CN106784331A - A kind of lamination cathode buffer layer organic polymer solar cell and preparation method thereof - Google Patents
A kind of lamination cathode buffer layer organic polymer solar cell and preparation method thereof Download PDFInfo
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Abstract
The present invention relates to a kind of lamination cathode buffer layer organic polymer solar cell, the battery uses eurymeric structure, is followed successively by from top to bottom：Transparent substrates, transparent conductive anode, anode buffer layer, photoactive layer, cathode buffer layer, metallic cathode；The photoactive layer is electron donor material PCDTBT and electron acceptor material PC71BM is according to 1:The composition of 4 mass ratio mixing；Polyvinylpyrrolidone cathode buffer layer is prepared on photoactive layer；Alq3Cathode buffer layer is prepared on polyvinylpyrrolidone cathode buffer layer, and its thickness is 0.5~1.5nm；CaF2Cathode buffer layer is prepared in Alq3Between cathode buffer layer and metallic cathode, its thickness is 0.6~1.2nm.Present invention reduces the series resistance of device, Carrier recombination probability is reduced, battery has more stability, effectively raises the photoelectric transformation efficiency of device.
Description
Technical field
The invention belongs to organic polymer photovoltaic device technical field, and in particular to a kind of lamination cathode buffer layer is organic poly-
Compound solar cell and preparation method thereof.
Background technology
In recent years, people increase year by year to demand of the traditional energy including the fossil energy including coal, oil, natural gas
Plus, this also directly results in the increasingly serious of environmental pollution, be raised including water pollution, atmosphere pollution, acid rain, global temperatures
The problems such as.Therefore, people replace traditional energy in the urgent need to seeking a kind of new clean energy resource, and solar energy exactly one kind is divided
Cloth is extensive, the regenerative resource of cleanliness without any pollution, becomes the study hotspot and emphasis of new energy field.
Solar cell can convert the solar into electric energy by photoelectric effect, be using solar energy important channel it
One.Inorganic solar cell production cost is high, energy consumption is big in manufacturing process, complex process, the requirement to material is harsh, be difficult into
Row large area is produced, therefore organic polymer solar cell arises at the historic moment, and it has low cost, less energy consumption, light weight, material
Wide material sources, preparation process is simple, can large area the advantages of prepare flexible device, extensive research has been obtained in recent years and has been closed
Note.However, compared with inorganic solar cell, the photoelectric transformation efficiency of organic solar batteries is relatively low, it is impossible to meet existing
The demand grown directly from seeds in living, people improve the opto-electronic conversion effect of organic polymer solar cell in the urgent need to seeking new method
Rate.
In organic polymer solar cell, electronics and hole pass through electron acceptor material and electron donor material respectively
Electrode is transferred to, electric current is produced.Therefore, transmission of the generation of electric current not only with electronics, hole is relevant, also with photoactive layer and electricity
Interfacial property between pole is closely related.Research shows that introducing is cloudy between the photoactive layer and metal electrode of solar cell
Pole cushion can promote the transmission of electric charge, be conducive to the collection of carrier at electrode, optimizes energy level and interface performance, enter
And improve the photoelectric transformation efficiency of battery.Conventional cathode buffer layer has ZnO, TiO at present2, PFN, more used in reciprocal form structure
In, the conventional cathode buffer layer of autologous battery has LiF, CsCO3, although electronics can be effectively transmitted, but it can not
Effectively stop active layer to the hole transport of negative electrode, the Carrier recombination probability of device is higher.
The content of the invention
It is low that the technical problems to be solved by the invention are to provide a kind of series resistance, open-circuit voltage, short-circuit current density, fills out
Fill the factor and photoelectric transformation efficiency lamination cathode buffer layer organic polymer solar cell high and preparation method thereof.
In order to solve the above-mentioned technical problem, lamination cathode buffer layer organic polymer solar cell of the invention, uses
Eurymeric structure, is followed successively by from top to bottom：Transparent substrates, transparent conductive anode, anode buffer layer, photoactive layer, cathode buffer layer,
Metallic cathode；It is characterized in that the photoactive layer is electron donor material PCDTBT and electron acceptor material PC71BM is according to 1:4
Mass ratio mixing composition；Cathode buffer layer is used by polyvinylpyrrolidone cathode buffer layer, Alq3Cathode buffer layer
And CaF2The lamination cathode buffer layer that cathode buffer layer is constituted；Polyvinylpyrrolidone cathode buffer layer is prepared in photoactive layer
On；Alq3Cathode buffer layer is prepared on polyvinylpyrrolidone cathode buffer layer, and its thickness is 0.5~1.5nm；CaF2Negative electrode
Cushion is prepared in Alq3Between cathode buffer layer and metallic cathode, its thickness is 0.6~1.2nm.
The polyvinylpyrrolidone cathode buffer layer is prepared on photoactive layer by spin coating method.
The polyvinylpyrrolidone cathode buffer layer can also be prepared on photoactive layer by self-assembling method, formed
SAM polyvinylpyrrolidone cathode buffer layers.
The SAM polyvinylpyrrolidones cathode buffer layer preparation method is as follows：By electron donor material PCDTBT and electricity
Sub- acceptor material PC71BM is according to 1:4 mass ratio is blended in solvent chlorobenzene and obtains photoactive layer material, then by polyvinyl pyrrole
Alkanone is configured to the mixed solution that polyvinylpyrrolidone mass fraction is 1~3wt% in being dissolved in photoactive layer material, then
12~14h is stirred in 50~80 DEG C of heating simultaneously on magnetic stirring apparatus；In the glove box of nitrogen atmosphere, carried out using sol evenning machine
The spin coating of photoactive layer material and polyvinylpyrrolidone mixed solution, rotating speed is 1000rpm/s, and the time is 60s；Spin coating is completed
Afterwards, 30~60min is stood in glove box, polyvinylpyrrolidone is moved to the upper of photoactive layer in self assembly effect
Fang Chengwei polyvinylpyrrolidone cathode buffer layers；It is last that 20~40min is made annealing treatment under the conditions of 60~80 DEG C.
Preferably, polyvinylpyrrolidone is dissolved in photoactive layer material, its mass fraction is 2wt%；Alq3It is cloudy
Pole cushion and CaF2Cathode buffer layer thickness is 1.0nm.
Described transparent substrates use glass substrate or transparent polymer substrate, and wherein transparent polymer includes poly- to benzene
One or more in naphthalate, polystyrene, polyethylene, vinyl chloride-vinyl acetate resin or polyacrylic acid.
The transparent conductive anode material therefor is tin indium oxide (ITO), and tin indium oxide is deposited on a transparent substrate, transparent
Conductive anode thickness is 150nm, and square resistance is 15 Ω/.
Described anode buffer layer material uses polytetrafluoroethylene (PTFE), PEDOT:PSS, or p-type oxide M oO3、WO3、V2O5,
One kind in high work function hole mobile material NiO or by two of which and it is two or more be prepared from from level to level in order, it is thick
It is 1~20nm to spend.
Described metallic cathode is using the one kind in Al, Ca, Mg or Li or by several alloys for constituting therein, its thickness
It is 80nm~180nm.
The preparation method of above-mentioned lamination cathode buffer layer organic polymer solar cell, comprises the following steps：
(1) substrate that cleaning is made up of transparent substrates and transparent conductive anode；
(2) after substrate is dried, anode buffer layer is deposited with transparent anode；
(3) after anode buffer layer evaporation is completed, photoactive layer and polyvinylpyrrolidone are prepared on anode buffer layer
Cathode buffer layer, preparation method is as follows：By electron donor material PCDTBT and electron acceptor material PC71BM is according to 1:4 quality
Photoactive layer material is obtained in solvent chlorobenzene than being blended in, then polyvinylpyrrolidone is dissolved in photoactive layer material is prepared
Into in the mixed solution that polyvinylpyrrolidone mass fraction is 1~3wt%, then 50~80 DEG C of heating on magnetic stirring apparatus
12~14h is stirred simultaneously；In the glove box of nitrogen atmosphere, photoactive layer material and polyvinylpyrrolidine are carried out using sol evenning machine
The spin coating of ketone mixed solution, rotating speed is 1000rpm/s, and the time is 60s；Spin coating complete after, in glove box stand 30~
60min, makes polyvinylpyrrolidone turn into polyvinylpyrrolidone in the top that self assembly effect is moved to photoactive layer cloudy
Pole cushion；It is last that 20~40min is made annealing treatment under the conditions of 60~80 DEG C；
(4) the evaporating Al q on polyvinylpyrrolidone cathode buffer layer3Cathode buffer layer, its thickness is 0.5~1.5nm,
Evaporation rate isNext in Alq3CaF is deposited with cathode buffer layer2Cathode buffer layer, its thickness is 0.6
~1.2nm, evaporation rate is
(5) the evaporation metal negative electrode on cathode buffer layer.
The present invention has advantages below compared with prior art：
First, the lamination cathode buffer layer organic polymer solar cell that the present invention is provided, is delayed by introducing lamination negative electrode
Layer is rushed, the series resistance of device is reduced, the impedance of device is reduced, promotes biography of the electronics from photoactive layer to metallic cathode
It is defeated, improve the transmission performance of electronics, while reducing contact resistance.
2nd, the lamination cathode buffer layer organic polymer solar cell that the present invention is provided, is delayed by introducing lamination negative electrode
Layer is rushed, compared to the cathode buffer layer of individual layer, its work function is more matched with electron acceptor material, advantageously forms good Europe
Nurse is contacted.
3rd, the lamination cathode buffer layer organic polymer solar cell that the present invention is provided, is delayed by introducing lamination negative electrode
Layer is rushed, fully dissociation electronics and hole, the recombination probability of electronics and hole can be reduced, adjust light field, solar energy is more filled
The absorption for dividing, prevents oxygen and hydrone from being permeated to photoactive layer.
4th, the lamination cathode buffer layer organic polymer solar cell that the present invention is provided, is delayed by introducing lamination negative electrode
Layer is rushed, negative electrode will not be corroded, device has more stability.
Brief description of the drawings
The present invention is described in further detail with reference to the accompanying drawings and detailed description.
Fig. 1 is the structural representation of lamination cathode buffer layer organic polymer solar cell of the invention.
Fig. 2 is the organic polymer solar cell of single cathode buffer layer with Alq3The J-V curves of thickness change.
Fig. 3 is the organic polymer solar cell of single cathode buffer layer with CaF2The J-V curves of thickness change.
Fig. 4 is lamination cathode buffer layer organic polymer solar cell of the invention slow with polyvinylpyrrolidone negative electrode
Rush the J-V curves of layer mass fraction change.
Specific embodiment
The technical scheme is that a kind of lamination cathode buffer layer organic polymer solar cell is provided, such as Fig. 1 institutes
Show, device uses eurymeric structure, is followed successively by from top to bottom：Transparent substrates, transparent conductive anode, anode buffer layer, photoactive layer,
Lamination cathode buffer layer, metallic cathode.The ground floor of lamination cathode buffer layer is polyvinylpyrrolidone cathode buffer layer, is passed through
Self-assembling method or spin coating method are prepared on photoactive layer；The second layer is Alq3Cathode buffer layer, prepares in polyvinyl pyrrole
On alkanone cathode buffer layer, its thickness is 0.5~1.5nm；Third layer is CaF2Cathode buffer layer, prepares in Alq3Negative electrode is buffered
On layer, its thickness is 0.6~1.2nm；Photoactive layer is by electron donor material PCDTBT and electron acceptor material PC71BM is according to 1:
4 mass ratio is mixed, and is prepared on anode buffer layer.
Comparative example 1
Be cleaned by ultrasonic with tin indium oxide (ITO) transparent conductive anode glass transparent substrate (transparent conductive anode with it is saturating
Bright substrate constitutes substrate), cleaning reagent is followed successively by toluene, acetone, deionized water, isopropanol, is respectively cleaned by ultrasonic using ultrasonic machine
20min.Use nitrogen (N2) dry up substrate, heating 10min in baking oven is placed on, carried out at plasma with Plasma cleaning machines
Reason 10min.Anode buffer layer uses polytetrafluoroethylene (PTFE) (PTFE), and film forming is prepared with the method for evaporation, and the evaporation rate of PTFE isThickness is 2.0nm.After the completion of evaporation, corona treatment 5min is carried out with Plasma cleaning machines.To steam
The substrate for having plated anode buffer layer moves on to nitrogen (N2) atmosphere glove box in, the spin coating of photoactive layer is carried out using sol evenning machine,
Rotating speed is 1000rpm/s, and the time is 60s, and thickness is about 100nm.Photoactive layer material is by electron donor material PCDTBT and electricity
Sub- acceptor material PC71BM in mass ratio 1:4 configurations are formed.The PC of the PCDTBT and 32mg of 8mg is weighed respectively71BM is dissolved in 1ml's
In chlorobenzene, concentration is obtained for PCDTBT:PC71BM=8mg/ml:The mixed solution of 32mg/ml, mixed solution is stirred in magnetic force
60 DEG C of heating stirring 12h on device are mixed, photoactive layer material is obtained.After the spin coating of photoactive layer material is completed, put on hot plate
Carry out thermal anneal process, process time is 30min, temperature is 60 DEG C, excess of solvent is volatilized and improve appearance structure.At annealing
The substrate with anode buffer layer and photoactive layer is moved on in plated film instrument from the junction of glove box and vacuum coater after reason,
Carry out the evaporation of cathode buffer layer.Using plated film instrument on photoactive layer evaporating Al q3Cathode buffer layer, evaporation rate isThickness is 0.5nm.Al metallic cathodes are equally prepared from by the way of evaporation, and evaporation rate isThickness is 150nm.The device effective area for preparing is 0.05cm2, in standard test condition：100mw/cm2,
Tested under the illumination simulation of AM1.5, Current density-voltage (J-V) curve is measured by Keithley2400 digital sourcemeters, surveyed
Examination process is carried out under atmospheric environment.Device architecture is：Transparent substrates/ITO/PTFE (thickness is 2.0nm)/PCDTBT:
PC71BM/Alq3(thickness is 0.5nm)/Al (thickness is 150nm).J-V curves such as Fig. 2 institutes measured by the device of comparative example 1
Show.
Comparative example 2
The substrate being made up of transparent conductive anode and transparent substrates is cleaned, transparent conductive anode material is tin indium oxide
(ITO), transparent substrates are glass.Use N2Substrate is dried up, heating 10min in baking oven is placed on, is processed with Plasma cleaning machines
10min.PTFE anode buffer layers are deposited with substrate, evaporation rate isThickness is 2.0nm.Evaporation is completed
Afterwards, 5min is processed with Plasma cleaning machines.Spin coating photoactive layer and made annealing treatment on anode buffer layer, method and contrast
Example 1 is identical.The substrate with anode buffer layer and photoactive layer is moved on in vacuum coater after annealing, is carried out negative electrode and is delayed
Rush the evaporation of layer.The evaporating Al q on photoactive layer3Cathode buffer layer, evaporation rate isThickness is 1.0nm.
Evaporating Al metallic cathode, evaporation rate isThickness is 150nm.Current density-voltage (J-V) curve is used
Keithley2400 digital sourcemeters are in 100mw/cm2, measured under conditions of AM1.5.Device architecture is：Transparent substrates ITO/PTFE
(thickness is 2.0nm)/PCDTBT:PC71BM/Alq3(thickness is 1.0nm)/Al (thickness is 150nm).The device institute of comparative example 2
The J-V curves for measuring are as shown in Figure 2.
Comparative example 3
The substrate being made up of transparent conductive anode and transparent substrates is cleaned, transparent conductive anode material is tin indium oxide
(ITO), transparent substrates are glass.Use N2Substrate is dried up, heating 10min in baking oven is placed on, is processed with Plasma cleaning machines
10min.PTFE anode buffer layers are deposited with, evaporation rate isThickness is 2.0nm.After the completion of evaporation, substrate is used
Plasma cleaning machines process 5min.Spin coating photoactive layer and made annealing treatment on anode buffer layer, method and the phase of comparative example 1
Together.The substrate with anode buffer layer and photoactive layer is moved on in vacuum coater after annealing, carries out cathode buffer layer
Evaporation, the evaporating Al q on photoactive layer3Cathode buffer layer, evaporation rate isThickness is 1.5nm.Evaporation
Al metallic cathodes, evaporation rate isThickness is 150nm.Current density-voltage (J-V) curve is used
Keithley2400 digital sourcemeters are in 100mw/cm2, measured under conditions of AM1.5.Device architecture is：Transparent substrates ITO/PTFE
(thickness is 2.0nm)/PCDTBT:PC71BM/Alq3(thickness is 1.5nm)/Al (thickness is 150nm).The device institute of comparative example 3
The J-V curves for measuring are as shown in Figure 2.
Table 1 is Alq3Single cathode buffer layer device is in different-thickness Alq3Under open-circuit voltage Voc (V), short-circuit current density
Jsc(mA/cm2), fill factor, curve factor FF (%), photoelectric transformation efficiency PCE (%), it can be seen that work as Alq3Thickness be 1.0nm when,
Device performance is the most excellent.
Table 1
| Voc(V) | Jsc(mA/cm2) | FF (%) | PCE (%) | |
| The device of comparative example 1 | 0.876 | 10.019 | 56.80 | 4.985 |
| The device of comparative example 2 | 0.883 | 11.377 | 59.01 | 5.929 |
| The device of comparative example 3 | 0.870 | 11.044 | 56.72 | 5.451 |
Comparative example 4
The substrate being made up of transparent conductive anode and transparent substrates is cleaned, transparent conductive anode material is tin indium oxide
(ITO), transparent substrates are glass.Use N2Substrate is dried up, heating 10min in baking oven is placed on, is processed with Plasma cleaning machines
10min.PTFE anode buffer layers are deposited with, evaporation rate isThickness is 2.0nm.After the completion of evaporation, use
Plasma cleaning machines process 5min.Spin coating photoactive layer and made annealing treatment on anode buffer layer, method and the phase of comparative example 1
Together.The substrate with anode buffer layer and photoactive layer is moved on in vacuum coater after annealing, carries out cathode buffer layer
Evaporation, CaF is deposited with photoactive layer2Cathode buffer layer, evaporation rate isThickness is 0.6nm.Evaporation
Al metallic cathodes, evaporation rate isThickness is 150nm.Current density-voltage (J-V) curve is used
Keithley2400 digital sourcemeters are in 100mw/cm2, measured under conditions of AM1.5.Device architecture is：Transparent substrates ITO/PTFE
(thickness is 2.0nm)/PCDTBT:PC71BM/CaF2(thickness is 0.6nm)/Al (thickness is 150nm).The device institute of comparative example 4
The J-V curves for measuring are as shown in Figure 3.
Comparative example 5
The substrate being made up of transparent conductive anode and transparent substrates is cleaned, transparent conductive anode material is tin indium oxide
(ITO), transparent substrates are glass.Use N2Substrate is dried up, heating 10min in baking oven is placed on, is processed with Plasma cleaning machines
10min.PTFE anode buffer layers are deposited with, evaporation rate isThickness is 2.0nm.After the completion of evaporation, use
Plasma cleaning machines process 5min.Spin coating photoactive layer and made annealing treatment on anode buffer layer, method and the phase of comparative example 1
Together.The substrate with anode buffer layer and photoactive layer is moved on in vacuum coater after annealing, carries out cathode buffer layer
Evaporation, CaF is deposited with photoactive layer2Cathode buffer layer, evaporation rate isThickness is 0.8nm.Evaporation
Al metallic cathodes, evaporation rate isThickness is 150nm.Current density-voltage (J-V) curve is used
Keithley2400 digital sourcemeters are in 100mw/cm2, measured under conditions of AM1.5.Device architecture is：Transparent substrates ITO/PTFE
(thickness is 2.0nm)/PCDTBT:PC71BM/CaF2(thickness is 0.8nm)/Al (thickness is 150nm).The device institute of comparative example 5
The J-V curves for measuring are as shown in Figure 3.
Comparative example 6
The substrate being made up of transparent conductive anode and transparent substrates is cleaned, transparent conductive anode material is tin indium oxide
(ITO), transparent substrates are glass.Use N2Substrate is dried up, heating 10min in baking oven is placed on, is processed with Plasma cleaning machines
10min.PTFE anode buffer layers are deposited with, evaporation rate isThickness is 2.0nm.After the completion of evaporation, use
Plasma cleaning machines process 5min.Spin coating photoactive layer and made annealing treatment on anode buffer layer, method and the phase of comparative example 1
Together.The substrate with anode buffer layer and cathode buffer layer is moved on in vacuum coater after annealing, carries out negative electrode buffering
The evaporation of layer, is deposited with CaF on photoactive layer2Cathode buffer layer, evaporation rate isThickness is 1.0nm.Steam
Al metallic cathodes are plated, evaporation rate isThickness is 150nm.Current density-voltage (J-V) curve is used
Keithley2400 digital sourcemeters are in 100mw/cm2, measured under conditions of AM1.5.Device architecture is：Transparent substrates ITO/PTFE
(thickness is 2.0nm)/PCDTBT:PC71BM/CaF2(thickness is 1.0nm)/Al (thickness is 150nm).The device institute of comparative example 6
The J-V curves for measuring are as shown in Figure 3.
Comparative example 7
The substrate being made up of transparent conductive anode and transparent substrates is cleaned, transparent conductive anode material is tin indium oxide
(ITO), transparent substrates are glass.Use N2Substrate is dried up, heating 10min in baking oven is placed on, is processed with Plasma cleaning machines
10min.PTFE anode buffer layers are deposited with, evaporation rate isThickness is 2.0nm.After the completion of evaporation, use
Plasma cleaning machines process 5min.Spin coating photoactive layer and made annealing treatment on anode buffer layer, method and the phase of comparative example 1
Together.The substrate with anode buffer layer and photoactive layer is moved on in vacuum coater after annealing, carries out cathode buffer layer
Evaporation, CaF is deposited with photoactive layer2Cathode buffer layer, evaporation rate isThickness is 1.2nm.Evaporation
Al metallic cathodes, evaporation rate isThickness is 150nm.Current density-voltage (J-V) curve is used
Keithley2400 digital sourcemeters are in 100mw/cm2, measured under conditions of AM1.5.Device architecture is：Transparent substrates ITO/PTFE
(thickness is 2.0nm)/PCDTBT:PC71BM/CaF2(thickness is 1.2nm)/Al (thickness is 150nm).The device institute of comparative example 7
The J-V curves for measuring are as shown in Figure 3.
Table 2 is CaF2Single cathode buffer layer device is in different-thickness CaF2Under open-circuit voltage Voc (V), short-circuit current density
Jsc(mA/cm2), fill factor, curve factor FF (%), photoelectric transformation efficiency PCE (%), when thickness be 0.6nm when, efficiency reaches
5.572%, work as CaF2Thickness when increasing to 1.0nm, device performance is optimal, and thickness continues to increase efficiency reduction.
Table 2
| Voc(V) | Jsc(mA/cm2) | FF (%) | PCE (%) | |
| The device of comparative example 4 | 0.874 | 10.997 | 57.94 | 5.572 |
| The device of comparative example 5 | 0.874 | 11.477 | 59.40 | 5.961 |
| The device of comparative example 6 | 0.882 | 11.848 | 60.27 | 6.296 |
| The device of comparative example 7 | 0.870 | 11.260 | 58.91 | 5.769 |
Comparative example 8
The substrate being made up of transparent conductive anode and transparent substrates is cleaned, transparent conductive anode material is tin indium oxide
(ITO), transparent substrates are glass.Use N2Substrate is dried up, heating 10min in baking oven is placed on, is processed with Plasma cleaning machines
10min.PTFE anode buffer layers are deposited with, evaporation rate isThickness is 2.0nm.After the completion of evaporation, use
Plasma cleaning machines process 5min.Spin coating photoactive layer and made annealing treatment on PTFE anode buffer layers, method and contrast
Example 1 is identical.The substrate with anode buffer layer and photoactive layer is moved on in vacuum coater after annealing, enters row metal cloudy
The evaporation of pole, the evaporating Al metallic cathode on photoactive layer, evaporation rate isThickness is 150nm.Electric current is close
Degree-voltage (J-V) curve is using Keithley2400 digital sourcemeters in 100mw/cm2, measured under conditions of AM1.5.Device junction
Structure is：Transparent substrates/ITO/PTFE (thickness is 2.0nm)/PCDTBT:PC71BM/Al (thickness is 150nm).
Embodiment 1
The substrate being made up of transparent conductive anode and transparent substrates is cleaned, transparent conductive anode material is tin indium oxide
(ITO), transparent substrates are glass.Use N2Substrate is dried up, heating 10min in baking oven is placed on, is processed with Plasma cleaning machines
10min.PTFE anode buffer layers are deposited with, evaporation rate isThickness is 2.0nm.After the completion of evaporation, use
Plasma cleaning machines process 5min.Substrate with anode buffer layer is moved on into N2In the glove box of atmosphere, entered using sol evenning machine
The spin coating of row photoactive layer material and polyvinylpyrrolidone mixed liquor, rotating speed is 1000rpm/s, and the time is 60s.Photoactive layer
Material is by electron donor material PCDTBT and electron acceptor material PC71BM in mass ratio 1:4 configurations are formed.Weigh 8mg's respectively
The PC of PCDTBT and 32mg71BM is dissolved in the chlorobenzene of 1ml, obtains concentration for PCDTBT:PC71BM=8mg/ml:32mg/ml's
Mixed solution, polyvinylpyrrolidone is dissolved in above-mentioned mixed solution, obtains polyvinylpyrrolidone mass fraction for 1wt%
Mixed solution, then 60 DEG C of heating stirring 12h on magnetic stirring apparatus.After spin coating is completed, stood in glove box
30min, because polyvinylpyrrolidone has self assembly effect, by the slow growth of 30min, moves to the upper of photoactive layer
Fang Chengwei polyvinylpyrrolidone cathode buffer layers, being then placed on carries out thermal anneal process in heating plate, process time is
30min, temperature is 60 DEG C, excess of solvent is volatilized and improves appearance structure.Above-mentioned substrate is moved on into Vacuum Deposition after annealing
In film instrument, the evaporation of follow-up cathode buffer layer is carried out, the evaporating Al q on polyvinylpyrrolidone cathode buffer layer3Negative electrode is buffered
Layer, evaporation rate isThickness is 1.0nm；In Alq3CaF is deposited with cathode buffer layer2Cathode buffer layer, steams
Sending out speed isThickness is 1.0nm.Al metallic cathodes are equally prepared from by the way of evaporation, evaporation speed
Rate isThickness is 150nm.Current density-voltage (J-V) curve is existed using Keithley2400 digital sourcemeters
100mw/cm2, measured under conditions of AM1.5.Device architecture is：Transparent substrates/ITO/PTFE (thickness is 2.0nm)/PCDTBT:
PC71BM/SAM polyvinylpyrrolidones (solution quality ratio is 1wt%)/Alq3 (thickness is 1.0nm)/CaF2(thickness is
1.0nm)/Al (thickness is 150nm).J-V curves measured by the device of embodiment 1 are as shown in Figure 4.
Embodiment 2
The substrate being made up of transparent conductive anode and transparent substrates is cleaned, transparent conductive anode material is tin indium oxide
(ITO), transparent substrates are glass.Use N2Substrate is dried up, heating 10min in baking oven is placed on, is processed with Plasma cleaning machines
10min.PTFE anode buffer layers are deposited with, evaporation rate isThickness is 2.0nm.After the completion of evaporation, use
Plasma cleaning machines process 5min.Substrate with anode buffer layer is moved on into N2In the glove box of atmosphere, entered using sol evenning machine
The spin coating of row photoactive layer material and polyvinylpyrrolidone mixed liquor, rotating speed is 1000rpm/s, and the time is 60s.Photoactive layer
Material is by electron donor material PCDTBT and electron acceptor material PC71BM in mass ratio 1:4 configurations are formed, and weigh 8mg's respectively
The PC of PCDTBT and 32mg71BM is dissolved in the chlorobenzene of 1ml, obtains concentration for PCDTBT:PC71BM=8mg/ml:32mg/ml's
Mixed solution, polyvinylpyrrolidone is dissolved in above-mentioned mixed solution, obtains polyvinylpyrrolidone mass fraction for 2wt%
Mixed solution, then 60 DEG C of heating stirring 12h on magnetic stirring apparatus.After spin coating is completed, stood in glove box
30min, because polyvinylpyrrolidone has self assembly effect, by the slow growth of 30min, moves to the upper of photoactive layer
Fang Chengwei cathode buffer layers, being then placed on carries out thermal anneal process in heating plate, process time is 30min, and temperature is 60 DEG C, is made
Excess of solvent volatilizees and improves appearance structure.Above-mentioned substrate is moved on in vacuum coater after annealing, carries out follow-up negative electrode
The evaporation of cushion, the evaporating Al q on polyvinylpyrrolidone cathode buffer layer3Cathode buffer layer, evaporation rate isThickness is 1.0nm；In Alq3CaF is deposited with cathode buffer layer2Cathode buffer layer, evaporation rate isThickness is 1.0nm.Al metallic cathodes are equally prepared from by the way of evaporation, and evaporation rate isThickness is 150nm.Current density-voltage (J-V) curve is using Keithley2400 digital sourcemeters in 100mw/
cm2, measured under conditions of AM1.5.Device architecture is：Transparent substrates/ITO/PTFE (thickness is 2.0nm)/PCDTBT:PC71BM/
Polyvinylpyrrolidone (solution quality ratio is 2wt%)/Alq3(thickness is 1.0nm)/CaF2(thickness is 1.0nm)/Al (thickness
It is 150nm).J-V curves measured by the device of embodiment 2 are as shown in Figure 4.
Embodiment 3
The substrate being made up of transparent conductive anode and transparent substrates is cleaned, transparent conductive anode material is tin indium oxide
(ITO), transparent substrates are glass.Use N2Substrate is dried up, heating 10min in baking oven is placed on, is processed with Plasma cleaning machines
10min.PTFE anode buffer layers are deposited with, evaporation rate isThickness is 2.0nm.After the completion of evaporation, use
Plasma cleaning machines process 5min.Substrate with anode buffer layer is moved on into N2In the glove box of atmosphere, entered using sol evenning machine
The spin coating of row photoactive layer material and polyvinylpyrrolidone, rotating speed is 1000rpm/s, and the time is 60s.Photoactive layer material by
Electron donor material PCDTBT and electron acceptor material PC71BM in mass ratio 1:4 configurations are formed, and the PCDTBT of 8mg is weighed respectively
With the PC of 32mg71BM is dissolved in the chlorobenzene of 1ml, obtains concentration for PCDTBT:PC71BM=8mg/ml:The mixing of 32mg/ml is molten
Liquid, polyvinylpyrrolidone is dissolved in mixed solution, obtains the solution that polyvinylpyrrolidone mass fraction is 3wt%, so
60 DEG C of heating stirring 12h on magnetic stirring apparatus afterwards.After spin coating is completed, 30min is stood in glove box, due to polyethylene pyrrole
Pyrrolidone has self assembly effect, and by the slow growth of 30min, the top for moving to photoactive layer turns into polyvinylpyrrolidine
Ketone cathode buffer layer, being then placed on carries out thermal anneal process in heating plate, process time is 30min, and temperature is 60 DEG C, and it is unnecessary to make
Solvent volatilizees and improves appearance structure.Above-mentioned substrate is moved on in vacuum coater after annealing, carries out follow-up negative electrode buffering
The evaporation of layer, the evaporating Al q on polyvinylpyrrolidone cathode buffer layer3Cathode buffer layer, evaporation rate isThickness is 1.0nm；In Alq3CaF is deposited with cathode buffer layer2Cathode buffer layer, evaporation rate isThickness is 1.0nm.Metallic cathode Al is equally prepared from by the way of evaporation, and evaporation rate isThickness is 150nm.Current density-voltage (J-V) curve is using Keithley2400 digital sourcemeters in 100mw/
cm2, measured under conditions of AM1.5.Device architecture is：Transparent substrates/ITO/PTFE (thickness is 2.0nm)/PCDTBT:PC71BM/
SAM polyvinylpyrrolidones (solution quality ratio is 3wt%)/Alq3(thickness is 1.0nm)/CaF2(thickness is 1.0nm)/Al is (thick
It is 150nm to spend).J-V curves measured by the device of embodiment 3 are as shown in Figure 4.
Table 3 is the performance that lamination cathode buffer layer device of the invention changes with polyvinylpyrrolidonesolution solution mass fraction
Parameter (Alq3Thickness be 1.0nm, CaF2Thickness be 1.0nm), the performance test of device is in 100mw/cm2, AM1.5's
Carried out under illumination simulation.When the mass fraction of polyvinylpyrrolidone is 2wt%, efficiency reaches 7.349%, and device performance reaches
To optimal, polyvinylpyrrolidone mass fraction continuation increase efficiency reduction.
Table 3
| Voc(V) | Jsc(mA/cm2) | FF (%) | PCE (%) | |
| The device of embodiment 1 | 0.891 | 12.154 | 61.98 | 6.711 |
| The device of embodiment 2 | 0.899 | 12.754 | 64.11 | 7.349 |
| The device of embodiment 3 | 0.898 | 12.266 | 63.22 | 6.961 |
Table 4 is the device of comparative example 8 (without cathode buffer layer), single cathode buffer layer device (1.0nmAlq3、1.0nmCaF2) with
The contrast of lamination cathode buffer layer organic polymer solar cell performance parameter of the present invention, the performance test of device exists
100mw/cm2, carried out under the illumination simulation of AM1.5.When using lamination cathode buffer layer, series resistance reduction, efficiency reaches
7.349%, device performance is optimal, and the device performance of single cathode buffer layer is better than comparative device (without cathode buffer layer), string
Connection resistance is less than comparative device.
Table 4
| Voc(V) | Jsc(mA/cm2) | FF (%) | PCE (%) | Rs(Ω·cm2) | |
| The device of comparative example 2 | 0.883 | 11.377 | 59.01 | 5.929 | 10.477 |
| The device of comparative example 6 | 0.882 | 11.848 | 60.27 | 6.296 | 9.144 |
| The device of embodiment 2 | 0.899 | 12.754 | 64.11 | 7.349 | 7.276 |
| The device of comparative example 8 | 0.872 | 10.140 | 52.62 | 4.651 | 16.358 |
Table 5 is for structure：Transparent substrates/ITO/PTFE (thickness is 2.0nm)/PCDTBT:PC71BM/ polyvinylpyrrolidines
Ketone (polyvinylpyrrolidone mass fraction is 2wt%)/Alq3(thickness is 1.0nm)/CaF2(thickness is 1.0nm)/Al (thickness
Be 150nm), transparent substrates/ITO/PTFE (thickness is 2.0nm)/PCDTBT:PC71BM/ polyvinylpyrrolidones (polyethylene pyrrole
Pyrrolidone mass fraction is 2wt%)/CaF2(thickness is 1.0nm)/Alq3(thickness is 1.0nm)/Al's (thickness is 150nm) is folded
The contrast of layer cathode buffer layer organic polymer solar cell performance parameter, the performance test of device is in 100mw/cm2,
Carried out under the illumination simulation of AM1.5.It can be seen that when cathode buffer layer of the device architecture using different order to device performance
Have a certain impact, only select suitable order, energy level could be made more to match, be conducive to transmission and extraction, the boundary of electronics
Good Ohmic contact is formed between face.
Table 5
In addition to the implementation, polyvinylpyrrolidone cathode buffer layer of the invention can also be straight by the method for spin coating
Connect and be prepared on photoactive layer.Wherein photoactive layer is prepared on anode buffer layer by following methods：By electron donor material
PCDTBT and electron acceptor material PC71BM is according to 1:4 mass ratio obtains photoactive layer material in being blended in solvent chlorobenzene, then
It is spun on anode buffer layer.Polyvinylpyrrolidone is dissolved in isopropanol after being made into the solution of 1mg/mL and is spun on photoactive layer
On.
Embodiment 4
The substrate being made up of transparent conductive anode and transparent substrates is cleaned, transparent conductive anode material is tin indium oxide
(ITO), transparent substrates are glass.Use N2Substrate is dried up, heating 10min in baking oven is placed on, is processed with Plasma cleaning machines
10min.PTFE anode buffer layers are deposited with, evaporation rate isThickness is 2.0nm.After the completion of evaporation, use
Plasma cleaning machines process 5min.Substrate with anode buffer layer is moved on into N2In the glove box of atmosphere, using sol evenning machine point
Other spin coating photoactive layer material and polyvinylpyrrolidone cathode buffer layer are simultaneously made annealing treatment, the wherein spin coating of photoactive layer
It is identical with comparative example 1.Polyvinylpyrrolidone is dissolved in isopropanol after being made into the solution of 1mg/mL and being spin-coated on photoactive layer, turns
Speed is 3000rpm/s, and the time is 45s.After the completion of spin coating, thermal anneal process is carried out, process time is 20min, and temperature is 120
℃.Above-mentioned substrate is moved on in vacuum coater after annealing, the evaporation of follow-up cathode buffer layer is carried out, in polyvinyl pyrrole
Evaporating Al q on alkanone cathode buffer layer3Cathode buffer layer, evaporation rate isThickness is 1.0nm；In Alq3
CaF is deposited with cathode buffer layer2Cathode buffer layer, evaporation rate isThickness is 1.0nm.Al metallic cathodes
Same to be prepared from by the way of evaporation, evaporation rate isThickness is 150nm.Current density-voltage (J-
V) curve uses Keithley2400 digital sourcemeters in 100mw/cm2, measured under conditions of AM1.5.Device architecture is：Transparent lining
Bottom/ITO/PTFE (thickness is 2.0nm)/PCDTBT:PC71BM/SAM polyvinylpyrrolidones (rotating speed is 3000rpm/s)/Alq3
(thickness is 1.0nm)/CaF2(thickness is 1.0nm)/Al (thickness is 150nm).Embodiment 5
The substrate being made up of transparent conductive anode and transparent substrates is cleaned, transparent conductive anode material is tin indium oxide
(ITO), transparent substrates are glass.Use N2Substrate is dried up, heating 10min in baking oven is placed on, is processed with Plasma cleaning machines
10min.PTFE anode buffer layers are deposited with, evaporation rate isThickness is 2.0nm.After the completion of evaporation, use
Plasma cleaning machines process 5min.Substrate with anode buffer layer is moved on into N2In the glove box of atmosphere, using sol evenning machine point
Other spin coating photoactive layer material and polyvinylpyrrolidone cathode buffer layer are simultaneously made annealing treatment, the wherein spin coating of photoactive layer
It is identical with comparative example 1.Polyvinylpyrrolidone is dissolved in isopropanol after being made into the solution of 1mg/mL and being spin-coated on photoactive layer, turns
Speed is 4000rpm/s, and the time is 45s.After the completion of spin coating, thermal anneal process is carried out, process time is 20min, and temperature is 120
℃.Above-mentioned substrate is moved on in vacuum coater after annealing, the evaporation of follow-up cathode buffer layer is carried out, in polyvinyl pyrrole
Evaporating Al q on alkanone cathode buffer layer3Cathode buffer layer, evaporation rate isThickness is 1.0nm；In Alq3
CaF is deposited with cathode buffer layer2Cathode buffer layer, evaporation rate isThickness is 1.0nm.Al metallic cathodes
Same to be prepared from by the way of evaporation, evaporation rate isThickness is 150nm.Current density-voltage (J-
V) curve uses Keithley2400 digital sourcemeters in 100mw/cm2, measured under conditions of AM1.5.Device architecture is：Transparent lining
Bottom/ITO/PTFE (thickness is 2.0nm)/PCDTBT:PC71BM/SAM polyvinylpyrrolidones (rotating speed is 4000rpm/s)/Alq3
(thickness is 1.0nm)/CaF2(thickness is 1.0nm)/Al (thickness is 150nm).Embodiment 6
The substrate being made up of transparent conductive anode and transparent substrates is cleaned, transparent conductive anode material is tin indium oxide
(ITO), transparent substrates are glass.Use N2Substrate is dried up, heating 10min in baking oven is placed on, is processed with Plasma cleaning machines
10min.PTFE anode buffer layers are deposited with, evaporation rate isThickness is 2.0nm.After the completion of evaporation, use
Plasma cleaning machines process 5min.Substrate with anode buffer layer is moved on into N2In the glove box of atmosphere, using sol evenning machine point
Other spin coating photoactive layer material and polyvinylpyrrolidone cathode buffer layer are simultaneously made annealing treatment, the wherein spin coating of photoactive layer
It is identical with comparative example 1.Polyvinylpyrrolidone is dissolved in isopropanol after being made into the solution of 1mg/mL and being spin-coated on photoactive layer, turns
Speed is 5000rpm/s, and the time is 45s.After the completion of spin coating, thermal anneal process is carried out, process time is 20min, and temperature is 120
℃.Above-mentioned substrate is moved on in vacuum coater after annealing, the evaporation of follow-up cathode buffer layer is carried out, in polyvinyl pyrrole
Evaporating Al q on alkanone cathode buffer layer3Cathode buffer layer, evaporation rate isThickness is 1.0nm；In Alq3
CaF is deposited with cathode buffer layer2Cathode buffer layer, evaporation rate isThickness is 1.0nm.Al metallic cathodes
Same to be prepared from by the way of evaporation, evaporation rate isThickness is 150nm.Current density-voltage (J-
V) curve uses Keithley2400 digital sourcemeters in 100mw/cm2, measured under conditions of AM1.5.Device architecture is：Transparent lining
Bottom/ITO/PTFE (thickness is 2.0nm)/PCDTBT:PC71BM/SAM polyvinylpyrrolidones (rotating speed is 5000rpm/s)/Alq3
(thickness is 1.0nm)/CaF2(thickness is 1.0nm)/Al (thickness is 150nm).
Table 6 is the performance parameter that lamination cathode buffer layer device of the invention changes with polyvinylpyrrolidonesolution solution rotating speed
(Alq3Thickness be 1.0nm, CaF2Thickness be 1.0nm), the performance test of device is in 100mw/cm2, the simulation of AM1.5
Carried out under illumination.When the rotating speed of polyvinylpyrrolidonesolution solution is 4000rpm/s, efficiency reaches 7.000%, and device performance reaches
To optimal, rotating speed continuation increase, thickness increase, efficiency reduction are caused.
Table 6
| Voc(V) | Jsc(mA/cm2) | FF (%) | PCE (%) | |
| The device of embodiment 4 | 0.885 | 11.699 | 61.70 | 6.387 |
| The device of embodiment 5 | 0.882 | 12.434 | 63.82 | 7.000 |
| The device of embodiment 6 | 0.875 | 12.387 | 61.37 | 6.611 |
Lamination cathode buffer layer organic polymer solar cell of the invention, its open-circuit voltage Voc (V), short circuit current
Density Jsc (mA/cm2), fill factor, curve factor FF (%), photoelectric transformation efficiency PCE (%) mainly with each cathode buffer layer material therefor,
Order is relevant with thickness, thus the material and preparation technology parameter of each layer choosing are not limited to above-described embodiment.For example, this area skill
Art personnel can be with reasonable prediction, and when anode buffer layer selects other materials and different-thickness, the performance of device can also reach
Essentially identical technique effect.
By introducing lamination cathode buffer layer, the interface modified between photoactive layer and metallic cathode reduces the present invention
The series resistance of device, the transmission resistance for reducing impedance and then electric charge diminishes, and promotes electronics from photoactive layer to metallic cathode
Transmission, improve electronic transmission performance, reduce Carrier recombination probability, at the same contact resistance reduction.Lamination cathode buffer layer
The corrosion of electrode is prevented, battery has more stability.The work function of other lamination cathode buffer layer with from photoactive layer
Electron acceptor material is more matched, and is conducive to forming good Ohmic contact between photoactive layer and negative electrode, further to promote
The transmission and extraction of electronics, and then can effectively improve the photoelectric transformation efficiency of device.
Claims (10)
1. a kind of lamination cathode buffer layer organic polymer solar cell, using eurymeric structure, is followed successively by from top to bottom：It is transparent
Substrate, transparent conductive anode, anode buffer layer, photoactive layer, cathode buffer layer, metallic cathode；It is characterized in that the light is lived
Property layer be electron donor material PCDTBT and electron acceptor material PC71BM is according to 1:The composition of 4 mass ratio mixing；Negative electrode delays
Layer is rushed to use by polyvinylpyrrolidone cathode buffer layer, Alq3Cathode buffer layer and CaF2The lamination that cathode buffer layer is constituted is cloudy
Pole cushion；Polyvinylpyrrolidone cathode buffer layer is prepared on photoactive layer；Alq3Cathode buffer layer is prepared in polyethylene
On pyrrolidones cathode buffer layer, its thickness is 0.5~1.5nm；CaF2Cathode buffer layer is prepared in Alq3Cathode buffer layer and gold
Between category negative electrode, its thickness is 0.6~1.2nm.
2. lamination cathode buffer layer organic polymer solar cell according to claim 1, it is characterised in that described poly-
Vinylpyrrolidone cathode buffer layer is prepared on photoactive layer by spin coating method.
3. lamination cathode buffer layer organic polymer solar cell according to claim 1, it is characterised in that described poly-
Vinylpyrrolidone cathode buffer layer can also be prepared on photoactive layer by self-assembling method, form SAM polyvinyl pyrroles
Alkanone cathode buffer layer.
4. lamination cathode buffer layer organic polymer solar cell according to claim 3, it is characterised in that the SAM
Polyvinylpyrrolidone cathode buffer layer preparation method is as follows：By electron donor material PCDTBT and electron acceptor material PC71BM
According to 1:4 mass ratio obtains photoactive layer material in being blended in solvent chlorobenzene, then polyvinylpyrrolidone is dissolved in into light work
The mixed solution that polyvinylpyrrolidone mass fraction is 1~3wt% is configured in property layer material, then on magnetic stirring apparatus
12~14h is stirred in 50~80 DEG C of heating simultaneously；In the glove box of nitrogen atmosphere, using sol evenning machine carry out photoactive layer material with
The spin coating of polyvinylpyrrolidone mixed solution, rotating speed is 1000rpm/s, and the time is 60s；After spin coating is completed, in glove box
30~60min of middle standing, makes polyvinylpyrrolidone turn into polyethylene in the top that self assembly effect is moved to photoactive layer
Pyrrolidones cathode buffer layer；It is last that 20~40min is made annealing treatment under the conditions of 60~80 DEG C.
5. lamination cathode buffer layer organic polymer solar cell according to claim 4, it is characterised in that described poly-
Vinylpyrrolidone is dissolved in photoactive layer material, and its mass fraction is 2wt%；Alq3Cathode buffer layer and CaF2Negative electrode delays
Rush thickness degree and be 1.0nm.
6. lamination cathode buffer layer organic polymer solar cell according to claim 1, it is characterised in that described
Transparent substrates include polyethylene terephthalate using glass substrate or transparent polymer substrate, wherein transparent polymer
One or more in ester, polystyrene, polyethylene, vinyl chloride-vinyl acetate resin or polyacrylic acid.
7. lamination cathode buffer layer organic polymer solar cell according to claim 1, it is characterised in that described
Bright conductive anode material therefor is tin indium oxide (ITO), and tin indium oxide is deposited on a transparent substrate, and transparent conductive anode thickness is
150nm, square resistance is 15 Ω/.
8. lamination cathode buffer layer organic polymer solar cell according to claim 1, it is characterised in that described
Anode buffer layer material uses polytetrafluoroethylene (PTFE), PEDOT:PSS, or p-type oxide M oO3、WO3、V2O5, high work function hole passes
One kind in defeated material Ni O or by two of which and it is two or more be prepared from from level to level in order, thickness is 1~20nm.
9. lamination cathode buffer layer organic polymer solar cell according to claim 1, it is characterised in that described
Using the one kind in Al, Ca, Mg or Li or by several alloys for constituting therein, its thickness is 80nm~180nm to metallic cathode.
10. a kind of preparation method of lamination cathode buffer layer organic polymer solar cell as claimed in claim 1, it is special
Levy is to comprise the following steps：
(1) substrate that cleaning is made up of transparent substrates and transparent conductive anode；
(2) after substrate is dried, anode buffer layer is deposited with transparent anode；
(3) after anode buffer layer evaporation is completed, photoactive layer and polyvinylpyrrolidone negative electrode are prepared on anode buffer layer
Cushion, preparation method is as follows：By electron donor material PCDTBT and electron acceptor material PC71BM is according to 1:4 mass ratio is mixed
Conjunction obtains photoactive layer material in solvent chlorobenzene, then polyvinylpyrrolidone is dissolved in photoactive layer material is configured to gather
Vinylpyrrolidone mass fraction is the mixed solution of 1~3wt%, and then 50~80 DEG C of heating are stirred simultaneously on magnetic stirring apparatus
Mix 12~14h；In the glove box of nitrogen atmosphere, carry out photoactive layer material using sol evenning machine and mix with polyvinylpyrrolidone
The spin coating of solution, rotating speed is 1000rpm/s, and the time is 60s；After spin coating is completed, 30~60min is stood in glove box, made
Polyvinylpyrrolidone turns into polyvinylpyrrolidone cathode buffer layer in the top that self assembly effect is moved to photoactive layer；
It is last that 20~40min is made annealing treatment under the conditions of 60~80 DEG C；
(4) the evaporating Al q on polyvinylpyrrolidone cathode buffer layer3Cathode buffer layer, its thickness is 0.5~1.5nm, evaporation
Speed isNext in Alq3CaF is deposited with cathode buffer layer2Cathode buffer layer, its thickness be 0.6~
1.2nm, evaporation rate is
(5) the evaporation metal negative electrode on cathode buffer layer.
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