CN103227287B - Three-terminal parallel polymer solar cell based on metal nanoparticle doping and preparation method of solar cell - Google Patents

Three-terminal parallel polymer solar cell based on metal nanoparticle doping and preparation method of solar cell Download PDF

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CN103227287B
CN103227287B CN201310140724.1A CN201310140724A CN103227287B CN 103227287 B CN103227287 B CN 103227287B CN 201310140724 A CN201310140724 A CN 201310140724A CN 103227287 B CN103227287 B CN 103227287B
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CN103227287A (en
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郭文滨
武健
阮圣平
沈亮
刘彩霞
董玮
张歆东
周敬然
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Jilin University
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    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
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Abstract

The invention discloses a three-terminal parallel polymer solar cell based on metal nanoparticle doping and a preparation method of the solar cell, and belongs to the technical field of polymer solar cells. The solar cell sequentially consists of ITO (Indium Tin Oxide) conductive glass serving as a substrate and a cathode, a TiO2 electronic transmission layer, a PSBTBT:PC70BM:NPs active layer, an MoO3 hole transmission layer, an Ag anode, a WO3 hole transmission layer, a P3HT:PC70BM:NPs active layer, an LiF electronic transmission layer and an Al cathode, wherein a mass ratio of the P3HT:PC70BM:NPs active layer is 1:1:(0.02-0.05), and NPs represents Au or Ag nanoparticles. According to the solar cell and the preparation method, two subcells form a parallel structure, light absorbing ranges of active layers of the subcells are complementary, metal nanoparticles are doped in the active layer of each subcell, and a utilization ratio of sunlight by the solar cell is increased by utilizing a plasma enhancement effect nearby the metal nanoparticles, so that the performance of the solar cell is improved.

Description

To adulterate three terminal parallel polymerization thing solar cells and preparation method thereof based on metal nanoparticle
Technical field
The invention belongs to polymer solar battery technical field, be specifically related to a kind of three terminal parallel-connection structure polymer solar batteries adulterated based on metal nanoparticle (NPs) and preparation method thereof.
Background technology
Polymer solar battery due to its material source extensively, low cost, flexibility, large area the research topic that advantage becomes very attractive in recent years such as can to prepare.Tradition transoid polymer solar battery structure is made up of negative electrode, electron transfer layer, active layer, hole transmission layer and anode.But active layer can only absorb a sunlight for fixed wave length, the utilization ratio of light greatly can be reduced like this.Current research finds, after metal nano particle-doped in active layer, nano particle local surface phasmon enhancement effect enhances the light absorpting ability of active layer, adds the generation of photoexciton in device, thus improve device photoelectric stream, improve the utilance for sunlight.
Summary of the invention
(namely so-called three terminal parallel connections have three electrodes to the object of this invention is to provide a kind of three terminal parallel connections based on metal nanoparticle doping, adopt the parallel-connection structure of common anode pole, twin cathode) structure polymer solar cell and preparation method thereof, by two sub-battery composition parallel-connection structures active layer being absorbed optical range complementation, and it is metal nano particle-doped in the active layer of every sub-battery, utilize the plasma enhancement effect near metal nanoparticle to improve the utilance of solar cell for sunlight, thus improve the performance of solar cell.
Polymer solar battery prepared by the present invention, from bottom to up, is followed successively by: as ITO electro-conductive glass, the TiO of substrate and negative electrode 2electron transfer layer, PSBTBT:PC 70bM:NPs active layer, MoO 3hole transmission layer, Ag anode, WO 3hole transmission layer, P3HT:PC 70bM:NPs active layer, LiF and Al negative electrode, namely structure is ITO/TiO 2/ PSBTBT:PC 70bM:NPs/MoO 3/ Ag/WO 3/ P3HT:PC 70bM:NPs/LiF/Al; Wherein NPs represents Au or Ag nano particle.
The thickness of ITO cathode layer is 50 ~ 100nm, TiO 2the thickness of electron transfer layer is 25 ~ 50nm, PSBTBT:PC 70the thickness of BM:NPs active layer is 200 ~ 300nm, MoO 3the thickness of hole transmission layer is the thickness of 3 ~ 5nm, Ag anode is 80 ~ 120nm, WO 3the thickness of hole transmission layer is 3 ~ 5nm, P3HT:PC 70the thickness of BM:NPs active layer is 200 ~ 300nm, and the thickness of LiF is the thickness of 1 ~ 3nm, Al negative electrode is 70 ~ 110nm.PSBTBT:PC 70the mass ratio of BM:NPs active layer is 1:1:0.02 ~ 0.05, P3HT:PC 70the mass ratio of BM:NPs active layer is 1:1:0.02 ~ 0.05.
The three terminal parallel-connection structure polymer solar batteries adopted in the present invention, selective polymer material system P3HT:PC 70bM and PSBTBT:PC 70bM is two active layers of stacking polymer battery, and the absorption spectrum of P3HT is the absorption spectrum of 400 ~ 600nm, PSBTBT is 600 ~ 800nm, and the absorption spectrum of this bi-material can realize complementary in visible region.And we adopt oneself synthesis Au, Ag nano particle and active layer material to carry out blended, realize metal nanoparticle to be uniformly distributed in active layer, and realize good being separated, ensure that the plasma resonance absorption effect of nano particle can be had an effect at each several part of active layer, ensure that active layer film forming is even, waviness is little, does not chap.Local surface phasmon enhancement effect around nano particle enhances the light absorpting ability of active layer, adds the generation of photoexciton in device, thus improves device photoelectric stream.
The synthesis of Ag nano particle: the deionized water silver nitrate of 0.4 ~ 0.6g being dissolved in 15 ~ 25ml, and the reactor being placed in 100ml, more respectively the ethanol of the linoleic acid of 1 ~ 3ml, the enuatrol of 0.4 ~ 0.6g and 40 ~ 60ml is successively put in reactor; Reaction temperature is 80 ~ 100 DEG C, and the reaction time is 8 ~ 12h; After reaction terminates, when being cooled to room temperature, brilliant to silver nanoparticle at the bottom collection of reactor; Then, by brilliant for silver nanoparticle ultrasonic disperse in ethanol, eccentric cleaning, 3 ~ 5 times repeatedly; Finally, silver nanoparticle crystalline substance is dispersed in toluene, obtains the toluene solution of Nano silver grain;
The synthesis of Au nano particle: add 20 ~ 40mg sodium citrate aqueous solution in 100mL beaker, is heated to 90 ~ 100 DEG C, then by the HAuCl of 2 ~ 3ml, 0.16mg/ml 4add in above-mentioned solution, keep temperature and cool after constant volume 20 ~ 40min.
The three terminal parallel-connection structure polymer solar batteries based on metal nanoparticle doping of the present invention, its step is as follows:
1) ITO electro-conductive glass (group of SHENZHEN NANBO) is put into beaker, use acetone, absolute ethyl alcohol, deionized water ultrasonic cleaning 20 ~ 30min respectively, dry up with nitrogen after cleaning, put into culture dish;
2) under room temperature, the butyl titanate (Yi Li chemical plant, Beijing) of 10 ~ 20ml is added drop-wise in the absolute ethyl alcohol (Beijing Chemical Plant) of 90 ~ 100ml, drip the glacial acetic acid (Beijing Chemical Plant) of 10 ~ 20ml again, magnetic agitation 30 ~ 40min, obtains the yellow solution of homogeneous transparent; Then add the acetylacetone,2,4-pentanedione (Tianjin chemical reagent factory) of 10 ~ 20ml, stir 20 ~ 30min, then 10 ~ 20ml deionized water is slowly added drop-wise in above-mentioned solution with the speed of 2 ~ 4ml/min, continue stirring 1 ~ 2h, obtain the flaxen TiO of homogeneous transparent 2colloidal sol, places ageing 6 ~ 8h; By the TiO after ageing 2colloidal sol is spin-coated on the ITO conductive glass surface that step 1) obtains and prepares TiO 2film, spin speed is 3000 ~ 5000rpm; Then will with TiO 2muffle furnace put into by the ITO electro-conductive glass of film, roasting 2 ~ 3h under 450 ~ 600 DEG C of conditions, and powered-down is by Temperature fall 10 ~ 12h in stove subsequently, can obtain TiO on ITO electro-conductive glass 2film, the thickness of film is 30 ~ 50nm;
3) under room temperature condition, by accurate for donor material PSBTBT(Nichem Science and Technology Ltd.) with acceptor material PC70BM(Nichem precision Science and Technology Ltd.) mix according to mass ratio 1:1 after be dissolved in polymer solvent dichloro-benzenes (Beijing lark prestige company), be configured to the solution of 15 ~ 20mg/mL, mix NPs(NPs afterwards and represent Au or Ag nano particle) solution, PSBTBT:PC 70the mass ratio of BM:NPs is 1:1:0.02 ~ 0.05, stirs 24 ~ 48h, namely can be configured to PSBTBT:PC under the mixing speed of 600 ~ 1000rpm 70the mixed solution of BM:NPs;
4) at TiO 2spin coating PSBTBT:PC on film 70bM:NPs mixed solution, rotating speed is 800 ~ 1200rpm; Then, sample is put into the glove box being full of argon gas, with 100 ~ 120 DEG C of annealing 10 ~ 30min in thermal station, thus at TiO 2obtained PSBTBT:PC on film 70bM:NPs active layer, thickness is 200 ~ 300nm;
5) being taken out by sample, is 1 × 10 at pressure -4~ 5 × 10 -4under Pa condition, evaporation MoO on active layer 3(Chemical Reagent Co., Ltd., Sinopharm Group) hole transmission layer, thickness is 3 ~ 5nm, and the speed of growth is
6) be 8 × 10 at pressure -4~ 1 × 10 -3under Pa condition, evaporation Ag(Chemical Reagent Co., Ltd., Sinopharm Group on hole transmission layer) electrode, thickness is 80 ~ 120nm, and the speed of growth is
7) be 9 × 10 at pressure -4~ 2 × 10 -3under Pa condition, evaporation WO on Ag electrode 3(Chemical Reagent Co., Ltd., Sinopharm Group) hole transmission layer, thickness is 3 ~ 5nm, and the speed of growth is
8) under room temperature condition, by accurate for donor material P3HT(Nichem Science and Technology Ltd.) and acceptor material PC 70the accurate Science and Technology Ltd. of BM(Nichem) be dissolved in polymer solvent dichloro-benzenes (Beijing lark prestige company) according to mass ratio 1:1, be configured to the solution of 15 ~ 20mg/mL, mix the solution containing Au or Ag nano particle afterwards, P3HT:PC 70the mass ratio of BM:NPs is 1:1:0.02 ~ 0.05, stirs 24 ~ 48h, namely can be configured to P3HT:PC under 600 ~ 1000rpm speed 70the mixed solution of BM:NPs;
9) sample is taken out, at WO 3spin coating P3HT:PC on hole transmission layer 70bM:NPs mixed solution, rotating speed is 800 ~ 1200rpm; Then, sample is put into the glove box being full of argon gas, with 140 ~ 160 DEG C of annealing 10 ~ 30min in thermal station, thus at WO 3obtained P3HT:PC on hole transmission layer 70bM:NPs active layer, thickness is 200 ~ 300nm;
10) being taken out by sample, is 1 × 10 at pressure -4~ 5 × 10 -4under Pa condition, evaporation LiF(Chemical Reagent Co., Ltd., Sinopharm Group on active layer) electron transfer layer, thickness is 1 ~ 3nm, and the speed of growth is
11) last, be 8 × 10 at pressure -4~ 1 × 10 -3under Pa condition, evaporating Al (Chemical Reagent Co., Ltd., Sinopharm Group) electrode in LiF, thickness is 70 ~ 110nm, and the speed of growth is thus prepare the three terminal parallel connections based on metal nanoparticle doping of the present invention (battery of this structure be exactly Ag in the centre of two element cells as common anode pole, ITO and Al is two negative electrodes) structure polymer solar cell.
Accompanying drawing explanation
Fig. 1: the structural representation of polymer solar battery of the present invention;
Fig. 2: the photocurrent curve of the polymer solar battery based on metal nanoparticle doping prepared by the present invention.
As shown in Figure 1,1 is ITO Conducting Glass negative electrode, and 2 is TiO 2electron transfer layer, 3 is PSBTBT:PC 70bM:NPs active layer, 4 is MoO 3hole transmission layer, 5 is Ag anode, 6 is WO 3hole transmission layer, 7 is P3HT:PC 70bM:NPs active layer, 8 is LiF, 9 is Al negative electrode.
As shown in Figure 2, at 100mw/cm 2xenon light shining under recorded V-I characteristic curve, we use Keithley, SMU2601 digital sourcemeter.Device is the polymer three terminal solar cell in parallel based on metal nanoparticle doping, and the structure of three terminal devices in parallel is: glass/ITO/TiO 2/ PSBTBT:PC 70bM:NPs/MoO 3/ Ag/WO 3/ P3HT:PC 70bM:NPs/LiF/Al.From figure, we can clearly compare, and the short circuit current of the solar cell based on metal nanoparticle doping prepared by the present invention is very high, reaches 15.26mA/cm 2, this mainly has benefited from parallel-connection structure, and the plasma resonance effect that metal nanoparticle causes in addition also contributes to the raising of photogenerated current.As can be seen from the figure device open circuit voltage reaches 0.86V, and fill factor, curve factor is 54.39% as calculated, and conversion efficiency reaches 6.67%, and these absolutely prove that the solar cell of this structure possesses good device performance.
Embodiment
Embodiment 1:
1) cut the ITO electro-conductive glass of 15mm × 20mm, put it in beaker, use acetone, absolute ethyl alcohol, deionized water ultrasonic cleaning 20min respectively, dry up with nitrogen after cleaning, put into culture dish;
2) at room temperature 25 DEG C by the Ti (OC of 10ml 4h 9) 4be added drop-wise in the absolute ethyl alcohol of 90ml, then drip the glacial acetic acid of 10ml, magnetic agitation 40min, obtain the yellow solution of homogeneous transparent; Then add the acetylacetone,2,4-pentanedione of 10ml, stir 30min, then 10ml deionized water is slowly added drop-wise in above-mentioned solution with the speed of 3ml/min, continue to stir 1h, obtain the faint yellow colloidal sol of homogeneous transparent, place ageing 7h;
3) by obtained TiO 2colloidal sol is spin-coated on ITO conductive glass surface and prepares TiO 2film, spin speed is 4000rpm; Then will with TiO 2muffle furnace put into by the ITO electro-conductive glass of film, roasting 2h under 450 DEG C of conditions, and powered-down is by Temperature fall 12h in stove subsequently, can obtain TiO on ITO 2film, the thickness of film is 40nm;
4) be dissolved in the deionized water of 20ml by the silver nitrate of 0.5g, then insert in the reactor of 100ml, then respectively by the linoleic acid of 2ml, the enuatrol of 0.5g and the ethanol of 50ml are successively put in reactor.Reaction temperature is set as 95 DEG C, and the reaction time is 10h.After reaction terminates, when being cooled to room temperature, silver nanoparticle crystalline substance can be collected in the bottom of reactor.Then, by brilliant for silver nanoparticle ultrasonic disperse in ethanol, eccentric cleaning, three times repeatedly.Finally, silver nanoparticle crystalline substance is dispersed in toluene, obtains the toluene solution of Nano silver grain.
5) in 100mL beaker, add 30mg sodium citrate aqueous solution, it is heated to 95 DEG C, then by 2ml, 0.16mg/ml HAuCl 4be added to the water, keep temperature and cool after constant volume 30min, obtaining the hydrosol of golden nanometer particle.
6) under room temperature condition, by PSBTBT and PC 70bM is dissolved in polymer solvent dichloro-benzenes according to mass ratio 1:1, is configured to the solution of 15mg/mL, mixes the solution containing Au or Ag nano particle afterwards, PSBTBT:PC 70the mass ratio of BM:NPs active layer is 1:1:0.04, stirs 36h, namely can be configured to PSBTBT:PC under the mixing speed of 800rpm 70the mixed solution of BM:NPs;
7) at TiO 2spin coating PSBTBT:PC on film 70bM:NPs mixed solution, rotating speed is 1000rpm; Then, sample is put into the glove box being full of argon gas, with 110 DEG C of annealing 20min in thermal station, thus at TiO 2obtained PSBTBT:PC on film 70bM:Au(Ag) NPs active layer, thickness is 200nm;
8) taken out by sample, putting into SD400B type multi-source temperature control Polymer Gas phase molecule depositing system, is 5 × 10 at pressure -4under Pa, evaporation MoO on active layer 3hole transmission layer, thickness is 4nm, and the speed of growth is
9) in SD400B type multi-source temperature control Polymer Gas phase molecule depositing system, be 9 × 10 at pressure -4under Pa, evaporation Ag electrode on Molybdenum Oxide Thin Films by Sol-Gel, thickness is 100nm, and the speed of growth is
10) in SD400B type multi-source temperature control Polymer Gas phase molecule depositing system, be 1 × 10 at pressure -3evaporation WO under Pa 3hole transmission layer, thickness is 4nm, and the speed of growth is
11) under room temperature condition, by P3HT and PC 70bM is dissolved in polymer solvent dichloro-benzenes according to mass ratio 1:1, is configured to the solution of 15mg/mL, mixes the solution containing Au or Ag nano particle afterwards, P3HT:PC 70the mass ratio of BM:NPs active layer is 1:1:0.04, stirs 36h, namely can be configured to P3HT:PC under the mixing speed of 1000rpm 70the mixed solution of BM:NPs;
12) sample is taken out, at WO 3spin coating P3HT:PC on film 70bM:NPs mixed solution, rotating speed is 1000rpm; Then, sample is put into the glove box being full of argon gas, with 150 DEG C of annealing 20min in thermal station, thus at WO 3obtained P3HT:PC on film 70bM:NPs active layer, thickness is 200nm;
13) taken out by sample, putting into SD400B type multi-source temperature control Polymer Gas phase molecule depositing system, is 5 × 10 at pressure -4under Pa, evaporation LiF on active layer, thickness is 1nm, and the speed of growth is
14) last, in SD400B type multi-source temperature control Polymer Gas phase molecule depositing system, be 8 × 10 at pressure -4evaporating Al electrode under Pa, thickness is 100nm, and the speed of growth is
15) by preparation device at 100mw/cm 2xenon light shining under test V-I characteristic curve, we use Keithley, SMU2601 digital sourcemeter, and as calculated, the Isc of device is 15.26mA/cm 2, Voc is 0.86V, FF is that 54.39%, PCE reaches 6.67%.

Claims (3)

1., based on a preparation method for three terminal parallel polymerization thing solar cells of metal nanoparticle doping, its step is as follows:
1) ITO electro-conductive glass is put into beaker, use acetone, absolute ethyl alcohol, deionized water ultrasonic cleaning 20 ~ 30min respectively, dry up with nitrogen after cleaning, put into culture dish;
2) under room temperature, the butyl titanate of 10 ~ 20mL is added drop-wise in the absolute ethyl alcohol of 90 ~ 100mL, then drips the glacial acetic acid of 10 ~ 20mL, magnetic agitation 30 ~ 40min, obtain the yellow solution of homogeneous transparent; Then add the acetylacetone,2,4-pentanedione of 10 ~ 20mL, stir 20 ~ 30min, then 10 ~ 20mL deionized water is slowly added drop-wise in above-mentioned solution with the speed of 2 ~ 4mL/min, continue stirring 1 ~ 2h, obtain the flaxen TiO of homogeneous transparent 2colloidal sol, places ageing 6 ~ 8h; By the TiO after ageing 2colloidal sol is spin-coated on step 1) the ITO conductive glass surface that obtains prepares TiO 2film, spin speed is 3000 ~ 5000rpm; Then will with TiO 2muffle furnace put into by the ITO electro-conductive glass of film, roasting 2 ~ 3h under 450 ~ 600 DEG C of conditions, and powered-down is by Temperature fall 10 ~ 12h in stove subsequently, can obtain TiO on ITO electro-conductive glass 2film, the thickness of film is 30 ~ 50nm;
3) under room temperature condition, by donor material PSBTBT and acceptor material PC 70bM is dissolved in polymer solvent dichloro-benzenes after mixing according to mass ratio 1:1, is configured to the solution of 15 ~ 20mg/mL, mixes the solution of NPs afterwards, PSBTBT:PC 70the mass ratio of BM:NPs is 1:1:0.02 ~ 0.05, stirs 24 ~ 48h, namely can be configured to PSBTBT:PC under the mixing speed of 600 ~ 1000rpm 70the mixed solution of BM:NPs, wherein NPs represents Au or Ag nano particle;
4) at TiO 2spin coating PSBTBT:PC on film 70bM:NPs mixed solution, rotating speed is 800 ~ 1200rpm; Then, sample is put into the glove box being full of argon gas, with 100 ~ 120 DEG C of annealing 10 ~ 30min in thermal station, thus at TiO 2obtained PSBTBT:PC on film 70bM:NPs active layer, thickness is 200 ~ 300nm;
5) being taken out by sample, is 1 × 10 at pressure -4~ 5 × 10 -4under Pa condition, evaporation MoO on active layer 3hole transmission layer, thickness is 3 ~ 5nm, and the speed of growth is
6) be 8 × 10 at pressure -4~ 1 × 10 -3under Pa condition, evaporation Ag electrode on hole transmission layer, thickness is 80 ~ 120nm, and the speed of growth is
7) be 9 × 10 at pressure -4~ 2 × 10 -3under Pa condition, evaporation WO on Ag electrode 3hole transmission layer, thickness is 3 ~ 5nm, and the speed of growth is
8) under room temperature condition, by donor material P3HT and acceptor material PC 70bM is dissolved in polymer solvent dichloro-benzenes according to mass ratio 1:1, is configured to the solution of 15 ~ 20mg/mL, mixes the solution containing Au or Ag nano particle afterwards, P3HT:PC 70the mass ratio of BM:NPs is 1:1:0.02 ~ 0.05, stirs 24 ~ 48h, namely can be configured to P3HT:PC under 600 ~ 1000rpm speed 70the mixed solution of BM:NPs;
9) sample is taken out, at WO 3spin coating P3HT:PC on hole transmission layer 70bM:NPs mixed solution, rotating speed is 800 ~ 1200rpm; Then, sample is put into the glove box being full of argon gas, with 140 ~ 160 DEG C of annealing 10 ~ 30min in thermal station, thus at WO 3obtained P3HT:PC on hole transmission layer 70bM:NPs active layer, thickness is 200 ~ 300nm;
10) being taken out by sample, is 1 × 10 at pressure -4~ 5 × 10 -4under Pa condition, evaporation LiF on active layer, thickness is 1 ~ 3nm, and the speed of growth is
11) last, be 8 × 10 at pressure -4~ 1 × 10 -3under Pa condition, evaporating Al electrode in LiF, thickness is 70 ~ 110nm, and the speed of growth is thus the three terminal parallel-connection structure polymer solar batteries prepared based on metal nanoparticle doping.
2. a kind of preparation method of three terminal parallel polymerization thing solar cells based on metal nanoparticle doping as claimed in claim 1, it is characterized in that: the synthesis of Ag nano-particle solution is the deionized water silver nitrate of 0.4 ~ 0.6g being dissolved in 15 ~ 25mL, and be placed in the reactor of 100mL, more respectively the ethanol of the linoleic acid of 1 ~ 3mL, the enuatrol of 0.4 ~ 0.6g and 40 ~ 60mL is successively put in reactor; Reaction temperature is 80 ~ 100 DEG C, and the reaction time is 8 ~ 12h; After reaction terminates, when being cooled to room temperature, brilliant to silver nanoparticle at the bottom collection of reactor; Then, by brilliant for silver nanoparticle ultrasonic disperse in ethanol, eccentric cleaning, 3 ~ 5 times repeatedly; Finally, silver nanoparticle crystalline substance is dispersed in toluene, obtains the toluene solution of Nano silver grain.
3. a kind of preparation method of three terminal parallel polymerization thing solar cells based on metal nanoparticle doping as claimed in claim 1, it is characterized in that: the synthesis of Au nano-particle solution adds 20 ~ 40mg sodium citrate aqueous solution in 100mL beaker, be heated to 90 ~ 100 DEG C, then by the HAuCl of 2 ~ 3mL, 0.16mg/mL 4add in above-mentioned solution, keep temperature and cool after constant volume 20 ~ 40min.
CN201310140724.1A 2013-04-23 2013-04-23 Three-terminal parallel polymer solar cell based on metal nanoparticle doping and preparation method of solar cell Expired - Fee Related CN103227287B (en)

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