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CN109148688A - A kind of efficient perovskite solar battery and preparation method thereof - Google Patents

A kind of efficient perovskite solar battery and preparation method thereof Download PDF

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CN109148688A
CN109148688A CN201810756629.7A CN201810756629A CN109148688A CN 109148688 A CN109148688 A CN 109148688A CN 201810756629 A CN201810756629 A CN 201810756629A CN 109148688 A CN109148688 A CN 109148688A
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transport layer
perovskite
solar cell
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詹义强
王鹏飞
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Fudan University
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    • H10K30/00—Organic devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation
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    • H10K30/00—Organic devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation
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    • H—ELECTRICITY
    • H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
    • 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
    • H—ELECTRICITY
    • H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
    • H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
    • H10K71/00—Manufacture or treatment specially adapted for the organic devices covered by this subclass
    • H10K71/10—Deposition of organic active material
    • H10K71/12—Deposition of organic active material using liquid deposition, e.g. spin coating
    • H—ELECTRICITY
    • H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
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Abstract

本发明属于半导体光电子器件领域，具体为一种高效钙钛矿太阳能电池及其制备方法。本发明钙钛矿太阳能电池的结构从下往上依次为：透明衬底、第一透明电极层、半透明功能层、第二电极层。其中半透明功能层由下至上依次为电子传输层、钾卤素盐层、钙钛矿光吸收层、空穴传输层，或者为空穴传输层、钾卤素盐层、钙钛矿光吸收层、电子传输层。本钙钛矿太阳能电池的制备方法包括：在电子传输层上旋涂钾卤素盐，通过钙钛矿的退火，钾卤素盐扩散到钙钛矿层，能够主动地有效地钝化钙钛矿层，增强钙钛矿的结晶性，提高光吸收，并最终提高太阳能电池的效率。本发明制备方法较为简单，具有实际应用意义。

The invention belongs to the field of semiconductor optoelectronic devices, in particular to a high-efficiency perovskite solar cell and a preparation method thereof. The structure of the perovskite solar cell of the present invention is, from bottom to top, a transparent substrate, a first transparent electrode layer, a semitransparent functional layer, and a second electrode layer. The translucent functional layer is, from bottom to top, an electron transport layer, a potassium halide salt layer, a perovskite light absorption layer, a hole transport layer, or a hole transport layer, a potassium halide salt layer, a perovskite light absorption layer, electron transport layer. The preparation method of the perovskite solar cell includes: spin-coating potassium halide salt on the electron transport layer, and by annealing the perovskite, the potassium halide salt diffuses into the perovskite layer, which can actively and effectively passivate the perovskite layer, enhancing the The crystallinity of perovskites improves light absorption and ultimately the efficiency of solar cells. The preparation method of the invention is relatively simple and has practical application significance.

Description

A kind of efficient perovskite solar battery and preparation method thereof
Technical field
The invention belongs to semiconductor photoelectronic device technical fields, and in particular to perovskite solar battery and its preparation side Method.
Background technique
Nowadays, solar energy has become the important component of renewable energy.Perovskite battery is due to its preparation cost The low, many advantages such as preparation process is simple, incident photon-to-electron conversion efficiency is high, it is considered to be most promising photovoltaic solar-electricity of new generation Pond.By fast-developing in recent years, incident photon-to-electron conversion efficiency is promoted from 3.8% in 2009 in July, 2017 22.7%.The efficiency has been able to compare favourably with silica-based solar cell.
The quality of perovskite absorbed layer will will have a direct impact on the photoelectric characteristic of perovskite solar battery.Perovskite solar energy There are many defect states for battery, these mainly play Carrier recombination center by the defect state that volume defect and surface defect are constituted Effect.Surface defect is present in the grain boundary and perovskite absorbed layer interface of perovskite, by surface dangling bonds and unsaturation Atom generates.Volume defect is present in perovskite crystal, is made of vacancy and interstitial atom.The surface topography of perovskite absorbed layer It also will affect defect state density with material property.The performance of device will effectively be promoted by reducing defect state density.
Summary of the invention
The purpose of the present invention is to provide a kind of low costs, efficient perovskite solar battery and preparation method thereof.
Efficient perovskite solar battery provided by the invention, by lamination, preparation process is prepared, and structure is under Supreme successively includes: transparent substrates, first transparency electrode layer, translucent functional layer, the second electrode lay；Wherein:
The transparent substrates are quartz material rigid glass substrates or flexibility PET or flexibility PEN substrate.Quartz material hard glass Substrate high temperature resistant, light transmittance are high.
The first transparency electrode layer is located on transparent substrates, material be metal oxide, for example, ITO or FTO, It is with a thickness of 100-200nm, and square resistance is less than 10 Ω/.
The translucent functional layer is located on first transparency electrode layer, and translucent functional layer is followed successively by electronics from the bottom to top Transport layer, potassium halogen salt deposit, perovskite light absorbing layer, hole transmission layer, or be hole transmission layer, potassium halogen salt deposit, calcium titanium Mine light absorbing layer, electron transfer layer；
The material of electron transfer layer can be but be not limited to TiO2、SnO2, ZnO, PCBM or C60, with a thickness of 25-200 nm；
The material of potassium halogen salt deposit is KF, KCl, KBr or KI, with a thickness of 30-300nm；
The material of perovskite light absorbing layer can be but be not limited to FA0.85MA0.15Pb(I0.85Br0.15)3、MAPbI3Or MAPbI3- xClx, thickness is less than 350 nm, for example, 100-350 nm；
The material of hole transmission layer can be but be not limited to Spiro-OMeTAD, PEDOT:PSS, NiOx, P3HT or PTAA, it is thick Degree is 40-200 nm；
The second electrode lay is located on semitransparent electrode layer, and material is gold or silver.With a thickness of 40-150nm.
The preparation method of perovskite solar battery of the present invention, the following steps are included:
(1) transparent conductive substrate is cleaned, dry and surface hydrophilicity improve；
(2) first transparency electrode layer is prepared on substrate；
(3) electron transfer layer is prepared on first transparency electrode layer in ultra-clean chamber, later spin coating potassium halogen on the electron transport layer Plain salt deposit is sequentially prepared perovskite using solwution method in the glove box that water oxygen content is below 1 ppm on the electron transport layer Light absorbing layer, hole transmission layer；
Or hole transmission layer is prepared on first transparency electrode layer in ultra-clean chamber, spin coating potassium halogen on the hole transport layer later Plain salt deposit is sequentially prepared perovskite using solwution method in the glove box that water oxygen content is below 1 ppm on the hole transport layer Light absorbing layer, electron transfer layer；
(4) substrate prepared is put into vacuum evaporating coating machine rapidly, vapor deposition forms the second electrode lay, completes perovskite too The preparation of positive energy battery.
Efficient perovskite solar battery provided by the invention, its working principle is that: when solar irradiation is mapped on electrode, calcium Titanium ore absorbed layer absorbs visible light, ultraviolet light, and exciton, excitonic motion to light-absorption layer, charge (electronics, sky are generated in light-absorption layer Cave) transmission bed boundary, under the action of built-in field, electrons and holes separation, electron transfer layer transmits electronics to cathode, hole Transport layer transporting holes reach anode, form series connection photoelectric current.Charge transport layer includes electron transfer layer and hole transmission layer.
Compared with prior art, the invention has the following advantages that
(1) compared to the perovskite solar battery of no potassium haloid, perovskite solar battery according to the present invention Light absorption is remarkably reinforced, and the crystal grain of calcium titanium ore bed will increase, and the crystallinity of perovskite can be remarkably reinforced.Meanwhile potassium haloid meeting It is diffused into calcium titanium ore bed in annealing process, the defects of passivation calcium titanium ore bed state is final to promote perovskite solar-electricity The performance in pond；
(2) perovskite solar battery preparation process according to the present invention uses solwution method, the simple, cost with preparation process Low advantage.It can effectively improve the photoelectric conversion efficiency of perovskite solar battery and make it have bigger market potential.
The present invention is a kind of efficient perovskite solar battery, and potassium haloid can be spread in the annealing process of perovskite Into perovskite light absorbing layer, enhance the crystallinity of perovskite, enhance the light absorption of perovskite, is slightly reduced the forbidden band of perovskite Width, and it is passivated the defect state of perovskite light absorbing layer, the final efficiency for promoting perovskite solar battery.
Detailed description of the invention
Fig. 1 is a kind of structural schematic diagram of efficient perovskite solar battery in the embodiment of the present invention 1.
Figure label: 101 be transparent substrates, and 102 be first transparency electrode layer, and 103 be electron transfer layer, and 104 be potassium halogen Plain salt deposit, 105 perovskite light absorbing layers, 106 be hole transmission layer, and 107 be the second electrode lay.
Specific embodiment
Present invention will be further explained below with reference to the attached drawings and examples.
Embodiment 1
A kind of structure of efficient perovskite solar battery 101 is as shown in Figure 1: transparent substrates, 102 is first transparency electrode Layer, 103 be electron transfer layer, 104 be potassium halogen salt deposit, 105 be perovskite light absorbing layer, 106 be hole transmission layer, 107 be The second electrode lay.Transparent substrates are quartz glass；First transparency electrode layer is ITO, with a thickness of 100 nm；Electron transfer layer is SnO2, with a thickness of 25 nm；Potassium halogen salt deposit is KCl, with a thickness of 15 nm；Calcium titanium ore bed is MAPbI3-xClx, with a thickness of 300 nm；Hole transmission layer is Spiro-OMeTAD, with a thickness of 50nm；The second electrode lay is gold, with a thickness of 50 nm.
Perovskite solar battery in embodiment 1 the preparation method is as follows:
ITO electro-conductive glass is successively cleaned with ethyl alcohol, acetone, deionized water, is removed after dry with UV ozone cleaning machine remaining Organic matter；The SnO for being 2.67% by concentration2Nano sol is spin-coated to clean transparent conductive glass surface, and at 180 DEG C Lower annealing 30min obtains the SnO with a thickness of 25nm2Electron transfer layer.The KCl aqueous solution that concentration is 25mg/ml is spin-coated to electricity In sub- transport layer, uniform KCl film is formed, 130 DEG C of annealing 15min in vacuum obtain KCl layers；It is 7:3's in volume ratio Lead iodide, lead chloride and iodine methylamine, the lead iodide, lead chloride are added in the mixed solution of gamma-butyrolacton and dimethyl sulfoxide Molar ratio with iodine methylamine is 1:0.1:1.2, and 50 DEG C of constant temperature stir 12h in glove box, forms the calcium of the 40wt% of yellow homogeneous Titanium ore precursor solution；Resulting perovskite precursor solution is spin-coated on KCl layer with anti-solwution method, is formed uniform MAPbI3-xClxFilm, anneal 14min at 100 DEG C, obtains fine and close perovskite light absorbing layer.It is added in 1ml chlorobenzene Spiro-OMeTAD 72.3mg, two (trifluoro methylsulfonyl) imine lithiums (Li-TFSI), 17.5 15 μ l, 4- tert-butyl pyrrole of μ l, FK209 29 μ l of pyridine is stirred at room temperature 3h and forms hole transport layer material solution；By resulting hole transport layer material solution spin coating calcium On titanium ore light absorbing layer, hole transmission layer is formed.Finally, gold electrode is deposited on the hole transport layer by thermal evaporation deposition, complete The preparation of perovskite solar battery.
Embodiment 2
The structure of perovskite solar battery is from the bottom up successively are as follows: transparent substrates, first transparency electrode layer, hole transmission layer, Potassium halogen salt deposit, perovskite light absorbing layer, electron transfer layer, the second electrode lay.Transparent substrates are quartz glass；First transparent electricity Pole layer is ITO, with a thickness of 100nm；Hole transmission layer is NiOx, with a thickness of 40 nm；Potassium halogen salt deposit is KCl, with a thickness of 15nm；Calcium titanium ore bed is MAPbI3-xClx, with a thickness of 300nm；Electron transfer layer is PCBM, with a thickness of 50nm；The second electrode lay For silver, with a thickness of 80 nm.
Perovskite solar battery in embodiment 1 the preparation method is as follows:
ITO electro-conductive glass is successively cleaned with ethyl alcohol, acetone, deionized water, is removed after dry with UV ozone cleaning machine remaining Organic matter；By the ethanol solution of nickel nitrate, it is spin-coated to clean transparent conductive glass surface, and is annealed at 280 DEG C 30min obtains the NiO with a thickness of 40 nmxHole transmission layer.The KCl aqueous solution that concentration is 25mg/ml is spin-coated to hole to pass On defeated layer, uniform KCl film is formed, 130 DEG C of annealing 15min in vacuum obtain KCl layers；In γ-fourth that volume ratio is 7:3 Lead iodide, lead chloride and iodine methylamine, the lead iodide, lead chloride and iodine first are added in the mixed solution of lactone and dimethyl sulfoxide The molar ratio of amine is 1:0.1:1.2, and 50 DEG C of constant temperature stir 12h in glove box, before forming the perovskite of the 40wt% of yellow homogeneous Drive liquid solution；Resulting perovskite precursor solution is spin-coated on KCl layer with anti-solwution method, forms uniform MAPbI3-xClx Film, anneal 14min at 100 DEG C, obtains fine and close perovskite light absorbing layer.PCBM20 mg is added in 1ml chlorobenzene, Stirring 3h forms electron transport layer materials solution at room temperature；By resulting electron transport layer materials solution spin coating perovskite light absorption On layer, electron transfer layer is formed.Finally, gold electrode is deposited on the electron transport layer by thermal evaporation deposition, the perovskite sun is completed The preparation of energy battery.
The energy conversion efficiency of perovskite solar battery according to the present invention can achieve 19.4%.
Finally, it is stated that the above examples are only used to illustrate the technical scheme of the present invention and not limits, although reference Preferred embodiment describes the invention in detail, those skilled in the art should understand that, it can be to of the invention Technical solution is modified or replaced equivalently, and without departing from the objective and range of technical solution of the present invention, should all be covered In scope of the presently claimed invention.

Claims (6)

1.一种高效钙钛矿太阳能电池，其特征在于，其结构由下至上依次为：透明衬底、第一透明电极层、半透明功能层、第二电极层；其中：1. a high-efficiency perovskite solar cell is characterized in that, its structure is followed from bottom to top: transparent substrate, first transparent electrode layer, semitransparent functional layer, second electrode layer; Wherein: 所述第一透明电极层位于透明衬底之上，其材质为金属氧化物；The first transparent electrode layer is located on the transparent substrate and is made of metal oxide; 所述半透明功能层位于第一透明电极层之上，半透明功能层由下至上依次为电子传输层、钾卤素盐层、钙钛矿光吸收层、空穴传输层，或者为空穴传输层、钾卤素盐层、钙钛矿光吸收层、电子传输层；The translucent functional layer is located on the first transparent electrode layer, and the translucent functional layer is, from bottom to top, an electron transport layer, a potassium halide salt layer, a perovskite light absorption layer, a hole transport layer, or a hole transport layer. layer, potassium halide salt layer, perovskite light absorption layer, electron transport layer; 所述顶第二电极层位于半透明功能上方，为金属金或者金属银。The top and second electrode layers are located above the translucent function and are metallic gold or metallic silver. 2. 根据权利要求1所述的高效钙钛矿太阳能电池，其特征在于，所述第一透明电极层材料采用金属氧化物ITO或FTO，其厚度为100-200 nm，方块电阻小于10Ω/□。2. The high-efficiency perovskite solar cell according to claim 1, wherein the first transparent electrode layer material adopts metal oxide ITO or FTO, and its thickness is 100-200 nm, and the sheet resistance is less than 10Ω/□ . 3. 根据权利要求1或2所述的高效钙钛矿太阳能电池，其特征在于，所述空穴传输层材料为Spiro-OMeTAD、PEDOT：PSS、NiOx、P3HT或PTAA，厚度为40-200 nm；电子传输层材料为TiO2、SnO2、ZnO、PCBM或C60，厚度为25-200 nm；3. high-efficiency perovskite solar cell according to claim 1 and 2, is characterized in that, described hole transport layer material is Spiro-OMeTAD, PEDOT: PSS, NiO x , P3HT or PTAA, thickness is 40-200 nm; the electron transport layer material is TiO 2 , SnO 2 , ZnO, PCBM or C 60 , and the thickness is 25-200 nm; 钾卤素盐层材料为KF、KCl、KBr或KI，厚度为30-300nm；The potassium halide salt layer material is KF, KCl, KBr or KI, and the thickness is 30-300nm; 钙钛矿光吸收层材料为FA0.85MA0.15Pb(I0.85Br0.15)3、MAPbI3或MAPbI3-xClx，其厚度为200-350 nm。The perovskite light absorption layer material is FA 0.85 MA 0.15 Pb(I 0.85 Br 0.15 ) 3 , MAPbI 3 or MAPbI 3-x Cl x , and its thickness is 200-350 nm. 4.根据权利要求3所述的高效钙钛矿太阳能电池，其特征在于，所述第二电极层在半透明功能层上方，为金属金或者金属银，厚度40-150nm。4 . The high-efficiency perovskite solar cell according to claim 3 , wherein the second electrode layer above the translucent functional layer is metal gold or metal silver, and has a thickness of 40-150 nm. 5 . 5.根据权利要求1、2或4所述的高效钙钛矿太阳能电池，其特征在于，所述透明衬底材料为石英材质硬质玻璃衬底或柔性PET或柔性PEN衬底。5. The high-efficiency perovskite solar cell according to claim 1, 2 or 4, wherein the transparent substrate material is a quartz hard glass substrate or a flexible PET or flexible PEN substrate. 6.一种如权利要求1-5之一所述的高效钙钛矿太阳能电池的制备方法，其特征在于，具体步骤为：6. a preparation method of the high-efficiency perovskite solar cell as described in one of claims 1-5, is characterized in that, concrete steps are: （1）对透明导电衬底进行清洗、干燥及表面亲水性改善；(1) Cleaning, drying and improving the surface hydrophilicity of the transparent conductive substrate; （2）在衬底上制备第一透明电极层；(2) preparing a first transparent electrode layer on the substrate; （3）在超净间中在第一透明电极层上制备电子传输层，之后在电子传输层上旋涂钾卤素盐层，在水氧含量均低于1 ppm的手套箱中，采用溶液法在电子传输层上依次制备钙钛矿光吸收层、空穴传输层；(3) Prepare an electron transport layer on the first transparent electrode layer in an ultra-clean room, and then spin-coat a potassium halide salt layer on the electron transport layer. A perovskite light absorption layer and a hole transport layer are sequentially prepared on the electron transport layer; 或者在超净间中在第一透明电极层上制备空穴传输层，之后在空穴传输层上旋涂钾卤素盐层，在水氧含量均低于1 ppm的手套箱中，采用溶液法在空穴传输层上依次制备钙钛矿光吸收层、电子传输层；Or prepare a hole transport layer on the first transparent electrode layer in an ultra-clean room, then spin-coat a potassium halide salt layer on the hole transport layer, and use a solution method in a glove box with water and oxygen content below 1 ppm On the hole transport layer, a perovskite light absorption layer and an electron transport layer are sequentially prepared; （4）将制备好的基片迅速放入真空蒸发镀膜机内，蒸镀形成第二电极层，完成钙钛矿太阳能电池的制备。(4) The prepared substrate is quickly put into the vacuum evaporation coating machine, and the second electrode layer is formed by evaporation to complete the preparation of the perovskite solar cell.
CN201810756629.7A 2018-07-11 2018-07-11 A kind of efficient perovskite solar battery and preparation method thereof Pending CN109148688A (en)

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* Cited by examiner, † Cited by third party
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CN110504362A (en) * 2019-07-17 2019-11-26 浙江浙能技术研究院有限公司 A Modification Method of SnO2 Electron Selective Transport Layer
CN111162179A (en) * 2019-12-30 2020-05-15 电子科技大学 A kind of semitransparent perovskite solar cell covered with high reflective film and preparation method thereof
CN111477745A (en) * 2020-04-08 2020-07-31 天合光能股份有限公司 Solar cell and manufacturing method thereof
CN111477745B (en) * 2020-04-08 2023-09-22 天合光能股份有限公司 Solar cell and manufacturing method thereof
CN112820832A (en) * 2021-02-08 2021-05-18 珠海复旦创新研究院 Efficient perovskite solar cell and preparation method thereof
WO2023143207A1 (en) * 2022-01-27 2023-08-03 西安隆基乐叶光伏科技有限公司 Solar cell and preparation method therefor
WO2025035826A1 (en) * 2023-08-17 2025-02-20 宁德时代新能源科技股份有限公司 Solar cell and preparation method therefor, and photovoltaic assembly, system and electric apparatus

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Application publication date: 20190104