CN103227287A - 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 PDFInfo
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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
Technical field
The invention belongs to the polymer solar battery technical field, be specifically related to a kind of three terminal parallel-connection structure polymer solar batteries that mix based on metal nanoparticle (NPs) and preparation method thereof.
Background technology
Polymer solar battery is because but advantages such as its material source is extensive, low-cost, flexible large-area preparation become the research topic of very attractive in recent years.Tradition transoid polymer solar battery structure is made of negative electrode, electron transfer layer, active layer, hole transmission layer and anode.But a kind of active layer can only absorb the sunlight of fixed wave length, can reduce the utilization ratio of light so greatly.Discover at present, in active layer metal nano particle-doped after, nano particle local surface phasmon enhancement effect has strengthened the light absorpting ability of active layer, has increased the generation of photoexciton in the device, thereby promoted device photoelectric stream, improved utilance for sunlight.
Summary of the invention
(so-called three terminal parallel connections promptly have three electrodes to the purpose of this invention is to provide a kind of three terminal parallel connections of mixing based on metal nanoparticle, adopt the parallel-connection structure of anode, twin cathode altogether) structure polymer solar cell and preparation method thereof, by two sub-batteries of active layer absorbing light scope complementation are formed parallel-connection structure, and it is metal nano particle-doped in the active layer of each sub-battery, utilize near the plasma enhancement effect of metal nanoparticle to improve the utilance of solar cell, thereby improve Solar cell performance for sunlight.
The polymer solar battery that the present invention is prepared 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 electron transfer layer and Al negative electrode, promptly 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 3~5nm, and the thickness of 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 electron transfer layer is 1~3nm, and the thickness of 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 that adopt among 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 400~600nm, and the absorption spectrum of PSBTBT is 600~800nm, and the absorption spectrum of these two kinds of materials can be realized complementary at visible region.And we adopt oneself synthetic Au, Ag nano particle and active layer material to carry out blend, realize that metal nanoparticle evenly distributes in active layer, and realize good being separated, the plasma resonance sink effect that guarantees nano particle can be had an effect at the each several part of active layer, guarantee that the active layer film forming is even, waviness is little, does not chap.Local surface phasmon enhancement effect around the nano particle has strengthened the light absorpting ability of active layer, has increased the generation of photoexciton in the device, thereby has promoted device photoelectric stream.
Synthesizing of Ag nano particle: the silver nitrate of 0.4~0.6g is dissolved in the deionized water of 15~25ml, and places the reactor of 100ml, successively put into the linoleic acid of 1~3ml, the enuatrol of 0.4~0.6g and the ethanol of 40~60ml in the reactor respectively again; Reaction temperature is 80~100 ℃, and the reaction time is 8~12h; After reaction finished, when being cooled to room temperature, collect silver in the bottom of reactor nanocrystalline; Then, with nanocrystalline ultrasonic being dispersed in the ethanol of silver, eccentric cleaning, 3~5 times repeatedly; At last, be dispersed in the toluene silver is nanocrystalline, obtain the toluene solution of Nano silver grain;
Au nano particle synthetic: in the 100mL beaker, add 20~40mg sodium citrate aqueous solution, be heated to 90~100 ℃, then with the HAuCl of 2~3ml, 0.16mg/ml
4Add in the above-mentioned solution, keep cooling off behind temperature and the constant volume 20~40min.
The three terminal parallel-connection structure polymer solar batteries that mix based on metal nanoparticle 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, clean the back and dry up, put into culture dish with nitrogen;
2) under the room temperature butyl titanate of 10~20ml (the sharp chemical plant of benefit, Beijing) 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; The acetylacetone,2,4-pentanedione (Tianjin chemical reagent factory) that adds 10~20ml then stirs 20~30min, the speed of 10~20ml deionized water with 2~4ml/min slowly is added drop-wise in the above-mentioned solution again, continues to stir 1~2h, obtains the flaxen TiO of homogeneous transparent
2Colloidal sol is placed ageing 6~8h; With the TiO after the ageing
2Colloidal sol is spin-coated on the ITO conductive glass surface that step 1) obtains and prepares TiO
2Film, spin speed are 3000~5000rpm; To have TiO then
2The ITO electro-conductive glass of film is put into Muffle furnace, roasting 2~3h under 450~600 ℃ of conditions, and powered-down can make TiO by the 10~12h that lowers the temperature naturally in the stove on the ITO electro-conductive glass subsequently
2Film, the thickness of film are 30~50nm;
3) under the room temperature condition, with the accurate Science and Technology Ltd. of donor material PSBTBT(Nichem) with acceptor material PC70BM(Nichem precision Science and Technology Ltd.) be dissolved in the polymer solvent dichloro-benzenes (Beijing lark prestige company) after mixing according to mass ratio 1:1, 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 under the mixing speed of 600~1000rpm, promptly can be configured to PSBTBT:PC
70The mixed solution of BM:NPs;
4) at TiO
2Spin coating PSBTBT:PC on the film
70BM:NPs mixed solution, rotating speed are 800~1200rpm; Then, sample is put into the glove box that is full of argon gas, on hot platform with 100~120 ℃ annealing 10~30min, thereby at TiO
2Make PSBTBT:PC on the film
70BM:NPs active layer, thickness are 200~300nm;
5) sample being taken out, is 1 * 10 at pressure
-4~5 * 10
-4Under the Pa condition, evaporation MoO on active layer
3(Chemical Reagent Co., Ltd., Sinopharm Group) hole transmission layer, thickness are 3~5nm, and the speed of growth is
6) be 8 * 10 at pressure
-4~1 * 10
-3Under the Pa condition, evaporation Ag(Chemical Reagent Co., Ltd., Sinopharm Group on hole transmission layer) electrode, thickness is 80~120nm, the speed of growth is
7) be 9 * 10 at pressure
-4~2 * 10
-3Under the Pa condition, evaporation WO on the Ag electrode
3(Chemical Reagent Co., Ltd., Sinopharm Group) hole transmission layer, thickness are 3~5nm, and the speed of growth is
8) under the room temperature condition, with the accurate Science and Technology Ltd. of donor material P3HT(Nichem) and acceptor material PC
70The accurate Science and Technology Ltd. of BM(Nichem) is dissolved in the polymer solvent dichloro-benzenes (Beijing lark prestige company) according to mass ratio 1:1, is configured to the solution of 15~20mg/mL, mix the solution that contains Au or Ag nano particle afterwards, P3HT:PC
70The mass ratio of BM:NPs is 1:1:0.02~0.05, stirs 24~48h under 600~1000rpm speed, promptly can be configured to P3HT:PC
70The mixed solution of BM:NPs;
9) sample is taken out, at WO
3Spin coating P3HT:PC on the hole transmission layer
70BM:NPs mixed solution, rotating speed are 800~1200rpm; Then, sample is put into the glove box that is full of argon gas, on hot platform with 140~160 ℃ annealing 10~30min, thereby at WO
3Make P3HT:PC on the hole transmission layer
70BM:NPs active layer, thickness are 200~300nm;
10) sample being taken out, is 1 * 10 at pressure
-4~5 * 10
-4Under the Pa condition, evaporation LiF(Chemical Reagent Co., Ltd., Sinopharm Group on active layer) electron transfer layer, thickness is 1~3nm, the speed of growth is
11) last, be 8 * 10 at pressure
-4~1 * 10
-3Under the Pa condition, evaporating Al on the LiF electron transfer layer (Chemical Reagent Co., Ltd., Sinopharm Group) electrode, thickness is 70~110nm, the speed of growth is
Thereby prepare three terminal parallel connections of mixing of the present invention (battery of this structure is exactly that Ag conduct in the middle of two element cells is total to anode, and ITO and Al are two negative electrodes) structure polymer solar cell based on metal nanoparticle.
Description of drawings
Fig. 1: the structural representation of polymer solar battery of the present invention;
Fig. 2: the photoelectric current curve of the polymer solar battery that mixes based on metal nanoparticle of the present invention preparation.
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 that Ag anode, 6 is WO
3Hole transmission layer, 7 is P3HT:PC
70BM:NPs active layer, 8 is that LiF electron transfer layer, 9 is the Al negative electrode.
As shown in Figure 2, at 100mw/cm
2Xenon lamp according to down having recorded the V-I characteristic curve, our use be Keithley, SMU2601 digital source table.Device is the polymer three terminals solar cell in parallel that mixes based on metal nanoparticle, and the structure of three terminals device in parallel is: glass/ITO/TiO
2/ PSBTBT:PC
70BM:NPs/MoO
3/ Ag/WO
3/ P3HT:PC
70BM:NPs/LiF/Al.We can clearly compare from figure, and the short circuit current of the solar cell that mixes based on metal nanoparticle of the present invention preparation is very high, has reached 15.26mA/cm
2, this mainly has benefited from parallel-connection structure, and the plasma resonance effect that causes of metal nanoparticle also helps the raising of photogenerated current in addition.As can be seen from the figure the device open circuit voltage has reached 0.86V, and fill factor, curve factor is 54.39% as calculated, and conversion efficiency has reached 6.67%, and these prove absolutely that the solar cell of this structure possesses good device performance.
Embodiment
Embodiment 1:
1) the ITO electro-conductive glass of cutting 15mm * 20mm puts it in the beaker, uses acetone, absolute ethyl alcohol, deionized water ultrasonic cleaning 20min respectively, cleans the back and dries up with nitrogen, puts into culture dish;
2) under 25 ℃ of the room temperatures with the Ti (OC of 10ml
4H
9)
4Be added drop-wise in the absolute ethyl alcohol of 90ml, drip the glacial acetic acid of 10ml again, magnetic agitation 40min obtains the yellow solution of homogeneous transparent; The acetylacetone,2,4-pentanedione that adds 10ml then stirs 30min, the speed of 10ml deionized water with 3ml/min slowly is added drop-wise in the above-mentioned solution again, continues to stir 1h, obtains the faint yellow colloidal sol of homogeneous transparent, places ageing 7h;
3) with the TiO that makes
2Colloidal sol is spin-coated on the ITO conductive glass surface and prepares TiO
2Film, spin speed are 4000rpm; To have TiO then
2The ITO electro-conductive glass of film is put into Muffle furnace, roasting 2h under 450 ℃ of conditions, and powered-down can make TiO by the 12h that lowers the temperature naturally in the stove on ITO subsequently
2Film, the thickness of film are 40nm;
4) silver nitrate with 0.5g is dissolved in the deionized water of 20ml, inserts then in the reactor of 100ml, and respectively with the linoleic acid of 2ml, the enuatrol of 0.5g and the ethanol of 50ml are successively put in the reactor then.Reaction temperature is set at 95 ℃, and the reaction time is 10h.After reaction finished, when being cooled to room temperature, can collect silver in the bottom of reactor nanocrystalline.Then, with nanocrystalline ultrasonic being dispersed in the ethanol of silver, eccentric cleaning, three times repeatedly.At last, be dispersed in the toluene silver is nanocrystalline, obtain the toluene solution of Nano silver grain.
5) add the 30mg sodium citrate aqueous solution in the 100mL beaker, it is heated to 95 ℃, then with 2ml, 0.16mg/ml HAuCl
4Add in the entry, keep cooling off behind temperature and the constant volume 30min, obtain the hydrosol of golden nanometer particle.
6) under the room temperature condition, with PSBTBT and PC
70BM is dissolved in the polymer solvent dichloro-benzenes according to mass ratio 1:1, is configured to the solution of 15mg/mL, mixes the solution that contains Au or Ag nano particle afterwards, PSBTBT:PC
70The mass ratio of BM:NPs active layer is 1:1:0.04, stirs 36h under the mixing speed of 800rpm, promptly can be configured to PSBTBT:PC
70The mixed solution of BM:NPs;
7) at TiO
2Spin coating PSBTBT:PC on the film
70BM:NPs mixed solution, rotating speed are 1000rpm; Then, sample is put into the glove box that is full of argon gas, on hot platform with 110 ℃ annealing 20min, thereby at TiO
2Make PSBTBT:PC on the film
70BM:Au(Ag) NPs active layer, thickness are 200nm;
8) sample being taken out, put into SD400B type multi-source temperature control polymer gas molecule in space depositing system, is 5 * 10 at pressure
-4Under the Pa, evaporation MoO on active layer
3Hole transmission layer, thickness are 4nm, and the speed of growth is
9) in SD400B type multi-source temperature control polymer gas molecule in space depositing system, be 9 * 10 at pressure
-4Under the Pa, evaporation Ag electrode on the molybdenum trioxide film, thickness is 100nm, the speed of growth is
10) in SD400B type multi-source temperature control polymer gas molecule in space depositing system, be 1 * 10 at pressure
-3Evaporation WO under the Pa
3Hole transmission layer, thickness are 4nm, and the speed of growth is
11) under the room temperature condition, with P3HT and PC
70BM is dissolved in the polymer solvent dichloro-benzenes according to mass ratio 1:1, is configured to the solution of 15mg/mL, mixes the solution that contains Au or Ag nano particle afterwards, P3HT:PC
70The mass ratio of BM:NPs active layer is 1:1:0.04, stirs 36h under the mixing speed of 1000rpm, promptly can be configured to P3HT:PC
70The mixed solution of BM:NPs;
12) sample is taken out, at WO
3Spin coating P3HT:PC on the film
70BM:NPs mixed solution, rotating speed are 1000rpm; Then, sample is put into the glove box that is full of argon gas, on hot platform with 150 ℃ annealing 20min, thereby at WO
3Make P3HT:PC on the film
70BM:NPs active layer, thickness are 200nm;
13) sample being taken out, put into SD400B type multi-source temperature control polymer gas molecule in space depositing system, is 5 * 10 at pressure
-4Under the Pa, evaporation LiF electron transfer layer on active layer, thickness is 1nm, the speed of growth is
14) last, in SD400B type multi-source temperature control polymer gas molecule in space depositing system, be 8 * 10 at pressure
-4Evaporating Al electrode under the Pa, thickness are 100nm, and the speed of growth is
15) with the preparation device at 100mw/cm
2Xenon lamp according to following test V-I characteristic curve, that we use is Keithley, SMU2601 digital source table, as calculated, the Isc of device is 15.26mA/cm
2, Voc is 0.86V, and FF is 54.39%, and PCE has reached 6.67%.
Claims (5)
1. three terminals polymer solar battery in parallel that mixes based on metal nanoparticle is characterized in that: from bottom to up, and successively by ITO electro-conductive glass, TiO as 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 electron transfer layer and Al negative electrode are formed, P3HT:PC
70The mass ratio of BM:NPs active layer is 1:1:0.02~0.05, and wherein NPs represents Au or Ag nano particle.
2. a kind of three terminals polymer solar battery in parallel that mixes based on metal nanoparticle as claimed in claim 1, it is characterized in that: 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 3~5nm, and the thickness of Ag anode is 80~120nm, and the thickness of LiF electron transfer layer is 1~3nm, and the thickness of Al negative electrode is 70~110nm.
3. the preparation method of the described three terminals polymer solar battery in parallel that mixes based on metal nanoparticle of a claim 1, its step is as follows:
1) the ITO electro-conductive glass is put into beaker, use acetone, absolute ethyl alcohol, deionized water ultrasonic cleaning 20~30min respectively, clean the back and dry up, put into culture dish with nitrogen;
2) under the room temperature butyl titanate of 10~20ml is added drop-wise in the absolute ethyl alcohol of 90~100ml, drips the glacial acetic acid of 10~20ml again, magnetic agitation 30~40min obtains the yellow solution of homogeneous transparent; The acetylacetone,2,4-pentanedione that adds 10~20ml then stirs 20~30min, the speed of 10~20ml deionized water with 2~4ml/min slowly is added drop-wise in the above-mentioned solution again, continues to stir 1~2h, obtains the flaxen TiO of homogeneous transparent
2Colloidal sol is placed ageing 6~8h; With the TiO after the ageing
2Colloidal sol is spin-coated on the ITO conductive glass surface that step 1) obtains and prepares TiO
2Film, spin speed are 3000~5000rpm; To have TiO then
2The ITO electro-conductive glass of film is put into Muffle furnace, roasting 2~3h under 450~600 ℃ of conditions, and powered-down can make TiO by the 10~12h that lowers the temperature naturally in the stove on the ITO electro-conductive glass subsequently
2Film, the thickness of film are 30~50nm;
3) under the room temperature condition, with donor material PSBTBT and acceptor material PC
70BM is dissolved in the 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 under the mixing speed of 600~1000rpm, promptly can be configured to PSBTBT:PC
70The mixed solution of BM:NPs;
4) at TiO
2Spin coating PSBTBT:PC on the film
70BM:NPs mixed solution, rotating speed are 800~1200rpm; Then, sample is put into the glove box that is full of argon gas, on hot platform with 100~120 ℃ annealing 10~30min, thereby at TiO
2Make PSBTBT:PC on the film
70BM:NPs active layer, thickness are 200~300nm;
5) sample being taken out, is 1 * 10 at pressure
-4~5 * 10
-4Under the Pa condition, evaporation MoO on active layer
3Hole transmission layer, thickness are 3~5nm, and the speed of growth is
6) be 8 * 10 at pressure
-4~1 * 10
-3Under the Pa condition, evaporation Ag electrode on hole transmission layer, thickness is 80~120nm, the speed of growth is
7) be 9 * 10 at pressure
-4~2 * 10
-3Under the Pa condition, evaporation WO on the Ag electrode
3Hole transmission layer, thickness are 3~5nm, and the speed of growth is
8) under the room temperature condition, with donor material P3HT and acceptor material PC
70BM is dissolved in the polymer solvent dichloro-benzenes according to mass ratio 1:1, is configured to the solution of 15~20mg/mL, mixes the solution that contains Au or Ag nano particle afterwards, P3HT:PC
70The mass ratio of BM:NPs is 1:1:0.02~0.05, stirs 24~48h under 600~1000rpm speed, promptly can be configured to P3HT:PC
70The mixed solution of BM:NPs;
9) sample is taken out, at WO
3Spin coating P3HT:PC on the hole transmission layer
70BM:NPs mixed solution, rotating speed are 800~1200rpm; Then, sample is put into the glove box that is full of argon gas, on hot platform with 140~160 ℃ annealing 10~30min, thereby at WO
3Make P3HT:PC on the hole transmission layer
70BM:NPs active layer, thickness are 200~300nm;
10) sample being taken out, is 1 * 10 at pressure
-4~5 * 10
-4Under the Pa condition, evaporation LiF electron transfer layer on active layer, thickness is 1~3nm, the speed of growth is
11) last, be 8 * 10 at pressure
-4~1 * 10
-3Under the Pa condition, evaporating Al electrode on the LiF electron transfer layer, thickness are 70~110nm, and the speed of growth is
Thereby prepare the three terminal parallel-connection structure polymer solar batteries that mix based on metal nanoparticle.
4. the preparation method of the three terminals polymer solar battery in parallel that mixes based on metal nanoparticle as claimed in claim 3, it is characterized in that: the synthetic of Ag nano particle is the deionized water that the silver nitrate of 0.4~0.6g is dissolved in 15~25ml, and place the reactor of 100ml, successively put into the linoleic acid of 1~3ml, the enuatrol of 0.4~0.6g and the ethanol of 40~60ml in the reactor respectively again; Reaction temperature is 80~100 ℃, and the reaction time is 8~12h; After reaction finished, when being cooled to room temperature, collect silver in the bottom of reactor nanocrystalline; Then, with nanocrystalline ultrasonic being dispersed in the ethanol of silver, eccentric cleaning, 3~5 times repeatedly; At last, be dispersed in the toluene silver is nanocrystalline, obtain the toluene solution of Nano silver grain.
5. the preparation method of the three terminals polymer solar battery in parallel that mixes based on metal nanoparticle as claimed in claim 3, it is characterized in that: the synthetic of Au nano particle is to add 20~40mg sodium citrate aqueous solution in the 100mL beaker, be heated to 90~100 ℃, then with the HAuCl of 2~3ml, 0.16mg/ml
4Add in the above-mentioned solution, keep cooling off behind temperature and the constant volume 20~40min.
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