CN107170891A - A kind of wide spectrum perovskite solar cell and preparation method thereof - Google Patents
A kind of wide spectrum perovskite solar cell and preparation method thereof Download PDFInfo
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- CN107170891A CN107170891A CN201710373892.3A CN201710373892A CN107170891A CN 107170891 A CN107170891 A CN 107170891A CN 201710373892 A CN201710373892 A CN 201710373892A CN 107170891 A CN107170891 A CN 107170891A
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- H—ELECTRICITY
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- H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
- H10K30/00—Organic devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation
- 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
- H10K30/151—Sensitised wide-bandgap semiconductor devices, e.g. dye-sensitised TiO2 the wide bandgap semiconductor comprising titanium oxide, e.g. TiO2
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- B—PERFORMING OPERATIONS; TRANSPORTING
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- B82Y20/00—Nanooptics, e.g. quantum optics or photonic crystals
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- B—PERFORMING OPERATIONS; TRANSPORTING
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- Y02E10/00—Energy generation through renewable energy sources
- Y02E10/50—Photovoltaic [PV] energy
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Abstract
The present invention provides a kind of wide spectrum perovskite solar cell and preparation method thereof, and the wide spectrum perovskite solar cell includes FTO glass substrates, the TiO being cascading2Compacted zone, TiO2Porous luminescent layer, perovskite light-absorption layer, hole transmission layer and metal electrode, the TiO2Contain Doped ions in porous luminescent layer, the Doped ions include Yb3+With other ions, other described ions include Ho3+、Er3+、Mn2+、Tm3+At least one of.Wide spectrum perovskite solar cell that the present invention is provided and preparation method thereof, can effectively widen the absorption spectrum of perovskite solar cell, improve perovskite solar cell photoelectric stream and conversion efficiency.
Description
Technical field
The invention belongs to perovskite technical field of solar batteries, more particularly to a kind of wide spectrum perovskite solar cell
And preparation method thereof.
Background technology
Solar cell cleans the reproducible energy as one kind and just received more and more attention, for solving energy danger
Machine has great importance.Therefore, exploitation novel efficient low-cost solar battery causes the interest of various countries researcher.Calcium titanium
Ore deposit structure solar cell is a kind of solar cell using perovskite structure as light absorbent, and its energy gap is about 1.5eV, is disappeared
Backscatter extinction logarithmic ratio is high, and the film of hundreds of nanometer thickness can fully absorb below 800nm sunshine.Perovskite solar cell has into
This cheap, preparation technology is simple, photoelectric transformation efficiency is high, and the development advanced by leaps and bounds was obtained in recent years, receives people's
Extensive concern.
Mainly there is TiO currently used for the orifice layer material of perovskite solar energy anode2, ZnO and Al2O3Deng porous layer master
Play the skeleton function of battery.The absorption spectrum of perovskite material concentrates on visible ray, for infrared more than its optical band gap
Light and ultraviolet light less than 400nm will not absorb, thus the Shortcomings in terms of light conversion efficiency, photoelectric current.
The A of Publication No. CN 105514279 Chinese patent application, discloses a kind of honeycomb sandwich Ca-Ti ore type sun
Energy battery and preparation method thereof, the Ca-Ti ore type solar cell includes the substrate stacked gradually, compacted zone, porous layer, extinction
Layer, hole transmission layer and metal electrode layer.The patent application is by using NaYF4For the up-conversion and TiO of matrix2Nanometer
The mixture of particle mixes to prepare porous layer.Although this solar cell also can absorb near infrared light and sends visible ray,
It is it due to adding NaYF4, fluoride stability is not as TiO2, charge transport ability is not as TiO2, it may be influenceed conductive
Property.
The content of the invention
There is provided a kind of wide spectrum perovskite solar cell and its system to make up the deficiencies in the prior art by the present invention
Preparation Method, can effectively widen the absorption spectrum of perovskite solar cell, improve perovskite solar cell photoelectric stream and conversion
Efficiency.
The present invention is reaches its purpose, and the technical scheme of use is as follows：
A kind of wide spectrum perovskite solar cell, including be cascading FTO glass substrates, TiO2Compacted zone,
TiO2Porous luminescent layer, perovskite light-absorption layer, hole transmission layer and metal electrode, the TiO2Contain doping in porous luminescent layer
Ion, the Doped ions include Yb3+With other ions, other described ions include Ho3+、Er3+、Mn2+、Tm3+In at least
It is a kind of.
It is preferred that, the TiO2In porous luminescent layer, Yb3+Mol ratio with other ions is 3~20：1, preferably 5：1,
The perovskite solar battery lighting performance that preferred scheme is obtained preferably, can effectively widen the absorption light of perovskite solar cell
Spectrum.
It is preferred that, in TiO2In porous luminescent layer, the molar percentage that the Doped ions account for Ti cases is 1-10%,
That is, the mol ratio of described Doped ions and Ti is 1:99~10:90.Mol ratio of the Doped ions in Ti cases is controlled excellent
Scope is selected, the perovskite solar battery lighting performance of acquisition preferably, effectively improves perovskite solar cell photoelectric stream and turned
Change efficiency.
It is used as a kind of preferred scheme, the Yb3+With other ions from the hydration containing these ions or non-hydrated nitric acid
Salt.Using nitrate, easily dissolving, and cost is low,
It is preferred that, the TiO2Porous luminescent layer is made according to the method comprised the following steps：By holmium nitrate, erbium nitrate,
The aqueous solution and the ytterbium nitrate aqueous solution of at least one of thulium nitrate, manganese nitrate are added dropwise in metatitanic acid ester solution, thermally treated, are obtained
The TiO of doping2Precipitation；Through drying, grind, calcine, cool down the TiO that must be adulterated2Powder, by the TiO of the doping of gained2Powder system
Carry out being thermally treated resulting in the porous luminescent layers of TiO2 for into colloid, being spun on after TiO2 compacted zones.
It is more highly preferred to, the porous luminescent layers of TiO2 are made according to the method comprised the following steps：By butyl titanate
It is added dropwise under agitation in deionized water, 15~45min is stirred in 60~75 DEG C of constant temperature, then by holmium nitrate, erbium nitrate, nitric acid
The aqueous solution and the ytterbium nitrate aqueous solution of at least one of thulium, manganese nitrate are added dropwise in solution of tetrabutyl titanate, 170~185
15~25h is heat-treated at DEG C, the TiO of doping is obtained2Precipitation；Calcined through drying, grinding, 700~850 DEG C, cool down the TiO that must be adulterated2
Powder, by the TiO of the doping of gained2Powder is added in polyethylene glycol, is prepared into colloid, colloid is spun on into TiO2After compacted zone
Progress is thermally treated resulting in TiO2Porous luminescent layer
It is preferred that, the polyethylene glycol is PEG 20000.
It is further preferred that characterized in that, the TiO2The thickness of porous luminescent layer is 50~500nm, and aperture is 5-
80nm；The TiO2The thickness of compacted zone is 40-80nm, and the thickness of the perovskite light-absorption layer is 200-800nm, the hole
The thickness of transport layer is 40-120nm, and the thickness of the metal electrode is 50-100nm.The thickness of each layer is selected in above-mentioned model
Enclose, can reach preferably properties of product.
It is further preferred that characterized in that, the square resistance of the FTO glass substrates is 5~20 Ω, transmitance is 75
~90%；The chemical composition of the perovskite light-absorption layer is CH3NH3PbI3；The hole transmission layer is spiro-MeOTAD；Institute
Metal electrode is stated for Au or Ag dorsum electrode layers.
Second aspect of the present invention provides the preparation method of wide spectrum perovskite solar cell described above, including as walked
Suddenly：
(1) cleaning FTO glass substrates, dry for standby；
(2) TiO is prepared in the conducting surface of FTO glass substrates2Compacted zone；
(3) in TiO2Fine and close layer surface prepares TiO2Porous luminescent layer；
(4) perovskite light-absorption layer is prepared：By perovskite presoma PbI2DMF solution be spun on TiO2On porous luminescent layer
Film is formed, 20~40min is heat-treated in 90~105 DEG C, is cooled to after room temperature, by CH3NH3I aqueous isopropanol is added drop-wise to thin
Film surface, spin coating obtains brown film, and 20~40min is heat-treated after 70~85 DEG C, then through 100~120 DEG C of heat treatments 5~
20min, obtains perovskite light-absorption layer.
(5) hole transmission layer is prepared：4- tert .-butylpyridines, two (trimethyl fluoride sulfonyl) imine lithiums are dissolved in spiro-
In OMeTAD chlorobenzene solution, it is spun on perovskite light-absorption layer；
(6) metal electrode is prepared on perovskite light-absorption layer.
The technical scheme that the present invention is provided has the advantages that：
By the present invention in that with doping TiO2Porous luminescent layer, utilizes the TiO with the characteristics of luminescence2Nano particle is made
Standby porous layer, while the Yb that adulterates3+And Ho3+、Er3+、Mn2+、Tm3+At least one of ion, be used as electron transfer layer and light to turn
Layer is changed, the infrared light and ultraviolet light that can not be absorbed by perovskite material can be effectively absorbed, be converted into visible ray, so that by calcium titanium
Pit wood material is absorbed, and improves the photoelectric current and conversion efficiency of battery.
Brief description of the drawings
Fig. 1 is Ho3+/Yb3+The TiO being co-doped with2Porous layer up-conversion luminescence figure；
Fig. 2 is the J-V performance curves of the battery of embodiment 1；
Fig. 3 is the J-V performance curves of the battery of embodiment 2；
Fig. 4 is the J-V performance curves of the battery of embodiment 3.
Embodiment
Technical scheme is described further below in conjunction with the accompanying drawings：
Experimental method used in following embodiments unless otherwise specified, be those skilled in the art grasped it is normal
Rule method, is repeated no more.
Embodiment 1
A kind of wide spectrum perovskite solar cell, is prepared as follows：
(1) cleaning of electro-conductive glass
FTO glass is cleaned into surface with liquid detergent, rinsed repeatedly with deionized water.With acetone and alcohol, ultrasound is clear respectively again
20min is washed, cleaned FTO is put into standby after vacuum drying chamber drying.
(2) TiO is prepared2Compacted zone
Prepare TiO2Compacted zone spin coating liquid：Take 25 μ l 2mol/L HCl solutions to add in 1.81m1 anhydrous isopropyl alcohols, shake
It is even, it is used as solution A；Take 264 μ l metatitanic acids isopropanols to add in 1.81ml anhydrous isopropyl alcohols, shake up, be used as solution B；In solution B
The magnetic stir bar of wash clean is put into, and is placed on high-speed stirred on magnetic stirrer, solution A is added dropwise just in high-speed stirred
In solution B, then filter.Solution carries out spin coating after preparing, and the FTO electro-conductive glass cleaned up is placed on glue evenning table, led
Electric that appropriate solution is dripped on its surface up, with low speed 500rpm/min, 10s, high speed 2000rp/min, 60s is revolved
Apply, make film is fully even to open, after spin coating terminates, 125 DEG C are heated 5 minutes on drying glue platform, finally with 500 DEG C of insulations of Muffle furnace
1h, is cooled to room temperature.
(3) doping TiO is prepared2Porous luminescent layer
Weigh a certain amount of ytterbium nitrate and holmium nitrate is dissolved in deionized water, be configured to 0.1mol/l ytterbium nitrate and nitric acid
Holmium, 20ml butyl titanates are added dropwise in 200m1 deionized waters under agitation, in 70 DEG C of constant temperature stirring 30min, are then measured
5ml Yb3+The Ho of solution and 1ml3+Solution is added drop-wise in this solution, and resulting solution is fitted into autoclave, and compactedness is
60%, 20h is heat-treated at 180 DEG C, Yb is obtained3+、Ho3+The TiO being co-doped with2Precipitation, beaker is poured into by gained precipitation, and 100 DEG C true
Sky drying becomes powder；After powder is ground, 5h is calcined at 800 DEG C, is cooled to after room temperature, the TiO adulterated2Nano powder
Body, particle size distribution is in 20-50nm；Gained powder is polished, adds 30% polyethylene glycol equivalent to powder quality
20000, the TiO adulterated2Nano-powder colloid；By the TiO of doping2Receive feed powder body spin coating 30s under 2000rpm rotating speeds, rotation
It is coated onto completed TiO2On compacted zone, 500 DEG C of exercise 40min naturally cool to after room temperature and taken out, obtain thickness for 600nm
Doping TiO2Porous luminescent layer.
(4) light-absorption layer is prepared
The presoma PbI2 of perovskite is dissolved in the PbI that 1mom/L is made into DMF2/ DMF solution, 20 μ l solution is applied
Cloth is on TiO 2 porous luminescent layer, and spin coating rotating speed is 6000rpm, and the time is 60s.Film is put into lockup immediately after end
Temperature is to heating 30min in 100 DEG C of heating plate.It is cooled to after room temperature, by 320 μ l 12mg/mlCH3NH3I aqueous isopropanol
The film surface in PbI2 is added dropwise, spin coating rotating speed is 2500rpm, and the time is 30s, and obtained brown film is placed on 80 DEG C of heating
30min is heated on plate, through 110 DEG C of heat treatment 10minm, perovskite light-absorption layer is obtained, thickness is 500nm.
(5) hole transmission layer is prepared
In glove box, prepare 50mmol/L spiro-OMeTAD chlorobenzene solutions, and add 4- tert .-butylpyridines (tBP,
50mmol/L) with two (trimethyl fluoride sulfonyl) imine lithiums (LiTFSI, 10nmol/L), it is sufficiently stirred for filtering after dissolving.With
3000r/min spin coating 30s, prepare thickness about 250nm hole transmission layers on perovskite light-absorption layer.
(6) prepare to electrode
Film obtained above is put into the thick Au layers of heat steaming deposition 100nm, vacuum are carried out in the vacuum chamber of evaporation instrument
Spend for 1.0 × 10-3Pa, thickness is 80nm.
(7) battery is carried out to light absorbs test and the performance test of battery under AM1.5,100mW/cm2 illumination.
Testing result is referring to Fig. 1-2, and wherein Fig. 1 is Ho3+/Yb3+The TiO being co-doped with2Porous layer up-conversion luminescence figure.After doping
Up-conversion luminescence peak be located at 549nm and 671nm, near infrared light can be converted into the visible of absorbable 549nm and 671nm
Light.Fig. 2 is the J-V performance curves of battery, and curve b is the testing result of the present embodiment battery, and photoelectric transformation efficiency is 16%, with
Under equal illumination condition undoped with battery (compared referring to curve a), its photoelectric transformation efficiency is significantly improved.
Embodiment 2
Embodiment 2 compared with Example 1, is different only in that TiO2The preparation method of porous luminescent layer is different, only right below
TiO2The preparation of porous luminescent layer is illustrated.
Weigh a certain amount of ytterbium nitrate, erbium nitrate, thulium nitrate to be dissolved in deionized water, be configured to 0.1mol/l nitric acid
Ytterbium, erbium nitrate and thulium nitrate, 20ml butyl titanates are added dropwise in 200m1 deionized waters under agitation, are stirred in 70 DEG C of constant temperature
30min is mixed, 5ml Yb is then measured3+The Tm3+ solution of solution, 1ml Er3+ and 1ml is added drop-wise in this solution, and gained is molten
Liquid is fitted into autoclave, and compactedness is 60%, is heat-treated 20h at 180 DEG C, obtains Yb3+、Er3+And Tm3+The TiO being co-doped with2It is heavy
Gained precipitation is poured into beaker by shallow lake, and 100 DEG C of vacuum drying become powder, after powder is ground, and 5h is calcined at 800 DEG C, cooling
After room temperature, the TiO of doping is obtained2Nano-powder, particle size distribution is in 20-50nm；Gained powder is polished, add equivalent to
30% PEG 20000 of powder quality, the TiO2 nano-powder colloids adulterated；By the TiO of doping2Nano-powder
The spin coating 30s under 2000rpm rotating speeds, is spun to completed TiO2On compacted zone, 500 DEG C of exercise 40min naturally cool to room
Taken out after temperature, obtain the porous TiO of doping that thickness is 600nm2。
The performance test results of battery manufactured in the present embodiment are referring to Fig. 3, as seen from Figure 3, the electricity obtained by the present embodiment
Pond photoelectric transformation efficiency is 16.5%.
Embodiment 3
Embodiment 3 compared with Example 1, is different only in that TiO2The preparation method of porous luminescent layer is different, only right below
TiO2The preparation of porous luminescent layer is illustrated.
Weigh a certain amount of ytterbium nitrate, manganese nitrate to be dissolved in deionized water, be configured to 0.1mol/l ytterbium nitrate, manganese nitrate
Solution, 20ml butyl titanates are added dropwise in 200m1 deionized waters under agitation, in 70 DEG C of constant temperature stirrings 30min, Ran Houliang
Take 5ml Yb3+The Mn of solution, 1ml2+Solution is added drop-wise in this solution, and resulting solution is fitted into autoclave, and compactedness is
60%, 20h is heat-treated at 180 DEG C, Yb is obtained3+And Mn2+The TiO being co-doped with2Precipitation.Gained precipitation is poured into beaker, 100 DEG C true
Sky drying becomes powder, after powder is ground, and is calcined at 800 DEG C after 5h, cooling room temperature, obtains rear-earth-doped TiO2Nanometer
Powder, particle size distribution is in 20-50nm；Gained powder is polished, adds the 30% poly- second two equivalent to powder quality
Alcohol 20000, the TiO2 nano-powder colloids adulterated；By the TiO of doping2Feed powder body colloid is received in 2000rpm rotating speed backspins
30s is applied, completed TiO is spun to2On compacted zone, 500 DEG C of exercise 40min naturally cool to after room temperature and taken out, obtain thickness
For the 600nm porous TiO of doping2。
Fig. 4 show the J-V performance curves that battery is made in the present embodiment, from fig. 4, it can be seen that battery obtained by the present embodiment
Photoelectric transformation efficiency is 17%.
The above described is only a preferred embodiment of the present invention, any formal limitation not is done to the present invention, therefore
All contents without departing from technical solution of the present invention, the technical spirit according to the present invention any is simply repaiied to made for any of the above embodiments
Change, equivalent variations and modification, in the range of still falling within technical solution of the present invention.
Claims (10)
1. a kind of wide spectrum perovskite solar cell, it is characterised in that including be cascading FTO glass substrates, TiO2
Compacted zone, TiO2Porous luminescent layer, perovskite light-absorption layer, hole transmission layer and metal electrode, the TiO2Contain in porous luminescent layer
There are Doped ions, the Doped ions include Yb3+With other ions, other described ions include Ho3+、Er3+、Mn2+、Tm3+In
At least one.
2. wide spectrum perovskite solar cell according to claim 1, it is characterised in that the TiO2Porous luminescent layer
In, Yb3+Mol ratio with other ions is 3~20：1, preferably 5：1.
3. wide spectrum perovskite solar cell according to claim 1, it is characterised in that in TiO2In porous luminescent layer,
The mol ratio of the Doped ions and Ti is 1:99~10：90.
4. wide spectrum perovskite solar cell according to claim 1, it is characterised in that the Yb3+With other ions
From the hydration containing these ions or non-hydrated nitrate.
5. wide spectrum perovskite solar cell according to claim 1, it is characterised in that the TiO2Porous luminescent layer
It is made according to the method comprised the following steps：
The aqueous solution of at least one of holmium nitrate, erbium nitrate, thulium nitrate, manganese nitrate and the ytterbium nitrate aqueous solution are added dropwise to metatitanic acid
In ester solution, hydrothermal treatment obtains the TiO of doping2Precipitation；Through drying, grind, calcine, cool down the TiO that must be adulterated2Powder, will
The TiO of the doping of gained2Powder is prepared into colloid, is spin-coated on TiO2On compacted zone, then carry out being thermally treated resulting in TiO2Porous hair
Photosphere.
6. wide spectrum perovskite solar cell according to claim 1 or 5, it is characterised in that the TiO2It is porous luminous
Layer is made according to the method comprised the following steps：Butyl titanate is added dropwise in deionized water under agitation, in 60~85 DEG C
Constant temperature stirs 15~60min, then by the aqueous solution and nitric acid of at least one of holmium nitrate, erbium nitrate, thulium nitrate, manganese nitrate
The ytterbium aqueous solution is added dropwise in solution of tetrabutyl titanate, 15~25h of hydro-thermal process at 170~185 DEG C, obtains the TiO of doping2It is heavy
Form sediment；Calcined through drying, grinding, 700~850 DEG C, cool down the TiO that must be adulterated2Powder, by the TiO of the doping of gained2Powder is added
In polyethylene glycol, colloid is prepared into, colloid is spin-coated on TiO2On compacted zone, TiO is thermally treated resulting in2Porous luminescent layer.
7. the wide spectrum perovskite solar cell according to any one of claim 1~6, it is characterised in that the TiO2It is many
The thickness of hole luminescent layer is 50~500nm, and aperture is 5-80nm；
The TiO2The thickness of compacted zone is 40-80nm, and the thickness of the perovskite light-absorption layer is 200-800nm, and the hole is passed
The thickness of defeated layer is 40-120nm, and the thickness of the metal electrode is 50-100nm.
8. the wide spectrum perovskite solar cell according to any one of claim 1~6, it is characterised in that the FTO glass
The square resistance of glass substrate is 5~20 Ω, and transmitance is 75~90%；The chemical composition of the perovskite light-absorption layer is
CH3NH3PbI3；The hole transmission layer is spiro-MeOTAD；The metal electrode is Au or Ag dorsum electrode layers.
9. the preparation method of the wide spectrum perovskite solar cell as described in any one of claim 1~8, it is characterised in that
Including such as step：
(1) cleaning FTO glass substrates, dry for standby；
(2) TiO is prepared in the conducting surface of FTO glass substrates2Compacted zone；
(3) in TiO2Fine and close layer surface prepares TiO2Porous luminescent layer；
(4) in TiO2Perovskite light-absorption layer is prepared on porous luminescent layer；
(5) hole transmission layer is prepared on perovskite light-absorption layer；
(6) metal electrode is prepared on perovskite light-absorption layer.
10. preparation method according to claim 9, it is characterised in that
In step (4), perovskite light-absorption layer is prepared according to the method including operating as follows：By perovskite presoma PbI2DMF it is molten
Liquid is spun on TiO2Film is formed on porous luminescent layer, 20~40min is heat-treated in 90~105 DEG C, is cooled to after room temperature, will
CH3NH3I aqueous isopropanol is added drop-wise to film surface, and spin coating obtains brown film, and it is heat-treated 20 after 70~85 DEG C~
40min, then through 100~120 DEG C of 5~20min of heat treatment, obtain perovskite light-absorption layer；
In step (5), hole transmission layer is prepared according to the method including operating as follows：By 4- tert .-butylpyridines, two (trifluoromethyls
Sulphonyl) imine lithium is dissolved in spiro-OMeTAD chlorobenzene solution, is spun on perovskite light-absorption layer.
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| CN108987581A (en) * | 2018-07-25 | 2018-12-11 | 中节能万润股份有限公司 | A kind of automatically cleaning perovskite solar battery and preparation method thereof |
| CN109888098A (en) * | 2019-04-04 | 2019-06-14 | 杨富强 | A kind of perovskite solar battery and preparation method thereof mixing cuprous sulfide in calcium titanium ore bed |
| US20220231233A1 (en) * | 2019-04-18 | 2022-07-21 | The University Of North Carolina At Chapel Hill | Perovskite solar cells with near-infrared sensitive layers |
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