Classifications

• • 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
  • H01L31/0248—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 characterised by their semiconductor bodies
  • H01L31/036—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 characterised by their semiconductor bodies characterised by their crystalline structure or particular orientation of the crystalline planes
  • H01L31/0392—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 characterised by their semiconductor bodies characterised by their crystalline structure or particular orientation of the crystalline planes including thin films deposited on metallic or insulating substrates ; characterised by specific substrate materials or substrate features or by the presence of intermediate layers, e.g. barrier layers, on the substrate
  • H01L31/03923—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 characterised by their semiconductor bodies characterised by their crystalline structure or particular orientation of the crystalline planes including thin films deposited on metallic or insulating substrates ; characterised by specific substrate materials or substrate features or by the presence of intermediate layers, e.g. barrier layers, on the substrate including AIBIIICVI compound materials, e.g. CIS, CIGS
• • C—CHEMISTRY; METALLURGY
  • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
  • C08G—MACROMOLECULAR COMPOUNDS OBTAINED OTHERWISE THAN BY REACTIONS ONLY INVOLVING UNSATURATED CARBON-TO-CARBON BONDS
  • C08G77/00—Macromolecular compounds obtained by reactions forming a linkage containing silicon with or without sulfur, nitrogen, oxygen or carbon in the main chain of the macromolecule
  • C08G77/60—Macromolecular compounds obtained by reactions forming a linkage containing silicon with or without sulfur, nitrogen, oxygen or carbon in the main chain of the macromolecule in which all the silicon atoms are connected by linkages other than oxygen atoms
  • C08G77/62—Nitrogen atoms
• • C—CHEMISTRY; METALLURGY
  • C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
  • C09D—COATING COMPOSITIONS, e.g. PAINTS, VARNISHES OR LACQUERS; FILLING PASTES; CHEMICAL PAINT OR INK REMOVERS; INKS; CORRECTING FLUIDS; WOODSTAINS; PASTES OR SOLIDS FOR COLOURING OR PRINTING; USE OF MATERIALS THEREFOR
  • C09D183/00—Coating compositions based on macromolecular compounds obtained by reactions forming in the main chain of the macromolecule a linkage containing silicon, with or without sulfur, nitrogen, oxygen, or carbon only; Coating compositions based on derivatives of such polymers
  • C09D183/16—Coating compositions based on macromolecular compounds obtained by reactions forming in the main chain of the macromolecule a linkage containing silicon, with or without sulfur, nitrogen, oxygen, or carbon only; Coating compositions based on derivatives of such polymers in which all the silicon atoms are connected by linkages other than oxygen atoms
• • 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
  • H01L31/072—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 heterojunction type
  • H01L31/0749—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 heterojunction type including a AIBIIICVI compound, e.g. CdS/CulnSe2 [CIS] heterojunction 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
  • 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 chalcopyrite solar cell comprising a substrate and a photovoltaic layer structure.
• a chalcopyrite solar cell comprising a substrate and a photovoltaic layer structure.
• it is a thin-film solar cell with a photovoltaic layer structure of the copper-indium-sulfide (CIS) or copper-indium-gallium-selenide (CIGSe) type.
• CIS copper-indium-sulfide
• CGSe copper-indium-gallium-selenide
• the invention relates to a process for the preparation of solar cells based on chalcopyrite.
• the solar cell is equipped with an encapsulation layer, which is prepared by curing a solution of
• Polysilazanes and additives at a temperature in the range of 20 to 1000 0 C, in particular 80 to 200 0 C is generated.
• Solar cells convert sunlight into electricity.
• Predominantly crystalline or amorphous silicon is used as a light-absorbing semiconductive material in solar cells.
• the use of silicon is associated with considerable costs.
• thin film solar cells can be made with an absorber of a chalcopyrcrical material such as copper indium sulfide (CIS) or copper indium gallium selenide (CIGSe) at a substantially lower cost.
• CIS copper indium sulfide
• CGSe copper indium gallium selenide
• the efficiency of a solar cell is defined as the ratio of electrical power, ie the product of voltage and photocurrent, to incident light power.
• the efficiency is proportional to the number of photons that can penetrate into the absorber layer and contribute to the generation of electron-hole pairs.
• Photons, which are reflected on the surface of the solar cell do not contribute to the photocurrent. Accordingly, the efficiency can be reduced by a reduction the light reflection at the surface of the solar cell can be increased.
• the lifetime of solar cells can be extended by improved protection against weather-related degradation processes. Penetrating water or water vapor accelerates the degradation processes.
• the prior art therefore uses an encapsulation of a layer composite which comprises glass and EVA and optionally PVA and other polymer films.
• SiO x layers are deposited from the gas phase by CVD methods such as microwave plasma assisted vapor deposition (MWPECVD) and PVD methods such as magnetron sputtering. These vacuum techniques are associated with high costs and also have the disadvantage that the layers produced therewith a low
• CVD processes also require the use of highly flammable (SiHU, CH 4 , H 2 ) and toxic (NH 3 ) gases.
• Glass As substrate materials for chalcopyrite solar cells glass or films of metal or polyimide are used. Glass proves to be advantageous in several respects because it is electrically insulating, has a smooth surface and, during the production of the chalcopyrite absorber layer, provides sodium, which diffuses out of the glass into the absorber layer and serves as dopant Properties of the absorber layer improved.
• a disadvantage of glass is its great weight and lack of flexibility.
• glass substrates can not be coated in cost-effective roll-to-roll processes because of their rigidity.
• Film-like substrates made of metal or plastic are lighter than glass and flexible, so that they are suitable for the production of solar cells by means of a cost-effective roll-to-roll process.
• metal or plastic films may adversely affect the property of the chalcopyrite layer composite and, moreover, do not have a sodium depot for absorber doping. Because of the elevated temperatures (in some cases above 500 ° C.) to which the substrate is exposed during the production of the solar cells, metal foils of steel or titanium are preferably used.
• the photovoltaic layer structure or the back contact must be electrically insulated from the substrate film.
• Substrate film applied a layer of an electrically insulating material.
• This electrically insulating layer should also act as a diffusion barrier to prevent the diffusion of metal ions that can damage the absorber layer.
• metal ions For example, iron atoms can increase the recombination rate of charge carriers (electrons and holes) in chalcopyrite absorber layers, thereby decreasing the photocurrent.
• the material used for insulating and diffusion-inhibiting barrier layers is silicon oxide (SiO x ).
• protective or encapsulation layers which essentially consist of SiO x or SiN x , for electronic components and solar cells based on silicon or other semiconductor materials.
• US 7,067,069 discloses an insulating encapsulation layer of SiO 2 for silicon-based solar cells, wherein the SiO 2 layer is produced by applying polysilanes and subsequent curing at a temperature of 100 to 800 0 C, preferably from 300 to 500 ° C.
• US Pat. No. 6,501,014 B1 relates to articles, in particular solar cells based on amorphous silicon, having a transparent, heat-resistant and weather-resistant protective layer of a silicate-like material.
• the protective layer is easily produced by using a polysilazane solution. Between the protective layer based on polysilazane and the photovoltaic layer system, a flexible rubber-like adhesive or buffer layer is arranged.
• No. 7,396,563 teaches the deposition of dielectric and passivating polysilazane layers by means of PA-CVD, wherein polysilanes are used as CVD precursor.
• US 4,751,191 discloses the deposition of polysilazane layers for solar cells by means of PA-CVD.
• the resulting polysilazane layer is patterned photolithographically and serves to mask metaiischen contacts as well as antirefiex harsh.
• the solar cells described in the prior art with encapsulation layers of SiO x or SiN x are expensive to produce and require the use of two- or multi-layer composite layers, which comprise a carrier film, a buffer layer, a primer layer and / or a reflector layer in addition to the encapsulation layer.
• buffer layers are required which compensate for the thermal mismatch with the encapsulation layer. Thermal mismatch, ie differences in the coefficient of thermal expansion of adjacent layers, induce mechanical stresses that often lead to cracking and peeling.
• this problem is counteracted by the fact that the encapsulation layer is deposited on the solar cell at low temperatures.
• such low-temperature encapsulant layers usually have insufficient barrier to water vapor and oxygen.
• the present invention has the object, a chalcopyrite solar cell with high efficiency and high durability against aging and to create a cost-effective process for their production.
• a chalcopyrite solar cell comprising a substrate, a photovoltaic layer structure and a polysilazane-based encapsulation layer.
• FIG. 1 shows a perspective section of a solar cell
• FIG. 2 shows reflection curves of a solar cell without and with encapsulation layer.
• the solar cell 10 is preferably configured as a thin-film solar cell and has a photovoltaic layer structure 4 of the copper Indium sulfide (CIS) or copper indium gallium selenide (CIGSe).
• CIS copper Indium sulfide
• CGSe copper indium gallium selenide
• the encapsulation layer 5 has a first and a second surface which lie opposite one another.
• the first surface of the encapsulation layer directly adjoins the photovoltaic layer structure 4 and the second surface of the encapsulation layer forms the outside of the solar cell.
• Layer structure 4 of the type copper indium sulfide (CIS) or copper indium gallium selenide (CIGSe) has; the photovoltaic layer structure 4 has a back contact 41 made of molybdenum, an absorber 42 of composition CuInSe 2 , CuInS 2 , CuGaSe 2 , CuIn 1-x Ga x Se 2 with 0 ⁇ x ⁇ 0.5 or Cu (InGa) (Sei -Y Sy ) 2 with 0 ⁇ y ⁇ 1.
• the substrate 1 is made of a material containing metal, metal alloys, glass, ceramic or plastic; - The substrate 1 is formed as a film, in particular as a steel or titanium foil;
• the encapsulation layer 5 has a thickness of from 100 to 3,000 nm, preferably from 200 to 2,500 nm, and in particular from 300 to 2,000 nm; the substrate 1 consists of an electrically conductive material and that one or more of the layers making up the photovoltaic
• Layer structure 4 composed, has been deposited by electrodeposition
• the solar cell 10 comprises a polysilazane-based barrier layer 2 arranged between the substrate 1 and the photovoltaic layer structure 4; the barrier layer 2 contains sodium or comprises a sodium-containing precursor layer 21;
• the encapsulation layer 5 and optionally the barrier layer 2 consists of a cured solution of polysilazanes and additives in a solvent, which is preferably dibutyl ether; the polysilazanes have the general structural formula (I)
• R 1 , R", R " 1 are identical or different and independently of one another represent hydrogen or an optionally substituted alkyl, aryl, vinyl or (trialkoxysilyl) alkyl radical, wherein n is an integer and n is such that the
• Polysilazane has a number average molecular weight of 150 to 150,000 g / mol, preferably 50,000 to 150,000 g / mol, and more preferably 100,000 to 150,000 g / mol;
• the solar cell 10 for light in the wavelength range of 300 to 900 nm has an average relative reflectivity of less than 97%, preferably less than 96%, and in particular less than 95%. based on the reflectivity of the solar cell 10 before application of the
• the solar cell 10 has a mean relative reflectivity of more than 120%, preferably more than 150%, and in particular more than 200% for light in the wavelength range from 1100 to 1500 nm, based on the reflectivity of the solar cell 10 before application of the solar cell
• FIG. 2 shows the results of a measurement of the spectral reflectivities of a chalcopyrite solar cell with and without a polysilazane-based encapsulation layer according to the invention (denoted in FIG. 2 by a solid "with SiO x " and a dashed line "without SiO x ").
• the spectral reflectivities are measured on the basis of DiN EN ISO 8980-4 on solar cells according to the invention with encapsulation layer and on reference solar cells without encapsulation layer.
• the inventive and the reference solar cells have - apart from the encapsulation layer - the same structure and have undergone the same manufacturing process.
• the spectral reflection curves obtained are superimposed and recorded in two wavelength intervals of 300 to
• the quotient of the reflection values of the solar cell according to the invention and the reference solar cell is calculated in each of the abovementioned wavelength intervals at equidistant support points whose distance from one another can be selected in the range from 1 to 20 nm, and the average of the quotients of all interpolation points contained in the interval educated.
• the solar cells according to the invention have an average relative reflectivity of less than 97% to less than 95%.
• the reflectivity is a factor in the external quantum efficiency (EQE) and the efficiency of a solar cell.
• the encapsulation layer according to the invention increases the external quantum efficiency of a solar cell on average by more than 3% to more than 5% compared with a reference solar cell.
• the mean reflectivity is raised by a maximum of 2% relative to the reference.
• the efficiency of a conventional chalcopyrite solar cell can be increased by a factor of 1.01 to 1. 03. With an efficiency of, for example, 15%, this corresponds to an improvement of more than 0.15% to 0.45%.
• the efficiency of chalcopyrite solar cells drops with increasing temperature. Due to increased reflectivity for infrared light, the encapsulation layer according to the invention reduces the heating of the solar cell caused by solar radiation and thus also contributes to an improvement in the efficiency in this way. In the wavelength range of 1100 to 1500 nm, the solar cell according to the invention has an average relative reflectivity of greater than 120% to more than 200%.
• solar cells of the invention exhibit after 800 h an efficiency of greater than 70%, preferably greater than 75%, and especially greater than 80%, based on the initial value, ie before the start of the aging test.
• the method for producing the solar cells according to the invention comprises the following steps a) to f): a) applying a chalcopyrite-based photovoltaic layer structure to a substrate optionally provided with a barrier layer, b) coating the photovoltaic layer structure with a solution containing at least one polysilazane general formula (I) - (SiR 1 R "-NR"') n- (I) wherein R 1, R ", R” 1 are identical or different and are independently hydrogen or an optionally substituted alkyl, aryl, vinyl or (trialkoxysilyl) alkyl radical, wherein n is an integer and n is such that the polysilazane has a number average molecular weight of 150 to 150,000 g / mol, preferably from 50,000 to 150,000 g / mol, and in particular from 100,000 to 150,000 g / mol, c) removing the solvent by evaporation to obtain a polysilazane layer having a thickness of from 100
• the chalcopyrite solar cells are fabricated on a flexible web-like substrate in a roll-to-roll process.
• the proportion of polysilazane is from 1 to 80% by weight, preferably from 2 to 50% by weight, and in particular from 5 to 20% by weight, based on the total weight of the solution.
• Particularly suitable solvents are organic, preferably aprotic, solvents which contain no water and no reactive groups such as hydroxyl or amino groups and which are inert to the polysilazane.
• aromatic or aliphatic hydrocarbons and mixtures thereof are, for example, aliphatic or aromatic hydrocarbons, halogenated hydrocarbons, esters such as ethyl acetate or butyl acetate, ketones such as acetone or methyl ethyl ketone, ethers such as tetrahydrofuran or dibutyl ether, and mono- and polyalkylene glycol dialkyl ethers (glymes) or mixtures of these solvents.
• Additional constituents of the polysilazane solution may be catalysts, for example organic amines, acids, as well as metals or metal salts or mixtures of these compounds, which accelerate the layer formation process.
• catalysts for example organic amines, acids, as well as metals or metal salts or mixtures of these compounds, which accelerate the layer formation process.
• Particularly suitable amine catalysts are N, N-diethylethanolamine, N, N-dimethylethanolamine, N, N-dimethylpropanolamine, triethylamine, triethanolamine and 3-morpholinopropylamine.
• the catalysts are preferably used in amounts of from 0.001 to 10% by weight, in particular from 0.01 to 6% by weight, particularly preferably from 0.1 to 5% by weight, based on the weight of the polysilazane.
• Further constituents may be additives for substrate wetting and film formation as well as inorganic nanoparticles of oxides such as SiO 2 , TiO 2 , ZnO, ZrO 2 or Al 2 O 3 .
• a chalcopyrite-based photovoltaic layer structure according to known methods is produced on a substrate such as a steel foil.
• the steel foil is preferably provided with an electrically insulating layer, in particular an SiO x barrier layer based on polysilazane.
• an approximately 1 ⁇ m thick molybdenum layer is deposited by means of DC magnetron sputtering and preferably structured for a monolithic interconnection (P1 cut).
• P1 cut monolithic interconnection
• the preparation of the chalcopyrite absorber layer is preferably carried out in a 3-stage PVD process at a pressure of about 3-10 6 mbar.
• the total duration of the PVD process is approximately 1.5 h. It is advantageous here to guide the processes such that the substrate assumes a maximum temperature below 400 ° C.
• the subsequent deposition of the CdS buffer layer is wet-chemically at a temperature of about 60 0 C.
• the window layer of i-ZnO and doped with aluminum ZnO is deposited by means of DC magnetron sputtering.
• a polysilazane solution of the above-described composition is applied to a substrate, preferably to a steel foil, by means of spray nozzles or dip bath and optionally smoothed with an elastic doctor blade to obtain a uniform thickness distribution or mass coverage on the photovoltaic layer structure to ensure.
• a substrate preferably to a steel foil
• slot nozzles can also be used as an application system for obtaining very thin homogeneous layers.
• the solvent is evaporated. This can be done
• Room temperature or when using suitable dryer at higher temperatures preferably from 40 to 60 0 C in the roll-to-roll process at speeds of> 1 m / min done.
• Evaporation of the solvent is optionally repeated one, two or more times to obtain a dry uncured ("green") polysilazane layer having a total thickness of 100 to 3,000 nm.
• green dry uncured
• the content of solvent in the green polysilazane layer is greatly reduced or eliminated.
• Another advantage of multiple coating and drying is that holes may be present in single layers or cracks are largely covered and closed, so that the water vapor permeability is further reduced.
• the dried or green polysilazane layer is converted by curing at a temperature in the range of 100 to 180 ° C over a period of 0.5 to 1 h in a transparent ceramic phase.
• Hardening is carried out in a convection oven, which is optionally operated with filtered and steam-humidified air or with nitrogen. Depending on the temperature, duration and furnace atmosphere - water vapor-containing air or nitrogen - the ceramic phase has a different composition. If the curing takes place, for example, in water containing steam, a phase of the composition SiN v H w O ⁇ C y with x>v; v ⁇ 1; 0 ⁇ x ⁇ 1, 3; 0 ⁇ w ⁇ 2.5 and y ⁇ 0.5.
• the water vapor permeability can also be reduced by curing the polysilazane layer once more.
• This "postcuring" takes place in particular at a temperature around 85 ° C. in air with a relative humidity of 85% over a period of 1 h. Spectroscopic analyzes show that the postcuring significantly lowers the nitrogen content of the polysilazane layer.

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