CN103904224A - Organic photovoltaic cell based on inorganic quantum dot and preparing method - Google Patents
Organic photovoltaic cell based on inorganic quantum dot and preparing method Download PDFInfo
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Abstract
An organic photovoltaic cell based on an inorganic quantum dot comprises a positive electrode, a hole transmission layer, an organic light absorbing layer, an electronic modification layer and a negative electrode, all of which are stacked in sequence. The organic light absorbing layer comprises an acceptor material and a donor material. The organic photovoltaic cell is characterized in that the hole transmission layer is at least one layer of inorganic quantum dot thin film, and the absorption spectrum of the inorganic quantum dot is in the visible light range and is wider than the light absorption range of the organic light absorbing layer material. According to the organic photovoltaic cell, the corrosion to the electrodes of the hole transmission layer is prevented, the stability of the cell performance is improved, the inorganic quantum dot serves as the hole transmission layer and is beneficial for transmission of a carrier, the incident light can be effectively absorbed, and the stability of the cell is improved.
Description
Technical field
The present invention relates to a kind of organic photovoltaic battery, relate in particular to a kind of organic photovoltaic battery of inorganic-quantum-dot as decorative layer that adopt, the invention still further relates to a kind of preparation method of the organic photovoltaic battery based on inorganic-quantum-dot.
Background technology
Organic photovoltaic battery because its material source is extensive, lightweight, can large area produce and with flexible substrate mutually the feature such as compatible be subject to the extensive concern of domestic and international researcher.Organic photovoltaic devices performance can regulate and control by synthetic and design novel organic semi-conductor material.Based on these unique advantages, organic battery becomes one of field that group study is the most popular in recent ten years both at home and abroad.By the organic light absorbent of narrow band gap and the optimization to device architecture of synthesizing new, the efficiency of organic photovoltaic battery has exceeded 10% at present, is expected to realize business-like large-scale production.
One think diffusion that the opto-electronic conversion of organic photovoltaic battery comprises the absorption of photon and the formation of exciton, exciton with separate, transmission and the collection process of electric charge.In the time that solar irradiation is mapped to light-absorption layer, while only having photon energy to be greater than the energy gap of organic light absorbent, be just absorbed.Be subject to light activated electronics to transit to LUMO track from the HOMO track of organic material, at this moment stay hole in HOMO and electronics in being energized into LUMO and together with being strapped in tightly, form exciton due to the interaction of Coulomb force.The exciton that is not all generations in organic material can resolve into electronics and hole freely, only has and just can separate to suitable interface when exciton diffusion.When exciton diffusion or while moving to the interface with energy potential difference, just can overcome the binding energy of exciton, be separated into electronics and hole freely.Electronics after separation and hole under internal electric field or DC Electric Field respectively negative electrode and the anode to battery move, then collected by electrode.
In order to improve the photoelectric conversion efficiency of organic photovoltaic battery, prerequisite is the abundant absorption of light-absorption layer to incident sunlight, next being that the photoproduction exciton producing is effectively separated at interface energy, is finally that electronics and the cavity energy after separating is collected by electrode fast.The photoelectric conversion efficiency of these three process joint effect batteries.Can guarantee the enhancing of light to absorb although increase the thickness of light-absorption layer, because photoproduction exciton diffusion length is limited, so the increase of light-absorption layer thickness can cause most of photoproduction exciton producing not being diffused into body/acceptor separating interface to have fallen with regard to cancellation.
Because the intrinsic carrier mobility of organic semiconducting materials is low, the increase of light-absorption layer thickness is electronics and the increase of hole-recombination probability freely after easily causing separating, and can not get effective collection in addition.Although the bulk-heterojunction light-absorption layer structure based on inierpeneirating network structure can make the efficiency of photoproduction exciton greatly improve at present, charge carrier and charge transfer state are compound also have been increased thereupon, causes the decline of battery open circuit voltage.In order to strengthen the light absorption of battery, do not affect again transmission and the collection of charge carrier simultaneously, can be by replacement and the optimization of the decorative layer to battery, reach and both increase the object that battery light absorption strengthens, do not affect again the transmission of charge carrier, thereby finally improve the efficiency of battery.
Traditional organic battery structure is TCO/PEDOT at present: PSS/ light-absorption layer/decorative layer/negative electrode.Wherein PEDOT: PSS is hole transmission layer, mainly plays the effect of collecting hole, block electrons, avoids photo-generated carrier to occur in ITO/ active layer interface compound, reduces short circuit current and energy conversion efficiency.But, experimental results show that PEDOT: PSS is acid, and ITO electrode is had to corrosiveness, affect the stability of battery performance, and traditional PEDOT: PSS can not extinction.
The effective ways that solve stability test adopt a transition metal oxide, as MoO
3, V
2o
5, NiO, WO
3deng, replace PEDOT: PSS, solve the stability problem of electrode and hole transport bed boundary, play positive effect.As the application number Chinese invention patent application " a kind of organic molecule solar cell of reciprocal form structure " (application publication number is CN101997085A) that is CN201010504075.5 discloses a kind of organic molecule solar cell of reciprocal form structure, be included on the conductive layer of ito glass substrate and prepare successively cathodic modification layer, organic molecule electron acceptor film and electron donor film, anode modification layer and metal electrode, wherein anode modification layer, hole transmission layer is WO
3, replace conventional PEDOT: PSS, efficiently solve the contaminated problem of metal electrode, but battery efficiency has much room for improvement.
The Chinese invention patent application " a kind of organic solar batteries and preparation method thereof " (application publication number is CN103151463A) that and for example application number is CN201310063285.9 discloses a kind of organic solar batteries, it comprises electrically conducting transparent substrate, hole transmission layer, organic active layer, electron transfer layer, metal electrode, and wherein hole transmission layer is CuS.This invention is by traditional hole transmission layer PEDOT: PSS substitutes with CuS, has avoided the corrosiveness of hole transmission layer to conductive substrates, strengthened stability, but battery efficiency has much room for improvement.
There is bibliographical information: between polymer and inorganic, metal oxide, also have Photoinduced Charge transfer phenomena fast, such as at SnO
2, TiO
2, or ZnO and polymer between.The Chinese invention patent application " a kind of polymer solar battery " (application publication number is CN103280528A) that is CN201310172619.6 as application number discloses a kind of polymer solar battery, it comprises cathode layer, cathode interface layer, photosensitive layer, anodic interface layer and anode layer, wherein cathode interface layer is inorganic semiconductor nanocrystalline-Conjugated Polymer Composites layer, is specially poly-fluorenes (PFEP) composite layer of zinc oxide (ZnO)-phosphate.This invention by introducing poly-fluorenes (PFEP) the composite cathode boundary layer of zinc oxide (ZnO)-phosphate between cathode layer and photosensitive layer, can effectively increase the conductivity of cathode interface layer, the volume resistance that has reduced this cathode interface layer, is conducive to electric transmission and collection.
Therefore, utilize inorganic nano material to there is possibility as organic battery decorative layer, and these inorganic nano/polymer hetero-junction solar cells had both utilized advantages such as inorganic nano material chemical stability is good, carrier mobility is high, wide spectral absorption, retain again the feature of polymeric material high absorption coefficient and wet method processing.
Summary of the invention
Technical problem to be solved by this invention is to provide a kind of organic photovoltaic battery based on inorganic-quantum-dot that can effectively increase light absorption.
Another technical problem to be solved by this invention is to provide the organic photovoltaic battery based on inorganic-quantum-dot that a kind of performance is more stable.
Another technical problem to be solved by this invention is to provide a kind of preparation method of the organic photovoltaic battery based on inorganic-quantum-dot.
The present invention solves the problems of the technologies described above adopted technical scheme: a kind of organic photovoltaic battery based on inorganic-quantum-dot, comprise the anode, hole transmission layer, organic light-absorption layer, electronics decorative layer and the negative electrode that stack gradually, described organic light-absorption layer comprises acceptor material and donor material, it is characterized in that: described hole transmission layer is one deck inorganic-quantum-dot film at least, the absorption spectrum of described inorganic-quantum-dot is in visible-range and be greater than the extinction scope of organic light-absorption layer material.
The selection of inorganic-quantum-dot need meet: the band gap of described inorganic-quantum-dot is 0.5eV～2.5eV.
Further, the valence band of described inorganic-quantum-dot approaches the work function of anode, the absolute value≤0.3eV of the difference of both potential barriers, and, the valence band of described inorganic-quantum-dot approaches the highest molecular orbital energy level that is occupied of donor material, the absolute value≤0.3eV of the difference of both potential barriers.
Further, the conduction band of described inorganic-quantum-dot approaches the minimum molecular orbital energy level that is not occupied of acceptor material, the absolute value≤0.3eV of the difference of both potential barriers.
Described inorganic-quantum-dot is made up of II-VI family or IV-VI family element.
Preferably, described inorganic-quantum-dot is vulcanized lead (PbS), lead selenide (PbSe), selenium vulcanized lead (PbSSe) or cadmium selenide (CdSe).
Particle diameter≤the 100nm of described inorganic-quantum-dot.
Thickness≤the 300nm of described hole transmission layer.
In addition, the shape of inorganic-quantum-dot comprises spherical, rhombus, tetrahedral and various irregular geometric shapes.
The hole mobility that meets the hole transmission layer of above-mentioned condition is greater than 10
-4m
2/ (vs), be both conducive to the transmission of holoe carrier, can also realize the effective absorption to incident light wave band direction.
The thickness of described organic light-absorption layer is 50～300nm, and the thickness of described electronics decorative layer is 5～100nm, and the thickness of described negative electrode is 60～120nm.
The performance of organic photovoltaic battery determines by this five part of anode, hole transmission layer, organic light-absorption layer, electronics decorative layer and negative electrode is common, in order to coordinate above-mentioned hole transmission layer, to obtain the organic photovoltaic battery of performance the best, other five parts need meet the following conditions respectively:
Anode is deposited on transparent material substrate by nesa coating and forms, and transparent material substrate comprises glass and plastics etc., and light transmission rate is greater than 90%, and nesa coating comprises fluorine-doped tin oxide electro-conductive glass FTO (SnO
2: F), aluminium-doped zinc oxide electro-conductive glass AZO (ZnO: A1), tin-doped indium oxide electro-conductive glass ITO (In
2o
3: Sn) etc.;
Organic light-absorption layer is by gathering 3-hexyl thiophene phenol (P3HT), CuPc (CuPc), poly-[[9-(1-octyl group nonyl)-9H-carbazole-2,7-bis-bases]-2,5-thiophene two base-2,1,3-diazosulfide-4,7-bis-base-2,5-thiophene two bases] (PCDTBT) etc. the organic receptor material such as organic extinction donor material and C60, C70, C84 and derivative thereof form.Organic light-absorption layer comprises individual layer, electron donor and the electron acceptor planar heterojunction bilayer etc. of the bulk-heterojunction structure of electron donor and acceptor, and the thickness of organic light-absorption layer is 50～300nm;
Electronics decorative layer is material oxidation zinc ZnO, the titanium dioxide TiO that is conducive to battery transmission
2deng; Or blocking hole transferring material 2,9-dimethyl-4,7-diphenyl-1,10-luxuriant and rich with fragrance sound of vomiting quinoline (BCP), 4,7-diphenyl-1,10-luxuriant and rich with fragrance sound of vomiting quinoline (Bphen) etc., thickness is 5～100nm;
Cathode material is the high reflecting metals such as aluminium, silver, and thickness is 60～120nm.
A kind of preparation method of organic photovoltaic battery, be included in and on anode, prepare hole transmission layer, on hole transmission layer, prepare organic light-absorption layer, on organic light-absorption layer, prepare electronics decorative layer, and prepare negative electrode on electronics decorative layer, it is characterized in that: adopt spin-coating method that inorganic-quantum-dot is covered at anode surface, form hole transmission layer, spin coating rotating speed is 1000～5000rpm, and the spin coating time is 10～60s.The selection matching standard of spin coating rotating speed and spin coating time is to make each spin coating thickness≤50nm.The preparation of organic light-absorption layer, electronics decorative layer and negative electrode can adopt the routine techniques such as spin-coating method or vapour deposition method, also can adopt other technologies.
Compared with prior art, the invention has the advantages that: the hole transmission layer in organic photovoltaic battery is specially at least inorganic-quantum-dot film of one deck, replace traditional PEDOT: PSS (poly-3,4-ethylenedioxy thiophene/poly styrene sulfonate), not only prevent the corrosion of hole transmission layer to electrode, thereby improve the stability of battery performance, and inorganic-quantum-dot is conducive to the transmission of charge carrier as hole transmission layer, can also increase the effective absorption to incident light, improve the stability of battery.In addition, the hole decorative layer being made up of inorganic-quantum-dot film is prepared simple, easy to operate, has retained the feature of organic photovoltaic battery wet method processing simultaneously.
Accompanying drawing explanation
Fig. 1 is the structural representation of embodiment 1 organic photovoltaic battery;
Fig. 2 be Fig. 1 organic photovoltaic battery can be with schematic diagram.
Embodiment
Below in conjunction with accompanying drawing, embodiment is described in further detail the present invention.
Embodiment 1:
The organic photovoltaic battery of the present embodiment, as shown in Figure 1, comprise the anode 2, hole transmission layer 3, organic light-absorption layer 4, electronics decorative layer 5 and the negative electrode 6 that stack gradually, wherein hole transmission layer 3 is inorganic-quantum-dot film, be specially PbS quantum dot decorative layer, organic light-absorption layer 4 comprises acceptor material polythiophene (P3HT) and donor material fullerene derivate [6,6]-phenyl-C61 methyl butyrate (PCBM), electronics decorative layer 5 is BCP, anode 2 is for being deposited on the FTO in transparent substrates 1, and negative electrode 6 is aluminium electrode.
The preparation method of the present embodiment organic photovoltaic battery, step is as follows:
1) anode using transparent conducting film glass (FTO) substrate as organic battery is clean in deionized water, ethanol and acetone ultrasonic cleaning respectively;
2) adopt spin-coating method to prepare PbS quantum dot decorative layer at dried anode surface, as hole transmission layer, its spin coating liquid is gluey PbS nanocrystal solution, spin coating number of times 10 times, inorganic-quantum-dot overall film thickness 200nm.
3) the inorganic-quantum-dot film surface preparing, prepare polythiophene and fullerene derivate (P3HT: PCBM) as organic light-absorption layer by spin-coating method, wherein P3HT: PCBM weight ratio is 1: 0.8, be dissolved in the chlorobenzene that concentration is 12mg/ml, the rotating speed 300rpm of spin coating, time 12s, the about 200nm of thickness of organic light-absorption layer;
4), on the acceptor material surface preparing, prepare BCP as electronics decorative layer by vapour deposition method, the about 10nm of thickness;
5) adopt vapour deposition method to prepare aluminium as back electrode, the about 100nm of thickness of electrode.
Being with as shown in Figure 2 of this enforcement organic photovoltaic battery, inorganic-quantum-dot is specially PbS, and particle diameter is 10～15nm, and band gap is 1.4eV, and conduction band 3a is 3.5eV, valence band 3b is 4.9eV; Anode is FTO electro-conductive glass, and anode work function 2a is 4.64eV; Organic light-absorption layer is P3HT: PCBM, the HOMO energy level 4b of donor material P3HT is 5.1eV, the lumo energy 4a of acceptor material PCBM is 3.7eV, the barrier potential difference of the valence band of PbS and anode FTO is 0.3eV, the lumo energy 4a barrier potential difference of the conduction band 3a of PbS and acceptor material PCBM is 0.2eV, and the HOMO energy level 4b barrier potential difference of the valence band 3b of PbS and donor material P3HT is 0.2eV.In Fig. 2,6a is representing negative electrode work function position.
Embodiment 2
The organic photovoltaic battery of the present embodiment structurally difference from Example 1 is: anode is AZO; Inorganic-quantum-dot is PbS
0.5se
0.5, thickness is 150nm; The thickness of organic light-absorption layer is 150nm; Electronics decorative layer is lithium fluoride LiF, and thickness is 1nm; Negative electrode is silver electrode.
The preparation method of the present embodiment organic photovoltaic battery, step is as follows:
1) anode using transparent conducting film glass (AZO) substrate of matte as organic battery, clean in deionized water, ethanol and acetone ultrasonic cleaning respectively;
2) adopt spin-coating method to prepare PbS on dried incident electrode surface
0.5se
0.5quantum dot decorative layer, as hole decorative layer, its spin coating liquid is gluey PbS
0.5se
0.5nanocrystal solution.Spin coating number of times 5 times, inorganic-quantum-dot overall film thickness 150nm.
3) the inorganic-quantum-dot film surface preparing, prepare polythiophene and fullerene derivate (P3HT: PCBM) as organic light-absorption layer by spin-coating method, wherein P3HT: PCBM weight ratio is 1: 0.8, be dissolved in the chlorobenzene that concentration is 10mg/ml, the rotating speed 300rpm of spin coating, time 12s, the about 150nm of thickness of organic light-absorption layer;
4), on the acceptor material surface preparing, prepare LiF as electronics decorative layer by vapour deposition method, the about 1nm of thickness;
5) adopt vapour deposition method to prepare Ag as back electrode, the about 100nm of thickness of electrode.
In this enforcement organic photovoltaic battery, inorganic-quantum-dot is specially PbS
0.5se
0.5, particle diameter is 10～15nm, and band gap is 1.3eV, and conduction band is 3.6eV, and valence band is 4.9eV; Anode is AZO electro-conductive glass, and work function is 5.05eV, PbS
0.5se
0.5with the barrier potential difference of anode A ZO be 0.15eV, PbS
0.5se
0.5conduction band and the lumo energy barrier potential difference of acceptor material PCBM be 0.1eV, PbS
0.5se
0.5valence band and the HOMO energy level barrier potential difference of donor material P3HT be 0.2eV.
Embodiment 3
The organic photovoltaic battery of the present embodiment structurally difference from Example 1 is: anode is ITO; The thickness of inorganic-quantum-dot film is 100nm; Organic light-absorption layer is CuPc: C60, and thickness is 60nm; Electronics decorative layer is C60, and thickness is 30nm; Negative electrode is silver electrode.
The preparation method of the organic photovoltaic battery of the present embodiment, step is as follows:
1) anode using transparent conducting film glass (ITO) substrate of matte as organic battery, clean in deionized water, ethanol and acetone ultrasonic cleaning respectively;
2) adopt spin-coating method to prepare PbS quantum dot decorative layer on dried incident electrode surface, as hole decorative layer, its spin coating liquid is gluey PbS nanocrystal solution, spin coating number of times 7 times, inorganic-quantum-dot overall film thickness 100nm.
3) at the inorganic-quantum-dot film surface preparing, the mixture by common steaming organic molecule P-type material titan bronze CuPc and N-shaped material fullerene C60 is as organic light-absorption layer, the about 60nm of thickness;
4) on organic light-absorption layer, prepare fullerene N-shaped material C 60 as electronics decorative layer by vapour deposition method again, the about 30nm of thickness;
5) adopt vapour deposition method to prepare Ag as back electrode, thickness is about 100nm.
In this enforcement organic photovoltaic battery, organic light-absorption layer is CuPc: C60, and anode is ITO electro-conductive glass, and work function is about 4.9eV.The HOMO energy level of donor material CuPc in organic light-absorption layer is 5.2eV, the lumo energy of acceptor material C60 is 3.8eV, the barrier potential difference of PbS valence band and anode ITO is 0.3eV, the lumo energy barrier potential difference of the conduction band of PbS and acceptor material C60 is 0.3eV, and the HOMO energy level barrier potential difference of the valence band of PbS and donor material CuPc is 0.3eV.
Comparative example 1
The present embodiment difference from Example 1 is: hole decorative layer is PEDOT: PSS, and other are all consistent.
Comparative example 2
The present embodiment difference from Example 2 is: hole decorative layer is PEDOT: PSS, and other are all consistent.
Comparative example 3
The present embodiment difference from Example 3 is: hole decorative layer is PEDOT: PSS, and other are all consistent.
The performance of above-described embodiment organic photovoltaic battery is as shown in the table:
As can be seen from the above table:
1, in embodiment 1, utilize inorganic-quantum-dot film PbS to replace decorative layer PEDOT: PSS, battery short circuit current density has increased by 28.4%, and this gives the credit to the absorption of PbS quanta point material to incident sunlight, and the separation of charge at PbS/PCBM interface increases the electric current of battery.Although battery open press and fill factor, curve factor decline to some extent, the efficiency of integral battery door is still improved.Experimental result also shows FTO/PbS/P3HT: the stability test of PCBM/BCP/A1 structure significantly improves.
2, in embodiment 2, utilize inorganic-quantum-dot film PbSSe to replace decorative layer PEDOT: PSS, battery short circuit current density has increased by 20.4%, and this gives the credit to the absorption of PbSSe quanta point material to incident sunlight, and the separation of charge at PbSSe/PCBM interface increases the electric current of battery.Although battery open press and fill factor, curve factor decline to some extent, the efficiency of integral battery door is slightly improved.Experimental result also shows AZO/PbSSe/P3HT: the stability test of PCBM/LiF/A1 structure significantly improves.
3, in embodiment 3, utilize inorganic-quantum-dot film PbS to replace decorative layer PEDOT: PSS, battery short circuit current density has increased by 25.3%, and this gives the credit to the absorption of PbS quanta point material to incident sunlight, and the separation of charge at PbS/C60 interface increases the electric current of battery.The efficiency of integral battery door improves 24.7%.Experimental result also shows ITO/PbS/CuPc: the stability test of C60/C60/Ag structure significantly improves.
Claims (10)
1. the organic photovoltaic battery based on inorganic-quantum-dot, comprise the anode, hole transmission layer, organic light-absorption layer, electronics decorative layer and the negative electrode that stack gradually, described organic light-absorption layer comprises acceptor material and donor material, it is characterized in that: described hole transmission layer is one deck inorganic-quantum-dot film at least, the absorption spectrum of inorganic-quantum-dot is in visible-range and be greater than the extinction scope of organic light-absorption layer material.
2. the organic photovoltaic battery based on inorganic-quantum-dot according to claim 1, is characterized in that: the band gap of described inorganic-quantum-dot is 0.5eV～2.5eV.
3. the organic photovoltaic battery based on inorganic-quantum-dot according to claim 2, it is characterized in that: the valence band of described inorganic-quantum-dot approaches the work function of anode, absolute value≤the 0.3eV of the difference of both potential barriers, and, the valence band of described inorganic-quantum-dot approaches the highest molecular orbital energy level that is occupied of donor material, the absolute value≤0.3eV of the difference of both potential barriers.
4. according to the organic photovoltaic battery based on inorganic-quantum-dot described in claim 2 or 3, it is characterized in that: the conduction band of described inorganic-quantum-dot approaches the minimum molecular orbital energy level that is not occupied of acceptor material, the absolute value≤0.3eV of the difference of both potential barriers.
5. the organic photovoltaic battery based on inorganic-quantum-dot according to claim 1, is characterized in that: described inorganic-quantum-dot is made up of II-VI family or IV-VI family element.
6. the organic photovoltaic battery based on inorganic-quantum-dot according to claim 5, is characterized in that: described inorganic-quantum-dot is vulcanized lead, lead selenide, selenium vulcanized lead or cadmium selenide.
7. the organic photovoltaic battery based on inorganic-quantum-dot according to claim 1, is characterized in that: the particle diameter≤100nm of described inorganic-quantum-dot.
8. the organic photovoltaic battery based on inorganic-quantum-dot according to claim 1, is characterized in that: the thickness≤300nm of described hole transmission layer.
9. the organic photovoltaic battery based on inorganic-quantum-dot according to claim 1, is characterized in that: the thickness of described organic light-absorption layer is 50～300nm, and the thickness of described electronics decorative layer is 5～100nm, and the thickness of described negative electrode is 60～120nm.
10. the preparation method of the organic photovoltaic battery described in any one in a claim 1 to 9, be included in and on anode, prepare hole transmission layer, on hole transmission layer, prepare organic light-absorption layer, on organic light-absorption layer, prepare electronics decorative layer, and prepare negative electrode on electronics decorative layer, it is characterized in that: adopt spin-coating method that inorganic-quantum-dot is covered at anode surface, form hole transmission layer, spin coating rotating speed is 1000～5000rpm, and the spin coating time is 10～60s, each spin coating thickness≤50nm.
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| CN109004048A (en) * | 2018-07-25 | 2018-12-14 | 合肥工业大学 | A kind of preparation method of the inorganic perovskite quantum dot film of caesium lead bromine and photovoltaic device based on it |
| CN109935698A (en) * | 2019-03-30 | 2019-06-25 | 华南理工大学 | One kind is with In2Se3For the organic solar batteries and preparation method thereof of hole transmission layer |
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| CN111443579A (en) * | 2020-04-29 | 2020-07-24 | Tcl华星光电技术有限公司 | Exposure machine, preparation method and use method thereof |
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