CN107316942A - A kind of perovskite solar cell and preparation method thereof - Google Patents
A kind of perovskite solar cell and preparation method thereof Download PDFInfo
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Abstract
The invention belongs to area of solar cell, a kind of perovskite solar cell is disclosed, it includes transparent conductive substrate, electron transfer layer, interface-modifying layer, modified perovskite active layer, hole transmission layer and anode successively;Wherein, the electron transfer layer is nano-titania particle layer, and interface-modifying layer is fullerene derivate layer.Using sol-gal process, using titanium tetrachloride as the highly crystalline TiO of precursor synthesis2Nano-particle, and applied it to using low temperature annealing process among perovskite solar cell, then the direct spin coating fullerene derivate of gained nano-titania particle layer surface is modified, it is passivated titanium dioxide and perovskite internal flaw, using new perovskite synthesis path, gained perovskite solar cell has high efficiency, no hysteresis effect and device can carry out stablizing output under low temperature preparation technique;And the preparation technology that is related to is simple, energy consumption is low, is adapted to popularization and application.
Description
Technical field
The invention belongs to area of solar cell, and in particular to a kind of perovskite solar cell and its low temperature preparation side
Method.
Background technology
In recent years, as industrialization and population are continuously increased, energy shortage problem has become the head for hindering economic development
Want problem.Fossil fuel supply and unfavorable climate change in face of increasingly reduction, find feasible regenerative resource and seem
It is particularly important.In all regenerative resources, solar energy is most promising one kind.At present, photovoltaic market is mainly by crystal
Occupied by the solar cell that silicon is made.However, even allow for being greatly reduced for crystalline silicon price, high production and it is mounted to
Most of regional recovery times caused by this are long, reduce widely used economic feasibility.Organic-inorganic composite perovskite
Solar cell is received much concern due to low cost, the characteristic such as solution processable and high efficiency, with all solid state perovskite structure
As the solar cell of light absorbent, its energy gap is about 1.5eV, and extinction coefficient is high, and the film of hundreds of nanometer thickness can be abundant
Below 800nm sunshine is absorbed, there is important application prospect in opto-electronic conversion field.
Electron transport material is to influence the key factor of device efficiency, TiO2Because having high conductivity and electron mobility,
And the level-density parameter good with perovskite, it is as one of elite clone of electron transfer layer.However, being in device preparation
Make amorphous phase TiOXBe converted to crystalline state TiO2, compacted zone and mesoporous layer TiO2Preparation there is the process of high temperature sintering, no
Only energy consumption is big, and greatly limits its application on a flexible substrate, is unfavorable for large-scale production.Lot of domestic and foreign seminar causes
Power is in solution TiO2The high-temperature calcination problem of layer, but most of TiO obtained using low temperature synthesis with processing mode2, often table
Reveal many limitations, its device usually contains the presence of a large amount of defect states, cause device show relatively low device efficiency with
And serious hysteresis effect, it is impossible to carry out stable output.Therefore, using suitable processing mode to TiO2Surface carries out interface and repaiied
Decorations, and perovskite active layer is modified, obtain under low temperature preparation process conditions still with high efficiency, without delayed calcium titanium
Ore deposit solar cell, with important research and application value.
The content of the invention
It is an object of the invention to provide a kind of perovskite solar cell, using sol-gel process, using titanium tetrachloride as
The highly crystalline TiO of precursor synthesis2Nano-particle, and using low temperature annealing process apply it to perovskite solar cell work as
In, then the direct spin coating fullerene derivate of gained nano-titania particle layer surface is modified, titanium dioxide is passivated
And perovskite internal flaw, and perovskite active layer is modified, make gained perovskite solar cell in low temperature preparation work
There is high efficiency, no hysteresis effect and device can effectively carry out stablizing output under skill;And the preparation technology that is related to is simple, energy consumption
It is low, it is adapted to popularization and application.
To achieve the above object, the technical solution adopted by the present invention is:
A kind of perovskite solar cell, it is characterised in that it includes transparent conductive substrate, electron transfer layer, boundary successively
Face decorative layer, modified perovskite active layer, hole transmission layer and anode;Wherein, the electron transfer layer is nano titanium oxide
Particle layer, interface-modifying layer is fullerene derivate layer.
In such scheme, the preparation method of the nano-titania particle layer comprises the following steps:In ice-water bath condition
Under, titanium tetrachloride and ethanol are sufficiently mixed uniformly, then added in phenmethylol, 8~10h is reacted under the conditions of 70~80 DEG C,
Precipitated, washed using ether, products therefrom is scattered in alcohol solvent again, control the quality of nano-titania particle
Concentration is eventually adding titanium chelate and obtains nano titanium oxide dispersion in 8~12mg/ml, then spin-coated, Low Temperature Heat Treatment is obtained
The nano-titania particle layer.
In such scheme, the titanium tetrachloride, ethanol, the volume ratio of phenmethylol are 1:(3.4~5):(17~25).
In such scheme, the titanium chelate is bis-acetylacetonate metatitanic acid diisopropyl ester, it and nano-titania particle
Mol ratio be 1:(8~12).
In such scheme, the low temperature heat-treatment process is:It is heated to 120~160 DEG C of 15~40min of annealing.
In such scheme, the thickness of the electron transfer layer is 30~50nm.
In such scheme, the thickness of described fullerene derivate layer is 40~60nm.
In such scheme, the modified perovskite active layer using two-step method prepare, wherein the precursor solution used by
Lead iodide and iodate carbonamidine press 1.3:The mol ratio of (0.2~0.4), is dissolved in volume ratio for (7~10):1 DMF's and DMSO
In the mixed solvent is formed, and the shared total concentration in precursor solution is 650~750mg/ml to lead iodide with iodate carbonamidine;Use
The aqueous isopropanol concentration of iodate methylamine is 30~50mg/ml;The mol ratio of iodate carbonamidine and iodate methylamine is 1:(1.2~
1.5);Specific preparation process is as follows:Precursor solution afterwards will with 5000~7000rpm rotating speed 10~20s of spin coating first
Iodate methylamine solution is with 3000~4500rpm rotating speed 30~50s of spin coating, finally by gained film under the conditions of 90~110 DEG C
20~40min is heat-treated, modified perovskite active layer is obtained.
In such scheme, the spin coating solution used of the hole transmission layer is that lithium salts and tert .-butylpyridine doping are improved
The fluorenes Spiro-OMeTAD solution of 2,2', 7,7'- tetra- [N, N- bis- (4- methoxyphenyls) amino] -9,9'- spiral shells two, it is by Spiro-
OMeTAD, the acetonitrile solution of double (fluoroform) sulfimide lithium salts and tert .-butylpyridine are blended and formed in chlorobenzene solvent.
In such scheme, the thickness of the hole transmission layer is 150~250nm.
In such scheme, the transparent conductive substrate can select electrically conducting transparent substrate FTO, ITO etc..
In such scheme, the anode material is Au, Ag etc..
In such scheme, the anode layer thickness is 100~150nm.
A kind of low temperature preparation method of above-mentioned perovskite solar cell, it comprises the following steps:
1) transparent conductive substrate is cleaned, pre-processed;
2) through step 1) pretreatment transparent conductive substrate on prepare electron transfer layer:Nano titanium oxide is prepared to disperse
Liquid, then spin-coated, Low Temperature Heat Treatment obtain nano-titania particle layer;
3) spin coating fullerene derivate solution on the electron transport layer, then carries out annealing and prepares interface-modifying layer;
4) modified perovskite active layer is prepared using two-step method;
5) spin coating hole transmission layer is placed in carrying out oxidation overnight in drier improving on modified perovskite active layer
The electrical conductivity and mobility of hole transmission layer;
6) anode material is deposited on hole transmission layer, the perovskite solar cell is produced.
In such scheme, step 1) described in cleaning step to be surpassed successively using deionized water, ethanol, acetone, isopropanol
Sound cleans 10~20min, is then dried up with nitrogen;The pre-treatment step is to be handled through UV-ozone.
In such scheme, step 2) described in spin coating proceeding be:With 2000~4000rpm 30~40s of rotating speed spin coating.
In such scheme, step 2) described in low temperature heat-treatment process be:Be heated to 120~160 DEG C annealing 15~
40min。
In such scheme, step 3) described in spin coating proceeding be:With 1000~2000rpm 20~40s of rotating speed spin coating;Move back
Ignition technique is:It is heated to 80~120 DEG C of 10~20min of insulation.
In such scheme, step 5) described in spin coating rotating speed be 3000~5000rpm.
The present invention principle be:
1) present invention synthesizes highly crystalline TiO using sol-gel process2Nano-particle, and carried by adding titanium chelate
The dispersiveness of high nano titanium oxide dispersion;Gained nano titanium oxide dispersion is subjected to spin coating and Low Temperature Heat Treatment system again
It is standby to obtain electron transfer layer, present invention gained TiO2Layer is compared to TiO prepared by existing high-temperature calcination2Compacted zone and mesoporous layer are low
The doping effect that the decomposition of titanium chelate is formed for film in warm annealing steps, can effectively improve TiO2The conductance of compacted zone
Rate, accelerates the extraction and transmission of electric charge.
2) present invention between electron transfer layer and modified perovskite active layer by setting fullerene boundary layer to carry out boundary
Face is modified, and further improves device performance.
3) present invention is improved to modified perovskite active layer two-step method, is introduced in two-step method in first step presoma
A small amount of iodate carbonamidine (FAI), expands iodate lead frame so that PbI using FAI2Framework is more loose, so as to be more beneficial for second
The intercalation of MAI molecules during step, suppresses the Volumetric expansion produced by conventional two-step, promotes the life of perovskite crystal
It is long, bigger crystallite dimension is obtained, body defects are reduced, while FAI can effectively improve the band gap width of perovskite, changes its suction
Optical range.
Compared with prior art, beneficial effects of the present invention are:
1) present invention proposes a kind of crystal type TiO2The low temperature preparation method of nano-particle, and use it for low temperature preparation
Perovskite solar cell electron transfer layer, titanium chela after compacted zone and mesoporous layer, low temperature thermal annealing is prepared compared to high-temperature calcination
The doping effect that the decomposition of compound is formed for film, can effectively improve TiO2The electrical conductivity of compacted zone, accelerates the extraction of electric charge
With transmission, and be conducive to the preparation of flexible perovskite solar cell.
2) present invention is not only solved by introducing fullerene boundary layer between electron transfer layer and modified perovskite active layer
The relatively low phenomenon of charge extraction efficiency certainly in planar heterojunction caused by limited contact area, and in fullerene interface layer surfaces
The interface diffusion formed during spin coating perovskite precursor solution, can effectively play fullerene to the blunt of passivation perovskite crystal boundary
Change is acted on, and is effectively reduced defect present in passivation calcium crystal, is suppressed Carrier recombination, so as to eliminate hysteresis.
3) present invention is incorporated into PbI by iodate carbonamidine (FAI)2In framework, perovskite thin film can be simply and effectively lifted
Crystalline rate, while reducing the band gap width of perovskite, the light absorption range for obtaining wider distribution simultaneously can further improve photoelectricity
Transformation efficiency, so as to obtain the electric current and device performance higher than MAI system.
4) preparation technology of the present invention is simple, reaction condition is gentle, energy consumption is low, gained perovskite solar cell tool
There is high efficiency, without hysteresis effect, and device can effectively carry out stablizing output, be adapted to popularization and application.
Brief description of the drawings
Fig. 1 is the structural representation of the gained perovskite solar cell of the embodiment of the present invention 1.
Fig. 2 is the current -voltage curve of perovskite solar cell prepared by embodiment 1.
Fig. 3 is the stable state curve of output of perovskite solar cell prepared by embodiment 1.
Fig. 4 is the current -voltage curve of perovskite solar cell prepared by comparative example 1 of the present invention.
Fig. 5 is the stable state curve of output of perovskite solar cell prepared by comparative example 1 of the present invention.
Fig. 6 is the external quantum efficiency figure for the perovskite solar cell that example 1 of the present invention is prepared with comparative example 3.
Embodiment
For a better understanding of the present invention, with reference to the specific embodiment content that the present invention is furture elucidated, but this hair
Bright content is not limited solely to the following examples.
In following examples, the transparent conductive substrate used is 15 Ω, the electrically conducting transparent substrate I TO of patterning for sheet resistance,
There is provided by Shenzhen Nan Po companies.
Embodiment 1
A kind of perovskite solar cell, its structure is ITO/TiO2/PCBM/MAxFA1-xPbI3/Spiro-OMeTAD/Au
(structural representation is shown in Fig. 1), specific preparation process is as follows:
1) it is 15 Ω by sheet resistance, the electrically conducting transparent substrate I TO of patterning is successively in deionized water, ethanol, acetone, isopropanol
Middle ultrasonic cleaning 10min, is placed in thermal station after nitrogen drying and dries, and UV-ozone processing removal remained on surface is carried out afterwards to be had
Machine thing;
2) through step 1) pretreatment transparent conductive substrate on prepare electron transfer layer:Using titanium tetrachloride as presoma,
2.3ml titanium tetrachlorides are weighed under the conditions of ice-water bath to be sufficiently mixed with 8ml ethanol, and gained mixture is moved into 40ml phenmethylols,
9h is reacted under the conditions of 80 DEG C;By 3ml reaction products and ether with 1:9 volume ratio carries out washing of precipitate, and products therefrom is again
It is scattered in 8ml alcohol solvents, controls the mass concentration of nano-titania particle in 8mg/ml, is eventually adding and accounts for titanium dioxide and rub
The bis-acetylacetonate metatitanic acid diisopropyl ester of your amount 10% is well mixed to obtain nano titanium oxide dispersion as stabilizer, then will
Dispersion liquid most obtains electron transfer layer, thickness is 45nm through 130 DEG C of annealing 30min afterwards with 3000rpm rotating speed spin coating 40s;
3) using chlorobenzene be solvent compound concentration as 15mg/ml PCBM solution, with 1000rpm rotating speed in electron transfer layer
Upper progress spin coating 30s, then by 100 DEG C of annealing 15min, interface-modifying layer is obtained, thickness is 50nm;
4) modified perovskite active layer is prepared using two-step method, wherein the precursor solution used is by lead iodide and iodate first
Amidine presses 1.3:0.3 mol ratio, it is 9 to be dissolved in volume ratio:1 DMF and DMSO in the mixed solvent are formed, lead iodide and iodate
Carbonamidine shared total concentration in precursor solution is 650mg/ml;Iodate methylamine in the aqueous isopropanol of the iodate methylamine of use
Concentration is 35mg/ml;The mol ratio of iodate carbonamidine and iodate methylamine is 1:1.3;Specific preparation process is as follows:First by presoma
Solution is with 6000rpm rotating speed spin coating 15s, afterwards by iodate methylamine solution with 3500rpm rotating speed spin coating 45s, finally by institute
Obtain film and be heat-treated 30min under the conditions of 100 DEG C, obtain modified perovskite active layer, its thickness is 340nm;
5) spin coating hole transmission layer on modified perovskite active layer, is comprised the following steps that:By 80mg Spiro-OMeTAD,
(double (fluoroform) sulfimide lithium salts are 520mg/ to the acetonitrile solution of double (fluoroform) the sulfimide lithium salts of 17.5 μ L
Ml), 28.8 μ L tert .-butylpyridines are blended in 1ml chlorobenzene solvents, obtain hole transmission layer solution;Then by gained hole transmission layer
Solution carries out spin coating with 4000rpm rotating speed on modified perovskite active layer, is positioned over afterwards in drier and carries out staying overnight oxygen
Change to improve the electrical conductivity and mobility of hole transmission layer, obtain hole transmission layer, its thickness is 180nm;
6) Ag metal levels are deposited by metal mask plate and are used as anode, its thickness is 100nm, and the system of device is completed to electrode
It is standby, obtain the perovskite solar cell;
The perovskite solar cell that the present embodiment is prepared is tested, after tested (result is shown in Fig. 2 and Fig. 3),
The electricity conversion of perovskite solar cell is issued to 20.5% in anti-swepting slip part obtained by the present embodiment, its short circuit currents
Density is 23.2mA/cm2, open-circuit voltage 1.1V, fill factor, curve factor 80.5%, and device is without hysteresis, in maximum power point
Apply constant bias, device can stablize the efficiency value of output 20.2%.
Embodiment 2
A kind of perovskite solar cell, its structure is ITO/TiO2/PCBM/MAxFA1-xPbI3/Spiro-OMeTAD/Au
(structural representation is shown in Fig. 1), specific preparation process is as follows:
1) it is 15 Ω by sheet resistance, the electrically conducting transparent substrate I TO of patterning is successively in deionized water, ethanol, acetone, isopropanol
Middle ultrasonic cleaning 10min, is placed in thermal station after nitrogen drying and dries, and UV-ozone processing removal remained on surface is carried out afterwards to be had
Machine thing;
2) through step 1) pretreatment transparent conductive substrate on prepare electron transfer layer:Using titanium tetrachloride as presoma,
2ml and 8ml ethanol is weighed under the conditions of ice-water bath to be sufficiently mixed, and gained mixture is moved into 40ml phenmethylols, in 70 DEG C of conditions
Lower reaction 9h;By 3ml reaction products and ether with 1:9 volume ratio carries out washing of precipitate, and 7ml alcohol solvents are scattered in again,
Control the mass concentration of nano-titania particle in 10mg/ml, be eventually adding the biacetyl for accounting for titanium dioxide mole 12%
Acetone metatitanic acid diisopropyl ester is well mixed to obtain nano titanium oxide dispersion as stabilizer, then by dispersion liquid with 3000rpm's
Rotating speed spin coating 40s, most afterwards through 150 DEG C of annealing 30min, the thickness for obtaining electron transfer layer is 35nm;
3) using chlorobenzene be solvent compound concentration as 15mg/ml PCBM solution, with 1000rpm rotating speed in electron transfer layer
Upper progress spin coating 30s, then by 100 DEG C of annealing 30min, interface-modifying layer is obtained, thickness is 50nm;
4) modified perovskite active layer is prepared using two-step method, wherein the precursor solution used is by lead iodide and iodate first
Amidine presses 1.3:0.2 mol ratio, it is 8 to be dissolved in volume ratio:2 DMF and DMSO in the mixed solvent are formed, lead iodide and iodate
Carbonamidine shared total concentration in precursor solution is 700mg/ml;The aqueous isopropanol concentration of the iodate methylamine used is 40mg/
ml;The mol ratio of iodate carbonamidine and iodate methylamine is 1:1.2;Specific preparation process is as follows:First by precursor solution with
5000rpm rotating speed spin coating 20s, afterwards by iodate methylamine solution with 4000rpm rotating speed spin coating 50s, finally by gained film
20min is heat-treated under the conditions of 100 DEG C, modified perovskite active layer is obtained, its thickness is 360nm;
5) spin coating hole transmission layer on modified perovskite active layer, is comprised the following steps that:By 80mg Spiro-OMeTAD,
(double (fluoroform) sulfimide lithium salts are 520mg/ to the acetonitrile solution of double (fluoroform) the sulfimide lithium salts of 17.5 μ L
Ml), 28.8 μ L tert .-butylpyridines are blended in 1ml chlorobenzene solvents, obtain hole transmission layer solution;Then by gained hole transmission layer
Solution carries out spin coating with 3000rpm rotating speed on modified perovskite active layer, is positioned over afterwards in drier and carries out staying overnight oxygen
Change to improve the electrical conductivity and mobility of hole transmission layer, obtain hole transmission layer, its thickness is 200nm;
6) Au metal levels are deposited by metal mask plate and are used as anode, its thickness is 80nm, and the system of device is completed to electrode
It is standby, obtain the perovskite solar cell;
The perovskite solar cell that the present embodiment is prepared is tested, after tested perovskite obtained by the present embodiment
The electricity conversion of solar cell is issued to 20.1% in anti-swepting slip part, and wherein short-circuit current density is 23.0mA/cm2,
Open-circuit voltage 1.09V, fill factor, curve factor 80%, and device apply constant bias, device can without hysteresis in maximum power point
The efficiency value of stable output 19.8%.
Embodiment 3
A kind of perovskite solar cell, its structure is ITO/TiO2/PCBM/MAxFA1-xPbI3/Spiro-OMeTAD/Ag
(structural representation is shown in Fig. 1), specific preparation process is as follows:
1) it is 15 Ω by sheet resistance, the electrically conducting transparent substrate I TO of patterning is successively in deionized water, ethanol, acetone, isopropanol
Middle ultrasonic cleaning 15min, is placed in thermal station after nitrogen drying and dries, and UV-ozone processing removal remained on surface is carried out afterwards to be had
Machine thing;
2) through step 1) pretreatment transparent conductive substrate on prepare electron transfer layer:Using titanium tetrachloride as presoma,
2ml and 10ml ethanol is weighed under the conditions of ice-water bath to be sufficiently mixed, and gained mixture is moved into 50ml phenmethylols, in 90 DEG C of conditions
Lower reaction 8h;By 3ml reaction products and ether with 1:9 volume ratio carries out washing of precipitate, and 10ml alcohol solvents are scattered in again,
Control the mass concentration of nano-titania particle in 12mg/ml, be eventually adding the biacetyl for accounting for titanium dioxide mole 12%
Acetone metatitanic acid diisopropyl ester is well mixed to obtain nano titanium oxide dispersion as stabilizer, then by dispersion liquid with 3000rpm's
Rotating speed spin coating 40s, eventually passes 100 DEG C of annealing 30min, and the thickness for obtaining electron transfer layer is 45nm;
3) using chlorobenzene be solvent compound concentration as 15mg/ml PCBM solution, with 2000rpm rotating speed in electron transfer layer
Upper progress spin coating 20s, then through 100 DEG C of annealing 20min, interface-modifying layer is obtained, thickness is 35nm;
4) modified perovskite active layer is prepared using two-step method, wherein the precursor solution used is by lead iodide and iodate first
Amidine presses 1.3:0.3 mol ratio, it is 10 to be dissolved in volume ratio:1 DMF and DMSO in the mixed solvent are formed, lead iodide and iodine
It is 730mg/ml to change carbonamidine shared total concentration in precursor solution;The aqueous isopropanol concentration of the iodate methylamine used for
35mg/ml;The mol ratio of iodate carbonamidine and iodate methylamine is 1:1.4;Specific preparation process is as follows:First by precursor solution with
7000rpm rotating speed spin coating 15s, afterwards by iodate methylamine solution with 4000rpm rotating speed spin coating 45s, finally by gained film
20min is heat-treated under the conditions of 100 DEG C, modified perovskite active layer is obtained, its thickness is 330nm;
5) spin coating hole transmission layer on modified perovskite active layer, is comprised the following steps that:By 80mg Spiro-OMeTAD,
(double (fluoroform) sulfimide lithium salts are 520mg/ to the acetonitrile solution of double (fluoroform) the sulfimide lithium salts of 17.5 μ L
Ml), 28.8 μ L tert .-butylpyridines are blended in 1ml chlorobenzene solvents, obtain hole transmission layer solution;Then by gained hole transmission layer
Solution carries out spin coating with 5000rpm rotating speed on modified perovskite active layer, is positioned over afterwards in drier and carries out staying overnight oxygen
Change to improve the electrical conductivity and mobility of hole transmission layer, obtain hole transmission layer, its thickness is 160nm;
6) Ag metal levels are deposited by metal mask plate and are used as anode, its thickness is 150nm, and the system of device is completed to electrode
It is standby, obtain the perovskite solar cell;
The perovskite solar cell that the present embodiment is prepared is tested, after tested perovskite obtained by the present embodiment
The electricity conversion of solar cell is issued to 20.3% in anti-swepting slip part, and wherein short-circuit current density is 22.8mA/cm2,
Open-circuit voltage 1.1V, fill factor, curve factor 80.3%, and device apply constant bias, device without hysteresis in maximum power point
The efficiency value of output 20.1% can be stablized.
Comparative example 1
A kind of perovskite solar cell, it is prepared, and amplification is roughly the same with embodiment 1, and difference is delete step
3) interface-modifying layer, the structure of gained perovskite solar cell is ITO/TiO2/MAxFA1-xPbI3/Spiro-
OMeTAD/Au。
Perovskite solar cell obtained by this comparative example is tested into (result is shown in Fig. 4 and Fig. 5), after tested, this implementation
The electricity conversion for the solar cell that example is prepared is issued to 18.8% in anti-swepting slip part, and wherein short-circuit current density is
22.6mA/cm2, open-circuit voltage 1.1V, fill factor, curve factor 76%, device shows serious hysteresis, efficiency under the conditions of just sweeping
Only 13%, apply constant bias in maximum power point, device delivery efficiency constantly decays, therefore PCBM modifying interfaces can be eliminated effectively
The hysteretic properties of device, improves the stable output performance of device.
Comparative example 2
A kind of perovskite solar cell, its preparation method is roughly the same with embodiment 1, and difference is step 2) in
The preparation process of the electron transfer layer is:Commercially available titanium tetraisopropylate solution is scattered in into isopropanol solvent, and to prepare presoma molten
Liquid, then with 3000rpm rotating speed spin coating 40s, then through 500 DEG C of annealing 30min.
Perovskite solar cell prepared by this comparative example is tested, and as a result shows the photoelectric conversion of solar cell
Efficiency is issued to 18.6% in anti-swepting slip part, and wherein short-circuit current density is 22.5mA/cm2, open-circuit voltage 1.08V, filling because
Son 77%, device is without obvious hysteresis after fullerene modifying interface, and efficiency is 18.7% under the conditions of just sweeping, therefore low temperature preparation
TiO2Electron transfer layer is prepared relative to high temperature can not only effectively simplify process, and performance is more excellent.
Comparative example 3
A kind of perovskite solar cell, its preparation method is roughly the same with embodiment 1, and difference is step 2) in
The preparation process of the perovskite is:Perovskite active layer is prepared using traditional two-step method, wherein the precursor solution used
1.3 are pressed by lead iodide and iodate methylamine:0.3 mol ratio, it is 9 to be dissolved in volume ratio:1 DMF and DMSO in the mixed solvent
Form, the shared total concentration in precursor solution is 650mg/ml to lead iodide with iodate methylamine;The isopropyl of the iodate methylamine of use
Alcoholic solution concentration is 35mg/ml;Specific preparation process is as follows:First by precursor solution with 7000rpm rotating speed spin coating 15s,
Gained film is finally heat-treated by iodate methylamine solution with 4000rpm rotating speed spin coating 45s under the conditions of 100 DEG C afterwards
20min, obtains perovskite active layer, and its thickness is 330nm, obtains device architecture for ITO/TiO2/CH3NH3PbI3/Spiro-
OMeTAD/Ag。
Perovskite solar cell prepared by this comparative example is tested, and as a result shows the photoelectric conversion of solar cell
Efficiency is issued to 19.6% in anti-swepting slip part, and wherein short-circuit current density is 22.5mA/cm2, open-circuit voltage 1.09V, filling because
Son 80%, device is without obvious hysteresis after fullerene modifying interface, and efficiency is 19.4% under the conditions of just sweeping, from the outer of Fig. 6
It can be apparent from quantum efficiency collection of illustrative plates, the perovskite device prepared using FAI is divided than individually being had using the device of MAI preparations
The broader light absorption range of cloth, therefore use bigger molecule FAI parts to substitute MAI, it can effectively widen light absorption range and improve photoelectricity turn
Change efficiency, obtain more excellent device performance.
Above example is only the preferred embodiment of the present invention, it is noted that to those skilled in the art,
Do not depart under the premise of raw material of the present invention, made some improvement also should be regarded as protection scope of the present invention.
Claims (10)
1. a kind of perovskite solar cell, it is characterised in that it includes transparent conductive substrate, electron transfer layer, interface successively
Decorative layer, modified perovskite active layer, hole transmission layer and anode;Wherein, the electron transfer layer is nano titanium oxide grain
Sublayer, interface-modifying layer is fullerene derivate layer.
2. perovskite solar cell according to claim 1, it is characterised in that the nano-titania particle layer
Preparation method comprises the following steps:Under the conditions of ice-water bath, titanium tetrachloride and ethanol are sufficiently mixed uniformly, benzene first is then added
In alcohol, 8~10h is reacted under the conditions of 70~80 DEG C, is precipitated, washed using ether, products therefrom is scattered in ethanol again
In solvent, control the mass concentration of nano-titania particle in 8~12mg/ml, be eventually adding titanium chelate and obtain nano-silica
Change titanium dispersion liquid, then spin-coated, Low Temperature Heat Treatment obtains the TiO 2 particles layer.
3. perovskite solar cell according to claim 2, it is characterised in that the titanium tetrachloride, ethanol, phenmethylol
Volume ratio be 1:(3.4~5):(17~25).
4. perovskite solar cell according to claim 2, it is characterised in that the titanium chelate is bis-acetylacetonate
Metatitanic acid diisopropyl ester, its mol ratio with nano titanium oxide is 1:(8~12).
5. perovskite solar cell according to claim 2, it is characterised in that the low temperature heat-treatment process is:Plus
Hot to 120~160 DEG C 15~40min of annealing.
6. according to the perovskite solar cell described in claim 1, it is characterised in that the thickness of the electron transfer layer is
30~50nm.
7. according to the perovskite solar cell described in claim 1, it is characterised in that the modified perovskite active layer uses two
Footwork prepare, wherein the precursor solution used by lead iodide and iodate carbonamidine by 1.3:The mol ratio of (0.2~0.4), dissolving
In volume ratio be (7~10):1 DMF and DMSO in the mixed solvent are formed, and lead iodide and iodate carbonamidine are in precursor solution
Shared total concentration is 650~750mg/ml;The aqueous isopropanol concentration of the iodate methylamine used is 30~50mg/ml;Iodate first
The mol ratio of amidine and iodate methylamine is 1:(1.2~1.5);Specific preparation process is as follows:First by precursor solution with 5000~
7000rpm rotating speed 10~20s of spin coating, afterwards by the aqueous isopropanol of iodate methylamine with 3000~4500rpm rotating speed spin coating
30~50s, is finally heat-treated 20~40min by gained film under the conditions of 90~110 DEG C, obtains modified perovskite active layer.
8. according to the perovskite solar cell described in claim 1, it is characterised in that the thickness of described fullerene derivate layer
For 40~60nm.
9. according to the perovskite solar cell described in claim 1, it is characterised in that the hole transport layer material be lithium salts and
Tert .-butylpyridine doping improved 2,2', the fluorenes Spiro- of 7,7'- tetra- [N, N- bis- (4- methoxyphenyls) amino] -9,9'- spiral shells two
OMeTAD。
10. the preparation method of any one of the claim 1~9 perovskite solar cell, it is characterised in that including following step
Suddenly:
1) transparent conductive substrate is cleaned, pre-processed;
2) through step 1) pretreatment transparent conductive substrate on prepare electron transfer layer:Nano titanium oxide dispersion is prepared, then
Spin-coated, Low Temperature Heat Treatment obtains nano-titania particle layer;
3) spin coating fullerene derivate solution on the electron transport layer, then carries out annealing and prepares interface-modifying layer;
4) modified perovskite active layer is prepared using two-step method;
5) spin coating hole transmission layer and it is dried on modified perovskite active layer;
6) anode material is deposited on hole transmission layer, the perovskite solar cell is produced.
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