CN109192859A - A kind of perovskite solar cell and preparation method thereof based on inorganic semiconductor electron transport material - Google Patents
A kind of perovskite solar cell and preparation method thereof based on inorganic semiconductor electron transport material Download PDFInfo
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Abstract
The present invention relates to the photovoltaic devices converted light into as electric energy, refer in particular to the perovskite solar cell of inorganic semiconductor electron transport material, the described method includes: the deposition of amorphous silicon films material on transparent conducting glass, it is then spin coated onto PCBM interface-modifying layer, spin coating perovskite light absorbent later, spin coating Spiro-OMeTAD material is as hole transmission layer, last evaporation metal electrode later.The present invention has the advantages that electron transfer layer of the N-type amorphous silicon as perovskite battery, band gap can regulate and control by doping concentration, can be very good to realize level-density parameter with perovskite material；Low temperature preparation makes it be more suitable for flexible substrate perovskite solar cell；Vacuum method prepares the uniformity of film and repeatability is that spin-coating method cannot compare.PCBM interface-modifying layer can improve amorphous silicon membrane/perovskite interface energy level matching, transport electronics and stop hole, so as to reduce photo-generated carrier in compound, the final raising solar cell transfer efficiency of electron transfer layer and absorbed layer interface.
Description
Technical field
The present invention relates to photovoltaic technology field, and in particular to arrives the calcium of inorganic semiconductor electron transport material (ETL)
Titanium ore battery and preparation method thereof.
Background technique
The new energy field constantly risen in recent years, such as solar energy, geothermal energy etc. all have been provided with mature industry
Change production model, and nuclear energy, tide energy also gradually obtain the extensive concern of government and street levels.The sun is especially among these energy
Can, there is environmentally friendly, from a wealth of sources, the convenient advantage of materials, this also allows solar energy to show one's talent in new energy.
Perovskite solar cell, which has, realizes that relatively easy large area production, preparation process, low temperature preparation, preparation cost are low
The advantages that, so that it has been obtained quick development and extensive concern in recent years, efficiency is also developed to by incipient 3.9%
Present 22.7%.Perovskite solar cell is to develop very fast solar cell at present, by conductive substrates, electron-transport material
Material, perovskite absorbed layer, hole mobile material and metal electrode are constituted.Perovskite absorbed layer have good light abstraction width,
Carrier lifetime length, controllable band gap and excellent photo-generated carrier transport property.The electron transfer layer of perovskite structure battery
It must assure that the electronics in photo-generated carrier is smoothly collected, transmits and collected by electrode, and stability wants excellent, price just
Preferably, it is easy preparation.And silica-base film is a kind of semiconductor material of function admirable, and it is nontoxic, in earth rich reserves.Amorphous
Silicon can realize adjusting band gap by adjusting doping concentration, and as its different film quality of sedimentary condition and electric conductivity can be with
Improved well, is the semiconductor material that performance is stable in thin film solar cell.
The N-type amorphous silicon thin-film materials of phosphorus doping, the doping concentration by regulating and controlling phosphorus can regulate and control silicon thin film level of energy
And band gap width, guarantee that energy level and perovskite material realize matching well, smoothly to realize carrier transport, reduces photoproduction and carry
Recombination rate of stream in interface.Its conduction band bottom energy level of N-type amorphous silicon membrane in -4.0eV or so, the LUMO of perovskite is -
3.93eV, for electronics, the conduction level of perovskite is higher than N-type amorphous silicon thin-film materials, this band scale can guarantee
Electronics in calcium titanium ore bed smoothly flows to N-type amorphous thin Film layers；The top of valence band of N-type amorphous silicon membrane is in -5.88eV or so, calcium
Titanium ore HOMO is -5.44eV, and N-type amorphous silicon thin-film materials top of valence band is higher than perovskite for hole, this band scale pair
Play the role of a potential barrier in hole, prevents hole transport to N-type noncrystal membrane layer.Simultaneously, in N-type amorphous silicon membrane
After adding PCBM interface-modifying layer between perovskite absorbed layer, the HOMO of PCBM material is -6.1eV, the HOMO with perovskite
Energy level difference is 0.66eV, may further effectively stop hole, to reduce the probability of electron-hole recombinations.
Summary of the invention
The purpose of the present invention: the main direction of development of the problem of existing in view of the above technology and the following solar cell, by N
Type amorphous silicon thin-film materials and perovskite intrinsic layer match, and prepare a kind of new be suitable as using plasma vapor phase deposition
The amorphous silicon silicon thin film material of perovskite battery electron transport layer.Feature is: using N-type amorphous silicon membrane as perovskite battery
Electron transfer layer, it is low in cost, it is easy preparation, low temperature preparation and can be had good stability.Meanwhile it being inhaled using PCBM as perovskite
The interface-modifying layer for receiving layer and amorphous silicon electron-transport interlayer can improve amorphous silicon membrane surface topography and stop hole, from
And photo-generated carrier can be reduced in the compound of electron transfer layer and absorbed layer interface, it is finally reached and improves carrier transport effect
Rate.
Technical solution of the present invention: the perovskite solar cell of the inorganic semiconductor electron transport material is led by transparent
Electric substrate, N-type amorphous silicon electron transfer layer, PCBM interface-modifying layer, perovskite material absorbed layer, hole transmission layer, metal electricity
Pole is constituted.
Electrically conducting transparent substrate is FTO transparent conducting glass；Amorphous silicon electron transfer layer is heavy using plasma vapor phase deposition
On FTO glass, energy level and perovskite material are mutually matched product, can regulate and control amorphous silicon layer energy by regulation doping concentration
Grade.Spin-coating method spin coating PCBM interface-modifying layer is used on amorphous silicon, later this absorbed layer of spin coating perovskite.Calcium titanium after above-mentioned spin coating
Pit wood material is after annealing, spin coating Spiro-OMeTAD hole transmission layer on it.Finally hole is plated in thermal evaporation
Evaporation metal electrode on transport layer.
Above-mentioned transparent conductive substrate is FTO transparent conducting glass, and transmitance 70-85%, square resistance is 10-30 Ω/.
The N-type amorphous silicon electron transfer layer uses plasma enhancingization by silane, phosphine, hydrogen under vacuum conditions
It learns vapor deposition (PECVD) to form, with a thickness of 30-50nm.
The interface-modifying layer of the electron transfer layer and perovskite absorbed layer is PCBM, with a thickness of 5-10nm.
The perovskite absorber thickness is 400-600nm.
The hole transmission layer is Spiro-OMeTAD, with a thickness of 300-400nm.
The electrode is silver/golden metal electrode.
Raw material, process equipment involved in above-mentioned are well known.
The invention has the advantages that electron transfer layer of the N-type amorphous silicon as perovskite battery, band gap can pass through doping
Concentration regulation can be very good to realize level-density parameter with perovskite material；PCBM interface-modifying layer can improve amorphous silicon membrane
Surface topography and stop hole, so as to reduce photo-generated carrier in the compound of electron transfer layer and absorbed layer interface, most
Reach eventually and improves carrier transport efficiency；Low temperature preparation makes it be more suitable for flexible substrate perovskite solar cell；Vacuum legal system
The uniformity and repeatability of standby N-type amorphous silicon membrane are the advantages of antivacuum method cannot compare.The simple valence of preparation method
Lattice are cheap and have good stability, and have important researching value and practical value.
Detailed description of the invention
Fig. 1 is the perovskite solar cell energy level schematic diagram of inorganic semiconductor electron transport material in the present invention.
Fig. 2 is the perovskite solar cell structural schematic diagram of inorganic semiconductor electron transport material.
Fig. 3 is the J-V figure of the perovskite solar cell of inorganic semiconductor electron transport material.
Fig. 4 is the quantum efficiency figure of the perovskite solar cell of inorganic semiconductor electron transport material.
Specific embodiment
Technical solutions according to the invention are described in detail below with reference to embodiment, the specific steps are as follows:
The processing of first step electrically conducting transparent substrate:
The electrically conducting transparent substrate is stannic oxide (FTO) electro-conductive glass of fluorine doped.By the electricity consumption of FTO transparent conducting glass elder generation
Sub- cleaning solution is clean by its surface clean, is then cleaned by ultrasonic 20min with the deionized water solution of electronics cleaning solution, then uses wine
Essence ultrasonic cleaning 10min, is cleaned by ultrasonic 10min with deionized water later, the transparent conducting glass after flushing is blown with nitrogen gun
It is dry and 15 minutes dry in drying box.High temperature gummed tape is sticked in the side of FTO glass, retains test electrode.
Second step N-type amorphous silicon membrane deposition:
Above-mentioned spare electrically conducting transparent substrate is put into plasma deposition chambers, the preparation of N-type amorphous silicon membrane is carried out.Reaction
The mixed gas that gas mixing ratio used is SiH4: PH3: H2=12: 3.6: 24.4, reaction chamber temperature are 140~260 DEG C.
Radio-frequency power 15-30W.Reaction pressure is 200P~230Pa.Sedimentation time maintains about 5~8min.Obtained by under this condition
Amorphous silicon membrane thickness about 30-50nm.
Third step prepares PCBM interface-modifying layer:
The PCBM of 15mg is dissolved in the aqueous isopropanol of 1ml.Be slowly stirred under the conditions of 55 DEG C 2 hours or more it is spare.
With desk-top sol evenning machine in above-mentioned substrate spin coating PCBM solution, spincoating conditions 5000rpm, spin-coating time 40s.In 120 DEG C of temperature
The lower 10min that anneals of degree.PCBM film thickness about 5-10nm obtained under this condition.
4th step prepares perovskite Intrinsic Gettering layer:
Using one step spin-coating method of solution, the specific steps are as follows:
A. perovskite precursor solution prepares.The PbI for being 99.999% by the mass percent bought2Solid powder with buy
FAI and MAI solid powder carry out molar ratio be PbI2: mixed powder is dissolved in the mixing of FAI: MAI=2: 1: 1 ratio
In the dimethylformamide (DFM) that the mass percent purity bought is 99.9%, with magnetic agitation 6 small at a temperature of 50 DEG C
When or so it is spare.
B. spin coating perovskite Intrinsic Gettering layer.The FTO electro-conductive glass that deposited amorphous silicon membrane is put on spin coating instrument,
Spare perovskite precursor solution is taken, with being covered on amorphous thin Film layers after the filtering of 0.22um filter tip, starting spin coating instrument turns
The chlorobenzene of 150ul is added dropwise in fast 3000rpm, 10s or so in spin coating process.Spin-coating time is 30~50s.
C. it is heat-treated, that is, anneals.The substrate of the good perovskite of the above-mentioned spin coating on amorphous silicon layer is placed on hot plate, 90
Perovskite light-absorption layer, thickness about 400-600nm, calcium titanium at this time is made in stepped annealing about 100min at a temperature of~140 DEG C
Mine light-absorption layer surface coverage, the uniformity and compactness are all greatly improved.Spin coating and annealing operate in glove box.
5th step prepares hole transmission layer:
Select Spiro-OMeTAD as hole transmission layer.Substrate after above-mentioned heat treatment is placed on spin coating instrument.
The Spiro-OMeTAD bought is dissolved in chlorobenzene solution, stirred under the conditions of 50 DEG C 2 hours or more it is spare.It will be obtained above
Spiro-OMeTAD solution, which drops evenly, is covered on substrate surface, opens spin coating instrument, 2000~2500rpm of revolving speed, spin coating 30
After~40s, fully oxidized 12 hours or more in dry air.
6th step electrode evaporation:
Filamentary silver is vaporized in the molten state on hole transmission layer made from the 5th step and forms electrode, and nothing is finally made
The perovskite solar cell of machine semiconductor electronic transmission material.Concrete operation method is vacuum thermal evaporation technique: in 60~100A
Silver/spun gold is melted into gaseous state under electric current, 20-30min is deposited.Metal electrode is made, complete inorganic semiconductor is finally made
The perovskite solar cell of electron transport material.
Claims (8)
1. a kind of perovskite solar cell and preparation method thereof based on inorganic semiconductor electron transport material, it is characterised in that:
(1) N-type amorphous silicon electron transfer layer is prepared using chemical vapor deposition (PECVD) method in electrically conducting transparent substrate；
(2) sol-gel method spin coating PCBM interface-modifying layer on amorphous silicon layer is used；
(3) calcium titanium ore bed is prepared on PCBM using a step spin-coating method；
(4) Spiro-OMeTAD hole transmission layer is prepared on calcium titanium ore bed using spin-coating method；
(5) metal electrode is steamed using vacuum vapour deposition on the hole transport layer.
2. perovskite structure solar cell according to claim 1, it is characterised in that: electrically conducting transparent substrate is that FTO is transparent
Electro-conductive glass, N-type amorphous silicon electron transfer layer, PCBM are interface-modifying layer, and absorbed layer is perovskite light absorbent, hole transport
Layer is Spiro-OMeTAD material, and metal electrode is silver electrode or gold electrode.
3. perovskite structure solar cell according to claim 1, it is characterised in that: the electron transfer layer is N-type
Amorphous silicon thin-film materials, with a thickness of 30-50nm.
4. perovskite structure solar cell according to claim 1, it is characterised in that: the electron transfer layer and calcium titanium
The interface-modifying layer of mine absorbed layer is PCBM, with a thickness of 5-10nm.
5. perovskite structure solar cell according to claim 1, it is characterised in that: the perovskite light-absorption layer is
FAxMA1-xPbI3(FA:CH (NH2)2, MA:CH3NH3), with a thickness of 400-600nm.
6. perovskite structure solar cell according to claim 1, it is characterised in that: the hole transmission layer is Spiro-
OMeTAD, with a thickness of 300-400nm.
7. perovskite structure solar cell according to claim 1, it is characterised in that: the metal electrode be silver electrode or
Gold electrode, with a thickness of 90-120nm.
8. perovskite structure solar cell preparation method according to claim 1, comprising the following specific steps
(1) processing of first step electrically conducting transparent substrate:
The electrically conducting transparent substrate is stannic oxide (FTO) electro-conductive glass of fluorine doped.FTO transparent conducting glass is first clear with electronics
Washing lotion is clean by its surface clean, is then cleaned by ultrasonic 20min with electronics cleaning solution and deionized water solution, then super with alcohol
Sound cleans 10min, is cleaned by ultrasonic 10min with deionized water later, the transparent conducting glass after flushing is dried up with nitrogen gun, and
It is 15 minutes dry in drying box.High temperature gummed tape is sticked in the side of FTO glass, retains test electrode.
(2) second step N-type amorphous silicon membrane deposits:
Above-mentioned spare electrically conducting transparent substrate is put into plasma deposition chambers, the preparation of N-type amorphous silicon membrane is carried out.Used in reaction
Gas be SiH4、PH3And H2Mixed gas, reaction chamber temperature be 140~260 DEG C, radio-frequency power 15-30W, reaction pressure
It is by force 200~230Pa, sedimentation time maintains about 5~8min.Obtained amorphous silicon membrane thickness about 30- under this condition
50nm。
(3) third step prepares PCBM interface-modifying layer:
The PCBM of 15mg is dissolved in the aqueous isopropanol of 1ml.Be slowly stirred under the conditions of 55 DEG C 2 hours or more it is spare.With platform
Formula sol evenning machine spin coating PCBM solution in above-mentioned substrate, spincoating conditions 5000rpm, spin-coating time 40s.At a temperature of 120 DEG C
Anneal 10min.PCBM film thickness about 5-10nm obtained under this condition.
(4) the 4th steps prepare perovskite absorbed layer:
Using one step spin-coating method of solution, the specific steps are as follows: open
A. perovskite precursor solution prepares.The PbI for being 99.999% by the mass percent bought2Solid powder and the FAI bought
Carrying out molar ratio with MAI solid powder is PbI2: mixed powder is dissolved in and buys by the mixing of FAI: MAI=2: 1: 1 ratio
Mass percent purity be 99.9% dimethylformamide (DFM) in, with 6 hours of magnetic agitation or so at a temperature of 50 DEG C
It is spare.
B. spin coating perovskite absorbed layer.The FTO electro-conductive glass that deposited amorphous silicon membrane is put on sol evenning machine, spare calcium is taken
Titanium ore precursor solution, drop coating starts spin coating instrument revolving speed 3000rpm on amorphous thin Film layers after being filtered with 0.45 μm of filter tip,
The chlorobenzene of 150ul is added dropwise in 10s or so in spin coating process.Spin-coating time is 30~50s.
C. it is heat-treated, that is, anneals.The substrate of the good perovskite of the above-mentioned spin coating on amorphous silicon layer is placed on hot plate, 90~
Perovskite absorbed layer, thickness about 400-600nm, perovskite at this time is made in stepped annealing about 100min at a temperature of 150 DEG C
Light-absorption layer surface coverage, the uniformity and compactness are all greatly improved.Spin coating and annealing operate in glove box.
(5) the 5th steps prepare hole transmission layer:
Select Spiro-OMeTAD as hole transmission layer.Substrate after above-mentioned heat treatment is placed on spin coating instrument.It will purchase
Spiro-OMeTAD be dissolved in chlorobenzene solution, stirred under the conditions of 50 DEG C 2 hours or more it is spare.It will be obtained above
Spiro-OMeTAD solution, which drops evenly, is covered on substrate surface, spin coating instrument, 2000~2500rpm of revolving speed, 30~40s of spin coating
Afterwards, fully oxidized 12 hours or more in dry air.
(6) the 6th step electrode evaporations:
Filamentary silver/spun gold is vaporized in the molten state on hole transmission layer made from the 5th step and forms electrode.Concrete operations side
Method is vacuum thermal evaporation technique: filamentary silver/spun gold being melted into gaseous state under 60~100A electric current, 20-30min is deposited.Gold is made
Belong to electrode, the perovskite solar cell of complete inorganic semiconductor electron transport material is finally made.
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| CN114709336B (en) * | 2022-04-01 | 2023-02-03 | 暨南大学 | Perovskite material and application thereof in solar cell |
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Application publication date: 20190111 |