Described preparation method's technique is simple, can carry out large-scale production.
One of object of the present invention is to provide a kind of perovskite solar cell, comprise transparency electrode, the hole transmission layer forming in described transparency electrode, the perovskite light-absorption layer forming on described hole transmission layer, the electron transfer layer forming on described perovskite light-absorption layer and the metal electrode forming on described electron transfer layer, or comprise transparency electrode, the electron transfer layer forming in described transparency electrode, the perovskite light-absorption layer forming on described electron transfer layer, the hole transmission layer forming on described perovskite light-absorption layer and the metal electrode forming on described hole transmission layer.
The hole transmission layer with the perovskite solar cell of said structure comprises PEDOT:PSS(Poly (3, 4-ethylenedioxythiophene)-polystyrene sulfonate, poly-(3, 4-ethylenedioxy thiophene)-polystyrolsulfon acid), P3HT(poly (3-hexylthiophene), poly-(3-hexyl thiophene)), PTAA(polytriarylamine, poly-three arylamine), PThTPTI(Poly{2, 5-thiophene-alt-2, 8-(4, 10-bis (2-hexyldecyl)) thieno[2', 3':5, 6] pyrido[3, 4-g] th ieno[3, 2-c] isoquinoline-5, 11 (4H, 10H)-dione}), at least one in metal oxide and graphene oxide, described electron transfer layer comprises 58 π-electronics fullerene PCBM([6, 6]-phenyl-C61-butyric acid methyl ester, [6, 6]-phenyl-C61-methyl butyrate), 56 π-electronics fullerene OQMF(o-quinodimethane-methano[60] fullerene, adjacent benzoquinones bismethane methylene [60] fullerene), 54 π-electronics fullerene OQBMF(o-quinodimethane-bis-methano[60] fullerene, adjacent benzoquinones bismethane dimethylene [60] fullerene), PFN(poly[(9, 9-bis (3 '-(N, N-dimethylamino) propyl)-2, 7-fluorene)-alt-2, 7-(9, 9 – dioctylfluorene)], [9, two (3 '-(the N of 9-, N-dimethyl amido) propyl group)-2, 7-fluorenes]-[2, 7-(9, 9 – dioctyl fluorene)] alternate copolymer), PEIE(ethoxylated polyethylenimine, ethoxylation polymine), ZnO, TiO
2, doping or modify ZnO or TiO
2in at least one.
As preferred version of the present invention, described metal oxide is MoO
x(wherein x=2~3), NiO, V
2o
5and/or WO
3.
As preferred version of the present invention, described hole transmission layer comprises at least one in PEDOT:PSS, P3HT, PTAA and PThTPTI.
As preferred version of the present invention, the ZnO of described doping or modification or TiO
2for example, for the ZnO of Al doping ZnO, PFN or PEIE modification, the ZnO of fullerene derivate (C-PCBSD and/or bis-DBMD) modification and/or the TiO that various resilient coating is modified
2.
As preferred version of the present invention, described electron transfer layer comprises 58 π-electronics fullerene PCBM, 56 π-electronics fullerene OQMF, 54 π-electronics fullerene OQBMF, ZnO and TiO
2in at least one, at least one in more preferably 58 π-electronics fullerene PCBM, 56 π-electronics fullerene OQMF and 54 π-electronics fullerene OQBMF.
As preferred version of the present invention, described perovskite light-absorption layer comprises CH
3nH
3mI
3-xb
x, wherein x=0~3, M is selected from Pb or Sn, and B is selected from I, Cl or Br.The example of the material typical case of described perovskite light-absorption layer but indefiniteness is such as CH
3nH
3pbCl
3, CH
3nH
3pbBr
3, CH
3nH
3pbI
3, CH
3nH
3pbIBr
2, CH
3nH
3pbI
2br, CH
3nH
3pbI
2cl, CH
3nH
3pbICl
2, CH
3nH
3snCl
3, CH
3nH
3snBr
3, CH
3nH
3snI
3, CH
3nH
3snIBr
2, CH
3nH
3snI
2br or CH
3nH
3snICl
2deng.
As preferred version of the present invention, described perovskite solar cell comprises transparency electrode, the hole transmission layer forming in described transparency electrode, the perovskite light-absorption layer forming on described hole transmission layer, the electron transfer layer forming on described perovskite light-absorption layer and the metal electrode that forms on described electron transfer layer; Wherein said hole transmission layer comprises at least one in PEDOT:PSS, metal oxide and graphene oxide, preferably PEDOT:PSS; Described electron transfer layer comprises at least one in 58 π-electronics fullerene PCBM, 56 π-electronics fullerene OQMF, 54 π-electronics fullerene OQBMF, PFN, PEIE and ZnO, at least one in preferably 58 π-electronics fullerene PCBM, 56 π-electronics fullerene OQMF and 54 π-electronics fullerene OQBMF; Described perovskite light-absorption layer comprises CH
3nH
3mI
3-xb
x, wherein x=0~3, M is selected from Pb or Sn, and B is selected from I, Cl or Br.
As preferred version of the present invention, described perovskite solar cell comprises transparency electrode, the electron transfer layer forming in described transparency electrode, the perovskite light-absorption layer forming on described electron transfer layer, the hole transmission layer forming on described perovskite light-absorption layer and the metal electrode that forms on described hole transmission layer; Wherein said hole transmission layer comprises at least one in P3HT, PTAA and PThTPTI; Described electron transfer layer comprises ZnO, TiO
2, the TiO that modifies of ZnO that Al doping ZnO, PFN or PEIE modify, ZnO that fullerene derivate is modified and/or various resilient coating
2in at least one; Described perovskite light-absorption layer comprises CH
3nH
3mI
3-xb
x, wherein x=0~3, M is selected from Pb or Sn, and B is selected from I, Cl or Br.
As preferred version of the present invention, described transparency electrode is the substrate of glass that tin indium oxide (ITO) or fluorine-doped tin oxide (FTO) cover, or PET(PETG, polyethylene terephthalate) flexible substrates.
As preferred version of the present invention, described metal electrode is gold, silver or aluminium electrode.
One of object of the present invention is also to provide a kind of method of preparing above-mentioned perovskite solar cell, comprises the steps:
(1) material of hole transmission layer is spun on to transparency electrode, at 100~170 DEG C, heats 10~50min, obtain the hole transport layer film that 15~60nm is thick;
(2) material of perovskite light-absorption layer is spun on described hole transport layer film, at 70~160 DEG C, heats 15min~2h, obtain the perovskite light-absorption layer film that 100~600nm is thick;
(3) material of electron transfer layer is spun on described perovskite light-absorption layer film, obtains the electric transmission layer film that 30~150nm is thick;
(4), under vacuum condition, evaporation 60~400nm metal electrode, makes described perovskite solar cell.
In said method, step (1) heating-up temperature can be 100 DEG C, 105 DEG C, 110 DEG C, 130 DEG C, 150 DEG C, 155 DEG C, 160 DEG C, 165 DEG C or 169 DEG C, can be 12min, 15min, 18min, 25min, 30min, 40min, 42min, 44min, 47min or 49min heating time, and the thickness of the hole transport layer film of formation can be 16nm, 18nm, 22nm, 28nm, 32nm, 35nm, 42nm, 45nm, 48nm, 54nm or 57nm; Step (2) heating-up temperature can be 71 DEG C, 73 DEG C, 76 DEG C, 80 DEG C, 100 DEG C, 120 DEG C, 140 DEG C, 145 DEG C, 148 DEG C, 155 DEG C or 157 DEG C, can be 15min, 25min, 30min, 40min, 50min, 60min, 80min, 95min, 100min, 110min or 115min heating time, and the thickness of the perovskite light-absorption layer film of formation can be 120nm, 150nm, 200nm, 300nm, 350nm, 450nm, 500nm, 540nm or 580nm; The thickness of the electric transmission layer film that step (3) forms can be 35nm, 40nm, 50nm, 70nm, 100nm, 120nm, 130nm, 140nm or 148nm; The thickness of the metal electrode that step (4) evaporation forms can be 70nm, 80nm, 90nm, 150nm, 200nm, 300nm, 350nm, 380nm or 390nm.
One of object of the present invention is also to provide a kind of method of preparing above-mentioned perovskite solar cell, comprises the steps:
(1) material of electron transfer layer is spun on to transparency electrode, at 150~510 DEG C, heats 20~80min, obtain the electric transmission layer film that 15~60nm is thick;
(2) material of perovskite light-absorption layer is spun on described electric transmission layer film, or after first lead iodide solution being spun on and being then soaked on described electric transmission layer film and taking out in iodate methylamine solution; At 70~160 DEG C, heat 15min~2h again, obtain the perovskite light-absorption layer film that 100~600nm is thick;
(3) material of hole transmission layer is spun on described perovskite light-absorption layer film, obtains the hole transport layer film that 30~250nm is thick;
(4), under vacuum condition, evaporation 60~300nm metal electrode, makes described perovskite solar cell.
In said method, step (1) heating-up temperature can be 150 DEG C, 155 DEG C, 160 DEG C, 165 DEG C, 172 DEG C, 178 DEG C, 190 DEG C, 250 DEG C, 310 DEG C, 360 DEG C, 400 DEG C, 442 DEG C or 510 DEG C, can be 25min, 30min, 40min, 50min, 60min, 65min, 70min, 75min or 78min heating time, and the thickness of the electric transmission layer film of formation can be 16nm, 18nm, 22nm, 28nm, 32nm, 35nm, 42nm, 45nm, 50nm, 55nm or 58nm, the preferred lead iodide dimethyl formamide of lead iodide solution (DMF) solution in step (2), the preferred iodate methylamine of iodate methylamine solution aqueous isopropanol, heating-up temperature can be 70 DEG C, 72 DEG C, 75 DEG C, 80 DEG C, 100 DEG C, 120 DEG C, 140 DEG C, 145 DEG C, 148 DEG C, 155 DEG C or 157 DEG C, can be 15min heating time, 25min, 30min, 40min, 50min, 60min, 80min, 95min, 100min, 110min or 115min, the thickness of the perovskite light-absorption layer film forming can be 120nm, 150nm, 200nm, 300nm, 350nm, 450nm, 500nm, 540nm or 580nm, the thickness of the hole transport layer film that step (3) forms can be 35nm, 40nm, 50nm, 70nm, 100nm, 120nm, 130nm, 140nm, 160nm, 180nm, 210nm, 230nm or 245nm, the thickness of the metal electrode that step (4) evaporation forms can be 70nm, 80nm, 90nm, 110nm, 130nm, 150nm, 200nm, 240nm, 280nm or 300nm.
As preferred version of the present invention, the rotating speed of described spin coating is all less than 5000rpm, preferably 500-4500rpm, more preferably 1000-4000rpm.
Beneficial effect of the present invention is: perovskite solar cell of the present invention adopts the material of lower-cost material as hole transmission layer and electron transfer layer, can realize higher energy conversion efficiency (more than 13%); Preparation method's technique of perovskite solar cell of the present invention is simple, does not relate to harsh process conditions.Therefore, perovskite solar cell of the present invention has high industrial application value.
Brief description of the drawings
Fig. 1 is the structural representation of perovskite solar cell representative in the embodiment of the present invention, and two of left and right figure shows respectively two kinds of tactic patterns of perovskite solar cell of the present invention.
Fig. 2 is the representative perovskite CH preparing in the embodiment of the present invention
3nH
3pbI
3-xcl
xthe uv-visible absorption spectra of film, tests the CH preparing in substrate of glass with Shimadzu UV-1800 ultraviolet-visible spectrometer
3nH
3pbI
3-xcl
xfilm obtains.
Description of reference numerals:
1-transparency electrode; 2-hole transmission layer; 3-perovskite light-absorption layer; 4-electron transfer layer; 5-metal electrode.
Embodiment
Below in conjunction with embodiment, embodiment of the present invention are described in detail.It will be understood to those of skill in the art that following examples are only the preferred embodiments of the present invention, so that understand better the present invention, thereby should not be considered as limiting scope of the present invention.
Experimental technique in following embodiment, if no special instructions, is conventional method; Experiment material used, if no special instructions, is and is purchased available from conventional chemical chemical reagent work.
The material source using in the embodiment of the present invention is described as follows: iodate methylamine CH
3nH
3i is according to Efficient inorganic – organic hybrid heterojunction solar cells containing perovskite compound and polymeric hole conductors.Seok et al, Nat.Photonics, 2013,7,486-491 preparation; OQMF is according to o-Quinodimethane-methano[60] fullerene and Thieno-o-quinodimethane-methano[60] fullerene as Efficient Acceptor Materials for Polymer Solar Cells.L.Ding et al, J.Mater.Chem., 2012,22,22374-22377 preparation; OQBMF is according to Methanofullerenes, C60 (CH2) n (n=1,2,3), as Building Blocks for High-Performance Acceptors Used in Organic Solar Cells.L.Ding et al, Org.Lett., 2014,16,612-615 preparation; C-PCBSD is according to Highly Efficient and Stable Inverted Polymer Solar Cells Integrated with a Cross-Linked Fullerene Material as an Interlayer.C.-S.Hsu et al, J.Am.Chem.Soc., 2010,132,4887 preparations; Bis-DBMD is according to Thermo-cleavable fullerene materials as buffer layers for efficient polymer solar cells.L.Ding et al, J.Mater.Chem.A, 2013,1,11170-11176 preparation; PThTPTI is according to Apentacyclic aromatic lactam building block for efficient polymer solar cells.L.Ding et al, Energy Environ.Sci., 2013,6,3224-3228 preparation; P3HT is purchased from Rieke Metals; PFN is purchased from 1-Material; PEIE is purchased from Sigma-Aldrich; PTAA is purchased from Merck.
Described material has chemical structural formula as follows:
Before specifically describing embodiments of the invention, the cleaning of paper transparent conduction base sheet (transparency electrode) and preprocess method and battery testing method.
The cleaning of transparent conduction base sheet and preprocess method: substrate is used glass cleaner, deionized water, acetone, isopropyl alcohol ultrasonic cleaning 20 minutes successively, then dries up with nitrogen; Afterwards, substrate is processed 10 minutes with UV ozone cleaning machine, further removes the residual organic matter of substrate surface, contributes to form uniform hole transmission layer or electric transmission layer film.
Battery testing method: light source is the 3A level solar simulator (Newport, Model91159A) based on xenon lamp, light intensity is proofreaied and correct (AM1.5G, 100mW/cm with standard silicon solar cell
2).Keithley2420 source table test for current-voltage curve.Battery testing at room temperature carries out in air.
Below in conjunction with specific embodiment, the present invention will be further described.
Preparation ITO/PEDOT:PSS/CH
3nH
3pbI
3-xcl
x/ OQBMF/Al perovskite solar cell
First by PEDOT:PSS (Clevios
tMp VP AI4083) be spun on pretreated ito glass surface with 2500rpm rotating speed, in air, 100 DEG C of heating 50min, obtain the PEDOT:PSS film that 50nm is thick; The CH that is 3:1 by mol ratio
3nH
3i and PbCl
2mixed dissolution, in DMF, obtains the solution that concentration is 51wt%, in glove box, is spun on PEDOT:PSS film with 4500rpm rotating speed, and 140 DEG C of heating 30min, obtain 230nm brownish black CH
3nH
3pbI
3-xcl
xfilm; OQBMF is dissolved in to chlorobenzene or other solvent obtains the solution that concentration is 30mg/mL, is spun on CH with 4000rpm rotating speed
3nH
3pbI
3-xcl
xon film, obtain 57nm OQBMF film; At high vacuum (<10
-4pa), under, evaporation 100nm aluminium electrode, completes battery preparation.After tested, battery efficiency is 12.5%.
Preparation ITO/PEDOT:PSS/CH
3nH
3pbI
3-xcl
x/ PC
61bM/Al perovskite solar cell
First by PEDOT:PSS (Clevios
tMp VP AI4083) be spun on pretreated ito glass surface with 2000rpm rotating speed, in air, 120 DEG C of heating 30min, obtain the PEDOT:PSS film that 57nm is thick; The CH that is 3.2:1 by mol ratio
3nH
3i and PbCl
2mixed dissolution, in DMF, obtains the solution that concentration is 40wt%, in glove box, is spun on PEDOT:PSS film with 1000rpm rotating speed, and 120 DEG C of heating 45min, obtain 460nm brownish black CH
3nH
3pbI
3-xcl
xfilm; By PC
61bM is dissolved in chlorobenzene or other solvent obtains the solution that concentration is 20mg/mL, is spun on CH with 1500rpm rotating speed
3nH
3pbI
3-xcl
xon film, obtain 40nm PC
61bM film; At high vacuum (<10
-4pa), under, evaporation 100nm aluminium electrode, completes battery preparation.After tested, battery efficiency is 10.8%.
Preparation ITO/PEDOT:PSS/CH
3nH
3pbI
3-xcl
x/ PC
61bM/Al perovskite solar cell
First by PEDOT:PSS (Clevios
tMp VP AI4083) be spun on pretreated ito glass surface with 3000rpm rotating speed, in air, 160 DEG C of heating 25min, obtain the PEDOT:PSS film that 41nm is thick; The CH that is 3.1:1 by mol ratio
3nH
3i and PbCl
2mixed dissolution, in DMF, obtains the solution that concentration is 45wt%, in glove box, is spun on PEDOT:PSS film with 2000rpm rotating speed, and 115 DEG C of heating 80min, obtain 360nm brownish black CH
3nH
3pbI
3-xcl
xfilm; By PC
61bM is dissolved in chlorobenzene or other solvent obtains the solution that concentration is 10mg/mL, is spun on CH with 800rpm rotating speed
3nH
3pbI
3-xcl
xon film, obtain 45nm PC
61bM film; At high vacuum (<10
-4pa), under, evaporation 150nm aluminium electrode, completes battery preparation.After tested, battery efficiency is 11.7%.
Preparation ITO/PEDOT:PSS/CH
3nH
3pbI
3-xcl
x/ OQMF/Al perovskite solar cell
First by PEDOT:PSS (Clevios
tMp VP AI4083) be spun on pretreated ito glass surface with 4500rpm rotating speed, in air, 170 DEG C of heating 30min, obtain the PEDOT:PSS film that 30nm is thick; The CH that is 3:1 by mol ratio
3nH
3i and PbCl
2mixed dissolution, in DMF, obtains the solution that concentration is 48wt%, in glove box, is spun on PEDOT:PSS film with 3500rpm rotating speed, and 130 DEG C of heating 80min, obtain 420nm brownish black CH
3nH
3pbI
3-xcl
xfilm; OQMF is dissolved in to chlorobenzene or other solvent obtains the solution that concentration is 27mg/mL, is spun on CH with 1500rpm rotating speed
3nH
3pbI
3-xcl
xon film, obtain 42nm OQMF film; At high vacuum (<10
-4pa), under, evaporation 150nm aluminium electrode, completes battery preparation.After tested, battery efficiency is 13.3%.
Preparation ITO/ZnO/CH
3nH
3pbI
3/ P3HT/Ag perovskite solar cell
0.3g bis-water zinc acetates and 60 μ L monoethanolamines are added in 3mL EGME to stirring and dissolving.Be spun on pretreated ito glass surface with 3500rpm rotating speed, in air, 180 DEG C of heating 40min, obtain the ZnO film that 35nm is thick.The lead iodide that is 460mg/mL by concentration (purchased from Sigma-Aldrich) DMF solution is spun on ZnO film with 4000rpm, and 70 DEG C are heated 20min, are then immersed in the CH of 10mg/mL
3nH
3in I aqueous isopropanol, after 30s, take out, 70 DEG C of heating 20min, obtain CH
3nH
3pbI
3film.P3HT is dissolved in to chlorobenzene or other solvent obtains the solution that concentration is 25mg/mL, is spun on CH with 2000rpm rotating speed
3nH
3pbI
3on film, obtain 90nm P3HT film.At high vacuum (<10
-4pa), under, evaporation 100nm silver electrode, completes battery preparation.After tested, battery efficiency is 13.5%.
Embodiment 6
Preparation ITO/ZnO/CH
3nH
3pbI
3/ PTAA/Ag perovskite solar cell
0.2g bis-water zinc acetates and 40 μ L monoethanolamines are added in 2mL EGME to stirring and dissolving.Be spun on pretreated ito glass surface with 2800rpm rotating speed, in air, 220 DEG C of heating 30min, obtain the ZnO film that 34nm is thick.The lead iodide that is 400mg/mL by concentration (purchased from Sigma-Aldrich) DMF solution is spun on ZnO film with 3000rpm, and 80 DEG C are heated 20min, are then immersed in the CH of 15mg/mL
3nH
3in I aqueous isopropanol, after 2min, take out, 100 DEG C of heating 20min, obtain CH
3nH
3pbI
3film.PTAA is dissolved in to chlorobenzene or other solvent obtains the solution that concentration is 15mg/mL, is spun on CH with 1100rpm rotating speed
3nH
3pbI
3on film, obtain 55nm PTAA film.At high vacuum (<10
-4pa), under, evaporation 110nm silver electrode, completes battery preparation.After tested, battery efficiency is 12.7%.
Embodiment 7
Preparation ITO/TiO
2/ CH
3nH
3pbI
3-xcl
x/ P3HT/Ag perovskite solar cell
The hydrochloric acid of the titanium tetraisopropylate of 0.36mL and 0.035mL2M is added in 5mL isopropyl alcohol, stirs and within 1 hour, obtain TiO 2 precursor.Be spun on pretreated ito glass surface with 3000rpm rotating speed, in air, 450 DEG C of heating 30min, obtain the TiO that 40nm is thick
2film.The CH that is 3:1 by mol ratio
3nH
3i and PbCl
2mixed dissolution, in DMF, obtains the solution that concentration is 45wt%, in glove box, is spun on TiO with 3000rpm rotating speed
2on film, 120 DEG C of heating 50min, obtain 400nm brownish black CH
3nH
3pbI
3-xcl
xfilm.P3HT is dissolved in to chlorobenzene or other solvent obtains the solution that concentration is 22mg/mL, is spun on CH with 1300rpm rotating speed
3nH
3pbI
3-xcl
xon film, obtain 54nm P3HT film.At high vacuum (<10
-4pa), under, evaporation 100nm silver electrode, completes battery preparation.After tested, battery efficiency is 12.4%.
Embodiment 8
Preparation ITO/TiO
2/ CH
3nH
3pbI
3-xcl
x/ PThTPTI/Ag perovskite solar cell
The hydrochloric acid of the titanium tetraisopropylate of 0.36mL and 0.035mL2M is added in 5mL isopropyl alcohol, stirs and within 1 hour, obtain TiO 2 precursor.Be spun on pretreated ito glass surface with 4000rpm rotating speed, in air, 500 DEG C of heating 40min, obtain the TiO that 32nm is thick
2film.The CH that is 3.1:1 by mol ratio
3nH
3i and PbCl
2mixed dissolution, in DMF, obtains the solution that concentration is 45wt%, in glove box, is spun on TiO with 2500rpm rotating speed
2on film, 90 DEG C of heating 2h, obtain 420nm brownish black CH
3nH
3pbI
3-xcl
xfilm.PThTPTI is dissolved in to chlorobenzene or other solvent obtains the solution that concentration is 15mg/mL, is spun on CH with 1200rpm rotating speed
3nH
3pbI
3-xcl
xon film, obtain 60nm PThTPTI film.At high vacuum (<10
-4pa), under, evaporation 120nm silver electrode, completes battery preparation.After tested, battery efficiency is 13.9%.
The molecular structure of perovskite light-absorption layer, hole transmission layer and the electron transfer layer of the present invention to perovskite solar cell and preparation are all optimized, and comprise the thickness of every layer film of spin coating rotating speed, heat treatment temperature, time and formation.By iodate methylamine CH
3nH
3i and lead halide PbB
2or tin halides SnB
2be dissolved in high polar solvent (gamma-butyrolacton, DMF DMF, dimethyl sulfoxide (DMSO) DMSO or mixed solvent etc.) and prepare perovskite precursor solution, spin coating, heating, obtain perovskite light-absorption layer.CH
3nH
3i and PbB
2(or SnB
2) parameter such as mol ratio, solvent, light-absorption layer thickness, heat treatment temperature and time etc. all carried out system optimization.Hole transmission layer and electron transfer layer are optimized by Molecular regulator structure, solvent, thickness, nanotopography, series resistance etc.
Perovskite solar battery structure provided by the invention is simple, and preparation technology is simple and easy to do, and production cost is low, and excellent performance can carry out large area preparation, realizes the industrialization of perovskite solar cell.
Applicant's statement, the present invention illustrates detailed features of the present invention and method detailed by above-described embodiment, but the present invention is not limited to above-mentioned detailed features and method detailed, do not mean that the present invention must rely on above-mentioned detailed features and method detailed could be implemented.Person of ordinary skill in the field should understand, any improvement in the present invention is selected the selection of the equivalence replacement of component and the interpolation of auxiliary element, concrete mode etc., within all dropping on protection scope of the present invention and open scope to the present invention.
Claims (10)
1. a perovskite solar cell, comprise transparency electrode, the hole transmission layer forming in described transparency electrode, the perovskite light-absorption layer forming on described hole transmission layer, the electron transfer layer forming on described perovskite light-absorption layer and the metal electrode forming on described electron transfer layer, or comprise transparency electrode, the electron transfer layer forming in described transparency electrode, the perovskite light-absorption layer forming on described electron transfer layer, the hole transmission layer forming on described perovskite light-absorption layer and the metal electrode forming on described hole transmission layer, wherein said hole transmission layer comprises PEDOT:PSS, P3HT, PTAA, PThTPTI, at least one in metal oxide and graphene oxide, described electron transfer layer comprises 58 π-electronics fullerene PCBM, 56 π-electronics fullerene OQMF, 54 π-electronics fullerene OQBMF, PFN, PEIE, ZnO, TiO
2, doping or modify ZnO or TiO
2in at least one.
2. perovskite solar cell according to claim 1, is characterized in that, described metal oxide is MoO
x, NiO, V
2o
5and/or WO
3, wherein x=2~3;
Preferably, described hole transmission layer comprises at least one in PEDOT:PSS, P3HT, PTAA and PThTPTI.
3. perovskite solar cell according to claim 1 and 2, is characterized in that, the ZnO of described doping or modification or TiO
2for the ZnO of Al doping ZnO, PFN or PEIE modification, the ZnO of fullerene derivate modification and/or the TiO that various resilient coating is modified
2;
Preferably, described electron transfer layer comprises 58 π-electronics fullerene PCBM, 56 π-electronics fullerene OQMF, 54 π-electronics fullerene OQBMF, ZnO and TiO
2in at least one, at least one in more preferably 58 π-electronics fullerene PCBM, 56 π-electronics fullerene OQMF and 54 π-electronics fullerene OQBMF.
4. according to the perovskite solar cell described in claim 1-3 any one, it is characterized in that, described perovskite light-absorption layer comprises CH
3nH
3mI
3-xb
x, wherein x=0~3, M is selected from Pb or Sn, and B is selected from I, Cl or Br.
5. according to the perovskite solar cell described in claim 1-4 any one, it is characterized in that, described perovskite solar cell comprises transparency electrode, the hole transmission layer forming in described transparency electrode, the perovskite light-absorption layer forming on described hole transmission layer, the electron transfer layer forming on described perovskite light-absorption layer and the metal electrode that forms on described electron transfer layer; Wherein said hole transmission layer comprises at least one in PEDOT:PSS, metal oxide and graphene oxide, preferably PEDOT:PSS; Described electron transfer layer comprises at least one in 58 π-electronics fullerene PCBM, 56 π-electronics fullerene OQMF, 54 π-electronics fullerene OQBMF, PFN, PEIE and ZnO, at least one in preferably 58 π-electronics fullerene PCBM, 56 π-electronics fullerene OQMF and 54 π-electronics fullerene OQBMF; Described perovskite light-absorption layer comprises CH
3nH
3mI
3-xb
x, wherein x=0~3, M is selected from Pb or Sn, and B is selected from I, Cl or Br.
6. according to the perovskite solar cell described in claim 1-4 any one, it is characterized in that, described perovskite solar cell comprises transparency electrode, the electron transfer layer forming in described transparency electrode, the perovskite light-absorption layer forming on described electron transfer layer, the hole transmission layer forming on described perovskite light-absorption layer and the metal electrode that forms on described hole transmission layer; Wherein said hole transmission layer comprises at least one in P3HT, PTAA and PThTPTI; Described electron transfer layer comprises ZnO, TiO
2, the TiO that modifies of ZnO that Al doping ZnO, PFN or PEIE modify, ZnO that fullerene derivate is modified and/or various resilient coating
2in at least one; Described perovskite light-absorption layer comprises CH
3nH
3mI
3-xb
x, wherein x=0~3, M is selected from Pb or Sn, and B is selected from I, Cl or Br.
7. according to the perovskite solar cell described in claim 1-6 any one, it is characterized in that, described transparency electrode is the substrate of glass that tin indium oxide or fluorine-doped tin oxide cover, or PET flexible substrates;
Preferably, described metal electrode is gold, silver or aluminium electrode.
8. a method of preparing the perovskite solar cell described in claim 1-7 any one, comprises the steps:
(1) material of hole transmission layer is spun on to transparency electrode, at 100~170 DEG C, heats 10~50min, obtain the hole transport layer film that 15~60nm is thick;
(2) material of perovskite light-absorption layer is spun on described hole transport layer film, at 70~160 DEG C, heats 15min~2h, obtain the perovskite light-absorption layer film that 100~600nm is thick;
(3) material of electron transfer layer is spun on described perovskite light-absorption layer film, obtains the electric transmission layer film that 30~150nm is thick;
(4), under vacuum condition, evaporation 60~400nm metal electrode, makes described perovskite solar cell.
9. a method of preparing the perovskite solar cell described in claim 1-7 any one, comprises the steps:
(1) material of electron transfer layer is spun on to transparency electrode, at 150~510 DEG C, heats 20~80min, obtain the electric transmission layer film that 15~60nm is thick;
(2) material of perovskite light-absorption layer is spun on described electric transmission layer film, or after first lead iodide solution being spun on and being then soaked on described electric transmission layer film and taking out in iodate methylamine solution; At 70~160 DEG C, heat 15min~2h again, obtain the perovskite light-absorption layer film that 100~600nm is thick;
(3) material of hole transmission layer is spun on described perovskite light-absorption layer film, obtains the hole transport layer film that 30~250nm is thick;
(4), under vacuum condition, evaporation 60~300nm metal electrode, makes described perovskite solar cell.
10. method according to claim 8 or claim 9, is characterized in that, the rotating speed of described spin coating is all less than 5000rpm, preferably 500-4500rpm, more preferably 1000-4000rpm.
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