CN107123693B - Efficient CdTe nanocrystalline solar cell with high-transparency window layer material based on solution method processing and preparation method thereof - Google Patents

Efficient CdTe nanocrystalline solar cell with high-transparency window layer material based on solution method processing and preparation method thereof Download PDF

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CN107123693B
CN107123693B CN201710242991.8A CN201710242991A CN107123693B CN 107123693 B CN107123693 B CN 107123693B CN 201710242991 A CN201710242991 A CN 201710242991A CN 107123693 B CN107123693 B CN 107123693B
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window layer
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覃东欢
温诗雅
李妙姿
刘鑫妍
刘松炜
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South China University of Technology SCUT
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Abstract

The invention discloses a high-efficiency CdTe nanocrystal solar cell with a high-transparency window layer material processed based on a solution method and a preparation method thereof. The solar cell is formed by sequentially laminating a glass substrate, a cathode interface layer, a window layer, a light activity layer and an anode. The cathode interface layer is ZnO, and the window layer is TiO doped with Mg, Sb, In, Al, Bi, Zr, Pb and Nb2Or a ZnS film, the photoactive layer consists of one or more CdTe nanocrystal layers; the cathode refers to at least one of an indium tin oxide conductive film, doped tin dioxide, a metal film and a metal oxide film; the anode is Au; the solar cell provided by the invention adopts a solution processing technology, realizes the ultrathin solar cell, and has excellent performance and the energy conversion efficiency as high as 3.53%. The preparation process is simple, the main process can be finished by solution processing in a common fume hood, and the low-temperature heat treatment is adopted, so that the manufacturing cost is greatly reduced.

Description

Efficient CdTe nanocrystalline solar cell with high-transparency window layer material based on solution method processing and preparation method thereof
Technical Field
The invention belongs to the field of photoelectric devices, and particularly relates to a high-efficiency CdTe nanocrystal solar cell with a high-transparency window layer material processed based on a solution method and a preparation method thereof.
Background
Fossil energy has been depleted through the large-scale exploitation for decades for the twenty-first century. The industrial revolution till now, the average temperature of the earth rises by 0.3-0.6 ℃ and the sea level rises by 10-25 cm due to the greenhouse effect. The main component of greenhouse gases is carbon dioxide, 80% of which are produced by the consumption of fossil fuels. It is seen that humans are encountering dual crises of energy shortages and environmental deterioration. The development of an efficient and clean energy source is a problem to be solved by the current mankind. The development of solar energy is a necessary trend of energy exploitation nowadays, because solar energy is the green energy meeting the above conditions. Compared with the traditional power generation principle, the solar photovoltaic power generation has the advantages of no other media, no rotating parts, modular structure, simple and easy operation and maintenance, short construction period, utilization of desert land and building roof resources and the like, and is a necessary way for large-scale development and utilization of solar energy.
Traditional crystal silicon battery, because it is great to raw materials and energy demand, the cost is high, and energy recuperation period is longer, and the price/performance ratio awaits improving. In recent years, thin film cells have been distinguished by their absolute advantage of low cost, and mainly include silicon-based thin film solar cells, inorganic compound thin film cells (copper indium gallium selenide (CIGS) thin film cells, cadmium telluride (CdTe) thin film cells), and organic polymer thin film cells. The inorganic compound thin film solar cell has the advantages of good matching with solar spectrum, large absorption coefficient and high energy conversion efficiency. Recently, the energy conversion efficiency of cadmium telluride thin film solar cells manufactured by the laboratories in the U.S. reaches 20.4%, which is very close to the highest conversion efficiency of polycrystalline silicon solar cells. However, the main production methods thereof are a close-space sublimation method, a vacuum evaporation method, an electrochemical deposition method, a magnetron sputtering method, and the like, and further reduction of the cost is restricted by a vacuum or high-temperature environment. The inorganic nanocrystalline solar cell processed by the solution method can realize the preparation of the flexible thin film solar cell with low cost, large area and light weight in industry by introducing a roll-to-roll solution processing method, and can keep the advantages of good solar spectrum response, carrier transmission performance and good stability of inorganic semiconductor materials. Nanocrystalline solar cells are a hot spot in current research. Moreover, the nanocrystalline material can adjust and control the band gap by adjusting the size of crystal grains, so that multiple band gaps of a single material are realized, which is an incomparable advantage of a polymer material.
In 2005, a research group of Alivisatos (i.gur, n.a.fromer, m.l.geier, a.p.alivisatos, Science, 2005, 310, 462) conducted a research on the preparation of inorganic nanocrystalline solar cells based on a spin coating method. Mainly by using an organic polymer solution film-forming method for reference, a solvothermal method is adopted to prepare the nano-crystalline material and the nano-crystalline material are respectively used as a donor material and an acceptor material, and a spin coating method is adopted to successfully prepare the all-inorganic nano-crystalline solar cell with the structure of ITO/CdTe (100nm)/CdSe (100 nm)/Al. Wherein the donor layer primarily absorbs electron-hole pairs generated by solar energy and the acceptor layer serves to transport electrons, forming a typical diode device structure. They improve crystal faces through sintering treatment, reduce defect state density, reduce series resistance and increase open-circuit voltage. Under the irradiation of standard AM1.5 simulated sunlight, the short-circuit current is 13.2mA/cm2The open circuit voltage was 0.45V, the fill factor was 49%, and the conversion efficiency was 2.9%. In fact, the open-circuit voltage can be further improved by reducing the mismatch rate of the sum, so that the photoelectric conversion efficiency is improved. Therefore, solution processing of all-inorganic nanocrystalline solar cells has been of great interest.
In 2010, a research group of Anderson (j.d. olson, y.w. rodriguez, l.d. yang, g.b. ers, s.a. carter, appl.phys.lett., 2010, 96, 242103.) developed a non-aluminum metal electrode and studied the effect of CdTe, CdSe layer thickness on device performance, and found that by increasing the CdTe layer thickness, better energy conversion efficiency could be obtained, but the conversion efficiency of the best device was only 2.6%. The main reasons are that the flatness of the film is not ideal and a large number of grain boundaries and defect states still exist, and in addition, the size of the grains is not well controlled. In the same year, a research group of Olson (j.d.0lson, y.w.rodriguez, l.d.yang, g.b.amers, s.a.carter, appl.phys.lett., 2010, 96, 242103.) prepared CdTe/Al schottky solar cells with an efficiency of up to 5%. They point out CdCl2The heat treatment makes CdTe crystal grains grow, quantum confinement effect is eliminated through optimizing heat treatment conditions, and sunlight absorption is enhanced. However, the schottky solar cell has a structure itself with some problems that limit the improvement of its efficiency. I.e. the light is from the anode (transparent)Electrode ITO) with one end incident and schottky junction at the cathode end, recombination occurs during electron transport, the diffusion length is limited, and the whole can not be absorbed.
In 2011, a research group of Jasieniak (J.Jasieniak, B.work. MacDonald, S.E.Watkins, P.Mulvaniy, Nano Lett., 2011, 11, 2856.) adopts a full-solution layer-by-layer stacking method to prepare the CdTe/ZnO nanocrystalline solar cell, and the energy conversion efficiency reaches 6.9%. The layer-by-layer method can reduce the damage of stress by reducing the thickness of each layer, and in addition, the next layer can play a good compensation role for the defects generated by the previous layer, thereby generally improving the quality of the crystal layer.
In 2013, a research group of Donghua Qin (Donghua Qin, Yiyao Tian, Yi J ie Zhang, Yizhao Lin, Kuo Gao, J Nanopart Re, (2013)15:2053) successfully prepares the inorganic nanocrystalline solar cell with an ITO/ZnO-In/CdS/CdTe/MoOx/Ag inverted structure for the first time by adopting a layer-by-layer spin coating sintering processing method, wherein the efficiency of the inorganic nanocrystalline solar cell reaches 3.73 percent, and the inorganic nanocrystalline solar cell is the highest level of similar devices In the current report. The design of the inverted structure cell is adopted, so that the path of light propagating in the device is reduced, the incident light is closer to a p-n junction, the collection of carriers is facilitated, and the absorption efficiency of light is improved. ZnO-In prepared by a sol method forms a compact and smooth interface layer through spin coating and sintering, and the leveling and uniform spreading of the CdS layer is ensured, so that larger leakage current caused by direct contact of the CdTe layer and ITO is effectively avoided, and the performance of the device is improved. However, the response of the device in the short wavelength range is poor, because the CdS of the window layer has poor response to light with short wavelength, the utilization of the active layer to the short wavelength is reduced, and the improvement of the conversion efficiency is restricted.
In 2014, a research group of Troy K.Townsend (Troy K.Townsend, Edwarde.Foos.Phys.chem.chem.Phys, 2014, 16, 16458) successfully prepared a full-solution inorganic nanocrystalline solar cell with the structure of ITO/CdSe/CdTe/Au by a solution method, wherein the cell conversion efficiency of ITO and Au electrodes processed by the full-solution method is 1.7%, the conversion efficiency of an ITO electrode prepared by the solution method is 2.0% by replacing a commercial ITO electrode with an Au electrode prepared by the solution method, the conversion efficiency of an Au electrode prepared by the solution method is 1.3% by replacing an Au electrode prepared by an evaporation method with an Au electrode prepared by the evaporation method, and the conversion efficiency of the commercial ITO electrode and the Au electrode prepared by the evaporation method reaches 3.8%. The nanocrystals generally have a lower melting point than bulk materials, and thus a relatively low heat treatment temperature can be used, making it possible to use ITO as an electrode for batteries. Although the low work function metal can form ohmic contact with the n-type layer, the low work function metal is easily oxidized and influences the service life of the device, so that the common high-efficiency battery adopts an inverted structure to enhance the stability of the device. The efficiency of the device with the structure is not ideal, and mainly, CdSe is directly deposited on ITO, so that more defects are generated, and the short circuit of the device is easily caused, so that the open-circuit voltage and the filling factor of the device are lower, and the energy conversion efficiency of the device is influenced.
For a positively-assembled cadmium telluride nanocrystalline heterojunction solar cell, the device structure is formed by sequentially laminating a glass substrate, an anode and a buffer layer thereof, an optical activity layer and a cathode. The active layer is arranged on an ITO substrate, and the n-type layer is arranged on the outermost layer, so that certain problems exist: the active layer CdTe is directly coated on the ITO in a spinning mode, light is incident from one side of the ITO, so that the p-n junction is located at the other side far away from the incident light, separation and transmission of carriers are extremely unfavorable, photogenerated carriers can reach a junction region through the thicker active layer, and recombination is inevitable in the transmission process, and the light absorption efficiency is reduced; on the other hand, the cathode mainly adopts low work function metal such as Al, the metal is easy to oxidize and generally needs heat treatment at 400 ℃, the performance of ITO is reduced at 400 ℃, and the stability of the device is difficult to ensure. It is urgent to find a low temperature heat treatment method.
Disclosure of Invention
Aiming at the problems, the invention provides a high-efficiency CdTe nanocrystal solar cell with a high-transparency window layer material based on solution processing.
Another object of the present invention is to provide a method for preparing the solar cell by a solution method.
The object of the present invention is achieved by the following means.
A high-efficiency CdTe nanocrystalline solar cell with a high-transparency window layer material based on solution processing is formed by sequentially laminating a glass substrate, a cathode interface layer, a window layer, an optical active layer and an anode from bottom to top; the thickness of the window layer is 10-100 nm, and one or more layers of TiO doped with Mg, Sb, In, Al, Bi, Zr, Pb and Nb2A thin film or ZnS thin film; the light active layer is a CdTe nanocrystal layer.
Compared with the traditional solar cell which consists of a glass substrate, an anode, a buffer layer of the anode, a photoactive layer and an anode, the solar cell is of an inverted structure, and a high-transparency window layer is additionally arranged. The inverted structure can ensure that the heterojunction region is close to the incident light surface, and the efficient collection and separation of carriers are ensured. The highly transparent window layer can realize effective absorption of electrons and increase the utilization of the light active layer to sunlight.
Preferably, the cathode is at least one of an indium tin oxide (FTO) conductive film, a fluorine-doped tin dioxide (ITO) conductive film, a metal film and a metal oxide thin film, preferably, the FTO is used, and the surface resistance of the used FTO transparent conductive glass is 15ohm/sq, the light transmittance is 83%, and the thickness is 1.6 mm. The thickness of the cathode is 80-200 nm.
Preferably, the cathode interface layer is a ZnO film, and the thickness of the cathode interface layer is 20-100 nm.
Preferably, the high transparent window layer is TiO2Or a ZnS thin film. TiO 22And ZnS are transparent n-type wide band gap semiconductor material, TiO2The HOMO and LUMO energy levels of (A) are respectively 7.1eV and 3.81eV, and TiO2Forming heterojunction with CdTe nanocrystal film to promote exciton separation, and TiO2The deeper HOMO energy level of the cathode has a blocking effect on holes, so that the holes can be prevented from entering the cathode, and the electrons can be promoted to move towards the cathode; due to TiO2The precursor (B) has poor wettability on the FTO surface and is difficult to form a high-quality thin film, so that the precursor (B) is present in TiO2A layer of ZnO is introduced between the FTO and the substrate to improve TiO2The quality of the film; meanwhile, ZnO can also be used as a barrier layer to prevent the formation of TiO2Defects in the layer cause the CdTe and FTO to be in direct contact.
Preferably, the preparation of the window layer comprises the following steps: dissolving tetrabutyl titanate in an organic solvent to obtain titanium dioxide gel, adding a doping substance into the titanium dioxide gel, fully stirring and volatilizing to obtain doped titanium dioxide gel, and depositing the doped titanium dioxide gel on a cathode interface layer in a spin coating, brush coating, spray coating, dip coating, roller coating, printing (preferably screen printing) or ink-jet printing mode to obtain a window layer; the organic solvent is one or more of triethanolamine, acetic acid and absolute ethyl alcohol. The doped medicine for forming the window layer comprises magnesium acetate, antimony ethoxide, indium acetate, aluminum acetate, bismuth acetate, zirconium ethoxide, lead acetate and niobium acetate.
Preferably, the window layer is subjected to a layer-by-layer sintering treatment method, namely, after each deposition and film formation, the film needs to be subjected to heat treatment, wherein the heat treatment is to heat the obtained film on a heating table at 400-500 ℃ for 30-60 min; it is further preferred that the thickness of the window layer is 40 nm.
Further preferably, the preparation of the photoactive layer comprises the following steps: preparing CdTe nano crystal by a solvothermal method, dissolving the CdTe nano crystal in an organic solvent to obtain a black solution, namely a nano crystal solution, depositing the nano crystal solution on a window layer in a spin coating, brush coating, spraying, printing (preferably screen printing) or ink-jet printing mode, then soaking the window layer in a saturated methanol solution for treatment, treating the window layer at a high temperature of 350 ℃ for a period of time to obtain a nano crystal single layer, and processing the nano crystal single layer by a layer-by-layer superposed solution to obtain a uniform and compact optical active layer capable of effectively reducing interface defects and internal stress; the photoactive layer is formed by one or more layers of cadmium telluride nanocrystals in an overlapping manner.
Preferably, the CdTe nanocrystal dissolving organic solvent is a polar organic solvent, such as one or more of n-propanol, pyridine, picoline and benzyl alcohol.
CdTe nanocrystals were prepared according to the literature (s.sun, h.m.liu, y.p.gao, d.h.qin, j.materials.chemistry, 2012,517,6853-6856).
Further optimally, the thickness of the photoactive layer can be obtained by adjusting the concentration of the nanocrystal, the spin-coating rotating speed and the number of spin-coating layers.
Preferably, the thickness of the photoactive layer is 100-700 nm, preferably 500-600 nm, and the photoactive layer is formed by stacking multiple layers of nanocrystals.
The anode is Au or Al, and the thickness of the anode is 80-200 nm. Au is a high work function metal, the work function is 5.1eV, and the Au can be matched with the HOMO energy level of CdTe to form ohmic contact. Preferably, the anode is Au, and the thickness of the anode is 20-100 nm.
The method for preparing the efficient CdTe nanocrystal solar cell with the high-transparency window layer material based on the solution processing comprises the following steps of:
(1) cleaning and drying the glass substrate attached with the cathode;
(2) depositing a cathode interface layer on the surface of the cathode in a solution processing mode;
(3) preparing a window layer on the cathode interface layer by adopting a solution processing method;
(4) preparing a photoactive layer on the window layer by a solution processing method;
(5) and (3) evaporating an anode on the photoactive layer by adopting an evaporation method to obtain the high-efficiency CdTe nanocrystal solar cell with the high-transparency window layer material.
Cathode interface layer and TiO prepared on cathode substrate in sequence2The film, CdTe film, is carried out in a conventional chemical fume hood without any gas shield or special cleaning measures.
The mechanism of the invention is as follows:
the solar cell adopts an inverted structure, ensures that the junction area is close to the incident light surface, and ensures the efficient collection and separation of carriers; the anode adopts Au with high work function as a hole collecting electrode, so that the stability of the anode is ensured; the CdTe ultrathin layer is prepared by adopting a solution processing technology, and the preparation process is simplified. Introducing a ZnO interface layer to make TiO2Uniform and compact film, no pinhole, and prevention of TiO in the upper layer2The metal oxide semiconductor is directly contacted with the FTO, so that the generation of leakage current is reduced, and the performance of the device is finally improved. Introduction of TiO2The high transparent window layer effectively improves the collection of electrons and realizes more effective matching with CdTe crystal latticeAnd the open circuit voltage of the battery device is increased.
Compared with the prior art, the invention has the following advantages and beneficial effects:
(1) the solar cell adopts an inverted structure, ensures that the junction area is close to the incident light surface, ensures the efficient collection and separation of current carriers, can greatly improve the performance of the cadmium telluride nanocrystalline heterojunction solar cell with the inverted structure, and has the energy conversion efficiency of 3.53 percent.
(2) The anode adopts Au as a hole collecting electrode, so that direct contact between low-work-function metal and the active layer is prevented, the stability of the anode is ensured, and the service life of the nanocrystalline solar cell is prolonged.
(3) By using TiO2The high-transparency window layer prepared by the gel effectively improves the carrier collection efficiency and improves the device performance.
(4) A transparent or semitransparent solar cell is realized by adopting a thin film with the transmittance of more than 10% to the solar spectrum (the wavelength is 250-2400 nm) as an anode and a cathode electrode at two ends.
(5) The solar cell provided by the invention adopts a solution processing technology to prepare the ultrathin layer, so that the ultrathin of the solar cell is realized.
(6) The solar cell has simple preparation process, saves raw materials and is easy to realize large-scale production.
Drawings
FIG. 1 is a structural diagram of the high efficiency CdTe nanocrystal solar cell with high transparent window layer material of the present invention.
Detailed Description
The solar cell of the invention is formed by sequentially laminating a glass substrate, a cathode interface layer, a high transparent window layer, a light activity layer and an anode (as shown in figure 1). And a cathode interface layer is added between the cathode and the high-transparency window layer, and a layer-by-layer sintering process is adopted to prepare the CdTe nanocrystal photoactive layer, wherein the cathode interface layer is a ZnO layer. The cathode interface layer is used as an electron transmission layer, the electrical performance of the device is enhanced, the CdTe thin film grows on the honeycomb-shaped high-transparency window layer, the electron collection area is increased, and the cell performance of the heterojunction is improved. Due to ZnODue to the existence of the layer, originally, FTO for collecting holes is changed into collecting electrons, and the optical path of incident light entering a p-n junction is shortened, so that the separation efficiency of carriers is improved. In addition, the inverted structure of the solar cell adopts metal (gold) with high work function, so that the performance of the device is more stable. Dissolving a precursor material in an organic solvent to prepare sol, and depositing the sol on the FTO in a spin coating, brush coating, spray coating, dip coating, roller coating, printing (silk screen printing) or ink-jet printing mode to form a cathode interface layer; the high-transparency window layer is prepared by a sol-gel method, tetrabutyl titanate is dissolved in an organic solvent to obtain titanium dioxide gel, then a doping medicine is added into the titanium dioxide gel, the mixture is fully stirred and volatilized to obtain doped titanium dioxide gel, and the gel is deposited on a cathode interface layer in a spin coating, brush coating, spray coating, dip coating, roller coating, printing (silk screen printing) or ink-jet printing mode to obtain the high-transparency window layer; dissolving CdTe nanocrystal in organic solvent to obtain nanocrystal dispersion, and depositing onto CdTe film by spin coating, brush coating, spray coating, dip coating, roller coating, printing (screen printing) or ink-jet printing, and passing through layer by layer of CdCl2Sintering to obtain a photoactive layer; and finally, depositing the anode material on the CdTe thin film in an evaporation mode to form the anode.
The present invention will be described in further detail with reference to examples and drawings, but the embodiments of the present invention are not limited thereto.
Example 1
Firstly, preparing a high-efficiency CdTe nanocrystal solar cell with a high-transparency window layer material based on solution processing:
(1) cleaning the FTO conductive glass substrate, (the specification is 15 mm multiplied by 15 mm, the thickness of the FTO is 130nm, the square resistance of the FTO is 20 ohm/square, purchased from Kyoto electronic components Co., Ltd.) the substrate is treated by ultrasonic treatment in toluene, acetone, special detergent for semiconductor, deionized water and isopropanol for l0min in sequence, the surface of the FTO substrate is cleaned, and then the FTO sheet is placed in a constant temperature oven to stand for 2h and dried at 80 ℃.
(2) Preparing ZnO sol by filling zinc acetate dihydrate (3.2925g), ethanolamine (0.905m1) and ethylene glycol monomethyl ether (30m1) into a three-necked bottle and sealing. The oil bath was heated for 2 hours while maintaining 80 ℃. (all of the above were analytical pure drugs, purchased from Guangzhou Qian Hui chemical glass Co., Ltd.), filtered through a 0.45 μm filter, and filled into a glass bottle and charged with nitrogen gas to obtain a ZnO sol.
(3) And (3) preparing a cathode interface layer, namely placing the dried FTO sheet on a spin coater ((KW-4A type), dropwise adding the ZnO sol prepared in the step (2), spin-coating at a high speed (3000rpm for 20s), scraping a ZnO layer at the cathode position, placing on a heating table, performing heat treatment at 200 ℃ for l0min, then heating at 400 ℃ for l0min, cooling to room temperature, respectively placing in acetone and isopropanol for l0min under ultrasonic power of 1000W, and drying by using a nitrogen gun to obtain the cathode interface layer with the thickness of 40 nm.
(4) Preparation of a high-transparency window layer:
①TiO2preparation of gel: measuring 25ml of anhydrous methanol by using a measuring cylinder, respectively extracting 4.25ml of tetrabutyl titanate and 3.75ml of triethanolamine by using an injector, adding the tetrabutyl titanate and the triethanolamine into a 50ml beaker, stirring for 2 hours, adding 5ml of acetic acid and 5ml of deionized water by using a plastic dropper, adding a proper amount of antimony ethoxide for doping, continuously stirring for 24 hours, recording the temperature and the humidity, and volatilizing the mixture to a gel state in a fume hood to obtain TiO2And (4) gelling. (all of the above are analytical pure drugs, purchased from Guangzhou Qian Hui chemical glass Co., Ltd.)
② placing the substrate treated in step (3) on a spin coater ((KW-4A type), and adding the TiO dropwise2And (3) gelling, spin-coating at a high speed (the speed is 2500rpm, the time is 15s), scraping the window layer at the cathode position, heating on a heating table at 500 ℃ for 1h, carrying out ultrasonic treatment in isopropanol for 8min, blow-drying by a nitrogen gun, and treating on the heating table at 150 ℃ for l5min to obtain the high-transparency window layer with the thickness of 40 nm.
(5) Preparation of photoactive layer:
① preparation of CdTe nanocrystal (S.Sun, H.M.Liu, Y.P.Gao, D.H.Qin, J.materials.chemistry, 2012,517,6853-6856.), the concrete preparation process is that cadmium tetradecanoate (l.6mmo1,906mg) and trioctylphosphine oxide 2.35g tetradecanoic acid (myristic acid, C.C.)13H26COOH,92mg) was added to a 50m1 three-necked flask (with a thermometer, a condenser, and a gas-guide tube on the neck) and heated to 240 deg.C under nitrogen protectionAt this point, cadmium tetradecanoate had decomposed (decomposition temperature 228 ℃ C.), and a pale yellow solution was obtained. Keeping at this temperature for 5min, rapidly injecting trioctylphosphine-tellurium (tellurium concentration of 0.8mmo1/mL, lml) into the reaction system (wherein trioctylphosphine and trioctylphosphine oxide are both available from Aladdin Chemicals, and the rest from Qian Hui chemical glass Co., Ltd.), and allowing the whole reaction to last at 240 deg.C for 30 min; then washing with methanol for 3 times, and centrifuging to separate the product; and adding the product into 20mL of pyridine, refluxing under the protection of nitrogen at 100 ℃, carrying out l0h refluxing, adding 60mL of n-hexane solvent after the refluxing is finished, carrying out centrifugal separation, and drying the final product by using a nitrogen gun to obtain the CdTe nanocrystal.
② dissolving the CdTe nanocrystal in mixed solvent of n-propanol and pyridine at volume ratio of 1:1, with concentration of 0.04g/mL, ultrasonic treating for 2 hr (ultrasonic power of 1000W), and filtering with 0.45m (organic system) filter to obtain CdTe nanocrystal solution.
Placing the substrate treated in the step (4) on a spin coater (KW-4A type), dropwise adding the CdTe nanocrystal solution, spin-coating at high speed (speed of 1100rpm for 20s), heating at 150 deg.C for 3min to remove organic solvent, scraping the nanocrystal layer of the window layer, and soaking in CdCl at 150 deg.C2L0s in saturated methanol solution, and then immersed in n-propanol at 120 ℃ to remove excess CdCl2Blow-drying with nitrogen, placing on a 350 deg.C heating table, heat treating for 40s, treating at 150 deg.C heating table for 2min, soaking in 120 deg.C methanol for rinsing for 4s, blow-drying with nitrogen gun, and treating at 400 deg.C for l5min to obtain CdTe nanocrystal layer with thickness of 100 nm. And repeating spin coating for 5 layers to obtain the multilayer CdTe nanocrystal.
(6) Evaporating the anode, namely putting the substrate obtained in the step (5) into a vacuum plating cavity, wherein the thickness of the substrate is 3 multiplied by 10-4Au (80nm) was deposited under Pa in a high vacuum to obtain an anode.
Packaging the obtained device to obtain the structure of FTO/ZnO/TiO2Inverted structure inorganic CdTe nanocrystalline heterojunction solar cell of/CdTe/Au (the structure schematic diagram is shown in figure 1).
Secondly, measuring the performance of the CdTe nanocrystal heterojunction solar cell:
the performance parameters of the solar cell device are measuredSunlight is the test standard. The irradiance measured in the laboratory with the AM1.5G standard was 1000W/m2. When the performance test of the nanocrystalline solar cell is carried out by using solar simulated light, firstly, a standard cell is used for judging whether a light source meets the irradiance of AM1.5G. The standard silicon solar cell is calibrated under the standard spectrum of AM1.5G, namely 1000W/m2The short-circuit current obtained under irradiation with the irradiation illuminance of (2) was 125 mA. And after the irradiation intensity is determined, testing the device. Solar simulated light is used for carrying out solar cell performance test, and the energy conversion efficiency of the solar cell is as follows:
Figure BDA0001269836530000081
wherein P isMAXThe maximum output power (unit: mW) and the Pin radiation illuminance (unit: mW/cm)2) S is the effective area of the device (unit: cm2). The apparatus for measuring the performance of the polymer bulk heterojunction solar cell is shown in table 1.
TABLE 1
Figure BDA0001269836530000082
Example 1
Influence of antimony ethoxide doping with different concentrations on CdTe nanocrystal solar cells:
respectively selecting TiO with the concentration of 3 wt%, 5 wt% and 8 wt% of undoped and doped antimony ethoxide2Film as window layer, TiO2The heat treatment temperature is 500 deg.C, ZnO is 40nm, cadmium telluride layer is 500nm, and CdCl2The sintering temperature was set at 400 ℃ and the sintering time was set at 15min, and other parameter conditions were carried out as in example 1.
TABLE 2
Figure BDA0001269836530000091
Table 2 compares the efficiency of the cadmium telluride solar cell under different doping concentrations of antimony ethoxide, and it can be seen that the efficiency reaches the maximum value when doping is carried out for 3 wt%, and then the efficiency is not changed greatly when the doping concentration is continuously increased.
Example 2
Different CdCl2Effect of sintering temperature on CdTe nanocrystal solar cells
CdCl of 370 deg.C, 380 deg.C, 390 deg.C and 400 deg.C is selected respectively2Sintering temperature, TiO2The heat treatment temperature is 500 deg.C, ZnO is 40nm, cadmium telluride layer is 500nm, and TiO doped with 3 wt% antimony ethoxide is selected2The film was used as a window layer, the sintering time was 15min, and other parameter conditions were performed as in example 1.
TABLE 2
Figure BDA0001269836530000092
Table 2 compares various CdCl2The change of the open-circuit voltage, the short-circuit current, the efficiency and the like of the cadmium telluride solar cell at the sintering temperature shows that the efficiency of the solar cell is gradually improved along with the change of the heating temperature between 370 ℃ and 400 ℃, and the higher heat treatment temperature is beneficial to the growth of CdTe nanocrystals and effectively reduces defects to generate more compact crystal lattices.
Example 3
Different CdCl2Effect of sintering time on CdTe nanocrystal solar cells
Selecting CdCl for 10min, 15min, 20min and 30min respectively2Sintering time, TiO2The heat treatment temperature is 500 deg.C, ZnO is 40nm, cadmium telluride layer is 500nm, and TiO doped with 3 wt% antimony ethoxide is selected2The film was used as a window layer and the sintering temperature was 400 ℃ and other parameter conditions were performed as in example 1.
TABLE 3
Figure BDA0001269836530000101
Table 3 compares various CdCl2The change of the open-circuit voltage, the short-circuit current, the efficiency and the like of the cadmium telluride solar cell under the sintering time can be found from the data, and the heat treatment time of 15minThe efficiency of the lower solar cell is obviously superior to that of other processing time, the nanocrystalline particles are in a stage of incomplete growth within the sintering time shorter than 15min, the efficiency of the device is limited, and the CdTe layer material reacts with water and oxygen in the air after the sintering time longer than 15min, so that the further improvement of the cell efficiency is influenced.
Example 4
Influence of different dopants on CdTe nanocrystalline solar cells:
respectively selecting and using antimony ethoxide, indium acetate, aluminum acetate and zirconium ethoxide doped TiO2The film was used as a window layer, the doping concentration was 3 wt%, the heat treatment temperature was 500 deg.C, ZnO was 40nm, the cadmium telluride layer was 500nm, the sintering temperature was 400 deg.C, 15min, and other parameter conditions were performed as in example 1.
TABLE 4
Figure BDA0001269836530000102
Figure BDA0001269836530000111
Table 4 compares the effect of doping different substances on CdTe solar cells, wherein the antimony ethoxide doped window layer material gives the cell device with the best performance. Different doping substances change TiO2The film-forming property and the structural change of the window layer cause the window layer to correspondingly change the electron collection efficiency.
Example 5
Effect of different window layers on CdTe nanocrystal solar cells
Respectively selecting TiO2The thin film, ZnS thin film as a window layer, was doped with antimony ethoxide at a concentration of 3 wt%, heat-treated at 500 deg.C, ZnO at 40nm, cadmium telluride at 500nm, and sintered at 400 deg.C for 15min, with the other parameters being as in example 1.
TABLE 5
Figure BDA0001269836530000112
Table 5 compares the effect of two different materials as window layers on the cell device, and the difference in film formation morphology on the ZnO film and the lattice match with the CdTe photoactive layer after the different materials are treated affect the device performance.
Example 6
Effect of different window layer thicknesses on CdTe nanocrystal solar cells
Respectively selecting TiO with the thickness of 20nm, 40nm, 60nm, 80nm and 100nm2Film as window layer, TiO2The film is doped with 3 wt% of antimony ethoxide, the heat treatment temperature is 500 ℃, the heat treatment time is 1h, ZnO is 500nm for a 40nm cadmium telluride layer, and CdCl2The sintering temperature was set at 400 ℃ and the sintering time was set at 15min, and other parameter conditions were carried out as in example 1.
TABLE 6
Figure BDA0001269836530000121
Table 6 compares the effect of different window layer thicknesses on the cell device, with different window layer thicknesses affecting the TiO2The interfacial shape of the thin film thus affects the collection of electrons. The thinner window layer has low electron absorption efficiency and generates leakage current; the thicker window layer affects the utilization of sunlight and is not beneficial to improving efficiency.
Example 7
Effect of Window layer treatment temperature on CdTe nanocrystal solar cells
Respectively selecting TiO at 400 deg.C, 450 deg.C and 500 deg.C2Temperature of heat treatment of film, TiO2The film is doped with 3 wt% antimony ethoxide, the thickness is 40nm, the heat treatment temperature is 500 ℃, and the time is 60 min. ZnO was set to 40nm, the cadmium telluride layer was set to 500nm, the sintering temperature was 400 ℃ for 15min, and other parameter conditions were performed as in example 1.
TABLE 7
Figure BDA0001269836530000122
Table 7 comparesThe influence of the window layer on the cell device under the same heat treatment needs higher heat treatment temperature to ensure that the TiO is subjected to heat treatment due to the larger thickness of the FTO conductive glass2The film is formed more densely, so the efficiency of the battery device is improved.
Example 8
Effect of Window layer Heat treatment time on CdTe nanocrystal solar cells
Selecting TiO respectively for 30min, 40min, 45min, 55min, and 60min2Film heat treatment time, TiO2The film was doped with 3 wt% antimony ethoxide to a thickness of 40nm, heat treated at 500 deg.C with 40nm ZnO, 500nm cadmium telluride layer, and sintered at 400 deg.C for 15min, with the other parameters being as in example 1.
TABLE 8
Figure BDA0001269836530000131
Table 8 compares the influence of the heat treatment time of different window layers on the battery device, and with the increase of the length of the heat treatment time, the battery efficiency is effectively changed, and the heat treatment time reaching a certain length is favorable for film formation of a thin film, so that the absorption of the window layer on electrons is improved, and the generation of leakage current is reduced.
The above embodiments are preferred embodiments of the present invention, but the present invention is not limited to the above embodiments, and any other changes, modifications, substitutions, combinations, and simplifications which do not depart from the spirit and principle of the present invention should be construed as equivalents thereof, and all such changes, modifications, substitutions, combinations, and simplifications are intended to be included in the scope of the present invention.

Claims (7)

1. A high-efficiency CdTe nanocrystalline solar cell with a high-transparency window layer material based on solution processing is characterized in that the solar cell is formed by sequentially laminating a glass substrate, a cathode interface layer, a window layer, an optical activity layer and an anode from bottom to top; the window layer material is prepared by a solution method and is deposited to form a film by adopting a layer-by-layer sintering method, the thickness of the window layer is 10-100 nm, and one or more layers of the window layer material are doped with Mg, Sb, In, Al, Bi, Zr,TiO of Pb or Nb2Film composition; the optical active layer is a CdTe nanocrystal layer;
the preparation of the window layer comprises the following steps: dissolving tetrabutyl titanate in an organic solvent to obtain titanium dioxide gel, adding a doping substance into the titanium dioxide gel, fully stirring and volatilizing to obtain doped titanium dioxide gel, and depositing the doped titanium dioxide gel on a cathode interface layer in a spin coating, brush coating, spray coating, dip coating, roller coating or printing mode to obtain a window layer;
the organic solvent is one or more of triethanolamine, acetic acid and absolute ethyl alcohol; the doping material is magnesium acetate, antimony ethoxide, indium acetate, aluminum acetate, bismuth acetate, zirconium ethoxide, lead acetate or niobium acetate;
the window layer adopts a layer-by-layer sintering treatment method, namely after each deposition film forming, the film needs to be subjected to heat treatment, and the heat treatment is to heat the obtained film on a heating table at 400-500 ℃ for 30-60 min.
2. The efficient CdTe nanocrystal solar cell with the high transparent window layer material based on the solution processing method as claimed in claim 1, wherein the cathode is at least one of an indium tin oxide conductive film and a fluorine-doped tin dioxide conductive film, and the thickness of the cathode is 80-200 nm.
3. The efficient CdTe nanocrystal solar cell with the high transparent window layer material based on the solution processing method as in claim 1, wherein the cathode interface layer is a ZnO thin film and has a thickness of 20-100 nm.
4. The high-efficiency CdTe nanocrystal solar cell with a high-transparency window layer material based on the solution process as claimed in claim 1, wherein the preparation of the photoactive layer comprises the following steps: preparing CdTe nano-crystals by a solvothermal method, dissolving the CdTe nano-crystals in an organic solvent to obtain a black solution, namely a nano-crystal solution, and depositing the nano-crystal solution on the window layer in a spin coating, brush coating, spraying or printing mode to obtain a CdTe nano-crystal layer; the photoactive layer is formed by overlapping a plurality of layers of cadmium telluride nanocrystals.
5. The efficient CdTe nanocrystal solar cell with the high transparent window layer material based on the solution processing method as in claim 1, wherein the thickness of the photoactive layer is 100-700 nm.
6. The efficient CdTe nanocrystal solar cell with the high transparent window layer material based on the solution processing method as in claim 1, wherein the anode is Au or Al and has a thickness of 80-200 nm.
7. The method for preparing the high-efficiency CdTe nanocrystal solar cell with the high-transparency window layer material based on the solution method processing is characterized by comprising the following steps of:
(1) cleaning and drying the glass substrate attached with the cathode;
(2) depositing a cathode interface layer on the surface of the cathode in a solution processing mode;
(3) preparing a window layer on the cathode interface layer by adopting a solution processing method;
(4) preparing a photoactive layer on the window layer by a solution processing method;
(5) and (3) evaporating an anode on the photoactive layer by adopting an evaporation method to obtain the high-efficiency CdTe nanocrystal solar cell with the high-transparency window layer material.
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