CN110459681A - Polymer solar battery and preparation method thereof based on the amine-modified zinc oxide electron-transport layer building flexible structure of polyethyleneimine - Google Patents
Polymer solar battery and preparation method thereof based on the amine-modified zinc oxide electron-transport layer building flexible structure of polyethyleneimine Download PDFInfo
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- CN110459681A CN110459681A CN201910700801.1A CN201910700801A CN110459681A CN 110459681 A CN110459681 A CN 110459681A CN 201910700801 A CN201910700801 A CN 201910700801A CN 110459681 A CN110459681 A CN 110459681A
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- H10K30/00—Organic devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation
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- H—ELECTRICITY
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- 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 of zinc oxide electron-transport layer building flexible structure amine-modified based on polyethyleneimine.The polymer solar battery, it is characterised in that: be followed successively by from bottom to top with the amine-modified zinc oxide electron transfer layer of the flexible and transparent substrate of OMO electrode, polyethyleneimine, non-fullerene system photoactive layer, Hole-injecting Buffer Layer for Improvement and anode electrode；Polyethyleneimine thin layer is covered on zinc oxide electron transfer layer.Rationally, preparation step is simple, by the modification of polyethyleneimine thin layer, while improving the absorbing properties and fill factor of flexible battery device, and then improve the incident photon-to-electron conversion efficiency of polymer solar battery for structure of the invention design.
Description
(1) technical field
The present invention relates to polymer solar battery field, in particular to a kind of zinc oxide electronics amine-modified based on polyethyleneimine
Transmit the polymer solar battery and preparation method thereof of 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
In order to compensate for the shortcomings of the prior art, the present invention provides a kind of structurally reasonable, preparations simply, photoelectric conversion efficiency is high
Polymer solar battery and its preparation side based on the amine-modified zinc oxide electron-transport layer building flexible structure of polyethyleneimine
Method.
The present invention is achieved through the following technical solutions:
A kind of polymer solar battery of the zinc oxide electron-transport layer building flexible structure amine-modified based on polyethyleneimine,
It is characterized in that: being followed successively by passed with the amine-modified zinc oxide electronics of the flexible and transparent substrate of OMO electrode, polyethyleneimine from bottom to top
Defeated layer, non-fullerene system photoactive layer, Hole-injecting Buffer Layer for Improvement and anode electrode；Polyethyleneimine is covered on zinc oxide electron transfer layer
Amine thin layer.
The present invention passes through the modification of polyethyleneimine thin layer, it is suppressed that electrons and holes are showed in zinc oxide electron transfer layer
The probability of recombination, improve the extraction efficiency of charge, flexible battery device finally made to obtain higher photoelectric conversion efficiency.
The flexible and transparent substrate is PET or PC film.
The OMO electrode is the three-decker electrode of sandwiched metal layer among two inorganic oxide layers；Wherein, the metal
Layer material is Au, Ag or Cu, with a thickness of 5-10nm；The material of inorganic oxide layer is metal oxide semiconductor；OMO structure electricity
Pole keeps higher charge transfer efficiency while visible region keeps high light transmitance.
The zinc oxide electron transfer layer includes Zinc oxide nanoparticle layer and polyethyleneimine thin layer, wherein zinc oxide
Nano-particle layer with a thickness of 30nm, zinc oxide is graininess, partial size 4nm, polyethyleneimine thin layer with a thickness of 5-
10nm；Flexible battery device architecture is further modified by polyethyleneimine amine-modified zinc oxide electron transfer layer, Ke Yixian
The extraction and transport efficiency for improving electronics are write, while improving the photoelectric current and fill factor of battery device, it is final to improve battery device
The incident photon-to-electron conversion efficiency of part.
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 polyethyleneimine second
Alcoholic solution, then anneal at 60 DEG C 10min, forms the amine-modified zinc oxide electron transfer layer of polyethyleneimine；
(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.
Preferably, in step (2), the Zinc oxide nanoparticle made from the liquid phase reduction is distributed to after washing of precipitate
Volume ratio is the n-butanol of 60:35:5, in the mixed solution of methanol, chloroform, and the concentration of zinc oxide thin layer of solution is 10mg/mL；
The concentration of polyethyleneimine ethanol solution is 0.1-0.2mg/mL, and the molecular weight of polyethyleneimine is 4000-8000, in zinc oxide
Thin layer surface is with the speed spin coating polyethylene glycol ethanol solution of 3000rpm.
Preferably, in step (3), photoactive layer solution is the donor material that mass ratio is 1:1 and acceptor material in chlorobenzene
The polymer blend solution being mixed to get in solution, concentration 9-10mg/mL；It is also added in polymer blend solution
The 1,8- diiodo-octane of 1.5vol%.
Structure of the invention design rationally, preparation step is simple, passes through the modification of polyethyleneimine thin layer, it is suppressed that electronics and
Hole zinc oxide electron-transport layer surface the probability of recombination, while improve flexible battery device absorbing properties and filling because
Son, and then improve the incident photon-to-electron conversion efficiency of polymer solar battery.
(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 that the photovoltaic property for the polymer solar battery that polyethyleneimine is amine-modified and unmodified in the embodiment of the present invention 1 is bent
Line chart.
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.
Technical program of the present invention lies in provide a kind of zinc oxide electron-transport layer building amine-modified based on polyethyleneimine
Flexible structure polymer solar battery, as shown in Fig. 1, battery structure include flexible and transparent substrate 1, OMO electrode 2, poly- second
The zinc oxide electron transfer layer 3 of alkene imines modification, non-fullerene system photoactive layer 4, Hole-injecting Buffer Layer for Improvement 5, anode 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.
OMO electrode 2 of the invention is cathode electrode, 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, polyethyleneimine thin layer.Wherein
ZnO is graininess, and size is about 4nm, and 3 thickness of zinc oxide electron transfer layer is about 30nm, and polyethyleneimine thickness is about 5-
10nm.By certain density polyethyleneimine ethanol solution, by spin coating method, one layer of spin coating on zinc oxide electron transfer layer
Polyethyleneimine thin layer, low-temperature annealing.
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 etc. has unsaturated structure in structure, band gap is moderate, inhales with non-fullerene acceptor material
Light is complementary, and energy match, and visible light can be absorbed and generate exciton.Acceptor material be non-fullerene fused-ring derivatives such as ITIC,
ITIC-m etc. has energy level adjustable relative to fullerene acceptor material, and light absorption range is wide, and it is good that stability is blended with donor material
The advantages that, 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 based on the amine-modified zinc oxide electron-transport layer building flexible structure polymer solar battery of polyethyleneimine is such as
Shown in Fig. 1.1 is the transparent base flexibility PET in figure；2 cathode electrodes are OMO conductive electrode, are made of ZnO/Ag/ZnO, thickness point
It Wei not 60nm, 10nm, 50nm；ZnO nano stratum granulosum and thickness containing thickness about 30nm in zinc oxide electron transfer layer 3 are about
The polyethyleneimine decorative layer of 10nm.Donor material is J71, non-fullerene acceptor material in non-fullerene system photoactive layer 4
For ITIC, non-fullerene system photoactive layer 4 with a thickness of 100nm；Electron buffer layer 5 is MoO3, with a thickness of 10nm；Anode electricity
Pole 6 is Ag, with a thickness of 100nm.
Its it is specific the preparation method is as follows:
(1) the OMO cathode electrode in flexibility PET transparent substrates is obtained by magnetron sputtering method, and PET/OMO substrate is without cleaning, In
Direct one layer of electron transfer layer of spin coating on OMO electrode；
(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), oxidation zinc concentration is about 10mg/ml.Polyethyleneimine ethanol solution is prepared, it is dense
Degree is 0.2mg/ml, and polyethyleneimine molecular weight is 8000.In zinc oxide films layer surface with 3000rpm speed spin coating polyethyleneimine
Amine ethanol solution, then 60 DEG C of annealing 10min form the amine-modified zinc oxide electron transfer layer of polyethyleneimine.Substrate is transferred to nitrogen
The preparation of photoactive layer is carried out in the glove box of gas shielded；
(3) photoactive layer solution is made of J71, ITIC, and the mass ratio of J71 and ITIC in chlorobenzene solution is 1:1, and polymer is dense
Degree 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 active layer respectively with the Ag anode of 100nm, in vacuum
≤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 of the corresponding modification of Fig. 2 and unmodified battery is not 6.16% and 4.98%, after polyethyleneimine is amine-modified, device
Part efficiency is obviously improved, and is mainly reflected in fill factor and is promoted by 51.05% to 57.25%, current density is by 16.53 mAcm-1It mentions
It is raised to 18.32mAcm-1.Being obviously improved of fill factor and current density prove the amine-modified ZnO of polyethyleneimine can play benefit its
Surface defect inhibits electron hole compound effect again.
Embodiment 2:
Structure based on the amine-modified zinc oxide electron-transport layer building flexible structure polymer solar battery of polyethyleneimine is such as
Shown in Fig. 1.1 is the transparent base flexibility PET in figure；2 cathode electrodes are OMO conductive electrode, are made of ZnO/Ag/ZnO, thickness point
It Wei not 60nm, 10nm, 50nm；ZnO nano stratum granulosum and thickness containing thickness about 30nm in zinc oxide electron transfer layer 3 are about
The polyethyleneimine decorative layer of 5nm.Donor material is J61 in non-fullerene system photoactive layer 4, and non-fullerene acceptor material is
ITIC-m, non-fullerene system photoactive layer 4 with a thickness of 100nm；Electron buffer layer 5 is MoO3, with a thickness of 10nm；Anode electricity
Pole 6 is Ag, with a thickness of 100nm.
Its it is specific the preparation method is as follows:
(1) the OMO cathode electrode in flexibility PET transparent substrates is obtained by magnetron sputtering method, and PET/OMO substrate is without cleaning, In
Direct one layer of electron transfer layer of spin coating on OMO electrode；
(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), oxidation zinc concentration is about 10mg/ml.Polyethyleneimine ethanol solution is prepared, it is dense
Degree is 0.1mg/ml, and polyethyleneimine molecular weight is 4000.In zinc oxide films layer surface with 3000rpm speed spin coating polyethyleneimine
Amine ethanol solution, then 60 DEG C of annealing 10min form the amine-modified zinc oxide electron transfer layer of polyethyleneimine.Substrate is transferred to nitrogen
The preparation of photoactive layer is carried out in the glove box of gas shielded；
(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, the fill factor and current density of device are obviously improved after tested, are turned to promote integral battery photoelectricity
Change efficiency.
Claims (10)
1. a kind of polymer solar battery of the zinc oxide electron-transport layer building flexible structure amine-modified based on polyethyleneimine,
It is characterized by: being followed successively by the oxidation amine-modified with the flexible and transparent substrate (1) of OMO electrode (2), polyethyleneimine from bottom to top
Zinc electron transfer layer (3), non-fullerene system photoactive layer (4), Hole-injecting Buffer Layer for Improvement (5) and anode electrode (6)；Zinc oxide electronics
Transport layer is covered with polyethyleneimine thin layer on (3).
2. the zinc oxide electron-transport layer building flexible structure amine-modified based on polyethyleneimine according to claim 1 is poly-
Close object solar battery, it is characterised in that: the flexible and transparent substrate (1) is PET or PC film.
3. the zinc oxide electron-transport layer building flexible structure amine-modified based on polyethyleneimine according to claim 1 is poly-
Close object solar battery, it is characterised in that: the OMO electrode (2) is three layers of sandwiched metal layer among two inorganic oxide layers
Structure electrode.
4. the zinc oxide electron-transport layer building flexible structure amine-modified based on polyethyleneimine according to claim 1 is poly-
Close object solar battery, it is characterised in that: the zinc oxide electron transfer layer (3) includes Zinc oxide nanoparticle layer and polyethylene
Imines thin layer, wherein Zinc oxide nanoparticle layer with a thickness of 30nm, zinc oxide is graininess, partial size 4nm, polyethyleneimine
Amine thin layer with a thickness of 5-10nm.
5. the zinc oxide electron-transport layer building flexible structure amine-modified based on polyethyleneimine according to claim 1 is poly-
Close object solar battery, it is characterised in that: the non-fullerene system photoactive layer (4) with a thickness of 100nm, wherein donor
Material is mid-gap polymer donor material J71 or J61, and acceptor material is non-fullerene fused-ring derivatives ITIC or ITIC-
The blending ratio of m, donor material and acceptor material is 1:1.
6. the zinc oxide electron-transport layer building flexible structure amine-modified based on polyethyleneimine according to claim 1 is poly-
Close 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 is Ag, with a thickness of 100nm.
7. the zinc oxide electron-transport layer building flexible structure amine-modified based on polyethyleneimine according to claim 1 is poly-
Close object solar battery, it is characterised in that: the metal layer material is Au, Ag or Cu, with a thickness of 5-10nm；Inorganic oxide layer
Material be metal oxide semiconductor.
8. the zinc oxide electron-transport layer building flexible structure amine-modified based on polyethyleneimine according to claim 1 is poly-
The preparation method of object solar battery is closed, it is characterized in that, include the following steps: (1) by magnetron sputtering method in flexible and transparent base
OMO cathode electrode is sputtered on bottom；(2) direct one layer of zinc oxide thin layer of spin coating on OMO cathode electrode, in zinc oxide films layer surface
Spin coating polyethyleneimine ethanol solution, then anneal at 60 DEG C 10min, forms the amine-modified zinc oxide electronics of polyethyleneimine and passes
Defeated layer；(3) with the speed spin coating photoactive layer solution 60s of 1200-1400rpm in the glove box of nitrogen protection；(4) in vacuum
In filming equipment, by the MoO of 10nm3It is deposited on photoactive layer respectively with the Ag anode of 100nm, in vacuum≤5 × 10-4Under Pa
Form 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 polyethyleneimine ethanol solution is 0.1-0.2mg/mL, polyethyleneimine
Molecular weight be 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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| CN112802863A (en) * | 2021-01-21 | 2021-05-14 | 上海大学 | Image sensor and preparation method thereof |
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