CN103746078A - Perovskite solar cell and preparation method thereof - Google Patents

Perovskite solar cell and preparation method thereof Download PDF

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CN103746078A
CN103746078A CN201410040145.4A CN201410040145A CN103746078A CN 103746078 A CN103746078 A CN 103746078A CN 201410040145 A CN201410040145 A CN 201410040145A CN 103746078 A CN103746078 A CN 103746078A
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light
absorption layer
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肖立新
郑灵灵
马英壮
陈志坚
曲波
王树峰
龚旗煌
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    • H—ELECTRICITY
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    • 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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    • H10K71/20—Changing the shape of the active layer in the devices, e.g. patterning
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    • 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
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Abstract

The invention discloses a perovskite solar cell and a preparation method thereof. The perovskite solar cell comprises a substrate, a transparent electrode, an electron transport layer, an electron transport and light adsorption layer, a light adsorption layer, a hole transport and light adsorption layer, a hole transport layer and a top electrode which are sequentially laminated, wherein the light adsorption layer is a photovoltaic material light adsorption layer with a perovskite structure; the electron transport and light adsorption layer is a composite functional layer formed by embedding an electron transport material and a perovskite structure photovoltaic material; and the hole transport and light adsorption layer is a composite functional layer formed by embedding a hole transport material and a perovskite structure photovoltaic material. Both sides of the light adsorption layer of the perovskite solar cell are of a certain micro nano structure, so that the composite functional layers of which the materials are embedded can be formed by the light adsorption layer and the transport layers outside the light adsorption layer; contact areas of the light adsorption layer and the transport layers are greatly increased and the perovskite solar cell is beneficial for improving exciton separation and charge transfer efficiency, so that compounding of photo-generated electrons and a hole is inhibited and performance of a device is improved.

Description

A kind of perovskite solar cell and preparation method thereof
Technical field
The invention belongs to perovskite solar cell (PSC, PerovskiteSolar Cells) field, specially refer to a kind of perovskite solar cell with composite heterogenous junction structure and preparation method 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 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 metal 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, by load, completes the conversion of luminous energy to electric energy.
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.
Since 2009, document " A.Kojima, K.Teshima, Y.Shirai; T.Miyasaka, J.Am.Chem.Soc.2009,131; 6050. " first adopted the light absorbent of perovskite material as solar cell, and along with going deep into of research, the efficiency of perovskite solar cell improves constantly.2012, document " M.M.Lee, J.Teuscher; T.Miyasak, T.N.Murakami, H.J.Snaith; Science2012,338,643. " and document " H.S.Kim; C.R.Lee, J.H.Im, K.B.Lee; T.Moehl; A.Marchioro, S.J.Moon, R.H.Baker, J.H.Yum, J.E.Moser, M.Gr tzel, N.G.Park, Sci.Rep.2012,2,591. " report respectively efficient solid-state perovskite solar cell, improved greatly the photoelectric conversion efficiency of perovskite solar cell.What these perovskite solar cells adopted is all the heterojunction structure based on p-i-n structure.
Summary of the invention
Perovskite not only can extensively absorb solar spectrum, and has splendid charge transport properties.In order to make full use of these character, the invention provides a kind of perovskite solar cell and preparation method thereof, the perovskite solar cell that adopts the inventive method to prepare, the both sides of its light-absorption layer all have certain micro-nano structure, thereby and between the transport layer in its outside, can form mutually chimeric complex functional layer of material, significantly improve the contact area of light-absorption layer and transport layer, be conducive to improve exciton dissociation and charge transfer efficiency, thereby suppress the compound of light induced electron and hole, improve device performance.
Technical scheme of the present invention is as follows:
A kind of perovskite solar cell, comprise the substrate, transparency electrode, electron transfer layer, electric transmission-light-absorption layer, light-absorption layer, hole transport-light-absorption layer, hole transmission layer and the top electrode that stack gradually, wherein: described light-absorption layer is the photovoltaic material light-absorption layer with perovskite structure; Described electric transmission-light-absorption layer is the complex functional layer of electron transport material and the chimeric formation of perovskite structure photovoltaic material; Described hole transport-light-absorption layer is the complex functional layer of hole mobile material and the chimeric formation of perovskite structure photovoltaic material.
The backing material that is applicable to perovskite solar cell of the present invention has the transparent materials such as glass, flexiplast.In addition, also can add antireflective film on the irradiation of substrate one side (outside) surface, improve the transmitance of incident light.
Transparency electrode is positioned on the inner surface of substrate, the material of transparency electrode can be indium tin oxide (ITO, Indium Tin Oxides), fluorine tin-oxide (FTO, fluorine doped tin oxide), the conventional transparent electrode material such as aluminium zinc oxide (AZO, aluminium-doped zinc oxide).Normal ITO electro-conductive glass or the FTO electro-conductive glass of adopting is as substrate and transparency electrode.
What in electron transfer layer and electric transmission-light-absorption layer, electron transport material used was common is metal oxide, as titanium oxide (TiO 2), zinc oxide (ZnO), zirconia (ZrO 2) etc.Wherein TiO 2it is the most frequently used electron transport material in current perovskite solar cell device.Electron transfer layer is that metal oxide is gathered in the film forming in transparency electrode, is generally the compacted zone of thickness between 10nm～100nm, plays the effect of transmission electronic, prevents that electrode from directly contacting with light-absorption layer simultaneously.
Light-absorption layer adopts perovskite crystal preparation, and its effect is to absorb incident light.The simple light-absorption layer of device of the present invention consists of the compact-grain of perovskite material, and thickness is conventionally at 100～200nm.In addition, if introduce the micro-nano structure that particle diameter forms at the perovskite crystal of 200nm～400nm left and right on light-absorption layer, not only can absorb incident light, also help and improve the scattering of light in whole device, thereby further improve the absorption to incident light.Common perovskite material mainly contains similar ABX 3(A=CH 3nH 3 +deng; B=Pb 2+, Sn 2+deng; X=Cl -, Br -, I -deng) the organic inorganic hybridization perovskite of type crystal structure, its energy gap is at 1.0-2.0eV.
Hole transmission layer be mainly by hole transport to metal electrode, thickness is generally 50～300nm.Hole mobile material in hole transmission layer and hole transport-light-absorption layer is generally the material with higher hole mobility, can be organic material and/or inorganic material, organic material is as Spiro-MeOTAD, P3HT, PTAA, TAPC, NPB, TPD etc., and inorganic material is as CuI, CuSCN, Cu 2o, CuO, NiO, MoOx etc.
Electric transmission-light-absorption layer, between electron transfer layer and light-absorption layer, is the micro-nano interpenetrating structure that porous metal oxide and perovskite material form, and plays extinction and electric transmission effect, conventionally the about 400nm～600nm of thickness.Porous metal oxide and perovskite material form interlaced nanoscale microstructure (10nm～100nm) film with high specific surface area, the multiple microscopic appearance structures such as such as nano-pore, nano wire, nano-pillar, nanotube, nano flower, nanotrees.The appearance structure of high-specific surface area is conducive to improve the contact area of material, contributes to improve electronic transmission performance.
Hole transport-light-absorption layer is between hole transmission layer and light-absorption layer, and by perovskite material and the mutual chimeric laminated film forming of hole mobile material, thickness between 100nm～200nm, plays extinction and hole transport effect conventionally.By controlling the growth conditions of perovskite material, regulate the surface topography of perovskite material, can form jagged material interface, thereby expand the contact area of hole transmission layer and light-absorption layer, thereby raising cavity transmission ability, reduces the compound of both hole and electron, improves battery efficiency.
The general material with higher work-functions that adopts of top electrode, as metal and conductive carbon materials such as gold, silver, copper, aluminium, can adopt the manufacture methods such as vacuum coating and solution film forming.
Perovskite solar cell of the present invention has the sandwich construction that is similar to p-(pi)-i-(in)-n, in device, introduced two composite beds of electric transmission-light-absorption layer and hole transport-light-absorption layer (pi and in), its preparation method comprises the following steps:
1) in substrate and transparency electrode, adopt electron transport material to prepare dense film, form electron transfer layer;
2) on electron transfer layer, utilize electron transport material to form micro-nano porous membrane, the perovskite material of then growing, form electric transmission-light-absorption layer and on light-absorption layer, the surface topography of simultaneously controlling light-absorption layer is the zigzag of continuous densification;
3) at surperficial spin coating or the evaporation hole mobile material of light-absorption layer, form hole transport-light-absorption layer and on hole transmission layer;
4) on hole transmission layer, prepare top electrode.
Above-mentioned steps 1) electron transfer layer can be by the precursor solution of coating electron transport material, then high temperature sintering preparation.
Above-mentioned steps 2) in utilize the thickness of porous membrane prepared by electron transport material at 400-600nm.Perovskite material grows in the hole of this porous membrane, form electric transmission-light-absorption layer, and the perovskite material of growing on porous membrane forms fine and close crystal grain, thickness 100-200nm, for light-absorption layer, the pattern of its upper surface such as, regulates and controls by the grow condition such as concentration (5mg/mL～50mg/mL) of reaction solution of perovskite of control, thereby guarantees finally to have the zigzag pattern of continuous densification.
Above-mentioned steps 4) can adopt the method for vacuum coating or solution film forming on hole transmission layer, to prepare top electrode.
The structure of perovskite battery is p-i-n structure substantially at present, and " the perovskite solar cells based on two composite heterogenous junctions " that the present invention proposes, what utilize is the sandwich construction that is similar to p-(pi)-i-(in)-n, introduce two composite beds (pi) and (in) in device architecture, increase the contact area of light light-absorption layer and charge transport layer, be conducive to the transmission of electric charge, thereby suppress the compound of light induced electron and hole, finally improve device performance.
Accompanying drawing explanation
Fig. 1 is perovskite solar cell device structure chart, wherein: 1-FTO electro-conductive glass; 2-electron transfer layer; 3-electric transmission-light-absorption layer; 4-light-absorption layer; 5-hole transport-light-absorption layer; 6-hole transmission layer; 7-metal electrode.
Fig. 2 is the electron microscope picture of the perovskite solar battery structure prepared of embodiment 1, and wherein, upper figure is the upper surface topography figure of perovskite light-absorption layer; Figure below is device architecture figure, is 1-FTO electro-conductive glass, 2-electron transfer layer, 3-electric transmission-light-absorption layer, 4-light-absorption layer, 5-hole transport-light-absorption layer and 6-hole transmission layer from the bottom to top successively.
Fig. 3 is the absorption spectrum of perovskite material in the device prepared of embodiment 1 and comparative example 1.
Fig. 4 is under AM1.5G illumination, the volt-ampere characteristic of the perovskite solar cell of embodiment 1 and comparative example 1.
Embodiment
Below by embodiment, describe device of the present invention and preparation method thereof in detail, but be not construed as limiting the invention.
Embodiment 1: the composite heterogenous junction structure (preparation of the device of p-(pi)-i-(in)-n)
1, preparation PbI 2solution: PbI 2concentration be 1.0M, solvent is dimethyl formamide.
2, preparation CH 3nH 3i solution: concentration 10mg/mL, is dissolved in isopropyl alcohol.
3, the preparation of device function layer, referring to Fig. 1, mainly comprises the each functional layer being laminated in substrate and transparency electrode 1: electron transfer layer 2, electric transmission-light-absorption layer 3, light-absorption layer 4, hole transport-light-absorption layer 4, hole transmission layer 6, and metal electrode 7.Preparation process is as follows:
1) adopt FTO electro-conductive glass as substrate and transparency electrode 1, thickness 2-5mm, surface resistance is below 50 ohm;
2) adopt spin-coating method on substrate, to be coated with two (acetylacetone based) diisopropyl titanate esters (titanium diisopropoxidebis (acetylacetonate)) precursor solutions of 0.15M, 350 ℃～500 ℃ high temperature sintering 30min～90min in Muffle furnace, obtain the TiO of the about 10-100nm of thickness 2dense film is as electron transfer layer 2;
3) electric transmission-light-absorption layer 3, light-absorption layer 4 and hole transport-light-absorption layer 5 are continuous productions.
First prepare the TiO of 400-600nm 2perforated membrane: adopt spin-coating method to be coated with nano-TiO on electron transfer layer 2precursor solution (the DHS-TPP3 of particle colloid, Dalian HeptaChroma SolarTech Co., Ltd.), put into 350 ℃～500 ℃ high temperature sintering 30min～90min of Muffle furnace, form nano level porous membrane, this porous membrane can be realized embedded structure with the perovskite material of follow-up preparation, forms electric transmission-light-absorption layer 3.
Perovskite material adopts solwution method original position synthetic: first at TiO 2spin coating PbI on perforated membrane 2solution, puts into CH after oven dry 3nH 3in I solution, soak growth perovskite material, in this process, perovskite material is grown in TiO 2in the hole of perforated membrane, form electric transmission-light-absorption layer, and can form fine and close crystal grain at electric transmission-light-absorption layer upper surface, the about 100-200nm of thickness, this is perovskite light-absorption layer 4.By the concentration of controlling solution growth, can regulate the upper surface topography of light-absorption layer, thereby improve the interfacial structure of the hole transport-light-absorption layer of follow-up formation.The upper surface topography of light-absorption layer is mainly controlled by following two aspects: the one, control PbI 2concentration, the 2nd, control CH 3nH 3the concentration of I reaction solution.By controlling reaction density, can obtain good perovskite pattern, can form fine and close light-absorption layer, there is again higher surface area.Surperficial spin coating hole mobile material spiro-MeOTAD(concentration at calcium titanium ore bed is 0.17M, solvent adopts chlorobenzene), form hole transport-light-absorption layer 5 with the coarse particles on light-absorption layer 4 surfaces, the about 100-200nm of thickness, the thick hole transmission layer 6 of 50-300nm of simultaneously also having an appointment on hole transport-light-absorption layer 5, is shown in Fig. 1 and Fig. 2.
4, metal electrode adopts silver, and vacuum thermal evaporation 80-150nm is at device upper surface.
Comparative example 1: without the preparation of the device of composite heterogenous junction structure (p-i-n)
1, preparation perovskite solution, the PbI of employing 1.0M 2, the CH of 1.0M 3nH 3i, solvent is dimethyl formamide.
2, the preparation of device function layer, mainly comprises the each functional layer being laminated in substrate and transparency electrode: electron transfer layer, light-absorption layer, hole transmission layer, and metal electrode.Preparation process is as follows:
1) adopt FTO electro-conductive glass as substrate and transparency electrode, thickness 2-5mm, surface resistance is below 50 ohm;
2) adopt spin-coating method on substrate, to be coated with titanium diisopropoxidebis (acetylacetonate) precursor solution of 0.15M, 350 ℃～500 ℃ high temperature sintering 30min～90min in Muffle furnace, obtain the TiO of the about 10-100nm of thickness 2dense film is as electron transfer layer;
3) perovskite solution is spun on electron transfer layer, by the lower 90 ℃ of annealing of vacuum, forms light-absorption layer.
4) on light-absorption layer, spin coating hole mobile material spiro-MeOTAD(concentration is 0.17M, and solvent adopts chlorobenzene), obtain the hole transmission layer of the about 50-300nm of thickness.
3, metal electrode adopts silver, and vacuum thermal evaporation 80-150nm is at device upper surface.
Device performance test
Device containing composite heterogenous junction prepared by embodiment 1 and the device without composite heterogenous junction prepared by comparative example 1 are placed under standard solar simulator, by transparency electrode and metal electrode connecting test instrument, test.
What Fig. 3 provided is the absorption spectrum of perovskite material in device, can find out that absorption containing composite heterogenous junction, higher than without composite heterogenous junction, captures thereby reach efficient light.
In experimentation, adopt at 100mW/cm 2current-voltage under solar simulator (Newport) AM1.5G illumination is measured in air at room temperature by current-voltage instrument (Keithley2611).Measurement result as shown in Figure 4, is read V by Fig. 4 oc, J sc, and calculate FF and η, as shown in table 1.
The volt-ampere performance parameter of table 1 perovskite battery
Figure BDA0000462857980000061
By embodiment, describe the perovskite solar cell based on MULTILAYER COMPOSITE heterojunction provided by the present invention in detail above.MULTILAYER COMPOSITE heterojunction, on general p-i-n architecture basics, has been introduced two-layer composite material transition zone, has formed p-(pi)-i-(in) heterojunction structure of-n.Such transition layer structure can increase the contact area of light-absorption layer and electron transfer layer and hole transmission layer, thereby is conducive to separation of charge in battery and electric charge transmission, effectively reduces electronics with hole is compound at inside battery, thus the performance of raising device.
It will be understood by those of skill in the art that not departing from the scope of essence of the present invention, can make certain distortion or modification to device architecture of the present invention, its preparation method is also not limited to disclosed content in embodiment.

Claims (10)

1. a perovskite solar cell, comprise the substrate, transparency electrode, electron transfer layer, electric transmission-light-absorption layer, light-absorption layer, hole transport-light-absorption layer, hole transmission layer and the top electrode that stack gradually, wherein: described light-absorption layer is the photovoltaic material light-absorption layer with perovskite structure; Described electric transmission-light-absorption layer is the complex functional layer of electron transport material and the chimeric formation of perovskite structure photovoltaic material; Described hole transport-light-absorption layer is the complex functional layer of hole mobile material and the chimeric formation of perovskite structure photovoltaic material.
2. perovskite solar cell as claimed in claim 1, is characterized in that, described backing material is glass or flexiplast; The material of described transparency electrode is indium tin oxide, fluorine tin-oxide or aluminium zinc oxide.
3. perovskite solar cell as claimed in claim 1, is characterized in that, the electron transport material in described electron transfer layer and electric transmission-light-absorption layer is metal oxide.
4. perovskite solar cell as claimed in claim 1, is characterized in that, described electric transmission-light-absorption layer is the micro-nano interpenetrating structure that porous metal oxide and perovskite structure photovoltaic material form.
5. perovskite solar cell as claimed in claim 1, is characterized in that, described perovskite structure photovoltaic material is ABX 3the organic inorganic hybridization perovskite of type crystal structure.
6. perovskite solar cell as claimed in claim 1, is characterized in that, in described hole transport-light-absorption layer, and the chimeric interface indentation of perovskite structure photovoltaic material and hole mobile material.
7. perovskite solar cell as claimed in claim 1, it is characterized in that, hole mobile material in described hole transport-light-absorption layer and hole transmission layer is organic material and/or inorganic material, and described organic material is selected from one or more in Spiro-MeOTAD, P3HT, PTAA, TAPC, NPB and TPD; Described inorganic material is selected from CuI, CuSCN, Cu 2one or more in O, CuO, NiO and MoOx.
8. perovskite solar cell as claimed in claim 1, is characterized in that, described top electrode is metal electrode or conductive carbon material electrode.
9. the preparation method of the arbitrary described perovskite solar cell of claim 1～8, comprises the following steps:
1) in substrate and transparency electrode, adopt electron transport material to prepare dense film, form electron transfer layer;
2) on electron transfer layer, utilize electron transport material to form the porous membrane of micro/nano level, then the perovskite structure photovoltaic material of growing, form electric transmission-light-absorption layer and on light-absorption layer, the surface topography of simultaneously controlling light-absorption layer is the zigzag of continuous densification;
3) at surperficial spin coating or the evaporation hole mobile material of light-absorption layer, form hole transport-light-absorption layer and on hole transmission layer;
4) on hole transmission layer, prepare top electrode.
10. preparation method as claimed in claim 9, it is characterized in that, in step 2) perovskite structure photovoltaic material grows in the hole of described porous membrane, form electric transmission-light-absorption layer, and the perovskite structure photovoltaic material of growing on described porous membrane forms light-absorption layer, by the grow upper surface topography of concentration regulation and control light-absorption layer of reaction solution of perovskite structure photovoltaic material of control, form fine and close continuously zigzag pattern.
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