CN103579419A - Grapheme/MoS2/Si heterojunction thin-film solar cell and manufacturing method thereof - Google Patents
Grapheme/MoS2/Si heterojunction thin-film solar cell and manufacturing method thereof Download PDFInfo
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Abstract
The invention relates to a grapheme/MoS2/Si heterojunction thin-film solar cell and a manufacturing method thereof. A chemical vapor deposition method that gases carry liquid phase MoS2 molecules is adopted, the flow and the response speed can be well controlled, and an MoS2 thin film which is ultra-thin, even in large area, smooth in surface and small in roughness is obtained. Interface special shapes of a p-MoS2/n-Si heterojunction are effectively reduced, leak currents are reduced, and the photoelectric conversion efficiency of the solar cell is improved. The grapheme film which is even in large area and good in transparency and electric conductivity and obtained with the chemical vapor deposition method is used as a transparent electric conduction electrode. The MoS2-Si heterojunction has strong collecting function on photoproduction electrons and holes, and the photovoltaic effect and the conversion efficiency of the solar cell are improved. The solar cell has the open-circuit voltage of 0.98V, the short-circuit currents of 4.6mA and the light energy conversion efficiency of 4.5% under 100mW white light illumination.
Description
Technical Field
The invention relates to a solar cell, in particular to graphene/MoS2A/Si heterojunction solar cell and a preparation method thereof.
Background
MoS2Also called molybdenite, a black solid material having a metallic luster at normal temperature, has excellent chemical stability, thermal stability (melting point 1185 ℃) and lubricity, and is generally used for surface coatings or lubricants of machines and cutting tools. Structurally, molybdenite is in a hexagonal close-packed graphite layer structure, and the layers are combined by weak interaction van der waals forces. Similar to graphene in which graphite is easily exfoliated into monoatomic layers, molybdenite is also easily exfoliated into single-layer MoS by micro-mechanical exfoliation2Membrane [ S. Bertolazzi, J. Brivio, A. Kis, Stretching and Breaking of Ultrathin MoS2, ACS Nano, V. 5(12): 9703-9709, 2011.]. The single-layer MoS2 is a regular hexagonal planar structure formed by covalently bonding S-Mo-S triatomic bonds and has the thickness of only 0.65 nm.
Block MoS2Is an indirect bandgap (1.2eV) semiconductor, single layer MoS due to quantum confinement effect2Conversion to direct bandgap (1.8eV) [ K.F. Mak, C.Lee, J.Hone, J.Shan, T.F. Heinz, atomicaly thin MoS2: a new direct-gap semiconductor. Phys. Rev. Lett. V.105: 136805-08, 2010]. The indirect band gap is converted into the direct band gap, and the photon transition gain can be improved by 104Make a single layer of MoS2Has very high light absorption and light emission efficiency for visible light (300-700 nm) [ G. Eda, H. Yamaguchi, D. Voiry, T. Fujita, M. Chen, M. Chowalla, Correction to photo luminescence from chemical extruded MoS2, Nano Lett.V. 12(1), 526–526, 2012.]。
The silicon solar cell (monocrystalline silicon, polycrystalline silicon, amorphous silicon) has the advantages of mature preparation process, long service life and the like, and has the market share of more than 90 percent all the time. However, Si is an indirect bandgap semiconductor, and the light absorption efficiency is very low, so that the conversion efficiency of commercial silicon solar cells is generally lower than 20%. Lower conversion efficiency and higher cost have become bottlenecks in solar cells, severely limiting the development of the photovoltaic industry. It is known that the conversion efficiency of solar cells is determined by the photovoltaic effect of semiconductors. Therefore, the search for a solar cell material with a significant photovoltaic effect and low cost, and the realization of high conversion efficiency has become the main direction in the research field of solar cells at present.
Si is an indirect band gap semiconductor, the light absorption efficiency is very low, in addition, the absorption peak wavelength of silicon is 930 nm, the radiation of the near infrared band has better absorption, and the absorption to the visible light of 300-700 nm is relatively weaker. The conversion efficiency of the silicon solar cell is low. Single layer MoS2The material has strong absorption in a visible light band of 400-700 nm, and the absorption spectrum of the material is just complementary with the advantage of a Si absorption spectrum, so that the material covers the whole visible light and near infrared bands. If the single layer MoS is formed2Contact with Si to form MoS2the/Si heterojunction can greatly enhance the absorption of the device in the visible light wave band, remarkably improve the photovoltaic effect and the photoelectric conversion efficiency of the device and prepare high-efficiency MoS2a/Si heterojunction solar cell.
Graphene is a single-layer two-dimensional (2D) honeycomb crystal with a thickness of only 0.35 nm, formed by tightly stacking carbon atoms in hexagonal cells. Graphene is the thinnest, hardest, and fastest conducting electron material recognized in the world. The carrier mobility of the material is as high as 2 multiplied by 105cm2And/v is 100 times higher than the electron mobility in silicon. The graphene also has good optical properties, has visible light transmittance as high as 98.5%, and can be used for transparent conductive films and solar cells. Thus, in MoS2Graphene in a/Si heterojunction solar cell can be used as a transparent conductive thin film.
Disclosure of Invention
The invention aims to overcome the defects in the prior art and provide graphene/MoS capable of effectively improving photoelectric conversion efficiency2A/Si heterojunction solar cell and a preparation method thereof.
The technical scheme for realizing the aim of the invention is to provide graphene/MoS2A preparation method of a/Si heterojunction thin-film solar cell,the method comprises the following steps:
(1) cleaning a substrate: to be provided withnUsing a Si (111) sheet as a substrate, soaking with dilute HF acid to remove silicon dioxide on the surface of the Si, then sequentially ultrasonically cleaning with acetone, ethanol and deionized water to remove organic matters on the silicon sheet, blow-drying with nitrogen, and putting into a quartz tube for deposition treatment; the degree of vacuum of the quartz tube was 10-2Pa, heating to 300 ℃ and maintaining for 10 minutes to remove water vapor on the surface of the silicon wafer;
（2）MoS2preparing a film: heating a quartz tube to 500-600 ℃, using argon as carrying gas, and introducing MoS using dilute sulfuric acid as a solvent2Solution in said MoS2Adding Al (NO) to the solution3)3Solution of Al (NO)3)3As Al dopant pair MoS2P-type doping by mass ratio, MoS2 ：Al(NO3)3Is 1: 20-1: 50; gas carrying MoS2And Al (NO)3)3Into a quartz tubenAfter the-Si (111) sheet is adsorbed, nucleated and grown for 5-10 minutes, heating the quartz tube to 950 ℃ for annealing for 20-40 minutes to obtain MoS2a/Si pn junction;
(3) maintaining the temperature of the quartz tube at 950 ℃, decomposing methane into carbon atoms and hydrogen, and allowing the carbon atoms to reach the formed MoS under the action of gas phase transport with the flow of argon of 10-30 sccm2MoS of/Si pn junction2The graphene film is characterized in that the graphene film is a hexagonal network structure, and is adsorbed to the surface, nucleates on the surface of the substrate after the migration of the surface of the substrate, attracts other carbon atoms through van der waals attraction force, and forms a hexagonal network structure with the bonded carbon atoms;
(4) to pairnEvaporating an aluminum electrode on the lower surface of the Si (111) sheet to form a cathode of the solar cell, thereby obtaining the graphene/MoS2a/Si heterojunction solar cell.
The technical scheme of the invention also comprises the graphene/MoS prepared by the method2A/Si heterojunction thin-film solar cell.
The technical scheme of the invention has the beneficial effects that: due to the adoption of gas carrying liquid phase MoS2The chemical vapor deposition method of the molecule can better control the flow and the reaction speed, and obtain the ultrathin MoS with large area, uniformity and small surface flatness and roughness2Thin film, thereby effectively reducing p-MoS2The interface characteristic of the/n-Si heterojunction reduces leakage current and improves the photoelectric conversion efficiency of the solar cell. Meanwhile, the graphene film with large area, uniformity, good transparency and good conductivity can be obtained by using a chemical vapor deposition method.
Drawings
FIG. 1 shows a graphene/p-MoS structure provided by an embodiment of the present invention2A structural schematic diagram of the/n-Si heterojunction solar cell;
FIG. 2 shows graphene/MoS according to an embodiment of the present invention2A schematic energy band structure diagram of the/Si heterojunction solar cell;
FIG. 3 shows a graphene/MoS structure provided by an embodiment of the present invention2The working principle of the/Si heterojunction solar cell;
FIG. 4 is a MoS provided by an embodiment of the present invention2The thin film adopts a structural schematic diagram of a chemical vapor deposition system device;
FIGS. 5, 6 and 7 are views of a MoS prepared by a chemical vapor deposition method according to an embodiment of the present invention2The surface morphology, the X-ray diffraction pattern and the Raman spectrogram of the film;
FIG. 8 is a MoS prepared using a chemical vapor deposition process according to an embodiment of the present invention2A light absorption spectrum of the film;
FIG. 9 is a MoS provided by an embodiment of the present invention2MoS in/Si heterojunction2A current-voltage characteristic curve graph of the film surface;
fig. 10, 11 and 12 are a surface atomic force microscope photograph, a raman spectrum and an ultraviolet-visible light transmission spectrum of a graphene thin film provided by an embodiment of the present invention, respectively;
FIG. 13 shows a graphene/MoS structure according to an embodiment of the invention2A dark current-voltage characteristic curve diagram of a/Si heterojunction solar cell without illumination;
FIG. 14 shows graphene/MoS provided by an embodiment of the invention under 100mW white light illumination2A voltage-current characteristic curve diagram of the/Si solar cell;
FIG. 15 shows graphene/MoS provided by an embodiment of the invention under 100mW white light illumination2Response curve of the/Si solar cell;
in the figure, 1, a graphene electrode; 2. p-MoS2A thin film layer; 3. an n-Si conductive layer; 4. And an Al electrode.
Detailed Description
The technical scheme of the invention is further explained by combining the drawings and the embodiment.
Example 1
Referring to the attached FIG. 1, it is the graphene/MoS provided in this example2The structural schematic diagram of the/Si heterojunction solar cell comprises a graphene electrode 1 and p-MoS2A thin film layer 2, an n-Si layer 3 and an Al electrode 4; in FIG. 1, the graphene electrode is the anode of the solar cell, p-MoS2And the pn junction formed by the n-Si layer is a core unit of photoelectric conversion of the solar cell, and the Al electrode is a cathode of the solar cell.
Growth of ultra-thin MoS on n-type silicon wafers (111) using chemical vapor deposition2And the thin film (several atomic layers) is doped by utilizing Al atoms in the growth process of the thin film to enable the conductive type of the thin film to be P type, and the thin film is contacted with an n-type silicon wafer substrate to form a P-n junction. In p-type MoS2Growing 10-20 films on the surface of the film by using a chemical vapor deposition methodGraphene thin film with thick atomic layer, graphene thin film with thick atomic layer and MoS2the/Si pn junction jointly forms graphene/p-MoS2a/n-Si heterojunction solar cell.
See FIG. 2, which is MoS2A schematic energy band structure diagram of the/Si pn junction solar cell; in FIG. 2(a), MoS is shown on the left and right sides2The band structure before contact with Si. Wherein, 0Ethe vacuum level is set to be a vacuum level,Ｗ m is MoS2The work function of (a) is, fmFis MoS2The fermi level of (a) is, cmE、 vmE、Egmare respectively MoS2Conduction band, valence band energy level and band gap of m Is MoS2Electron affinity.Ｗ s Is a work function of Si and is, csE、 vsE、 gsErespectively the conduction band, the valence band energy level and the band gap, chi, of Si s Is the electron affinity of Si and is, fsFis the fermi level of Si. Delta Ec、ΔEvAre respectively MoS2Energy level difference with conduction band and valence band of Si.
MoS2Work function mW=E 0- fmESilicon wafer work function of 4.6 eV sW=E 0- fsE=χ+[ cE- fsE]For Si, χ =4.05 eV. cE- fsEDepending on the carrier concentration and doping type in the silicon wafer. Band gap of Si g EIs 1.12 eV, therefore,n-Si, mW> sWdue to MoS2Is greater than the work function of Si, i.e.Ｗ m >Ｗ s When they are in contact with each other, as shown in FIG. 2(b), holes on the surface of the Si wafer are oriented toward MoS2One side flows, and immobile negative ions (positive centers) are left on the surface of the Si sheet to form a space charge layer. Due to the movement of the n-side electrons to MoS2One side ofnThe surface of the Si sheet is formed with electron accumulation to form positive potential to make the conduction band csEValence band vsEThe end points are bent upwards as shown in fig. 2 (b). DqVIs MoS2The barrier height of the Si heterojunction. MoS2Andpp-n junction formation on-type silicon surface to form MoS2a/Si heterojunction solar cell.
The graphene/MoS provided by the embodiment2The photoelectric conversion principle of the/Si heterojunction solar cell is shown in the attached figure 3. Graphene layer, MoS2Thin film, p-MoS2The photoelectric conversion principle of the space charge region and the n-Si substrate formed by the/n-Si interface is as follows:
the transmissivity of the graphene is very high, and more than 85% of light is irradiated to MoS through the graphene under illumination2Film in MoS2Generating electron-hole pairs on the surface, and when the diffusion length of the photo-generated electrons is larger than MoS2Thickness of the film to diffuse into MoS2At the edge of the/Si heterojunction, the electric field in the space charge region of the heterojunctionＥ mS Under the action of the electron beam, the photo-generated electrons are quickly swept ton-a Si region forming an electron accumulation at the n-Si surface; MoS2The generated photo-generated holes are swept to the MoS2And forming a hole accumulation layer. Therefore, holes and electrons generated by light irradiation are respectively in the MoS2Surface andnsi formation accumulation, MoS2The voltage difference is generated by illumination without external bias voltage, so that the photovoltaic effect is achieved.
Due to the ultra-thin MoS2After only a few atomic layers, a portion of the light is also transparent to the MoS2Layer by layer intonThe Si layer is in turn absorbed by the Si layer (in particular near-infrared radiation around 900 nm), generating electron-hole pairs, which diffuse into the MoS2When the/Si heterojunction boundary is swept to the pn heterojunction under the action of the built-in electric field of the pn heterojunctionp-MoS2And photo-generated electrons are inn-Si-face accumulation. MoS2And further generating a voltage difference on two sides of the/Si heterojunction, thereby generating a photovoltaic effect. The photovoltaic effect will be superimposed on the above photovoltaic effect.
Photovoltaic effect on heterojunction solar cellsIn the course of formation, MoS2Built-in electric field in/SiＥ mS Which acts to accelerate the movement of the electrons. Compared with the traditional silicon pn junction solar cell, the heterojunction solar cell has double absorption effect, MoS2The solar cell mainly absorbs light radiation of 300-700 nm, Si mainly absorbs radiation of near-infrared bands, the absorption rate and the internal quantum efficiency of the solar cell are increased, the photovoltaic effect is remarkably increased, and therefore the conversion efficiency is greatly improved. By measuring the open circuit voltage of the deviceＶ oc And short circuit current density scJThe energy conversion efficiency of the double-junction solar cell can be calculated.
Referring to FIG. 4, the present example shows the preparation of MoS by Chemical Vapor Deposition (CVD)2The device structure of the film is shown schematically. The device is composed of four parts: a reaction deposition chamber consisting of a quartz tube, a vacuum pumping system, a gas mass flowmeter and a temperature control system. The substrate material adopts a material with the resistivity of 3-5 omega-cm and the crystal orientation (111)nSilicon (Si) plate of 12X 12 mm size2×500 μm。
The preparation method comprises the following steps:
cleaning a substrate: firstly, soaking with dilute HF acid for 15 minutes to remove silicon dioxide on the surface of Si, then sequentially carrying out ultrasonic cleaning with acetone, ethanol and deionized water to remove organic matters on a silicon wafer, finally blowing dry with nitrogen, and then placing into a quartz tube. Before deposition, the quartz tube was evacuated to 10 deg.C-2Pa, heating to 300 ℃ for 10 minutes to remove the moisture on the surface of the silicon wafer.
MoS2Preparing a film: heating a quartz tube to 500 ℃, using Ar gas as carrier gas, and introducing analytically pure MoS2Solution (dilute sulfuric acid as solvent). And analytically pure Al (NO)3)3As Al dopant pair MoS2P-type doping is performed. To at MoS2Doping while growing the film, in MoS2Adding Al (NO) into the solution at a mass ratio of 1:203)3And (3) solution. Argon carrying MoS2And Al (NO)3)3Into a quartz tubenThe Si (111) wafer was adsorbed, nucleated and grown for 10 minutes, and then the quartz tube was raised to 950 ℃ for annealing for 30 minutes.
Electrode manufacturing: the graphene is a transparent conductive film with excellent conductivity, has excellent conductivity, and can be used as an anode in a solar cell. And (3) growing graphene: the temperature of the quartz tube is still maintained at 950 ℃, methane is decomposed into carbon atoms and hydrogen at the high temperature of 800-950 ℃, and the carbon atoms reach the formed MoS under the action of gas phase transport with the flow of 10 sccm (10-30 sccm) of argon2MoS of/Si pn junction2The graphene film is characterized in that the graphene film is adsorbed to the surface, nucleation is finally carried out on the surface of the substrate after the surface of the substrate is migrated, other carbon atoms are attracted by Van der Waals attraction force and bonded with the other carbon atoms to form the graphene film with the hexagonal network structure. In general, the speed of CVD deposition of thin films is very fast with sufficient reactants. In the embodiment, the flow rate of the adopted methane is very small, only a small amount of carbon atoms reach the surface of the silicon wafer in unit time, and the ultrathin graphene film can be obtained by controlling the reaction time to be 5-10 minutes. After the reaction is finished, the temperature of the quartz tube is raised to 950-1000 ℃, and the sample is annealed for 10 minutes. And after the annealing is finished, taking out the sample after the quartz tube is naturally cooled to the room temperature.
And evaporating an aluminum electrode on the lower surface of the n-silicon wafer to form the cathode of the solar cell. Complete the graphene/MoS2And preparing the/Si heterojunction solar cell.
Preparing the obtained graphene/MoS2The method comprises the steps of measuring the surface appearance and the photovoltaic effect of the/Si heterojunction solar cell, and analyzing the surface appearance and the photocurrent characteristic of the device by utilizing an atomic force microscope, a current/voltage testing device and a Hall effect. Observing the thin film structure by using Raman spectrum, analyzing the transmittance of a sample by using an ultraviolet-visible light (UV-vis) spectrophotometer (Shimadzu UV-3600), and finally, obtaining the graphene/MoS2Photocurrent characteristics of the/Si heterojunction solar cells were measured using Keithley 4200 SCS.
Referring to FIGS. 5-7, FIG. 5 is a drawingnMultilayer MoS prepared on Si wafer2Typical atomic force microscopy of thin films. As can be seen, many MoS2The platelets are uniformly distributed on the surface of the Si wafer. The layer of MoS2The thickness of the thin film is about 5 to 10 nm, which is equivalent to a thickness of more than ten atomic layers. FIG. 6 shows the MoS prepared2X-ray diffraction spectra of the films. It was found that there were 6 very strong diffraction seams at angles 2 θ of 13.482 °, 32.997 °, 47.786 °, 14.460 °, 33.212 °, 47.898 °, which corresponded to MoS2Comparing the XRD standard cards of the crystals, wherein the diffraction peaks respectively correspond to MoS2(002) Diffraction peak positions of crystal planes of (104), (100), (105), (106) and (110) are substantially matched, which indicates that MoS grows2MoS with polycrystalline film2A film of (2). FIG. 7 is the MoS prepared2Raman spectroscopy of the film. The figure has 2 strong Raman vibration peaks at 385.5 cm−1Vibration peak of (E) corresponds to1 2gIn-plane vibration mode, and is located at 408.1cm-1Then correspond to (A)1g) Out-of-plane vibration mode1 2gAnd A1gIs MoS2Typical vibration modes, further demonstrating MoS2Existence of Structure in addition, A1gAnd E1 2gThe position difference (Δ) of the patterns can be used to roughly estimate the MoS2 Thickness of the film, larger Δ, MoS2 The greater the number of layers of film. Typically a single layer of MoS2 The difference Δ in position between these two modes of the membrane is 18. These two modes Δ in our samples are 22.6, illustrating the MoS grown in this example2 The film is a multilayer film.
See FIG. 8 for the MoS prepared2 The visible absorption spectrum of the film. The prepared MoS was measured using a UV-3600 spectrophotometer2Absorption spectra of film samples. It can be seen that molybdenum sulfide has strong absorption for visible light with a wavelength of 300-700 nm, which indicates that molybdenum sulfide can be used as a good light absorption material. Above 732nm, the absorption intensity decreases rapidly. Then 732nm is the absorption edge of the molybdenum sulfide thin film, and according to the relationship between the band gap width and the wavelength of the semiconductor material: eg=1.24/λ(eV) the prepared molybdenum sulfide thin film has a band gap width of 1.69 eV. The band gap width (1.8eV) of the single-layer molybdenum disulfide is smaller in the experiment because the band gap width of the molybdenum sulfide is reduced along with the increase of the layer number.
Referring to fig. 9, which is the surface I-V characteristics of the prepared molybdenum sulfide thin film, the conductive characteristics of the surface of the molybdenum sulfide thin film were measured using an HMS-3000 hall effect tester. Voltage Vab、Vbc、Vcd、VdaThe voltages between four symmetrical electrodes are respectively the surface a, b, c and d of the molybdenum sulfide film. It can be seen that the voltage between the four electrodes and the applied current I are approximately in a linear relationship, which shows that the molybdenum sulfide film has good surface conductivity. The line fluctuates a little because of some undulations in the sample surface or asymmetry between the electrodes. Hall coefficient of Hall Effect measurement RHThe conductivity type of the sample can be deduced according to the positive and negative values of the (A) and the (B), and the R of the sample provided by the inventionHIs 1.830X 107And the molybdenum sulfide film shows P-type characteristics through Al in-situ doping.
Referring to FIGS. 10-12, FIG. 10 shows a MoS2Atomic Force Microscope (AFM) photos of graphene thin film electrodes prepared on the thin film. It can be seen that many graphene platelets are uniformly distributed on the substrate. The thickness of the graphene film is about 3-5 nm, which is equivalent to a thickness of more than ten atomic layers. Fig. 11 is a raman spectrum of the graphene thin film electrode. The spectrum has 2 remarkable Raman vibration peaks, one is a G peak and is located at 1590 cm-1At wave number, the peak is the characteristic vibration peak of graphite; the other is that the 2D peak is positioned at 2690 cm-1At wave number, the data report that the peak position is the characteristic vibration peak of graphene. The intensity ratio of the two peaks isI 2D : I G=2.8, the larger the ratio, the larger the graphene phase contained in the film, the less the graphite phase; the graphene film prepared by the chemical vapor deposition method with low pressure and low flow rate has good quality. Fig. 12 is a visible light transmission spectrum of a graphene thin film electrode, which is a light transmission spectrum of the graphene thin film provided in this embodiment. It is composed ofThe light transmittance in the visible light region reaches more than 80%. In addition, the light transmittance thereof changes constantly with the change in wavelength. For the longer wavelength of 600-800 nm band, the transmittance exceeds 85%, and the high transmittance of the spectral band can effectively improve the conversion efficiency of the solar cell. And the carrier concentration and the electron mobility of the surface of the graphene are measured by using a Hall effect instrument. The carrier concentration of the surface of the prepared graphene film is 1010 cm-2Electron mobility of 9.5X 104 cm2 V-1 s-1This value is 2X 10 from the ideal value for graphene5 cm2 V-1 s-1The close proximity indicates that the graphene film prepared by the invention has good conductivity.
See FIG. 13 for graphene/MoS examples2Dark current characteristic (no-light characteristic) graph of/Si heterojunction solar cell; the result shows that the device has good rectification characteristic, and the current increases exponentially with the increase of the applied voltage. Under reverse bias, the reverse saturation leakage current is very small and almost zero.
See FIG. 14, which is at 100mW cm-2graphene/MoS provided by the embodiment under white light irradiation2Photocurrent characteristic curve of the/Si heterojunction solar cell. It can be seen that the open circuit voltage of the solar cellV oc0.89V, short-circuit current densityJ scIs 4.6 mA cm-2Can calculate, the graphene/MoS2The energy conversion efficiency of the/Si heterojunction solar cell is 4.5%.
Referring to fig. 15, it is a time response diagram of the solar cell provided in this embodiment. It can be seen that under illumination, the device has a steep rising edge; when the illumination is removed, the device has a vertical falling edge and good repeatability. Current on-off ratioI on/I offOver 103. The device has high response speed and high repeatability, and can be used as a high-performance optical detection and photoelectronic device.
Claims (2)
1. graphene/MoS2The preparation method of the/Si heterojunction thin-film solar cell is characterized by comprising the following steps:
(1) cleaning a substrate: to be provided withnUsing a Si (111) sheet as a substrate, soaking with dilute HF acid to remove silicon dioxide on the surface of the Si, then sequentially ultrasonically cleaning with acetone, ethanol and deionized water to remove organic matters on the silicon sheet, blow-drying with nitrogen, and putting into a quartz tube for deposition treatment; the degree of vacuum of the quartz tube was 10-2Pa, heating to 300 ℃ and maintaining for 10 minutes to remove water vapor on the surface of the silicon wafer;
（2）MoS2preparing a film: heating a quartz tube to 500-600 ℃, using argon as carrying gas, and introducing MoS using dilute sulfuric acid as a solvent2Solution in said MoS2Adding Al (NO) to the solution3)3Solution of Al (NO)3)3As Al dopant pair MoS2P-type doping by mass ratio, MoS2 ：Al(NO3)3Is 1: 20-1: 50; gas carrying MoS2And Al (NO)3)3Into a quartz tubenAfter the-Si (111) sheet is adsorbed, nucleated and grown for 5-10 minutes, heating the quartz tube to 950 ℃ for annealing for 20-40 minutes to obtain MoS2a/Si pn junction;
(3) maintaining the temperature of the quartz tube at 950 ℃, decomposing methane into carbon atoms and hydrogen, and allowing the carbon atoms to reach the formed MoS under the action of gas phase transport with the flow of argon of 10-30 sccm2MoS of/Si pn junction2The graphene film is characterized in that the graphene film is a hexagonal network structure, and is adsorbed to the surface, nucleates on the surface of the substrate after the migration of the surface of the substrate, attracts other carbon atoms through van der waals attraction force, and forms a hexagonal network structure with the bonded carbon atoms;
(4) to pairnEvaporating an aluminum electrode on the lower surface of the Si (111) sheet to form a cathode of the solar cell, thereby obtaining the graphene/MoS2a/Si heterojunction solar cell.
2. graphene/MoS prepared according to claim 12A/Si heterojunction thin-film solar cell.
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