CN107528002A - A kind of perovskite solar cell based on the insertion of dye sensitization upconverter - Google Patents
A kind of perovskite solar cell based on the insertion of dye sensitization upconverter Download PDFInfo
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Abstract
A kind of perovskite solar cell based on the insertion of dye sensitization upconverter, belongs to organic/inorganic composite material and optoelectronic materials technology.Mainly comprise the following steps and prepare the perovskite precursor liquid containing dye sensitization upconverter, the perovskite solar cell of this preparation dye sensitization upconverter insertion of base.This perovskite solar cell based on the insertion of dye sensitization upconverter has widened battery spectrum absorption region, has improved the opto-electronic conversion performance of solar cell by the absorbable near infrared light using 800 1000nm of dye sensitization upconverter.Present invention process is simple, and cost is cheap, has widened the absorption spectrum of perovskite solar cell, improves the photoelectric properties of battery, to perovskite too can the development of battery serve impetus.
Description
Technical field
The invention belongs to organic/inorganic composite material and optoelectronic materials technology, more particularly to based in dye sensitization turns
Application of the parallel operation in perovskite solar cell.
Background technology
In recent years, energy shortage problem, not only reserves are limited, non-renewable for traditional fossil energy, and it uses process
In huge pollution can be also brought to environment.And solar energy cleans renewable, the inexhaustible energy as a kind of
Just receive more and more attention.In this context, exploitation novel efficient low-cost solar battery causes various countries researcher
Huge interest, especially perovskite solar cell relies on good light absorptive and charge transport rate, and huge opens
Send out potentiality, 3.8% efficiency till now 22.1% risen since 2009, development is particularly rapid, be described as " photovoltaic art it is new
Wish ".The film of hundreds of nanometer thickness can fully absorb the sunshine below wavelength 800nm in perovskite solar cell.Though
Right absorption region is very wide, but utilizes upconverter, can be obvious so as to make infrared light invisible to the human eye be changed into visible ray
Improve the photoelectric efficiency of perovskite.But upconverter problem present in perovskite solar cell application is such as infrared/near
The absorption band of infrared light district is narrower, charge-conduction poor performance, hinders electron-stream transmission, causes the reduction of carrier collection efficiency,
Intermiscibility of the up-conversion nanoparticles in perovskite precursor liquid is poor.Researcher has found to take on up-conversion nanoparticles surface
Carry organic dyestuff IR-806 structure dye sensitization upconverter (absorption spectrum ranges are 800~1000nm) shapes of carboxyl-functional
Into energy and connection mode, the luminous intensity of upper conversion nano particle is obviously improved, has widened the absorption spectrum of nano-particle
[Wenqiang Zou1, Cindy Visser1, Jeremio A.Maduro, Nature Photonics 6,560-564
(2012)].Therefore, by using dye sensitization up-conversion, widen the absorption spectrum of perovskite solar cell, improve electricity
The application study of pond photoelectric properties does not have document report also so far.
The content of the invention
The problem of present invention is difficult by near infrared light for existing perovskite thin film material, it is therefore an objective to provide a kind of dye
Application of the material sensitization upconverter in perovskite solar cell.Dye sensitization upconverter is added in precursor solution,
Method, silk screen print method, scalpel knife coating, spraying process are applied by spin-coating method, drop, dye sensitization is formed in the presence of anti-solvent
The perovskite thin film of upconverter insertion, by this film with solar cells, widen the absorption of perovskite solar cell
Spectrum, improve cell photoelectric performance.
Perovskite solar cell based on the insertion of dye sensitization upconverter prepared by the present invention, is comprised the following steps that:
1) preparation of hydrophilic group dye sensitization upconverter:
The upconverter of coated by hydrophobic group is prepared, then prepared composition dispersion liquid, then add excessive inorganic salts NOBF4
Polar organic solvent so that hydrophobic grouping part is by BF4 -Substitute, the upconverter polarity after isolated ligand exchange is organic molten
Liquid;The organic dyestuff that excessive carboxyl-functional is added into the upconverter organic solution after ligand exchange carries out overlap joint reaction
Hydrophilic group dye sensitization upconverter is prepared, precipitation is then carried out and isolates hydrophilic group dye sensitization upconverter, redisperse arrives
In polar organic solvent, hydrophilic group dye sensitization upconverter dispersion liquid is formed;Polar organic solvent preferred DMF or DMSO;Bag
The material for including hydrophobic grouping preferably is selected from oleyl amine, oleic acid etc..
2) preparation of the perovskite precursor liquid of the upconverter containing dye sensitization:
The dispersion liquid of the upconverter containing dye sensitization prepared by step 1) is added to perovskite precursor liquid by a certain percentage
In, it is not higher than 100mg/mL to obtain the concentration of upconverter containing dye sensitization in mixed liquor;
3) assembling of the perovskite solar cell of dye sensitization upconverter insertion:
In conductive substrates spin coating prepare one layer of 2~800nm electron transfer layer, after dyestuff will be contained prepared by step 2)
The perovskite precursor liquid for being sensitized upconverter applies method, silk screen print method, scalpel knife coating or spraying process by spin-coating method, drop,
Form the perovskite thin film i.e. dye sensitization of dye sensitization upconverter insertion on the electron transport layer in the presence of anti-solvent
Upper converter is coated by perovskite crystal, and after annealed processing, then spin coating prepares the thick hole transmission layers of 2~500nm, finally
Prepare 10~1000nm it is thick to electrode, integrate perovskite solar cell.
Wherein, the upconverter described in step 1) be selected from undoped with β-NaYF4:Yb,Er、NaLnF4(Ln=Y, Gd,
Lu), oxysulfide M2O2S (M=Gd, Y, La), triplet state-triplet state annihilation (Triplet-triplet annihilation,
), and Er TTA3+、Yb3+-Er3+、Yb3+-Tm3+、Yb3+-Ho3+In one or more of doping, and doping, undoped with
Any at least two between core shell structure on turn device.
The organic dyestuff of carboxyl-functional described in step 1) is selected from IR-783, IR-806, IR-808, IR-820, IR-
845、Er(TTA)4(IR-806) one or more in.
The compound method of perovskite solution described in step 2) is by the one or more in AX, MX2In one kind or several
Kind is mixed in organic solvent, is configured to the perovskite solution that total mass concentration is 10~60wt%, wherein AX and MX2Mole
Than for 1:1;A groups in wherein AX are selected from CH3NH3、NH2- CH=NH2、CH3CH2NH3、CH3(CH2)2NH3、CH3(CH2)3NH3、
C6H5(CH2)2NH3Group and Cs;MX2Metal M be Pb, Sn in one kind, the mixture of two or more compounds;AX and
MX2In X be a kind of in I, Br, Cl;Perovskite precursor liquid uses organic solvent, and organic solvent is DMF
(DMF), at least one of dimethyl sulfoxide (DMSO), gamma-butyrolacton (GBL).
Anti-solvent described in step 3) is chlorobenzene, the one or more in toluene, ether, hexamethylene.
Conductive substrates described in step 3) are FTO electro-conductive glass, ITO electro-conductive glass or flexible conducting substrate.
Electron transfer layer described in step 3) for zinc oxide, tin ash, titanium dioxide, the barium stannate of La doped, richness
Strangle the one or more in alkene and derivative.
Annealing on hot plate described in step 3) is 50~300 DEG C of 5~120min of heating.
Hole transmission layer described in step 3) for Spiro-OMeTAD, PEDOT:PSS、CuPc、P3HT、PTAA、FDT、
CuI、MoO3, one or more in CuSCN and NiO.
Described in step 3) is the one or more in Ag, Au, Al, C electrode to electrode.
Compared with prior art, the invention has the advantages that:
The absorption that perovskite solar cell prepared by the present invention improves infrared/near-infrared all band solar spectrum is strong
Degree, the especially absorbable near infrared light using 800-1000nm, have widened battery spectrum absorption region, have improved solar cell
Opto-electronic conversion performance., battery spectrum absorption region has further been widened, has improved the photoelectric properties of solar cell.
Brief description of the drawings
The ultraviolet-visible absorption spectroscopy of dye sensitization upconverter insertion perovskite thin film material prepared by Fig. 1, embodiment 1
Figure.
The I-V curve of dye sensitization upconverter insertion perovskite solar cell prepared by Fig. 2, embodiment 1.
Fig. 3 is perovskite solar cell frame assumption diagram.
Embodiment
Below in conjunction with accompanying drawing and example, the invention will be further described, but the present invention is not limited to following examples.
Embodiment 1
1) preparation of dye sensitization upconverter:
(1) oleyl amine coating beta-NaYF4:The preparation of Yb, Er upconverter:Prepared using rare earth trifluoroacetate pyrolysis method
544mg CF3COONa,667.7mg Y(CF3COO)3,204.8mg Yb(CF3COO)3, 20.3mg Er (CF3COO)3And 30mL
It is added to after oleyl amine mixing in 100mL three-necked flask, is heated to 100 DEG C, is vacuumized 30min and remove H2O and O2, after in N2Atmosphere
Be heated under enclosing 330 DEG C, keep 1h, react completely after cooling down to 80 DEG C, then add 30mL ethanol with separate out β-
NaYF4:Yb, Er particle, last 5000rpm centrifuge 5min, precipitation are scattered in n-hexane solvent, formed 30mg/mL β-
NaYF4:Yb, Er n-hexane dispersion liquid.
(2) IR-806 organic dyestuff is carried:Take 3mL β-NaYF4:Yb, Er n-hexane dispersion liquid and 3mLNOBF4DMF it is molten
It is stirred vigorously after liquid (100mg/mL) mixing, after stratification, upper conversion nano particle is transferred to down from upper strata n-hexane solvent
In layer DMF solvent, oleyl amine part is by BF4 -Substitution, after take subnatant, add 2~4mg IR-806 organic dyestuff, stirred at 40 DEG C
12h is mixed, the rear isopropanol and toluene Mixed Solvent (volume ratio 1 for adding equal volume amounts:1) precipitation, 5000rpm centrifugations are separated out
5min, after take precipitation to be scattered in DMF solvent, form in 60mg/mL dye sensitization conversion DMF dispersion liquids.
2) preparation of the perovskite precursor liquid of the upconverter containing dye sensitization:
162.5mg iodine methylamine and 470mg lead iodides are mixed and added in 1ml DMF (DMF), normal temperature
It is stirred overnight, is configured to the perovskite precursor solution that weight/mass percentage composition is 40%.Can be by changing CH3NH3I、PbI2、
The amount of DMF three, change the mass fraction and molar fraction of perovskite.Then again by dispersion liquid prepared by step 1) by certain ratio
Example is added in perovskite precursor liquid, forms mixing precursor aqueous solution.
3) assembling of perovskite solar cell:
(1) cleaning of glass:The adhesive tape remained on glass is first washed with acetone, then respectively with liquid detergent, running water, go from
Son, acetone, (twice) of the order of isopropanol clean glass, every time the ultrasonic 10min in excusing from death is bathed.It is put into UV-ozone cleaning
Processing is irradiated in machine to substrate of glass.
(2) preparation of electron transfer layer (ETM)
Electron transfer layer (ETM) play the role of in the structure of perovskite solar cell it is irreplaceable, on the one hand not
Electronics can be only transmitted, on the other hand can stop the transmission in hole.In general electronics collecting layer selects ZnO, is coagulated using colloidal sol
Glue method prepares ZnO solution, and one layer of fine and close ZnO film is formed after the rear method calcining using spin coating.
(3) preparation of calcium titanium ore bed
Different volumes are dispersed with to the β-NaYF for carrying IR-8064:(polarity is organic by Yb, Er dye sensitization upconverter DMF
Solvent) dispersion liquid is added in perovskite precursor liquid, form mixing precursor aqueous solution.Using the method for one-step method spin coating in sol evenning machine
Upper spin coating (5000r/min, 30s), be added dropwise in spin coating the 6th second in the presence of chlorobenzene anti-solvent and form perovskite thin film, after
70 DEG C of heating 30min in heating plate.After spin coating, converter is coated by perovskite crystal in dye sensitization, forms one layer of dyestuff
It is sensitized β-NaYF4:Yb, Er@perovskite crystal nucleocapsid light-absorption layers.
(4) preparation of hole transmission layer (HTM)
HTM layers play transporting holes in whole battery structure, obstruct the effect of electronics.This experiment HTM materials used
For Spiro-MeOTAD.72.3mg Spiro-MeOTAD solid powders are taken, are dissolved in 1ml chlorobenzene, 60 DEG C of heating stirrings
20min, then the second for the lithium salts for being 520mg/mL toward the tetra-tert pyridine (TBP) and 17.5 μ L concentration that 28.8 μ L are added in solution
Nitrile solution stirring at normal temperature 2h, drip on perovskite-based bottom, spin coating 30s under 2500rpm.Under the conditions of lucifuge, it is allowed slowly to dry in the air naturally
It is dry.
(5) evaporation of metal electrode
The battery assembled is put into evaporator, two Argent grains is put into, control evaporation temperature and time, 70nm is deposited
Silver metal electrodes.
Claims (10)
- A kind of 1. preparation method of the perovskite solar cell based on the insertion of dye sensitization upconverter, it is characterised in that bag Include following steps:1) preparation of hydrophilic group dye sensitization upconverter:The upconverter of coated by hydrophobic group is prepared, then prepared composition dispersion liquid, then add excessive inorganic salts NOBF4Polarity Organic solution so that hydrophobic grouping part is by BF4 -Substitute, the upconverter polar organic solvent after isolated ligand exchange; The organic dyestuff that excessive carboxyl-functional is added into the upconverter organic solution after ligand exchange carries out overlap joint reaction system Standby hydrophilic group dye sensitization upconverter, then carries out precipitation and isolates hydrophilic group dye sensitization upconverter, redisperse to pole Property organic solution in, formed hydrophilic group dye sensitization upconverter dispersion liquid;2) preparation of the perovskite precursor liquid of the upconverter containing dye sensitization:The dispersion liquid of the upconverter containing dye sensitization prepared by step 1) is added in perovskite precursor liquid by a certain percentage, obtains Into mixed liquor, the concentration of upconverter containing dye sensitization is not higher than 100mg/mL;3) assembling of the perovskite solar cell of dye sensitization upconverter insertion:In conductive substrates spin coating prepare one layer of 2~800nm electron transfer layer, after dye sensitization will be contained prepared by step 2) The perovskite precursor liquid of upconverter applies method, silk screen print method, scalpel knife coating or spraying process by spin-coating method, drop, anti- The perovskite thin film for forming the insertion of dye sensitization upconverter in the presence of solvent on the electron transport layer turns i.e. in dye sensitization Change device to be coated by perovskite crystal, after annealed processing, then spin coating prepares the thick hole transmission layers of 2~500nm, finally prepares 10~1000nm it is thick to electrode, integrate perovskite solar cell.
- 2. according to the preparation method described in claim 1, it is characterised in that upconverter described in step 1) be selected from undoped with β-NaYF4:Yb,Er、NaLnF4, oxysulfide M2O2S, triplet state-triplet state annihilation (Triplet-triplet Annihilation, TTA), and Er3+、Yb3+-Er3+、Yb3+-Tm3+、Yb3+-Ho3+In one or more of doping, and Doping, undoped with any at least two between core shell structure on turn device, Ln=Y, Gd, Lu, M=Gd, Y, La.
- 3. according to the preparation method described in claim 1, it is characterised in that the organic dyestuff of carboxyl-functional be selected from IR-783, IR-806、IR-808、IR-820、IR-845、Er(TTA)4(IR-806) one or more in.
- 4. according to the preparation method described in claim 1, it is characterised in that the compound method of the perovskite solution described in step 2) For by the one or more in AX, MX2In one or more be mixed in organic solvent, be configured to total mass concentration for 10~ 60wt% perovskite solution, wherein AX and MX2Mol ratio be 1:1;A groups in wherein AX are selected from CH3NH3、NH2- CH= NH2、CH3CH2NH3、CH3(CH2)2NH3、CH3(CH2)3NH3、C6H5(CH2)2NH3Group and Cs;MX2Metal M be Pb, Sn in One kind, the mixture of two or more compounds;AX and MX2In X be a kind of in I, Br, Cl;Perovskite precursor liquid is adopted With organic solvent, organic solvent is in DMF (DMF), dimethyl sulfoxide (DMSO), gamma-butyrolacton (GBL) It is at least one.
- 5. according to the preparation method described in claim 1, it is characterised in that the anti-solvent described in step 3) is chlorobenzene, toluene, second One or more in ether, hexamethylene.
- 6. according to the preparation method described in claim 1, it is characterised in that the conductive substrates described in step 3) are FTO conduction glass Glass, ITO electro-conductive glass or flexible conducting substrate;Electron transfer layer described in step 3) is selected from zinc oxide, tin ash, titanium dioxide One or more in titanium, the barium stannate of La doped, fullerene and derivative.
- 7. according to the preparation method described in claim 1, it is characterised in that the annealing described in step 3) is 50~300 DEG C 5~120min is heated, is made annealing treatment on hot plate.
- 8. according to the preparation method described in claim 1, it is characterised in that hole transmission layer described in step 3) is selected from Spiro-OMeTAD、PEDOT:PSS、CuPc、P3HT、PTAA、FDT、CuI、MoO3, one or more in CuSCN and NiO; Described in step 3) is the one or more in Ag, Au, Al, C electrode to electrode.
- 9. according to the preparation method described in claim 1, it is characterised in that step 1) polar organic solvent preferred DMF or DMSO; Material including hydrophobic grouping preferably is selected from the one or more in oleyl amine, oleic acid.
- 10. according to any one of claim 1-9 method be prepared based on dye sensitization upconverter insertion perovskite too Positive energy battery.
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CN108574046A (en) * | 2018-05-24 | 2018-09-25 | 中节能万润股份有限公司 | A kind of perovskite solar cell and preparation method thereof |
CN108682702A (en) * | 2018-06-06 | 2018-10-19 | 北京大学 | A kind of photoelectric device composite hole transporting layer material and preparation method thereof |
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CN108682702A (en) * | 2018-06-06 | 2018-10-19 | 北京大学 | A kind of photoelectric device composite hole transporting layer material and preparation method thereof |
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WO2020029205A1 (en) * | 2018-08-09 | 2020-02-13 | 苏州大学张家港工业技术研究院 | Method for preparing inorganic perovskite battery based on synergistic effect of gradient annealing and antisolvent, and prepared inorganic perovskite battery |
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