WO2009133688A1 - 光電変換素子の製造方法、及び、それにより製造される光電変換素子、及び、光電変換素子モジュールの製造方法、及び、それにより製造される光電変換素子モジュール - Google Patents
光電変換素子の製造方法、及び、それにより製造される光電変換素子、及び、光電変換素子モジュールの製造方法、及び、それにより製造される光電変換素子モジュール Download PDFInfo
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- WO2009133688A1 WO2009133688A1 PCT/JP2009/001908 JP2009001908W WO2009133688A1 WO 2009133688 A1 WO2009133688 A1 WO 2009133688A1 JP 2009001908 W JP2009001908 W JP 2009001908W WO 2009133688 A1 WO2009133688 A1 WO 2009133688A1
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- WIPO (PCT)
- Prior art keywords
- electrode
- photoelectric conversion
- terminal
- conversion element
- oxide semiconductor
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- 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 method for manufacturing a photoelectric conversion element, a photoelectric conversion element manufactured thereby, a method for manufacturing a photoelectric conversion element module, and a photoelectric conversion element module manufactured thereby.
- Dye-sensitized solar cells were developed by Gretzel, Switzerland, and have the advantages of high photoelectric conversion efficiency and low manufacturing costs, and are attracting attention as a new type of solar cell.
- the schematic structure of the dye-sensitized solar cell is as follows: a working electrode in which a porous oxide semiconductor layer carrying a photosensitizing dye is provided on a transparent substrate provided with a transparent conductive film; And an electrolyte containing a redox pair is filled between the working electrode and the counter electrode.
- the electrolyte it is common to use an electrolytic solution in which a redox couple such as I ⁇ / I 3 ⁇ is dissolved in an organic solvent such as acetonitrile.
- a configuration using a non-volatile ionic liquid, a liquid There are known a structure in which the electrolyte is gelled with an appropriate gelling agent to make it pseudo-solid, a structure using a solid semiconductor such as a p-type semiconductor, and the like.
- the counter electrode must be made of a material that prevents corrosion due to chemical reaction with the electrolyte.
- a material that prevents corrosion due to chemical reaction with the electrolyte a titanium substrate formed of platinum, a glass electrode substrate formed of platinum, or the like can be used.
- the glass electrode substrate on which the conductive layer made of platinum is formed has a problem that the thickness of the photoelectric conversion element is increased because the glass has to have a certain thickness or more in order to secure the strength of the glass.
- a titanium substrate has an oxide film formed on the surface of titanium, it is difficult to connect lead wires or the like to the titanium substrate.
- Patent Document 1 a film made of a dissimilar metal (such as Cu) that can be easily soldered is formed on the surface of an electrode composed of a titanium substrate by sputtering.
- the present invention has been made in view of the above circumstances, and a method for manufacturing a photoelectric conversion element capable of easily manufacturing a photoelectric conversion element including a terminal firmly bonded to an electrode using titanium, and thereby It aims at providing the manufacturing method of the photoelectric conversion element manufactured, the photoelectric conversion element module, and the photoelectric conversion element module manufactured by it.
- the method for producing a photoelectric conversion element of the present invention is the method for producing a photoelectric conversion element on the surface of the catalyst layer in the first electrode having a metal plate made of titanium or an alloy containing titanium and the catalyst layer, or the second electrode having a transparent conductor.
- a terminal forming step of forming a terminal on the metal plate, and in the terminal forming step, the terminal is formed by heating and melting a high melting point solder and applying an ultrasonic wave. Also features It is.
- a porous oxide semiconductor layer is formed on the catalyst layer of the first electrode or the transparent conductor of the second electrode, and photosensitization is performed on the porous oxide semiconductor layer.
- the dye is supported. That is, in the first electrode and the second electrode, the electrode on which the porous oxide semiconductor layer is formed becomes an electrode on the working electrode, and the electrode on which the porous oxide semiconductor layer is not formed becomes an electrode on the counter electrode. Then, the electrolyte is surrounded and sealed with a sealing material between the first electrode and the second electrode.
- the first electrode has a metal plate made of titanium or an alloy containing titanium, and the metal plate has corrosion resistance to the electrolyte.
- a terminal is formed on the metal plate on the surface other than the surface surrounded by the outer periphery of the sealing material in the first electrode.
- the terminal is made of a high melting point solder, and is formed by heating and melting the high melting point solder and applying ultrasonic waves to the high melting point solder.
- the wettability with respect to the metal plate surface of a high melting point solder improves. Therefore, the high melting point solder can be firmly bonded to the electrode using titanium, and the terminal can be easily formed without using equipment such as a vacuum apparatus.
- the porous oxide semiconductor layer may be formed on the transparent conductor.
- the first electrode is surrounded by an outer periphery of the sealing material when the first electrode is viewed from a direction perpendicular to the surface of the first electrode. It is preferable that an extending portion is provided extending outward from the region, and the terminal is formed in the extending portion.
- the surface on the surface opposite to the second electrode side of the first electrode is The distance between the terminal and the photosensitizing dye or electrolyte is larger than when the terminal is formed in the region surrounded by the sealing material. For this reason, it can suppress that a heat
- the terminal is formed from a surface of the first electrode opposite to the second electrode side to a surface of the second electrode side.
- the terminal is bonded to the metal plate of the first electrode from the surface on the opposite side to the second electrode side of the first electrode to the surface on the second electrode side.
- the terminal can be more firmly connected on the metal plate.
- a collection of metal is formed on a surface of the second electrode on the first electrode side from a region surrounded by the sealing material to an outer periphery of the sealing agent.
- the terminal is on the opposite side of the first electrode from the second electrode side.
- it is preferably formed at a position overlapping the current collector wiring.
- the current collector wiring is made of a metal material, it has excellent thermal conductivity. And since the current collection wiring is provided from the area
- a current collecting wiring made of metal on a surface of the second electrode on the first electrode side from a region overlapping with the sealing material to an outer periphery of the sealing material. And when the first electrode is viewed from a direction perpendicular to the surface of the first electrode, the terminal is on a surface opposite to the second electrode side of the first electrode. In the region that overlaps with the sealing material, the layer is preferably formed at a position that overlaps with the current collector wiring.
- the current collector wiring is made of a metal material, it has excellent thermal conductivity. And since the current collection wiring is provided from the area
- the method for producing a photoelectric conversion element of the present invention includes a terminal forming step of forming a terminal on the surface of the metal plate in the first electrode having a metal plate made of titanium or an alloy containing titanium and a catalyst layer, and transparent A semiconductor forming step of forming a porous oxide semiconductor layer on the surface of the transparent conductor of the second electrode having a conductor; a dye supporting step of supporting a photosensitizing dye on the porous oxide semiconductor layer; The first electrode and the second electrode face each other, the porous oxide semiconductor layer and the electrolyte are surrounded by a sealing material between the first electrode and the second electrode, and the terminal is sealed A sealing step of sealing so as not to be surrounded by a stopper, and in the terminal forming step, the terminal is formed by heating and melting high melting point solder and applying ultrasonic waves. Characterized by A.
- a terminal is formed on a metal plate on a first electrode, a porous oxide semiconductor layer is formed on a second electrode, and a porous oxide semiconductor layer is formed. Is loaded with a photosensitizing dye.
- heat applied in the terminal formation step is applied to the second electrode. Does not conduct. For this reason, deterioration of the photosensitizing dye due to heat in the terminal forming step can be prevented. Further, the heat applied in the terminal forming process is not conducted to the electrolyte through the first electrode. For this reason, deterioration of the electrolyte due to heat in the terminal forming step can be prevented.
- the method for producing a photoelectric conversion element of the present invention is a semiconductor in which a porous oxide semiconductor layer is formed on the surface of the catalyst layer in the first electrode having a metal plate made of titanium or an alloy containing titanium and a catalyst layer.
- Forming a terminal on the metal plate in a forming step, a dye carrying step for carrying a photosensitizing dye on the porous oxide semiconductor layer, and a region where the porous semiconductor is not formed on the surface of the first electrode A terminal forming step, a second electrode having a transparent conductor and the first electrode face each other, and the porous oxide semiconductor layer and the electrolyte are sealed between the first electrode and the second electrode And a sealing step of sealing the terminal so as not to be surrounded by the sealing material, and in the terminal forming step, the terminal is heated and melted by a high melting point solder. Both It is characterized in that the ultrasonic wave is formed is applied.
- the terminal forming step is before the dye supporting step.
- the photoelectric conversion element of the present invention is manufactured by the above-described method for manufacturing a photoelectric conversion element.
- a photoelectric conversion element According to such a photoelectric conversion element, wettability with respect to the metal plate surface of the first electrode of the high melting point solder is improved in the manufacturing process, and the first electrode using titanium and the terminal formed on the first electrode are provided. Strongly joined. For this reason, when connecting a lead wire etc. to a terminal, a photoelectric conversion element and a lead wire etc. can be connected firmly.
- the manufacturing method of the photoelectric conversion element module of this invention is equipped with the photoelectric conversion element preparation process of preparing multiple photoelectric conversion elements manufactured by said manufacturing method of a photoelectric conversion element,
- the said in the at least 1 said photoelectric conversion element It has the connection process which electrically connects the terminal formed on a 1st electrode, and the said 2nd electrode in another at least 1 photoelectric conversion element with a conductive member.
- the high melting point solder can be easily and firmly joined to the first electrode using titanium. Therefore, a photoelectric conversion module capable of firmly connecting the photoelectric conversion elements via the conductive member can be manufactured.
- the photoelectric conversion element has a terminal formed outside a region surrounded by an outer periphery of the sealing material on the surface of the second electrode on the first electrode side.
- the terminal formed on the first electrode in at least one of the photoelectric conversion elements may be connected to the terminal formed on the second electrode in the other at least one photoelectric conversion element by the conductive member. .
- the photoelectric conversion element module of the present invention is manufactured by the above-described method for manufacturing a photoelectric conversion element module.
- the connection between the photoelectric conversion elements is strong, and it is possible to suppress the disconnection between the photoelectric conversion elements due to an external force or the like.
- the manufacturing method of the photoelectric conversion element which can manufacture easily a photoelectric conversion element provided with the terminal firmly joined with the electrode which uses titanium, the photoelectric conversion element manufactured by it, and a photoelectric conversion element A module manufacturing method and a photoelectric conversion element module manufactured thereby are provided.
- FIG. 1 is a schematic cross-sectional view showing a photoelectric conversion element according to the first embodiment of the present invention.
- the photoelectric conversion element 100 includes a working electrode 11, a counter electrode 12 disposed so as to face the working electrode 11, an electrolyte 5 disposed between the working electrode 11 and the counter electrode 12, A sealing material 14 surrounding the electrolyte 5 and a terminal 7 formed on the surface of the counter electrode 12 opposite to the working electrode 11 are provided as main components.
- the working electrode 11 is provided on the transparent substrate 1 and the second electrode 20 made of the transparent conductor 1 provided on one surface of the transparent substrate 2 and the transparent substrate 2, and carries a photosensitizing dye. And a porous oxide semiconductor layer 3.
- the transparent base material 2 is composed of a substrate made of a light transmissive material. Examples of such materials include glass, polyethylene terephthalate (PET), polycarbonate (PC), polyethersulfone (PES), polyethylene naphthalate (PEN), and are usually used as a transparent substrate for photoelectric conversion elements. Any material can be used.
- the transparent substrate 2 is appropriately selected from these in consideration of resistance to the electrolyte and the like. Further, the transparent substrate 2 is preferably a substrate that is as excellent in light transmission as possible, and more preferably a substrate having a light transmittance of 90% or more.
- the transparent conductor 1 is a transparent conductive film, and is a thin film formed on a part of one surface or the entire surface of the transparent substrate 2.
- the transparent conductor 1 is preferably a thin film made of a conductive metal oxide.
- conductive metal oxides include indium tin oxide (ITO), fluorine-added tin oxide (FTO), and tin oxide (SnO 2 ).
- the transparent conductor 1 may be a single layer or a laminate of a plurality of layers made of different conductive metal oxides.
- the transparent conductor 1 is preferably ITO or FTO from the viewpoint of easy film formation and low manufacturing cost, and has high heat resistance and chemical resistance. From the viewpoint of having, it is more preferable that it is composed of FTO.
- the transparent conductor 1 is composed of a laminated body composed of a plurality of layers because the characteristics of each layer can be reflected.
- a laminated film in which a film made of FTO is laminated on a film made of ITO is preferable.
- the transparent conductor 1 having high conductivity, heat resistance, and chemical resistance can be realized, and a transparent conductive substrate with low light absorption in the visible range and high conductivity can be configured.
- the thickness of the transparent conductor 1 may be in the range of 0.01 ⁇ m to 2 ⁇ m, for example.
- the oxide semiconductor that forms the porous oxide semiconductor layer 3 is not particularly limited, and any oxide semiconductor can be used as long as it is usually used to form a porous oxide semiconductor layer for a photoelectric conversion element. be able to.
- oxide semiconductor include titanium oxide (TiO 2 ), tin oxide (SnO 2 ), tungsten oxide (WO 3 ), zinc oxide (ZnO), niobium oxide (Nb 2 O 5 ), and strontium titanate.
- the average particle diameter of these oxide semiconductor particles is 1 to 1000 nm, which increases the surface area of the oxide semiconductor covered with the dye, that is, widens the field for photoelectric conversion and generates more electrons. This is preferable.
- the porous oxide semiconductor layer 3 is preferably configured by stacking oxide semiconductor particles having different particle size distributions. In this case, light can be repeatedly reflected in the semiconductor layer, and incident light that escapes to the outside of the porous oxide semiconductor layer 3 can be reduced, and light can be efficiently converted into electrons.
- the thickness of the porous oxide semiconductor layer 3 may be, for example, 0.5 to 50 ⁇ m.
- the porous oxide semiconductor layer 3 can also be comprised with the laminated body of the some oxide semiconductor which consists of a different material.
- the porous oxide semiconductor layer 3 for example, a dispersion in which commercially available oxide semiconductor particles are dispersed in a desired dispersion medium or a colloidal solution that can be prepared by a sol-gel method is used as necessary. After adding a desired additive, the coating is performed by a known coating method such as a screen printing method, an ink jet printing method, a roll coating method, a doctor blade method, or a spray coating method, and then a void is formed by heat treatment or the like. It is possible to apply a method to make it.
- a coating method such as a screen printing method, an ink jet printing method, a roll coating method, a doctor blade method, or a spray coating method, and then a void is formed by heat treatment or the like. It is possible to apply a method to make it.
- the photosensitizing dye examples include a ruthenium complex containing a bipyridine structure, a terpyridine structure and the like as a ligand, a metal-containing complex such as polyphylline and phthalocyanine, and organic dyes such as eosin, rhodamine and merocyanine.
- a ruthenium complex containing a bipyridine structure, a terpyridine structure and the like as a ligand a metal-containing complex such as polyphylline and phthalocyanine
- organic dyes such as eosin, rhodamine and merocyanine.
- the electrolyte 5 is obtained by impregnating the porous oxide semiconductor layer 3 with an electrolytic solution, or after impregnating the porous oxide semiconductor layer 3 with the electrolytic solution, the electrolytic solution is appropriately gelled. Gelled (quasi-solidified) using an agent and formed integrally with the porous oxide semiconductor layer 3, or a gel electrolyte containing an ionic liquid, oxide semiconductor particles, or conductive particles Can be used.
- an electrolytic solution in which an electrolyte component such as iodine, iodide ion or tertiary-butylpyridine is dissolved in an organic solvent such as ethylene carbonate or methoxyacetonitrile is used.
- an electrolytic solution in which an electrolyte component such as iodine, iodide ion or tertiary-butylpyridine is dissolved in an organic solvent such as ethylene carbonate or methoxyacetonitrile is used.
- the gelling agent used for gelling the electrolytic solution include polyvinylidene fluoride, a polyethylene oxide derivative, and an amino acid derivative.
- Room temperature meltable salt which is a liquid at room temperature and made the compound which has the quaternized nitrogen atom into a cation or an anion is mentioned.
- the cation of the room temperature melting salt include quaternized imidazolium derivatives, quaternized pyridinium derivatives, quaternized ammonium derivatives and the like.
- the anion of the ambient temperature molten salt BF 4 -, PF 6 - , F (HF) n-, bis (trifluoromethylsulfonyl) imide [N (CF 3 SO 2) 2 -], and the like iodide ion.
- Specific examples of the ionic liquid include salts composed of a quaternized imidazolium cation and iodide ion or bistrifluoromethylsulfonylimide ion.
- the oxide semiconductor particles are not particularly limited in terms of the type and particle size of the substance, but those that are excellent in mixing with an electrolytic solution mainly composed of an ionic liquid and that gel the electrolytic solution are used. .
- the oxide semiconductor particles are required to have excellent chemical stability against other coexisting components contained in the electrolyte without reducing the conductivity of the electrolyte.
- the oxide semiconductor particles are preferably those that do not deteriorate due to an oxidation reaction.
- oxide semiconductor particles examples include TiO 2 , SnO 2 , WO 3 , ZnO, Nb 2 O 5 , In 2 O 3 , ZrO 2 , Ta 2 O 5 , La 2 O 3 , SrTiO 3 , Y 2 O 3 ,
- TiO 2 , SnO 2 , WO 3 , ZnO, Nb 2 O 5 , In 2 O 3 , ZrO 2 , Ta 2 O 5 , La 2 O 3 , SrTiO 3 , Y 2 O 3 One or a mixture of two or more selected from the group consisting of Ho 2 O 3 , Bi 2 O 3 , CeO 2 , and Al 2 O 3 is preferable, and titanium dioxide fine particles (nanoparticles) are particularly preferable.
- the average particle diameter of the titanium dioxide is preferably about 2 nm to 1000 nm.
- conductive particles such as conductors and semiconductors are used.
- the range of the specific resistance of the conductive particles is preferably 1.0 ⁇ 10 ⁇ 2 ⁇ ⁇ cm or less, and more preferably 1.0 ⁇ 10 ⁇ 3 ⁇ ⁇ cm or less.
- the type and particle size of the conductive particles are not particularly limited, and those that are excellent in miscibility with an electrolytic solution mainly composed of an ionic liquid and that gel the electrolytic solution are used.
- Such conductive particles are required to have excellent chemical stability with respect to other coexisting components contained in the electrolyte, since the conductivity is not easily lowered in the electrolyte.
- the electrolyte contains an oxidation / reduction pair such as iodine / iodide ion or bromine / bromide ion, an electrolyte that does not deteriorate due to oxidation reaction or the like is preferable.
- Such conductive particles include those composed of carbon-based materials, and specific examples include particles such as carbon nanotubes, carbon fibers, and carbon black. All methods for producing these substances are known, and commercially available products can also be used.
- the counter electrode 12 is configured by the first electrode 10.
- the first electrode includes a metal plate 4 and a catalyst layer 6 made of titanium or a titanium alloy.
- the catalyst layer 6 that promotes the reduction reaction is formed on the surface of the metal plate 4 on the working electrode 11 side.
- the catalyst layer 6 is made of platinum or carbon.
- the sealing material 14 connects the working electrode 11 and the counter electrode 12, and the electrolyte 5 between the working electrode 11 and the counter electrode 12 is sealed by being surrounded by the sealing material 14.
- the material constituting the sealing material 14 include an ionomer, an ethylene-vinyl acetic anhydride copolymer, an ethylene-methacrylic acid copolymer, an ethylene-vinyl alcohol copolymer, an ultraviolet curable resin, and a vinyl alcohol polymer. Is mentioned.
- the sealing material 14 may be comprised only with resin, and may be comprised with resin and an inorganic filler.
- a terminal 7 is formed on the surface of the counter electrode 12 opposite to the working electrode 11 side, that is, on the surface of the metal plate 4 of the first electrode 10.
- the terminal 7 is composed of a high melting point solder.
- the high melting point solder it is preferable to use a solder having a melting point of 200 ° C. or higher (for example, 210 ° C. or higher).
- a solder having a melting point of 200 ° C. or higher for example, 210 ° C. or higher.
- a solder 13 for connecting a conductive wire or the like and the terminal 7 is formed on the terminal 7.
- the solder 13 is not particularly limited, but when the terminal 7 is a high melting point solder, a solder having a lower melting point than the high melting point solder (hereinafter, sometimes referred to as a low melting point solder) is preferable.
- a solder having a melting point of less than 200 ° C. is preferably used.
- solder include eutectic type (eg Sn-Pb), lead-free type (eg Sn-Ag, Sn-Cu, Sn-Ag-Cu, Sn-Zn, Sn-Zn-B). Is mentioned.
- the terminal 8 is formed in the outer region surrounded by the outer periphery of the sealing material 14 on the surface of the second electrode 20 on the first electrode side.
- the material constituting the terminal 8 include metals such as gold, silver, copper, platinum, and aluminum.
- the working electrode 11 and the counter electrode 12 are prepared (preparation process).
- the working electrode 11 can be obtained by the following process. First, the transparent conductor 1 is formed on one surface of the transparent substrate 2 to form the second electrode 20. Next, the porous oxide semiconductor layer 3 is formed on the transparent conductor 1 in the second electrode 20 (semiconductor forming step). Next, a photosensitizing dye is carried (dye carrying process).
- Examples of the method for forming the transparent conductor 1 on the transparent substrate 2 include thin film forming methods such as sputtering, CVD (chemical vapor deposition), spray pyrolysis (SPD), and vapor deposition. .
- the spray pyrolysis method is preferable.
- the haze ratio can be easily controlled.
- the spray pyrolysis method is preferable because a vacuum system is unnecessary, and thus the manufacturing process can be simplified and the cost can be reduced.
- the method for forming the porous oxide semiconductor layer 3 on the transparent conductor 1 mainly includes a coating process and a drying / firing process.
- a coating process for example, a paste of TiO 2 colloid obtained by mixing TiO 2 powder, a surfactant and a thickener at a predetermined ratio is applied to the surface of the transparent conductor 1 that has been made hydrophilic. It is done.
- a pressing means is used so that the applied colloid keeps a uniform thickness while pressing the colloid on the transparent conductor 1 using a pressing means (for example, a glass rod).
- a pressing means for example, a glass rod
- drying / firing step for example, a method of leaving the coated colloid in an air atmosphere at room temperature for about 30 minutes and drying the applied colloid, followed by firing at a temperature of 450 ° C. for about 60 minutes using an electric furnace. Can be mentioned.
- a very small amount of dye solution for supporting the dye for example, a solvent having a volume ratio of 1: 1 acetonitrile and t-butanol.
- a solution prepared by adding N3 dye powder was prepared in advance.
- a porous oxide semiconductor layer 3 is formed in a solution containing a photosensitizing dye as a solvent in a petri dish-like container, which is separately heated to about 120 to 150 ° C. in an electric furnace.
- the second electrode 20 is immersed, and is immersed for a whole day and night (approximately 20 hours) in a dark place.
- the second electrode 20 on which the porous oxide semiconductor layer 3 is formed is taken out of the solution containing the photosensitizing dye, and washed with a mixed solution of acetonitrile and t-butanol. This gives a working electrode 11 having the porous oxide semiconductor layer 3 made of TiO 2 thin film carrying a photosensitizing dye.
- the terminal 8 formed on the working electrode 11 is formed, for example, by applying a silver paste by printing or the like, and heating and baking.
- the terminal 8 is preferably formed before the dye carrying step.
- a metal plate 4 made of titanium or a titanium alloy is prepared.
- a catalyst layer 6 made of platinum or the like is formed on the surface of the prepared metal plate 4.
- the catalyst layer 6 is formed by a sputtering method or the like. Thereby, the 1st electrode 10 which has the metal plate 4 and the catalyst layer 6 can be obtained, and the 1st electrode 10 becomes the counter electrode 12 as it is.
- the electrolyte 5 is surrounded and sealed by the sealing material 14 between the working electrode 11 and the counter electrode 12 (sealing process).
- a resin or its precursor for forming the sealing material 14 is formed on the working electrode 11.
- the resin or its precursor is formed so as to surround the porous oxide semiconductor layer 3 of the working electrode 11.
- the resin is a thermoplastic resin
- the molten resin is applied on the working electrode 11 and then naturally cooled at room temperature, or a film-like resin is brought into contact with the working electrode 11 and the resin is heated and melted by an external heat source. Then, the resin can be obtained by natural cooling at room temperature.
- the thermoplastic resin for example, an ionomer or an ethylene-methacrylic acid copolymer is used.
- an ultraviolet curable resin an ultraviolet curable resin that is a precursor of the resin is applied on the working electrode 11.
- an aqueous solution containing the resin is applied on the working electrode 11.
- a vinyl alcohol polymer is used as the water-soluble resin.
- a resin or its precursor for forming the sealing material 14 is formed on the counter electrode 12.
- the resin or its precursor on the counter electrode 12 is formed at a position overlapping the resin on the working electrode 11 or its precursor when the working electrode 11 and the counter electrode 12 face each other.
- the resin on the counter electrode 12 or its precursor may be formed in the same manner as the resin or its precursor formed on the working electrode 11.
- an electrolyte is filled in a region surrounded by the resin on the working electrode 11 or its precursor.
- the working electrode 11 and the counter electrode 12 are opposed to each other, and the resin on the counter electrode 12 and the working electrode 11 are overlapped. Thereafter, when the resin is a thermoplastic resin in a reduced pressure environment, the resin is heated and melted to bond the working electrode 11 and the counter electrode 12 together. Thus, the sealing material 14 is obtained.
- the resin is an ultraviolet curable resin
- the ultraviolet curable resin of the resin on the counter electrode 12 and the working electrode 11 are overlapped, and then the ultraviolet curable resin is cured by ultraviolet rays, whereby the sealing material 14 is obtained.
- the resin is a water-soluble resin, after the laminate is formed, the finger is dried at room temperature and then dried in a low-humidity environment, whereby the sealing material 14 is obtained.
- the terminal 7 is formed on the surface of the counter electrode 12 opposite to the working electrode 11 side, that is, on the metal plate 4 of the first electrode 10 (terminal forming step).
- the counter electrode 12 First, on the surface of the counter electrode 12 opposite to the working electrode 11 side, the counter electrode 12, the high melting point solder, and the tip of the soldering iron are placed in contact.
- the tip of the soldering iron is heated so that the high-melting-point solder can be melted and generates ultrasonic waves.
- the high melting point solder is melted by the heat transmitted from the tip of the soldering iron and vibrated by the ultrasonic waves from the tip of the soldering iron. Therefore, the high melting point solder improves the wettability with the metal plate 4 and is fixed on the surface of the metal plate 4.
- the terminal 7 is formed on the surface of the counter electrode 12.
- the temperature of the tip of the soldering iron is not particularly limited as long as a high melting point solder can be melted, but is preferably 200 to 450 ° C. from the viewpoint of sufficiently melting the solder, for example, 250 to 350 ° C. It is more preferable from the viewpoint of preventing oxidation of the solder and preventing deterioration of the photosensitizing dye due to heat.
- the vibration frequency of the ultrasonic wave generated from the tip of the soldering iron is preferably 10 to 200 kHz, and more preferably 20 to 100 kHz from the viewpoint of preventing the metal plate 4 from being damaged.
- the terminal 7 is formed by removing the soldering iron from the molten high melting point solder and cooling the high melting point solder.
- the solder 13 on the terminals 7 and 8 is formed by melting the solder on the terminals 7 and 8 and then solidifying it.
- the porous oxide semiconductor layer 3 is formed on the transparent conductor 1 of the second electrode composed of the transparent substrate 2 and the transparent conductor 1 to increase the photosensitivity.
- the working electrode 11 is obtained by supporting the dye.
- the catalyst layer 6 is formed on the surface of the metal plate 4 made of titanium or a titanium alloy, and the first electrode is used as the counter electrode 12 as it is as the first electrode 10.
- the working electrode 11 and the counter electrode 12 are prepared, and the electrolyte 5 is surrounded and sealed by the sealing material 14 between the working electrode 11 and the counter electrode 12. Since the counter electrode 12 includes the metal plate 4 made of titanium or an alloy containing titanium and the catalyst layer 6, the counter electrode 12 has corrosion resistance to the electrolyte 5.
- the terminal 7 is formed on the surface of the metal plate 4 of the counter electrode 12.
- the terminal 7 is formed by heating and melting the high melting point solder and applying ultrasonic waves to the high melting point solder. For this reason, when the terminal 7 is formed, the wettability of the high melting point solder to the surface of the metal plate 4 is improved. For this reason, the terminal 7 made of high melting point solder can be easily and firmly fixed to the surface of the metal plate 4 made of a titanium plate or an alloy plate containing titanium.
- the photoelectric conversion element 100 including the terminal 7 firmly fixed on the surface of the metal plate 4 of the counter electrode 12 can be easily manufactured.
- the photoelectric conversion element 100 manufactured in the above-described manufacturing process the first electrode 10 using titanium and the terminal 7 formed on the first electrode 10 are firmly bonded. Etc., the photoelectric conversion element 100 and the lead wire can be firmly connected.
- FIG. 2 is a schematic cross-sectional view showing the photoelectric conversion device of the present embodiment.
- the photoelectric conversion element 110 when the metal plate 4 is viewed from a direction perpendicular to the surface of the metal plate 4 constituting the counter electrode 12, the counter electrode 12 is It has the extension part 18a extended outside the area
- the terminal 7 is formed on the extending portion 18a.
- Such a photoelectric conversion element 110 is manufactured as follows.
- the counter electrode 12 having a region outside the region where the region surrounded by the outer periphery of the sealing material 14 is planned is prepared. That is, the counter electrode 12 having a region that becomes the extending portion 18a is prepared.
- Other processes in the preparation process are the same as those in the first embodiment.
- sealing is performed with the sealing material 14 so that the extended portion 18a is secured.
- the sealing method may be performed in the same manner as the sealing process in the first embodiment.
- the terminal 7 is formed on the extended portion 18a.
- the terminals may be formed in the same manner as the terminal forming process in the first embodiment.
- the photoelectric conversion element 110 when heat is applied in the terminal formation step, when the counter electrode 12 is viewed from a direction perpendicular to the surface of the metal plate 4 constituting the counter electrode 12, The distance between the terminal 7 and the electrolyte 5 is greater than when the terminal 7 is connected to the region surrounded by the sealing material 14. For this reason, heat can be prevented from being transmitted to the photosensitizing dye or the electrolyte 5 through the counter electrode 12. Therefore, even when heat is applied in the terminal forming step, deterioration of the photosensitizing dye and the electrolyte 5 due to heat can be suppressed.
- FIG. 3 the same or equivalent components as those in the first embodiment are denoted by the same reference numerals, and redundant description is omitted.
- FIG. 3 is a schematic cross-sectional view showing the photoelectric conversion device of the present embodiment.
- the working electrode 11 has a plurality of porous oxide semiconductor layers 3 a and 3 b, and a porous oxide is formed on the surface of the working electrode 11 on the counter electrode 12 side.
- a current collecting wiring 35 made of metal is provided between the semiconductor layers 3a and 3b.
- the terminal is connected to the current collecting wiring 35 in the region 19 surrounded by the sealing material 14 of the metal plate 4. It is formed at the overlapping position.
- the current collection wiring 35 is provided from the region 19 surrounded by the sealing material 14 to the outside of the outer periphery of the sealing agent, and is connected to the terminal 8. Further, the current collecting wiring 35 is entirely covered with the wiring protective layer 36, and the contact between the electrolyte 5 and the current collecting wiring 35 is prevented. Note that the wiring protective layer 36 may or may not be in contact with the transparent conductor 1 of the working electrode 11 as long as the entire current collecting wiring 35 is covered.
- the material constituting the current collector wiring 35 may be any material having a lower resistance than the transparent conductor 1, and examples of such a material include metals such as gold, silver, copper, platinum, aluminum, titanium, and nickel. Is mentioned.
- Examples of the material constituting the wiring protective layer 36 include inorganic insulating materials such as non-lead transparent low melting point glass frit.
- the wiring protective layer 36 prevents contact between the electrolyte 5 and the current collector wiring 35 over a longer period of time, and generation of dissolved components of the wiring protective layer 36 when the electrolyte 5 comes into contact with the wiring protective layer 36.
- Such a photoelectric conversion element 120 is manufactured as follows.
- the porous oxide semiconductor layers 3a and 3b are formed in the semiconductor formation process.
- the porous semiconductor is formed at two locations using the same method as the method of forming the porous oxide semiconductor layer 3. Should be provided.
- the current collecting wiring 35 and the wiring protective layer 36 are formed.
- the current collector wiring 35 is formed by coating the metal particles constituting the current collector wiring between the porous oxide semiconductor layers 3a and 3b after forming the porous oxide semiconductor layers 3a and 3b. It can be obtained by heating and baking.
- the terminal 8 is preferably formed simultaneously with the current collecting wiring 35.
- the wiring protective layer 36 is made of, for example, a paste obtained by blending a thickener, a binder, a dispersant, a solvent, or the like with an inorganic insulating material such as the above-described low-melting glass frit as necessary, by a screen printing method. It can be obtained by coating the entire current collecting wiring 35 so as to cover it, heating and baking.
- the molten chemical resistant resin is applied to the wiring protective layer 36 and then naturally cooled at room temperature, or a film-like chemical resistant resin is applied.
- the chemical-resistant resin can be obtained by bringing the conductive resin into contact with the wiring protective layer 36, heating and melting the film-shaped chemical-resistant resin with an external heat source, and then naturally cooling at room temperature.
- the thermoplastic chemical-resistant resin for example, an ionomer or an ethylene-methacrylic acid copolymer is used.
- the chemical resistant resin is an ultraviolet curable resin
- an ultraviolet curable resin which is a precursor of the chemical resistant resin
- the above ultraviolet curable resin is cured by ultraviolet rays.
- a chemical resistant resin can be obtained.
- the chemical resistant resin is a water soluble resin
- the chemical resistant resin can be obtained by applying an aqueous solution containing the chemical resistant resin on the wiring protective layer 36.
- sealing step sealing is performed in the same manner as the sealing step of the first embodiment.
- the terminal 7 is formed in the terminal forming step.
- the terminal 7 is connected to the current collecting wiring 35 in the region 19 surrounded by the sealing material 14 of the metal plate 4. It is formed at the overlapping position.
- the terminals may be formed in the same manner as the terminal forming process in the first embodiment.
- heat transmitted to the electrolyte 5 through the counter electrode 12 is transmitted to the current collector wiring 35 in the terminal forming step.
- the current collection wiring 35 is comprised with a metal, it is excellent in thermal conductivity. And since it is provided from the area
- FIG. 4 is a schematic cross-sectional view showing the photoelectric conversion device of the present embodiment.
- current collection wiring 35 is provided from a position overlapping the sealing material 14 to the outside of the outer periphery of the sealing material 14, and is connected to the terminal 8.
- the terminal 7 is formed at a position where the sealing material 14 and the current collecting wiring 35 overlap when the metal plate 4 is viewed from a direction perpendicular to the surface of the metal plate 4.
- Such a photoelectric conversion element 130 is manufactured as follows.
- the porous oxide semiconductor layer 3 is formed in the same manner as in the first embodiment, and then the current collector wiring 35 is formed at a position overlapping the sealing material 14.
- the current collecting wiring 35 is formed around the porous oxide semiconductor layer 3 at a place where the sealing material 14 is to be formed. .
- the method of forming the current collector wiring 35 is the same method as the current collector wiring 35 of the third embodiment.
- the wiring protective layer 36 is formed.
- the wiring protective layer 36 may be formed by the same method as the wiring protective layer in the third embodiment.
- the terminal 8 is preferably formed simultaneously with the current collecting wiring 35.
- the working electrode 11 and the counter electrode 12 are overlapped and sealed so that the sealing material 14 and the current collecting wiring 35 overlap each other.
- the sealing method may be performed in the same manner as the sealing process in the first embodiment.
- the terminal 7 is formed at a position where the sealing material 14 and the current collecting wiring 35 overlap.
- the terminals may be formed in the same manner as in the first embodiment.
- heat transmitted to the sealing material 14 via the counter electrode 12 is transmitted to the current collector wiring 35 in the terminal forming step. Since the current collecting wiring 35 is provided from the position where it overlaps with the sealing material 14 to the outside of the outer periphery of the sealing material 14, the heat transmitted to the current collecting wiring 35 escapes to the outside of the outer periphery of the sealing material 14. For this reason, it can suppress that the heat transmitted to the sealing material 14 through the counter electrode 12 stays in the sealing material 14 or stays in the electrolyte 5 through the sealing material 14. Therefore, in the terminal formation step, deterioration of the sealing material 14, the photosensitizing dye, and the electrolyte 5 due to heat can be suppressed.
- the present embodiment is a photoelectric conversion element module using a photoelectric conversion element having the same configuration as the photoelectric conversion element 100 of the first embodiment.
- FIG. 5 is a schematic cross-sectional view showing the photoelectric conversion element module according to the present embodiment.
- the photoelectric conversion element module 200 includes a set of photoelectric conversion elements 100. Moreover, the photoelectric conversion elements 100 and 100 share one transparent substrate 2.
- one end of the conductive wire 9 is connected to the terminal 7 of one photoelectric conversion element 100 by solder 13. Furthermore, the other end of the conductive wire 9 is connected to the terminal 8 of the other photoelectric conversion element 100 by a solder 13. Thus, the pair of photoelectric conversion elements 100, 100 are connected in series.
- the conductive wire 9 is a wire made of a conductive material such as copper or solder, and can be a lead wire, a solder ribbon wire, or the like.
- the photoelectric conversion element module 200 can be manufactured as follows.
- photoelectric conversion element preparation step First, a set of photoelectric conversion elements 100 and 100 is prepared (photoelectric conversion element preparation step).
- Preparation of a set of photoelectric conversion elements is performed by first forming a set of transparent conductors 1 on the transparent substrate 2 in a preparation process for manufacturing the photoelectric conversion elements 100.
- the transparent conductor 1 may be formed in the same manner as the transparent conductor 1 in the first embodiment.
- a porous oxide semiconductor layer 3 is formed on each transparent conductor 1 by the same method as in the first embodiment, and a photosensitizing dye is carried.
- a plurality of counter electrodes are prepared by the same method as in the first embodiment.
- terminal 8 is formed on the working electrode 11 of each photoelectric conversion element 100 by the same method as in the first embodiment.
- the electrolyte 5 is sealed between each working electrode 11 and the counter electrode 12 by the same method as the sealing step in the first embodiment.
- the terminal 7 is formed on each counter electrode 12 by the same method as the terminal forming step in the first embodiment.
- the terminal 7 on the counter electrode 12 of one photoelectric conversion element 100 and the terminal 8 on the working electrode of the other photoelectric conversion element 100 are connected by a conductive wire 9 (connection process).
- one end of the conductive wire 9 is soldered to the terminal 7 on the counter electrode 12 of one photoelectric conversion element 100 by solder 13, and the other end of the conductive wire 9 is connected to the working electrode 11 of the other photoelectric conversion element 100. This is performed by soldering the terminals 8 with solder 13.
- the conductive wire 9 includes the terminal 7 formed on the surface of the counter electrode 12 opposite to the working electrode 11 after the photoelectric conversion elements 100 and 100 are manufactured. Since the terminals 8 formed on the transparent conductor 1 can be connected with the solder 13 from the same direction, the photoelectric conversion element module 200 can be easily manufactured. Moreover, the connection of the conductive wire 9 can be easily changed after the photoelectric conversion element module 200 is manufactured.
- the photoelectric conversion element module 200 has a strong connection between the photoelectric conversion elements 100, and can prevent the connection between the photoelectric conversion elements 100 from being disconnected due to an external force or the like.
- the photoelectric conversion element module 200 connects the conductive wires 9 with solder, thereby using a silver paste or the like between the working electrode 11 of one photoelectric conversion element 100 and the counter electrode 12 of the other photoelectric conversion element 100.
- the resistance can be reduced as compared with the case of electrical connection. Therefore, although the titanium plate is used as the counter electrode 12, the resistance can be reduced and the durability can be improved.
- FIG. 6 the same or equivalent components as those in the second embodiment and the fifth embodiment are denoted by the same reference numerals, and redundant description is omitted.
- This embodiment is a photoelectric conversion element module using a photoelectric conversion element having the same configuration as the photoelectric conversion element 110 of the set of the second embodiment.
- FIG. 6 is a schematic cross-sectional view showing the photoelectric conversion element module according to the present embodiment.
- the photoelectric conversion element module 210 includes a pair of photoelectric conversion elements 110 and 110. Moreover, the photoelectric conversion elements 110 and 110 share one transparent substrate 2.
- the terminal 7 on the counter electrode of one photoelectric conversion element 110 and the terminal 8 on the working electrode of the other photoelectric conversion element 100 are connected by a conductive adhesive 9a.
- the two photoelectric conversion elements 110 and 110 are connected in series.
- conductive adhesive 9a various metal pastes such as silver paste and carbon paste can be used.
- Such a photoelectric conversion element module 210 can be manufactured as follows.
- photoelectric conversion element preparation step First, a set of photoelectric conversion elements 110 and 110 is prepared (photoelectric conversion element preparation step).
- Preparation of a set of photoelectric conversion elements 110 and 110 is performed by forming a set of transparent conductors 1 on the transparent substrate 2 in a preparation process for manufacturing the photoelectric conversion element 110 in the second embodiment.
- the transparent conductor 1 can be formed by the same method as the formation of the transparent conductor 1 in the second embodiment.
- a porous oxide semiconductor layer 3 is formed on each transparent conductor 1 by the same method as in the second embodiment, and a photosensitizing dye is carried.
- the several counter electrode 12 is prepared by the method similar to 2nd Embodiment.
- the electrolyte 5 is sealed between each working electrode 11 and the counter electrode 12 by the same method as the sealing step in the second embodiment.
- the terminals 7 are formed on the extending portions 18a on the respective counter electrodes 12 by the same method as the terminal forming step in the second embodiment. Moreover, the terminal 8 is formed on the working electrode 11 of each photoelectric conversion element 110 by the method similar to 2nd Embodiment.
- the terminal 7 on the counter electrode 12 of one photoelectric conversion element 110 and the terminal 8 on the working electrode of the other photoelectric conversion element 110 are connected by the conductive adhesive 9a (connection process).
- the terminal 8 formed thereon can be connected from the same direction by the conductive adhesive 9a.
- the photoelectric conversion element module 210 can be manufactured easily.
- the connection of one photoelectric conversion element 110 and the other photoelectric conversion element 110 can be easily changed after manufacture of a photoelectric conversion element module.
- the conductive adhesive 9a can be firmly connected to the counter electrode 12 via the terminal 7.
- the present embodiment is a photoelectric conversion element module using a set of photoelectric conversion elements.
- FIG. 7 is a schematic cross-sectional view showing the photoelectric conversion element module according to the present embodiment.
- the photoelectric conversion element module 220 includes a pair of photoelectric conversion elements 110a and 110a.
- the photoelectric conversion element 110a is a second embodiment in that the terminal 15 is made of a high melting point solder, and the terminal 15 is formed from the surface opposite to the working electrode 11 side of the counter electrode 12 to the surface on the working electrode 11 side. It differs from the photoelectric conversion element 110 of the form. Further, in the photoelectric conversion element module 220, the terminal 15 formed on the counter electrode 12 of one photoelectric conversion element 110 a and the terminal 8 formed on the working electrode 11 of the other photoelectric conversion element 110 a have the surface of the counter electrode 12. When the counter electrode 12 is viewed from a direction perpendicular to the direction, they overlap each other.
- the terminal 15 of one photoelectric conversion element 110 a and the terminal 8 on the other working electrode 11 are connected by solder 16.
- the solder 16 is preferably composed of low melting point solder.
- Such a photoelectric conversion element can be manufactured as follows.
- photoelectric conversion element preparation step First, a set of photoelectric conversion elements 110a and 110a is prepared (photoelectric conversion element preparation step).
- Preparation of a set of photoelectric conversion elements 110a and 110a is performed by first preparing a working electrode and a counter electrode in the same manner as the preparation step in the fifth embodiment.
- the terminal 15 is formed with a high melting point solder from one surface of the counter electrode 12 to the other surface at the end of the region that becomes the extending portion 18a of the counter electrode 12.
- the terminal 15 may be formed in the same manner as the terminal 7 is formed with the high melting point solder in the second embodiment.
- the catalyst layer 6 is formed on the working electrode 11 side in the extending portion 18a of the counter electrode 12, the catalyst layer 6 is destroyed by applying ultrasonic waves to the high melting point solder. Therefore, the high melting point solder is directly formed on the metal plate 4 of the counter electrode 12 on the working electrode 11 side in the extending portion 18a.
- the terminal 8 is formed outside the region that is expected to be surrounded by the outer periphery of the sealing material 14.
- the terminal 8 may be formed in the same manner as the terminal 8 in the second embodiment.
- a solder 16 made of low melting point solder is provided on the terminal 8.
- the counter electrode 12 and the working electrode 11 are overlapped so that the terminal 15 formed on one counter electrode 12 and the solder 16 of the terminal 8 formed on the working electrode 11 serving as the other photoelectric conversion element are in contact with each other.
- the electrolyte 5 is sealed between each working electrode 11 and the counter electrode 12 by the same method as the sealing step in the second embodiment.
- the terminal 15 and the solder 16 are connected by heating the solder 16 (connection process).
- the photoelectric conversion element module 220 can firmly join the counter electrode 12 of one photoelectric conversion element 110a to the other photoelectric conversion element 110a via the terminal 15 and the solder 16. Moreover, electrical connectivity can be improved by adopting soldering. Therefore, although the metal plate 4 of the counter electrode 12 is made of titanium, the electrical connectivity and durability can be improved. In addition, since the terminals 15 and the solder 16 are made of solder, they are easy to form and are inexpensive, so that manufacturing can be facilitated and costs can be reduced. Further, in the photoelectric conversion element module 220, the extension portion 18a located outside the region surrounded by the outer periphery of the sealing material 14 in one photoelectric conversion element 110a is connected to the other photoelectric conversion element 110a. It is possible to suppress the porous oxide semiconductor layer 3 and the electrolyte 5 from becoming high temperature during soldering, and to suppress the deterioration of the porous oxide semiconductor layer 3 and the electrolyte 5.
- the terminal forming step is performed after the sealing step, but the present invention is not limited to this.
- a terminal formation process may be performed before the sealing process.
- the terminal 7 is formed on one surface of the counter electrode 12 before sealing.
- the terminals may be formed in the same manner as the terminal forming process in the first embodiment.
- the sealing step in the first embodiment may be performed in the same manner.
- the porous oxide semiconductor layer 3 is formed on the second electrode 20.
- the working electrode 11 is composed of the second electrode 20 and the porous oxide semiconductor layer 3 carrying the photosensitizing dye
- the counter electrode 12 is composed of the first electrode 10.
- the present invention is not limited thereto, and the porous oxide semiconductor layer 3 is formed on the first electrode 10, and the working electrode 11 is a porous oxide on which the first electrode 10 and the photosensitizing dye are supported.
- the counter electrode 12 may be composed of the second electrode 20 and the semiconductor layer 3.
- FIG. 8 is a cross-sectional view showing such a modification of the photoelectric conversion element 100 shown in FIG.
- the 1st electrode 10 is comprised with the metal plate 4, and the working electrode 11 is comprised with the 1st electrode 10 and the porous oxide semiconductor layer 3 with which a photosensitizing dye is carry
- the second electrode 20 is composed of the transparent substrate 2, the transparent conductor 1, and the catalyst layer 6 provided on the transparent conductor 1, and the counter electrode 12 is composed of the second electrode 20.
- the catalyst layer 6 is made of, for example, platinum or the like that is thinly formed so that light can be transmitted.
- the manufacture of the photoelectric conversion element 140 is performed as follows. First, the 1st electrode 10 comprised from the metal plate 4 is prepared. Next, a porous oxide semiconductor layer is formed on the first electrode 10. The method for forming the porous oxide semiconductor layer 3 may be performed in the same manner as the semiconductor forming step in the first embodiment. Next, a photosensitizing dye is supported on the porous oxide semiconductor layer 3. The photosensitizing dye may be supported in the same manner as the dye supporting process in the first embodiment. Thus, the working electrode 11 in which the porous oxide semiconductor layer 3 is formed on the first electrode 10 is obtained.
- the counter electrode 12 is prepared.
- the counter electrode 12 is prepared by forming the transparent conductor 1 on the transparent substrate 2 and forming the catalyst layer 6 on the transparent conductor 1 to form the second electrode.
- the method for forming the transparent conductor 1 may be performed in the same manner as the method for forming the transparent conductor 1 on the transparent substrate 2 in the first embodiment.
- a method similar to the method of forming the catalyst layer on the metal plate 4 may be performed.
- the second electrode thus obtained becomes the counter electrode 12.
- the porous oxide semiconductor layer 3 and the electrolyte 5 are sealed with the sealing material 14 between the working electrode 11 and the counter electrode 12.
- the sealing method may be performed in the same manner as the sealing process in the first embodiment.
- the terminal 7 is formed.
- the terminal 7 may be formed in the same manner as the terminal forming process in the first embodiment. Other processes are the same as those in the first embodiment.
- the terminal 7 is formed after the sealing step in the above, but the terminal 7 may be formed before the sealing step. By doing so, heat in the terminal forming process is not conducted to the electrolyte 5, and deterioration of the electrolyte 5 due to heat in the terminal forming process can be prevented.
- the terminal 7 may be formed before the dye supporting step. By doing so, heat in the terminal forming step is not conducted to the photosensitizing dye, and deterioration of the photosensitizing dye due to heat in the terminal forming step can be prevented.
- the photoelectric conversion element module includes a set of photoelectric conversion elements, but the photoelectric conversion element module of the present invention may include three or more photoelectric conversion elements. Good. In a photoelectric conversion element module having three or more photoelectric conversion elements, when two of the photoelectric conversion elements are connected to each other by a conductive line, the photoelectric conversion element to which the conductive line is connected is easily changed after the element is assembled. Can do.
- the terminal 7 is formed on the metal plate 4 on the side opposite to the working electrode 11 side of the counter electrode 12, but the terminal 7 is on the working electrode 11 side of the counter electrode 12. It may be provided on the metal plate 4. In order to provide the terminal 7 on the metal plate 4 on the working electrode 11 side of the counter electrode 12, the terminal 7 may be provided on the working electrode 11 side of the counter electrode 12 in the terminal forming step in the second embodiment.
- the catalyst layer 6 is formed on the working electrode 11 side of the counter electrode 12, but when the ultrasonic wave is applied to the high melting point solder in the terminal formation step, the catalyst layer 6 is destroyed and the terminal 7 is replaced with the metal plate 4. Can be formed on top.
- the terminal 7 may be formed from the side opposite to the working electrode 11 side of the counter electrode 12 to the working electrode 11 side of the counter electrode 12.
- the method of forming the terminal 7 may be performed in the same manner as the formation of the terminal 15 in the seventh embodiment.
- the 2nd electrode was comprised from the transparent conductor 1 provided on the transparent base material 2 and the transparent base material 2, it may be comprised with the conductive glass as a transparent conductor.
- Titanium foil with a thickness of 40 ⁇ m was prepared as a metal plate.
- the high melting point solder shown in Table 1 was used for one part of this titanium foil, the high melting point solder was melted with an ultrasonic soldering iron, and then solidified to form a terminal. At this time, the temperature of the high melting point solder in the molten state was set to a temperature higher than the melting point shown in Table 1, and the ultrasonic vibration frequency was set to 10 kHz.
- the lead wires were soldered onto the terminals using the joining solder shown in Table 1.
- the material of the lead wire is copper.
- Example 9 Copper was coated on the same metal plate as in Example 1 to a thickness of 1 ⁇ m by sputtering. A lead wire was soldered to this coating in the same manner as in Example 1. Next, as in Example 1, a tensile force was applied to the lead wire.
- the terminal can be easily and firmly formed on the counter electrode composed of the titanium plate without using a vacuum device for forming the terminal.
- Example 7 The photoelectric conversion element module shown in FIG. 7 was produced.
- Counter electrode A conductive film made of Pt formed on a titanium foil having a thickness of 40 ⁇ m by a sputtering method was used as a counter electrode. A terminal was formed in the extended portion of the counter electrode of the photoelectric conversion element. For forming the terminals, Cerasolzer # 297 was used as a high melting point solder. When forming the terminals, the temperature was set higher than the melting point solder higher than the melting point, and ultrasonic waves with a vibration frequency of 60 kHz were applied.
- the extension part of one photoelectric conversion element was provided with solder on the terminal on the working electrode of the other photoelectric conversion element.
- Assembly of photoelectric conversion element Combine the working electrode and the counter electrode so that the terminal formed on the counter electrode serving as one photoelectric conversion element and the terminal on the working electrode serving as the other photoelectric conversion element overlap.
- An electrolyte layer was formed by injecting an electrolyte into and sealing.
- connection using the silver paste was performed by applying the silver paste to the extending portion of one photoelectric conversion element and the terminal on the working electrode of the other photoelectric conversion element, and placing the paste at 80 ° C. for 1 hour.
- the measurement result of the photoelectric conversion efficiency of only one photoelectric conversion element is also shown.
- Example 7 As shown in Table 2, the photoelectric conversion efficiency of Example 7 was superior to the photoelectric conversion efficiency of Comparative Example 10. This is presumably because, in Example 7, the electrical connectivity between the terminal on the counter electrode of one photoelectric conversion element and the terminal on the working electrode of the other photoelectric conversion element is good.
- Example 7 can easily produce a photoelectric conversion element module using a photoelectric conversion element having a terminal on the counter electrode, and that the photoelectric conversion efficiency of the photoelectric conversion element module is good.
- the manufacturing method of the photoelectric conversion element which can manufacture easily a photoelectric conversion element provided with the terminal firmly joined with the electrode which uses titanium, the photoelectric conversion element manufactured by it, and a photoelectric conversion element A module manufacturing method and a photoelectric conversion element module manufactured thereby are provided.
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Abstract
Description
図1は、本発明の第1実施形態にかかる光電変換素子を示す概略断面図である。
作用極11は、透明基材2及び透明基材2の一方の面に設けられる透明導電体1から成る第2電極20と、透明導電体1上に設けられ、光増感色素が担持される多孔質酸化物半導体層3とを備える。
電解質5は、多孔質酸化物半導体層3内に電解液を含浸させてなるものか、または、多孔質酸化物半導体層3内に電解液を含浸させた後に、この電解液を適当なゲル化剤を用いてゲル化(擬固体化)して、多孔質酸化物半導体層3と一体に形成されてなるもの、あるいは、イオン性液体、酸化物半導体粒子若しくは導電性粒子を含むゲル状の電解質を用いることができる。
対極12は、第1電極10により構成される。第1電極は、チタンまたはチタン合金からなる金属板4と触媒層6とで構成される。なお、還元反応を促進する触媒層6は、金属板4における作用極11側の表面に形成される。触媒層6は、白金や炭素などからなる。
封止材14は、作用極11と対極12とを連結しており、作用極11と対極12との間の電解質5は、封止材14によって包囲されることで封止される。封止材14を構成する材料としては、例えばアイオノマー、エチレン-ビニル酢酸無水物共重合体、エチレン-メタクリル酸共重合体、エチレン-ビニルアルコール共重合体、紫外線硬化樹脂、及び、ビニルアルコール重合体が挙げられる。なお、封止材14は樹脂のみで構成されてもよいし、樹脂と無機フィラーとで構成されていてもよい。
対極12における作用極11側とは反対側の表面、すなわち第1電極10の金属板4の表面には、端子7が形成される。端子7は、高融点はんだから構成される。
次に、本発明の光電変換装置の第2実施形態について図2を用いて説明する。なお、図2において、第1実施形態と同一又は同等の構成要素については同一符号を付し、重複する説明を省略する。
次に、本発明の光電変換装置の第3実施形態について図3を用いて説明する。なお、図3において、第1実施形態と同一又は同等の構成要素については同一符号を付し、重複する説明を省略する。
次に、本発明の光電変換装置の第4実施形態について図4を用いて説明する。なお、図4において、第1実施形態、第3実施形態と同一又は同等の構成要素については同一符号を付し、重複する説明を省略する。
次に、本発明の第5実施形態について、図5を用いて説明する。なお、図5において、第1実施形態と同一又は同等の構成要素については同一符号を付し、重複する説明を省略する。本実施形態は、第1実施形態の光電変換素子100と同様の構成の光電変換素子を用いた光電変換素子モジュールである。
次に本発明の第6実施形態について図6を用いて説明する。なお、図6において、第2実施形態、第5実施形態と同一又は同等の構成要素については同一符号を付し、重複する説明を省略する。本実施形態は、一組の第2実施形態の光電変換素子110と同様の構成の光電変換素子を用いた光電変換素子モジュールである。
次に本発明の第7実施形態について図7を用いて説明する。なお、図7において、第2実施形態、第6実施形態と同一又は同等の構成要素については同一符号を付し、重複する説明を省略する。本実施形態は、一組の光電変換素子を用いた光電変換素子モジュールである。
端子を高融点はんだにより形成する場合において、端子と金属板との接合強度を確認するため、次の検討を行った。
端子を表1に示す低融点はんだにより形成したこと以外は、実施例1と同様に行った。
表1に示す高融点はんだを用いて、端子と金属板上に形成した。このとき高融点はんだに超音波を印加しないこと以外については、実施例1と同様にして接合した。次に表1に示す接合用のはんだを用いて、リード線をはんだ付けした。
実施例1と同様の金属板に銅を厚さ1μmとなるようにスパッタで被膜した。この被膜に、実施例1と同様にしてリード線をはんだ付けした。次に実施例1と同様にリード線に引張力を与えた。
図7に示す光電変換素子モジュールを作製した。
端子及びはんだを使用せず、これに代えて一方の光電変換素子の延設部と他方の光電変換素子の作用極上の端子とを銀ペーストにより接続したこと以外は実施例7と同様にして光電変換素子モジュールを作製した。
2・・・透明基材
3、3a、3b・・・多孔質酸化物半導体層
5・・・電解質
7・・・端子
8・・・端子
9・・・導電線
9a・・・導電性接着剤
10・・・第1電極
11・・・作用極
12・・・対極
14・・・封止材
20・・・第2電極
35・・・集電配線
100、110、120、130、140・・・光電変換素子
200、210、220・・・光電変換素子モジュール
Claims (13)
- チタン或いはチタンを含む合金からなる金属板と触媒層とを有する第1電極における前記触媒層の表面上、又は、透明導電体を有する第2電極の前記透明導電体の表面上に、多孔質酸化物半導体層を形成する半導体形成工程と、
前記多孔質酸化物半導体層に光増感色素を担持させる色素担持工程と、
前記第1電極と前記第2電極との間に前記多孔質酸化物半導体層及び電解質を封止材により包囲して封止する封止工程と、
前記第1電極における前記封止材の外周により包囲される表面以外の表面において、前記金属板上に端子を形成する端子形成工程と、
を備え、
前記端子形成工程において、前記端子は、高融点はんだが加熱されて溶融されると共に超音波が印加されて形成される
ことを特徴とする光電変換素子の製造方法。 - 前記多孔質酸化物半導体層は、前記透明導電体上に形成されることを特徴とする請求項1に記載の光電変換素子の製造方法。
- 前記第1電極は、前記第1電極の表面に対して垂直な方向から前記第1電極を見た場合に、前記封止材の外周により包囲される領域よりも外側に延設される延設部を有し、
前記端子は、前記延設部に形成される
ことを特徴とする請求項1または2に記載の光電変換素子の製造方法。 - 前記端子は、前記第1電極における前記第2電極側と反対側の表面から前記第2電極側の表面にかけて形成されることを特徴とする請求項3に記載の光電変換素子の製造方法。
- 前記第2電極における前記第1電極側の表面上には、前記封止材により包囲される領域から前記封止剤の外周の外側にかけて金属からなる集電配線が設けられており、
前記端子は、前記第1電極の表面に対して垂直な方向から前記第1電極を見た場合に、前記第1電極の前記第2電極側とは反対側の表面上における前記封止材により包囲される領域において、前記集電配線と重なる位置に形成される
ことを特徴とする請求項1または2に記載の光電変換素子の製造方法。 - 前記第2電極における前記第1電極側の表面上には、前記封止材と重なる領域から前記封止材の外周の外側にかけて金属からなる集電配線が設けられており、
前記端子は、前記第1電極の表面に対して垂直な方向から前記第1電極を見た場合に、前記第1電極の前記第2電極側とは反対側の表面上における前記封止材と重なる領域において、前記集電配線と重なる位置に形成されることを特徴とする請求項1または2に記載の光電変換素子の製造方法。 - チタン或いはチタンを含む合金からなる金属板と触媒層とを有する第1電極における前記金属板の表面上に端子を形成する端子形成工程と、
透明導電体を有する第2電極の前記透明導電体の表面上に多孔質酸化物半導体層を形成する半導体形成工程と、
前記多孔質酸化物半導体層に光増感色素を担持させる色素担持工程と、
前記第1電極と前記第2電極とを対面させ、前記第1電極と前記第2電極との間に前記多孔質酸化物半導体層と電解質とが封止材により包囲され、前記端子が前記封止材により包囲されないようにして封止する封止工程と、
を備え、
前記端子形成工程において、前記端子は、高融点はんだが加熱されて溶融されると共に超音波が印加されて形成される
ことを特徴とする光電変換素子の製造方法。 - チタン或いはチタンを含む合金からなる金属板と触媒層とを有する第1電極における前記触媒層の表面上に多孔質酸化物半導体層を形成する半導体形成工程と、
前記多孔質酸化物半導体層に光増感色素を担持させる色素担持工程と、
前記第1電極の表面上における前記多孔質半導体が形成されない領域において、前記金属板上に端子を形成する端子形成工程と、
透明導電体を有する第2電極と前記第1電極とを対面させ、前記第1電極と前記第2電極との間に前記多孔質酸化物半導体層と電解質とが封止材により包囲され、前記端子が前記封止材により包囲されないようにして封止する封止工程と、
を備え、
前記端子形成工程において、前記端子は、高融点はんだが加熱されると共に超音波が印加されて形成される
ことを特徴とする光電変換素子の製造方法。 - 前記端子形成工程は、前記色素担持工程の前にあることを特徴とする請求項8に記載の光電変換素子の製造方法。
- 請求項1から9のいずれか1項に記載の光電変換素子の製造方法により製造されることを特徴とする光電変換素子。
- 請求項1から9のいずれか1項に記載の光電変換素子の製造方法により製造される光電変換素子を複数準備する光電変換素子準備工程を備え、
少なくとも1つの前記光電変換素子における前記第1電極上に形成される端子と、他の少なくとも1つの光電変換素子における前記第2電極とを導電部材により電気的に接続する接続工程を有することを特徴とする光電変換素子モジュールの製造方法。 - 前記光電変換素子は、前記第2電極の前記第1電極側の表面上における前記封止材の外周により包囲される領域の外側に端子が形成され、
少なくとも1つの前記光電変換素子における前記第1電極上に形成される端子と、他の少なくとも1つの光電変換素子における第2電極上に形成される端子とを前記導電部材により接続することを特徴とする請求項11に記載の光電変換素子モジュールの製造方法。 - 請求項11または12に記載の光電変換素子モジュールの製造方法により製造されることを特徴とする光電変換素子モジュール。
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JP2012182038A (ja) * | 2011-03-02 | 2012-09-20 | Fujikura Ltd | 色素増感太陽電池、その製造方法、色素増感太陽電池モジュール及びその製造方法 |
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JP2014053111A (ja) * | 2012-09-05 | 2014-03-20 | Fujikura Ltd | 色素増感太陽電池モジュール |
US9257237B2 (en) | 2010-04-13 | 2016-02-09 | Fujikura Ltd. | Dye-sensitized solar cell module and manufacturing method for same |
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AU2009241138B2 (en) | 2012-02-02 |
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