CN105845829B - A kind of perovskite solar battery - Google Patents

A kind of perovskite solar battery Download PDF

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CN105845829B
CN105845829B CN201610190114.6A CN201610190114A CN105845829B CN 105845829 B CN105845829 B CN 105845829B CN 201610190114 A CN201610190114 A CN 201610190114A CN 105845829 B CN105845829 B CN 105845829B
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zinc oxide
single crystal
oxide single
electron
heteroatom doping
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CN105845829A (en
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黄丰
刘渊
郑伟
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Fujian Institute of Research on the Structure of Matter of CAS
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    • H10K30/00—Organic devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation
    • H10K30/451—Organic devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation comprising a metal-semiconductor-metal [m-s-m] structure
    • H—ELECTRICITY
    • H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
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    • H10K71/10—Deposition of organic active material
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Abstract

This application discloses a kind of perovskite solar batteries, including electron-transport substrate, perovskite photoactive layer, hole transmission layer and to electrode, it is characterized in that, the electron-transport substrate is selected from Zinc oxide single crystal, the Heteroatom doping Zinc oxide single crystal that Heteroatom doping Zinc oxide single crystal, the Zinc oxide single crystal of micro-structure is contained on surface, micro-structure is contained on surface.The perovskite solar battery, by directlying adopt the Zinc oxide single crystal of Zinc oxide single crystal, Heteroatom doping or using the Zinc oxide single crystal of chemical vapor deposition, sputtering method, the processed Zinc oxide single crystal of ion etching or Heteroatom doping as electron-transport substrate, light transmitting electro-conductive is had both simultaneously and electron-transport collects the function of electronics, reduce the number of plies of battery, the structure for greatlying simplify perovskite solar battery, optimizes preparation process.

Description

A kind of perovskite solar battery
Technical field
This application involves a kind of perovskite solar batteries, belong to technical field of microelectronic devices.
Background technique
With the increasingly consumption of non-renewable energy resources in world wide, energy shortage and environmental degradation have become the new century The more serious problem that the mankind are faced.Development and utilization cleaning renewable new energy is increasingly paid attention to by people.Solar energy Exactly one of green, cleaning, renewable energy, it is inexhaustible, it is potential to become in future source of energy supply Important component.As the solar battery of electrooptical device, its research and application has been subjected to more and more weight Depending on.
Perovskite hybrid perovskite material ABX used for solar batteries3As photoactive layer, with traditional silicon Based solar battery is compared, it has again, and low in cost, the absorption coefficient of light is high, carrier diffusion length is big, quality is light, flexibility The advantages that good.With deepening continuously for domestic and international correlative study in recent years, perovskite solar battery mainly uses mesoporous knot Two kinds of structures of structure and planar heterojunction, the photoelectric conversion efficiency and stability of perovskite solar battery are constantly promoted.
Usually require to choose suitable transparent conductive material in efficient perovskite solar battery structure as substrate, There are commonly the FTO electro-conductive glass (SnO of doping fluorine2Transparent conducting glass, referred to as FTO), ITO is (in sodium calcium base or silicon boryl On the basis of substrate glass, indium oxide layer tin film is plated using a variety of methods such as sputtering, evaporations and is manufactured, abbreviation ITO) Deng；It also needs to prepare suitable electron transfer layer on substrate basis to conduct electronics at the same time, there are commonly titanium dioxides Titanium, zinc oxide, tin oxide etc..In general, the preparation of these electron transfer layers is needed by first spin coating precursor solution on substrate, Then the process for carrying out high temperature sintering again could be formed, both time- and labor-consuming in this way, while increase the structure of battery, preparation step It is rapid cumbersome.
Summary of the invention
According to the one aspect of the application, provide a kind of perovskite solar battery, by directly adopt Zinc oxide single crystal, The Zinc oxide single crystal of Heteroatom doping or using chemical vapor deposition, sputtering method, the processed Zinc oxide single crystal of ion etching or The Zinc oxide single crystal of Heteroatom doping has both the function of light transmitting electro-conductive and electron-transport collection electronics as electron-transport substrate Can, instead of in the prior art using transparent conductive materials+electron transfer layer TiO such as ITO or FTO2Or SnO2Structure, reduce The number of plies of battery, largely simplifies the structure of perovskite solar battery, eliminates cumbersome preparation process.
The perovskite solar battery, including electron-transport substrate, perovskite photoactive layer, hole transmission layer and to electricity Pole, which is characterized in that the electron-transport substrate contains micro- selected from Zinc oxide single crystal, Heteroatom doping Zinc oxide single crystal, surface The Zinc oxide single crystal of structure, surface contain the Heteroatom doping Zinc oxide single crystal of micro-structure.
The Zinc oxide single crystal, Heteroatom doping Zinc oxide single crystal, the Zinc oxide single crystal of micro-structure is contained on surface, surface contains The crystal structure for having the Heteroatom doping Zinc oxide single crystal of micro-structure is hexagonal wurtzite structure.
The perovskite photoactive layer includes the light active material of perovskite type crystal structure, such as has perovskite crystal form (ABX3) organic metal halide light absorbent, such as lead iodide methylamine CH3NH3PbI3。
Preferably, the hetero atom in the Heteroatom doping Zinc oxide single crystal in group III A metallic element at least It is a kind of.It is further preferred that the hetero atom in the Heteroatom doping Zinc oxide single crystal is aluminium and/or gallium.
Preferably, the Heteroatom doping Zinc oxide single crystal is selected from gallium-doped zinc oxide monocrystalline (being abbreviated as GZO) or mixes aluminium Zinc oxide single crystal (is abbreviated as AZO).
Preferably, the Zinc oxide single crystal and surface that micro-structure is contained on the surface contain the Heteroatom doping oxidation of micro-structure Micro-structure in zinc monocrystalline is micrometer structure and/or nanostructure.
Preferably, the micrometer structure and/or nanostructure pass through in Zinc oxide single crystal surface or Heteroatom doping oxidation Ion etching is carried out on zinc single-crystal surface to obtain.
Preferably, the micrometer structure and/or nanostructure pass through in Zinc oxide single crystal surface or Heteroatom doping oxidation The oxidation with micrometer structure and/or nanostructure is formed using vapour deposition process and/or magnetron sputtering method on zinc single-crystal surface Zinc, the Heteroatom doping zinc oxide with micrometer structure and/or nanostructure, the oxygen with micrometer structure and/or nanostructure Change at least one of titanium, tin oxide with micrometer structure and/or nanostructure to obtain.
The Zinc oxide single crystal and surface that micro-structure is contained on the surface contain the Heteroatom doping Zinc oxide single crystal of micro-structure Micrometer structure and nanostructure can be contained simultaneously.
As a kind of embodiment, the Zinc oxide single crystal that micro-structure is contained on the surface is the oxygen that nanostructure is contained on surface When changing zinc monocrystalline, the Zinc oxide single crystal of nanostructure is contained by using vapour deposition process on Zinc oxide single crystal surface in surface And/or magnetron sputtering method forms the zinc oxide with nanostructure, the Heteroatom doping zinc oxide with nanostructure, has and receive At least one of the rice titanium oxide of structure, tin oxide with nanostructure obtain.
As a kind of embodiment, the Heteroatom doping Zinc oxide single crystal that micro-structure is contained on the surface is that surface is contained and received When the Heteroatom doping Zinc oxide single crystal of rice structure, the Zinc oxide single crystal that nanostructure is contained on surface passes through in Heteroatom doping oxygen Change the zinc oxide on zinc single-crystal surface using vapour deposition process and/or magnetron sputtering method formation with nanostructure, there is nanometer At least one of the Heteroatom doping zinc oxide of structure, the titanium oxide with nanostructure, tin oxide with nanostructure It obtains.
Preferably, the micrometer structure is selected from micro wire, micron ball, micron chip, micron wall, micro-flowers, micro belt, micron At least one of pipe, micron bar, micron membranes.
Preferably, the nanostructure is selected from nano wire, nanosphere, nanometer sheet, nm wall, nano flower, nanobelt, nanometer At least one of pipe, nanometer rods, nanometer film.
According to the another aspect of the application, a kind of preparation method of perovskite solar battery is provided, which is characterized in that packet Include following steps:
S1 provides electron-transport substrate；
S2 forms perovskite photoactive layer in the top of the electron-transport substrate；
S3 forms hole transmission layer in the top of the perovskite photoactive layer；And
S4, on the hole transport layer rectangular paired electrode.
As an implementation, the preparation method of perovskite solar battery, which is characterized in that by following steps group At:
S1 provides electron-transport substrate；
S2 forms perovskite photoactive layer in the top of the electron-transport substrate；
S3 forms hole transmission layer in the top of the perovskite photoactive layer；And
S4, on the hole transport layer rectangular paired electrode.
Electron-transport substrate described in step S1 uses Zinc oxide single crystal；Or
Electron-transport substrate uses Heteroatom doping Zinc oxide single crystal；Or
Electron-transport substrate uses Zinc oxide single crystal-nano-zinc oxide composite material, and the Zinc oxide single crystal-is nano oxidized Zinc composite material by carrying out chemical vapor deposition formation on Zinc oxide single crystal surface there is the zinc oxide film of nanostructure to obtain It arrives；Or
Electron-transport substrate uses Zinc oxide single crystal-micron zinc oxide composite, the Zinc oxide single crystal-micron oxidation Zinc composite material is obtained by carrying out ion etching formation micrometer structure on Zinc oxide single crystal surface；Or
Electron-transport substrate uses Heteroatom doping Zinc oxide single crystal-nanometer Heteroatom doping zinc oxide composite, institute Heteroatom doping Zinc oxide single crystal-nanometer Heteroatom doping zinc oxide composite is stated to pass through in Heteroatom doping Zinc oxide single crystal Chemical vapor deposition formation is carried out on surface, and there is the Heteroatom doping zinc oxide film of nanostructure to obtain；Or
Electron-transport substrate uses Heteroatom doping Zinc oxide single crystal-micron Heteroatom doping zinc oxide composite, institute Heteroatom doping Zinc oxide single crystal-micron Heteroatom doping zinc oxide composite is stated to pass through in Heteroatom doping Zinc oxide single crystal Ion etching formation micrometer structure is carried out on surface to obtain.
The beneficial effect of the application includes but is not limited to:
Perovskite solar battery described herein, the ZnO monocrystalline or GZO monocrystalline or AZO monocrystalline of use have good Electric conductivity, excellent translucency and material the features such as high thermal stability as substrate, light transmitting electro-conductive can be used as simultaneously Material and electron transport material collect electronics, instead of the transparent conductive materials such as ITO or FTO+electron transport material TiO2Or SnO2 Structure, reduce the number of plies of battery, largely simplify the structure of perovskite solar battery, eliminate cumbersome system Standby process.
Detailed description of the invention
Fig. 1 is the structural schematic diagram of herein described perovskite solar battery.
Specific embodiment
Referring to Figure 1, perovskite photoactive layer 2 is laminated on electricity to the structural schematic diagram of herein described perovskite solar battery On sub- transferring substrate 1；Hole transmission layer 3 is laminated on perovskite photoactive layer 2；To electrode 4 be laminated on hole transmission layer 3 it On.In the battery of this structure, sunlight enters perovskite photoactive layer from the 1 side incidence of electron-transport substrate, generates exciton, At the interface of perovskite photoactive layer 2, electron-transport substrate 1 and hole transmission layer 3 separation of charge occurs for exciton, and electronics is direct It imports in the monocrystalline of electron-transport substrate 1, hole is passed to hole transmission layer 2, and then electron hole is conducted to external circuit, then complete At photoelectric conversion process.
The application is described in detail below with reference to embodiment, but the application is not limited to these embodiments.
In embodiment, ZnO monocrystalline, GZO monocrystalline and AZO monocrystalline " improve hydro-thermal method according to patent of inventor's Huang before rich Grow the seed crystal suspension equipment of monocrystalline quality and efficiency " equipment that is previously mentioned in (Patent No. ZL 2,012 2 0277751.4) It is prepared with method.
Embodiment 1
Dimethylformamide (the being abbreviated as DMF) solution for the lead iodide that 40 μ l concentration are 461mg/ml is added drop-wise to as electricity The ZnO single-crystal surface (15.5mm × 13.5mm × 0.5mm) of sub- transferring substrate 1, then again on sol evenning machine with 2000r.p.m.'s Revolving speed spin coating 30s；After spin coating is uniform, spin coating there are into the ZnO monocrystalline of lead iodide 70 DEG C of heating 20min on hot plate；Then The ZnO single-chip for being coated with lead iodide cooled down is placed on sol evenning machine, the methylpyridinium iodide that 100 μ l concentration are 35mg/ml is added dropwise On the aqueous isopropanol to lead iodide films of ammonium, 1min is stood, lead iodide is made to come into full contact with to react with iodine methylamine to form methylamine iodine Change lead perovskite photoactive layer 2, then with the revolving speed spin coating 30s of 2000r.p.m.；To the end of spin coating, methylamine iodate will be formd The single-chip of lead perovskite photoactive layer is placed in 90 DEG C of heating 1h on warm table；It will be covered with methylamine lead iodide perovskite again later The single-chip of photoactive layer is placed in sol evenning machine, and the Spiro-MeOTAD (2,2', 7,7'- tetra- that 30 μ l concentration are 80mg/ml is added dropwise [N, N- bis- (4- methoxyphenyl) amino] -9,9'- spiral shell, two fluorenes) chlorobenzene solution, then with 2000r.p.m. revolving speed spin coating 30s is subsequently placed in drier and aoxidizes 12h, forms hole transmission layer 3.It is deposited on the hole transport layer by thermal evaporation 80nm gold shape paired electrode 4.
The effective area of gained battery is 0.0725cm2, photoelectric conversion efficiency 6.27%, current density 12.99mA/ cm2, open-circuit voltage 915.3mV, fill factor FF are 52.68%.
Embodiment 2
The specific preparation step of battery with embodiment 1, the difference is that, using gallium-doped zinc oxide GZO as electron-transport serve as a contrast Bottom 1.
The effective area of gained battery is 0.0725cm2, photoelectric conversion efficiency 6.45%, current density 13.50mA/ cm2, open-circuit voltage 910.0mV, fill factor FF are 52.50%.
Embodiment 3
The specific preparation step of battery with embodiment 1, the difference is that, using Al-Doped ZnO AZO as electron-transport serve as a contrast Bottom 1.
The effective area of gained battery is 0.0725cm2, photoelectric conversion efficiency 6.14%, current density 12.73mA/ cm2, open-circuit voltage 915.1mV, fill factor FF are 52.70%
Embodiment 4
The specific preparation step of battery with embodiment 1, the difference is that, pass through chemical vapor deposition on ZnO monocrystalline Product (CVD) prepares one layer of zinc oxide nanosphere and forms composite construction as electron-transport substrate 1.The method of chemical vapor deposition is joined Examining Zhejiang University's Xia Xianhui Master's thesis, " ss-cvd method prepares grinding for ZnO nano-structure and its growth mechanism Study carefully " in method, on ZnO monocrystalline formed 100~200nm zinc oxide nanosphere.
Embodiment 5
The specific preparation step of battery with embodiment 1, the difference is that, pass through chemical vapor deposition on GZO monocrystalline Product (CVD) prepares one layer of zinc oxide nano rod and forms composite construction as electron-transport substrate 1.The method of chemical vapor deposition is joined Examining Zhejiang University's Xia Xianhui Master's thesis, " ss-cvd method prepares grinding for ZnO nano-structure and its growth mechanism Study carefully " in method, on GZO monocrystalline formed 60~110nm zinc oxide nano rod.
Embodiment 6
The specific preparation step of battery with embodiment 1, the difference is that, pass through chemical vapor deposition on AZO monocrystalline Product (CVD) prepares one layer of zinc oxide nanosphere and forms composite construction as electron-transport substrate 1.The method of chemical vapor deposition is joined Examining Zhejiang University's Xia Xianhui Master's thesis, " ss-cvd method prepares grinding for ZnO nano-structure and its growth mechanism Study carefully " in method, on AZO monocrystalline formed 100~200nm zinc oxide nanosphere.
Embodiment 7
The specific preparation step of battery with embodiment 1, the difference is that, on ZnO monocrystalline prepare one layer of zinc oxide Nano-wire array forms composite construction as electron-transport substrate 1, and the preparation method of zinc oxide nano-wire array is big with reference to Beijing The method for learning the part 3.2.4 in Wang Wei's doctoral thesis " studying based on nanowire array structure solar battery ", gained film are thick The zinc oxide nano-wire array of 1.7~1.8 μm of degree.
Embodiment 8
The specific preparation step of battery with embodiment 1, the difference is that, on GZO monocrystalline prepare one layer of zinc oxide Nano-wire array forms composite construction as electron-transport substrate 1, and the preparation method of zinc oxide nano-wire array is big with reference to Beijing The method for learning the part 3.2.4 in Wang Wei's doctoral thesis " studying based on nanowire array structure solar battery ", gained film are thick The zinc oxide nano-wire array of 1.7~1.8 μm of degree.
Embodiment 9
The specific preparation step of battery with embodiment 1, the difference is that, on AZO monocrystalline prepare one layer of zinc oxide Nano-wire array forms composite construction as electron-transport substrate 1, and the preparation method of zinc oxide nano-wire array is big with reference to Beijing The method for learning the part 3.2.4 in Wang Wei's doctoral thesis " studying based on nanowire array structure solar battery ", gained film are thick The zinc oxide nano-wire array of 1.7~1.8 μm of degree.
Embodiment 10
The specific preparation step of battery with embodiment 1, the difference is that, pass through magnetron sputtering method on ZnO monocrystalline Prepare one layer of TiO2Film forms composite construction as electron-transport substrate 1, and the method for specific magnetron sputtering method is big with reference to Beijing Learn the method in Wang Wei's doctoral thesis " studying based on nanowire array structure solar battery ", gained TiO2The thickness of film is about For 5nm.
Embodiment 11
The specific preparation step of battery with embodiment 1, the difference is that, pass through magnetron sputtering method on GZO monocrystalline Prepare one layer of TiO2Film forms composite construction as electron-transport substrate 1, and the method for specific magnetron sputtering method is big with reference to Beijing Learn the method in Wang Wei's doctoral thesis " studying based on nanowire array structure solar battery ", gained TiO2The thickness of film is about For 5nm.
Embodiment 12
The specific preparation step of battery with embodiment 1, the difference is that, pass through magnetron sputtering method on AZO monocrystalline Prepare one layer of TiO2Film forms composite construction as electron-transport substrate 1, and the method for specific magnetron sputtering method is big with reference to Beijing Learn the method in Wang Wei's doctoral thesis " studying based on nanowire array structure solar battery ", gained TiO2The thickness of film is about For 5nm.
Through detecting, the effective area of gained battery is 0.0725cm in 4~embodiment of embodiment 122, photoelectric conversion effect Rate is between 6%~7%, and current density is in 12mA/cm2~14mA/cm2Between, open-circuit voltage between 910mV~916mV, Fill factor FF is between 52%~53%.
The above is only several embodiments of the application, not does any type of limitation to the application, although this Shen Please disclosed as above with preferred embodiment, however not to limit the application, any person skilled in the art is not taking off In the range of technical scheme, a little variation or modification are made using the technology contents of the disclosure above and is equal to Case study on implementation is imitated, is belonged in technical proposal scope.

Claims (10)

1. perovskite solar battery, including electron-transport substrate, perovskite photoactive layer, hole transmission layer and to electrode, It is characterized in that, the electron-transport substrate contains micro-structure selected from Zinc oxide single crystal, Heteroatom doping Zinc oxide single crystal, surface Zinc oxide single crystal, surface contain the Heteroatom doping Zinc oxide single crystal of micro-structure；The electron-transport substrate is used as light transmission simultaneously Conductive material and electron transport material；Sunlight enters the perovskite active layer from electron-transport one side of substrate incidence.
2. perovskite solar battery according to claim 1, which is characterized in that the Heteroatom doping Zinc oxide single crystal In hetero atom be selected from least one of group III A metallic element.
3. perovskite solar battery according to claim 1, which is characterized in that the Heteroatom doping Zinc oxide single crystal Selected from gallium-doped zinc oxide monocrystalline or Al-Doped ZnO monocrystalline.
4. perovskite solar battery according to claim 1, which is characterized in that contain the oxidation of micro-structure in the surface The micro-structure in Heteroatom doping Zinc oxide single crystal that micro-structure is contained on zinc monocrystalline and surface is micrometer structure and/or nano junction Structure.
5. perovskite solar battery according to claim 4, which is characterized in that the micrometer structure and/or nano junction Structure is obtained by carrying out ion etching on Zinc oxide single crystal surface or Heteroatom doping Zinc oxide single crystal surface.
6. perovskite solar battery according to claim 4, which is characterized in that the micrometer structure and/or nano junction Structure on Zinc oxide single crystal surface or Heteroatom doping Zinc oxide single crystal surface by using vapour deposition process and/or magnetron sputtering Method forms the zinc oxide with micrometer structure and/or nanostructure, the Heteroatom doping with micrometer structure and/or nanostructure Zinc oxide, the titanium oxide with micrometer structure and/or nanostructure, in the tin oxide with micrometer structure and/or nanostructure At least one obtain.
7. perovskite solar battery according to claim 4, which is characterized in that the micrometer structure be selected from micro wire, At least one of micron ball, micron chip, micron wall, micro-flowers, micro belt, micron tube, micron bar, micron membranes.
8. perovskite solar battery according to claim 4, which is characterized in that the nanostructure be selected from nano wire, At least one of nanosphere, nanometer sheet, nm wall, nano flower, nanobelt, nanotube, nanometer rods, nanometer film.
9. the preparation method of any one of claim 1 to the 8 perovskite solar battery, which is characterized in that including following step It is rapid:
S1 provides electron-transport substrate；
S2 forms perovskite photoactive layer in the top of the electron-transport substrate；
S3 forms hole transmission layer in the top of the perovskite photoactive layer；And
S4, on the hole transport layer rectangular paired electrode.
10. preparation method according to claim 9, which is characterized in that electron-transport substrate described in step S1 uses oxygen Change zinc monocrystalline；Or
Electron-transport substrate uses Heteroatom doping Zinc oxide single crystal；Or
Electron-transport substrate uses Zinc oxide single crystal-nano-zinc oxide composite material, and the Zinc oxide single crystal-nano zine oxide is multiple Condensation material by carrying out chemical vapor deposition formation on Zinc oxide single crystal surface there is the zinc oxide film of nanostructure to obtain；Or Person
Electron-transport substrate uses Zinc oxide single crystal-micron zinc oxide composite, and the Zinc oxide single crystal-micron zinc oxide is multiple Condensation material is obtained by carrying out ion etching formation micrometer structure on Zinc oxide single crystal surface；Or
Electron-transport substrate uses Heteroatom doping Zinc oxide single crystal-nanometer Heteroatom doping zinc oxide composite, described miscellaneous Atom doped Zinc oxide single crystal-nanometer Heteroatom doping zinc oxide composite passes through on Heteroatom doping Zinc oxide single crystal surface Upper progress chemical vapor deposition is formed, and there is the Heteroatom doping zinc oxide film of nanostructure to obtain；Or
Electron-transport substrate uses Heteroatom doping Zinc oxide single crystal-micron Heteroatom doping zinc oxide composite, described miscellaneous Atom doped Zinc oxide single crystal-micron Heteroatom doping zinc oxide composite passes through on Heteroatom doping Zinc oxide single crystal surface Upper progress ion etching forms micrometer structure and obtains；Or
Electron-transport substrate uses Zinc oxide single crystal-nano-titanium oxide/oxidation tin composite material, the Zinc oxide single crystal-nanometer Zinc oxide composite has the nano oxidized of nanostructure by using magnetron sputtering method to be formed on Zinc oxide single crystal surface Titanium and/or nm tin oxide layer obtain；Or
Electron-transport substrate uses Heteroatom doping Zinc oxide single crystal-nano-titanium oxide/oxidation tin composite material, the hetero atom Doping zinc-oxide monocrystalline-nano-zinc oxide composite material on Heteroatom doping Zinc oxide single crystal surface by using magnetron sputtering Method is formed, and there is the nano-titanium oxide of nanostructure and/or nm tin oxide layer to obtain.
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CN108023017B (en) * 2016-11-04 2019-12-27 中国科学院化学研究所 Single crystal film of organic-inorganic composite perovskite material and preparation method and application thereof
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