CN101976710A - Method for preparing crystalline silicon hetero-junction solar cell based on hydrogenated microcrystalline silicon film - Google Patents

Method for preparing crystalline silicon hetero-junction solar cell based on hydrogenated microcrystalline silicon film Download PDF

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CN101976710A
CN101976710A CN2010105101072A CN201010510107A CN101976710A CN 101976710 A CN101976710 A CN 101976710A CN 2010105101072 A CN2010105101072 A CN 2010105101072A CN 201010510107 A CN201010510107 A CN 201010510107A CN 101976710 A CN101976710 A CN 101976710A
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孟凡英
汪建强
张松
程雪梅
韩涛
司新文
李翔
黄建华
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Shanghai Jiaotong University
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Abstract

The invention relates to a method for preparing a crystalline silicon hetero-junction solar cell based on a hydrogenated microcrystalline silicon film in the technical field of solar energy application. Combined a low temperature process of crystalline silicon and the hydrogenated silicon-based film with the characteristics of adjustable physical property, a surface of a P-type silicon chip can be effectively passivated and a PN junction can be manufactured. An Al2O3 or Al2O3/SiOx passive film is prepared on the back surface of the silicon chip by using atomic layer deposition (and plasma-reinforced chemical vapor deposition). Because the density of a negative charge in the Al2O3 film reaches as high as 10<11>cm<-2>, the passive film can reduce the probability of photo-induced minority carriers recombined on the back surface, improve the long wave quantum efficiency of the cell and create conditions for transporting and collecting the photo-induced carriers, therefore, the photoelectric conversion efficiency of the cell is enhanced.

Description

Preparation method based on the crystal silicon heterojunction solar battery of microcrystalline hydrogenated silicon film
Technical field
What the present invention relates to is a kind of method of application of solar, specifically is a kind of preparation method of the crystal silicon heterojunction solar battery based on the microcrystalline hydrogenated silicon film.
Background technology
21st century, energy crisis and environmental pollution have become the problem that the whole world is paid close attention to.The exploitation green energy resource becomes the main method that solves energy crisis.Wherein the development of solar cell along with the whole world for the attention of new energy development and significant progress is arranged, no matter be crystal silicon cell or hull cell, reducing cost, raising the efficiency is the main flow direction of its development.The cost of crystal silicon cell is subjected to the restriction of silicon materials, and the space that cost reduces is limited; Hull cell is because conversion efficiency is low and influence that be vulnerable to the S-W effect causes its less stable.In order to reduce cost in the high efficiency while of acquisition, the low cost of binding crystal silicon high stability, high efficiency and amorphous silicon becomes the focus of research and development in the heterojunction battery of one.
Find through retrieval prior art, Japanese Sanyo group developed a kind of novel battery structure in 1994, promptly in crystalline silicon and highly doped amorphous silicon layer, add one deck intrinsic amorphous silicon layer, form HIT (Heterojunction with intrinsic thin layer) structure.Owing to contain certain amount of H in the intrinsic amorphous silicon, when depositing to surface of crystalline silicon surface of crystalline silicon is played certain passivation, play simultaneously the effect of resilient coating between crystalline silicon and highly doped amorphous silicon, it is low effectively to have improved in the efficient of battery and the manufacturing process temperature.
Further retrieval is found, the research and development of Sanyo group be that the HIT battery laboratory of substrate has obtained 23% conversion efficiency with N type crystalline silicon, and industrialization produced certain amount of H IT battery component, efficient is also up to 19%.Because interfacial characteristics is the key factor that influence the heterojunction battery performance, except Sanyo group, other research unit all fails to reach so high conversion efficiency, even also still be that experimental result with Sanyo group has certain distance on software simulation.Sanyo group makes substrate with N type crystalline silicon to obtain very high efficient, yet because the high-quality P type amorphous silicon membrane difficulty of making is bigger, and when making substrate with N type crystalline silicon, back surface field cannot use Al back of the body field, therefore consider the factor on technology and the cost, it is on the heterojunction battery of substrate that at present a lot of research units still are placed on research emphasis with P type crystalline silicon.Amorphous silicon/crystalline silicon heterojunction battery is owing to the low deposition temperature of battery emitter region less than 200 ℃, and high open circuit voltage and low-temperature coefficient (<-0.25%) make this structure battery become the focus of research recent years.
The passivation film that crystalline silicon is commonly used is SiO at present 2, films such as SiNx, a-SiC, the positive charge of these film middle-high densities is disadvantageous to the surface passivation of highly doped P-type crystalline silicon.This is because the high density positive charge can cause the gathering of electronics, thereby causes the enhancing of recombination-rate surface.And for doped with P-type c-Si, these media that are rich in positive charge have tangible dependence in the passivation of P-type surface of crystalline silicon to charge carrier injection level, and along with its passivation quality of reduction of charge carrier injection level also decreases, and this is for injecting under the level conditions 510 low 14Cm -3, the battery of AM1.5 work is disadvantageous.
Summary of the invention
The present invention is directed to the prior art above shortcomings, a kind of preparation method of the crystal silicon heterojunction solar battery based on the microcrystalline hydrogenated silicon film is provided, combine crystalline silicon and hydrosilyl group thin film low temperature technology and the regulatable characteristics of rerum natura, can realize that the effective passivation and the PN junction of P type silicon chip surface make, adopt ald (chemical vapour deposition (CVD) that strengthens with plasma) preparation Al on silicon chip back of the body surface 2O 3Or Al 2O 3/ SiO xPassivating film is because Al 2O 3The density of negative electrical charge is up to 10 in the film 11Cm -2, this passivating film can reduce the probability of photoproduction minority carrier in back of the body surface recombination, improves the longwave optical quantum efficiency of battery, for photo-generated carrier transport and collection creates conditions, thereby improve the photoelectric conversion efficiency of battery.
The present invention is achieved by the following technical solutions, the present invention includes following steps:
The first step, employing aqueous slkali and acid solution carry out surperficial prerinse texture processing to p type single crystal silicon and polysilicon chip respectively, obtain the etch pit that is positioned at the pyramid structure of monocrystalline silicon surface and is positioned at polysilicon surface.
Described aqueous slkali is NaOH or KOH or its combination;
Described acid solution is HNO 3, HF or HCl or its combination.
The thickness of described silicon chip is 200 μ m, and the area of this silicon chip is 125 * 125mm 2, its resistivity is 1 Ω cm.
Described surperficial prerinse texture is handled and is meant: the SiO that removes silicon chip surface with the acid solution of 1-5% 2Layer about 50-100 ℃ prepares Pyramid matte in concentration less than 5% aqueous slkali to the p type single crystal silicon sheet, adopts the deionized water ultrasonic cleaning then and dries up.
Second goes on foot, prepares the microcrystalline hydrogenated silicon film and form PN junction at silicon chip surface with the hot-wire chemical gas-phase deposition system, specifically be meant: adopt hot-wire chemical gas-phase deposition equipment, with silane, phosphine and hydrogen is reacting gas, deposition obtains intrinsic micro crystal silicon thin film and doped microcrystalline silicon thin film successively on the p type monocrystalline silicon piece after the making herbs into wool, in order to form PN junction.
The Al on surface is carried on the back in the 3rd step, the chemical vapour deposition technique preparation of adopting ald and plasma to strengthen 2O 3Film or Al 2O 3/ SiO xThe dual layer passivation film, the back of the body surface field of formation battery reduces the compound of minority carrier, improves battery open circuit voltage.
The 4th step, employing sputtering method are at microcrystalline hydrogenated silicon film surface deposit transparent conductive oxide film, as surface electrode;
Described sputtering method is meant: as sputtering target material, feed argon gas and oxygen that volume ratio is 1/0.2-1/1 with ITO at ambient temperature, setting sputtering power is 20-200 watt, base vacuum about 1 * 10 -3Pa, by sputtering target material with atomic deposition to the emitter region of silicon chip, the thickness of the transparent conductive oxide film for preparing is 50-100nm.
The 5th step, employing silk screen printing backplate, silk screen printing front electrode through behind the alloying process, form solar cell.
Described silk screen printing back side Al slurry and back electrode are: adopt silk-screen printing technique printing back of the body surface field and back electrode.
Described silk screen printing front electrode is: adopt silk-screen printing technique printed silver slurry to form positive electrode.
Described alloying process is: carry out the alloying process of metal electrode and silicon in 100-800 ℃, purpose is to form ohmic contact, finally finishes the solar cell preparation.
The present invention relates to the crystal silicon heterojunction solar battery that method for preparing obtains based on the microcrystalline hydrogenated silicon film, comprise: front electrode, the ITO nesa coating, N-type microcrystalline hydrogenated silicon layer, the hydrogenation intrinsic microcrystalline silicon layer, P type crystalline silicon, back side aluminum membranous layer, back of the body surface field and backplate, wherein: intrinsic microcrystalline hydrogenated silicon layer is positioned at the front (being sensitive surface) of P-type silicon substrate, ITO nesa coating and N-type microcrystalline hydrogenated silicon layer are positioned at the hydrogenation intrinsic microcrystalline silicon layer outside successively, back side aluminum membranous layer and back of the body surface field are positioned at the back side (being shady face) of P-type silicon substrate successively, and front electrode and backplate lay respectively at the ITO nesa coating and the back of the body surface field outside.
The present invention has determined solar cell to have high open circuit voltage because the emitter region of the regulatable microcrystalline hydrogenated silicon thin-film material of rerum natura as battery arranged, and there is the Al of high-quality on battery back of the body surface 2O 3Film or Al 2O 3/ SiO xThe dual layer passivation film has determined that battery has stronger spectral response in the longwave optical scope, means under the same photoirradiation intensity, and this structure battery power output will be bigger.In addition, used chemical gas-phase deposition system equipment cost is low, technology is simple and film-forming temperature is low, energy consumption is little, process window is big, and the band gap and the degree of crystallization of microcrystalline hydrogenated silicon film are adjustable, and optical energy gap is in the 1.5-2.3eV scope, the aluminium that combines with conventional silk-screen printing technique is carried on the back the field, can promote the thermal stability of battery.
Solar battery structure of the present invention is transparent conductive oxide film/N type microcrystalline hydrogenated silicon/intrinsic microcrystalline hydrogenated silicon/P type crystalline silicon/Al 2O 3Film or Al 2O 3/ SiO xThe dual layer passivation film, this structure battery process processing procedure is finished under cryogenic conditions substantially, help industrialization, the cost that is increased is very low, but the output performance of battery has very big lifting, and the present invention simultaneously is subjected to the subsidy of the Shanghai City State Scientific and Technological Commission-Material Used International Technology cooperative fund source problem (No.08520741400).
Description of drawings
Fig. 1 is a schematic flow sheet of the present invention.
Fig. 2 is a solar cell junction composition of the present invention.
Embodiment
Below embodiments of the invention are elaborated, present embodiment is being to implement under the prerequisite with the technical solution of the present invention, provided detailed execution mode and concrete operating process, but protection scope of the present invention is not limited to following embodiment.
As shown in Figure 1, present embodiment adopts the semiconductor cleaning to surface prerinse of p type single crystal silicon sheet and surperficial texture.The about 200 μ m of used silicon wafer thickness, area 125 * 125mm 2Standard side's sheet, resistivity 1 Ω cm, the hydrofluoric acid of the about 1-5% of usefulness is removed the SiO of silicon chip surface 2Layer.Next to the p type single crystal silicon sheet concentration less than the mixed solution of 3% NaOH and isopropyl alcohol (IPA) in about 80 ℃ preparation Pyramid matte.Adopt the deionized water ultrasonic cleaning then, and dry up with nitrogen.
Prepare the microcrystalline hydrogenated silicon film of intrinsic and the microcrystalline hydrogenated silicon film of doping successively with the hot-wire chemical gas-phase deposition system on the p type single crystal silicon matte, film thickness forms PN junction between doped microcrystalline silicon thin film and the crystal silicon chip between 5-50nm.
The surperficial Al of the chemical vapour deposition technique preparation back of the body that adopts ald and plasma to strengthen 2O 3Film, the about 100nm of thickness forms the backside passivation layer of battery and carries on the back the field.
Sputtering target material adopts the ITO material, feeds argon gas and oxygen at ambient temperature, and the ratio of argon gas and oxygen is about 1/0.2-1/1, and sputtering power is about 20-200 watt, base vacuum about 1 * 10 -3Pa, by sputtering target material with atomic deposition to the emitter region of silicon chip, the thickness of transparent conductive oxide film is about 80nm as surface electrode;
Adopt silk screen printing backplate, silk screen printing front electrode,, form solar cell through behind the alloying process.
Present embodiment is to microcrystalline hydrogenated silicon thin film passivation surface of crystalline silicon dangling bonds and defective, adopt hot wire chemical vapor deposition (HWCVD) system under<250 ℃ of cryogenic conditions, to prepare silicon thin film, by control process conditions (temperature, air pressure, time, power etc.), obtain microcrystalline hydrogenated silicon (μ c-Si:H) thin-film material, according to hydrogen at unstrpped gas (silane, hydrogen etc.) the ratio difference in, the crystallite dimension of microcrystalline hydrogenated silicon film is 20-100nm, and crystalline state is than being 5-50%, and growth for Thin Film speed is
Figure BDA0000028610840000041
Optical energy gap is 1.5-2.3eV, deposit this mixing phase film after the silicon chip minority carrier life time can improve about 90%.This mixing phase equipment for producing thin film is not expensive, the film deposition rate height, no plasma is to the bombardment damage of silicon face, the film crystalline state is bigger than adjustable scope, the material energy gap is big, hydrogen content is adjustable in the film, because of not containing a large amount of fixed positive charges in the film, so be fit to very much to P type silicon face carry out microcrystalline silicon film that passivation and N type mix in conjunction with after can form the PN junction of high-quality.
As shown in Figure 1, the crystallite silicon/crystalline silicon heterojunction solar battery structure that present embodiment relates to, i.e. microcrystalline hydrogenated silicon/crystalline silicon/Al 2O 3Film/aluminium back of the body field adopts hot-wire chemical gas-phase deposition (HWCVD) method to prepare the microcrystalline hydrogenated silicon film, as the emitter region and the resilient coating of solar cell front surface, thereby forms the PN heterojunction, in P type crystalline silicon back of the body surface employing ALD method depositing Al 2O 3Film as the surface passivated membrane of P type silicon, is made aluminium back of the body field by silk-screen printing technique afterwards, and the preceding electrode of battery and back electrode adopt conventional silk-screen printing technique to form alloy.This structure battery can effectively reduce the photoproduction minority carrier and carry on the back the compound of surface, and helps to improve the open circuit voltage and the short circuit current of solar cell, finally strengthens the photoelectric conversion efficiency of solar cell.
Present embodiment prepares high efficiency crystallite silicon/crystalline silicon heterojunction solar battery.Adopt the microcrystalline hydrogenated silicon film that mixes to form PN junction, and intrinsic microcrystalline hydrogenated silicon film is applied to dangling bonds and the defect state that comes the passivation surface of crystalline silicon between this PN, help the lifting of battery open circuit voltage as emitter region and crystalline silicon substrates.It is compound overleaf that present embodiment adopts the Al2O3 film can effectively reduce minority carrier as back of the body surface passivation layer, improves the long wave spectral response and the open circuit voltage of battery.The formation of the preparation of electrode and the back of the body is screen printing technique cheaply, this passivating technique is extremely important to more and more thinner crystal-silicon solar cell, its technological process as shown in Figure 1, can obviously improve spectral response and the open circuit voltage of battery, thereby improve the conversion efficiency of battery in the longwave optical part.
At first use chemical reagent (acid solution, aqueous slkali) to remove the affected layer of silicon chip surface, and texturing is carried out on the surface handled, purpose is the light capture ability that strengthens silicon chip surface.Next is to adopt HWCVD systems produce microcrystalline hydrogenated silicon film emitter region, forms PN junction with crystalline silicon, is being lower than under 500 ℃ the temperature Al (CH as reactant gas source with Al (CH3) and oxygen by the ALD system 3) decompose, and combine with oxygen, thereby acquisition has the film of passivation to P type silicon face.Ensuing processing step is conventional screen printing electrode and alloying, finally forms microcrystalline hydrogenated silicon/crystal silicon heterojunction solar battery.
As shown in Figure 2, the solar cell that present embodiment prepares comprises: front electrode 1, ITO nesa coating 2, N-type microcrystalline hydrogenated silicon layer 3, intrinsic microcrystalline hydrogenated silicon layer 4, back side aluminum membranous layer 5, backplate 6, back of the body surface field 7 and P-type silicon substrate 8, wherein: hydrogenation intrinsic microcrystalline silicon layer 4 and back side aluminum membranous layer 5 lay respectively at the front and back of P-type silicon substrate 8, ITO nesa coating 2 and N-type microcrystalline hydrogenated silicon layer 3 are positioned at hydrogenation intrinsic microcrystalline silicon layer 4 outsides successively, back of the body surface field 7 is positioned at back side aluminum membranous layer 5 outsides, and front electrode 1 and backplate 6 lay respectively on ITO nesa coating 2 and the back of the body surface field 7.
Present embodiment can adopt P type CZ monocrystalline silicon piece to prepare solar cell, is not carrying on the back surfaces A l 2O 3Passivating film and amorphous silicon membrane are done under the condition of emitter region, and the obtainable solar cell peak efficiency in laboratory is 18.4%.Adopt the preparation method of patent of the present invention, by setting up model and computer simulation, find that the open circuit voltage of battery can reach 680mV, photoelectric conversion efficiency can reach 22.7%, and the result is as shown in table 1.
Table 1N-type microcrystalline hydrogenated silicon/experiment of P-type crystal silicon heterojunction solar battery and analogue data
Solar battery structure/output parameter V oc(mV) Eff.%
ITO/n-μ c-Si:H/i-μ c-Si:H/pc-Si/ does not have the back of the body (experiment) 645.1 18.4
ITO/n-μ c-Si:H/i-μ c-Si:H/pc-Si/ does not have the back of the body (simulation) 646.1 19.0
ITO/n-μc-Si:H/i-μc-Si:H/pc-Si/Al 2O 3/ the back of the body (simulation) 680.2 22.7

Claims (6)

1. the preparation method based on the crystal silicon heterojunction solar battery of microcrystalline hydrogenated silicon film is characterized in that, may further comprise the steps:
The first step, employing aqueous slkali and acid solution carry out surperficial prerinse texture processing to p type single crystal silicon and polysilicon chip respectively, obtain the etch pit that is positioned at the pyramid structure of monocrystalline silicon surface and is positioned at polysilicon surface;
Second goes on foot, prepares the microcrystalline hydrogenated silicon film and form PN junction at silicon chip surface with the hot-wire chemical gas-phase deposition system, specifically be meant: adopt hot-wire chemical gas-phase deposition equipment, with silane, phosphine and hydrogen is reacting gas, deposition obtains intrinsic micro crystal silicon thin film and doped microcrystalline silicon thin film successively on the p type monocrystalline silicon piece after the making herbs into wool, in order to form PN junction;
The Al on surface is carried on the back in the 3rd step, the chemical vapour deposition technique preparation of adopting ald and plasma to strengthen 2O 3Film or Al 2O 3/ SiO xThe dual layer passivation film, the back of the body surface field of formation battery reduces the compound of minority carrier, improves battery open circuit voltage;
The 4th step, employing sputtering method are at microcrystalline hydrogenated silicon film surface deposit transparent conductive oxide film, as surface electrode;
The 5th step, employing silk screen printing backplate, silk screen printing front electrode through behind the alloying process, form solar cell.
2. the preparation method of the crystal silicon heterojunction solar battery based on the microcrystalline hydrogenated silicon film according to claim 1 is characterized in that described aqueous slkali is NaOH or KOH or its combination.
3. the preparation method of the crystal silicon heterojunction solar battery based on the microcrystalline hydrogenated silicon film according to claim 1 is characterized in that described acid solution is HNO 3, HF or HCl or its combination.
4. the preparation method of the crystal silicon heterojunction solar battery based on the microcrystalline hydrogenated silicon film according to claim 1 is characterized in that the thickness of described silicon chip is 200 μ m, and the area of this silicon chip is 125 * 125mm 2, its resistivity is 1 Ω cm.
5. the preparation method of the crystal silicon heterojunction solar battery based on the microcrystalline hydrogenated silicon film according to claim 1 is characterized in that, described surperficial prerinse texture is handled and is meant: the SiO that removes silicon chip surface with the acid solution of 1-5% 2Layer about 50-100 ℃ prepares Pyramid matte in concentration less than 5% aqueous slkali to the p type single crystal silicon sheet, adopts the deionized water ultrasonic cleaning then and dries up.
6. the preparation method of the crystal silicon heterojunction solar battery based on the microcrystalline hydrogenated silicon film according to claim 1, it is characterized in that, described sputtering method, be meant: with ITO as sputtering target material, feed argon gas and oxygen that volume ratio is 1/0.2-1/1 at ambient temperature, setting sputtering power is 20-200 watt, base vacuum about 1 * 10 -3Pa, by sputtering target material with atomic deposition to the emitter region of silicon chip, the thickness of the transparent conductive oxide film for preparing is 50-100nm.
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CN102222703A (en) * 2011-06-21 2011-10-19 中国科学院上海技术物理研究所 Hetero-junction-structured crystalline silicon solar cell with intrinsic layer and preparation method thereof
CN102364691A (en) * 2011-10-19 2012-02-29 中国科学院宁波材料技术与工程研究所 Crystalline silicon solar battery with upper/lower conversion luminescent structure and manufacturing method for crystalline silicon solar battery
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CN102386253A (en) * 2011-11-02 2012-03-21 北京汇天能光电技术有限公司 Interface treatment technology for hetero junction solar cell
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CN102364691A (en) * 2011-10-19 2012-02-29 中国科学院宁波材料技术与工程研究所 Crystalline silicon solar battery with upper/lower conversion luminescent structure and manufacturing method for crystalline silicon solar battery
CN102386253A (en) * 2011-11-02 2012-03-21 北京汇天能光电技术有限公司 Interface treatment technology for hetero junction solar cell
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CN102751369A (en) * 2012-06-20 2012-10-24 常州天合光能有限公司 Solar cell with N/P silicon-based heterojunction
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CN103594541A (en) * 2013-10-12 2014-02-19 南昌大学 Polycrystalline silicon/monocrystalline silicon heterojunction structure applied to solar cell and preparation method thereof
CN104393067A (en) * 2014-10-23 2015-03-04 天威新能源控股有限公司 Nanostructured solar cell and manufacturing method thereof
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