CN105895809A - Preparation method of ZnO film for inverted polymer solar cell - Google Patents
Preparation method of ZnO film for inverted polymer solar cell Download PDFInfo
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Abstract
The invention relates to a preparation method of a ZnO film for an inverted polymer solar cell. A multilayer AZO buffering film is prepared as an electron transport layer in the inverted polymer solar cell, so that the structure characteristic and the electric performance of the AZO film can be improved, and the problem of mismatching between the AZO and the ITO substrate heat expansion system of the cell is solved; high-temperature annealing is not needed, and the film can be prepared in the atmospheric environment, so that current carrier recombination is effectively reduced, the short current density and the filling factor of the cell are significantly improved, and the energy conversion efficiency of the cell is improved. Particularly, the method is simple and feasible, and is compatible with a commercial large-area production process, so that the industrial process of the solar cell can be accelerated to meet social requirements.
Description
Technical field
The present invention relates to the technical field of solar batteries in new forms of energy, effectively reduce Carrier recombination particularly to one, aobvious
Write and improve battery short circuit current density and fill factor, curve factor, it is achieved cell power conversion efficiency for reversed structure polymer solar electricity
The preparation method of the ZnO film in pond.
Background technology
Society, economic fast development brings the such as Tough questions such as energy crisis and global warming, renewable cleaning
The development of the energy and utilization have been subjected to global extensive concern.It is different from the traditional energies such as coal, oil, natural gas, the sun
During energy, one green, cleaning, regenerative resource, inexhaustible, the potential important component part become in supply.
Solar cell is as a kind of electrooptical device, and its research has been subjected to more and more pay attention to application.With with high costs
Silica-based solar cell is compared, polymer solar battery use organic semiconducting materials as photoactive layer, have with low cost,
The features such as the absorption coefficient of light is high, quality is light, and pliability is good, and manufacturing process is simple.Due to carrier diffusion length in organic material
Short, active layer is relatively thin, to the absorption of incident light insufficient.Realize spectrum is fully absorbed under limited absorber thickness
Become and improve the problem that organic battery efficiency needs urgent solution.Light trapping structure is introduced, by right in the middle of organic polymer battery
The reflection of incident light, reflect, scatter and effective modulation of distribution of light intensity distribution, active layer can be realized light is fully absorbed,
Promote the energy conversion efficiency of battery.
Due to nontoxic, cheap, outstanding stability, high electron mobility and visible light wave range high transmission characteristic, ZnO
Film is widely studied in reversed structure polymer solar cells and applies.By a small amount of metal Al3+Doping, it is possible to the biggest
The electric property of ZnO film is improved in degree.But, when preparing collosol and gel Al-doped ZnO (AZO) film, heat is moved back
In fire processing procedure inevitably there is thermal expansion, due to the thermal expansion of AZO film Yu ITO substrate in ito glass substrate
Coefficient does not mates, and affects the structural and optical characteristic of AZO film, thus increases between AZO film surface and battery-active layer
The defect state density at interface so that the photoelectric transformation efficiency of organic photovoltaic cell promotes further and is restricted.
Summary of the invention
It is an object of the invention in order to solution prepare collosol and gel Al-doped ZnO (AZO) film time, thermal anneal process mistake
In journey inevitably there is thermal expansion in ito glass substrate, due to AZO film and ITO substrate thermal coefficient of expansion not
Join, affect the defect of the structural and optical characteristic of AZO film and provide one effectively to reduce Carrier recombination, significantly improve battery
Short-circuit current density and fill factor, curve factor, it is achieved the ZnO for reversed structure polymer solar battery of cell power conversion efficiency is thin
The preparation method of film.
To achieve these goals, the present invention is by the following technical solutions:
A kind of preparation method of the ZnO film for reversed structure polymer solar battery, described preparation method comprises the following steps:
A) weigh 1-3 gram of Zinc diacetate dihydrate and 0.01-0.1 gram of ANN aluminium nitrate nonahydrate is dissolved in 10-30 milliliter ethanol solution, take 0.1-0.5
Milliliter MEA adds solution;The solution configured is stirred 0.1-1h at 30-80 DEG C;After solution is as clear as crystal, in room
24h it is aged under the conditions of temperature;
B) being spin-coated on ito glass substrate by the precursor liquid that step a) obtains, sol evenning machine rotating speed is 1000-3000rpm, spin-coating time
For 10-40s;After spin coating, sample is placed on 200-300 DEG C of hot plate heating 30-50min and carries out thermal anneal process,
To AZO cushion one;
C) on this basis, repeat step b), and then prepare AZO cushion two, and preparation buffering on the basis of cushion two
Layer three, obtains multilayer AZO buffer stack structure sample: ITO/AZO/AZO/AZO;After sample is cooled to room temperature, ultrasonic
Processing 10min, with deionized water rinsing, nitrogen dries up stand-by;
D) donor material and acceptor material that mass ratio is 1:0.8 are dissolved in 1 milliliter of chlorobenzene solution and are configured to active layer solution, keep away
Thermal agitation is added 12 hours at light 30-50 DEG C;Active layer solution is spin-coated on the AZO film that step c) obtains, spin coating is set
Machine rotating speed be 300-800rpm spin-coating time be 15-30s, sample is placed on 80-120 DEG C of hot plate and carries out 1-20min annealing
Process;
E) sample that step d) obtains is put in coating machine, 10-41-10nm MoO it is deposited with under the conditions of Pa3With 50-100nm Ag electricity
Pole.In the technical program, ito glass substrate is prepared multilayer AZO film slow as the negative electrode of organic polymer battery
Rush layer, AZO crystalline quality can not only be effectively improved, optimize AZO optical characteristics, reduce AZO surface defect, Er Qieji
Big improve transporting and collecting efficiency of carrier in device.The method is based on sol-gel method, it is not necessary to expensive vacuum equipment,
Without high annealing, can at room temperature prepare in air, to commercially produce preparation technology mutually compatible with large area.Multilayer AZO is delayed
Rush the introducing of layer, it is possible to effectively reduce Carrier recombination, hence it is evident that improve battery short circuit current density, fill factor, curve factor and energy and turn
Change efficiency.
As preferably, donor material is P3HT, and acceptor material is PCBM.
As preferably, in step b), ito glass substrate immersion adhesive force promotes in liquid, ultrasonically treated 45-60min;Then
Take out and add the ultrasonically treated 15-30min of acetone, after taking-up, use deionized water rinsing, then use nitrogen to be dried up by substrate, then
Carry out spin coating precursor liquid.
As preferably, adhesive force promotes that liquid is made up of the raw material of following weight portion: hydroxyethyl cellulose 10-15 part, positive silicic acid
Methyl esters 20-35 part, algae clay 5-10 part, ethyl acetate 80-100 part, silane coupler 15-25 part and acetic acid 0.1-0.3 part.
In the technical program, adhesive force promotes that liquid promotes adhesive force and the wellability of substrate surface, in order to during the follow-up plated film of follow-up raising
Substrate film coating adhesive force and uniformity.
As preferably, adhesive force promotes that the preparation method of liquid is: by hydroxyethyl cellulose, methyl silicate, silane coupler
Joining in ethyl acetate with algae clay, add acetic acid after stirring and dissolving is complete, ultrasonic 60KHz obtains after processing 35-50min.
As preferably, adhesive force promotes that the temperature of liquid is 65-80 DEG C.
As preferably, cell area is 0.08cm2。
As preferably, in step b), the thickness of AZO cushion one is 5-10nm.
The reversed structure polymer sun that more than one described ZnO films for reversed structure polymer solar battery prepare
Can battery.
The beneficial outcomes of the present invention is: the method using the preparation multilayer AZO buffer layer thin film of present invention proposition, as falling
Electron transfer layer in structural polymer solar cell, is not only able to improve architectural characteristic and the electric property of AZO film, solves
AZO and the battery ITO unmatched problem of substrate hot expansion system, and without high annealing, under atmospheric environment
Preparation completes, and effectively reduces Carrier recombination, significantly improves battery short circuit current density and fill factor, curve factor, it is achieved the energy content of battery turns
Change the lifting of efficiency.Particularly the method is simple, compatible with commercialization large area process for producing such that it is able to accelerate
The industrialization process of the type solar cell, satisfies social needs.
On ito glass substrate, preparation multilayer AZO film is as the cathode buffer layer of organic polymer battery, can not only have
Effect improves AZO crystalline quality, optimizes AZO optical characteristics, reduces AZO surface defect, and improves device greatly
The transporting and collect efficiency of middle carrier.The method is based on sol-gel method, it is not necessary to expensive vacuum equipment, it is not necessary to high annealing,
Can at room temperature prepare in air, to commercially produce preparation technology mutually compatible with large area.The introducing of multilayer AZO cushion, energy
Enough effectively reduce Carrier recombination, hence it is evident that improve battery short circuit current density, fill factor, curve factor and energy conversion efficiency.
Accompanying drawing explanation
Fig. 1 is reversed structure polymer solar cells structural representation.
In Fig. 1: 1. simple glass carrier;2.ITO transparent conductive film;3.AZO cushion one;4.AZO cushion two;
5.AZO cushion three;6.P3HT:PCBM film;7.MoO3Film;8.Ag electrode.
Fig. 2 is that reversed structure polymer solar cells is at AM 1.5G (1mW/cm2) solar simulator irradiate under electric current-electricity
Pressure characteristic curve.
Detailed description of the invention
Technical scheme in the embodiment of the present invention will be carried out clear, complete description below, it is clear that described embodiment
It is only a part of embodiment of the present invention rather than whole embodiments.Based on the embodiment in the present invention, the common skill in this area
All other embodiments that art personnel are obtained under not making creative work premise, broadly fall into the scope of protection of the invention.
With reference to Fig. 1,1. simple glass carrier;2.ITO transparent conductive film;3.AZO cushion one;4.AZO cushion two;
5.AZO cushion three;6.P3HT:PCBM film;7.MoO3Film;8.Ag electrode.
Embodiment 1
A kind of preparation method of the ZnO film for reversed structure polymer solar battery, described preparation method comprises the following steps:
A) weigh 1 gram of Zinc diacetate dihydrate and 0.01 gram of ANN aluminium nitrate nonahydrate is dissolved in 10 milliliters of ethanol solutions, take 0.1 milliliter of list
Monoethanolamine adds solution;The solution configured is stirred 0.1h at 30 DEG C;After solution is as clear as crystal, the oldest
Change 24h;
B) being spin-coated on ito glass substrate by the precursor liquid that step a) obtains, sol evenning machine rotating speed is 1000rpm, and spin-coating time is 10s;
After spin coating, sample is placed on 200 DEG C of hot plates heating 30min and carries out thermal anneal process, obtain AZO cushion one,
Thickness is 5nm;
C) on this basis, repeat step b), and then prepare AZO cushion two, and preparation buffering on the basis of cushion two
Layer three, obtains multilayer AZO buffer stack structure sample: ITO/AZO/AZO/AZO;After sample is cooled to room temperature, ultrasonic
Processing 10min, with deionized water rinsing, nitrogen dries up stand-by;
D) be P3HT by the donor material that mass ratio is 1:0.8 and acceptor material is that PCBM is dissolved in 1 milliliter of chlorobenzene solution configuration
Viability layer solution, adds thermal agitation 12 hours at lucifuge 30 DEG C;Active layer solution is spin-coated on the AZO that step c) obtains thin
On film, arrange sol evenning machine rotating speed be 300rpm spin-coating time be 15s, sample is placed on 80 DEG C of hot plates and carries out 1min annealing
Process;
E) sample that step d) obtains is put in coating machine, 10-41nm MoO it is deposited with under the conditions of Pa3With 50nm Ag electrode, electricity
Pool area is 0.08cm2。
Embodiment 2
A kind of preparation method of the ZnO film for reversed structure polymer solar battery, described preparation method comprises the following steps:
A) weigh 2 grams of Zinc diacetate dihydrates and 0.02 gram of ANN aluminium nitrate nonahydrate is dissolved in 20 milliliters of ethanol solutions, take 0.2 milliliter of list
Monoethanolamine adds solution;The solution configured is stirred 0.5h at 50 DEG C;After solution is as clear as crystal, the oldest
Change 24h;
B) during ito glass substrate immerses adhesive force promotion liquid, ultrasonically treated 50min;Then take out the addition ultrasonically treated 20min of acetone,
Use deionized water rinsing after taking-up, then use nitrogen to be dried up by substrate;Adhesive force promotes that the temperature of liquid is 70 DEG C;
Being spin-coated on ito glass substrate by the precursor liquid that step a) obtains, sol evenning machine rotating speed is 2000rpm, and spin-coating time is 20s;
After spin coating, sample is placed on 250 DEG C of hot plates heating 40min and carries out thermal anneal process, obtain AZO cushion one,
Thickness is 7nm;
Adhesive force promotes that liquid is made up of the raw material of following weight portion: hydroxyethyl cellulose 12 parts, methyl silicate 25 parts, algae clay 7
Part, 90 parts of ethyl acetate, silane coupler 20 parts and acetic acid 0.1 part;Adhesive force promotes that the preparation method of liquid is: by hydroxyl second
Base cellulose, methyl silicate, silane coupler and algae clay join in ethyl acetate, add acetic acid after stirring and dissolving is complete,
Ultrasonic 60KHz obtains after processing 40min;
C) on this basis, the precursor liquid repeating step b) is spin-coated on AZO cushion one, and then prepares AZO cushion two,
And on the basis of AZO cushion two, prepare cushion three, obtain multilayer AZO buffer stack structure sample:
ITO/AZO/AZO/AZO;After sample is cooled to room temperature, ultrasonically treated 10min, with deionized water rinsing, nitrogen dries up to be treated
With;
D) be P3HT by the donor material that mass ratio is 1:0.8 and acceptor material is that PCBM is dissolved in 1 milliliter of chlorobenzene solution configuration
Viability layer solution, adds thermal agitation 12 hours at lucifuge 40 DEG C;Active layer solution is spin-coated on the AZO that step c) obtains thin
On film, arrange sol evenning machine rotating speed be 500rpm spin-coating time be 20s, sample is placed on 100 DEG C of hot plates and carries out 10min
Annealing;
E) sample that step d) obtains is put in coating machine, 10-45nm MoO it is deposited with under the conditions of Pa3With 80nm Ag electrode, electricity
Pool area is 0.08cm2。
Embodiment 3
A kind of preparation method of the ZnO film for reversed structure polymer solar battery, described preparation method comprises the following steps:
A) weigh 3 grams of Zinc diacetate dihydrates and 0.1 gram of ANN aluminium nitrate nonahydrate is dissolved in 30 milliliters of ethanol solutions, take 0.5 milliliter of single second
Hydramine adds solution;The solution configured is stirred 1h at 80 DEG C;After solution is as clear as crystal, it is aged at ambient temperature
24h;
B) during ito glass substrate immerses adhesive force promotion liquid, ultrasonically treated 60min;Then take out the addition ultrasonically treated 30min of acetone,
Use deionized water rinsing after taking-up, then use nitrogen to be dried up by substrate;Adhesive force promotes that the temperature of liquid is 80 DEG C;
Being spin-coated on ito glass substrate by the precursor liquid that step a) obtains, sol evenning machine rotating speed is 3000rpm, and spin-coating time is 40s;
After spin coating, sample is placed on 300 DEG C of hot plates heating 50min and carries out thermal anneal process, obtain AZO cushion one,
Thickness is 10nm;
Adhesive force promotes that liquid is made up of the raw material of following weight portion: hydroxyethyl cellulose 15 parts, methyl silicate 35 parts, algae clay 10
Part, 100 parts of ethyl acetate, silane coupler 25 parts and acetic acid 0.3 part;Adhesive force promotes that the preparation method of liquid is: by hydroxyl second
Base cellulose, methyl silicate, silane coupler and algae clay join in ethyl acetate, add acetic acid after stirring and dissolving is complete,
Ultrasonic 60KHz obtains after processing 50min;
C) on this basis, the precursor liquid repeating step b) is spin-coated on AZO cushion one, and then prepares AZO cushion two,
And on the basis of cushion two, prepare cushion three, obtain multilayer AZO buffer stack structure sample:
ITO/AZO/AZO/AZO;After sample is cooled to room temperature, ultrasonically treated 10min, with deionized water rinsing, nitrogen dries up to be treated
With;
D) be P3HT by the donor material that mass ratio is 1:0.8 and acceptor material is that PCBM is dissolved in 1 milliliter of chlorobenzene solution configuration
Viability layer solution, adds thermal agitation 12 hours at lucifuge 50 DEG C;Active layer solution is spin-coated on the AZO that step c) obtains thin
On film, arrange sol evenning machine rotating speed be 800rpm spin-coating time be 30s, sample is placed on 120 DEG C of hot plates and carries out 20min
Annealing;
E) sample that step d) obtains is put in coating machine, 10-410nm MoO it is deposited with under the conditions of Pa3With 100nm Ag electrode,
Cell area is 0.08cm2。
With reference to Fig. 2, battery device 1: the initial devices of individual layer AZO film;Battery device 2: based on three layers of AZO buffering
The battery device of layer.As seen from the figure, the method for the present invention short-circuit current density of the polymer solar cells prepared and fill because of
Son is obviously higher than initial devices.
On ito glass substrate, preparation multilayer AZO film is as the cathode buffer layer of organic polymer battery, can not only have
Effect improves AZO crystalline quality, optimizes AZO optical characteristics, reduces AZO surface defect, and improves device greatly
The transporting and collect efficiency of middle carrier.The method is based on sol-gel method, it is not necessary to expensive vacuum equipment, it is not necessary to high annealing,
Can at room temperature prepare in air, to commercially produce preparation technology mutually compatible with large area.The introducing of multilayer AZO cushion, energy
Enough effectively reduce Carrier recombination, hence it is evident that improve battery short circuit current density, fill factor, curve factor and energy conversion efficiency.
Embodiment described above is the one preferably scheme of the present invention, and the present invention not makees any pro forma limit
System, also has other variant and remodeling on the premise of without departing from the technical scheme described in claim.
Claims (9)
1. the preparation method for the ZnO film of reversed structure polymer solar battery, it is characterised in that described preparation method bag
Include following steps:
A) weigh 1-3 gram of Zinc diacetate dihydrate and 0.01-0.1 gram of ANN aluminium nitrate nonahydrate is dissolved in 10-30 milliliter ethanol solution, take 0.1-0.5
Milliliter MEA adds solution;The solution configured is stirred 0.1-1h at 30-80 DEG C;After solution is as clear as crystal, in room
24h it is aged under the conditions of temperature;
B) being spin-coated on ito glass substrate by the precursor liquid that step a) obtains, sol evenning machine rotating speed is 1000-3000rpm, spin-coating time
For 10-40s;After spin coating, sample is placed on 200-300 DEG C of hot plate heating 30-50min and carries out thermal anneal process,
To AZO cushion one;
C) on this basis, repeat step b), and then prepare AZO cushion two, and preparation buffering on the basis of cushion two
Layer three, obtains multilayer AZO buffer stack structure sample: ITO/AZO/AZO/AZO;After sample is cooled to room temperature, ultrasonic
Processing 10min, with deionized water rinsing, nitrogen dries up stand-by;
D) donor material and acceptor material that mass ratio is 1:0.8 are dissolved in 1 milliliter of chlorobenzene solution and are configured to active layer solution, keep away
Thermal agitation is added 12 hours at light 30-50 DEG C;Active layer solution is spin-coated on the AZO film that step c) obtains, spin coating is set
Machine rotating speed be 300-800rpm spin-coating time be 15-30s, sample is placed on 80-120 DEG C of hot plate and carries out 1-20min annealing
Process;
E) sample that step d) obtains is put in coating machine, 10-41-10nm MoO it is deposited with under the conditions of Pa3With 50-100nm Ag electricity
Pole.
The preparation method of a kind of ZnO film for reversed structure polymer solar battery the most according to claim 1, its feature
Being, donor material is P3HT, and acceptor material is PCBM.
The preparation method of a kind of ZnO film for reversed structure polymer solar battery the most according to claim 1, its feature
It is, during in step b), ito glass substrate immerses adhesive force promotion liquid, ultrasonically treated 45-60min;Then take out addition third
The ultrasonically treated 15-30min of ketone, uses deionized water rinsing after taking-up, then use nitrogen to be dried up by substrate, then before carrying out spin coating
Drive liquid.
The preparation method of a kind of ZnO film for reversed structure polymer solar battery the most according to claim 3, its feature
Being, adhesive force promotes that liquid is made up of the raw material of following weight portion: hydroxyethyl cellulose 10-15 part, methyl silicate 20-35
Part, algae clay 5-10 part, ethyl acetate 80-100 part, silane coupler 15-25 part and acetic acid 0.1-0.3 part.
The preparation method of a kind of ZnO film for reversed structure polymer solar battery the most according to claim 4, its feature
Being, adhesive force promotes that the preparation method of liquid is: hydroxyethyl cellulose, methyl silicate, silane coupler are added with algae clay
Entering in ethyl acetate, add acetic acid after stirring and dissolving is complete, ultrasonic 60KHz obtains after processing 35-50min.
6. according to the preparation method of a kind of ZnO film for reversed structure polymer solar battery described in claim 3 or 4 or 5,
It is characterized in that, adhesive force promotes that the temperature of liquid is 65-80 DEG C.
The preparation method of a kind of ZnO film for reversed structure polymer solar battery the most according to claim 1, its feature
Being, cell area is 0.08cm2。
The preparation method of a kind of ZnO film for reversed structure polymer solar battery the most according to claim 1, its feature
Being, in step b), the thickness of AZO cushion one is 5-10nm.
9. the reversed structure polymer that the ZnO film for reversed structure polymer solar battery used described in claim 1 prepares
Solar cell.
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CN108198939B (en) * | 2017-12-15 | 2021-06-18 | 浙江海洋大学 | Organic solar cell with multi-layer magnesium-aluminum-doped zinc oxide composite film as electron transport layer |
CN109994609A (en) * | 2017-12-29 | 2019-07-09 | 浙江沐光新能源科技有限公司 | A kind of preparation method of the ZnO film for reversed structure polymer solar battery |
CN108640532A (en) * | 2018-06-04 | 2018-10-12 | 中建材蚌埠玻璃工业设计研究院有限公司 | A kind of thin-film solar cells preparation method for falling into light glass |
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