CN102544223A - Method for preparing transparent electrode of crystalline silicon solar cell - Google Patents
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Abstract
The invention relates to a method for preparing a transparent electrode of a crystalline silicon solar cell, which comprises the following steps: A, an electrode sample is prepared, wherein a silver ink solution is dripped to the surface of a silicon chip with a pyramidal textured structure, and a uniformly distributed nano silver particle aggregate structure is formed on the surface of the whole silicon chip by adopting a dripping and coating method; and B, the electrode sample is sintered, wherein the electrode sample is heated through the microwave radiation so as to allow the nano silver particles to mutually fuse, thereby forming mutually connected metal nano wire/rod network structure. The preparation method provided by the invention is simple and has a low cost. The transparent electrode prepared by the method comprises micropores and mutually connected metal nano wires. The transparent electrodes prepared by the invention are arranged at the bottom of the pyramidal textured surface of the crystalline silicon solar cell and mutually connected, has the advantages of lower light reflection rate, better conductibility, and excellent potential carrier collection efficiency, can serve as a perfect substituent for a traditional silver grid electrode, and can improve the conversion efficiency of the solar battery, with reduced manufacturing cost.
Description
Technical field
The invention belongs to photovoltaic application and photovoltaic applications technical field, particularly a kind of preparation method of crystal silicon solar energy battery transparency electrode.
Background technology
Along with traditional energies such as oil, coal storage capacity on earth gradually reduces, green energy resource solar energy more and more receives the concern in the world as the substitute of traditional energy.In Application of Solar Energy, solar cell is that sunlight is converted into the key element in the photoelectric technology of electric energy, and is widely used among the various fields.
The core texture of solar cell is the P-N knot.When the P-N that the sunlight that is higher than the semiconductor gap energy when energy incides solar cell ties, produce electron hole pair.Tie at P-N under the effect of built-in field, electron transfer is to the N layer, and the P layer is transferred in the hole simultaneously, between P layer and N layer, produces photoelectric effect thus.When the two ends of solar cell are connected in load or the system, can produce the electric energy of current forms.
Material according to being used to form intrinsic layer (being light absorbing zone) is divided into polytype with solar cell.Generally speaking, the silicon solar cell that has an intrinsic layer of being processed by silicon is the most general a kind of.Existing two types silicon solar cell: crystal type (monocrystalline or polycrystalline) solar cell and film-type (amorphous or crystallite) solar cell.Except this solar film battery of two types, also have cadmium telluride or CIS compound film solar cell, solar cell, DSSC, organic solar batteries or the like based on III-V family material.
Thin film solar cell can be practiced thrift cost, but that its fatal shortcoming is an efficient is very low, poor stability; Amorphous silicon thin-film solar cell efficient decay simultaneously is serious; Though cadmium telluride or CIS compound film solar battery efficiency are higher, its toxicity and need a large amount of factors such as rare elements of using to make a large amount of a lot of problems that exist of using of thin-film solar cells.
Crystal silicon solar energy battery is compared with the solar cell of other type has significant high conversion efficiency; Crystal silicon solar energy battery efficient has reached 25% in the laboratory; Monocrystalline silicon efficient is 18.8% in the industrialization, and polysilicon efficient is 16%, has occupied main photovoltaic market.It is higher that but its shortcoming is exactly raw material and manufacturing cost, therefore, if can reduce the prices of raw and semifnished materials and simplified manufacturing technique, will significantly reduce production costs and reduce the battery component price.Though near the theoretical efficiency of solar cell, solar cell industry efficient has very big gap from theoretical efficiency to the efficient of laboratory solar cell in addition.This real industrialization efficient mainly comes from the manufacture process of solar cell with the hysteresis of laboratory efficient.Preceding electrode is the important component part of solar cell, and to the efficient important influence of solar cell, its production cost approximately is 10% of an entire cell assembly cost simultaneously.The characteristic of preceding electrode is low reflection and high conductivity.The preceding electrode of conventional crystal silicon solar cell is to accomplish the collection of charge carrier and the conduction of electric current through the silver-colored grid of macro-size.
The laboratory solar battery sheet can prepare the preceding electrode part that the micro-dimension channelizing line is realized battery through the methods such as offset printing of costliness.And produce in the line at crystal silicon solar cell sheet, mainly be to obtain mm size silver grid now through silk screen printing silver slurry, realize the preceding electrode part of battery then through high temperature (~ 900 degrees centigrade) sintering silver grid.The purpose of high temperature sintering is to make silver slurry see through the silicon nitride film layer (this layer is mainly used in silicon face passivation and antireflective, is electric insulation layer) below the electrode, realizes the connection of electrode and emitter.
Like Fig. 1 is the typical monocrystalline silicon solar battery sheet (sketch map of 156mm * 156mm); 1 is the main grid line; 2 is time grid line; The grid line of this millimeter level height and width has caused tangible shadow effect to the battery front surface, has increased front surface to reflection of incident light rate (probably be total surface reflectivity ~ 15%).And the spacing between these grid lines is very big; In order to obtain electric conductivity (reducing the contact resistance of battery) preferably; Commercial crystal silicon solar energy battery emitter has all adopted n+ heavy doping; And the probability that the doping of excessive concentrations can cause auger recombination to take place increases, thereby has reduced the performance of whole emitter and the efficient of battery (~ 10% reduces).Simultaneously, the follow-up high-temperature sintering process of silver-colored grid also can impact the performance of p-n junction, thereby reduces the performance (~ 10% reduces) of battery.In conventional crystal silicon solar cell production process; The structure of electrode and the difference that manufacture craft has caused the efficient of laboratory battery and commercialization battery before the silvery grid of class; Therefore need new structure and new production technology replace traditional structure and technology, the efficient that improves crystal silicon solar energy battery with reduce cost.
For monocrystalline silicon, use the suede structure that anisotropy chemistry corroding method can be made pyramid shape on (100) surface, reduce the surface light reflection.Common this suede structure adopts chemical alkaline etching to realize.Through etching, on whole silicon wafer, obtain the pyramidal tetrahedron structure of random distribution.This microstructure has reduced the surface of silicon chip significantly to the reflection of incident light rate, from polished silicon slice ~ 40% reflectivity be reduced to etch silicon ~ 10% reflectivity, add that industrialized standard silicon nitride anti-reflection layer plated film can further reduce reflectivity to 4 ~ 7%.
The inventor is at patent (SUPER-TRANSPARENT ELECTRODE FOR PHOTOVOLTAIC APPLICATIONS; Attorney Docket No.:094505-013600/PRO, Electronically Filed) proposes between crystalline silicon pyramid matte deposition layer of metal network thin-film in and can realize electrode before low reflection and the high conductivity.Like Fig. 2, this before electrode be the bottom of surface of crystalline silicon pyramid suede structure or between, the metalolic network shape that it is shaped as at random mainly comprises the micropore 3 and interconnective metal nano spider lines 4 of pyramid diameter.
Summary of the invention
The technical problem that the present invention will solve is the preparation method that a kind of crystal silicon solar energy battery transparency electrode is provided to the deficiency of prior art, and this preparation method can improve the efficient of crystal silicon solar energy battery and reduce cost.The transparency electrode of making through this method shows lower light reflectivity and conductivity preferably, has the carrier collection efficient of potential excellence.
For solving the problems of the technologies described above, technical scheme of the present invention is: a kind of preparation method of crystal silicon solar energy battery transparency electrode comprises the steps:
Steps A is made electrode sample: promptly be added to the silicon chip surface with pyramid suede structure with silver-colored black drips of solution, make the surface of whole silicon wafer form equally distributed nano-Ag particles aggregate structure through drop-coating;
Step B, sintered electrode sample: promptly make the nano-Ag particles fusion and form interconnective metal nanometer line/excellent network with the carry out microwave radiation heating electrode sample.
Further preferred scheme is: the power of microwave radiation is 10 ~ 1000W among the step B, and the microwave temperature is 200 ~ 900 degrees centigrade, and the microwave time is 0.1 ~ 100 minute.
Further preferred scheme is: in the said steps A, the concentration that silver-colored black drips of solution is added to silicon chip surface is 0.51 mg/cm
2To 1.02 mg/cm
2
Further preferred scheme is: in the said steps A, and after silver-colored black drips of solution is added to silicon chip surface, at room temperature dry 1 to 5 minute.
Further preferred scheme is: said nano-Ag particles is spherical or bar-shaped or shaped particles such as cube or tetrahedron, helps the bottom of nano particle landing to pyramid suede structure.
Further preferred scheme is: silver-colored black formulations prepared from solutions process is described in the steps A:
A1: the ethylene glycol solvent of certain volume is heated to 160 degrees centigrade, kept 10 minutes;
A2: liquor argenti nitratis ophthalmicus and surfactant (PVP) solution are at the uniform velocity joined in the above-mentioned 160 degrees centigrade ethylene glycol solvent simultaneously, and high-speed stirred 10 minutes is treated to stop heating after solution colour becomes khaki;
A3: after treating that the A2 resultant solution cools off, get a certain amount of resultant solution with 5-10 ethanol or methyl alcohol dilution doubly, washing, and, after centrifugal the finishing, remove top clear liquid with 5000 commentaries on classics high speed centrifugations;
A4: repeat above-mentioned A3 twice, dilute according to the 1:1 volume ratio with methyl alcohol at last, the uniform Nano Silver methyl alcohol of ultrasonic formation soliquid, i.e. silver China ink.
Further preferred scheme is: the molar concentration rate of said liquor argenti nitratis ophthalmicus and surfactant (PVP) solution is 1:4.5 to 1:10.
Further preferred scheme is: the electrode sample of step B is in the microwave sintering process, and surfactant (PVP) layer on nano-Ag particles surface is removed, nano-Ag particles fusion and form interconnective metal nanometer line/excellent network.
Further preferred scheme is: the said nano-Ag particles diameter or the length of side are the 1-500 nanometers.
Compared with prior art, the present invention has following beneficial effect:
Preparation method of the present invention is easy, with low cost, adopts the transparency electrode of the present invention's preparation to comprise micron order micropore and interconnective metal nano spider lines.The transparency electrode of the present invention's preparation; Network is sprawled and be interconnected in pyramid matte bottom on the crystal silicon cell surface; Show conductivity (the battery series resistance is little) and lower light reflectivity (more multi-photon is absorbed by active layer) preferably simultaneously, electrode only leaves 2 ~ 3 microns in the entire cell surface distributed between the electrode simultaneously; With respect to conventional silver gate electrode (thousands of microns between the electrode), the electrode that the inventive method is made has the carrier collection efficient of potential excellence.And the electrode of the crystal silicon cell of employing the present invention making; Only need follow-up silicon nitride anti-reflection layer filming process; And do not need (perhaps reduce use) silk screen printing gate line electrode; Also do not need high-temperature sintering process, the crystal silicon cell electrode that the present invention proposes is not only the excellent replacer of conventional silver gate electrode, and can improve the conversion efficiency and the production cost that reduces battery of solar cell.
Description of drawings
Fig. 1 is the typical monocrystalline silicon solar battery sheet (sketch map of 156mm * 156mm);
Fig. 2 is the illustraton of model of transparency electrode;
Fig. 3 is the preparation flow figure of crystal silicon solar energy battery transparency electrode of the present invention;
Fig. 4 forms the continuous aggregate structure electron micrograph of nano particle in pyramid matte bottom later on for the black drop-coating of the present invention's silver;
The continuous metal nanometer line network structure electron micrograph that Fig. 5 forms later on for microwave radiation annealing of the present invention;
Fig. 6 (a) is the electron micrograph before electrode sample 1 sintering of the present invention;
Fig. 6 (b) is the electron micrograph behind electrode sample 1 sintering of the present invention;
Fig. 7 (a) is the electron micrograph before electrode sample 2 sintering of the present invention;
Fig. 7 (b) is the electron micrograph behind electrode sample 2 sintering of the present invention;
Fig. 8 (a) is the electron micrograph before electrode sample 3 sintering of the present invention;
Fig. 8 (b) is the electron micrograph behind electrode sample 3 sintering of the present invention;
Fig. 9 is electrode sample 2 reflectance maps of the present invention.
Embodiment
Below in conjunction with embodiment and accompanying drawing the present invention is carried out detailed description.
Show like Fig. 3; The invention discloses a kind of preparation method of crystal silicon solar energy battery transparency electrode; It comprises three key steps: the one, and Yin Mo (Silver ink) solution synthetic; The 2nd, have the deposition of the silicon face nano-Ag particles aggregate of pyramid suede structure, the 3rd, the annealing of metal nano silver particle sintering forms interconnective metal wire/metal bar network.
1, the preparation of the solution of Yin Mo (silver ink)
Used argent nano particle can be synthetic through wet chemical method in the electrode.It is synthetic that the present invention adopts more simple synthetic method promptly not have seed ethylene glycol solvent method.Ethylene glycol solvent with certain volume is heated to 160 degrees centigrade earlier, keeps 10 minutes.In ethylene glycol solvent, configure simultaneously liquor argenti nitratis ophthalmicus and surfactant (PVP) solution (the molar concentration rate 1:4.5 to 1:10 of silver nitrate and PVP) respectively; Liquor argenti nitratis ophthalmicus and two kinds of solution of surfactant (PVP) are at the uniform velocity joined in the above-mentioned 160 degrees centigrade ethylene glycol solvent simultaneously; High-speed stirred 10 minutes is treated to stop heating after solution colour becomes khaki.After the original solution cooling, get a certain amount of original solution with 5-10 ethanol or methyl alcohol dilution doubly, washing; And 5000 change high speed centrifugation, removes top clear liquid, dilution above repeating; Twice of washing and high speed centrifugation process; Use methyl alcohol according to 1:1 (volume of original solution is used the methyl alcohol volume ratio with dilution) dilution, the uniform Nano Silver methyl alcohol of ultrasonic formation soliquid, i.e. silver China ink at last.The nano-Ag particles that obtain this moment is a spheric granules, helps the bottom of nanosphere landing to pyramid suede structure like this.
2, the deposition process that has the silicon face silver nano-grain aggregate of pyramid suede structure
Utilize drop-coating to make electrode sample in the present embodiment; Specifically be on silicon face, to drip to many silver China inks through dripping 1 with pyramid suede structure; And at room temperature dry 1 to 5 minute; Let silver-colored black suspension spread at silicon face, nano-Ag particles is slipped to the bottom of pyramid structure (0.01 ~ 10 micron height and width) in diffusion process, form equally distributed nano-Ag particles aggregate structure on the surface of whole silicon wafer.
See Fig. 4; The electron microscope picture has explained that clearly nano-Ag particles has been slipped to the bottom of pyramid structure and has formed the also interconnective nano-Ag particles aggregate that comparatively evenly distributes, but each nano-Ag particles still independently exists and can under the observation of electron microscope, differentiate clearly.
3, the annealing of nano-Ag particles sintering forms interconnective metal wire/metal bar network development process
In order to improve the conductivity of pyramid structure bottom nano-Ag particles aggregate, can realize that the fusion between the nano-Ag particles forms interconnective metal nanometer line/excellent network through the method for sintering annealing, thereby improve its conductivity.
Carry out microwave radiation heating is at the metal particle (Fe on polished silicon slice or other materials surface; Cu; Ag and alloy thereof); Being used to improve it has had some research in the conductivity on surface, and the present invention is used in crystal silicon solar energy battery to microwave radiation, and is that the directed sintering that has the metallic particles under the structure that the pyramid matte is a template belongs to reported first.
We adopt microwave radiation to realize that the nano-Ag particles fusion obtains the metal nano network configuration in the present embodiment.The electrode sample that will have the nano-Ag particles aggregate places microwave irradiation, and the power of microwave radiation is 10 ~ 1000W, and the microwave temperature is 200 ~ 900 degrees centigrade, and the microwave time is 0.1 ~ 100 minute.Like Fig. 5, the explanation of electron microscope picture has formed interconnective metalolic network through nano-Ag particles aggregate after the microwave radiation.Electrode sample through having the nano-Ag particles aggregate structure is in the microwave sintering process, and the PVP layer on nano-Ag particles surface is removed, and nano-Ag particles fuses each other and forms interconnective meshed nano line.Fig. 5 shows that clearly the later electrode sample of process microwave annealing shows good network connectivity, has effectively improved the conductivity of electrode.
Introduce three kinds of electrodes that adopt the above-mentioned steps preparation below; Its difference is the used black amount difference of silver; Through controlling the number that drips of silver China ink, the silver-colored black concentration of silicon chip surface is respectively 0.255 mg/cm2,0.51 mg/cm2 and 1.02 mg/cm2; Three kinds of sample difference called after electrode sample 1,2 and 3.Like Fig. 6 (a) and (b) are electron micrographs of electrode sample 1 sintering front and back, and Fig. 7 (a) and (b) are the electron micrographs before and after electrode sample 2 sintering, and Fig. 8 (a) and (b) are the electron micrographs before and after electrode sample 3 sintering.
The nano-Ag particles diameter or the length of side are the 1-500 nanometers in the electrode sample, and the preferred diameter or the length of side are of a size of 200 nanometers in the present embodiment.Adopt the sheet resistance of four-point method specimen.The sheet resistance of sample 1,2 and 3 three kind of electrode sample is respectively before the annealing: 5000 Ω/, and 3000 Ω/ and 2000 Ω/, the resistance of three kinds of samples becomes respectively after stepping back: 3000 Ω/, 11 Ω/ and 3 Ω/.
Electrode sample 1 can't interconnect because the density of nano surface silver particle is too low; So its sheet resistance is still very high after the annealing; And electrode sample 2 with electrode sample 3 since the density of nano surface silver particle is enough and annealing process in obviously improved its conductivity, its sheet resistance has significant change before and after annealing.Yet along with the increase of nano surface silver grain density, its reflectivity obviously improves after the sintering, and the reflectivity of electrode sample 3 reaches 15% after annealing.And the density of the nano surface of electrode sample 2 silver particle is moderate, has lower reflectivity and conductivity preferably simultaneously.
As shown in Figure 7, be the electrode sample reflectivity in 2 each stages.The surface reflectivity of electrode sample 2 (crystalline silicon, silver-colored network electrode and industrial anti-reflection layer) is far smaller than 10% at visible light and near infrared region, and is almost equal with the reflectivity that is coated with the silicon nitride etch silicon face.Because its lower sheet resistance and conductivity preferably, this silver-colored network electrode will substitute or obviously reduce the use that conventional silver is starched, this will reduce the cost of manufacture of battery greatly.In fact, because the only several microns of distance between electrodes, this will improve the carrier collection rate greatly.
Compare with the manufacturing process of conventional batteries, use transparency electrode crystal silicon solar energy battery of the present invention can obviously reduce its operational sequence and equipment.Transparency electrode with crystal silicon cell of the present invention only needs follow-up silicon nitride anti-reflection layer (passivation layer) depositing of thin film, and does not need (perhaps reduce and use) silkscreen process, does not also need the high temperature sintering operation.
Because only several microns of the distances in the network electrode of the present invention between each small electrode; Photo-generated carrier only need transmit several microns (from silicon chip Anywhere to nano-electrode) just can arrive electrode, thousands of microns distance makes a sharp contrast between this and the conventional silver gate electrode.This superior characteristic can significantly reduce the doping of n+ layer to optimum level, and guarantees best p-n junction quality.
Above embodiment only is used to explain technical scheme of the present invention, but not to its restriction; Although the present invention has been carried out detailed explanation with reference to preferred embodiment; The those of ordinary skill in affiliated field is to be understood that; Still can specific embodiments of the invention make amendment or the part technical characterictic is equal to replacement; And not breaking away from the spirit of technical scheme of the present invention, it all should be encompassed in the middle of the technical scheme scope that the present invention asks for protection.
Claims (9)
1. the preparation method of a crystal silicon solar energy battery transparency electrode is characterized in that: comprise the steps:
Steps A is made electrode sample: promptly be added to the silicon chip surface with pyramid suede structure with silver-colored black drips of solution, make the surface of whole silicon wafer form equally distributed nano-Ag particles aggregate structure through drop-coating;
Step B, sintered electrode sample: promptly make the nano-Ag particles fusion and form interconnective metal nanometer line/excellent network configuration with the carry out microwave radiation heating electrode sample.
2. the preparation method of crystal silicon solar energy battery transparency electrode according to claim 1 is characterized in that: the power of microwave radiation is 10 ~ 1000W among the step B, and the microwave temperature is 200 ~ 900 degrees centigrade, and the microwave time is 0.1 ~ 100 minute.
3. the preparation method of crystal silicon solar energy battery transparency electrode according to claim 1 is characterized in that: in the said steps A, the concentration that silver-colored black drips of solution is added to silicon chip surface is 0.51 mg/cm
2To 1.02 mg/cm
2
4. the preparation method of crystal silicon solar energy battery transparency electrode according to claim 1 is characterized in that: in the said steps A, and after silver-colored black drips of solution is added to silicon chip surface, at room temperature dry 1 ~ 5 minute.
5. according to the preparation method of each described crystal silicon solar energy battery transparency electrode of claim 1 to 4, it is characterized in that: said nano-Ag particles is ball shape or bar-shaped or cubic shaped or tetrahedron shape.
6. according to the preparation method of each described crystal silicon solar energy battery transparency electrode of claim 1 to 4, it is characterized in that: silver-colored black formulations prepared from solutions process is described in the steps A:
A1: the ethylene glycol solvent of certain volume is heated to 160 degrees centigrade, kept 10 minutes;
A2: liquor argenti nitratis ophthalmicus and surfactant (PVP) solution are at the uniform velocity joined in the above-mentioned 160 degrees centigrade ethylene glycol solvent simultaneously, and high-speed stirred 10 minutes is treated to stop heating after solution colour becomes khaki;
A3: after treating that the A2 resultant solution cools off, get a certain amount of resultant solution with 5-10 ethanol or methyl alcohol dilution doubly, washing, and, after centrifugal the finishing, remove top clear liquid with 5000 commentaries on classics high speed centrifugations;
A4: repeat above-mentioned A3 twice, dilute according to the 1:1 volume ratio with methyl alcohol at last, the uniform Nano Silver methyl alcohol of ultrasonic formation soliquid, i.e. silver China ink.
7. the preparation method of crystal silicon solar energy battery transparency electrode according to claim 6 is characterized in that: the molar concentration of said liquor argenti nitratis ophthalmicus and surfactant (PVP) solution is 1:4.5 to 1:10.
8. the preparation method of crystal silicon solar energy battery transparency electrode according to claim 6; It is characterized in that: the electrode sample of step B is in the microwave sintering process; Surfactant (PVP) layer on nano-Ag particles surface is removed, nano-Ag particles fusion and form interconnective metal nanometer line/excellent network.
9. the preparation method of crystal silicon solar energy battery transparency electrode according to claim 8 is characterized in that: the said nano-Ag particles diameter or the length of side are the 1-500 nanometers.
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| US11417441B2 (en) * | 2015-01-30 | 2022-08-16 | Kuprion Inc. | Method of interconnecting nanowires, nanowire network and transparent conductive electrode |
| CN105118776A (en) * | 2015-07-01 | 2015-12-02 | 复旦大学 | Method for preparing high-performance TFT |
| CN105551687A (en) * | 2016-01-11 | 2016-05-04 | 电子科技大学 | Low-temperature microwave annealing method for lowering contact resistance among conductive micro nanowires |
| CN105845755A (en) * | 2016-05-12 | 2016-08-10 | 苏州协鑫集成科技工业应用研究院有限公司 | Heterojunction solar cell and manufacture method therefor |
| CN107302040B (en) * | 2017-06-22 | 2018-11-20 | 烟台南山学院 | The preparation method of Ag nano wire light trapping structure is inlayed based on wet etching silicon face |
| CN107302040A (en) * | 2017-06-22 | 2017-10-27 | 烟台南山学院 | The preparation method of Ag nano wire light trapping structures is inlayed based on wet etching silicon face |
| CN112054070A (en) * | 2020-07-27 | 2020-12-08 | 隆基绿能科技股份有限公司 | Silicon heterojunction solar cell and manufacturing method thereof |
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