CN107180915A - Polymer solar cells based on double-decker cathode interface layer and preparation method thereof - Google Patents
Polymer solar cells based on double-decker cathode interface layer and preparation method thereof Download PDFInfo
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Abstract
The invention discloses a kind of polymer solar cells based on double-decker cathode interface layer and preparation method thereof.The battery employs the cathode interface layer of double-decker；The cathode interface layer is made up of cathode interface layer 1 and the superposition of cathode interface layer 2；The material of the cathode interface layer 1 is water-soluble polymer, and the material of the cathode interface layer 2 is alcohol soluble polymer, and the alcohol soluble polymer is that side chain carries the conjugated polymer of polar group, backbone units containing fluorenes or carbazole.The present invention is relative to existing polymer solar cells, with high open circuit voltage, high short circuit current flow and high fill factor, and higher photoelectric transformation efficiency, and cathode interface layer is prepared using simple coating thin film-forming method, high-temperature process is not needed, preparation process is simply and readily controlled, suitable for flexible device and large-scale industrial production.
Description
Technical field
The present invention relates to field of new energy technologies, and in particular to a kind of polymer based on double-decker cathode interface layer is too
Positive electricity pond and preparation method thereof.
Background technology
In recent years, organic/polymer solar cells due to preparation technology is simple, light weight, it is cheap, can prepare it is big
The advantages of area flexible device and receive significant attention.Polymer solar cells, with the new and potential device junction of one kind
Structure, its use electron donor material (such as conjugated polymer, conjugation small molecule) and electron acceptor material (such as fullerene derivate,
Non- fullerene small molecule or polymer) composition microphase-separated type mixture as photoactive layer (Science 1995,270,
1789；Acc.Chem.Res.2009,42,1709；Adv.Mater.2016,28,7821).In the routine of polymer solar cells
In structure, generally by ITO and PEDOT:PSS is respectively as anode and anode buffer layer, and vacuum-deposited metal is used as negative electrode.Most
Closely, it is effectively used to prepare high-efficiency polymerization as the flip-chip device structure of anode as negative electrode and high work function metal using ITO
Thing solar cell, and this structure is proved to have more superior stability (Sol.Energy Mater.Sol.Cells
2010,95,1785；Energy Environ.Sci.2015,8,3442).Wherein, negative electrode is used as using suitable boundary material
Boundary layer is used for polymer solar cells, is a very important engineering, influences very big to device performance.At present, with ITO
For in the upside-down mounting polymer solar cells of negative electrode, conventional cathode interface layer material mainly has：1. inorganic salts, such as Cs2CO3,CsF
(Appl.Phys.Lett.2006,88,253503；Appl.Phys.Lett.2011,98,053303), its filming performance is bad；
2. metal oxide, such as TiOx,ZnO(Appl.Phys.Lett.2006,89,233517；J.Phys.Chem.C 2010,114,
6849), it prepares Chang Yaoyong high-temperature process (more than 200 DEG C) in processing, and this is incompatible with flexible substrate；3. surfactant,
Such as PEO (Sol.Energy Mater.Sol.Cells 2010,94,497), device performance performance is typically.
The content of the invention
Based on above-mentioned background, the present invention provides a kind of polymer solar cells with double-decker cathode interface layer, with
And the preparation method of the battery.The present invention is relative to existing polymer solar cells, with high open circuit voltage, high short circuit current flow
And high fill factor, and higher photoelectric transformation efficiency, and cathode interface layer is prepared using simple coating thin film-forming method,
High-temperature process is not needed, preparation process is simply and readily controlled, suitable for flexible device and large-scale industrial production.
The polymer solar cells scheme that the present invention is provided, employs the cathode interface layer of double-decker；Negative electrode circle
Surface layer is made up of cathode interface layer 1 and the superposition of cathode interface layer 2.The material of the cathode interface layer 1 is water-soluble polymer,
The Water-soluble Polymer Molecules formula has following structure：
Wherein：
Z-For halide ion, x=0-0.5, y=0.5-1, x+y=1, m=1-6, n=100-100000.Negative electrode circle
The material of surface layer 2 is alcohol soluble polymer, and the alcohol soluble polymer is that molecular formula side chain contains with polar group, backbone units
The conjugated polymer of fluorenes or carbazole.
Double-decker cathode interface layer in the present invention is applied to the polymer solar cells of inverted structure or conventional structure,
The cathode interface layer 1 and cathode interface layer 2 of double-decker cathode interface layer are constituted, its mutual alignment can be exchanged.
Present invention also offers the preparation method of the polymer solar cells, methods described includes：
(1) water-soluble polymer with preceding formulae structure is prepared：
(2) prepare molecular formula side chain and carry the alcohol soluble polymer of polar group, backbone units containing fluorenes or carbazole；
(3) for the polymer solar cells of inverted structure, with reference to existing process, the water-soluble polymer is spun on
Cathode interface layer 1 is formed on ITO negative electrodes, the alcohol soluble polymer is spun on cathode interface layer 1 and forms cathode interface layer
2, photoactive layer is made on cathode interface layer 2, anode interface layer and anode are made on photoactive layer.Or, by the alcohol
Soluble polymer, which is spun on ITO negative electrodes, forms cathode interface layer 2, and the water-soluble polymer is spun on into cathode interface layer 2
Upper formation cathode interface layer 1, makes photoactive layer on cathode interface layer 1, anode interface layer and sun is made on photoactive layer
Pole.
(4) for the polymer solar cells of conventional structure, with reference to existing process, using ITO as anode, in ITO sun
It is extremely upper to prepare PEDOT:PSS anode buffer layers, in PEDOT:Photoactive layer is prepared on PSS anode buffer layers, afterwards in photolytic activity
Cathode interface layer 1 and cathode interface layer 2 are sequentially prepared on layer, then negative electrode is prepared on cathode interface layer 2.Or, use ITO
As anode, PEDOT is prepared on ito anode:PSS anode buffer layers, in PEDOT:Photolytic activity is prepared on PSS anode buffer layers
Layer, is sequentially prepared cathode interface layer 2 and cathode interface layer 1 on photoactive layer afterwards, is then prepared on cathode interface layer 1 cloudy
Pole.
Brief description of the drawings
Fig. 1 is a kind of structural representation of heretofore described upside-down mounting polymer solar cells.
Fig. 2 is the current -voltage curve figure of the upside-down mounting polymer solar cells without cathode interface layer.
Fig. 3 is electric current-electricity as the upside-down mounting polymer solar cells of cathode interface layer based on water-soluble polymer PDMC
Buckle line chart.
Fig. 4 is the current-voltage as the upside-down mounting polymer solar cells of cathode interface layer based on alcohol soluble polymer PFN
Curve map.
Fig. 5 is the PDMC/PFN double-decker negative electrodes constituted based on water-soluble polymer PDMC and alcohol soluble polymer PFN
The current -voltage curve figure of the upside-down mounting polymer solar cells of boundary layer.
Embodiment
Below by taking upside-down mounting polymer solar cells as an example, the present invention is described in further detail.
(1) preparation of water-soluble polymer 1 (PDMC)：By 207.7 grams of MethacryloyloxyethylTrimethyl Trimethyl Ammonium Chlorides point
It is dispersed in 114.7 grams of deionized waters, adds 1 milliliter of the ammonium persulfate aqueous solution that concentration is 1 mol/L, poured into after stirring mixing
In one polyethylene plastic bag.The charging polybag is fixed on to the centre for two stainless sheet steels that separation distance is 1 centimetre, placed
The polymerisation 6 hours in temperature is 65 degree of thermostat water bath.Resulting polymers obtain water-soluble polymer 1 after drying,
That is polymer P DMC.The molecular weight of the polymer is 1,000,000, is expressed as follows with molecular formula：
(2) preparation of water-soluble polymer 2：28.4 grams of acrylamides (0.4 mole) are dissolved in 28.4 grams at room temperature
Ionized water.124.62 grams of MethacryloyloxyethylTrimethyl Trimethyl Ammonium Chlorides (0.6 mole) are dispersed in 130 grams of deionized waters.
The MethacryloyloxyethylTrimethyl Trimethyl Ammonium Chloride aqueous solution is mixed with aforesaid propylene amide aqueous solution, concentration is added and is rubbed for 1
You/liter 1 milliliter of ammonium persulfate aqueous solution, stirring mixing after pour into a polyethylene plastic bag.The charging polybag is fixed
In centre of the separation distance for 1 centimetre of two stainless sheet steels, polymerisation 6 in the thermostat water bath that temperature is 65 degree is placed on
Hour.Resulting polymers obtain water-soluble polymer 2 after drying.The molecular weight of the polymer is 3,000,000, is expressed with molecular formula
It is as follows：
(3) alcohol soluble polymer PFN preparation：According to document Chem.Mater.2004,16,708 synthesis PFN, polymerization side
Method and route are as follows：
(4) preparation of the upside-down mounting polymer solar cells without cathode interface layer and performance：
There is conductive cathode ITO transparent glass substrate some with lot number sputtering, specification is 15 millimeters × 15 millimeters, ITO's
Thickness is about 110 nanometers, and its square resistance is about 10 ohm/.Successively with acetone, micron level semiconductor special purpose detergent, go
Ionized water (twice), isopropanol are subsequently placed into constant temperature oven at 80 DEG C and done to clean ITO substrate surfaces for ultrasonically treated 20 minutes
It is dry to stay overnight.In anhydrous, anaerobic, the special gloves case full of high pure nitrogen, by 10 milligrams every milliliter of PTB7 and PC71BM (matter
Amount is than being 1:1.5) chlorobenzene mixed solution (containing the 1,8- diiodo-octanes additive that volume content is 3%) is at 1500 revs/min
It is spun under the rotating speed of clock or so on the negative electrode ITO of above-mentioned dried and clean, obtains the photoactive layer of 80-90 rans.Finally,
3 × 10-4The molybdenum trioxide of 10 nanometers of vacuum evaporation is used as anode as anode interface layer and 100 nanometers of aluminium successively under handkerchief.
Curve in Fig. 2 gives the device in 100 milliwatts (mW/cm every square centimeter2) simulated solar light irradiation under
Current -voltage curve.The open-circuit voltage of obtained device is 0.33 volt, and short circuit current flow is 16.26 milliamperes every square centimeter,
Fill factor, curve factor is 44.9%, and photoelectric transformation efficiency is 2.41%.
(5) preparation based on water-soluble polymer PDMC as the upside-down mounting polymer solar cells of cathode interface layer and property
Energy：
With the aqueous solution that the water-soluble polymer PDMC configuration concentrations prepared by step (1) are 1 milligram every milliliter, fully stir
Mix, stand, and filtered with 0.45 micron of filter, it is stand-by.
Conductive ITO/glass substrate is cleaned and dried according to step (4).By the PDMC aqueous solution filtered with 3000 revs/min
The rotating speed of clock is spun on the ITO negative electrodes of above-mentioned dried and clean, and in heat drying 20 minutes at 100 DEG C, obtains 3 nano thickness
Cathode interface layer.Then the above-mentioned ITO for coating cathode interface layer is transferred to anhydrous, anaerobic, full of the special of high pure nitrogen
In glove box, by 10 milligrams every milliliter of PTB7 and PC71(mass ratio is 1 to BM:1.5) chlorobenzene mixed solution (contains containing volume
Measure 1, the 8- diiodo-octanes additive for 3%) it is spun under 1500 revs/min or so of rotating speed on cathode interface layer, then
In being dried 10 minutes at 70 DEG C, the photoactive layer of 80-90 rans is obtained.Finally, 3 × 10-4Vacuum evaporation successively under handkerchief
10 nanometers of molybdenum trioxide is used as anode as anode interface layer and 100 nanometers of aluminium.
Curve in Fig. 3 gives the device in 100mW/cm2Simulated solar light irradiation under current -voltage curve.
The open-circuit voltage of obtained device is 0.72 volt, and short circuit current flow is 16.68 milliamperes every square centimeter, and fill factor, curve factor is
64.3%, photoelectric transformation efficiency is 7.72%.Compared with the battery without cathode interface layer prepared in step (4), open circuit electricity
Pressure improves 0.39 volt, and short circuit current flow improves 2.6%, and fill factor, curve factor increases 43.2%, and efficiency is improved more than twice.
(6) preparation based on alcohol soluble polymer PFN as the upside-down mounting polymer solar cells of cathode interface layer and performance：
With the alcohol soluble polymer PFN configuration concentrations prepared by step (3) for 0.5 milligram every milliliter methanol solution (plus
Enter the acetic acid hydrotropy that volume content is 1%), it is sufficiently stirred for, stands, and filtered with 0.45 micron of filter, it is stand-by.
Conductive ITO/glass substrate is cleaned and dried according to step (4).By the PFN methanol solutions filtered with 2000 revs/min
The rotating speed of clock is spun on the ITO negative electrodes of above-mentioned dried and clean, and in heat drying 10 minutes at 100 DEG C, obtains 5 nano thickness
Cathode interface layer.Then the above-mentioned ITO for coating cathode interface layer is transferred to anhydrous, anaerobic, full of the special of high pure nitrogen
In glove box, by 10 milligrams every milliliter of PTB7 and PC71(mass ratio is 1 to BM:1.5) chlorobenzene mixed solution (contains containing volume
Measure 1, the 8- diiodo-octanes additive for 3%) it is spun under 1500 revs/min or so of rotating speed on cathode interface layer, then
In being dried 10 minutes at 70 DEG C, the photoactive layer of 80-90 rans is obtained.Finally, 3 × 10-4Vacuum evaporation successively under handkerchief
10 nanometers of molybdenum trioxide is used as anode as anode interface layer and 100 nanometers of aluminium.
Curve in Fig. 4 gives the device in 100mW/cm2Simulated solar light irradiation under current -voltage curve.
The open-circuit voltage of obtained device is 0.75 volt, and short circuit current flow is 16.22 milliamperes every square centimeter, and fill factor, curve factor is
70.8%, photoelectric transformation efficiency is 8.61%.With it is prepared in embodiment 5 be cathode interface based on water-soluble polymer PDMC
The battery of layer is compared, and open-circuit voltage improves 0.03 volt, and short circuit current flow, which has, slightly to be reduced, and fill factor, curve factor increases 10.1%, effect
Rate improves 11.5%.
(7) based on the water-soluble polymer PDMC and alcohol soluble polymer PFN PDMC/PFN twin cathode boundary layers constituted
The preparation of upside-down mounting polymer solar cells and performance：
The PDMC aqueous solution and PFN methanol solutions has been respectively configured according to step (5) and step (6), it is stand-by.
Conductive ITO/glass substrate is cleaned and dried according to step (4).The PDMC aqueous solution filtered is used 3000 first
Rev/min rotating speed be spun on the ITO negative electrodes of above-mentioned dried and clean, and in heat drying 20 minutes at 100 DEG C, obtain 3 and receive
Meter Hou Du PDMC cathode interfaces layer.Then the PFN methanol solutions filtered are spun on 2000 revs/min of rotating speed above-mentioned
On PDMC cathode interfaces layer, and in heat drying 10 minutes at 100 DEG C, obtain the PFN cathode interfaces layer of 5 nano thickness.In ITO
On PDMC cathode interfaces layer and PFN cathode interfaces layer composition PDMC/PFN twin cathode boundary layers.Coated again by above-mentioned afterwards
The ITO of PDMC/PFN twin cathode boundary layers is transferred to anhydrous, anaerobic, in the special gloves case full of high pure nitrogen, by 10 milligrams
Every milliliter of PTB7 and PC71(mass ratio is 1 to BM:1.5) chlorobenzene mixed solution (contains the 1,8- diiodo-s that volume content is 3%
Octane additive) it is spun under 1500 revs/min or so of rotating speed on cathode interface layer, then in dry 10 points at 70 DEG C
Clock, obtains the photoactive layer of 80-90 rans.Finally, 3 × 10-4The molybdenum trioxide of 10 nanometers of vacuum evaporation successively under handkerchief
Anode is used as anode interface layer and 100 nanometers of aluminium.
Curve in Fig. 5 gives the device in 100mW/cm2Simulated solar light irradiation under current -voltage curve.
The open-circuit voltage of obtained device is 0.76 volt, and short circuit current flow is 17.18 milliamperes every square centimeter, and fill factor, curve factor is
69.0%, photoelectric transformation efficiency is 9.01%.With it is prepared in embodiment 5 be cathode interface based on water-soluble polymer PDMC
The battery of layer is compared, and open-circuit voltage improves 0.04 volt, and short circuit current flow is slightly increased, and fill factor, curve factor increases 7.3%, efficiency
Improve 16.7%；Compared with the battery based on alcohol soluble polymer PFN for cathode interface layer prepared in embodiment 6, open
Road voltage improves 0.01 volt, and short circuit current flow adds 5.9%, and fill factor, curve factor is substantially suitable, and efficiency improves 4.6%.
Foregoing PC71BM is English " methanofullerene [6,6]-phenyl C71-butyric acid
Methyl ester " are referred to as；PTB7 is document Adv.Mater.2010,22, the donor polymer material that E135. is reported.
Claims (4)
1. a kind of polymer solar cells based on double-decker cathode interface layer, include the polymerization of inverted structure or conventional structure
Cathode interface layer in thing solar cell, it is characterised in that：The cathode interface layer is by cathode interface layer 1 and cathode interface layer
The double-decker of 2 superposition compositions；The material of the cathode interface layer 1 is water-soluble polymer, the Water-soluble Polymer Molecules
Formula has following structure：
Wherein：
R1=H or CH3, R2=ONa or
Z- is halide ion, x=0-0.5, y=0.5-1, x+y=1, m=1-6, n=100-100000；The cathode interface layer
2 material is alcohol soluble polymer, the alcohol soluble polymer be molecular formula side chain with polar group, backbone units containing fluorenes or
The conjugated polymer of carbazole.
2. polymer solar cells according to claim 1, in addition to photoactive layer, it is characterised in that：Negative electrode circle
Surface layer 2 is adjacent with the photoactive layer, and the cathode interface layer 1 is adjacent with cathode interface layer 2.
3. polymer solar cells according to claim 1, in addition to photoactive layer, it is characterised in that：Negative electrode circle
Surface layer 1 is adjacent with the photoactive layer, and the cathode interface layer 2 is adjacent with cathode interface layer 1.
4. a kind of preparation method of the polymer solar cells based on double-decker cathode interface layer, methods described includes：
(1) water-soluble polymer with following structural formula is prepared：
Wherein：
R1=H or CH3, R2=ONa or
Z- is halide ion, x=0-0.5, y=0.5-1, x+y=1, m=1-6, n=100-100000；
(2) prepare molecular formula side chain and carry the alcohol soluble polymer of polar group, backbone units containing fluorenes or carbazole；
(3) with reference to existing process, the water-soluble polymer is spun on ITO negative electrodes and forms cathode interface layer 1, by the alcohol
Soluble polymer, which is spun on cathode interface layer 1, forms cathode interface layer 2, photoactive layer is prepared on cathode interface layer 2, in light
Anode interface layer and anode are prepared on active layer；Or using ITO as anode, photoactive layer, Zhi Hou are prepared on ito anode
Cathode interface layer 1 and cathode interface layer 2 are sequentially prepared on photoactive layer, then negative electrode is prepared on cathode interface layer 2.
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| CN103035844A (en) * | 2012-12-14 | 2013-04-10 | 华南理工大学 | Inversion organic bulk heterojunction solar battery and preparation method thereof |
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Application publication date: 20170919 |