CN110459682A - A kind of polymer solar battery and preparation method thereof based on polyethyleneglycol modified zinc oxide electron-transport layer building flexible structure - Google Patents
A kind of polymer solar battery and preparation method thereof based on polyethyleneglycol modified zinc oxide electron-transport layer building flexible structure Download PDFInfo
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- CN110459682A CN110459682A CN201910701604.1A CN201910701604A CN110459682A CN 110459682 A CN110459682 A CN 110459682A CN 201910701604 A CN201910701604 A CN 201910701604A CN 110459682 A CN110459682 A CN 110459682A
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- zinc oxide
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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
- H10K30/30—Organic devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation comprising bulk heterojunctions, e.g. interpenetrating networks of donor and acceptor material domains
- H10K30/35—Organic devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation comprising bulk heterojunctions, e.g. interpenetrating networks of donor and acceptor material domains comprising inorganic nanostructures, e.g. CdSe nanoparticles
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- 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
- H10K71/10—Deposition of organic active material
- H10K71/12—Deposition of organic active material using liquid deposition, e.g. spin coating
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- H—ELECTRICITY
- H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
- H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
- H10K2102/00—Constructional details relating to the organic devices covered by this subclass
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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
Abstract
The present invention relates to polymer solar battery fields, particularly disclose a kind of polymer solar battery and preparation method thereof based on polyethyleneglycol modified zinc oxide electron-transport layer building flexible structure.The polymer solar battery, it is characterised in that: be followed successively by the flexible and transparent substrate with OMO electrode, polyethyleneglycol modified zinc oxide electron transfer layer, non-fullerene system photoactive layer, Hole-injecting Buffer Layer for Improvement and anode electrode from bottom to top；Polyethylene glycol thin layer is covered on zinc oxide electron transfer layer.The present invention passes through the modification of polyethylene glycol thin layer, inhibit electrons and holes in the probability of recombination of zinc oxide electron-transport layer surface, the extraction efficiency of charge is improved, while improving the photoelectric current and fill factor of battery device, the final incident photon-to-electron conversion efficiency for improving battery device.
Description
(1) technical field
It is the present invention relates to polymer solar battery field, in particular to a kind of to be passed based on polyethyleneglycol modified zinc oxide electronics
The polymer solar battery and preparation method thereof of defeated layer building flexible structure.
(2) background technique
With the exhaustion of fossil energy and getting worse for environmental pollution, the reproducible energy of development and utilization cleaning is extremely urgent,
Wherein solar energy cleans, is renewable, being convenient for local use, is the emphasis of various countries' research.Solar battery is the development and utilization sun
Can core equipment, polymer solar battery compared to inorganic solar cell have light, manufacture craft it is simple, it is cheap,
The advantages that rollable, however the problems such as its current photoelectric conversion efficiency and stability, still limits its industrialized production.
To pursue high incident photon-to-electron conversion efficiency, currently, polymer solar battery is mostly in hard glass/indium tin oxide transparent
Constructed in substrate, although this obtains higher photoelectric conversion efficiency, with its pursued it is light, rollable the advantages that phase
It is contrary to.Thus, it is more meaningful that polymer solar battery is constructed in flexible and transparent substrate.In order to make between photoactive layer and electrode
Form ideal Ohmic contact, it usually needs electron transfer layer is inserted between photoactive layer and cathode, in photoactive layer and sun
Hole transmission layer is inserted between pole.Electron transport layer materials are usually ZnO, TiO2Equal transparent oxide semiconductors material, however
When ZnO is as electron transfer layer, surface defect be easy to cause the compound again of electrons and holes, to reduce the extraction effect of charge
Rate.To make up its surface defect, generallys use the modifying interfaces such as chemically synthesized PFN or PFN-Br material and its surface is repaired
Decorations, can significantly improve the photoelectric conversion performance of device.But the materials synthesis step such as PFN, PFN-Br is more, more complex, because
And it finds alternative cheap modifying interface material and has great importance.
(3) summary of the invention
That in order to compensate for the shortcomings of the prior art, the present invention provides a kind of absorbing properties is good, incident photon-to-electron conversion efficiency it is high based on
The polymer solar battery and preparation method thereof of polyethyleneglycol modified zinc oxide electron-transport layer building flexible structure.
The present invention is achieved through the following technical solutions:
A kind of polymer solar battery based on polyethyleneglycol modified zinc oxide electron-transport layer building flexible structure, it is special
Sign is: being followed successively by the flexible and transparent substrate with OMO electrode, polyethyleneglycol modified zinc oxide electron-transport from bottom to top
Layer, non-fullerene system photoactive layer, Hole-injecting Buffer Layer for Improvement and anode electrode；It is thin that polyethylene glycol is covered on zinc oxide electron transfer layer
Layer.
The present invention passes through modification of the polyethylene glycol thin layer to zinc oxide electron transfer layer, it is suppressed that electrons and holes are aoxidizing
The probability of recombination of zinc electron-transport layer surface, improves the extraction efficiency of charge, finally obtains flexible battery device higher
Photoelectric conversion efficiency.
More excellent technical solution of the invention are as follows:
The flexible and transparent substrate is PET film.
The OMO electrode is the three-decker electrode of sandwiched metal layer among two oxide skin(coating)s, wherein the metal layer material
Material is Au, Ag or Cu, with a thickness of 5-10nm；The material of oxide skin(coating) is metal oxide semiconductor；OMO structure electrode is visible
While light area keeps high light transmitance, higher charge transfer efficiency is kept.
The zinc oxide electron transfer layer includes Zinc oxide nanoparticle layer and polyethylene glycol thin layer, wherein zinc oxide nano
Rice grain layer with a thickness of 30nm, zinc oxide is graininess, partial size 4nm, polyethylene glycol thin layer with a thickness of 5-10nm.It is logical
It crosses polyethyleneglycol modified zinc oxide electron transfer layer further to modify flexible battery device architecture, electronics can be significantly improved
Extraction and transport efficiency.
The non-fullerene system photoactive layer with a thickness of 100nm, wherein donor material be mid-gap polymer give
Body material J71 or J61, acceptor material are non-fullerene fused-ring derivatives ITIC or ITIC-m, donor material and acceptor material
Blending ratio is 1:1.
The material of the Hole-injecting Buffer Layer for Improvement is MoO3, with a thickness of 10nm；The material of anode electrode is Ag, with a thickness of 100nm.
The preparation method of above-mentioned polymer solar battery, includes the following steps:
(1) OMO cathode electrode is sputtered in flexible and transparent substrate by magnetron sputtering method；
(2) direct one layer of zinc oxide thin layer of spin coating on OMO cathode electrode, in zinc oxide films layer surface spin coating polyethylene glycol ethyl alcohol
Solution, then anneal at 60 DEG C 10min, forms polyethyleneglycol modified zinc oxide electron transfer layer；
(3) with the speed spin coating photoactive layer solution 60s of 1200-1400rpm in the glove box of nitrogen protection；
(4) in vacuum coating equipment, by the MoO of 10nm3It is deposited on photoactive layer respectively with the Ag anode of 100nm, true
Empty≤5 × 10-4Anode is formed under Pa.
In step (2), after washing of precipitate, be distributed to volume ratio is the Zinc oxide nanoparticle made from the liquid phase reduction
The n-butanol of 60:35:5, methanol, chloroform mixed solution in, the concentration of zinc oxide thin layer of solution is 10mg/mL；Polyethylene glycol
The concentration of ethanol solution is 0.1-0.2mg/mL, and the molecular weight of polyethylene glycol is 4000-8000, zinc oxide films layer surface with
The speed spin coating polyethylene glycol ethanol solution of 3000rpm.
In step (3), photoactive layer solution is that the donor material that mass ratio is 1:1 and acceptor material mix in chlorobenzene solution
Close obtained polymer blend solution, concentration 9-10mg/mL；The 1 of 1.5vol% is also added in polymer blend solution,
8- diiodo-octane.
The present invention passes through the modification of polyethylene glycol thin layer, it is suppressed that electrons and holes are in zinc oxide electron-transport layer surface
The probability of recombination, improves the extraction efficiency of charge, while improving the photoelectric current and fill factor of battery device, finally improves battery
The incident photon-to-electron conversion efficiency of device.
(4) Detailed description of the invention
The present invention will be further described below with reference to the drawings.
Fig. 1 is the structural diagram of the present invention;
Fig. 2 is the photovoltaic property curve of polymer solar battery polyethyleneglycol modified and unmodified in the embodiment of the present invention 1.
In figure, 1 flexible and transparent substrate, 2 OMO electrodes, 3 zinc oxide electron transfer layers, 4 non-fullerene system photoactive layers,
5 Hole-injecting Buffer Layer for Improvement, 6 anode electrodes.
(5) specific embodiment
The present invention will be further explained below with reference to the attached drawings.
It is a kind of soft based on polyethyleneglycol modified zinc oxide electron-transport layer building technical program of the present invention lies in providing
The polymer solar battery and preparation method thereof of property structure, as shown in Fig. 1, battery structure includes flexible and transparent substrate 1,
OMO electrode 2, polyethyleneglycol modified zinc oxide electron transfer layer 3, non-fullerene system photoactive layer 4, Hole-injecting Buffer Layer for Improvement 5, sun
Pole electrode 6.
Flexible and transparent substrate 1 of the invention is flexible the polymeric substrates such as PET, PC, as flexible polymer solar
The substrate of battery, it is desirable that it has higher transmitance within the scope of near ultraviolet, visible light, near infrared region, can with blocking oxygen and
Water, and flatness is higher.
Cathode electrode of the invention is OMO electrode 2, is three-decker electrode, and wherein oxide is ZnO, TiO2Deng partly leading
Body metal oxide, metal layer Au, Ag, Cu etc., metal layer thickness are about 5-10nm, and OMO electrode 2 is in visible wavelength range
While interior holding high light transmitance, while keeping higher conductivity.
Zinc oxide electron transfer layer 3 of the invention is made of Zinc oxide nanoparticle layer, polyethylene glycol thin layer.Wherein, oxygen
The ZnO for changing zinc nanoparticles layer is graininess, and size is about 4nm, and Zinc oxide nanoparticle thickness degree is about 30nm, polyethylene glycol
Thickness of thin layer is about 5-10nm.By certain density polyethylene glycol ethanol solution, by spin coating method, in Zinc oxide nanoparticle
One strata ethylene glycol thin layer of spin coating, low-temperature annealing on layer.
Non- fullerene system photoactive layer 4 of the invention by polymer donor material, non-fullerene acceptor material mixing and
At.Polymer donor material such as J71, J61 etc. have unsaturated structure in structure, band gap is moderate, with non-fullerene acceptor material
Expect that extinction is complementary, and energy match, visible light can be absorbed and generate exciton.Acceptor material be non-fullerene fused-ring derivatives such as
ITIC, ITIC-m etc. have energy level adjustable relative to fullerene acceptor material, and light absorption range is wide, is blended with donor material surely
The advantages that qualitative good, therefore can be with the higher more stable flexible polymer solar battery device of producing efficiency.
Hole-injecting Buffer Layer for Improvement 5 of the invention is MoO3, it is in vacuum evaporation equipment, forming a layer thickness by vapor deposition is about
The hole transmission layer of 10nm.
Anode electrode 6 of the invention is Ag, and good conductivity, work function is higher, high stability.
Embodiment 1:
Structure such as Fig. 1 based on polyethyleneglycol modified zinc oxide electron-transport layer building flexible structure polymer solar battery
It is shown.In figure, 1 is flexibility PET transparent substrates；2 cathode electrodes are OMO conductive electrode, are made of ZnO/Ag/ZnO, thickness difference
For 60nm, 10nm, 50nm；Contain ZnO nano stratum granulosum thickness about 30nm in zinc oxide electron transfer layer 3 and thickness is about 10nm
Polyethyleneglycol modified layer.Donor material is J71 in non-fullerene system photoactive layer 4, and non-fullerene acceptor material is ITIC,
Photoactive layer 4 with a thickness of 100nm；Hole-injecting Buffer Layer for Improvement 5 is MoO3, with a thickness of 10nm；Anode electrode 6 is Ag, with a thickness of
100nm。
Its specifically the production method is as follows:
(1) the OMO electrode 2 in flexibility PET transparent substrates 1 is obtained by magnetron sputtering method, and PET/OMO substrate is without cleaning, in OMO
Direct one layer of zinc oxide electron transfer layer 3 of spin coating on electrode 2；
(2) ZnO nano particle is made by liquid phase reduction, after multiple washing of precipitate, redisperse to n-butanol, methanol, chlorine
In imitative mixed solution (volume ratio 60:35:5), burnett's solution concentration is about 10mg/ml.Polyethylene glycol ethanol solution is prepared,
Concentration is 0.2mg/ml, molecular weight polyethylene glycol 8000；In zinc oxide films layer surface with 3000rpm speed spin coating polyethylene glycol
Ethanol solution, then 60 DEG C of annealing 10min, form polyethyleneglycol modified zinc oxide electron transfer layer 3；Substrate is transferred to nitrogen
The preparation of photoactive layer 4 is carried out in the glove box of protection；
(3) photoactive layer solution is made of J71, ITIC, and the mass ratio of J71 and ITIC in chlorobenzene solution is 1:1, polymer
Concentration is 9mgmL-1.In addition, 1, the 8- diiodo-octane (DIO) of 1.5vol% is added in light active material blend solution,
To form the ideal interpenetrating networks with suitable donor and receptor size range in active layer, spin coating is with 1200-
1400rpm spin coating 60s；
(4) in vacuum coating equipment, by the MoO of 10nm3It is deposited on photoactive layer 4 respectively with the Ag anode of 100nm, true
Empty≤5 × 10-4Anode is formed under Pa；
(5) incident photon-to-electron conversion efficiency of prepared flexible polymer solar battery is tested, corresponding I-V curve is as shown in Figure 2.
The incident photon-to-electron conversion efficiency that Fig. 2 corresponds to polyethyleneglycol modified and unmodified battery is not 6.04% and 4.78%, is repaired through polyethylene glycol
After decorations, device efficiency is obviously improved, and is mainly reflected in fill factor and is promoted by 51.43% to 57.52%, current density by
15.78mAcm-1Promote 16.87mAcm-1.Fill factor and being obviously improved for current density prove that polyethyleneglycol modified ZnO can
Its surface defect is mended to play, inhibits electron hole compound effect again.
Embodiment 2:
Structure such as Fig. 1 based on polyethyleneglycol modified zinc oxide electron-transport layer building flexible structure polymer solar battery
It is shown.1 is the transparent base flexibility PET in figure；2 cathode electrodes are OMO conductive electrode, are made of ZnO/Ag/ZnO, thickness difference
For 60nm, 10nm, 50nm；The poly- second for being about 5nm containing ZnO nano stratum granulosum thickness about 30nm and thickness in electron transfer layer 3
Glycol decorative layer.Donor material is J61 in photoactive layer 4, and non-fullerene acceptor material is ITIC-m, the thickness of photoactive layer 4
For 100nm；Hole-injecting Buffer Layer for Improvement 5 is MoO3, with a thickness of 10nm；Anode electrode 6 is Ag, with a thickness of 100nm.
Its specifically the production method is as follows:
(1) the OMO electrode 2 in flexibility PET transparent substrates 1 is obtained by magnetron sputtering method, and PET/OMO substrate is without cleaning, in OMO
Direct one layer of electron transfer layer 3 of spin coating on electrode 2；
(2) ZnO nano particle is made by liquid phase reduction, after multiple washing of precipitate, redisperse to n-butanol, methanol, chlorine
In imitative mixed solution (volume ratio 60:35:5), burnett's solution concentration is about 10mg/ml.Polyethylene glycol ethanol solution is prepared,
Concentration is 0.1mg/ml, molecular weight polyethylene glycol 4000.In zinc oxide films layer surface with 3000rpm speed spin coating polyethylene glycol
Ethanol solution, then 60 DEG C of annealing 10min, form polyethyleneglycol modified zinc oxide electron transfer layer；Substrate is transferred to nitrogen
The preparation of photoactive layer 4 is carried out in the glove box of protection；
(3) photoactive layer solution is made of J61, ITIC-m, and the mass ratio of J61 and ITIC-m in chlorobenzene solution is 1:1, is gathered
Conjunction object concentration is 10mgmL-1.In addition, it is molten that 1, the 8- diiodo-octane (DIO) of 1.5vol% is added to light active material blend
In liquid, in active layer formed have suitable donor and receptor size range ideal interpenetrating networks, spin coating be with
1200-1400rpm spin coating 60s；
(4) in vacuum coating equipment, by the MoO of 10nm3It is deposited on active layer respectively with the Ag anode of 100nm, in vacuum
≤5×10-4Anode is formed under Pa；
(5) device efficiency after tested, the fill factor and current density for introducing device after polyethylene glycol are obviously improved, to be promoted
Integral battery incident photon-to-electron conversion efficiency.
Claims (10)
1. a kind of polymer solar battery based on polyethyleneglycol modified zinc oxide electron-transport layer building flexible structure,
It is characterized in that: being followed successively by the flexible and transparent substrate (1) with OMO electrode (2), polyethyleneglycol modified zinc oxide electricity from bottom to top
Sub- transport layer (3), non-fullerene system photoactive layer (4), Hole-injecting Buffer Layer for Improvement (5) and anode electrode (6)；Zinc oxide electron-transport
Polyethylene glycol thin layer is covered on layer (3).
2. the polymerization according to claim 1 based on polyethyleneglycol modified zinc oxide electron-transport layer building flexible structure
Object solar battery, it is characterised in that: the flexible and transparent substrate (1) is PET film.
3. the polymerization according to claim 1 based on polyethyleneglycol modified zinc oxide electron-transport layer building flexible structure
Object solar battery, it is characterised in that: the OMO electrode (2) is the three-layered node of sandwiched metal layer among two inorganic oxide layers
Structure electrode.
4. the polymerization according to claim 1 based on polyethyleneglycol modified zinc oxide electron-transport layer building flexible structure
Object solar battery, it is characterised in that: the zinc oxide electron transfer layer (3) includes Zinc oxide nanoparticle layer and polyethylene glycol
Thin layer, wherein Zinc oxide nanoparticle layer with a thickness of 30nm, zinc oxide is graininess, partial size 4nm, polyethylene glycol thin layer
With a thickness of 5-10nm.
5. the polymerization according to claim 1 based on polyethyleneglycol modified zinc oxide electron-transport layer building flexible structure
Object solar battery, it is characterised in that: the non-fullerene system photoactive layer (4) with a thickness of 100nm, wherein donor material
Material be mid-gap polymer donor material J71 or J61, acceptor material be non-fullerene fused-ring derivatives ITIC or ITIC-m,
The blending ratio of donor material and acceptor material is 1:1.
6. the polymerization according to claim 1 based on polyethyleneglycol modified zinc oxide electron-transport layer building flexible structure
Object solar battery, it is characterised in that: the material of the Hole-injecting Buffer Layer for Improvement (5) is MoO3, with a thickness of 10nm；Anode electrode (6)
Material be Ag, with a thickness of 100nm.
7. the polymerization according to claim 3 based on polyethyleneglycol modified zinc oxide electron-transport layer building flexible structure
Object solar battery, it is characterised in that: the metal layer material is Au, Ag or Cu, with a thickness of 5-10nm；The material of oxide skin(coating)
For metal oxide semiconductor.
8. the polymerization according to claim 1 based on polyethyleneglycol modified zinc oxide electron-transport layer building flexible structure
The preparation method of object solar battery, it is characterized in that, include the following steps: (1) by magnetron sputtering method in flexible and transparent substrate
Upper sputtering OMO cathode electrode；(2) direct one layer of zinc oxide thin layer of spin coating on OMO cathode electrode is revolved in zinc oxide films layer surface
Polyethylene glycol ethanol solution is applied, then anneal at 60 DEG C 10min, forms polyethyleneglycol modified zinc oxide electron transfer layer；
(3) with the speed spin coating photoactive layer solution 60s of 1200-1400rpm in the glove box of nitrogen protection；(4) in vacuum coating
In equipment, by the MoO of 10nm3It is deposited on photoactive layer respectively with the Ag anode of 100nm, in vacuum≤5 × 10-4It is formed under Pa
Anode.
9. preparation method according to claim 8, it is characterised in that: in step (2), through being aoxidized made from liquid phase reduction
Zinc nanoparticles are distributed in the mixed solution of n-butanol, methanol, chloroform that volume ratio is 60:35:5, oxygen after washing of precipitate
The concentration for changing zinc thin layer of solution is 10mg/mL；The concentration of polyethylene glycol ethanol solution is 0.1-0.2mg/mL, point of polyethylene glycol
Son amount is 4000-8000, in zinc oxide films layer surface with the speed spin coating polyethylene glycol ethanol solution of 3000rpm.
10. preparation method according to claim 8, it is characterised in that: in step (3), photoactive layer solution is mass ratio
For the polymer blend solution that the donor material and acceptor material of 1:1 are mixed to get in chlorobenzene solution, concentration 9-10mg/
mL；The 1,8- diiodo-octane of 1.5vol% is also added in polymer blend solution.
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