CN106410032A - Flexible perovskite solar cell with metal grid graphene composite electrode and preparation method thereof - Google Patents
Flexible perovskite solar cell with metal grid graphene composite electrode and preparation method thereof Download PDFInfo
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- CN106410032A CN106410032A CN201610722923.7A CN201610722923A CN106410032A CN 106410032 A CN106410032 A CN 106410032A CN 201610722923 A CN201610722923 A CN 201610722923A CN 106410032 A CN106410032 A CN 106410032A
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- H—ELECTRICITY
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- H—ELECTRICITY
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- H10K30/00—Organic devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation
- H10K30/80—Constructional details
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- H10K30/82—Transparent electrodes, e.g. indium tin oxide [ITO] electrodes
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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
- H10K30/80—Constructional details
- H10K30/81—Electrodes
- H10K30/82—Transparent electrodes, e.g. indium tin oxide [ITO] electrodes
- H10K30/83—Transparent electrodes, e.g. indium tin oxide [ITO] electrodes comprising arrangements for extracting the current from the cell, e.g. metal finger grid systems to reduce the serial resistance of transparent electrodes
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
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Abstract
The invention belongs to the field of semiconductor photo-electronic devices and particularly relates to a flexible perovskite solar cell with a metal grid graphene composite electrode and a preparation method thereof. The flexible perovskite solar cell with the metal grid graphene composite electrode sequentially comprises a flexible substrate, a metal grid graphene composite photo-electrode, a first carrier transporting layer, a perovskite light absorption layer, a second carrier transporting layer and a back electrode. The metal grid graphene composite photo-electrode is a composite electrode structure which is composed of an embedded metal grid and graphene; the grid structure is a regular triangle, a regular quadrangle or a regular hexagon. The solar cell structure has the advantages of being flexible, light, thin, low in cost, high in efficiency and etc.; various products can be developed by utilizing the flexibility of the solar cell, so that the flexible perovskite solar cell with the metal grid graphene composite electrode is more diversified in application; meanwhile, a road is opened up for adoption of a large-batch and large-area reel-to-reel technology, and a new idea is provided for final commercialization of perovskite.
Description
Technical field
The invention belongs to semiconductor photoelectronic device field is and in particular to a kind of flexibility is frivolous, high efficiency, low cost flat
Face hetero-junctions perovskite solaode and its preparation.
Background technology
With the nonrenewable resources increasingly depleted such as coal, oil and natural gas, new forms of energy particularly solaode becomes
A focus for domestic and international research concern.Traditional silion cell comparatively high cost, dye-sensitized cell is in preparation skill
A lot of restrictions are had on art, although and the simple stability extreme difference of organic solar batteries battery structure, therefore, they are in industry
A lot of problems are also existed on change.Since perovskite solaode was reported for the first time from 2009, with its Ultra Low Cost solwution method
Preparation technology and favored by research worker, energy conversion efficiency has risen to 20.2% by initial 3.8%, with research
Deepen continuously, the efficiency of battery very likely exceedes monocrystaline silicon solar cell full-fledged at present.Perovskite solar energy
Battery finally can directly make hull cell again from initial one layer of porous layer support of needs, also has in industrialized production
There is very big application prospect.Meanwhile, to be prepared on a large scale method compatible for the rotary coating solwution method technique of employing and volume to volume,
Make fabulous place mat for industrialization.
Rigid perovskite solaode is thick and heavy, volume is big, can not be with volume to volume process compatible.And, some special
In application, need solaode to be curved or even folds.Therefore, the research and development of flexible perovskite solaode become
Obtain abnormal important, limited by flexible and transparent conductive substrate, the temperature in flexible perovskite cell manufacturing process not can exceed that
150 DEG C, so needing the meso-hole structure of high temperature sintering to be not appropriate for the exploitation of flexible perovskite solaode.Meanwhile, tradition
ITO, FTO optoelectronic pole flexibility extreme difference, flexible good, Graphene that high transmission rate, good conductivity, work function coupling, stability are strong
It is a kind of fabulous flexible transparent electrode, but the sheet resistance of Graphene is higher, single-layer graphene sheet resistance is higher than 100 Ω/.
Content of the invention
In view of this, higher in order to solve the problems, such as Graphene sheet resistance, it is an object of the invention to provide a kind of wire netting
Lattice graphene combination electrode flexibility perovskite solaode and preparation method thereof, reduces Graphene sheet resistance using composite construction,
Ensure high light transmittance simultaneously.
To achieve these goals, the invention provides a kind of metal grill graphene combination electrode flexibility the perovskite sun
Energy battery, specifically includes：Flexible substrate, metal grill Graphene complex light electrode, carrier blocking layers one, perovskite extinction
Layer, carrier blocking layers two, back electrode.Carrier blocking layers one, carrier blocking layers two are respectively hole transmission layer and electronics
One kind of transport layer, and different.
Further, described flexible substrate is PET, PEN etc..
Further, the combination electrode knot of described metal grill Graphene composite photoelectric extremely metal grill and Graphene composition
Structure, metal grill is embedded, and network is equilateral triangle, square or regular hexagon.
Further, in described combined electrode structure, metal material is Ag, and Graphene is graphene film, oxidoreduction stone
One of black alkene (RGO).
Further, coated UV solidified resin in described flexible substrate, is carried out to it using photoetching or nano-imprint process
Graphically, unnecessary ink is finally wiped off by filler metal ink in groove, forms embedded metal network.Using change
Learn vapour deposition process (CVD) to prepare graphene film and transfer them on metal grill, form composition metal grid graphite
Alkene complex light electrode.
Further, described ultraviolet curable resin thickness is 1-20um, preferably 5-8um.
Further, described combination electrode light transmittance is higher than 80%, and square resistance is less than 50 Ω/.
Further, described hole mobile material includes：PEDOT:PSS, spiro-OMeTAD, PTAA, thickness is about：40-
100 nanometers.Electron transport material includes：PCBM、TiO2Or ZnO, thickness about 30-200 nanometer.Perovskite light-absorption layer includes
MAI/PbI2Or MAI/PbI2/PbCl2System, thickness is 100-500 nanometer.Functional layer is all prepared using solwution method.
Further, described solwution method includes：Rotary coating, doctor blade method, slot coated, inkjet printing etc..
Further, described back electrode is obtained by thermal resistance evaporation, and including Al, Ag or Au, thickness is 100-200 nanometer.
The preparation method of above-mentioned metal grill graphene combination electrode flexibility perovskite solaode, walks including following
Suddenly：
(1) coated UV solidified resin in flexible substrate, is patterned to it using photoetching or nano-imprint process, knot
Structure is equilateral triangle, square or regular hexagon, filler metal ink in groove, finally wipes unnecessary ink off, is formed
Embedded metal network.Prepare graphene film and transfer them to metal grill using chemical vapour deposition technique (CVD)
On, form composition metal grid Graphene complex light electrode.Subsequently, carry out hydrophilic using UV ozone machine to its surface to change
Conduct oneself well reason；
(2) carrier blocking layers one, extinction are sequentially prepared on metal grill Graphene complex light electrode using solwution method
Layer, carrier blocking layers two, prepare carrier blocking layers one, the preparation of light-absorption layer and carrier blocking layers two in super-clean environment
It is below in the glove box of 1ppm carrying out in water oxygen content；
(3) substrate preparing is put into rapidly in vacuum coating equipment, plated film forms back electrode, completes the preparation of device.
Brief description
In order that the object, technical solutions and advantages of the present invention are clearer, below in conjunction with accompanying drawing the present invention is made into
The detailed description of one step, wherein：
Fig. 1 is the metal grill graphene combination electrode flexibility perovskite solar battery structure schematic diagram of the present invention；Its
In, 101 is flexible substrate, and 102 is metal grill graphene combination electrode, and 103 is carrier blocking layers one, and 104 is perovskite
Light-absorption layer, 105 is carrier blocking layers two, and 106 is back electrode.
Fig. 2 is metal grill graphene combination electrode structural representation；Wherein, 201 is embedded metal grid, and 202 are
Graphene.
Specific embodiment
Below in conjunction with the accompanying drawings the specific embodiment of the present invention is elaborated, make those skilled in the art to the present invention
Have deeper into understanding.
Embodiment one
Structure such as Fig. 1 institute based on metal grill graphene combination electrode flexibility perovskite solaode of the present embodiment
Show, the preparation method step based on metal grill graphene combination electrode flexibility perovskite solaode for the present embodiment is as follows:
1. prepare metal grill 201：Coated UV solidified resin 7um in flexible substrate 101PET, using nano impression
Technique is patterned to it, square nickel mold is obtained by electroforming, and its length of side is 80um, and width is 2um, is highly
1um.Under ultraviolet light, imprint, using nickel mold (0.25g pressure), the resin obtaining there is square groove structure, in groove
Unnecessary ink is finally wiped off, so that groove is completely filled in triplicate by filling Ag ink.Form Embedded A g grid knot
Structure.
2. single-layer graphene film 202 is prepared on Copper Foil using chemical vapour deposition technique (CVD), and transfer them to gold
Belong on grid, form composition metal grid Graphene complex light electrode 102.Combination electrode light transmittance is 86%, square resistance
For 35 Ω/, bend 1000 power resistiveizations 3%.
3. prepare functional layer 103,104,105, in super-clean environment, using UV ozone machine, hydrophilic is carried out to its surface
Improvement is processed, empty improving spin coating preparation 30nm on the composition metal grid Graphene complex light electrode processing through hydrophilic
Cave transport layer 103 PEDOT:PSS AI4083.Substrate is transferred to water oxygen content be below in the glove box of 1ppm, spin coating system
Standby light-absorption layer 104 CH3NH3PbI3With electron transfer layer 105 PCBM, by 1:The MAI/PbI of 1 mol ratio2It is dissolved in DMF and formed
The CH of 40wt%3NH3PbI3Precursor solution, heats 30 minutes under 60 degree, adds 100ul HI in 1ml perovskite solution,
By the 70 degree of heating of perovskite presoma, rotary coating 200 seconds under the rotating speed of 3000RPM, annealing 2 minutes under 100 degree, formed thick
Degree is about the light-absorption layer of 300nm.PCBM is dissolved in chlorobenzene, is made into the solution of 20mg/ml, be obtained under the rotating speed of 3000RPM
Thickness is about the electron transfer layer of 50nm.
4. substrate is transferred to thermal resistance evaporation coating machine cavity room, is deposited with 100nm Al electrode 106, completes the preparation of device.
The efficiency of battery is 13%, bends the photoelectric transformation efficiency change 5% of battery after 1000 times.
Embodiment two
Structure such as Fig. 1 institute based on metal grill graphene combination electrode flexibility perovskite solaode of the present embodiment
Show, the preparation method step based on metal grill graphene combination electrode flexibility perovskite solaode for the present embodiment is as follows:
1. prepare metal grill 201：Coated UV solidified resin 7um in flexible substrate 101PET, using nano impression
Technique is patterned to it, regular hexagon nickel mold is obtained by electroforming, and its diagonal is 90um, and width is 4um, is highly
2um.Under ultraviolet light, imprint, using nickel mold (0.25g pressure), the resin obtaining there is regular hexagon groove structure, in groove
Unnecessary ink is finally wiped off, so that groove is completely filled in triplicate by filling Ag ink.Form Embedded A g grid knot
Structure.
2. spin coating preparation oxidoreduction Graphene (RGO) 202, forms composition metal grid Graphene complex light electrode 102.
Combination electrode light transmittance is 88%, and square resistance is 46 Ω/, bends 1000 power resistiveizations 2%.
3. prepare functional layer 103,104,105, in super-clean environment, prepare 5.3%ZnO Nano sol, 2000rpm rotating speed
Under through UV ozone surface hydrophilicity improve process composition metal grid Graphene complex light electrode on spin coating preparation
ZnO electron transfer layer 103, is dried 10min under 150 degree, obtains the thick nano thin-film of 40nm.Substrate is transferred to water oxygen content
It is below in the glove box of 1ppm, spin coating is obtained light-absorption layer 104 CH3NH3PbI3With hole transmission layer 105 PTAA, by 1:1 rubs
The MAI/PbI of your ratio2It is dissolved in the CH forming 40wt% in DMF3NH3PbI3Precursor solution, heats 30 minutes under 60 degree,
100ul HI is added, by the 70 degree of heating of perovskite presoma, rotary coating under the rotating speed of 3000RPM in 1ml perovskite solution
200 seconds, made annealing treatment under 100 degree, formed the light-absorption layer that thickness is about 300nm.Under 3000rpm rotating speed, rotary coating adds
There is the PTAA solution of Li-TFSI and t-BP, form the thick hole transmission layer of 50nm.
4. substrate is transferred to thermal resistance evaporation coating machine cavity room, is deposited with 60nm Au electrode 106, completes the preparation of device.Electricity
The efficiency in pond is 11%, bends the photoelectric transformation efficiency change 4% of battery after 1000 times.
Embodiment three
Structure such as Fig. 1 institute based on metal grill graphene combination electrode flexibility perovskite solaode of the present embodiment
Show, the preparation method step based on metal grill graphene combination electrode flexibility perovskite solaode for the present embodiment is as follows:
1. prepare metal grill 201：Coated UV solidified resin 7um in flexible substrate 101PEN, using photoetching process
It is patterned, under ultraviolet light, obtains the resin with equilateral triangle groove structure, its length of side is 100um, width is
2um, highly for 1um.Fill Ag ink in groove, finally unnecessary ink is wiped off, so that groove is filled out completely in triplicate
Fill.Form Embedded A g network.
2. single-layer graphene film 202 is prepared on Copper Foil using chemical vapour deposition technique (CVD), and transfer them to gold
Belong on grid, form composition metal grid Graphene complex light electrode 102.Combination electrode light transmittance is 82%, square resistance
For 26 Ω/, bend 1000 power resistiveizations 3%.
3. it is sequentially prepared functional layer 103,104,105, in super-clean environment, using spraying high-temperature decomposition preparation 30nm
TiO2 electron transfer layer 103.Substrate is transferred to water oxygen content be below in the glove box of 1ppm, spin coating is obtained light-absorption layer 104
CH3NH3PbI3-XClXWith hole transmission layer 105 spiro-OMeTAD, CH3NH3PbI3-XClXBy 0.08M PbCl2、0.97M
PbI2Being dissolved in volume ratio with 1M MAI is 3:In 7 DMSO/GBL mixed organic solvents, by the 70 degree of heating of perovskite presoma, revolve
Painting condition is first step 1000RPM (20 seconds), second step 5500RPM (60 seconds), is extracted with 160ul dry toluene when 40 seconds
Take, obtain the perovskite thin film of smooth surface, anneal 20 minutes under 100 degree, form the light-absorption layer that thickness is about 260nm.Rotation
Apply the spiro-OMeTAD solution added with Li-TFSI and t-BP for the preparation, form the thick hole transmission layer of 180nm.
4. substrate is transferred to thermal resistance evaporation coating machine cavity room, is deposited with 70nm Ag electrode 106, completes the preparation of device.Electricity
The efficiency in pond is 12%, bends the photoelectric transformation efficiency change 4% of battery after 1000 times.
Finally illustrate, above example only in order to technical scheme to be described and unrestricted, although with reference to relatively
Good embodiment has been described in detail to the present invention, it will be understood by those within the art that, can be to the skill of the present invention
Art scheme is modified or equivalent, the objective without deviating from technical solution of the present invention and scope, and it all should be covered at this
In the middle of the right of invention.
Claims (9)
1. a kind of metal grill graphene combination electrode flexibility perovskite solaode it is characterised in that：This device is from lower past
On include successively：Flexible substrate, metal grill Graphene complex light electrode, carrier blocking layers one, perovskite light-absorption layer, current-carrying
Sub- transport layer two, back electrode.Wherein, the compound electric of metal grill Graphene composite photoelectric extremely metal grill and Graphene composition
Pole structure, metal grill is embedded, and network is equilateral triangle, square or regular hexagon.Carrier blocking layers one,
Carrier blocking layers two are respectively one kind of hole transmission layer and electron transfer layer, and different.
2. metal grill graphene combination electrode flexibility perovskite solaode according to claim 1, its feature exists
In：Described flexible substrate is PET, PEN etc..In metal grill Graphene complex light electrode, metal material is Ag, and Graphene is stone
One of black alkene thin film, oxidoreduction Graphene (RGO).Hole mobile material includes：PEDOT:PSS、spiro-OMeTAD
Or PTAA, electron transport material includes：PCBM、TiO2Or ZnO, perovskite light-absorption layer includes MAI/PbI2Or MAI/PbI2/
PbCl2System.
3. metal grill graphene combination electrode flexibility perovskite solaode according to claim 1, its feature exists
In：Coated UV solidified resin in flexible substrate, is patterned to it using photoetching or nano-imprint process, fills in groove
Unnecessary ink is finally wiped off by metallic ink, forms embedded metal network.
4. metal grill graphene combination electrode flexibility perovskite solaode according to claim 1, its feature exists
In：Graphene film is prepared using chemical vapour deposition technique (CVD) and transfers them on metal grill, form composition metal
Grid Graphene complex light electrode.
5. metal grill graphene combination electrode flexibility perovskite solaode according to claim 4, its feature exists
In：The light transmittance of described metal grill Graphene complex light electrode is higher than 80%, and square resistance is less than 50 Ω/.
6. metal grill graphene combination electrode flexibility perovskite solaode according to claim 1, its feature exists
In：Carrier blocking layers one, perovskite light-absorption layer, carrier blocking layers two are sequentially prepared using solwution method.
7. metal grill graphene combination electrode flexibility perovskite solaode according to claim 6, its feature exists
In：Described solwution method includes：Rotary coating, spraying high-temperature decomposition.
8. metal grill graphene combination electrode flexibility perovskite solaode according to claim 1, its feature exists
In：Described back electrode is obtained by thermal resistance evaporation, including Al, Ag or Au.
9. a kind of preparation method of metal grill graphene combination electrode flexibility perovskite solaode is it is characterised in that wrap
Include following steps：
Coated UV solidified resin in flexible substrate, is patterned to it using photoetching or nano-imprint process, and structure is just
Triangle, square or regular hexagon, filler metal ink in groove, finally unnecessary ink is wiped off, formed embedded
Metal mesh structure.Graphene film is prepared using chemical vapour deposition technique (CVD) and transfers them on metal grill, shape
Become composition metal grid Graphene complex light electrode.Subsequently, using UV ozone machine, its surface is carried out with hydrophilic improvement process.
Carrier blocking layers one, light-absorption layer, current-carrying are sequentially prepared on metal grill Graphene complex light electrode using solwution method
Sub- transport layer two, prepares carrier blocking layers one, the preparation of light-absorption layer and carrier blocking layers two is in water oxygen in super-clean environment
Content is below carrying out in the glove box of 1ppm；The substrate preparing is put into rapidly in vacuum coating equipment, plated film forms back of the body electricity
Pole, completes the preparation of device.
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Cited By (11)
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| CN108425425A (en) * | 2018-01-25 | 2018-08-21 | 苏坤 | Sponge city catchment disappear big vast regulator control system and regulation and control method |
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| CN109888107A (en) * | 2019-03-06 | 2019-06-14 | 杭州众能光电科技有限公司 | A kind of perovskite solar components and preparation method thereof |
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| CN108425425A (en) * | 2018-01-25 | 2018-08-21 | 苏坤 | Sponge city catchment disappear big vast regulator control system and regulation and control method |
| CN108963082A (en) * | 2018-06-07 | 2018-12-07 | 华中科技大学鄂州工业技术研究院 | A kind of embedding grid type perovskite mould group and preparation method thereof |
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| CN111525032A (en) * | 2020-04-06 | 2020-08-11 | 杭州纤纳光电科技有限公司 | Two-dimensional mesh back contact type perovskite solar cell and preparation method thereof |
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| CN111653667B (en) * | 2020-05-19 | 2022-12-02 | 深圳大学 | Flexible photodetector and preparation method and application thereof |
| CN112420931A (en) * | 2020-11-27 | 2021-02-26 | 江苏集萃分子工程研究院有限公司 | Composite structure back electrode for perovskite solar cell |
| CN114171706A (en) * | 2021-12-08 | 2022-03-11 | 深圳市华星光电半导体显示技术有限公司 | Cathode, flexible organic light emitting diode and preparation method thereof |
| CN114171706B (en) * | 2021-12-08 | 2024-02-13 | 深圳市华星光电半导体显示技术有限公司 | Cathode, flexible organic light-emitting diode and preparation method thereof |
| CN116496658A (en) * | 2022-01-20 | 2023-07-28 | 中国科学院苏州纳米技术与纳米仿生研究所 | Crystalline amorphous hybrid zinc oxide nanoparticle ink, preparation method and application |
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