WO2018155349A1 - Cellule solaire et son procédé de production - Google Patents

Cellule solaire et son procédé de production Download PDF

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Publication number
WO2018155349A1
WO2018155349A1 PCT/JP2018/005581 JP2018005581W WO2018155349A1 WO 2018155349 A1 WO2018155349 A1 WO 2018155349A1 JP 2018005581 W JP2018005581 W JP 2018005581W WO 2018155349 A1 WO2018155349 A1 WO 2018155349A1
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Prior art keywords
layer
solar cell
light absorption
group
absorption layer
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PCT/JP2018/005581
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English (en)
Japanese (ja)
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尚吾 石塚
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国立研究開発法人産業技術総合研究所
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Priority to JP2019501293A priority Critical patent/JP6738078B2/ja
Publication of WO2018155349A1 publication Critical patent/WO2018155349A1/fr

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    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
    • H01L31/00—Semiconductor devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation and specially adapted either for the conversion of the energy of such radiation into electrical energy or for the control of electrical energy by such radiation; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof
    • H01L31/04—Semiconductor devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation and specially adapted either for the conversion of the energy of such radiation into electrical energy or for the control of electrical energy by such radiation; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof adapted as photovoltaic [PV] conversion devices
    • H01L31/06—Semiconductor devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation and specially adapted either for the conversion of the energy of such radiation into electrical energy or for the control of electrical energy by such radiation; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof adapted as photovoltaic [PV] conversion devices characterised by potential barriers
    • H01L31/068—Semiconductor devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation and specially adapted either for the conversion of the energy of such radiation into electrical energy or for the control of electrical energy by such radiation; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof adapted as photovoltaic [PV] conversion devices characterised by potential barriers the potential barriers being only of the PN homojunction type, e.g. bulk silicon PN homojunction solar cells or thin film polycrystalline silicon PN homojunction solar cells
    • 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
    • Y02E10/541—CuInSe2 material PV cells
    • 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
    • Y02E10/547—Monocrystalline silicon PV cells
    • 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
    • Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
    • Y02P70/00—Climate change mitigation technologies in the production process for final industrial or consumer products
    • Y02P70/50—Manufacturing or production processes characterised by the final manufactured product

Definitions

  • the present invention relates to a solar cell and a method for manufacturing the solar cell, and more particularly to a solar cell using an I-III-VI 2 chalcopyrite material as a light absorption layer and a method for manufacturing the solar cell.
  • a solar cell using an I-III-VI 2 polycrystal chalcopyrite material composed of an element as a light absorption layer has a negative electrode transparent electrode layer such as conductive zinc oxide, an n-type buffer layer, a p-type The light absorption layer, the positive electrode back electrode layer, and the substrate are stacked in this order (for example, see Non-Patent Document 1).
  • the n-type buffer layer is made of CdS, ZnS (O, OH), In 2 S 3 or the like
  • the positive electrode back electrode layer is generally made of molybdenum (Mo)
  • the substrate is made of glass, metal foil, It is made of resin material such as polyimide, plastic, or ceramic.
  • the light absorbing layer is polycrystalline chalcopyrite materials as for example Cu (In, Ga) constructed using Se 2 (so-called CIGS).
  • the buffer layer is mainly formed by solution growth (wet process), and includes heavy metals as compared with the manufacturing process of other constituent layers such as an electrode layer and a light absorption layer formed by a dry process.
  • the problem was the generation of waste liquid. For this reason, proposals have been made to form the buffer layer by a dry process, but if a solar cell structure that does not use the buffer layer itself can be established, drastic time reduction and cost reduction in the solar cell manufacturing process can be expected.
  • Non-Patent Documents 2 to 5 After forming a Cu (In, Ga) Se 2 light absorption layer, a group II element (such as cadmium (Cd) or zinc (Zn)) is ion-implanted into the thin film surface, or a solution Methods such as water immersion are disclosed.
  • Non-Patent Documents 4 and 5 disclose configurations in which the buffer layer is not used by optimally coupling the energy band offset of the negative electrode transparent electrode layer with that of the light absorption layer.
  • Non-Patent Documents 2 and 3 cannot reduce the number of solar cell device manufacturing steps, and cannot solve the generation of heavy metal waste. Moreover, the method of a nonpatent literature 4 and 5 has the subject that the photoelectric conversion efficiency of the produced solar cell has remained as low as about 10%.
  • the present invention has been made in view of the above points, and an object of the present invention is to provide a highly efficient solar cell having a thin buffer layer or completely eliminating the buffer layer and a method for manufacturing the solar cell.
  • a solar cell of the present invention includes a first electrode layer, a second electrode layer having optical transparency, and light provided between the first and second electrode layers.
  • An absorption layer, wherein the light absorption layer is an I-III-VI 2 based polycrystalline chalcopyrite material to which Si or Ge is added.
  • the method for manufacturing a solar cell of the present invention includes a step of forming a first electrode layer on a substrate, and Si or Ge is added to the first electrode layer. Forming a light absorption layer using the I-III-VI 2- based polycrystalline chalcopyrite material, and forming a light-transmitting second electrode layer above the light absorption layer.
  • the step of forming the light absorption layer includes a step of adding Si or Ge during a period in which an excess region of the group I element is formed with respect to the group III element.
  • a highly efficient solar cell can be realized without having a thin buffer layer or completely eliminating the buffer layer.
  • FIG. 1 It is a schematic structure sectional view of one embodiment of a solar cell concerning the present invention. It is a flowchart for outline explanation of one embodiment of a manufacturing method of a solar cell concerning the present invention. It is a structure ratio vs. time characteristic figure of the light absorption layer of the principal part of one Embodiment of the manufacturing method of the solar cell which concerns on this invention. It is a film growth model figure of an element section in each step of the three-step vapor deposition method of FIG. Si is added Cu (In, Ga) Se 2 film cross-section SEM image, Cu (In, Ga) to and Si were not added is a view showing a sectional SEM image of the Se 2 film.
  • FIG. 3 is a diagram showing an example of current-voltage characteristics of a solar cell of one embodiment of the present invention and current-voltage characteristics of a solar cell of Comparative Example 1.
  • EBIC measurement image of solar absorption layer and cross section of solar cell of one embodiment of the present invention, solar cell of comparative example 2 having no buffer layer, and solar cell of comparative example 1 having a buffer layer and a high resistance layer It is a figure which shows a SEM image.
  • FIG. 1 shows a schematic cross-sectional view of one embodiment of a solar cell according to the present invention.
  • the solar cell 10 of the present embodiment includes a back electrode layer 12, which is a first electrode layer made of Mo, and the like, a light absorption layer 13, and a second electrode layer having light transmittance on a glass substrate 11.
  • the light absorption layer 13 is an I-III-VI 2 compound light absorption layer to which a group IV element such as silicon (Si) or germanium (Ge) is added, and a buffer layer.
  • a group IV element such as silicon (Si) or germanium (Ge) is added
  • the negative transparent electrode layer 14 formed immediately above the light absorption layer 13 is made of conductive zinc oxide or the like.
  • FIG. 2 is a flowchart for explaining the outline of one embodiment of the method for manufacturing a solar cell according to the present invention.
  • a back electrode layer (12 in FIG. 1) is formed on a blue glass substrate (11 in FIG. 1) by a known method by sputtering (step S1 in FIG. 2).
  • Stainless steel or metal plate can be used for the substrate.
  • the back electrode layer for example, a metal film made of Mo is used.
  • a light absorption layer (13 in FIG. 1) is formed on the back electrode layer by a three-stage vapor deposition method (step S2 in FIG. 2).
  • the present embodiment is characterized in that an I-III-VI 2- based polycrystalline chalcopyrite material is used as the light absorption layer, and the light absorption layer is formed by a three-stage vapor deposition method described in detail later.
  • a transparent electrode film (14 in FIG. 1) having a thickness of 2 to 3 ⁇ m is directly formed by sputtering, vacuum evaporation, metal organic chemical vapor deposition or the like. It forms by a well-known method (step S3 of FIG. 2).
  • ZnO: Al containing ZnO: B or alumina (Al 2 O 3 ) doped with boron (B) from diborane is necessary because it has translucency and conductivity. Is used.
  • the solar cell of this embodiment is manufactured.
  • FIG. 3 is a diagram showing the composition ratio versus time characteristic of the light absorption layer of the main part of one embodiment of the method for manufacturing a solar cell according to the present invention, and FIG. Indicates.
  • the vertical axis represents the [Cu] / ([In] + [Ga]) ratio of the Cu (In, Ga) Se 2 film constituting the light absorption layer 13, and the horizontal axis represents time.
  • group III elements In and Ga and group VI element Se are simultaneously deposited on the back electrode. Since Cu is not deposited in this first stage, the [Cu] / ([In] + [Ga]) ratio is “0” as shown in FIG. Further, the film growth model on the back electrode is as shown in FIG.
  • a Cu—Se liquid phase is formed on the surface of the deposited film due to excessive deposition of Cu.
  • Si group IV elements are simultaneously deposited.
  • the film growth model at the start of the third stage is as shown in FIG.
  • the deposition time elapses the deposition amounts of In and Ga are relatively increased as compared with the deposition amount of Cu, so that the [Cu] / ([In] + [Ga]) ratio is as shown in FIG.
  • the third stage deposition is completed.
  • the film growth model at the end of the third stage of deposition is such that Si dissolves in the CIGS film and becomes Cu (In, Ga) Se 2 : Si.
  • the formation of the Cu (In, Ga) Se 2 film to which Si is added as the light absorption layer 13 of the present embodiment is completed.
  • Si may be deposited from the point in time when the [Cu] / ([In] + [Ga]) ratio exceeds “1” in the second stage of the process.
  • FIG. 5A shows a cross-sectional SEM image of a Cu (In, Ga) Se 2 film to which Si, which is the light absorption layer 13 of this embodiment, is added.
  • FIG. 5B shows a cross-sectional SEM image of a Cu (In, Ga) Se 2 film to which Si is not added.
  • a cross-sectional SEM image of a Cu (In, Ga) Se 2 film added with Si, which is the light absorption layer 13 of this embodiment, obtained by a scanning electron microscope (SEM) is shown in FIG. ), A layer formed between CIGS polycrystalline grains (hereinafter referred to as “coating layer” in this specification) exists.
  • This coating layer is presumed to be a layer having a slightly different composition from the crystal grains, or a layer having the same composition but a different crystal orientation. It was confirmed by an experiment described later that this coating layer performs a function similar to the buffer layer of Comparative Example 1 described later. On the other hand, the cross-sectional SEM image of the Cu (In, Ga) Se 2 film to which Si is not added has no coating film as shown in FIG. 5B.
  • FIG. 6A shows an example of current-voltage characteristics of the solar cell of this embodiment
  • FIG. 6B shows an example of current-voltage characteristics of the solar cell of Comparative Example 1.
  • the current-voltage characteristics at the time of light incidence of the solar cell of the present embodiment having the light absorption layer 13 which is the Cu (In, Ga) Se 2 film added with Si and having the cross-sectional structure shown in FIG. 6 (a) is indicated by A1, and the dark current-voltage characteristic is indicated by A2 in FIG.
  • a Cu (In, Ga) Se 2 film to which Si is not added is provided as a light absorption layer, and a buffer layer, a high resistance layer, and a transparent electrode layer are stacked in this order on the light absorption layer.
  • the current-voltage characteristic at the time of light incidence of the solar cell of Comparative Example 1 having the structure is indicated by B1 in FIG. 6B
  • the current-voltage characteristic at the dark time is indicated by B2 in FIG. 6B.
  • EBIC Electron Beam Induced Current
  • an electron-hole pair excited by irradiating an electron beam to a cross section of a measurement sample is detected as an EBIC signal (current), but there is no pn junction in the measurement sample (depletion)
  • the electron-hole pair is recombined in the part where the layer is not formed) and carrier loss occurs and disappears, whereas the pn junction part (the part where the depletion layer is formed) does not recombine.
  • the magnitude of the measurement sample in which the depletion layer is not formed is relatively smaller than that of the EBIC signal in which the depletion layer is formed. Therefore, the presence or absence of a depletion layer in the measurement sample can be observed from an image in which the luminance is changed according to the magnitude of the EBIC signal.
  • a monochrome image indicated by 31 in FIG. 7A shows an EBIC measurement image of the light absorption layer of the solar cell of the present embodiment.
  • a coating layer is formed in the Cu (In, Ga) Se 2 film to which Si is added.
  • Ga) Se 2 film and the covering layer form a charge separation interface, and a depletion layer is formed. Therefore, the bright monochrome image 31 shows that the depletion layer exists uniformly in the entire light absorption layer.
  • the monochrome image 30 is an SEM image of the back electrode layer of the solar cell of this embodiment.
  • Monochrome image 32 shows an SEM image of the transparent (surface) electrode layer.
  • a monochrome image indicated by 41 in FIG. 7B shows an EBIC measurement image of the light absorption layer made of a Cu (In, Ga) Se 2 film to which Si is not added.
  • the solar cell of Comparative Example 2 having this light absorption layer is the same as the present embodiment in that the transparent electrode layer is directly laminated on the upper surface of the light absorption layer without a buffer layer. Since the layer is a Cu (In, Ga) Se 2 film to which Si is not added, the above-described coating layer is not formed as shown in FIG. For this reason, as can be seen from the monochrome image 41 in FIG.
  • 7B in the solar cell of Comparative Example 2, there are many dark portions indicating portions where there is no coating layer in the light absorption layer, and almost no depletion layer. Indicates that it does not exist.
  • 7B shows the intensity distribution of the EBIC signal image 41 of the light absorption layer
  • the monochrome image 30 is an SEM image of the back electrode layer of the solar cell
  • the monochrome image 32 is transparent ( The SEM image of the (surface) electrode layer is shown.
  • the transparent (surface) electrode layer is 2 ⁇ m thick ZnO: B.
  • FIG. 7C shows a Cu (In, Ga) Se 2 film to which Si is not added as a light absorption layer, and a buffer layer, a high resistance layer, and a transparent electrode on the light absorption layer.
  • stacked in this order are shown. That is, a monochrome image 51 shown in FIG. 7C shows an EBIC measurement image of a light absorption layer made of a Cu (In, Ga) Se 2 film to which Si is not added, and 51 ′ in FIG.
  • the image indicated by is an image showing the intensity distribution of the EBIC measurement signal of the light absorption layer.
  • an image 30 shows an SEM image of the back electrode layer
  • an image 52 shows an SEM image of the buffer layer and the high resistance layer
  • an image 53 shows an SEM image of the transparent (front) electrode layer.
  • the transparent (surface) electrode layer represented by the SEM image 53 is ZnO: Al having a thickness of 0.3 ⁇ m.
  • the buffer layer and the high resistance layer each have a thickness of only 50 nm, their SEM images 52 exist, but in FIG. However, when enlarged and looked closely, it was confirmed that the SEM images of the buffer layer and the high resistance layer were slightly whitish images.
  • the solar cell of Comparative Example 1 can confirm the region where the depletion layer hardly exists in the light absorption layer as can be seen from the EBIC measurement image 51.
  • the depletion layer uniformly spreads in the entire light absorption layer as compared with the solar cells of Comparative Examples 1 and 2, so that even if the buffer layer is not provided, the solar cell is high. Efficiency can be realized.
  • the solar cell of the present embodiment does not have a buffer layer, it is possible to omit a device manufacturing process necessary for buffer layer manufacturing and solve the problem of heavy metal waste liquid generated by buffer layer manufacturing. be able to.
  • the present invention is not limited to the above-described embodiment, and includes various other modifications.
  • Ge can be used in place of Si as a group IV element to be vapor-deposited at the same time in addition to In, Ga and Se.
  • a buffer layer was not provided in embodiment, you may provide a very thin buffer layer 30 nm or less. Also in this case, since the depletion layer spreads uniformly throughout the light absorption layer, high efficiency can be realized.
  • the buffer layer is not limited to a single buffer layer composed of CdS or the like, but also includes a broad buffer layer that is a composite layer composed of a buffer layer and a high resistance layer.
  • the I-III-VI 2 polycrystal chalcopyrite material is formed by three-stage vapor deposition, but in addition, the I-III-VI 2 polycrystal chalcopyrite material may be formed by a selenization method.
  • a selenization method for example, in order to form a Cu (Se, Ga) Se 2 film by a selenization method, a Cu—Ga / In metal precursor film is formed and then selenized using a selenium source such as solid selenium or hydrogen selenide. To do.
  • a selenium source such as solid selenium or hydrogen selenide.

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Abstract

La présente invention permet d'obtenir une cellule solaire à haut rendement, sans utiliser une couche tampon. Une cellule solaire 10, selon la présente invention, possède une structure dans laquelle une couche d'électrode arrière 12, qui est formée à partir de Mo ou analogue, une couche d'absorption de lumière 13 et une couche d'électrode transparente 14 sont stratifiées sur un substrat en verre 11. Cette cellule solaire 10 est conçue de telle sorte que la couche d'absorption de lumière 13 est une couche d'absorption de lumière composée d'éléments I-III-VI2 dans laquelle un élément du groupe IV, tel que du silicium (Si) ou du germanium (Ge) est ajouté. La couche d'absorption de lumière 13 est obtenue par dépôt en phase vapeur d'un élément du groupe IV, à savoir Si, simultanément avec des éléments du groupe III, à savoir In et Ga et un élément du groupe VI, à savoir Se, dans la troisième étape d'un procédé de dépôt en phase vapeur en trois étapes. Par conséquent, une couche de revêtement est formée à l'intérieur de la couche d'absorption de lumière 13, ce qui permet d'obtenir un haut rendement.
PCT/JP2018/005581 2017-02-27 2018-02-16 Cellule solaire et son procédé de production WO2018155349A1 (fr)

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Citations (4)

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Publication number Priority date Publication date Assignee Title
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JP2014024717A (ja) * 2012-07-27 2014-02-06 Asahi Glass Co Ltd Ｃｕ−Ｉｎ−Ｇａ−Ｓｅ太陽電池用ガラス板およびそれを用いた太陽電池とその製造方法
US20140238486A1 (en) * 2011-10-17 2014-08-28 Lg Innotek Co., Ltd. Solar cell and method of fabricating the same
JP2015164164A (ja) * 2014-02-28 2015-09-10 富士フイルム株式会社 光電変換素子および太陽電池

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Publication number Priority date Publication date Assignee Title
JPH11145500A (ja) * 1997-11-11 1999-05-28 Asahi Chem Ind Co Ltd 不純物半導体の製造方法、ｐ型半導体、ｎ型半導体、半導体装置
US20140238486A1 (en) * 2011-10-17 2014-08-28 Lg Innotek Co., Ltd. Solar cell and method of fabricating the same
JP2014024717A (ja) * 2012-07-27 2014-02-06 Asahi Glass Co Ltd Ｃｕ−Ｉｎ−Ｇａ−Ｓｅ太陽電池用ガラス板およびそれを用いた太陽電池とその製造方法
JP2015164164A (ja) * 2014-02-28 2015-09-10 富士フイルム株式会社 光電変換素子および太陽電池

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Title
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RUSU, M. ET AL.: "CuGaxSey chalcopyrite-related thin films grown by chemical close-spaced vapor transport (CCSVT) for photovoltaic application: Surface- and bulk material properties, oxidation and surface Ge-doping", SOLAR ENERGY MATERIALS & SOLAR CELLS, vol. 95, no. 6, June 2011 (2011-06-01), pages 1555 - 1580, XP028191988, Retrieved from the Internet <URL:https://doi.org/10.1016/j.solmat.2011.01.016> *
SUGIYAMA, TAKESHI ET AL.: "Formation of pn Homojunction in Cu (InGa) Se2 Thin Film Solar Cells by Zn Doping", JAPANESE JOURNAL OF APPLIED PHYSICS PART 1, vol. 39 pt1, no. 8, 2000, pages 4816 - 4819, XP001014871 *
THIRU, SATHIABAMA ET AL.: "Photoluminescence study of Si doped and undoped Chalcopyrite CuGaSe2 thin films", APPLIED PHYSICS A, vol. 113, no. 2, November 2013 (2013-11-01), pages 257 - 261, XP055543081, Retrieved from the Internet <URL:DOI10.1007/s00339-013-7951-5> *

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