CN110473968A - Flexible structure polymer solar battery and preparation method thereof based on europium rare-earth complex doping zinc-oxide electron-transport layer building - Google Patents
Flexible structure polymer solar battery and preparation method thereof based on europium rare-earth complex doping zinc-oxide electron-transport layer building Download PDFInfo
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- H10K30/10—Organic devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation comprising heterojunctions between organic semiconductors and inorganic semiconductors
- H10K30/15—Sensitised wide-bandgap semiconductor devices, e.g. dye-sensitised TiO2
- H10K30/152—Sensitised wide-bandgap semiconductor devices, e.g. dye-sensitised TiO2 the wide bandgap semiconductor comprising zinc oxide, e.g. ZnO
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Abstract
The present invention relates to polymer solar battery fields, particularly disclose a kind of flexible structure polymer solar battery and preparation method thereof based on europium rare-earth complex doping zinc-oxide electron-transport layer building.The polymer solar battery, it is characterised in that: be followed successively by flexible and transparent substrate, europium rare-earth complex doping zinc-oxide electron transfer layer, non-fullerene system photoactive layer, Hole-injecting Buffer Layer for Improvement and anode electrode with OMO electrode from bottom to top；Doped with europium rare-earth complex on zinc oxide electron transfer layer.Rationally, preparation method is simple for step design of the present invention, using the light transfer effect of europium rare-earth complex, improves non-fullerene system flexible battery device and improves photoelectric current in the light utilization efficiency of black light song, and then improves the incident photon-to-electron conversion efficiency of battery device.
Description
(1) technical field
The present invention relates to polymer solar battery fields, in particular to a kind of to be based on europium rare-earth complex doping zinc-oxide electronics
Transmit the flexible structure polymer solar battery and preparation method thereof of layer building.
(2) background technique
With the exhaustion of fossil energy and getting worse for environmental pollution, the reproducible energy of development and utilization cleaning is extremely urgent,
Wherein solar energy cleans, is renewable, being convenient for local use, is the emphasis of various countries' research.Solar battery is the development and utilization sun
Can core equipment, polymer solar battery compared to inorganic solar cell have light, manufacture craft it is simple, it is cheap,
The advantages that rollable, however the problems such as its current photoelectric conversion efficiency and stability, still limits its industrialized production.
To pursue high incident photon-to-electron conversion efficiency, currently, polymer solar battery is mostly in hard glass/indium tin oxide transparent
Constructed in substrate, although this obtains higher photoelectric conversion efficiency, with its pursued it is light, rollable the advantages that phase
It is contrary to.Thus, it is more meaningful that polymer solar battery is constructed in flexible and transparent substrate.By battery light active material light utilization efficiency
The influence of poor, light active material electronics, the more low factor of hole transport efficiency, the photo absorption performance of battery device are poor.How
In the case where not reducing electrons efficiency of transmission, the photo absorption performance for improving battery device is to improve flexible battery device light
The key of electrotransformation efficiency.
Rare-earth complex luminescent material is a kind of luminescent material with excellent luminance performance, can absorb the light of high-energy
Wave is converted into the light wave of visible region.According to the difference of selected rare earth element, change its emission wavelength, such as selects Eu element
The feux rouges of 610nm or so can be emitted；Selection Tb element can emit the blue light of 550nm or so.Ligand in rare-earth complex
Introducing can make it through " antenna " effect for the energy transfer absorbed to the centre of luminescence, and the addition of Ligands can be with
Significantly improve the luminescent properties of luminescent material.Rare-earth complex mainly absorbs the light wave of near ultraviolet attachment, rather than fullerene system
Light utilization efficiency of the light active material in this region is lower, thus can use the light transfer effect of rare-earth complex, improves electricity
The light utilization ratio of pond device improves the photoelectric current of device.
(3) summary of the invention
In order to compensate for the shortcomings of the prior art, the present invention provides a kind of reasonable in design, photoelectric conversion efficiency it is high based on
The flexible structure polymer solar battery and preparation method thereof of europium rare-earth complex doping zinc-oxide electron-transport layer building.
The present invention is achieved through the following technical solutions:
A kind of flexible structure polymer solar battery based on europium rare-earth complex doping zinc-oxide electron-transport layer building,
It is characterized in that: being followed successively by the flexible and transparent substrate with OMO electrode from bottom to top, europium rare-earth complex doping zinc-oxide electronics passes
Defeated layer, non-fullerene system photoactive layer, Hole-injecting Buffer Layer for Improvement and anode electrode；Doped with europium rare earth on zinc oxide electron transfer layer
Complex compound.
Europium rare-earth complex is doped in zinc oxide electron transfer layer by the present invention, is shifted using the light of europium rare-earth complex
Effect significantly improves the light utilization efficiency of the near ultraviolet region of flexible battery device, improves the photoelectric current of battery, is keeping higher
The colleague of fill factor finally obtains higher photoelectric conversion efficiency.
More excellent technical solution of the invention are as follows:
The flexible and transparent substrate is PET or PC film.
The OMO electrode is the three-decker electrode of sandwiched metal layer among two inorganic oxide layers；Wherein, the metal
Layer material is Au, Ag or Cu, with a thickness of 5-10nm；The material of oxide skin(coating) is metal oxide semiconductor；OMO structure electrode exists
While visible region keeps high light transmitance, higher charge transfer efficiency is kept.
In the europium rare-earth complex doping zinc-oxide electron transfer layer, europium rare-earth complex is doped to zinc-oxide nano
In granulosa, doping mass ratio is 2-7%, has rare-earth complex for disordered structure, under this concentration, the presence of europium rare-earth complex
It will not influence the electron-transport efficiency of zinc oxide electron transfer layer；Zinc oxide is graininess, partial size 4nm.By europium rare earth complex
Object, which is embedded into zinc oxide electron transfer layer to can effectively improve it and contact with light active material, occurs electrochemical action, and utilization is dilute
The luminous energy of near ultraviolet region light utilization efficiency difference is absorbed and utilized in the light transferance of native complex compound, is converted into visible light, improves battery
Extinction be newly more difficult, while the higher fill factor of retainer member, the final incident photon-to-electron conversion efficiency for improving battery device.
The non-fullerene system photoactive layer with a thickness of 100nm, wherein donor material be mid-gap polymer give
Body material J51 or J61, acceptor material are non-fullerene fused-ring derivatives ITIC or ITIC-m, donor material and acceptor material
Blending ratio is 1:1.
The material of the Hole-injecting Buffer Layer for Improvement is MoO3, with a thickness of 10nm；The material of anode electrode is Ag, with a thickness of 100nm.
The preparation method of above-mentioned flexible structure polymer solar battery, includes the following steps:
(1) OMO cathode electrode is sputtered in flexible and transparent substrate by magnetron sputtering method；
(2) on OMO cathode electrode one layer of europium doped rare-earth complex of direct spin coating burnett's solution, anneal at 60 DEG C
10min forms europium rare-earth complex doping zinc-oxide electron transfer layer；
(3) with the speed spin coating photoactive layer solution 60s of 1200-1400rpm in the glove box of nitrogen protection；
(4) in vacuum coating equipment, by the MoO of 10nm3It is deposited on photoactive layer respectively with the Ag anode of 100nm, true
Empty≤5 × 10-4Anode is formed under Pa.
Preferably, in step (2), the Zinc oxide nanoparticle made from the liquid phase reduction is distributed to after washing of precipitate
Volume ratio is the n-butanol of 60:35:5, in the mixed solution of methanol, chloroform, and the concentration of burnett's solution is 15mg/mL；Concentration
For the Eu (tta) of 0.9-1.5mg/ml3The suspension of phen ethyl alcohol is added in burnett's solution, and adjusting pH is 7, obtains concentration
For the europium rare-earth complex doping zinc-oxide solution of 10mg/mL, in OMO electrode surface with the revolving speed spin coating nano silver of 3000rpm
Piece doping zinc-oxide solution 30s, after annealing.
Preferably, in step (3), photoactive layer solution is the donor material that mass ratio is 1:1 and acceptor material in chlorobenzene
The polymer blend solution being mixed to get in solution, concentration 9-10mg/mL；It is also added in polymer blend solution
The 1,8- diiodo-octane of 1.5vol%.
Rationally, preparation method is simple for step design of the present invention, using the light transfer effect of europium rare-earth complex, improves non-lipid
It strangles alkene system flexible battery device and improves photoelectric current in the light utilization efficiency of black light song, and then improve the photoelectricity of battery device
Transformation efficiency.
(4) Detailed description of the invention
The present invention will be further described below with reference to the drawings.
Fig. 1 is the structural diagram of the present invention;
Fig. 2 is europium doped rare-earth complex and the polymer solar electricity undoped with europium rare-earth complex in the embodiment of the present invention 1
The photovoltaic property curve graph in pond.
In figure, 1 flexible and transparent substrate, 2 OMO electrodes, 3 europium rare-earth complex doping zinc-oxide electron transfer layers, 4 is non-lipid
Strangle alkene system photoactive layer, 5 Hole-injecting Buffer Layer for Improvement, 6 anode electrodes.
(5) specific embodiment
The present invention will be further explained below with reference to the attached drawings.
It is a kind of based on europium rare-earth complex doping zinc-oxide electron-transport layer building technical program of the present invention lies in providing
Flexible structure polymer solar battery, as shown in Fig. 1, battery structure include flexible and transparent substrate 1, and OMO electrode 2, europium is dilute
Native complex dopes zinc oxide electron transfer layer 3, non-fullerene system photoactive layer 4, Hole-injecting Buffer Layer for Improvement 5, anode electrode 6.
Flexible and transparent substrate 1 of the invention is flexible the polymeric substrates such as PET, PC, as flexible polymer solar
The substrate of battery, it is desirable that it has higher transmitance within the scope of near ultraviolet, visible light, near infrared region, can with blocking oxygen and
Water, and flatness is higher.
OMO electrode 2 of the invention is the cathode electrode of three-decker, and wherein oxide is ZnO, TiO2Equal semiconductor alloys
Oxide, metal layer Au, Ag, Cu etc., metal layer thickness are about 5-10nm, and OMO electrode 2 is kept in visible wavelength range
While high light transmitance, while keeping higher conductivity.
Europium rare-earth complex doping zinc-oxide electron transfer layer 3 of the invention is by Zinc oxide nanoparticle, europium rare earth complex
Object mixes.Wherein ZnO is graininess, and size is about 4nm, and europium rare-earth complex is amorphous, europium rare-earth complex
Doping mass percent is 2%-7%, and under this concentration, the presence of europium rare-earth complex will not influence the electricity of zinc oxide electron transfer layer
Sub- efficiency of transmission.Europium rare-earth complex is directly doped in Zinc oxide nanoparticle colloidal sol aaerosol solution by certain mass, is filled
Divide and is uniformly mixed.By spin coating method, one layer of europium rare-earth complex doping zinc-oxide electron transfer layer of spin coating on OMO electrode 2
3, low-temperature annealing removes solvent.
Non- fullerene system photoactive layer 4 of the invention by polymer donor material, non-fullerene acceptor material mixing and
At.Polymer donor material such as J51, J61 etc. have unsaturated structure in structure, band gap is moderate, with non-fullerene acceptor material
Expect that extinction is complementary, and energy match, visible light can be absorbed and generate exciton.Acceptor material be non-fullerene fused-ring derivatives such as
ITIC, ITIC-m etc. have energy level adjustable relative to fullerene acceptor material, and light absorption range is wide, is blended with donor material surely
The advantages that qualitative good, therefore can be with the higher more stable flexible polymer solar battery device of producing efficiency.
Hole-injecting Buffer Layer for Improvement 5 of the invention is MoO3, it is in vacuum evaporation equipment, forming a layer thickness by vapor deposition is about
The hole transmission layer of 10nm.
Anode electrode 6 of the invention is Ag, and good conductivity, work function is higher, high stability.
Embodiment 1:
Structure based on europium rare-earth complex doping zinc-oxide electron-transport layer building flexible structure polymer solar battery is such as
Shown in Fig. 1.1 is the transparent base flexibility PET in figure；2 cathode electrodes are OMO electrode, are made of ZnO/Ag/ZnO, thickness is respectively
40nm,10nm,60nm；Europium rare-earth complex in electron transfer layer 3 containing ZnO nano particle and 5wt%, ZnO size are about
4nm.In photoactive layer 4 donor material be J61, non-fullerene acceptor material be ITIC, photoactive layer with a thickness of 100nm；Electricity
Sub- buffer layer 5 is MoO3, with a thickness of 10nm；Anode electrode 6 is Ag, with a thickness of 100nm.
Its specifically the production method is as follows:
(1) the OMO cathode electrode in flexibility PET transparent substrates is obtained by magnetron sputtering method, and PET/OMO substrate is without cleaning, In
Direct one layer of electron transfer layer of spin coating on OMO electrode；
(2) ZnO nano particle is made by liquid phase reduction, after multiple washing of precipitate, redisperse to n-butanol, methanol, chlorine
In imitative mixed solution (volume ratio 60:35:5), oxidation zinc concentration is about 15mg/ml.It is added in 10ml zinc oxide suspension
The Eu (tta) that 5ml concentration is about 1.5mg/ml3The suspension of phen ethyl alcohol, control solution PH are 7 or so, are prevented big
Precipitating.Finally obtain the burnett's solution for the rare-earth complex doping that mass concentration is about 10mg/ml.It is revolved on OMO electrode molten
Liquid, revolving speed 3000rpm, time 30s, then 60 DEG C of annealing 10min form the zinc oxide electron-transport of nano silver slice doping
Layer.Substrate is transferred to the preparation that photoactive layer is carried out in the glove box of nitrogen protection；
(3) photoactive layer solution is made of J61, ITIC, and the mass ratio of J61 and ITIC in chlorobenzene solution is 1:1, polymer
Concentration is 10mgmL-1.In addition, 1, the 8- diiodo-octane (DIO) of 1.5vol% is added to light active material blend solution
In, to form the ideal interpenetrating networks with suitable donor and receptor size range in active layer, spin coating is with 1200-
1400rpm spin coating 60s；
(4) in vacuum coating equipment, by the MoO of 10nm3It is deposited on active layer respectively with the Ag anode of 100nm, in vacuum
≤5×10-4Anode is formed under Pa；
(5) incident photon-to-electron conversion efficiency of prepared flexible polymer solar battery is tested, corresponding I-V curve is as shown in Figure 2.
Fig. 2 corresponds to other 7.98% He of incident photon-to-electron conversion efficiency of europium doped rare-earth complex and the battery undoped with europium rare-earth complex
7.12%, after the doping of europium rare-earth complex, device efficiency is obviously improved, and is mainly reflected in current density by 16.87mAcm-1It mentions
It is raised to 18.45mAcm-1.Being obviously improved for current density proves that the doping of europium rare-earth complex can play the work of light transfer regulation
With i.e. absorption ultraviolet light converts visible light, to promote the incident photon-to-electron conversion efficiency of battery.
Embodiment 2:
Structure based on europium rare-earth complex doping zinc-oxide electron-transport layer building flexible structure polymer solar battery is such as
Shown in Fig. 1.1 is the transparent base flexibility PET in figure；2 cathode electrodes are OMO conductive electrode, are made of ZnO/Ag/ZnO, thickness point
It Wei not 60nm, 10nm, 60nm；Europium rare-earth complex in electron transfer layer 3 containing ZnO nano particle and 3wt%, ZnO size is about
For 4nm.In photoactive layer 4 donor material be J51, non-fullerene acceptor material be ITIC, photoactive layer with a thickness of 100nm；
Electron buffer layer 5 is MoO3, with a thickness of 10nm；Anode electrode 6 is Ag, with a thickness of 100nm.
Its specifically the production method is as follows:
(1) the OMO cathode electrode in flexibility PET transparent substrates is obtained by magnetron sputtering method, and PET/OMO substrate is without cleaning, In
Direct one layer of electron transfer layer of spin coating on OMO electrode；
(2) ZnO nano particle is made by liquid phase reduction, after multiple washing of precipitate, redisperse to n-butanol, methanol, chlorine
In imitative mixed solution (volume ratio 60:35:5), oxidation zinc concentration is about 15mg/ml.It is added in 10ml zinc oxide suspension
The Eu (tta) that 5ml concentration is about 0.9mg/ml3The suspension of phen ethyl alcohol, control solution PH are 7 or so, are prevented big
Precipitating.Finally obtain the burnett's solution for the rare-earth complex doping that mass concentration is about 10mg/ml.It is revolved on OMO electrode molten
Liquid, revolving speed 3000rpm, time 30s, then 60 DEG C of annealing 10min form the zinc oxide electronics of europium rare-earth complex doping
Transport layer.Substrate is transferred to the preparation that photoactive layer is carried out in the glove box of nitrogen protection；
(3) photoactive layer solution is made of J51, ITIC, and the mass ratio of J51 and ITIC in chlorobenzene solution is 1:1, polymer
Concentration is 9mgmL-1.In addition, 1, the 8- diiodo-octane (DIO) of 1.5vol% is added in light active material blend solution,
To form the ideal interpenetrating networks with suitable donor and receptor size range in active layer, spin coating is with 1200-
1400rpm spin coating 60s；
(4) in vacuum coating equipment, by the MoO of 10nm3It is deposited on active layer respectively with the Ag anode of 100nm, in vacuum
≤5×10-4Anode is formed under Pa；
(5) device efficiency after tested, after europium doped rare-earth complex, device current density is obviously improved, to promote whole electricity
Pond incident photon-to-electron conversion efficiency.
Claims (10)
1. a kind of flexible structure polymer solar battery based on europium rare-earth complex doping zinc-oxide electron-transport layer building,
It is characterized by: being followed successively by the flexible and transparent substrate (1) with OMO electrode (2), the doping oxidation of europium rare-earth complex from bottom to top
Zinc electron transfer layer (3), non-fullerene system photoactive layer (4), Hole-injecting Buffer Layer for Improvement (5) and anode electrode (6)；Zinc oxide electronics
Doped with europium rare-earth complex in transport layer (3).
2. the flexible structure according to claim 1 based on europium rare-earth complex doping zinc-oxide electron-transport layer building is poly-
Close object solar battery, it is characterised in that: the flexible and transparent substrate (1) is PET or PC film.
3. the flexible structure according to claim 1 based on europium rare-earth complex doping zinc-oxide electron-transport layer building is poly-
Close object solar battery, it is characterised in that: the OMO electrode (2) is three layers of sandwiched metal layer among two inorganic oxide layers
Structure electrode.
4. the flexible structure according to claim 1 based on europium rare-earth complex doping zinc-oxide electron-transport layer building is poly-
Close object solar battery, it is characterised in that: in the europium rare-earth complex doping zinc-oxide electron transfer layer (3), europium rare earth network
It closes object to be doped in Zinc oxide nanoparticle layer, doping mass ratio is 2-7%；Zinc oxide is graininess, partial size 4nm.
5. the flexible structure according to claim 1 based on europium rare-earth complex doping zinc-oxide electron-transport layer building is poly-
Close object solar battery, it is characterised in that: the non-fullerene system photoactive layer (4) with a thickness of 100nm, wherein donor
Material is mid-gap polymer donor material J51 or J61, and acceptor material is non-fullerene fused-ring derivatives ITIC or ITIC-
The blending ratio of m, donor material and acceptor material is 1:1.
6. the flexible structure according to claim 1 based on europium rare-earth complex doping zinc-oxide electron-transport layer building is poly-
Close object solar battery, it is characterised in that: the material of the Hole-injecting Buffer Layer for Improvement (5) is MoO3, with a thickness of 10nm；Anode electrode
(6) material is Ag, with a thickness of 100nm.
7. the flexible structure according to claim 3 based on europium rare-earth complex doping zinc-oxide electron-transport layer building is poly-
Close object solar battery, it is characterised in that: the metal layer material is Au, Ag or Cu, with a thickness of 5-10nm；The material of oxide skin(coating)
Material is metal oxide semiconductor.
8. the flexible structure according to claim 1 based on europium rare-earth complex doping zinc-oxide electron-transport layer building is poly-
The preparation method of object solar battery is closed, it is characterized in that, include the following steps: (1) by magnetron sputtering method in flexible and transparent base
OMO cathode electrode is sputtered on bottom；(2) zinc oxide of one layer of europium doped rare-earth complex of direct spin coating is molten on OMO cathode electrode
Liquid, anneal 10min at 60 DEG C, forms europium rare-earth complex doping zinc-oxide electron transfer layer；(3) in the gloves of nitrogen protection
With the speed spin coating photoactive layer solution 60s of 1200-1400rpm in case；(4) in vacuum coating equipment, by the MoO of 10nm3
It is deposited on photoactive layer respectively with the Ag anode of 100nm, in vacuum≤5 × 10-4Anode is formed under Pa.
9. preparation method according to claim 8, it is characterised in that: in step (2), through being aoxidized made from liquid phase reduction
Zinc nanoparticles are distributed in the mixed solution of n-butanol, methanol, chloroform that volume ratio is 60:35:5, oxygen after washing of precipitate
The concentration for changing zinc solution is 15mg/mL；Concentration is the Eu (tta) of 0.9-1.5mg/ml3The suspension of phen ethyl alcohol is added to oxygen
Change in zinc solution, adjusting pH is 7, the europium rare-earth complex doping zinc-oxide solution that concentration is 10mg/mL is obtained, in OMO electrode
Surface with the revolving speed spin coating nano silver slice doping zinc-oxide solution 30s of 3000rpm, after annealing.
10. preparation method according to claim 8, it is characterised in that: in step (3), photoactive layer solution is mass ratio
For the polymer blend solution that the donor material and acceptor material of 1:1 are mixed to get in chlorobenzene solution, concentration 9-10mg/
mL；The 1,8- diiodo-octane of 1.5vol% is also added in polymer blend solution.
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