CN104134752A - Perovskite solar cell and preparation method for thermoplastic carbon counter electrode - Google Patents
Perovskite solar cell and preparation method for thermoplastic carbon counter electrode Download PDFInfo
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- CN104134752A CN104134752A CN201410323037.8A CN201410323037A CN104134752A CN 104134752 A CN104134752 A CN 104134752A CN 201410323037 A CN201410323037 A CN 201410323037A CN 104134752 A CN104134752 A CN 104134752A
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- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 title claims abstract description 174
- 229910052799 carbon Inorganic materials 0.000 title claims abstract description 146
- 238000002360 preparation method Methods 0.000 title claims abstract description 40
- 229920001169 thermoplastic Polymers 0.000 title claims abstract description 36
- 239000004416 thermosoftening plastic Substances 0.000 title abstract description 8
- 239000000758 substrate Substances 0.000 claims abstract description 38
- 239000003575 carbonaceous material Substances 0.000 claims abstract description 28
- 239000003960 organic solvent Substances 0.000 claims abstract description 25
- 239000000463 material Substances 0.000 claims description 36
- 238000000034 method Methods 0.000 claims description 31
- 229920002725 thermoplastic elastomer Polymers 0.000 claims description 22
- 238000007731 hot pressing Methods 0.000 claims description 14
- 229920002689 polyvinyl acetate Polymers 0.000 claims description 13
- 239000011118 polyvinyl acetate Substances 0.000 claims description 13
- 229910002804 graphite Inorganic materials 0.000 claims description 12
- 239000010439 graphite Substances 0.000 claims description 12
- 239000012752 auxiliary agent Substances 0.000 claims description 11
- 239000002184 metal Substances 0.000 claims description 10
- 229910052751 metal Inorganic materials 0.000 claims description 10
- 230000032683 aging Effects 0.000 claims description 8
- 229920005992 thermoplastic resin Polymers 0.000 claims description 7
- 239000001856 Ethyl cellulose Substances 0.000 claims description 6
- ZZSNKZQZMQGXPY-UHFFFAOYSA-N Ethyl cellulose Chemical compound CCOCC1OC(OC)C(OCC)C(OCC)C1OC1C(O)C(O)C(OC)C(CO)O1 ZZSNKZQZMQGXPY-UHFFFAOYSA-N 0.000 claims description 6
- GWEVSGVZZGPLCZ-UHFFFAOYSA-N Titan oxide Chemical compound O=[Ti]=O GWEVSGVZZGPLCZ-UHFFFAOYSA-N 0.000 claims description 6
- 239000006229 carbon black Substances 0.000 claims description 6
- 229920001249 ethyl cellulose Polymers 0.000 claims description 6
- 235000019325 ethyl cellulose Nutrition 0.000 claims description 6
- 239000011521 glass Substances 0.000 claims description 6
- 239000005038 ethylene vinyl acetate Substances 0.000 claims description 5
- 229920001200 poly(ethylene-vinyl acetate) Polymers 0.000 claims description 5
- 239000002041 carbon nanotube Substances 0.000 claims description 4
- 229910021393 carbon nanotube Inorganic materials 0.000 claims description 4
- -1 olefin hydrocarbons Chemical class 0.000 claims description 4
- 229920000049 Carbon (fiber) Polymers 0.000 claims description 3
- RWCCWEUUXYIKHB-UHFFFAOYSA-N benzophenone Chemical compound C=1C=CC=CC=1C(=O)C1=CC=CC=C1 RWCCWEUUXYIKHB-UHFFFAOYSA-N 0.000 claims description 3
- 239000012965 benzophenone Substances 0.000 claims description 3
- 239000004917 carbon fiber Substances 0.000 claims description 3
- 150000001993 dienes Chemical class 0.000 claims description 3
- 229910021389 graphene Inorganic materials 0.000 claims description 3
- 229930195733 hydrocarbon Natural products 0.000 claims description 3
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 claims description 3
- JRZJOMJEPLMPRA-UHFFFAOYSA-N olefin Natural products CCCCCCCC=C JRZJOMJEPLMPRA-UHFFFAOYSA-N 0.000 claims description 3
- 229920002635 polyurethane Polymers 0.000 claims description 3
- 239000004814 polyurethane Substances 0.000 claims description 3
- 229920000036 polyvinylpyrrolidone Polymers 0.000 claims description 3
- 239000001267 polyvinylpyrrolidone Substances 0.000 claims description 3
- 235000013855 polyvinylpyrrolidone Nutrition 0.000 claims description 3
- 125000003011 styrenyl group Chemical class [H]\C(*)=C(/[H])C1=C([H])C([H])=C([H])C([H])=C1[H] 0.000 claims description 3
- 239000004408 titanium dioxide Substances 0.000 claims description 3
- 239000004793 Polystyrene Substances 0.000 claims description 2
- 229920000058 polyacrylate Polymers 0.000 claims description 2
- 229920002223 polystyrene Polymers 0.000 claims description 2
- 238000006243 chemical reaction Methods 0.000 abstract description 26
- 238000001035 drying Methods 0.000 abstract description 3
- 239000003795 chemical substances by application Substances 0.000 abstract 5
- 238000004513 sizing Methods 0.000 abstract 5
- 239000010409 thin film Substances 0.000 abstract 1
- YXFVVABEGXRONW-UHFFFAOYSA-N Toluene Chemical compound CC1=CC=CC=C1 YXFVVABEGXRONW-UHFFFAOYSA-N 0.000 description 18
- 239000010936 titanium Substances 0.000 description 14
- 230000031700 light absorption Effects 0.000 description 13
- XEKOWRVHYACXOJ-UHFFFAOYSA-N Ethyl acetate Chemical compound CCOC(C)=O XEKOWRVHYACXOJ-UHFFFAOYSA-N 0.000 description 12
- 230000005540 biological transmission Effects 0.000 description 12
- 230000027756 respiratory electron transport chain Effects 0.000 description 7
- 229910010413 TiO 2 Inorganic materials 0.000 description 6
- 239000006230 acetylene black Substances 0.000 description 5
- 230000000052 comparative effect Effects 0.000 description 5
- 238000004528 spin coating Methods 0.000 description 5
- 229910000806 Latten Inorganic materials 0.000 description 4
- 239000003153 chemical reaction reagent Substances 0.000 description 4
- ZMXDDKWLCZADIW-UHFFFAOYSA-N dimethylformamide Substances CN(C)C=O ZMXDDKWLCZADIW-UHFFFAOYSA-N 0.000 description 4
- 238000005516 engineering process Methods 0.000 description 4
- 239000002245 particle Substances 0.000 description 4
- 239000002002 slurry Substances 0.000 description 4
- CSCPPACGZOOCGX-UHFFFAOYSA-N Acetone Chemical compound CC(C)=O CSCPPACGZOOCGX-UHFFFAOYSA-N 0.000 description 3
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 description 3
- 239000002250 absorbent Substances 0.000 description 3
- 230000002745 absorbent Effects 0.000 description 3
- 239000011248 coating agent Substances 0.000 description 3
- 238000000576 coating method Methods 0.000 description 3
- 230000000694 effects Effects 0.000 description 3
- 239000002994 raw material Substances 0.000 description 3
- 238000007650 screen-printing Methods 0.000 description 3
- KFZMGEQAYNKOFK-UHFFFAOYSA-N Isopropanol Chemical compound CC(C)O KFZMGEQAYNKOFK-UHFFFAOYSA-N 0.000 description 2
- 238000007605 air drying Methods 0.000 description 2
- 239000013078 crystal Substances 0.000 description 2
- 230000006378 damage Effects 0.000 description 2
- 238000001548 drop coating Methods 0.000 description 2
- 239000007791 liquid phase Substances 0.000 description 2
- 238000004519 manufacturing process Methods 0.000 description 2
- 230000004048 modification Effects 0.000 description 2
- 238000012986 modification Methods 0.000 description 2
- 239000000843 powder Substances 0.000 description 2
- 239000002904 solvent Substances 0.000 description 2
- 238000005507 spraying Methods 0.000 description 2
- 238000003756 stirring Methods 0.000 description 2
- 239000000126 substance Substances 0.000 description 2
- 238000010345 tape casting Methods 0.000 description 2
- XDXWNHPWWKGTKO-UHFFFAOYSA-N 207739-72-8 Chemical compound C1=CC(OC)=CC=C1N(C=1C=C2C3(C4=CC(=CC=C4C2=CC=1)N(C=1C=CC(OC)=CC=1)C=1C=CC(OC)=CC=1)C1=CC(=CC=C1C1=CC=C(C=C13)N(C=1C=CC(OC)=CC=1)C=1C=CC(OC)=CC=1)N(C=1C=CC(OC)=CC=1)C=1C=CC(OC)=CC=1)C1=CC=C(OC)C=C1 XDXWNHPWWKGTKO-UHFFFAOYSA-N 0.000 description 1
- YEJRWHAVMIAJKC-UHFFFAOYSA-N 4-Butyrolactone Chemical compound O=C1CCCO1 YEJRWHAVMIAJKC-UHFFFAOYSA-N 0.000 description 1
- XDTMQSROBMDMFD-UHFFFAOYSA-N Cyclohexane Chemical compound C1CCCCC1 XDTMQSROBMDMFD-UHFFFAOYSA-N 0.000 description 1
- AFCARXCZXQIEQB-UHFFFAOYSA-N N-[3-oxo-3-(2,4,6,7-tetrahydrotriazolo[4,5-c]pyridin-5-yl)propyl]-2-[[3-(trifluoromethoxy)phenyl]methylamino]pyrimidine-5-carboxamide Chemical compound O=C(CCNC(=O)C=1C=NC(=NC=1)NCC1=CC(=CC=C1)OC(F)(F)F)N1CC2=C(CC1)NN=N2 AFCARXCZXQIEQB-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
- 238000010521 absorption reaction Methods 0.000 description 1
- 238000004458 analytical method Methods 0.000 description 1
- 238000000498 ball milling Methods 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- FFBHFFJDDLITSX-UHFFFAOYSA-N benzyl N-[2-hydroxy-4-(3-oxomorpholin-4-yl)phenyl]carbamate Chemical compound OC1=C(NC(=O)OCC2=CC=CC=C2)C=CC(=C1)N1CCOCC1=O FFBHFFJDDLITSX-UHFFFAOYSA-N 0.000 description 1
- 239000002800 charge carrier Substances 0.000 description 1
- 238000010276 construction Methods 0.000 description 1
- 238000001514 detection method Methods 0.000 description 1
- 238000009792 diffusion process Methods 0.000 description 1
- 239000002003 electrode paste Substances 0.000 description 1
- 229920002457 flexible plastic Polymers 0.000 description 1
- 239000010931 gold Substances 0.000 description 1
- 229910052737 gold Inorganic materials 0.000 description 1
- 238000010438 heat treatment Methods 0.000 description 1
- 239000011810 insulating material Substances 0.000 description 1
- 238000002844 melting Methods 0.000 description 1
- 230000008018 melting Effects 0.000 description 1
- 239000012046 mixed solvent Substances 0.000 description 1
- 239000000203 mixture Substances 0.000 description 1
- 230000005693 optoelectronics Effects 0.000 description 1
- 239000002985 plastic film Substances 0.000 description 1
- 229920001343 polytetrafluoroethylene Polymers 0.000 description 1
- 239000004810 polytetrafluoroethylene Substances 0.000 description 1
- 239000004065 semiconductor Substances 0.000 description 1
- 230000008313 sensitization Effects 0.000 description 1
- 238000000926 separation method Methods 0.000 description 1
- 229910052710 silicon Inorganic materials 0.000 description 1
- 239000010703 silicon Substances 0.000 description 1
- 238000001132 ultrasonic dispersion Methods 0.000 description 1
- 238000007738 vacuum evaporation Methods 0.000 description 1
Classifications
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- 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
- H10K85/50—Organic perovskites; Hybrid organic-inorganic perovskites [HOIP], e.g. CH3NH3PbI3
-
- H—ELECTRICITY
- H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
- H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
- H10K71/00—Manufacture or treatment specially adapted for the organic devices covered by this subclass
- H10K71/60—Forming conductive regions or layers, e.g. electrodes
-
- 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
- H10K30/10—Organic devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation comprising heterojunctions between organic semiconductors and inorganic semiconductors
- H10K30/15—Sensitised wide-bandgap semiconductor devices, e.g. dye-sensitised TiO2
-
- 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
- H10K30/10—Organic devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation comprising heterojunctions between organic semiconductors and inorganic semiconductors
- H10K30/15—Sensitised wide-bandgap semiconductor devices, e.g. dye-sensitised TiO2
- H10K30/151—Sensitised wide-bandgap semiconductor devices, e.g. dye-sensitised TiO2 the wide bandgap semiconductor comprising titanium oxide, e.g. TiO2
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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
- H10K30/40—Organic devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation comprising a p-i-n structure, e.g. having a perovskite absorber between p-type and n-type charge transport layers
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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
- H10K30/80—Constructional details
- H10K30/81—Electrodes
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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
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- Physics & Mathematics (AREA)
- Electromagnetism (AREA)
- Engineering & Computer Science (AREA)
- Materials Engineering (AREA)
- Inorganic Chemistry (AREA)
- Manufacturing & Machinery (AREA)
- Photovoltaic Devices (AREA)
Abstract
The invention discloses a perovskite solar cell and a preparation method for a thermoplastic carbon counter electrode. The perovskite solar cell comprises a photo anode and a thermoplastic carbon counter electrode formed on the photo anode. The preparation method for the thermoplastic carbon counter electrode comprises the following steps of: S1, dissolving and dispersing a conductive carbon material and a thermoplastic polymer in an organic solvent to form an uniform carbon sizing agent; S2, providing a substrate, and forming a carbon sizing agent layer on the surface of the substrate by using the carbon sizing agent; and S3, drying the carbon sizing agent layer to remove the organic solvent in the carbon sizing agent layer, thereby obtaining the thermoplastic carbon counter electrode which is of a thin film shape and is conductive. Since a finished product serving as the thermoplastic carbon counter electrode is prepared in advance and the finished product of the thermoplastic carbon counter electrode is directly hot-pressed onto the photo anode, the perovskite solar cell having good flexibility is prepared, the conversion efficiency and the stability of the perovskite solar cell are improved, and the preparation process is simple and is applicable for perovskite solar cells having various structures.
Description
Technical field
The present invention relates to perovskite technical field of solar batteries, relate in particular to a kind of perovskite solar cell and the preparation method of thermoplasticity carbon to electrode thereof.
Background technology
Solar cell is the device that directly light energy conversion is become to electric energy by photoelectric effect or Photochemical effects, is called again photovoltaic cell.Perovskite solar cell (Perovskite Solar Cells) is a comparatively novel at present class solar cell, is mainly to utilize similar ABX
3(A=CH
3nH
3 +deng; B=Pb
2+, Sn
2+deng; X=Cl
-, Br
-, I
-deng) photovoltaic material with perovskite structure realizes opto-electronic conversion, has that manufacture craft is simple, raw material wide material sources, the advantage such as cheap.
The basic structure of perovskite solar cell comprises substrate, transparency electrode, electron transport material, perovskite material light-absorption layer, hole mobile material and electrode.Perovskite solar cell becomes electric energy can be divided into three main process transform light energy: (1) light-absorption layer absorbs the photon of certain energy and produces electron hole pair (exciton); (2) when exciton diffusion is to material interface place, there is separation of charge; (3) electronics enters external circuit along electron transport material through electrode, and hole enters external circuit along hole mobile material through electrode, completes the conversion of luminous energy to electric energy by load.
The parameter that characterizes solar cell properties mainly contains short-circuit current density, open circuit voltage, fill factor, curve factor, photoelectric conversion efficiency.The operating current of the unit light-receiving area of solar cell under short circuit condition is called short-circuit current density (J
sc), the voltage of now battery output is zero.The output voltage of solar cell under open-circuit condition is called open circuit voltage (V
oc), the electric current of now battery output is zero.Fill factor, curve factor (FF) is the peak power output P of unit light-receiving area
maxwith J
scv
ocratio, FF is larger, the performance of solar cell is better.Photoelectric conversion efficiency is the peak power output P of unit light-receiving area
maxsolar energy metric density P with incident
inpercentage, it is an important output characteristic of solar cell, main relevant with characteristic, material character and the environment etc. of device architecture, heterojunction.
In order to realize the industrialization of Ca-Ti ore type solar cell, the problem of current most critical is improve the stability of battery efficiency and reduce the production costs such as technique and raw material.An important component part in Ca-Ti ore type solar battery structure to electrode, in current research, in order to realize high efficiency and the stability of battery, general is all to utilize the method for vacuum evaporation that Precious Metals-Gold is made into electrode, and this is all very expensive undoubtedly on technique and raw material.Conductive carbon material is because having good chemical stability, suitable Fermi level and the advantage such as cheap and easy to get, had at present some seminar successfully material with carbon element has been used in Ca-Ti ore type solar cell on electrode, obtained good effect.
But it should be noted that the current carbon of having reported to electrode normally for the Ca-Ti ore type solar cell without hole transmission layer structure.This is because preparation is when this structure, the general electron transfer layer of first preparing on substrate, on electron transfer layer, apply porous dielectric layer, then carbon pastes is coated on porous dielectric layer, finally apply light-absorption layer material, light-absorption layer material forms through carbon pastes like this porous carbon layer and porous dielectric layer penetrate into electron transfer layer surface, just obtain the structure of electron transfer layer-light-absorption layer-insulating barrier-porous carbon layer, owing to being to be prepared from prior to perovskite light-absorption layer as carbon to the porous carbon layer of electrode, so that cannot add again hole transmission layer, and then what obtain is the Ca-Ti ore type solar cell without hole transmission layer structure.
Although preparation is conducive to the reduction of battery cost without the perovskite solar cell of hole mobile material, this has also embodied the limitation of current carbon to electrode preparation method.And adopt existing carbon to prepare perovskite solar cell to electrode preparation method, battery efficiency is low, poor stability and be difficult to realize cell flexible, therefore, the carbon of the more general perovskite solar cell that makes new advances of exploitation is to electrode preparation method, and the Ca-Ti ore type solar cell that has high battery conversion efficiency and can adapt to different particular types is very necessary.
Summary of the invention
Object of the present invention aims to provide a kind of perovskite solar cell and the preparation method of thermoplasticity carbon to electrode thereof, and battery conversion efficiency is high, good stability and can adapt to the Ca-Ti ore type solar cell of different particular types.
According to an aspect of the present invention, provide the preparation method of a kind of thermoplasticity carbon for perovskite solar cell to electrode, perovskite solar cell comprises light anode and is formed on thermoplasticity carbon on light anode to electrode; Preparation method comprises the following steps: step S1, conductive carbon material and thermoplastic polymer are dissolved and be dispersed in organic solvent, to form uniform carbon pastes; Step S2, provide a substrate, and on the surface of substrate, form carbon pastes layer with carbon pastes; And step S3, dried carbon pulp layer to be to remove the organic solvent in carbon pastes layer, thereby the thermoplasticity carbon that obtains film-form and conduction is to electrode.
Further, the weight ratio of conductive carbon material and thermoplastic polymer is 1:1～10:1.
Further, conductive carbon material is selected from one or more in graphite, carbon black, carbon fiber, carbon nano-tube and Graphene, and preferably, conductive carbon material is graphite and carbon black.
Further, thermoplastic polymer is that fusing point is thermoplastic resin and the thermoplastic elastomer of 50 DEG C～200 DEG C; Preferably, thermoplastic resin is selected from one or more in polyvinyl acetate, ethylene-vinyl acetate copolymer, polyacrylate and polystyrene; Thermoplastic elastomer is selected from one or more in styrene analog thermoplastic elastomer, olefin hydrocarbons thermoplasticity elastic body, dienes thermoplastic elastomer (TPE) and polyurethanes thermoplastic elastomer (TPE).
Further, step S1 also comprises to adding in carbon pastes for adjusting viscosity, preventing the process of aging auxiliary agent; Preferably, auxiliary agent is selected from one or more in ethyl cellulose, polyvinylpyrrolidone, benzophenone and titanium dioxide.
Further, thermoplasticity carbon is 0.005～1mm to the thickness of electrode, is preferably 0.1～0.2mm.
Further, also comprise: step S41, thermoplasticity carbon is peeled off from substrate electrode, then the thermoplasticity carbon of self-supporting form is transferred on light anode electrode.
Further, also comprise: step S42, by thermoplasticity carbon to the electrode substrate global transfer accompanying with it to light anode.
Further, the material of substrate is selected from one or more in metal forming, sheet metal, graphite paper and electro-conductive glass; Alternatively, the thickness of substrate is 0.01～5mm, and the resistivity of base material is 10
-8～10
-3Ω m.
Further, adopt the mode of hot pressing that thermoplasticity carbon is transferred on light anode electrode; Alternatively, the temperature of hot pressing is 100 DEG C～120 DEG C, and pressure is 0.2～0.5MPa, and the time is 20～30 seconds.
According to a further aspect in the invention, provide a kind of perovskite solar cell, comprised that thermoplasticity carbon is to electrode, this thermoplasticity carbon is to adopt above-mentioned any method to be prepared to electrode.
Further, adopt stirring, mode ultrasonic or that grind that conductive carbon material and thermoplastic polymer are disperseed and be dissolved in organic solvent.
Further, adopt drop-coating, knife coating, spraying process, spin-coating method, silk screen print method or czochralski method on the surface of substrate, to form carbon pastes layer.
Apply technical scheme of the present invention, be main body by adopting conductive carbon material and thermoplastic polymer, first be prepared into the thermoplasticity carbon of film-form and conduction to electrode, and then by the mode of hot pressing, thermoplasticity carbon be incorporated on the light anode of perovskite solar cell electrode paste.Preparation method provided by the present invention is due to using previously prepared the completing of material with carbon element film to electrode as thermoplasticity carbon, again finished thermoplastic carbon is pressed onto and on light anode, prepares perovskite solar cell electrode direct heat, inventor is surprised to find, perovskite conversion efficiency of solar cell prepared by the method is high, stability and flexibility good, and preparation technology is simple.
Trace it to its cause, inventor finds because the chemical stability of hole mobile material and organic metal perovskite material is not good, very responsive for solvent contained in carbon pastes, hole mobile material and organic metal perovskite material form in light anode like this hole transmission layer and light-absorption layer are easily destroyed by the organic solvent in carbon pastes, and then affect the stability of battery conversion efficiency and battery use.And the present invention creatively first prepares thermoplasticity carbon to electrode finished product, afterwards thermoplasticity carbon is hot-pressed onto on light anode electrode finished product, in this preparation process, do not relate to carbon pastes solution, avoid the organic solvent in carbon pastes solution to destroy the light-absorption layer in perovskite solar cell and/or hole transmission layer, and then improve the stability of battery conversion efficiency and use, and preparation technology is simple, be suitable for the Ca-Ti ore type solar cell of various structures.
According to the detailed description to the specific embodiment of the invention below, those skilled in the art will understand above-mentioned and other objects, advantage and feature of the present invention more.
Embodiment
While electrode being prepared to perovskite solar cell in order to solve available technology adopting carbon, the problem of the low and poor stability of battery conversion efficiency, the invention provides the preparation method of a kind of thermoplasticity carbon for perovskite solar cell to electrode.Particularly, perovskite solar cell comprises light anode and is formed on thermoplasticity carbon on light anode to electrode, and wherein the structure of light anode will be described in detail below.
In a kind of exemplary embodiments of the present invention, thermoplasticity carbon comprises the preparation method of electrode: step S1, conductive carbon material and thermoplastic polymer are dissolved and be dispersed in organic solvent, to form uniform carbon pastes.Step S2, provide a substrate, and on the surface of substrate, form carbon pastes layer with carbon pastes.Step S3, dried carbon pulp layer are to remove the organic solvent in carbon pastes layer, thereby the thermoplasticity carbon that obtains film-form and conduction is to electrode.
Consider the factor such as electric conductivity, material particle size size, preferably, conductive carbon material is selected from one or more in graphite, carbon black, carbon fiber, carbon nano-tube and Graphene.Above-mentioned conductive carbon material conductivity is good and be easy to be dispersed into sub-micron particle, can be prepared to the film with superior electrical conductivity.The present invention preferably but be not limited to above-mentioned material, as long as can there is good electric conductivity and be easy to be dispersed into sub-micron.Further preferably, conductive carbon material is graphite and carbon black.
In an embodiment of the present invention, thermoplastic polymer is that fusing point is thermoplastic resin and the thermoplastic elastomer of 50 DEG C～200 DEG C.Preferably, thermoplastic resin be selected from polyvinyl acetate, ethylene-vinyl acetate copolymer and in one or more; Thermoplastic elastomer is selected from one or more in styrene analog thermoplastic elastomer, olefin hydrocarbons thermoplasticity elastic body, dienes thermoplastic elastomer (TPE) and polyurethanes thermoplastic elastomer (TPE).Consider the factor such as melting range and dissolubility, the present invention preferably adopts above-mentioned thermoplastic resin and thermoplastic elastomer, but is not limited to this, as long as can have lower fusing point, can be dissolved in preferably in organic solvent.
Wherein, organic solvent be can heat of solution thermoplastic polymer single or mixed solvent.Particularly, organic solvent can be ethyl acetate, toluene, ethanol, acetone or cyclohexane.
Preferably, the weight ratio of conductive carbon material and thermoplastic polymer is 1:1～10:1.The present invention is limited to both weight ratios in above-mentioned scope, is mainly to consider conductivity and the film internal connectivity of thermoplasticity carbon to electrode film.If the weight ratio of conductive carbon material and thermoplastic polymer is less than 1:1, there will be the thermoplasticity carbon problem excessive to electrode resistance, and then reduce fill factor, curve factor and the efficiency of battery.If the weight ratio of conductive carbon material and thermoplastic polymer is greater than 10:1, thermoplasticity carbon is poor to electrode film internal connectivity, film is easy to crack, and then causes thermoplasticity carbon to electrode and the loose contact of light anode, has finally reduced short circuit current and the stability of battery.
Particularly, adopt stirring, mode ultrasonic or that grind that conductive carbon material and thermoplastic polymer are disperseed and be dissolved in organic solvent, to obtain uniform carbon pastes.After conductive carbon material and thermoplastic polymer are disperseed and being dissolved in organic solvent, in order to improve uniformity and the useful life of thermoplasticity carbon to electrode of stability, film forming of carbon pastes, step S1 is also to adding for adjusting viscosity in carbon pastes, preventing aging auxiliary agent.Preferably, auxiliary agent is selected from one or more in ethyl cellulose, polyvinylpyrrolidone, benzophenone and titanium dioxide.Preferably, taking thermoplastic polymer as benchmark, the addition of auxiliary agent accounts for 1%～50% of thermoplastic polymer weight.Be conducive to stability and the film forming procedure of carbon pastes by adjusting viscosity, prevent the aging useful life of thermoplasticity carbon to electrode of can extending, and then extended the useful life of solar cell, saved cost.
Prepare after carbon pastes, preferably adopt drop-coating, knife coating, spraying process, spin-coating method, silk screen print method or czochralski method on the surface of substrate, to form carbon pastes layer, adopt afterwards the mode of nature or artificial drying to remove the organic solvent in carbon pastes layer, thereby the thermoplasticity carbon that obtains film-form and conduction is to electrode.Wherein, substrate adopts glass, silicon chip, sheet metal or flexible plastic film, metal forming, the graphite paper of smooth smooth rigidity.
Light anode in the present invention comprises the substrate, transparency electrode, electron transfer layer, the light-absorption layer that stack gradually, can also comprise the hole transmission layer being arranged on light-absorption layer.Wherein, light-absorption layer is perovskite material, is typical for CH
3nH
3pbI
3perovskite, is a kind of low-energy zone semiconductor with good carrier mobility, CH
3nH
3pbI
3the free charge carrier (or exciton) generating in layer can be transferred under electron transfer layer by electronics, or transfers in hole mobile material by hole.
In a kind of exemplary embodiments of the present invention, also comprise step S41: thermoplasticity carbon is peeled off from substrate electrode, then the thermoplasticity carbon of self-supporting form is transferred on light anode electrode.Which is conducive to save material, and is expected to produce by the mode of volume to volume.
In another kind of exemplary embodiments of the present invention, also comprise step S42: by thermoplasticity carbon to the electrode substrate global transfer accompanying with it to light anode.The method does not need thermoplasticity carbon to peel off from substrate electrode, and then has avoided destroying in stripping process the integrality of film-form thermoplasticity electrode.But while adopting the mode of global transfer, base material is had to higher requirement.Preferably, base material is selected from one or more in metal forming, sheet metal, graphite paper and electro-conductive glass.The present invention preferably but be not limited to above-mentioned base material, as long as can there is good conductivity and with carbon, electrode integral is transferred to the performance that does not affect battery on light anode.The present invention adopts above-mentioned material as substrate, is mainly to consider that it has good conductivity, heat conduction and planarization, can and be attached to suprabasil thermoplasticity carbon by this substrate like this electrode integral is transferred on light anode.
In a preferred embodiment of the present invention, in order not affect hot pressing transfer process, the THICKNESS CONTROL of substrate, in the scope of 0.01～5mm, is controlled to 10 by the resistivity of base material
-8～10
-3in the scope of Ω m.If the thickness of substrate is greater than 5mm, can reduce rate of heat transfer, hinder hot pressing.If substrate thickness is less than 0.01mm, can causes substrate to occur distortion, thereby affect the planarization of substrate.
In a kind of exemplary embodiments of the present invention, adopt the mode of hot pressing that thermoplasticity carbon is transferred on light anode electrode.Preferably, the temperature of hot pressing is 100 DEG C～120 DEG C, and pressure is 0.2～0.5MPa, and the time is 20～30 seconds.Under the condition of said temperature, pressure and time, carry out hot pressing, can ensure that thermoplasticity carbon has better stickiness to electrode and light anode.Too high or the excessive battery structure that all can destroy of pressure of hot pressing temperature, the too low or too small meeting of pressure of hot pressing temperature causes thermoplasticity carbon to electrode and the loose contact of light anode, and then cannot obtain the perovskite solar cell of high conversion efficiency.
Thermoplasticity carbon provided by the present invention is suitable for various dissimilar perovskite solar cells to electrode preparation method, specifically includes TiO
2, the semi-conductive support layer such as ZnO sensitization perovskite solar cell, have Al
2o
3see superstructure heterojunction type perovskite solar cell Deng Jie of insulating material support layer, have the planar heterojunction perovskite solar cell of plane electron transfer layer etc., in above several structures, can there is or not have hole transmission layer.
According to a further aspect in the invention, provide a kind of perovskite solar cell, comprised that thermoplasticity carbon is to electrode, this thermoplasticity carbon is to adopt above-mentioned any method to be prepared to electrode.In a preferred embodiment of the present invention, thermoplasticity carbon is 5～1000 μ m to the thickness of electrode.If thermoplasticity carbon is excessive to the thickness of electrode, can cause the resistance of battery excessive, reduce battery fill factor, curve factor and battery conversion efficiency.If thickness is too small, the lack of homogeneity can cause thermoplasticity carbon to electrode film forming time.By thermoplasticity carbon to the THICKNESS CONTROL of electrode in above-mentioned scope, can make it be hot-pressed to better on light anode, and then improve the performance of perovskite solar cell.
Further illustrate beneficial effect of the present invention below in conjunction with embodiment more specifically.
Embodiment 1
1) (particle diameter is 1～3 μ m to take 0.6 gram of graphite powder, by Aladdin reagent, Co., Ltd provides) and 0.2 gram to electrode acetylene black (being provided by A Faaisha Chemical Co., Ltd.), 0.2 gram of polyvinyl acetate (PVAc) (being provided by Chemical Reagent Co., Ltd., Sinopharm Group), they are joined in the ethyl acetate of 10 milliliters, with 200r/min ball milling 4 hours, and add 0.1g for adjusting viscosity, prevent aging auxiliary agent ethyl cellulose, obtain uniformly to electrode carbon slurry.
2) carbon pastes is dripped equably and is coated onto on substrate polytetrafluoroethylene film, form carbon pastes layer, natural air drying is to remove the organic solvent ethyl acetate in carbon pastes layer, then take off with blade is complete, obtain the conductive carbon film that thickness is the self-supporting of 0.1mm, be thermoplasticity carbon to electrode, can be used for the thermoplasticity carbon of Ca-Ti ore type solar cell to electrode finished product.
3) the perovskite battery light anode without hole mobile material according to the method preparation in list of references (Appl.Phys.Lett., 2014,104,063901.): first at FTO silk screen printing one deck on glass TiO
2thin layer, afterwards again at TiO
2on thin layer, print one deck TiO
2nanometer crystal layer heats 30 minutes at 450 DEG C, obtains thickness and is about the porous support layer that the compacted zone of 50nm and thickness are about 500nm.Adopt two step liquid phase methods to deposit perovskite CH in porous support layer
3nH
3pbI
3light absorbent: the PbI that is first 1.2M by concentration
2dimethyl formamide (DMF) solution under the rotating speed of 3000rpm, be spin-coated on the surface of porous support layer, continue spin coating after 30 seconds, at 90 DEG C, heat 2 minutes, with the CH that is 10mg/mL in concentration by porous support layer
3nH
3in the aqueous isopropanol of I, soak 10 minutes, finally at the temperature of 90 DEG C, heat 45 minutes, obtain perovskite solar battery light anode.
4) by step 2) in preparation self-supporting conductive carbon film fit in Ca-Ti ore type CH
3nH
3pbI
3light absorbent surface, and hot pressing 20 seconds under 120 DEG C, the condition of 0.2MPa, obtain complete Ca-Ti ore type solar cell.
Embodiment 2
1) (particle diameter is 400nm to take 0.4 gram of graphite powder, by Aladdin reagent, Co., Ltd provides), 0.2 gram of carbon nano-tube (Co., Ltd provides by Aladdin reagent), 0.4 gram of ethylene-vinyl acetate copolymer (EVA) (Co., Ltd provides by Aladdin reagent), they are added in the organic solvent toluene of 10 milliliters, ultrasonic dispersion 3 hours at 50 DEG C, and add 0.04g for adjusting viscosity, prevent aging auxiliary agent ethyl cellulose, obtain uniformly to electrode carbon slurry.
2) by carbon pastes equably blade coating to smooth latten(-tin), form carbon pastes layer, after natural air drying, the conductive carbon film obtaining is peeled off to latten(-tin) substrate, obtain the conductive carbon film that thickness is 0.2mm, thermoplasticity carbon is to electrode.
3) the perovskite solar battery light anode containing hole mobile material according to the method preparation in list of references (Sci.Rep., 2012,2,591.): first at FTO silk screen printing one deck on glass TiO
2thin layer, subsequently silk screen printing one deck TiO
2nanometer crystal layer, after 450 DEG C of heating 30 minutes, obtains thickness and is about the porous support layer that the compacted zone of 50nm and thickness are about 500nm.Subsequently, adopt a step liquid phase method to deposit perovskite CH in porous support layer
3nH
3pbI
3light absorbent: first by etc. the PbI of stoichiometric proportion
2with CH
3nH
3i is dissolved in gamma-butyrolacton, and both gross mass percentage compositions are 40%, is spun on the surface of porous support layer under the rotating speed of 3000rpm, continues spin coating after 30 seconds, heats 10 minutes at 70 DEG C.Last again with hole mobile material spiro-OMeTAD in the rotating speed spin coating of 2000rpm, can obtain perovskite solar battery light anode.
4) conductive carbon film of self-supporting is fitted in to the surface of the hole transmission layer on perovskite solar battery light anode, and hot pressing 30 seconds under 100 DEG C, the condition of 0.5MPa, complete Ca-Ti ore type solar cell obtained.
Embodiment 3～6
Its preparation process 2), 3) with 4) identical with embodiment 2.
Difference is in embodiment 3 0.6 gram of graphite powder, 0.2 gram of acetylene black and 0.8 gram of polyvinyl acetate (PVAc) to join in the organic solvent toluene of 15ml.Be that conductive carbon material in embodiment 3 and the weight ratio of thermoplastic polymer are 1:1.
In embodiment 4,6 grams of graphite powders and 2 grams of acetylene black and 0.8 gram of polyvinyl acetate (PVAc) are joined in the organic solvent toluene of 50ml.Be that conductive carbon material in embodiment 4 and the weight ratio of thermoplastic polymer are 10:1.
In embodiment 5,6 grams of graphite powders and 6 grams of acetylene black and 1.0 grams of polyvinyl acetate (PVAc) are joined in the organic solvent toluene of 50ml.Be that conductive carbon material in embodiment 5 and the weight ratio of thermoplastic polymer are 12:1.
In embodiment 6, adopt 0.5 gram of graphite powder and 0.5 gram of acetylene black and 2 grams of polyvinyl acetate (PVAc) to join in the organic solvent toluene of 20ml.Be that conductive carbon material in embodiment 6 and the weight ratio of thermoplastic polymer are 1:2.
Embodiment 7
Its preparation process is all identical with embodiment 2, and difference is, the step 1 of embodiment 7) in do not add for adjusting viscosity, prevent aging auxiliary agent ethyl cellulose.
Embodiment 8
Its preparation process is all identical with embodiment 2, and difference is, in embodiment 8, thermoplasticity carbon is not peeled off out from latten(-tin) substrate to electrode, but directly by thermoplasticity carbon to the electrode substrate global transfer accompanying with it to light anode.
Comparative example 1
Prepare perovskite solar battery light anode according to the method in embodiment 1.
Its preparation process 1) identical with embodiment 1, difference is, in comparative example 1, do not have previously prepared thermoplasticity carbon to electrode finished product, but directly by step 1) in obtain to the direct blade coating of electrode carbon slurry to the light-absorption layer surface of light anode, through natural drying, obtain the Ca-Ti ore type solar cell of carbon to electrode.
Comparative example 2
Prepare perovskite solar battery light anode according to the method in embodiment 2.
According to step 1 in embodiment 1) identical method prepared electrode carbon, difference be not have in comparative example 2 previously prepared go out thermoplasticity carbon to electrode finished product, but directly by the direct blade coating of electrode carbon slurry to the surface of the hole transmission layer of light anode, find that hole transmission layer is dissolved by solvent ethyl acetate, cannot make the battery of corresponding construction, also cannot carry out subsequent detection.
Under standard solar simulator, the performance of the perovskite solar cell of preparing in embodiment 1-8 and comparative example 1-2 is detected with potentiostat, the concrete data that wherein short-circuit current density, open circuit voltage, fill factor, curve factor, conversion efficiency characterize stability are in table 1.
Table 1
As can be seen from Table 1, in embodiment 1-8, adopt the preparation method of thermoplasticity carbon of the present invention to electrode, owing to having avoided the destruction of the organic solvent in carbon pastes to hole transmission layer and light-absorption layer, obtained having the perovskite solar cell of higher energy conversion efficiency, general conversion efficiency can reach more than 9%.And after 1000 hours, find that its battery conversion efficiency and the ratio of initial battery conversion efficiency still can reach more than 85%, illustrate and adopt thermoplasticity carbon of the present invention also to there is good stability to the preparation method of electrode, and the method technique is simple, the flexibility of battery is better.
Conductive carbon material in embodiment 5 and embodiment 6 and the weight ratio of thermoplastic polymer all not in the scope of 1:1～10:1, thereby cause its battery conversion efficiency relatively low with respect to embodiment 2-4.Concrete analysis, conductive carbon material in embodiment 5 and the weight ratio of thermoplastic polymer are 12:1, because wherein contained thermoplastic polymer content is less, easily cause thermoplasticity carbon poor to electrode film internal connectivity, film is easy to crack, and then cause thermoplasticity carbon to electrode and the loose contact of light anode, and finally reduce short circuit current and the stability of battery, cause conversion efficiency low.
In embodiment 6, because the weight ratio of conductive carbon material and thermoplastic polymer is 1:2, because thermoplastic polymer content is more, can cause thermoplasticity carbon excessive to the resistance of electrode, and then affect fill factor, curve factor and the battery conversion efficiency of battery.
The battery conversion efficiency of embodiment 7 is not low, but its conversion efficiency but significantly reduces with the ratio of initial value after 1000 hours, is mainly owing to not adding for adjusting viscosity and preventing aging auxiliary agent, thereby causes the stability of battery to reduce.
Although it does not peel off out from latten(-tin) substrate to electrode by thermoplasticity carbon in embodiment 8, but directly by thermoplasticity carbon to the electrode substrate global transfer accompanying with it to light anode, its battery conversion efficiency and stability do not have variation, and which can obtain complete thermoplasticity carbon to electrode film, good to electrode conductivuty, battery fill factor, curve factor is higher.
Visible, the present invention adopt first previously prepared go out the material with carbon element film of thermoplasticity carbon to electrode, and then be hot-pressed onto on light anode, avoid the damage of the organic solvent in carbon pastes to light-absorption layer and hole transmission layer, and then improved the conversion efficiency of perovskite solar cell.And it is simple to the method technique of electrode to the invention provides thermoplasticity carbon, be applicable on the Ca-Ti ore type solar cell of various structures.
So far, those skilled in the art will recognize that, illustrate and described of the present invention multiple exemplary embodiment although detailed herein, but, without departing from the spirit and scope of the present invention, still can directly determine or derive many other modification or the amendment that meet the principle of the invention according to content disclosed by the invention.Therefore, scope of the present invention should be understood and regard as and cover all these other modification or amendments.
Claims (10)
1. the preparation method to electrode for the thermoplasticity carbon of perovskite solar cell, described perovskite solar cell comprises light anode and is formed on thermoplasticity carbon on described smooth anode to electrode; Described preparation method comprises the following steps:
Step S1, conductive carbon material and thermoplastic polymer are dissolved and be dispersed in organic solvent, to form uniform carbon pastes;
Step S2, provide a substrate, and on the surface of described substrate, form carbon pastes layer with described carbon pastes; And
Step S3, dry described carbon pastes layer are to remove the described organic solvent in described carbon pastes layer, thereby the thermoplasticity carbon that obtains film-form and conduction is to electrode.
2. preparation method according to claim 1, wherein, the weight ratio of described conductive carbon material and described thermoplastic polymer is 1:1～10:1.
3. according to the preparation method described in any one in claim 1-2, wherein,
Described conductive carbon material is selected from one or more in graphite, carbon black, carbon fiber, carbon nano-tube and Graphene, and preferably, described conductive carbon material is graphite and carbon black;
Described thermoplastic polymer is that fusing point is thermoplastic resin and the thermoplastic elastomer of 50 DEG C～200 DEG C;
Preferably, described thermoplastic resin is selected from one or more in polyvinyl acetate, ethylene-vinyl acetate copolymer, polyacrylate and polystyrene;
Described thermoplastic elastomer is selected from one or more in styrene analog thermoplastic elastomer, olefin hydrocarbons thermoplasticity elastic body, dienes thermoplastic elastomer (TPE) and polyurethanes thermoplastic elastomer (TPE).
4. according to the preparation method described in any one in claim 1-3, wherein, described step S1 also comprises to adding in described carbon pastes for adjusting viscosity, preventing the process of aging auxiliary agent; Preferably, described auxiliary agent is selected from one or more in ethyl cellulose, polyvinylpyrrolidone, benzophenone and titanium dioxide.
5. according to the preparation method described in any one in claim 1-4, wherein, described thermoplasticity carbon is 0.005～1mm to the thickness of electrode, is preferably 0.1～0.2mm.
6. according to the preparation method described in any one in claim 1-5, wherein, also comprise:
Step S41, described thermoplasticity carbon is peeled off from described substrate electrode, then the described thermoplasticity carbon of self-supporting form is transferred on described smooth anode electrode.
7. according to the preparation method described in any one in claim 1-5, wherein, also comprise:
Step S42, by described thermoplasticity carbon to the electrode described substrate global transfer accompanying with it to described smooth anode.
8. preparation method according to claim 7, wherein, the material of described substrate is selected from one or more in metal forming, sheet metal, graphite paper and electro-conductive glass; Alternatively, the thickness of described substrate is 0.01～5mm, and the resistivity of described base material is 10
-8～10
-3Ω m.
9. according to the preparation method described in any one in claim 1-8, wherein, adopt the mode of hot pressing that described thermoplasticity carbon is transferred on described smooth anode electrode; Alternatively, the temperature of described hot pressing is 100 DEG C～120 DEG C, and pressure is 0.2～0.5MPa, and the time is 20～30 seconds.
10. a perovskite solar cell, comprises that thermoplasticity carbon is to electrode, and described thermoplasticity carbon is to adopt the method described in any one in claim 1-9 to be prepared to electrode.
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