CN104201284A - Integrated solar battery based on perovskite solar battery and bulk heterojunction solar battery and preparation method thereof - Google Patents
Integrated solar battery based on perovskite solar battery and bulk heterojunction solar battery and preparation method thereof Download PDFInfo
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- CN104201284A CN104201284A CN201410436893.4A CN201410436893A CN104201284A CN 104201284 A CN104201284 A CN 104201284A CN 201410436893 A CN201410436893 A CN 201410436893A CN 104201284 A CN104201284 A CN 104201284A
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- 239000000126 substance Substances 0.000 claims abstract description 44
- 229910052751 metal Inorganic materials 0.000 claims abstract description 16
- 239000002184 metal Substances 0.000 claims abstract description 16
- 230000005525 hole transport Effects 0.000 claims abstract description 3
- 239000000463 material Substances 0.000 claims description 46
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- 238000000034 method Methods 0.000 claims description 18
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- OYPRJOBELJOOCE-UHFFFAOYSA-N Calcium Chemical compound [Ca] OYPRJOBELJOOCE-UHFFFAOYSA-N 0.000 claims description 10
- 229910052791 calcium Inorganic materials 0.000 claims description 10
- 239000011575 calcium Substances 0.000 claims description 10
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims description 8
- 229910021389 graphene Inorganic materials 0.000 claims description 8
- PQXKHYXIUOZZFA-UHFFFAOYSA-M lithium fluoride Chemical compound [Li+].[F-] PQXKHYXIUOZZFA-UHFFFAOYSA-M 0.000 claims description 8
- 239000000758 substrate Substances 0.000 claims description 8
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- XLOMVQKBTHCTTD-UHFFFAOYSA-N Zinc monoxide Chemical compound [Zn]=O XLOMVQKBTHCTTD-UHFFFAOYSA-N 0.000 claims description 4
- 229910003472 fullerene Inorganic materials 0.000 claims description 4
- 229910000480 nickel oxide Inorganic materials 0.000 claims description 4
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- 230000004888 barrier function Effects 0.000 claims description 3
- 239000002243 precursor Substances 0.000 claims description 3
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- FJDQFPXHSGXQBY-UHFFFAOYSA-L caesium carbonate Chemical compound [Cs+].[Cs+].[O-]C([O-])=O FJDQFPXHSGXQBY-UHFFFAOYSA-L 0.000 claims description 2
- 229910000024 caesium carbonate Inorganic materials 0.000 claims description 2
- 229920000547 conjugated polymer Polymers 0.000 claims description 2
- PCHJSUWPFVWCPO-UHFFFAOYSA-N gold Chemical compound [Au] PCHJSUWPFVWCPO-UHFFFAOYSA-N 0.000 claims description 2
- 229910052737 gold Inorganic materials 0.000 claims description 2
- 239000010931 gold Substances 0.000 claims description 2
- MRNHPUHPBOKKQT-UHFFFAOYSA-N indium;tin;hydrate Chemical compound O.[In].[Sn] MRNHPUHPBOKKQT-UHFFFAOYSA-N 0.000 claims description 2
- 229910052745 lead Inorganic materials 0.000 claims description 2
- 229910044991 metal oxide Inorganic materials 0.000 claims description 2
- 150000004706 metal oxides Chemical class 0.000 claims description 2
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- 239000011787 zinc oxide Substances 0.000 claims description 2
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- MARUHZGHZWCEQU-UHFFFAOYSA-N 5-phenyl-2h-tetrazole Chemical compound C1=CC=CC=C1C1=NNN=N1 MARUHZGHZWCEQU-UHFFFAOYSA-N 0.000 description 1
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- AZSFNTBGCTUQFX-UHFFFAOYSA-N C12=C3C(C4=C5C=6C7=C8C9=C(C%10=6)C6=C%11C=%12C%13=C%14C%11=C9C9=C8C8=C%11C%15=C%16C=%17C(C=%18C%19=C4C7=C8C%15=%18)=C4C7=C8C%15=C%18C%20=C(C=%178)C%16=C8C%11=C9C%14=C8C%20=C%13C%18=C8C9=%12)=C%19C4=C2C7=C2C%15=C8C=4C2=C1C12C3=C5C%10=C3C6=C9C=4C32C1(CCCC(=O)OC)C1=CC=CC=C1 Chemical compound C12=C3C(C4=C5C=6C7=C8C9=C(C%10=6)C6=C%11C=%12C%13=C%14C%11=C9C9=C8C8=C%11C%15=C%16C=%17C(C=%18C%19=C4C7=C8C%15=%18)=C4C7=C8C%15=C%18C%20=C(C=%178)C%16=C8C%11=C9C%14=C8C%20=C%13C%18=C8C9=%12)=C%19C4=C2C7=C2C%15=C8C=4C2=C1C12C3=C5C%10=C3C6=C9C=4C32C1(CCCC(=O)OC)C1=CC=CC=C1 AZSFNTBGCTUQFX-UHFFFAOYSA-N 0.000 description 1
- VEXZGXHMUGYJMC-UHFFFAOYSA-M Chloride anion Chemical compound [Cl-] VEXZGXHMUGYJMC-UHFFFAOYSA-M 0.000 description 1
- 229910001218 Gallium arsenide Inorganic materials 0.000 description 1
- CBENFWSGALASAD-UHFFFAOYSA-N Ozone Chemical compound [O-][O+]=O CBENFWSGALASAD-UHFFFAOYSA-N 0.000 description 1
- 206010070834 Sensitisation Diseases 0.000 description 1
- XUIMIQQOPSSXEZ-UHFFFAOYSA-N Silicon Chemical compound [Si] XUIMIQQOPSSXEZ-UHFFFAOYSA-N 0.000 description 1
- MCEWYIDBDVPMES-UHFFFAOYSA-N [60]pcbm Chemical compound C123C(C4=C5C6=C7C8=C9C%10=C%11C%12=C%13C%14=C%15C%16=C%17C%18=C(C=%19C=%20C%18=C%18C%16=C%13C%13=C%11C9=C9C7=C(C=%20C9=C%13%18)C(C7=%19)=C96)C6=C%11C%17=C%15C%13=C%15C%14=C%12C%12=C%10C%10=C85)=C9C7=C6C2=C%11C%13=C2C%15=C%12C%10=C4C23C1(CCCC(=O)OC)C1=CC=CC=C1 MCEWYIDBDVPMES-UHFFFAOYSA-N 0.000 description 1
- KTSFMFGEAAANTF-UHFFFAOYSA-N [Cu].[Se].[Se].[In] Chemical compound [Cu].[Se].[Se].[In] KTSFMFGEAAANTF-UHFFFAOYSA-N 0.000 description 1
- 239000002253 acid Substances 0.000 description 1
- 235000019270 ammonium chloride Nutrition 0.000 description 1
- 230000015572 biosynthetic process Effects 0.000 description 1
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- 238000004140 cleaning Methods 0.000 description 1
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- 229910052757 nitrogen Inorganic materials 0.000 description 1
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- 229910021420 polycrystalline silicon Inorganic materials 0.000 description 1
- -1 polyethylene terephthalate Polymers 0.000 description 1
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- FHNFHKCVQCLJFQ-UHFFFAOYSA-N xenon atom Chemical compound [Xe] FHNFHKCVQCLJFQ-UHFFFAOYSA-N 0.000 description 1
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- H—ELECTRICITY
- H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
- H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
- H10K30/00—Organic devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation
- H10K30/20—Organic devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation comprising organic-organic junctions, e.g. donor-acceptor junctions
-
- H—ELECTRICITY
- H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
- H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
- H10K85/00—Organic materials used in the body or electrodes of devices covered by this subclass
- H10K85/10—Organic polymers or oligomers
- H10K85/111—Organic polymers or oligomers comprising aromatic, heteroaromatic, or aryl chains, e.g. polyaniline, polyphenylene or polyphenylene vinylene
-
- H—ELECTRICITY
- H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
- H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
- H10K85/00—Organic materials used in the body or electrodes of devices covered by this subclass
- H10K85/30—Coordination compounds
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- 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
- Y02E10/549—Organic 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
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- Chemical & Material Sciences (AREA)
- Engineering & Computer Science (AREA)
- Materials Engineering (AREA)
- Inorganic Chemistry (AREA)
- Physics & Mathematics (AREA)
- Electromagnetism (AREA)
- Photovoltaic Devices (AREA)
Abstract
The invention relates to an integrated solar battery based on a perovskite solar battery and a bulk heterojunction solar battery and a preparation method thereof. The integrated solar battery comprises a transparent electrode, a hole transport layer, a perovskite light absorbing layer, an organic substance blending layer, a random hole block layer and a metal electrode in sequence from the bottom to top. Through preparing the perovskite solar battery and the bulk heterojunction solar battery into the integrated battery, the integrated solar battery based on the perovskite solar battery and the bulk heterojunction solar battery overcomes the disadvantages of narrow light absorbing range of the perovskite solar battery and weak visible light region absorption of the narrow-gap bulk heterojunction solar battery, improves the sunlight use range and improves the energy conversion efficiency. The integrated battery has the similar features to a parallel battery, the conversion efficiency is capable of breaking through the theoretical boundary of the energy conversion efficiency of the single-junction solar battery, and the application prospect is good.
Description
Technical field
The present invention relates to solar cell field, relate in particular to a kind of integrated solar cell based on perovskite solar cell and bulk heterojunction solar cell and preparation method thereof.
Background technology
In recent years, energy crisis is more and more serious.Finding novel alternative energy source is mankind's problem demanding prompt solutions.Solar cell, as the important channel that solves energy problem, always is study hotspot.
Solar cell, through the development of more than 60 years, has had a lot of different types.Main bag silica-based solar cell, thin film solar cell (as GaAs, cadmium telluride and Copper Indium Gallium Selenide) and the three generations's solar cell taking dye sensitization, quantum dot, bulk heterojunction solar cell as representative.Although monocrystalline/polycrystalline silicon solar cell is widely applied, but production cost is high, the solar cell of other types because of raw material rareness, the shortcoming such as poisonous, efficiency is low, poor stability is restricted in actual applications, finds novel solar cell and be still the focus of current research.
CH
3nH
3mI
3-xb
xtype perovskite material has been increased to 19.3% less than 5 year energy conversion efficiencies from 3.8% from first Application in 2009 so far solar cell, efficiency has approached silica-based solar cell, production cost is but far below silica-based solar cell, so perovskite solar cell becomes the solar cell that is hopeful to obtain large-scale application most.But along with going deep into of research, perovskite efficiency of solar cell has approached the theoretical efficiency limit, because unijunction efficiency of solar cell is subject to the restriction of the band gap of light absorbent own.Most effective perovskite light absorbent mainly contains CH at present
3nH
3pbI
3and CH
3nH
3pbI
3-xcl
x, both band gap all, more than 1.5eV, this means and can only absorbing wavelength be less than the sunlight of 800nm, so limited the raising of energy conversion efficiency.People are to having carried out large quantity research by changing perovskite light absorbent chemical constituent to obtain more high efficiency, but do not obtain good effect.The light absorbent of bulk heterojunction solar cell is mainly polymer and little molecule, and both relative perovskite light absorbents have band gap easily to regulate by changing chemical composition and molecular structure.The narrow organic material of band gap can absorb the more sunlight of wide region, but short light absorption is not so good as perovskite material to wavelength.If narrow band gap organic material can be combined with perovskite material, may obtain higher energy conversion efficiency.
Do not obtain good effect owing to changing perovskite light absorbent chemical constituent, the important channel of improving perovskite efficiency of solar cell is exactly development of new device architecture, exploitation can be widened the new device structure of perovskite solar cell light abstraction width, to improving perovskite efficiency of solar cell, and then realize industrialization, significant.
Summary of the invention
The present invention is directed to the narrow problem of perovskite solar cell light abstraction width, a kind of new device structure of widening perovskite solar cell light abstraction width is proposed, by by integrated to perovskite solar cell and narrow band gap bulk heterojunction solar cell, more than perovskite solar cell light abstraction width can being widened to 950nm from 800nm, improve battery short circuit electric current and energy conversion efficiency.This new device structure has the feature of batteries in parallel connection, and energy conversion efficiency is not subject to the restriction of the unijunction solar cell theoretical efficiency limit.The present invention also provides the method for preparing this integrated battery in addition, and described method is simple, has good application prospect.
In order to achieve the above object, the present invention has adopted following technical scheme:
A kind of integrated solar cell based on perovskite solar cell and bulk heterojunction solar cell, it is characterized in that, described integrated solar cell comprises transparency electrode, hole transmission layer, perovskite light-absorption layer, organic substance blended layer, optionally hole blocking layer and metal electrode from bottom to top successively, wherein, described organic substance blended layer refers to the hybrid films of bulk heterojunction solar cell donor material and acceptor material.
; a kind of integrated solar cell based on perovskite solar cell and bulk heterojunction solar cell; it comprises transparency electrode, the hole transmission layer forming in transparency electrode, the perovskite light-absorption layer forming on hole transmission layer, the organic substance blended layer forming on perovskite light-absorption layer, the hole blocking layer forming in organic substance blended layer and the metal electrode forming on hole blocking layer from bottom to top successively; wherein, described organic substance blended layer refers to the hybrid films of bulk heterojunction solar cell donor material and acceptor material;
Or,
A kind of integrated solar cell based on perovskite solar cell and bulk heterojunction solar cell, it comprises transparency electrode, the hole transmission layer forming in transparency electrode, the perovskite light-absorption layer forming on hole transmission layer, the organic substance blended layer forming on perovskite light-absorption layer, the metal electrode forming in organic substance blended layer from bottom to top successively, wherein, described organic substance blended layer refers to the hybrid films of bulk heterojunction solar cell donor material and acceptor material.
Preferably, the thickness of described perovskite light-absorption layer is 100～500nm, for example 140nm, 180nm, 220nm, 260nm, 300nm, 340nm, 380nm, 420nm or 460nm.The beneficial effect that described perovskite light-absorption layer produces is: the sunlight that absorbing wavelength is shorter, can make battery have higher energy conversion efficiency.
The thickness of described organic substance blended layer is 30～200nm, for example 40nm, 60nm, 80nm, 100nm, 120nm, 140nm, 160nm or 180nm.In organic substance blended layer, the ratio of donor material and acceptor material (mass ratio) is 1:0.5～1:6, for example 1:0.5,1:0.8,1:1,1:1.5,1:2,1:2.5,1:3,1:4,1:5,1:6.The beneficial effect that described organic substance blended layer produces is: the sunlight that absorbing wavelength is grown, make up the narrow shortcoming of perovskite material light abstraction width, and improve energy conversion efficiency.
The thickness of described hole blocking layer is 0～20nm.The beneficial effect that described hole blocking layer produces is: blocking hole when high efficiency of transmission electronics, reduce the compound of electronics and hole, and improve battery performance.
The thickness of metal electrode is 70～390nm.The beneficial effect that described metal electrode produces is that, in economizing in raw materials, the conductivity of guarantee electrode, makes battery have higher energy conversion efficiency.
According to integrated solar cell of the present invention, described transparency electrode comprises any one in substrate of glass that tin indium oxide (ITO), fluorine-doped tin oxide (FTO) cover, substrate of glass or PET (PETG, polyethylene terephthalate) flexible substrates that aluminium-doped zinc oxide (AZO) covers.
According to integrated solar cell of the present invention, the material of described hole transmission layer comprises PEDOT:PSS (Poly (3,4-ethylenedioxythiophene)-polystyrene sulfonate, poly-(3,4-ethylene dioxythiophene)-polystyrolsulfon acid), graphene oxide, metal oxide NiO
xor VO
xin the mixture of any one or at least two kinds, x=1～3, for example 2, preferably PEDOT:PSS, graphene oxide or nickel oxide NiO
xin the mixture of any one or at least two kinds, x=1～3, for example 2.
According to integrated solar cell of the present invention, the material of described perovskite light-absorption layer is 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, preferably CH
3nH
3pbI
3, CH
3nH
3pbI
3-xcl
xor CH
3nH
3pbI
2the mixture of any one in Br or at least two kinds.
The material of exemplary perovskite light-absorption layer is: CH
3nH
3pbI
3-xbr
x, CH
3nH
3snI
3-xbr
x, CH
3nH
3pbI
3-xcl
x, CH
3nH
3snI
3-xcl
x.
According to integrated solar cell of the present invention, described organic substance blended layer refers to the hybrid films of bulk heterojunction solar cell donor material and acceptor material.Described donor material is to be applied to conjugated polymer that the optical band gap of bulk heterojunction solar cell is less than 1.5eV or/and little molecule, preferably PDPP3T (Poly[{2, 5-bis (2-hexyldecyl)-2, 3, 5, 6-tetrahydro-3, 6-dioxopyrrolo[3, 4-c] pyrrole-1, 4-diyl}-alt-{[2, 2':5', 2 " terthiophene]-5, 5 " diyl}]), PMDPP3T (poly[[2, 5-bis (2-hexyldecyl-2, 3, 5, 6-tetrahydro-3, 6-dioxopyrrolo[3, 4-c] pyrrole-1, 4-diyl]-alt-[3 ', 3 " dimethyl-2, 2 ': 5 ', 2 " terthiophene]-5, 5 " diyl]), PDPPBTT (coalescence two thiophene pyrroles pyrroledione-thiophene) or PDTP-DFBT (poly[2, 6-(4, 4-bis-(2-ethylhexyl)-4H-cyclopenta[2, 1-b, 3,4-b0]-dithiophene)-alt-4,7-(2,1,3-difluorobenzothiadiazole)) in the mixture of any one or at least two kinds.
Described acceptor material is the mixture of any one fullerene derivate or at least two kinds of fullerene derivates, preferably PC
61bM ([6,6]-phenyl-C61-butyric acid methyl ester, [6,6]-phenyl-C61-methyl butyrate) is or/and PC
71bM ([6,6]-phenyl-C71-butyric acid methyl ester, [6,6]-phenyl-C71-methyl butyrate).
According to integrated solar cell of the present invention, the material of described hole blocking layer comprises the mixture of any one or at least two kinds in calcium, lithium fluoride or cesium carbonate, and preferably calcium is or/and lithium fluoride.
According to integrated solar cell of the present invention, described metal electrode is aluminium, gold or silver electrode.
Two of object of the present invention is to provide a kind of method of preparing the above-mentioned integrated solar cell based on perovskite solar cell and bulk heterojunction solar cell, comprises the steps:
(1) material of hole transmission layer is spun on to transparency electrode, obtains hole transmission layer;
(2) perovskite precursor solution is spun on hole transport layer film, at 80～130 DEG C, heats 0～2h, obtain perovskite light-absorption layer;
(3) mixed solution of bulk heterojunction solar cell donor material and acceptor material is spun on described perovskite light-absorption layer, obtains organic substance blended layer;
(4) optionally, under vacuum condition, evaporation hole blocking layer;
(5) evaporation metal electrode, makes the integrated solar cell based on perovskite solar cell and bulk heterojunction solar cell.
Preferably, described heating-up temperature is between 90～120 DEG C, and described heating time is between 1min～60min.Adopt the beneficial effect that this heating-up temperature and heating time produce to be: to make the crystallization of perovskite light-absorption layer better, can make battery have higher energy conversion efficiency.
In said method, step (2) heating-up temperature can be 81 DEG C, 83 DEG C, 85 DEG C, 88 DEG C, 90 DEG C, 94 DEG C, 98 DEG C, 100 DEG C, 105 DEG C, 110 DEG C, 115 DEG C, 120 DEG C, 125 DEG C or 130 DEG C, and can be 0s, 30s, 60s, 8min, 15min, 30min, 60min or 120min heating time.
The thickness of the perovskite light-absorption layer forming is 100～500nm, for example 100nm, 150nm, 200nm, 300nm, 350nm, 450nm or 500nm.
The thickness of the organic substance blended layer that step (3) forms is 30～200nm, for example 35nm, 40nm, 50nm, 70nm, 100nm, 120nm, 130nm, 140nm, 160nm or 200nm.In organic substance blended layer, the ratio of donor material and acceptor material (mass ratio) is 1:0.5～1:6, for example 1:0.5,1:0.8,1:1,1:1.5,1:2,1:2.5,1:3,1:4,1:5,1:6.
The hole barrier layer thickness that step (4) evaporation forms is 0～20nm, for example 0nm, 0.5nm, 1nm, 20nm, 5nm, 15nm or 20nm.
The thickness of metal electrode is 70～390nm, for example, can be 70nm, 80nm, 90nm, 150nm, 200nm, 300nm, 350nm, 380nm or 390nm.
In addition, the present invention proposes a kind of integrated solar cell structure based on perovskite solar cell and bulk heterojunction solar cell first, and preparation condition is studied, to the perovskite light-absorption layer of perovskite solar cell, hole transmission layer, the preparation of organic substance blended layer is all optimized, comprise 90～120 DEG C of heat treatment temperatures, (thickness of perovskite light-absorption layer is 100～500nm to the thickness of every layer film of time 1～60min and formation, the thickness of organic substance blended layer is 30～200nm, hole barrier layer thickness is 0～20nm, the thickness of metal electrode is 70～390nm) and organic substance blended layer in the ratio (in organic substance blended layer, the mass ratio of donor material and acceptor material is 1:0.5～1:6) etc. of material, adopt the preparation condition after optimizing, the battery efficiency obtaining can reach more than 10%.
Compared with the prior art, the present invention has following beneficial effect:
Perovskite efficiency of solar cell is subject to the restriction of perovskite light absorbent band gap, and energy conversion efficiency can not break through the theoretical limit of unijunction efficiency of solar cell.The advantage that the light absorbent of bulk heterojunction solar cell has band gap easily to regulate by changing chemical composition and molecular structure, but low bandgap material to the shorter visible absorption of wavelength a little less than, cause energy conversion efficiency not high.The present invention is by being prepared into integrated battery by perovskite solar cell and bulk heterojunction solar cell, make up the narrower and narrow band gap bulk heterojunction solar cell of perovskite solar cell light abstraction width and absorbed weak shortcoming in visible region, the scope of utilizing that has improved sunlight, has improved energy conversion efficiency.This integrated battery has and the similar feature of batteries in parallel connection, and transformation efficiency is likely broken through the theoretical limit of unijunction solar cell energy conversion efficiency.Described method is simply effective, has good application prospect.
The present invention adopts technique scheme, can obviously widen more than battery light abstraction width widens 950nm from 800nm, and the current density that short-circuits the battery is from less than 14mA/cm
2bring up to 15mA/cm
2above, can realize higher energy conversion efficiency (more than 10%) simultaneously.In addition; organic substance blended layer has protective effect to perovskite light-absorption layer; improve stability test; in not encapsulation situation of battery; battery prepared by commonsense method was placed after 5 hours in air; energy conversion efficiency is only 30% of starting efficiency, and battery prepared by method of the present invention is placed energy conversion efficiency after 5 hours still can reach 80% of starting efficiency.
In addition, the integrated battery of perovskite solar cell of the present invention and bulk heterojunction solar cell adopts lower-cost material and simple preparation technology, has high industrial application value.
Brief description of the drawings
Fig. 1 is perovskite solar cell representative in the embodiment of the present invention and the integrated battery structural representation of bulk heterojunction solar cell.
Description of reference numerals:
1-transparency electrode; 2-hole transmission layer; 3-perovskite light-absorption layer; 4-organic substance blended layer; 5-hole blocking layer; 6-metal electrode.
Embodiment
Further illustrate technical scheme of the present invention below in conjunction with accompanying drawing and by embodiment.
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.
Described material has chemical structural formula as follows:
Before specifically describing embodiments of the invention, preprocess method and the battery testing method of paper transparent conduction base sheet (transparency electrode).
Transparent conduction base sheet 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.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).Keithley 2420 source table tests 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.
Embodiment 1
First by PEDOT:PSS (Clevios
tMp VP AI 4083) be spun on pretreated ito glass surface with 4000rpm rotating speed, in air, 150 DEG C of heating 10min, 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 20wt%, in glove box, is spun on PEDOT:PSS film with 3000rpm rotating speed, and 80 DEG C of heating 120min, obtain 100nm CH
3nH
3pbI
3-xcl
xfilm; By PDPP3T and PC
61bM mixes and is dissolved in chlorobenzene or other solvent obtains the solution of total concentration as 8mg/mL taking mass ratio 1:2, is spun on CH with 1200rpm rotating speed
3nH
3pbI
3-xcl
xon film, obtain 30nm organic substance blended layer; At high vacuum (<10
-4pa) under, evaporation 0.5nm fluoridizes reason and 70nm aluminium electrode, completes battery preparation.After tested, battery efficiency is 11.5%.
Embodiment 2
First by PEDOT:PSS (Clevios
tMp VP AI 4083) be spun on pretreated ito glass surface with 4000rpm rotating speed, in air, 150 DEG C of heating 10min, 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 30wt%, in glove box, is spun on PEDOT:PSS film with 3000rpm rotating speed, and 90 DEG C of heating 90min, obtain 150nm CH
3nH
3pbI
3-xcl
xfilm; By PMDPP3T and PC
61bM mixes and is dissolved in chlorobenzene or other solvent obtains the solution of total concentration as 12mg/mL taking mass ratio 1:1.5, is spun on CH with 1200rpm rotating speed
3nH
3pbI
3-xcl
xon film, obtain 50nm organic substance blended layer; At high vacuum (<10
-4pa) under, evaporation 0.8nm fluoridizes reason and 100nm aluminium electrode, completes battery preparation.After tested, battery efficiency is 11.1%.
Embodiment 3
First by PEDOT:PSS (Clevios
tMp VP AI 4083) be spun on pretreated ito glass surface with 4000rpm rotating speed, in air, 150 DEG C of heating 10min, 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 50wt%, in glove box, is spun on PEDOT:PSS film with 3000rpm rotating speed, and 100 DEG C of heating 60min, obtain 400nm CH
3nH
3pbI
3-xcl
xfilm; By PMDPP3T and PC
71bM mixes and is dissolved in chlorobenzene or other solvent obtains the solution of total concentration as 20mg/mL taking mass ratio 1:4, is spun on CH with 1200rpm rotating speed
3nH
3pbI
3-xcl
xon film, obtain 120nm organic substance blended layer; At high vacuum (<10
-4pa), under, evaporation 10nm calcium and 150nm aluminium electrode, complete battery preparation.After tested, battery efficiency is 12.2%.
Embodiment 4
First by PEDOT:PSS (Clevios
tMp VP AI 4083) be spun on pretreated ito glass surface with 4000rpm rotating speed, in air, 150 DEG C of heating 10min, 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 55wt%, in glove box, is spun on PEDOT:PSS film with 2000rpm rotating speed, and 120 DEG C of heating 50min, obtain 500nm CH
3nH
3pbI
3-xcl
xfilm; By PMDPP3T and PC
61bM mixes and is dissolved in chlorobenzene or other solvent obtains the solution of total concentration as 30mg/mL taking mass ratio 1:5, is spun on CH with 1000rpm rotating speed
3nH
3pbI
3-xcl
xon film, obtain 200nm organic substance blended layer; At high vacuum (<10
-4pa), under, evaporation 20nm calcium and 300nm aluminium electrode, complete battery preparation.After tested, battery efficiency is 10.2%.
Embodiment 5
First by PEDOT:PSS (Clevios
tMp VP AI 4083) be spun on pretreated ito glass surface with 4000rpm rotating speed, in air, 150 DEG C of heating 10min, obtain the PEDOT:PSS film that 30nm is thick; The CH that is 1:1 by mol ratio
3nH
3i and PbI
2mixed dissolution, in DMF, obtains the solution that concentration is 45wt%, in glove box, is spun on PEDOT:PSS film with 3000rpm rotating speed, in the time that the spin coating time is 6s, drips toluene, makes the rapid crystallization of perovskite light-absorption layer, and 100 DEG C of heating 20min, obtain 400nmCH
3nH
3pbI
3film; By PDTP-DFBT and PC
61bM mixes and is dissolved in chlorobenzene or other solvent obtains the solution of total concentration as 25mg/mL taking mass ratio 1:3, is spun on CH with 1000rpm rotating speed
3nH
3pbI
3on film, obtain 150nm organic substance blended layer; At high vacuum (<10
-4pa), under, evaporation 10nm calcium and 300nm aluminium electrode, complete battery preparation.After tested, battery efficiency is 11.6%.
Embodiment 6
First by PEDOT:PSS (Clevios
tMp VP AI 4083) be spun on pretreated ito glass surface with 4000rpm rotating speed, in air, 150 DEG C of heating 10min, obtain the PEDOT:PSS film that 30nm is thick; The CH that is 1:1 by mol ratio
3nH
3i and PbI
2mixed dissolution is in the mixed solvent of DMF and DMSO, DMF and DMSO volume ratio are 7:3, obtain the solution that concentration is 45wt%, in glove box, be spun on PEDOT:PSS film with 3000rpm rotating speed, in the time that the spin coating time is 6s, toluene is dropped on the film rotating, make the rapid crystallization of perovskite light-absorption layer, 100 DEG C of heating 10min, obtain 350nmCH
3nH
3pbI
3film; By PDTP-DFBT and PC
61bM mixes and is dissolved in chlorobenzene or other solvent obtains the solution of total concentration as 20mg/mL taking mass ratio 1:3, is spun on CH with 1000rpm rotating speed
3nH
3pbI
3on film, obtain 120nm organic substance blended layer; At high vacuum (<10
-4pa), under, evaporation 10nm calcium and 400nm aluminium electrode, complete battery preparation.After tested, battery efficiency is 11.5%.
Embodiment 7
First by PEDOT:PSS (Clevios
tMp VP AI 4083) be spun on pretreated ito glass surface with 4000rpm rotating speed, in air, 150 DEG C of heating 10min, obtain the PEDOT:PSS film that 30nm is thick; The CH that is 1:1 by mol ratio
3nH
3i and PbBr
2mixed dissolution is in the mixed solvent of DMF and DMSO, DMF and DMSO volume ratio are 7:3, obtain the solution that concentration is 25wt%, by chloride leach in above-mentioned solution, making ammonium chloride concentration is that 17mg/mL is spun on PEDOT:PSS film with 3000rpm rotating speed in glove box, 100 DEG C of heating 15s, obtain 150nm CH
3nH
3pbI
2br film; By PDPPBTT and PC
71bM mixes and is dissolved in chlorobenzene or other solvent obtains the solution of total concentration as 20mg/mL taking mass ratio 1:3, is spun on CH with 1000rpm rotating speed
3nH
3pbI
2on Br film, obtain 120nm organic substance blended layer; At high vacuum (<10
-4pa), under, evaporation 10nm calcium and 200nm aluminium electrode, complete battery preparation.After tested, battery efficiency is 11.3%.
Embodiment 8
First graphene oxide solution is spun on to pretreated ito glass surface with 4000rpm rotating speed, obtains the graphene oxide 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 50wt%, in glove box, is spun on graphene oxide film with 3000rpm rotating speed, and 130 DEG C of heating 20min obtain 300nm CH
3nH
3pbI
3-xcl
xfilm; By PDPPBTT and PC
71bM mixes and is dissolved in chlorobenzene or other solvent obtains the solution of total concentration as 15mg/mL taking mass ratio 1:3, is spun on CH with 1000rpm rotating speed
3nH
3pbI
3-xcl
xon film, obtain 100nm organic substance blended layer; At high vacuum (<10
-4pa), under, evaporation 10nm calcium and 150nm aluminium electrode, complete battery preparation.After tested, battery efficiency is 10.1%.
Embodiment 9
First nickel oxide precursor solution is spun on to pretreated ito glass surface with 4000rpm rotating speed, 300 DEG C of heating 30min obtain the nickel oxide film that 40nm 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 40wt%, in glove box, is spun on graphene oxide film with 3000rpm rotating speed, obtains 260nm CH
3nH
3pbI
3-xcl
xfilm, 110 DEG C of heating 40min.By PDPP3T and PC
71bM mixes and is dissolved in chlorobenzene or other solvent obtains the solution of total concentration as 15mg/mL taking mass ratio 1:3, is spun on CH with 1000rpm rotating speed
3nH
3pbI
3-xcl
xon film, obtain 100nm organic substance blended layer; At high vacuum (<10
-4pa), under, evaporation 150nm aluminium electrode, completes battery preparation.After tested, battery efficiency is 9.5%.
Novel 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 industrialization.
Applicant's statement, the present invention illustrates method detailed of the present invention by above-described embodiment, but the present invention is not limited to above-mentioned method detailed, does not mean that the present invention must rely on above-mentioned method detailed and could implement.Person of ordinary skill in the field should understand, any improvement in the present invention, and the selections of the equivalence replacement to the each raw material of product of the present invention and the interpolation of auxiliary element, concrete mode etc., within all dropping on protection scope of the present invention and open scope.
Claims (10)
1. the integrated solar cell based on perovskite solar cell and bulk heterojunction solar cell, it is characterized in that, described integrated solar cell comprises transparency electrode, hole transmission layer, perovskite light-absorption layer, organic substance blended layer, optionally hole blocking layer and metal electrode from bottom to top successively, wherein, described organic substance blended layer refers to the hybrid films of bulk heterojunction solar cell donor material and acceptor material.
2. integrated solar cell as claimed in claim 1, is characterized in that, the thickness of described perovskite light-absorption layer is 100～500nm;
Preferably, the thickness of described organic substance blended layer is 30～200nm;
Preferably, in organic substance blended layer, the mass ratio of donor material and acceptor material is 1:0.5～1:6.
3. integrated solar cell as claimed in claim 1 or 2, is characterized in that, the thickness of described hole blocking layer is 0～20nm;
Preferably, the thickness of metal electrode is 70～390nm.
4. the integrated solar cell as described in one of claim 1-3, is characterized in that, described transparency electrode comprises any one in substrate of glass that tin indium oxide, fluorine-doped tin oxide cover, substrate of glass or PET flexible substrates that aluminium-doped zinc oxide covers;
Preferably, the material of described hole transmission layer comprises PEDOT:PSS, graphene oxide, metal oxide NiO
xor VO
xin the mixture of any one or at least two kinds, x=1～3, preferably PEDOT:PSS, graphene oxide or nickel oxide NiO
xin the mixture of any one or at least two kinds, x=1～3.
5. the integrated solar cell as described in one of claim 1-4, is characterized in that, the material of described perovskite light-absorption layer is 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, preferably CH
3nH
3pbI
3, CH
3nH
3pbI
3-xcl
xor CH
3nH
3pbI
2the mixture of any one in Br or at least two kinds;
Preferably, described donor material be the optical band gap that is applied to bulk heterojunction solar cell be less than 1.5eV conjugated polymer or/and little molecule, the preferably mixture of any one in PDPP3T, PMDPP3T, PDPPBTT or PDTP-DFBT or at least two kinds;
Preferably, described acceptor material is the mixture of any one fullerene derivate or at least two kinds of fullerene derivates, preferably PC
61bM is or/and PC
71bM.
6. the integrated solar cell as described in one of claim 1-5, is characterized in that, the material of described hole blocking layer comprises the mixture of any one or at least two kinds in calcium, lithium fluoride or cesium carbonate, and preferably calcium is or/and lithium fluoride;
Preferably, described metal electrode is aluminium, gold or silver electrode.
7. a method of preparing the described integrated solar cell based on perovskite solar cell and bulk heterojunction solar cell of one of claim 1-6, is characterized in that, described method comprises the steps:
(1) material of hole transmission layer is spun on to transparency electrode, obtains hole transmission layer;
(2) perovskite precursor solution is spun on hole transport layer film, at 80～130 DEG C, heats 0～2h, obtain perovskite light-absorption layer;
(3) mixed solution of bulk heterojunction solar cell donor material and acceptor material is spun on described perovskite light-absorption layer, obtains organic substance blended layer;
(4) optionally, under vacuum condition, evaporation hole blocking layer;
(5) evaporation metal electrode, makes the integrated solar cell based on perovskite solar cell and bulk heterojunction solar cell.
8. method as claimed in claim 7, is characterized in that, step (2) heating-up temperature is 90～120 DEG C, and be 1～60min heating time;
Preferably, the thickness of perovskite light-absorption layer is 100～500nm.
9. method as claimed in claim 7 or 8, is characterized in that, the thickness of the organic substance blended layer that step (3) forms is 30～200nm;
Preferably, in organic substance blended layer, the mass ratio of donor material and acceptor material is 1:0.5～1:6.
10. the method as described in one of claim 7-9, is characterized in that, the hole barrier layer thickness that step (4) evaporation forms is 0～20nm, and the thickness of metal electrode is 70～390nm.
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| HENRY J. SNAITH: "《Perovskites The Emergence of a New Era for Low-Cost, High-Efficiency Solar Cells》", 《J. PHYS. CHEM. LETT.》 * |
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