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WO2016060181A1 - Cellule solaire - Google Patents

Cellule solaire Download PDF

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Publication number
WO2016060181A1
WO2016060181A1 PCT/JP2015/079089 JP2015079089W WO2016060181A1 WO 2016060181 A1 WO2016060181 A1 WO 2016060181A1 JP 2015079089 W JP2015079089 W JP 2015079089W WO 2016060181 A1 WO2016060181 A1 WO 2016060181A1
Authority
WO
WIPO (PCT)
Prior art keywords
sealing material
solar cell
photoelectric conversion
organic
inorganic
Prior art date
Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
Ceased
Application number
PCT/JP2015/079089
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English (en)
Japanese (ja)
Inventor
明伸 早川
元彦 浅野
智仁 宇野
麻由美 堀木
雄一郎 福本
哲也 榑林
峻士 小原
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
Sekisui Chemical Co Ltd
Original Assignee
Sekisui Chemical Co Ltd
Priority date (The priority date is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the date listed.)
Filing date
Publication date
Application filed by Sekisui Chemical Co Ltd filed Critical Sekisui Chemical Co Ltd
Priority to JP2015552927A priority Critical patent/JP6196685B2/ja
Publication of WO2016060181A1 publication Critical patent/WO2016060181A1/fr
Anticipated expiration legal-status Critical
Ceased legal-status Critical Current

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Classifications

    • H—ELECTRICITY
    • H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
    • H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
    • H10K85/00—Organic materials used in the body or electrodes of devices covered by this subclass
    • H10K85/50—Organic perovskites; Hybrid organic-inorganic perovskites [HOIP], e.g. CH3NH3PbI3
    • 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
    • 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
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E10/00—Energy generation through renewable energy sources
    • Y02E10/50—Photovoltaic [PV] energy
    • Y02E10/549—Organic PV cells

Definitions

  • the present invention relates to a solar cell that has excellent photoelectric conversion efficiency, little deterioration during sealing (initial deterioration), sputtering resistance, and excellent high-humidity durability.
  • a photoelectric conversion element including a stacked body in which an N-type semiconductor layer and a P-type semiconductor layer are arranged between opposing electrodes.
  • photocarriers are generated by photoexcitation, and an electric field is generated by electrons moving through an N-type semiconductor and holes moving through a P-type semiconductor.
  • inorganic solar cells manufactured using an inorganic semiconductor such as silicon.
  • inorganic solar cells are expensive to manufacture and difficult to increase in size, and the range of use is limited, organic solar cells manufactured using organic semiconductors instead of inorganic semiconductors are attracting attention. .
  • Fullerene In organic solar cells, fullerene is almost always used. Fullerenes are known to work mainly as N-type semiconductors.
  • Patent Document 1 describes a semiconductor heterojunction film formed using an organic compound that becomes a P-type semiconductor and fullerenes.
  • the cause of deterioration is fullerenes (see, for example, Non-Patent Document 1), and materials that replace fullerenes are required.
  • an organic solar cell it is general to seal a laminated body in which an N-type semiconductor layer and a P-type semiconductor layer are arranged between opposing electrodes using a sealing resin such as a sealing material (for example, refer nonpatent literature 2).
  • a sealing resin such as a sealing material
  • the semiconductor material deteriorates during sealing and the photoelectric conversion efficiency decreases. (Initial deterioration).
  • An object of the present invention is to provide a solar cell that has little deterioration (initial deterioration) at the time of sealing, has sputtering resistance, and is excellent in high-humidity durability.
  • the present invention provides a laminate having an electrode, a counter electrode, and a photoelectric conversion layer disposed between the electrode and the counter electrode, and sealing for covering the counter electrode and sealing the laminate.
  • the photoelectric conversion layer is represented by the general formula R-MX 3 (where R is an organic molecule, M is a metal atom, and X is a halogen atom or a chalcogen atom).
  • R is an organic molecule
  • M is a metal atom
  • X is a halogen atom or a chalcogen atom
  • the organic inorganic perovskite compound is used, and the sealing material is a solar cell including a resin having an alicyclic skeleton. The present invention is described in detail below.
  • the present inventor has disclosed a photoelectric conversion in a solar cell in which a laminated body having an electrode, a counter electrode, and a photoelectric conversion layer disposed between the electrode and the counter electrode is sealed with a sealing material.
  • the use of a specific organic / inorganic perovskite compound in the layer was studied. By using the organic / inorganic perovskite compound, an improvement in the photoelectric conversion efficiency of the solar cell can be expected.
  • the present inventor considered using a specific organic-inorganic perovskite compound for the photoelectric conversion layer in a laminate having an electrode, a counter electrode, and a photoelectric conversion layer disposed between the electrode and the counter electrode. did.
  • the organic / inorganic perovskite compound By using the organic / inorganic perovskite compound, an improvement in the photoelectric conversion efficiency of the solar cell can be expected.
  • a laminated body including a photoelectric conversion layer using an organic / inorganic perovskite compound was sealed with a conventional sealing material, it was found that the photoelectric conversion efficiency was lowered at the time of sealing (initial deterioration). Therefore, the present inventors have examined in detail the cause of deterioration when a laminate including a photoelectric conversion layer using an organic / inorganic perovskite compound is sealed with a sealing material.
  • a sealing material containing a resin having an alicyclic skeleton is excellent in sputtering resistance required when forming an inorganic layer by a sputtering method or the like, and completes the present invention. It came to.
  • the solar cell according to the present invention includes an electrode, a counter electrode, a laminate having a photoelectric conversion layer disposed between the electrode and the counter electrode, and encapsulates the laminate so as to cover the counter electrode. And a sealing material.
  • the term “layer” means not only a layer having a clear boundary but also a layer having a concentration gradient in which contained elements gradually change.
  • the elemental analysis of the layer can be performed, for example, by performing FE-TEM / EDS line analysis measurement of the cross section of the solar cell and confirming the element distribution of the specific element.
  • a layer means not only a flat thin film-like layer but also a layer that can form a complicated and complicated structure together with other layers.
  • the material of the said electrode and the said counter electrode is not specifically limited, A conventionally well-known material can be used.
  • the counter electrode is often a patterned electrode.
  • the material for the electrode and the counter electrode include FTO (fluorine-doped tin oxide), sodium, sodium-potassium alloy, lithium, magnesium, aluminum, magnesium-silver mixture, magnesium-indium mixture, aluminum-lithium alloy, Al / lithium Al 2 O 3 mixture, Al / LiF mixture, metal such as gold, CuI, ITO (indium tin oxide), SnO 2 , AZO (aluminum zinc oxide), IZO (indium zinc oxide), GZO (gallium zinc oxide) Conductive transparent materials, conductive transparent polymers, and the like. These materials may be used alone or in combination of two or more. Further, the electrode and the counter electrode may be a cathode or an anode, respectively.
  • the photoelectric conversion layer includes an organic / inorganic perovskite compound represented by the general formula R-MX 3 (where R is an organic molecule, M is a metal atom, and X is a halogen atom or a chalcogen atom).
  • R-MX 3 an organic / inorganic perovskite compound represented by the general formula R-MX 3 (where R is an organic molecule, M is a metal atom, and X is a halogen atom or a chalcogen atom).
  • the R is an organic molecule, and is preferably represented by C 1 N m H n (l, m, and n are all positive integers). Specifically, R is, for example, methylamine, ethylamine, propylamine, butylamine, pentylamine, hexylamine, dimethylamine, diethylamine, dipropylamine, dibutylamine, dipentylamine, dihexylamine, trimethylamine, triethylamine, tripropyl.
  • methylamine, formamidine, ethylamine, propylamine, butylamine, pentylamine, hexylamine and their ions and phenethylammonium are preferred, and methylamine, formamidine, ethylamine, propylamine and these ions are more preferred.
  • M is a metal atom, for example, lead, tin, zinc, titanium, antimony, bismuth, nickel, iron, cobalt, silver, copper, gallium, germanium, magnesium, calcium, indium, aluminum, manganese, chromium, molybdenum, Europium etc. are mentioned. These metal atoms may be used independently and 2 or more types may be used together.
  • X is a halogen atom or a chalcogen atom, and examples thereof include chlorine, bromine, iodine, sulfur, and selenium. These halogen atoms or chalcogen atoms may be used alone or in combination of two or more. Among these, the halogen atom is preferable because the organic / inorganic perovskite compound becomes soluble in an organic solvent and can be applied to an inexpensive printing method by containing halogen in the structure. Furthermore, iodine is more preferable because the energy band gap of the organic-inorganic perovskite compound becomes narrow.
  • the organic / inorganic perovskite compound preferably has a cubic structure in which a metal atom M is disposed at the body center, an organic molecule R is disposed at each vertex, and a halogen atom or a chalcogen atom X is disposed at the face center.
  • FIG. 1 shows an example of a crystal structure of an organic / inorganic perovskite compound having a cubic structure in which a metal atom M is arranged at the body center, an organic molecule R is arranged at each vertex, and a halogen atom or a chalcogen atom X is arranged at the face center. It is a schematic diagram.
  • the organic / inorganic perovskite compound is preferably a crystalline semiconductor.
  • the crystalline semiconductor means a semiconductor capable of measuring the X-ray scattering intensity distribution and detecting a scattering peak.
  • the organic / inorganic perovskite compound is a crystalline semiconductor, the mobility of electrons in the organic / inorganic perovskite compound is increased, and the photoelectric conversion efficiency of the solar cell is improved.
  • the degree of crystallization can be evaluated as an index of crystallization.
  • the degree of crystallinity is determined by separating the crystalline-derived scattering peak detected by the X-ray scattering intensity distribution measurement and the halo derived from the amorphous part by fitting, obtaining the respective intensity integrals, Can be obtained by calculating the ratio.
  • a preferable lower limit of the crystallinity of the organic-inorganic perovskite compound is 30%. When the crystallinity is 30% or more, the mobility of electrons in the organic / inorganic perovskite compound is increased, and the photoelectric conversion efficiency of the solar cell is improved.
  • a more preferred lower limit of the crystallinity is 50%, and a more preferred lower limit is 70%. Examples of the method for increasing the crystallinity of the organic / inorganic perovskite compound include thermal annealing, irradiation with intense light such as laser, and plasma irradiation.
  • the photoelectric conversion layer may further contain an organic semiconductor or an inorganic semiconductor in addition to the organic / inorganic perovskite compound as long as the effects of the present invention are not impaired.
  • the organic semiconductor or inorganic semiconductor referred to here may serve as an electron transport layer or a hole transport layer described later.
  • the organic semiconductor include compounds having a thiophene skeleton such as poly (3-alkylthiophene).
  • conductive polymers having a polyparaphenylene vinylene skeleton, a polyvinyl carbazole skeleton, a polyaniline skeleton, a polyacetylene skeleton, and the like can be given.
  • the alicyclic skeleton is not particularly limited, and examples thereof include skeletons such as norbornene, isobornene, adamantane, cyclohexane, dicyclopentadiene, dicyclohexane, cyclopentane, and dicyclopentene. These skeletons may be used alone or in combination of two or more.
  • the resin having an alicyclic skeleton may be a copolymer of a monomer having an alicyclic skeleton and a monomer having no alicyclic skeleton.
  • the monomer having no alicyclic skeleton is not particularly limited, and examples thereof include ethylhexyl (meth) acrylate, butyl (meth) acrylate, phenyl (meth) acrylate, and phenylalkyl (meth) acrylate.
  • the content of the component derived from the monomer having an alicyclic skeleton in the copolymer is more preferably 50% by weight or more, and further preferably 70% by weight or more.
  • a calculation method of the content of the component derived from the monomer having an alicyclic skeleton in the above-mentioned copolymer it is calculated from a method of calculating from the addition weight of the raw material monomer or a composition analysis result by GC-MS or the like There are methods.
  • Examples of commercially available resins having the above alicyclic skeleton include, for example, a polymer of TOPAS 6013 (manufactured by Polyplastics, having a norbornene skeleton), light ester IB-X (manufactured by Kyoeisha Chemical Co., Ltd., having an isobornene skeleton), MA-DM And a polymer of Mitsubishi Gas Chemical Co., Ltd. (having an adamantane skeleton).
  • the SP value is called a solubility parameter, and is an index that can express the ease of dissolution.
  • the SP value is calculated by using a method proposed by Fedors (R. F. Fedors, Polym. Eng. Sci., 14 (2), 147-154 (1974)). It can be calculated according to the following formula (1) from the evaporation energy ( ⁇ ecoh) (cal / mol) and the molar volume ( ⁇ v) (cm 3 / mol) with respect to the atomic group.
  • ⁇ represents an SP value (cal / mol) 1/2 .
  • the content of the resin having the alicyclic skeleton contained in the sealing material is not particularly limited, but the weight of the alicyclic skeleton in the entire sealing material is preferably 30% by weight or more. When the weight of the alicyclic skeleton is 30% by weight or more, deterioration (initial deterioration) during sealing of the solar cell can be sufficiently suppressed.
  • the said sealing material should just contain resin which has the said alicyclic skeleton, and may further contain resin which does not have alicyclic skeleton.
  • the solar cell of this invention it is also preferable to have an inorganic layer between the said laminated body and the said sealing material. Also in this case, since the said inorganic layer has water vapor
  • the inorganic layer preferably contains a metal oxide, a metal nitride, or a metal oxynitride.
  • the metal oxide, metal nitride or metal oxynitride is not particularly limited as long as it has a water vapor barrier property.
  • oxides, nitrides or oxynitrides of Si, Al, Zn or Sn are preferable, oxides, nitrides or oxynitrides of Zn or Sn are more preferable. Since flexibility can be imparted, an oxide, nitride, or oxynitride of a metal element containing both Zn and Sn metal elements is more preferable.
  • the method for producing the solar cell of the present invention is not particularly limited. For example, after forming the electrode, the photoelectric conversion layer, and the counter electrode in this order on the substrate in this order, the encapsulant is formed. And a method of sealing the laminate and further covering the sealing material with an inorganic layer.
  • the method for sealing the laminate with the sealant is not particularly limited.
  • the method for sealing the laminate using a sheet-like sealant, or the sealing in which the sealant is dissolved in an organic solvent A method of applying a material solution to the laminate, a method of crosslinking or polymerizing a compound having a reactive functional group with heat or UV after applying a compound having a reactive functional group to be a sealing material to the laminate and a method of cooling the sealing material after applying heat to the sealing material.
  • a 10% cyclohexane solution of a resin having a norbornene skeleton as a sealing material (TOPAS 6013, manufactured by Polyplastics, content of a component derived from norbornene monomer is 77% by weight) is applied onto the obtained laminate by a doctor blade.
  • the organic solvent was dried, and a sealing material (weight of alicyclic skeleton (norbornene) occupying 77% by weight in the whole sealing material) was laminated to a thickness of 10 ⁇ m.
  • Example 6 In the sealing of the laminated body, a solar cell was obtained in the same manner as in Example 1 except that the thickness was changed to the sealing material thickness shown in Table 1.
  • Example 7 In the sealing of the laminate, a solar cell was obtained in the same manner as in Example 1 except that the sealing material shown in Table 1 was changed.
  • a 4 mol% peroxide as a curing agent Park Mill D, manufactured by NOF Corporation
  • a liquid monomer having an adamantane skeleton as a sealing material MADM, Mitsubishi Gas Chemical
  • a liquid monomer was polymerized by heating at 120 ° C. for 1 hour to form a sealing material having a thickness of 10 ⁇ m.
  • Example 15 In the sealing of the laminate, a solar cell was obtained in the same manner as in Example 1 except that the sealing material shown in Table 1 was changed.
  • 4 mol% peroxide (Park Mill D, manufactured by NOF Corporation) as a curing agent and a liquid monomer (light ester CH, Kyoeisha) having a cyclohexane skeleton serving as a sealing material on the laminate.
  • a liquid monomer is polymerized by heating at 120 ° C. for 1 hour to form a sealing material having a thickness of 10 ⁇ m.
  • Comparative Example 2 a mixture containing 4 mol% of imidazole compound 2MZA (manufactured by Shikoku Kasei Kogyo Co., Ltd.) and a bisphenol A type epoxy resin (manufactured by Mitsubishi Chemical Corporation) as a curing agent was applied onto the laminate, and 120 A sealing material having a thickness of 10 ⁇ m was formed by heating and curing at 1 ° C. for 1 hour.
  • Comparative Example 3 a 5% cyclohexane solution of polyisobutylene resin (OPPANOL B 50, manufactured by BASF) was applied onto the laminate, and the organic solvent was dried to form a 10 ⁇ m thick sealing material.
  • OPPANOL B 50 polyisobutylene resin
  • Example 9 A solar cell was fabricated in the same manner as in Example 20 except that the mixing ratio of 50% by weight of the liquid monomer having an isobornene skeleton and 50% by weight of the liquid monomer having an ethylhexyl skeleton was changed to 100% by weight of the liquid monomer having an ethylhexyl skeleton. Obtained.
  • a power source (manufactured by KEITHLEY, 236 model) is connected between the electrodes of the laminate before sealing, and photoelectric conversion efficiency is measured using a solar simulation (manufactured by Yamashita Denso Co., Ltd.) with an intensity of 100 mW / cm 2 , and initial conversion is performed. The efficiency.
  • a power source (made by KEITHLEY, 236 model) is connected between the electrodes of the solar cell immediately after sealing, and the photoelectric conversion efficiency is measured using a solar simulation (manufactured by Yamashita Denso Co., Ltd.) having an intensity of 100 mW / cm 2.
  • ADVANTAGE OF THE INVENTION According to this invention, it is excellent in photoelectric conversion efficiency, there is little deterioration at the time of sealing (initial deterioration), sputtering resistance, and the solar cell excellent in high-humidity durability can be provided.

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  • Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Materials Engineering (AREA)
  • Physics & Mathematics (AREA)
  • Electromagnetism (AREA)
  • Photovoltaic Devices (AREA)

Abstract

La présente invention est caractérisée en ce qu'elle procure une cellule solaire présentant un excellent rendement de conversion photoélectrique, peu de détérioration pendant l'étanchéification (détérioration initiale), de la résistance à la pulvérisation, et une excellente durabilité en milieu très humide. Cette cellule solaire comporte : un stratifié comportant une électrode, une contre-électrode, et une couche de conversion photoélectrique agencée entre l'électrode et la contre-électrode ; et un matériau d'étanchéité recouvrant la contre-électrode et étanchéifiant le stratifié. La couche de conversion photoélectrique comprend un composé pérovskite organique-inorganique représenté par la formule générale R-M-X3 (R représentant une molécule organique, M représentant un atome de métal, et X représentant un atome d'halogène ou un atome de chalcogène.) Le matériau d'étanchéité comprend une résine ayant un squelette alicyclique.
PCT/JP2015/079089 2014-10-14 2015-10-14 Cellule solaire Ceased WO2016060181A1 (fr)

Priority Applications (1)

Application Number Priority Date Filing Date Title
JP2015552927A JP6196685B2 (ja) 2014-10-14 2015-10-14 太陽電池

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
JP2014-210191 2014-10-14
JP2014210191 2014-10-14

Publications (1)

Publication Number Publication Date
WO2016060181A1 true WO2016060181A1 (fr) 2016-04-21

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WO (1) WO2016060181A1 (fr)

Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN109560205A (zh) * 2018-11-26 2019-04-02 西安交通大学 一种钙钛矿/硅叠层太阳能电池组件的去湿除氧封装方法

Families Citing this family (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
EP3518301A1 (fr) * 2018-01-24 2019-07-31 Ecole Polytechnique Fédérale de Lausanne (EPFL) Agents d'atténuation des défauts cristallins pour une efficacité de conversion de puissance et une stabilité élevées des dispositifs photovoltaïques en pérovskite

Citations (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JP2007231163A (ja) * 2006-03-01 2007-09-13 Tokyo Univ Of Agriculture & Technology 重合体および重合体の製造方法
WO2014042449A2 (fr) * 2012-09-12 2014-03-20 한국화학연구원 Cellule solaire qui présente une structure absorbant la lumière
JP2014146582A (ja) * 2013-01-30 2014-08-14 Furukawa Electric Co Ltd:The 封止シートおよび有機電子デバイス用素子の封止方法
JP2014156059A (ja) * 2013-02-15 2014-08-28 Daicel Corp 低温溶融封止性及びバリア性を有する複合フィルム及びその製造方法
JP2014192188A (ja) * 2013-03-26 2014-10-06 Rohm Co Ltd 有機薄膜太陽電池およびその製造方法、および電子機器

Family Cites Families (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JP2004165512A (ja) * 2002-11-14 2004-06-10 Matsushita Electric Works Ltd 有機光電変換素子

Patent Citations (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JP2007231163A (ja) * 2006-03-01 2007-09-13 Tokyo Univ Of Agriculture & Technology 重合体および重合体の製造方法
WO2014042449A2 (fr) * 2012-09-12 2014-03-20 한국화학연구원 Cellule solaire qui présente une structure absorbant la lumière
JP2014146582A (ja) * 2013-01-30 2014-08-14 Furukawa Electric Co Ltd:The 封止シートおよび有機電子デバイス用素子の封止方法
JP2014156059A (ja) * 2013-02-15 2014-08-28 Daicel Corp 低温溶融封止性及びバリア性を有する複合フィルム及びその製造方法
JP2014192188A (ja) * 2013-03-26 2014-10-06 Rohm Co Ltd 有機薄膜太陽電池およびその製造方法、および電子機器

Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN109560205A (zh) * 2018-11-26 2019-04-02 西安交通大学 一种钙钛矿/硅叠层太阳能电池组件的去湿除氧封装方法

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JPWO2016060181A1 (ja) 2017-04-27

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