CN111370520A - Silicon-based array laminated solar cell and preparation method thereof - Google Patents
Silicon-based array laminated solar cell and preparation method thereof Download PDFInfo
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- XUIMIQQOPSSXEZ-UHFFFAOYSA-N Silicon Chemical compound [Si] XUIMIQQOPSSXEZ-UHFFFAOYSA-N 0.000 title claims abstract description 76
- 229910052710 silicon Inorganic materials 0.000 title claims abstract description 75
- 239000010703 silicon Substances 0.000 title claims abstract description 75
- 238000002360 preparation method Methods 0.000 title claims description 14
- 239000000758 substrate Substances 0.000 claims abstract description 86
- 239000010409 thin film Substances 0.000 claims abstract description 80
- 229910021421 monocrystalline silicon Inorganic materials 0.000 claims abstract description 58
- 229910052751 metal Inorganic materials 0.000 claims abstract description 47
- 239000002184 metal Substances 0.000 claims abstract description 47
- 230000000737 periodic effect Effects 0.000 claims abstract description 36
- 238000010521 absorption reaction Methods 0.000 claims abstract description 27
- GWEVSGVZZGPLCZ-UHFFFAOYSA-N titanium dioxide Inorganic materials O=[Ti]=O GWEVSGVZZGPLCZ-UHFFFAOYSA-N 0.000 claims abstract description 26
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N silicon dioxide Inorganic materials O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 claims abstract description 22
- 230000005525 hole transport Effects 0.000 claims abstract description 21
- 239000000377 silicon dioxide Substances 0.000 claims abstract description 20
- 229910052681 coesite Inorganic materials 0.000 claims abstract description 18
- 229910052906 cristobalite Inorganic materials 0.000 claims abstract description 18
- 229910052682 stishovite Inorganic materials 0.000 claims abstract description 18
- 229910052905 tridymite Inorganic materials 0.000 claims abstract description 18
- OGIDPMRJRNCKJF-UHFFFAOYSA-N titanium oxide Inorganic materials [Ti]=O OGIDPMRJRNCKJF-UHFFFAOYSA-N 0.000 claims abstract description 16
- 238000005530 etching Methods 0.000 claims abstract description 14
- 238000000137 annealing Methods 0.000 claims description 32
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- XKRFYHLGVUSROY-UHFFFAOYSA-N Argon Chemical compound [Ar] XKRFYHLGVUSROY-UHFFFAOYSA-N 0.000 claims description 16
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- ZOXJGFHDIHLPTG-UHFFFAOYSA-N Boron Chemical compound [B] ZOXJGFHDIHLPTG-UHFFFAOYSA-N 0.000 claims description 13
- 229910052796 boron Inorganic materials 0.000 claims description 13
- 239000007788 liquid Substances 0.000 claims description 13
- 238000009792 diffusion process Methods 0.000 claims description 12
- 238000001755 magnetron sputter deposition Methods 0.000 claims description 10
- 229910052709 silver Inorganic materials 0.000 claims description 10
- XDXWNHPWWKGTKO-UHFFFAOYSA-N 207739-72-8 Chemical compound C1=CC(OC)=CC=C1N(C=1C=C2C3(C4=CC(=CC=C4C2=CC=1)N(C=1C=CC(OC)=CC=1)C=1C=CC(OC)=CC=1)C1=CC(=CC=C1C1=CC=C(C=C13)N(C=1C=CC(OC)=CC=1)C=1C=CC(OC)=CC=1)N(C=1C=CC(OC)=CC=1)C=1C=CC(OC)=CC=1)C1=CC=C(OC)C=C1 XDXWNHPWWKGTKO-UHFFFAOYSA-N 0.000 claims description 8
- MHAJPDPJQMAIIY-UHFFFAOYSA-N Hydrogen peroxide Chemical compound OO MHAJPDPJQMAIIY-UHFFFAOYSA-N 0.000 claims description 8
- BQCADISMDOOEFD-UHFFFAOYSA-N Silver Chemical compound [Ag] BQCADISMDOOEFD-UHFFFAOYSA-N 0.000 claims description 8
- 229910052786 argon Inorganic materials 0.000 claims description 8
- 239000000084 colloidal system Substances 0.000 claims description 8
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- 230000008569 process Effects 0.000 claims description 6
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- GRYLNZFGIOXLOG-UHFFFAOYSA-N Nitric acid Chemical compound O[N+]([O-])=O GRYLNZFGIOXLOG-UHFFFAOYSA-N 0.000 claims description 3
- 230000005540 biological transmission Effects 0.000 claims description 3
- 238000004519 manufacturing process Methods 0.000 claims description 3
- 229910017604 nitric acid Inorganic materials 0.000 claims description 3
- 238000003486 chemical etching Methods 0.000 claims description 2
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- 229910052737 gold Inorganic materials 0.000 claims description 2
- 229910000480 nickel oxide Inorganic materials 0.000 claims description 2
- QGLKJKCYBOYXKC-UHFFFAOYSA-N nonaoxidotritungsten Chemical compound O=[W]1(=O)O[W](=O)(=O)O[W](=O)(=O)O1 QGLKJKCYBOYXKC-UHFFFAOYSA-N 0.000 claims description 2
- GNRSAWUEBMWBQH-UHFFFAOYSA-N oxonickel Chemical compound [Ni]=O GNRSAWUEBMWBQH-UHFFFAOYSA-N 0.000 claims description 2
- 235000012239 silicon dioxide Nutrition 0.000 claims description 2
- 239000000126 substance Substances 0.000 claims description 2
- 229910001930 tungsten oxide Inorganic materials 0.000 claims description 2
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- 239000000969 carrier Substances 0.000 abstract description 2
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- 239000003292 glue Substances 0.000 description 24
- 229910015845 BBr3 Inorganic materials 0.000 description 12
- ILAHWRKJUDSMFH-UHFFFAOYSA-N boron tribromide Substances BrB(Br)Br ILAHWRKJUDSMFH-UHFFFAOYSA-N 0.000 description 12
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- ZMXDDKWLCZADIW-UHFFFAOYSA-N N,N-Dimethylformamide Chemical compound CN(C)C=O ZMXDDKWLCZADIW-UHFFFAOYSA-N 0.000 description 6
- 239000011248 coating agent Substances 0.000 description 6
- 238000000576 coating method Methods 0.000 description 6
- 229910021419 crystalline silicon Inorganic materials 0.000 description 6
- 239000008367 deionised water Substances 0.000 description 6
- 229910021641 deionized water Inorganic materials 0.000 description 6
- 238000000605 extraction Methods 0.000 description 6
- RQQRAHKHDFPBMC-UHFFFAOYSA-L lead(ii) iodide Chemical compound I[Pb]I RQQRAHKHDFPBMC-UHFFFAOYSA-L 0.000 description 6
- 230000003647 oxidation Effects 0.000 description 6
- 238000007254 oxidation reaction Methods 0.000 description 6
- 239000002994 raw material Substances 0.000 description 6
- 238000007711 solidification Methods 0.000 description 6
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- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Chemical compound O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 6
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- 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
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- H01L31/0687—Multiple junction or tandem solar cells
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Abstract
The invention discloses a silicon-based array laminated solar cell, which comprises a bottom cell structure and a top cell structure laminated on the bottom cell structure, wherein the bottom cell structure comprises an n-type monocrystalline silicon substrate, and SiO is arranged around a nanopore periodic array structure in the vertical direction prepared by etching the surface of the n-type monocrystalline silicon substrate2The insulating layer is used for preparing a p-type doping layer in the middle of the n-type monocrystalline silicon substrate and on the inner wall of the nano hole, and the lower surface of the n-type monocrystalline silicon substrate is provided with a metal thin film layer; the top cell structure sequentially comprises TiO from bottom to top2A thin film layer, a perovskite absorption layer, a hole transport layer, a transparent conductive thin film layer, a metal electrode, TiO2A thin film layer laminated on SiO2Filling the insulating layer and the p-type doped layerIs filled and embedded in the nanometer hole. The invention utilizes the excellent light capture capability of the silicon pore array and simultaneously utilizes TiO2The silicon hole array is filled to improve the collection efficiency of carriers, and improve the photocurrent density while improving the photon absorption efficiency.
Description
Technical Field
The invention relates to a solar cell and a preparation method thereof, in particular to a silicon-based array laminated solar cell and a preparation method thereof.
Background
Solar energy is a renewable clean energy source and has important significance for the sustainable development of human beings. The solar cell directly converts light energy into electric energy, and the photoelectric conversion efficiency and the preparation cost are key factors for determining the industrial application of the solar cell. Currently, silicon-based solar cells are the mainstream of solar cells, occupy 90% of the global photovoltaic market, have the efficiency of 25.6% and approach the Shockley-queeiser limit efficiency (29.4%), but have high preparation cost. The development of silicon-based solar cells requires a reduction in manufacturing costs while increasing the efficiency of the cell.
Because of the wide energy distribution of the solar spectrum, only photons with energy values larger than the forbidden band width can be absorbed by any semiconductor material. Therefore, a laminated cell is formed by superposing the wide-bandgap light absorption material on the top layer of the silicon-based cell, and the cell efficiency can be improved while the silicon cell maturation process is considered [ M.A.Green.prog.Phototactics 2018,26 and 427 ]. The theoretical ultimate efficiency of silicon-based laminate cells that has been reported to date can be increased from 29% to 42.5%.
The perovskite solar cell adopts CH with a perovskite structure3NH3PbX3The (X ═ I, C and Br) is used as a photoelectric conversion material, the performance is obviously improved in a few years, and the photoelectric conversion efficiency is 3.8% from 2009 and can reach as high as 22.1% until now. Perovskite materials are also considered to be the most promising next-generation low-cost solar cell light absorbing material. When perovskiteWith a band gap of 1.55eV, it can absorb photons with a wavelength of less than 800nm, while crystalline silicon with a band gap of 1.12eV can absorb photons with a wavelength of less than 800nm in the solar spectrum. When the two form a laminated cell from top to bottom, the absorption spectra of the two are complementary, the utilization rate of solar spectrum is greatly improved, and the preparation cost is reduced. Compared with a silicon-based battery, the perovskite-crystalline silicon laminated solar battery researched and developed by hong Kong university of science and technology has the advantages that the cost is reduced by 30.6%, and the efficiency reaches 25.5%.
Chinese patent publication No. CN109935690A employs the preparation of a tunnel junction and a perovskite absorption layer at low temperature. The efficiency of the silicon heterojunction/perovskite two-electrode laminated solar cell prepared by a simple and low-cost solution method can finally reach 22.22%. The chinese patent with publication number CN209709024U designs a double-sided light-receiving perovskite/p-type crystalline silicon substrate laminated solar cell, so that the back of the crystalline silicon solar cell as the substrate can absorb extra scattered light, and the overall performance of the laminated device is improved to a certain extent.
Although the performance of the existing perovskite-crystalline silicon tandem cell is remarkably improved, the existing perovskite-crystalline silicon tandem cell cannot meet the requirement of industrialization, so that a better light absorption structure is required to be searched for so as to improve the light absorption of the device and further prepare a high-performance cell device.
Disclosure of Invention
An object of the present invention is to provide a silicon-based array tandem solar cell, which solves the problems of low absorption efficiency of long wavelength photons and low collection efficiency of carriers in a tandem cell by utilizing the excellent light capturing capability of a silicon pore array, and improves the photocurrent density while improving the photon absorption efficiency. The invention also aims to provide a preparation method of the silicon-based array laminated solar cell.
The technical scheme of the invention is as follows: a silicon-based array laminated solar cell comprises a bottom cell structure and a top cell structure, wherein the top cell structure is laminated on the bottom cell structure, the bottom cell structure comprises an n-type monocrystalline silicon substrate, and SiO (silicon dioxide) is arranged on the periphery of the upper surface of the n-type monocrystalline silicon substrate2Insulating layer on said n-type single crystal silicon substrateA light receiving window is formed in the central area, a nanopore periodic array structure in the vertical direction is etched and prepared on the n-type monocrystalline silicon substrate in the light receiving window area, p-type doping layers are prepared on the n-type monocrystalline silicon substrate in the light receiving window area and the inner walls of the nanopores of the nanopore periodic array structure, and a metal thin film layer is arranged on the lower surface of the n-type monocrystalline silicon substrate; the top cell structure sequentially comprises TiO from bottom to top2A thin film layer, a perovskite absorption layer, a hole transport layer, a transparent conductive thin film layer and a metal electrode, wherein the TiO is2A thin film layer laminated on the SiO2An insulating layer and the p-type doping layer are arranged above the substrate and are filled and embedded into the nano holes; the metal electrode and the metal film layer are respectively led out to be used as a conductive electrode to supply power to an external circuit.
Preferably, the period of the nanopore periodic array structure is 200-900 nm, the diameter of the nanopore periodic array structure is 50-800 nm, the depth of the nanopore is 100-1000 nm, and the duty ratio of the nanopore periodic array structure is 0.4-0.8.
Preferably, the TiO is2The thickness of the thin film layer stacked on the surface of the p-type doped layer is 100-150 nm.
Preferably, the thickness of the perovskite absorption layer is 100-500 nm.
Preferably, the hole transport layer is one of nickel oxide, tungsten oxide and Spiro-OMeTAD, and the thickness is 150-800 nm.
Preferably, the metal electrode is made of one of Au, Ag, Al, Gu and Pt, and the thickness of the metal electrode is 10-500 nm.
A preparation method of a silicon-based array tandem solar cell is characterized by sequentially comprising the following steps: firstly, preparing a nanopore periodic array structure in the vertical direction on the upper surface of an n-type monocrystalline silicon substrate by using a metal-assisted chemical etching method; secondly, depositing a layer of SiO on the periphery of the n-type monocrystalline silicon substrate2The insulating layer forms a light receiving window; thirdly, preparing PN junctions on the upper surface of the n-type monocrystalline silicon substrate in the light receiving window region and the inner wall surface of the nano holes of the periodic array structure of the nano holes by utilizing high-temperature diffusion of a liquid boron source; fourthly, utilizing a magnetron sputtering method to form SiO2Preparation of TiO on the surface of insulating layer and PN junction2The thin film layer is used as an electron transmission layer, and the TiO2The thin film layer is filled and embedded into the nano holes; fifthly, annealing and curing are carried out and the TiO2Preparing a perovskite absorption layer and a hole transport layer on the thin film layer in sequence by using a spin coating method; sixthly, respectively preparing a transparent conductive thin film layer and a metal electrode on the surface of the hole transport layer by adopting an electron beam evaporation process; and seventhly, depositing a metal thin film layer lead-out wire on the lower surface of the n-type monocrystalline silicon substrate to serve as the cathode of the silicon-based array laminated solar cell, wherein the metal electrode lead-out wire serves as the anode of the silicon-based array laminated solar cell.
Preferably, in the process of preparing the periodic array structure of the vertical nano holes by using a metal-assisted chemical method, a spin coater is used for spin-coating silver nano colloid on the n-type monocrystalline silicon substrate at the rotating speed of 2500-5000 r/min, and the diameter of the silver nano particles is 50-800 nm; after spin coating, immersing the substrate into a hydrogen peroxide solution for etching, wherein the concentration of the solution is 0.2-2 mol/L, and the time is 0.5-2 h; and removing the silver nanoparticles by using a nitric acid solution after the nanopore periodic array is formed.
Preferably, the resistivity of the n-type monocrystalline silicon substrate is 1.2-1.3 omega-cm, and the concentration of the liquid boron source is 15-16 mg/cm when the liquid boron source is used for preparing the PN junction through high-temperature diffusion3BBr of3And (3) performing high-temperature diffusion on the liquid boron source at 1200-1250 ℃ to prepare the p-type doped layer.
Preferably, the TiO is prepared by using a magnetron sputtering method2In the case of a thin film layer, the purity of the TiO2 target material is 99.99 percent, and the local vacuum is 10 percent-3～10-5torr, argon is used as working gas, the annealing temperature is 380-650 ℃ during annealing and curing, the annealing time is 1-3 h, and the TiO2The thickness of the film laminated on the surface of the p-type doped layer is 50-300 nm.
The technical scheme provided by the invention has the advantages that: the silicon hole array with better light trapping property is used as a bottom cell structure of the perovskite silicon-based array laminated solar cell, and compared with a planar silicon structure, the light absorption property is better; compared with the prior suede light trapping structure technology, the surface of the silicon pore array is smoother and smootherThe mechanical property is more stable; the silicon-based nano-pore array is used as a bottom battery structure, the excellent light absorption of the periodic nano-pore array is utilized, and the pore array is used for filling TiO2The layer improves the charge transmission performance, comprehensively improves the utilization efficiency of the cell long-wave photons, and improves the photoelectric conversion efficiency of the laminated solar cell while being compatible with the silicon-based cell process.
Drawings
Fig. 1 is a schematic structural diagram of a silicon-based array tandem solar cell.
Fig. 2 is a prepared silicon pore array structure.
Fig. 3 is a graph comparing the spectral absorption of the silicon-based array tandem solar cell of examples 1, 2, 3 with that of the planar structure perovskite silicon-based solar cell.
FIG. 4 is a plot of photocurrent density curves for the nanopore periodic array at different periods.
FIG. 5 is a graph comparing the electric field density distribution of the silicon-based array tandem solar cell of example 4 under the action of 600nm photons.
FIG. 6 is a graph comparing the electric field density distribution of the silicon-based array tandem solar cell of example 4 under the action of 900nm photons.
FIG. 7 is a graph comparing the electric field density distribution of the silicon-based array tandem solar cell of example 5 under the action of 600nm photons.
FIG. 8 is a graph comparing the electric field density distribution of the silicon-based array tandem solar cell of example 5 under the action of 900nm photons.
FIG. 9 is a graph comparing the electric field density distribution of the silicon-based array tandem solar cell of example 6 under the action of 600nm photons.
FIG. 10 is a graph comparing the electric field density distribution of the silicon-based array tandem solar cell of example 6 under the action of 900nm photons.
FIG. 11 is a graph comparing the electric field density distribution under 600nm photons for a comparative example planar structure perovskite silicon-based solar cell.
FIG. 12 is a graph comparing the electric field density distribution under the action of 900nm photons for a comparative example planar structure perovskite silicon-based solar cell.
Detailed Description
The present invention is further illustrated by the following examples, which are not to be construed as limiting the invention thereto.
Example 1, referring to fig. 1 and 2, firstly, an n-type czochralski silicon wafer with a size of 8cm × 8cm is selected as an n-type single crystal silicon substrate 1, the thickness of the n-type czochralski silicon wafer is 200 μm, the resistivity of the n-type czochralski silicon wafer is 1.6 Ω · cm., after cleaning, silver nano colloid is spin-coated on the silicon substrate by a spin coater at a rotation speed of 3200r/min, the diameter of silver nano particles is 350nm, the spin-coated silicon wafer is immersed in hydrogen peroxide solution for etching, the concentration of the solution is 1.2mol/L, the time is 0.5h, a vertical nano-hole periodic array structure 10 is formed, the period of the nano-hole periodic array structure 10 is 800nm, the diameter of nano holes is 320nm, the duty ratio is 0.4, and the depth is 400nm, and the silver nano particles are removed by.
After a sample is cleaned and dried, SiO is formed on the periphery of the surface of the n-type monocrystalline silicon substrate 1 by an oxidation etching process2Insulating layer 3 on SiO2The exposed area in the middle of the insulating layer 3 is a light receiving window, the size of the light receiving window is 5cm × 5 cm., the light receiving window is cleaned and dried by deionized water, and then the light receiving window is placed in a diffusion furnace to be BBr3The liquid boron source is diffused at high temperature of 1100 ℃ to prepare a p-type doping layer 2 to form an emitting region to form a PN junction, BBr3The concentration is 12mg/cm3. The p-type doping layer 2 covers the surface of the n-type monocrystalline silicon substrate 1 and the inner wall of the nano hole.
After a sample is cleaned and dried, TiO is prepared by utilizing magnetron sputtering2A thin film layer 4 of high purity TiO2The target material is raw material with purity of 99.99 percent and local vacuum of 10 percent-5torr, argon is used as working gas, the temperature of the substrate is controlled at 350 ℃, annealing is carried out after film forming, the annealing temperature is 400 ℃, and the annealing time is 1.5 h. TiO22The thin film layer 4 is laminated on SiO2 An insulating layer 3 and a p-type doped layer 2 are formed on the substrate and filled in the embedded nano-holes. TiO22The thickness of the thin film layer 4 laminated on the surface of the p-type doped layer 2 was 100 nm.
After annealing and solidification, in TiO2Preparing a perovskite absorbing layer 5 on the thin film layer 4 by using a spin coating method, and coating 0.003molCH3NH3I (purity 99.5%) and 0.003mol PbI2(purity 99%) was added to a small beaker containing 1ml of N-dimethylformamide solution. ThroughStirring to obtain CH3NH3PbI3And (3) spin-coating the solution, dripping the perovskite solution on the substrate by using a glue homogenizing machine, homogenizing the solution, placing the homogenized solution on a glue baking machine, and fixing glue for 200 minutes at the glue fixing temperature of 85 ℃ to obtain a perovskite thin film with the thickness of 300nm to form the perovskite absorption layer 5. Arranging a Spiro-OMeTAD hole transport layer 6 with the thickness of 150nm on the perovskite absorption layer 5; an ITO film with the thickness of 50nm is arranged on the hole transport layer 6 and is a transparent conductive thin film layer 7, finally, an Ag metal electrode 8 with the thickness of 30nm is deposited on the upper surface of the transparent conductive thin film layer 7 and serves as an extraction electrode, an Al metal thin film layer 9 with the thickness of 50nm is deposited on the lower surface of the n-type monocrystalline silicon substrate 1, and the Ag metal electrode 8 and the Al metal thin film layer 9 serve as conductive electrodes to extract photo-generated charges to achieve power supply for an external circuit.
Example 2, referring to example 1, first, an n-type czochralski silicon wafer 8cm in size of × 8cm is selected as an n-type czochralski silicon substrate 1, the thickness of the n-type czochralski silicon wafer is 200 μm, the resistivity of the n-type czochralski silicon substrate is 1.6 Ω · cm., after cleaning, silver nano colloid is spin-coated on the silicon substrate by a spin coater, the rotation speed is 3200r/min, the diameter of silver nano particles is 350nm, the spin-coated silicon wafer is immersed in hydrogen peroxide solution for etching, the concentration of the solution is 1.2mol/L, the time is 0.5h, a vertical nano-hole periodic array structure 10 is formed, the period of the nano-hole periodic array structure 10 is 800nm, the diameter of a nano-hole is 480nm, the duty ratio is 0.6, the depth is 400nm, and the silver nano particles are.
After a sample is cleaned and dried, SiO is formed on the periphery of the surface of the n-type monocrystalline silicon substrate 1 by an oxidation etching process2Insulating layer 3 on SiO2The exposed area in the middle of the insulating layer 3 is a light receiving window, the size of the light receiving window is 5cm × 5 cm., the light receiving window is cleaned and dried by deionized water, and then the light receiving window is placed in a diffusion furnace to be BBr3The liquid boron source is diffused at high temperature of 1100 ℃ to prepare a p-type doping layer 2 to form an emitting region to form a PN junction, BBr3The concentration is 12mg/cm3. The p-type doping layer 2 covers the surface of the n-type monocrystalline silicon substrate 1 and the inner wall of the nano hole.
After a sample is cleaned and dried, TiO is prepared by utilizing magnetron sputtering2A thin film layer 4 of high purity TiO2The target material is raw material with purity of 99.99 percent and local vacuum of 10 percent-5torr, argon is used as working gas, the temperature of the substrate is controlled at 350 ℃, annealing is carried out after film forming, the annealing temperature is 400 ℃, and the annealing time is 1.5 h. TiO22The thin film layer 4 is laminated on SiO2 An insulating layer 3 and a p-type doped layer 2 are formed on the substrate and filled in the embedded nano-holes. TiO22The thickness of the thin film layer 4 laminated on the surface of the p-type doped layer 2 was 100 nm.
After annealing and solidification, in TiO2Preparing a perovskite absorbing layer 5 on the thin film layer 4 by using a spin coating method, and coating 0.003molCH3NH3I (purity 99.5%) and 0.003mol PbI2(purity 99%) was added to a small beaker containing 1ml of N-dimethylformamide solution. Stirring to obtain CH3NH3PbI3And (3) spin-coating the solution, dripping the perovskite solution on the substrate by using a glue homogenizing machine, homogenizing the solution, placing the homogenized solution on a glue baking machine, and fixing glue for 200 minutes at the glue fixing temperature of 85 ℃ to obtain a perovskite thin film with the thickness of 300nm to form the perovskite absorption layer 5. Arranging a Spiro-OMeTAD hole transport layer 6 with the thickness of 150nm on the perovskite absorption layer 5; an ITO film with the thickness of 50nm is arranged on the hole transport layer 6 and is a transparent conductive thin film layer 7, finally, an Ag metal electrode 8 with the thickness of 30nm is deposited on the upper surface of the transparent conductive thin film layer 7 and serves as an extraction electrode, an Al metal thin film layer 9 with the thickness of 50nm is deposited on the lower surface of the n-type monocrystalline silicon substrate 1, and the Ag metal electrode 8 and the Al metal thin film layer 9 serve as conductive electrodes to extract photo-generated charges to achieve power supply for an external circuit.
Example 3, referring to example 1, first, an n-type czochralski silicon wafer 8cm in size of × 8cm is selected as an n-type czochralski silicon substrate 1, the thickness of the n-type czochralski silicon wafer is 200 μm, the resistivity of the n-type czochralski silicon substrate is 1.6 Ω · cm., after cleaning, silver nano colloid is spin-coated on the silicon substrate by a spin coater, the rotation speed is 3200r/min, the diameter of silver nano particles is 350nm, the spin-coated silicon wafer is immersed in hydrogen peroxide solution for etching, the concentration of the solution is 1.2mol/L, the time is 0.5h, a vertical nano-hole periodic array structure 10 is formed, the period of the nano-hole periodic array structure 10 is 800nm, the diameter of a nano-hole is 640nm, the duty ratio is 0.8, the depth is 400nm, and the silver nano particles are.
Cleaning and drying the sample, and performing oxidation etching process on the periphery of the surface of the n-type monocrystalline silicon substrate 1Formation of SiO2Insulating layer 3 on SiO2The exposed area in the middle of the insulating layer 3 is a light receiving window, the size of the light receiving window is 5cm × 5 cm., the light receiving window is cleaned and dried by deionized water, and then the light receiving window is placed in a diffusion furnace to be BBr3The liquid boron source is diffused at high temperature of 1100 ℃ to prepare a p-type doping layer 2 to form an emitting region to form a PN junction, BBr3The concentration is 12mg/cm3. The p-type doping layer 2 covers the surface of the n-type monocrystalline silicon substrate 1 and the inner wall of the nano hole.
After a sample is cleaned and dried, TiO is prepared by utilizing magnetron sputtering2A thin film layer 4 of high purity TiO2The target material is raw material with purity of 99.99 percent and local vacuum of 10 percent-5torr, argon is used as working gas, the temperature of the substrate is controlled at 350 ℃, annealing is carried out after film forming, the annealing temperature is 400 ℃, and the annealing time is 1.5 h. TiO22The thin film layer 4 is laminated on SiO2 An insulating layer 3 and a p-type doped layer 2 are formed on the substrate and filled in the embedded nano-holes. TiO22The thickness of the thin film layer 4 laminated on the surface of the p-type doped layer 2 was 100 nm.
After annealing and solidification, in TiO2Preparing a perovskite absorbing layer 5 on the thin film layer 4 by using a spin coating method, and coating 0.003molCH3NH3I (purity 99.5%) and 0.003mol PbI2(purity 99%) was added to a small beaker containing 1ml of N-dimethylformamide solution. Stirring to obtain CH3NH3PbI3And (3) spin-coating the solution, dripping the perovskite solution on the substrate by using a glue homogenizing machine, homogenizing the solution, placing the homogenized solution on a glue baking machine, and fixing glue for 200 minutes at the glue fixing temperature of 85 ℃ to obtain a perovskite thin film with the thickness of 300nm to form the perovskite absorption layer 5. Arranging a Spiro-OMeTAD hole transport layer 6 with the thickness of 150nm on the perovskite absorption layer 5; an ITO film with the thickness of 50nm is arranged on the hole transport layer 6 and is a transparent conductive thin film layer 7, finally, an Ag metal electrode 8 with the thickness of 30nm is deposited on the upper surface of the transparent conductive thin film layer 7 and serves as an extraction electrode, an Al metal thin film layer 9 with the thickness of 50nm is deposited on the lower surface of the n-type monocrystalline silicon substrate 1, and the Ag metal electrode 8 and the Al metal thin film layer 9 serve as conductive electrodes to extract photo-generated charges to achieve power supply for an external circuit.
Example 4, referring to example 1, first, an n-type czochralski silicon wafer having a size of 8cm × 8cm, a thickness of 200 μm, a resistivity of 1.6 Ω · cm. was selected as an n-type single crystal silicon substrate 1, and after cleaning, silver nano colloid was spin-coated on the silicon substrate by a spin coater at a rotation speed of 3200r/min and a diameter of silver nano particles of 350nm, and the spin-coated silicon wafer was immersed in an aqueous hydrogen peroxide solution to be etched at a concentration of 1.2mol/L for 0.5h to form a vertical periodic array structure 10 of nano holes, wherein the period of the periodic array structure 10 of nano holes was 600nm, the diameter of nano holes was 300nm, a duty ratio of 0.5 and a depth of 100nm, and the silver nano particles were removed by a nitric acid solution after forming the silicon hole array.
After a sample is cleaned and dried, SiO is formed on the periphery of the surface of the n-type monocrystalline silicon substrate 1 by an oxidation etching process2Insulating layer 3 on SiO2The exposed area in the middle of the insulating layer 3 is a light receiving window, the size of the light receiving window is 5cm × 5 cm., the light receiving window is cleaned and dried by deionized water, and then the light receiving window is placed in a diffusion furnace to be BBr3The liquid boron source is diffused at high temperature of 1100 ℃ to prepare a p-type doping layer 2 to form an emitting region to form a PN junction, BBr3The concentration is 12mg/cm3. The p-type doping layer 2 covers the surface of the n-type monocrystalline silicon substrate 1 and the inner wall of the nano hole.
After a sample is cleaned and dried, TiO is prepared by utilizing magnetron sputtering2A thin film layer 4 of high purity TiO2The target material is raw material with purity of 99.99 percent and local vacuum of 10 percent-4torr, argon is used as working gas, the temperature of the substrate is controlled at 350 ℃, annealing is carried out after film forming, the annealing temperature is 450 ℃, and the annealing time is 2 hours. TiO22The thin film layer 4 is laminated on SiO2 An insulating layer 3 and a p-type doped layer 2 are formed on the substrate and filled in the embedded nano-holes. TiO22The thin film layer 4 was laminated on the surface of the p-type doped layer 2 to a thickness of 150 nm.
After annealing and solidification, in TiO2Preparing a perovskite absorbing layer 5 on the thin film layer 4 by using a spin coating method, and coating 0.003molCH3NH3I (purity 99.5%) and 0.003mol PbI2(purity 99%) was added to a small beaker containing 1ml of N-dimethylformamide solution. Stirring to obtain CH3NH3PbI3Spin coating solution, dripping the perovskite solution on a substrate by using a glue homogenizing machine, homogenizing the solution, placing the solution on a glue baking machine for glue fixing for 200 minutes at the glue fixing temperature of 85 ℃, and obtaining the perovskite thin film with the thickness of 300nmThe film constitutes the perovskite absorption layer 5. Arranging a Spiro-OMeTAD hole transport layer 6 with the thickness of 150nm on the perovskite absorption layer 5; an ITO film with the thickness of 50nm is arranged on the hole transport layer 6 and is a transparent conductive thin film layer 7, finally, an Ag metal electrode 8 with the thickness of 30nm is deposited on the upper surface of the transparent conductive thin film layer 7 and serves as an extraction electrode, an Al metal thin film layer 9 with the thickness of 50nm is deposited on the lower surface of the n-type monocrystalline silicon substrate 1, and the Ag metal electrode 8 and the Al metal thin film layer 9 serve as conductive electrodes to extract photo-generated charges to achieve power supply for an external circuit.
Example 5, referring to example 1, first, an n-type czochralski single crystal silicon wafer 8cm in size of × 8cm is selected as an n-type czochralski single crystal silicon substrate 1, the thickness of the n-type czochralski single crystal silicon wafer is 200 μm, the resistivity of the n-type czochralski single crystal silicon substrate is 1.6 Ω · cm., after cleaning, silver nano colloid is spin-coated on the silicon substrate by a spin coater, the rotation speed is 3200r/min, the diameter of silver nano particles is 350nm, the spin-coated silicon wafer is immersed in hydrogen peroxide solution for etching, the concentration of the solution is 1.2mol/L, the time is 0.5h, a vertical nano-hole periodic array structure 10 is formed, the period of the nano-hole periodic array structure 10 is 600nm, the diameter of a nano hole is 300nm, the duty ratio is 0.5, the depth is 300 nm.
After a sample is cleaned and dried, SiO is formed on the periphery of the surface of the n-type monocrystalline silicon substrate 1 by an oxidation etching process2Insulating layer 3 on SiO2The exposed area in the middle of the insulating layer 3 is a light receiving window, the size of the light receiving window is 5cm × 5 cm., the light receiving window is cleaned and dried by deionized water, and then the light receiving window is placed in a diffusion furnace to be BBr3The liquid boron source is diffused at high temperature of 1100 ℃ to prepare a p-type doping layer 2 to form an emitting region to form a PN junction, BBr3The concentration is 12mg/cm3. The p-type doping layer 2 covers the surface of the n-type monocrystalline silicon substrate 1 and the inner wall of the nano hole.
After a sample is cleaned and dried, TiO is prepared by utilizing magnetron sputtering2A thin film layer 4 of high purity TiO2The target material is raw material with purity of 99.99 percent and local vacuum of 10 percent-4torr, argon is used as working gas, the temperature of the substrate is controlled at 350 ℃, annealing is carried out after film forming, the annealing temperature is 450 ℃, and the annealing time is 2 hours. TiO22The thin film layer 4 is laminated on SiO2 An insulating layer 3 and a p-type doped layer 2 filled with embedded nano-particlesIn the hole. TiO22The thin film layer 4 was laminated on the surface of the p-type doped layer 2 to a thickness of 150 nm.
After annealing and solidification, in TiO2Preparing a perovskite absorbing layer 5 on the thin film layer 4 by using a spin coating method, and coating 0.003molCH3NH3I (purity 99.5%) and 0.003mol PbI2(purity 99%) was added to a small beaker containing 1ml of N-dimethylformamide solution. Stirring to obtain CH3NH3PbI3And (3) spin-coating the solution, dripping the perovskite solution on the substrate by using a glue homogenizing machine, homogenizing the solution, placing the homogenized solution on a glue baking machine, and fixing glue for 200 minutes at the glue fixing temperature of 85 ℃ to obtain a perovskite thin film with the thickness of 300nm to form the perovskite absorption layer 5. Arranging a Spiro-OMeTAD hole transport layer 6 with the thickness of 150nm on the perovskite absorption layer 5; an ITO film with the thickness of 50nm is arranged on the hole transport layer 6 and is a transparent conductive thin film layer 7, finally, an Ag metal electrode 8 with the thickness of 30nm is deposited on the upper surface of the transparent conductive thin film layer 7 and serves as an extraction electrode, an Al metal thin film layer 9 with the thickness of 50nm is deposited on the lower surface of the n-type monocrystalline silicon substrate 1, and the Ag metal electrode 8 and the Al metal thin film layer 9 serve as conductive electrodes to extract photo-generated charges to achieve power supply for an external circuit.
Example 6, referring to example 1, first, an n-type czochralski single crystal silicon wafer 8cm in size of × 8cm is selected as an n-type czochralski single crystal silicon substrate 1, the thickness of the n-type czochralski single crystal silicon wafer is 200 μm, the resistivity of the n-type czochralski single crystal silicon substrate is 1.6 Ω · cm., after cleaning, silver nano colloid is spin-coated on the silicon substrate by a spin coater, the rotation speed is 3200r/min, the diameter of silver nano particles is 350nm, the spin-coated silicon wafer is immersed in hydrogen peroxide solution for etching, the concentration of the solution is 1.2mol/L, the time is 0.5h, a vertical nano-hole periodic array structure 10 is formed, the period of the nano-hole periodic array structure 10 is 600nm, the diameter of a nano hole is 300nm, the duty ratio is 0.5, the depth is 600 nm.
After a sample is cleaned and dried, SiO is formed on the periphery of the surface of the n-type monocrystalline silicon substrate 1 by an oxidation etching process2Insulating layer 3 on SiO2The exposed area in the middle of the insulating layer 3 is a light receiving window, the size of the light receiving window is 5cm × 5 cm., the light receiving window is cleaned and dried by deionized water, and then the light receiving window is placed in a diffusion furnace to be BBr3The liquid boron source is subjected to high temperature of 1100 DEG CDiffusion preparation of the p-type doped layer 2 to form an emitter region, forming a PN junction, BBr3The concentration is 12mg/cm3. The p-type doping layer 2 covers the surface of the n-type monocrystalline silicon substrate 1 and the inner wall of the nano hole.
After a sample is cleaned and dried, TiO is prepared by utilizing magnetron sputtering2A thin film layer 4 of high purity TiO2The target material is raw material with purity of 99.99 percent and local vacuum of 10 percent-4torr, argon is used as working gas, the temperature of the substrate is controlled at 350 ℃, annealing is carried out after film forming, the annealing temperature is 450 ℃, and the annealing time is 2 hours. TiO22The thin film layer 4 is laminated on SiO2 An insulating layer 3 and a p-type doped layer 2 are formed on the substrate and filled in the embedded nano-holes. TiO22The thin film layer 4 was laminated on the surface of the p-type doped layer 2 to a thickness of 150 nm.
After annealing and solidification, in TiO2Preparing a perovskite absorbing layer 5 on the thin film layer 4 by using a spin coating method, and coating 0.003molCH3NH3I (purity 99.5%) and 0.003mol PbI2(purity 99%) was added to a small beaker containing 1ml of N-dimethylformamide solution. Stirring to obtain CH3NH3PbI3And (3) spin-coating the solution, dripping the perovskite solution on the substrate by using a glue homogenizing machine, homogenizing the solution, placing the homogenized solution on a glue baking machine, and fixing glue for 200 minutes at the glue fixing temperature of 85 ℃ to obtain a perovskite thin film with the thickness of 300nm to form the perovskite absorption layer 5. Arranging a Spiro-OMeTAD hole transport layer 6 with the thickness of 150nm on the perovskite absorption layer 5; an ITO film with the thickness of 50nm is arranged on the hole transport layer 6 and is a transparent conductive thin film layer 7, finally, an Ag metal electrode 8 with the thickness of 30nm is deposited on the upper surface of the transparent conductive thin film layer 7 and serves as an extraction electrode, an Al metal thin film layer 9 with the thickness of 50nm is deposited on the lower surface of the n-type monocrystalline silicon substrate 1, and the Ag metal electrode 8 and the Al metal thin film layer 9 serve as conductive electrodes to extract photo-generated charges to achieve power supply for an external circuit.
In other embodiments of the present invention, the periodic array structure of the nano-pores can be prepared according to the following parameters, wherein the period is 200-900 nm, the diameter of the nano-pores is 50-800 nm, the depth is 100-1000 nm, and the duty ratio is 0.4-0.8.
The comparative example is a planar structure perovskite silicon-based solar cell, and it can be seen from fig. 3 that, in examples 1, 2 and 3, compared with the comparative example, the photon absorption efficiency of the whole solar band (300-.
As can be seen from FIG. 4, based on example 1, the photocurrent density at different periods (100-900nm) was calculated for the nanopore periodic array structure with the pore diameter of 320nm and the pore depth of 400nm, and as the period of the nanopore periodic array increases, the photocurrent density gradually becomes saturated at 600nm and an inflection point appears at 800 nm.
From fig. 5 to fig. 12, it can be seen that in examples 4, 5 and 6, compared with the comparative example, as the depth of the nanopore is increased, the electric field density under the action of both 600nm photons and 900nm photons is increased, but the resonant absorption mechanism of the long-wave photons is increased more obviously, and the complementary photon absorption of the tandem cell is realized.
Claims (10)
1. A silicon-based array laminated solar cell comprises a bottom cell structure and a top cell structure, and is characterized in that the top cell structure is laminated on the bottom cell structure, the bottom cell structure comprises an n-type monocrystalline silicon substrate, and SiO (silicon dioxide) is arranged on the periphery of the upper surface of the n-type monocrystalline silicon substrate2The insulating layer is used for forming a light receiving window in the central area of the n-type monocrystalline silicon substrate, the n-type monocrystalline silicon substrate in the light receiving window area is etched to prepare a vertical nanopore periodic array structure, a p-type doped layer is prepared on the n-type monocrystalline silicon substrate in the light receiving window area and the inner wall of a nanopore of the nanopore periodic array structure, and a metal thin film layer is arranged on the lower surface of the n-type monocrystalline silicon substrate; the top cell structure sequentially comprises TiO from bottom to top2A thin film layer, a perovskite absorption layer, a hole transport layer, a transparent conductive thin film layer and a metal electrode, wherein the TiO is2A thin film layer laminated on the SiO2An insulating layer and the p-type doping layer are arranged above the substrate and are filled and embedded into the nano holes; the metal electrode and the metal film layer are respectively led out to be used as a guideThe electrode supplies power to an external circuit.
2. The silicon-based array tandem solar cell according to claim 1, wherein the period of the periodic array structure of the nano-holes is 200-900 nm, the diameter of the nano-holes of the periodic array structure of the nano-holes is 50-800 nm, the depth of the nano-holes is 100-1000 nm, and the duty ratio of the periodic array structure of the nano-holes is 0.4-0.8.
3. The silicon-based array tandem solar cell of claim 1, wherein said TiO is2The thickness of the thin film layer stacked on the surface of the p-type doped layer is 100-150 nm.
4. The silicon-based array tandem solar cell according to claim 1, wherein the thickness of the perovskite absorption layer is 100-500 nm.
5. The silicon-based array tandem solar cell of claim 1, wherein the hole transport layer is one of nickel oxide, tungsten oxide, and Spiro-OMeTAD, and has a thickness of 150-800 nm.
6. The silicon-based array tandem solar cell of claim 1, wherein the metal electrode is made of one of Au, Ag, Al, Gu and Pt and has a thickness of 10-500 nm.
7. A preparation method of a silicon-based array tandem solar cell is characterized by sequentially comprising the following steps: firstly, preparing a nanopore periodic array structure in the vertical direction on the upper surface of an n-type monocrystalline silicon substrate by using a metal-assisted chemical etching method; secondly, depositing a layer of SiO on the periphery of the n-type monocrystalline silicon substrate2The insulating layer forms a light receiving window; thirdly, preparing PN junctions on the upper surface of the n-type monocrystalline silicon substrate in the light receiving window region and the inner wall surface of the nano holes of the periodic array structure of the nano holes by utilizing high-temperature diffusion of a liquid boron source; fourthly, utilizing a magnetron sputtering method to form SiO2Insulating layer and PN junction surfacePreparation of TiO2The thin film layer is used as an electron transmission layer, and the TiO2The thin film layer is filled and embedded into the nano holes; fifthly, annealing and curing are carried out and the TiO2Preparing a perovskite absorption layer and a hole transport layer on the thin film layer in sequence by using a spin coating method; sixthly, respectively preparing a transparent conductive thin film layer and a metal electrode on the surface of the hole transport layer by adopting an electron beam evaporation process; and seventhly, depositing a metal thin film layer lead-out wire on the lower surface of the n-type monocrystalline silicon substrate to serve as the cathode of the silicon-based array laminated solar cell, wherein the metal electrode lead-out wire serves as the anode of the silicon-based array laminated solar cell.
8. The method for preparing the silicon-based array tandem solar cell according to claim 7, wherein during the preparation of the periodic array structure of the nano holes in the vertical direction by using the metal-assisted chemical method, a spin coater is used to spin-coat silver nano colloid on the n-type monocrystalline silicon substrate at a rotation speed of 2500-5000 r/min, and the diameter of the silver nano particles is 50-800 nm; after spin coating, immersing the substrate into a hydrogen peroxide solution for etching, wherein the concentration of the solution is 0.2-2 mol/L, and the time is 0.5-2 h; and removing the silver nanoparticles by using a nitric acid solution after the nanopore periodic array is formed.
9. The method for manufacturing a silicon-based array tandem solar cell according to claim 7, wherein the resistivity of the n-type single crystal silicon substrate is 1.2-1.3 Ω -cm, and the concentration of the n-type single crystal silicon substrate is 15-16 mg/cm when the n-type single crystal silicon substrate is used for manufacturing the PN junction by high temperature diffusion of a liquid boron source3BBr of3And (3) performing high-temperature diffusion on the liquid boron source at 1200-1250 ℃ to prepare the p-type doped layer.
10. The method of claim 9, wherein the method comprises magnetron sputtering TiO to form the silicon-based array tandem solar cell2In the case of a thin film layer, the purity of the TiO2 target material is 99.99 percent, and the local vacuum is 10 percent-3～10-5torr, argon is used as working gas, the annealing temperature is 380-650 ℃ during annealing and curing, the annealing time is 1-3 h, and the TiO2The thickness of the film laminated on the surface of the p-type doped layer is 100-150 nm.
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