CN102280590B - Solar cell by virtue of taking colloid quantum dots and graphene as light anode and manufacturing method thereof - Google Patents
Solar cell by virtue of taking colloid quantum dots and graphene as light anode and manufacturing method thereof Download PDFInfo
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- CN102280590B CN102280590B CN 201110237982 CN201110237982A CN102280590B CN 102280590 B CN102280590 B CN 102280590B CN 201110237982 CN201110237982 CN 201110237982 CN 201110237982 A CN201110237982 A CN 201110237982A CN 102280590 B CN102280590 B CN 102280590B
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Abstract
The invention relates to a solar cell by virtue of taking colloid quantum dots and graphene as a light anode and a manufacturing method thereof and belongs to the field of photoelectric conversion, new energy materials and technologies. In the manufacturing method, ITO (indium tin oxide) is taken as a framework, and the graphene and the colloid quantum dots with the different grain sizes are deposited on the framework in sequence layer by layer to form a {graphene/quantum dots} laminated film which is taken as the light anode; mixtures of organic polymers are deposited on the light anode in a film spinning mode; and finally vacuum evaporation is carried out on an electrode on the organic polymer film to finish the manufacturing of a solar cell device. The solar cell is simple and low in structure and manufacturing and can absorb the most of light energy of incident sunlight. The light anode is provided with the graphene film with high carrier mobility, thus greatly improving the extraction of photon-generated carriers to the electrode and the transmission process, thereby improving the photoelectric conversion efficiency of the solar cell.
Description
Technical field
The present invention relates to a kind of is solar cell of light anode and preparation method thereof based on Colloidal Quantum Dots and Graphene, belongs to opto-electronic conversion, new energy materials and technical field.
Background technology
At present; the mankind are being faced with that environment constantly worsens and the energy short serious problems day by day; strengthen environmental protection and exploitation clean energy resource are the focuses that national governments show great attention to, and the research of the development and utilization of solar energy is received people's fervent concern always, and its progress is also very rapid.The photovoltaic device that sunlight is converted to electric energy is a promising technology, can obtain a large amount of electric energy.In present photovoltaic device market, based on silicon sheet (monocrystalline and polycrystalline) solar cell and based on amorphous silicon, CdTe, CuInGaSe
2With III-V family semi-conductive thin film solar cell in occupation of main share.Yet the energy conversion efficiency of these photovoltaic devices is expensive far below its theoretical prediction value and its preparation cost.Although people have adopted the whole bag of tricks to make the conversion efficiency of solar cell obtain certain improvement, but it is increased substantially, find a kind of more effective approach or countermeasure, make the actual energy conversion efficiency of solar cell near its theoretical prediction value, become key subjects of Material Physics, photovoltaic device and energy science.
The energy range of solar spectrum is between 0.5～3.5eV, but main energy only concentrates on 1.8eV (near～700nm) the near infrared region.For this reason, it is particularly important how effectively utilizing the energy of this wave band.In fact, concerning present solar cell on the market, there is quite a few solar spectrum (the particularly spectrum of 600～1100nm wave band) to be absorbed seldom! The thickness of the solar cell of Here it is common based single crystal silicon chip is generally the reason of 180～300 μ m.But high efficiency solar cell requires its minority carrierdiffusion length times over the thickness of material, so that all photo-generated carriers can both be collected into, this requirement is easy to satisfy for hull cell.The opposed requirement of optical absorption length and Carrier collection length, the structural design and the material that impel us must consider solar cell carefully are selected.
We know, because quantum confined effect, semiconductor-quantum-point (or nano particle) has wide absorption spectrum, narrow transmitted bandwidth and large absorption cross-section.The quantum size effect of quantum dot is so that people can obtain according to the quantum dot that synthesizes different size the quantum dot of different energy gaps and light emitting region.And these quantum dots have been opened up a kind of method of utilizing hot electron or utilizing single photon generation multi-photon.For example, the many excitons in the PbSe quantum dot that it has been found that and the PbS quantum dot produce (Multiple excitongeneration, MEG) phenomenon, and it can greatly increase power conversion efficiency.Adding Graphene itself has very high carrier mobility and (can reach 10
4Cm
2/ Vs), therefore, we can " intersperse quantum dot " on graphene film, and the laminated film that obtains like this can improve the generation efficiency of electron-hole pair, also can improve charge carrier to the transmission course of two end electrodes, provide possibility for obtaining efficient solar battery.Method by electrophoretic deposition just can be with the aqueous solution of electronation Graphene at ito glass preparation Graphene thin layer, and and then the CdS quantum dot is prepared on the graphene layer as the light anode.Reported with Na in the document
2S is the solar cell of electrolyte, and its photoelectric conversion efficiency IPCE=16% and its optical responsivity are 1.08mA/cm
2(at 100mW/cm
2Under the illumination condition)----this is the best result in relevant carbon/quantum dot (Carbon/QD) solar cell of so far bibliographical information! And also the someone has reported with semiconductor-quantum-point (TiO
2And ZnO) and metallic nano crystal (Au and Pt) " interspersing " to the method for carbon nano-tube and Graphene, confirm that Graphene can be used as a two-dimentional carrier that disperses semiconductor-quantum-point and metallic nano crystal fully.Therefore, the graphene film that we just can " intersperse " with metallic nano crystal and semiconductor-quantum-point as the light anode and with high conductive SOLID ORGANIC thin-film material (or polymer) as active layer, will obtain a kind of Novel photovoltaic device of high-photoelectric transformation efficiency.
In addition, organic polymer itself has relatively large exciton bind energy and the higher characteristics such as electron mobility.Therefore with semiconductor nano and organic (polymer) Material cladding and to prepare organic-inorganic compounding photoconductive device be one of focus of present application study.This photoconductive device is the device that makes up the donor-acceptor heterojunction, at the interface requirement at bi-material exists because the electrostatic force that the difference of electron affinity energy and ionization energy forms, this just requires the electron affinity of polymer molecule and ionization energy ratio nano crystalline substance to want large, so just can form internal electric field, thereby order about separation of charge.If potential energy difference is greater than exciton bind energy, these local internal electric fields can be very strong and make the photoproduction exciton fission.Because P3HT and PCBM generally are applied in the solar cell, have good carrier transmission performance and higher light transfer characteristic.Therefore, we also select the mixture of P3HT and PCBM to be used as active layer, the main luminous energy that absorbs visible light wave range in the solar spectrum, add based on the absorption near infrared spectrum of the light anode of Colloidal Quantum Dots and Graphene, thereby make the absorption spectrum of whole device expand to infrared band from visible light.Therefore, the photoelectric conversion efficiency of solar cell correspondingly can increase a lot.
Summary of the invention
The objective of the invention is in order to provide a kind of is solar cell of light anode and preparation method thereof based on Colloidal Quantum Dots and Graphene.Namely utilize the PbS Colloidal Quantum Dots of different-grain diameter " to intersperse " to graphene film, make the light anode of multi-layer quantum point laminated construction, and further the mixture of organic polymer is made film on this basis, so, the absorption spectrum of the whole device that obtains will be extended to infrared band by visible light wave range, strengthen the absorption of solar cell device to solar energy, and then improved the photoelectric conversion efficiency of solar cell.
The objective of the invention is to be achieved through the following technical solutions.
Of the present invention a kind of be the solar cell of light anode based on Colloidal Quantum Dots and Graphene, comprise light anode, organic polymer active layer and electrode based on Colloidal Quantum Dots and Graphene; Wherein the light anode based on Colloidal Quantum Dots and Graphene is take ito glass as skeleton, and the Colloidal Quantum Dots of different-grain diameter is formed { Graphene/quantum dot } film as the light anode with the method for electrophoresis with Graphene and quantum dot successively layer by layer deposition; Wherein the organic polymer active layer refers to the mixture of electric transmission polymeric material and hole transport polymer material, and then the mixture of this organic polymer deposited on the light anode by the mode of getting rid of film, last again on this thin polymer film the vacuum evaporation metal electrode finish the preparation of solar cell device;
Above-mentioned Colloidal Quantum Dots be absworption peak at the low-gap semiconductor material of infrared band (wavelength is greater than 800nm), be preferably PbS or PbSe;
Above-mentioned organic polymer active layer is preferably the mixture of P3HT or MEH-PPV and PCBM.Wherein poly--3 hexyl thiophenes (P3HT) are poly (3-hexylthiophene), poly-(2-methoxyl group-5-(2-ethyl hexyl oxy)-1,4-phenylene ethylene) (MEH-PPV) be Poly[2-methoxy-5-(2-ethylhexyloxy)-1,4-phenylenevinylene], (6,6)-phenyl-C61 methyl butyrate (PCBM) is [6,6]-Phenyl C
61Butyric acid methyl ester;
Above-mentioned electrode is that work function is less than or equal to metal electrode, multilayer metallic electrode or the metal alloy electrodes of 4.3eV; Metal electrode is preferably the aluminium electrode, and multilayer metallic electrode is preferably Ca/Al, and metal alloy electrodes is preferably the Mg/Ag alloy;
Can also comprise one deck hole transmission layer and one deck electron transfer layer in the above-mentioned solar battery structure.Usually, add one deck hole transmission layer between based on the light anode of Colloidal Quantum Dots and Graphene and organic polymer active layer, electron transfer layer is added between organic polymer active layer and the electrode.
Of the present invention a kind of be the preparation method of the solar cell of light anode based on Colloidal Quantum Dots and Graphene, concrete steps are:
1) method by electrophoresis prepares first one deck graphene film on the ito glass surface, then prepares one deck Colloidal Quantum Dots film at graphene film again with the method for getting rid of film;
2) according to step 1) method again prepare one or more layers graphene film and Colloidal Quantum Dots film; The light anode based on Colloidal Quantum Dots and Graphene of different near infrared bands is absorbed;
3) in step 2) be prepared with the organic polymer active layer by the mode of getting rid of film on the light anode that obtains, at last under vacuum condition on the organic polymer active layer electrode evaporation, obtaining based on Colloidal Quantum Dots and Graphene is the solar cell of light anode.
Step 1) with step 2) in the quantum point grain diameter of Colloidal Quantum Dots film of preparation be different; In addition, can also add respectively one deck electron transfer layer and hole transmission layer in the both sides of organic polymer active layer.Can further improve like this photoelectric properties of solar cell.
This based on behind the absorption of the Colloidal Quantum Dots in the light anode of Colloidal Quantum Dots and the Graphene photon, the photo-generated carrier that disassociation produces is easy to be transferred on the Graphene by Colloidal Quantum Dots, transport by the graphene film with high carrier mobility again, so just realize the quick extraction of photo-generated carrier to electrode, can improve the photoelectric conversion efficiency of device.
With after PCBM mixes, the absorption spectrum of its mixed solution is the linear superposition of the absorption spectrum of single component material, can cover most of visible light wave range with P3HT.Add this PbS Colloidal Quantum Dots based on different-grain diameter in the light anode of Colloidal Quantum Dots and Graphene to after the infrared Optical Absorption, the absorption spectrum of whole device expands to infrared band by whole visible light wave range.Therefore, this is that the solar cell of light anode significantly strengthens the absorbability of solar energy based on Colloidal Quantum Dots and Graphene, and photoelectric conversion efficiency significantly improves.
Beneficial effect
Solar battery structure of the present invention prepares simple, cheap; Can absorb most luminous energy of incident sunlight, the adding with graphene film of high carrier mobility has greatly improved extraction and the transport process of photo-generated carrier to electrode, thereby can increase the photoelectric conversion efficiency of solar cell; The PbS Colloidal Quantum Dots " is interspersed " to graphene film, strengthens the interaction between them, is conducive to the effective separation of charge carrier, improves photo-generated carrier density; The use of PCBM and P3HT mixture can form good inierpeneirating network structure, and also fast transport is to Graphene or electrode so that the photoproduction exciton separates effectively, and recombination probability reduces greatly, improves energy conversion efficiency.
Description of drawings
Fig. 1 is the light anode construction schematic diagram based on Colloidal Quantum Dots and Graphene that can absorb near infrared band in the solar spectrum of embodiment 1 preparation;
Fig. 2 is that particle diameter is the abosrption spectrogram of PbS quantum dot solution, MEH-PPV solution and the PCBM solution of 3.9nm;
Fig. 3 is that particle diameter is the abosrption spectrogram of mixed solution of PbS solution, MEH-PPV solution and the PCBM solution of 3.9nm;
Fig. 4 is the structural representation of the whole solar cell of embodiment 1 preparation;
Fig. 5 is the structural representation of the whole solar cell of embodiment 2 preparations.
Embodiment
The present invention will be further described below in conjunction with drawings and Examples.
A kind of is the solar cell of light anode based on Colloidal Quantum Dots and Graphene, comprises light anode, organic polymer active layer and electrode based on Colloidal Quantum Dots and Graphene;
Above-mentioned Colloidal Quantum Dots is low energy gap Colloidal Quantum Dots PbS;
Above-mentioned organic polymer active layer is the mixture of P3HT and PCBM, and wherein the mass ratio of P3HT and PCBM is 1: 1; P3HT, PCBM have good energy level coupling, are conducive to the collection of electric charge;
Above-mentioned electrode is the aluminium electrode, and aluminium is stable in the air; Its work function is 4.28eV.
A kind of is the preparation method of the solar cell of light anode based on Colloidal Quantum Dots and Graphene, and concrete steps are:
1) at first uses repeatedly wiping ito glass of absorbent cotton and washing agent, and rinse well with deionized water, and then used respectively deionized water, acetone and isopropyl alcohol each ultrasonic 15 minutes, after whenever carrying out, all with nitrogen ito glass is dried up before a ultrasonic cleaning, after ultrasonic cleaning is complete ito glass is put into the ozone treatment machine and carried out ozone treatment 15 minutes, after cooling with for subsequent use; Ito surface (4cm with the ito glass that obtains
2) and gauze platinum electrode (5cm
2) to form spacing be the parallel-plate electrode of 3mm, be positioned in the electrophoretic deposition pond.In being the graphene aqueous solution of 0.2mg/mL, concentration remains on 0.5mA/cm
2Electrophoretic deposition graphene film under the current density can obtain the graphene film layer that thickness is 30nm through behind the 75s.Then the method by getting rid of film is at graphene film surface spin coating one deck Colloidal Quantum Dots thin layer, like this, just obtained the graphene film that one deck point is embroidered with Colloidal Quantum Dots.Wherein transmitance is greater than 85% in visible light and near-ultraviolet range for ito glass, and its square resistance is 10 Ω/;
2) according to step 1) method, prepare the graphene film that six layers of point are embroidered with the Colloidal Quantum Dots of other particle diameter, form laminated construction.Prepare one deck point at every turn and be embroidered with after the graphene film of Colloidal Quantum Dots, all will carry out drying.The light anode based on Colloidal Quantum Dots and Graphene of different infrared bands is absorbed; As shown in Figure 1, each layer point is embroidered with the Graphene laminated construction schematic diagram of different-grain diameter Colloidal Quantum Dots.The Graphene of different colours represents that with quantum dot the quantum point grain diameter size on this graphene layer is different, and it is representing the light (from top to bottom, corresponding optical wavelength is elongated gradually) that can absorb different wave length (color) separately;
3) in step 2) prepare the mixture film of one layer of polymeric P3HT and PCBM on the light anode that obtains by the mode of getting rid of film, its thickness is 100nm.At last on the organic polymer active layer 4 * 10
-3The aluminium electrode that evaporation 150nm is thick under the vacuum condition of Pa, namely obtaining based on Colloidal Quantum Dots and Graphene is the solar cell of light anode, as shown in Figure 4.
Remove outside the absorption spectrum of organic polymer active layer in visible-range step 1) and step 2) in the corresponding absorption spectrum of different-grain diameter quantum dot of Colloidal Quantum Dots film of preparation and the near infrared spectrum in the solar spectrum be complementary.
A kind of is the solar cell of light anode based on Colloidal Quantum Dots and Graphene, comprises light anode, PEDOT:PSS hole transmission layer, organic polymer active layer, PCBM electron transfer layer and electrode based on Colloidal Quantum Dots and Graphene;
Above-mentioned Colloidal Quantum Dots is low energy gap Colloidal Quantum Dots PbS;
Above-mentioned organic polymer active layer is the mixture of P3HT and PCBM, and wherein the mass ratio of P3HT and PCBM is 1: 1; P3HT, PCBM have good energy level coupling, are conducive to the collection of electric charge;
Above-mentioned electrode is the aluminium electrode; Its work function is 4.28eV.
A kind of is the preparation method of the solar cell of light anode based on Colloidal Quantum Dots and Graphene, and concrete steps are:
1) at first uses repeatedly wiping ito glass of absorbent cotton and washing agent, and rinse well with deionized water, and then used respectively deionized water, acetone and isopropyl alcohol each ultrasonic 15 minutes, after whenever carrying out, all with nitrogen ito glass is dried up before a ultrasonic cleaning, after ultrasonic cleaning is complete ito glass is put into the ozone treatment machine and carried out ozone treatment 15 minutes, after cooling with for subsequent use; Ito surface (4cm with the ito glass that obtains
2) and gauze platinum electrode (5cm
2) to form spacing be the parallel-plate electrode of 3mm, be positioned in the electrophoretic deposition pond.In being the graphene aqueous solution of 0.2mg/mL, concentration remains on 0.5mA/cm
2Electrophoretic deposition graphene film under the current density can obtain the graphene film layer that thickness is 30nm through behind the 75s.Then the method by getting rid of film is at graphene film surface spin coating one deck Colloidal Quantum Dots thin layer, like this, just obtained the graphene film that one deck point is embroidered with Colloidal Quantum Dots.Wherein transmitance is greater than 85% in visible light and near-ultraviolet range for ito glass, and its square resistance is 10 Ω/;
2) according to step 1) method, prepare the graphene film that six layers of point are embroidered with the Colloidal Quantum Dots of other particle diameter, form laminated construction.Prepare one deck point at every turn and be embroidered with after the graphene film of Colloidal Quantum Dots, all will carry out drying.The light anode based on Colloidal Quantum Dots and Graphene of different infrared bands is absorbed;
3) in step 2) prepare first the thick PEDOT:PSS hole transmission layer of one deck 40nm by the mode of getting rid of film on the light anode that obtains, then prepare the mixture film of one layer of polymeric P3HT and PCBM thereon, its thickness is 100nm.Then evaporation prepares the thick PCBM electron transfer layer of one deck 30nm on the organic polymer active layer; At last on electron transfer layer, 4 * 10
-3The aluminium electrode that evaporation 150nm is thick under the vacuum condition of Pa, namely obtaining based on Colloidal Quantum Dots and Graphene is the solar cell of light anode, as shown in Figure 5.
Remove outside the absorption spectrum of organic polymer active layer in visible-range step 1) and step 2) in the corresponding absorption spectrum of different-grain diameter quantum dot of Colloidal Quantum Dots film of preparation and the near infrared spectrum in the solar spectrum be complementary.
Comparative Examples 1
A kind of based on Colloidal Quantum Dots and Graphene be the solar cell and preparation method thereof of light anode with embodiment 1, the difference is that with MEH-PPV to replace P3HT that obtaining at last based on Colloidal Quantum Dots and Graphene is the efficient solar battery of light anode.
Comparative Examples 2
A kind of based on Colloidal Quantum Dots and Graphene be the solar cell and preparation method thereof of light anode with embodiment 2, the difference is that with MEH-PPV to replace P3HT that obtaining at last based on Colloidal Quantum Dots and Graphene is the efficient solar battery of light anode.
Comparative Examples 3
A kind of is that the solar cell and preparation method thereof of light anode is with embodiment 2 based on Colloidal Quantum Dots and Graphene, the difference is that with P3HT to replace PEDOT:PSS as hole transmission layer, making at last based on Colloidal Quantum Dots and Graphene is the efficient solar battery of light anode.
Comparative Examples 4
A kind of based on Colloidal Quantum Dots and Graphene be the solar cell and preparation method thereof of light anode with embodiment 2, the difference is that with C
60Replace PCBM as electron transfer layer, making at last based on Colloidal Quantum Dots and Graphene is the efficient solar battery of light anode.
PbS Colloidal Quantum Dots in above-described embodiment 1, embodiment 2, Comparative Examples 1, Comparative Examples 2, Comparative Examples 3 and the Comparative Examples 4 can replace with the PbSe Colloidal Quantum Dots, and making at last based on Colloidal Quantum Dots and Graphene is the solar cell of light anode.
Above-mentioned PEDOT:PSS is made of PEDOT and two kinds of materials of PSS, and PEDOT is the polymer of EDOT (3,4-ethylene dioxythiophene monomer), and PSS is poly styrene sulfonate, and the mass ratio of PEDOT and PSS is 1: 2.5.
Particle diameter be 3.9nm PbS solution, MEH-PPV solution and PCBM solution abosrption spectrogram as shown in Figure 2.Fig. 3 is that particle diameter is the absorption spectrum of mixed solution of PbS solution, MEH-PPV solution and the PCBM solution of 3.9nm among Fig. 2, and as seen, the absorption spectrum of this mixed solution is the linear superposition of the absorption spectrum of this PbS solution, MEH-PPV solution and PCBM solution.As a same reason, the absorption spectrum of the mixed solution of PbS Colloidal Quantum Dots solution, P3HT solution and PCBM solution also is the linear superposition of the absorption spectrum of PbS Colloidal Quantum Dots solution, P3HT solution and PCBM solution.
As can be known, this based on this mixed solution be organic polymer active layer preparation be that the efficient solar battery of light anode can absorb visible light wave range and infrared band based on Colloidal Quantum Dots and Graphene, its photoelectric conversion efficiency obviously improves.
Claims (7)
1. one kind is the solar cell of light anode based on Colloidal Quantum Dots and Graphene, it is characterized in that: comprise light anode, organic polymer active layer and electrode based on Colloidal Quantum Dots and Graphene;
Colloidal Quantum Dots is that absworption peak is at the low-gap semiconductor material of infrared band wavelength greater than 800nm;
The organic polymer active layer is the mixture of P3HT and PCBM or the mixture of MEH-PPV and PCBM; Wherein poly--3 hexyl thiophenes (P3HT) are poly (3-hexylthiophene), poly-(2-methoxyl group-5-(2-ethyl hexyl oxy)-1,4-phenylene ethylene) (MEH-PPV) be Poly[2-methoxy-5-(2-ethylhexyloxy)-1,4-phenylenevinylene], (6,6)-phenyl-C61 methyl butyrate (PCBM) is [6,6]-Phenyl C
61Butyric acid methyl ester;
Electrode is that work function is less than or equal to the metal electrode of 4.3eV.
According to claim 1 a kind of be the solar cell of light anode based on Colloidal Quantum Dots and Graphene, it is characterized in that: Colloidal Quantum Dots is PbS or PbSe.
According to claim 1 a kind of be the solar cell of light anode based on Colloidal Quantum Dots and Graphene, it is characterized in that: metal electrode is the aluminium electrode.
According to claim 1 a kind of be the solar cell of light anode based on Colloidal Quantum Dots and Graphene, it is characterized in that: metal electrode is multilayer metallic electrode or metal alloy electrodes.
According to claim 4 a kind of be the solar cell of light anode based on Colloidal Quantum Dots and Graphene, it is characterized in that: multilayer metallic electrode is Ca layer and Al layer.
According to claim 4 a kind of be the solar cell of light anode based on Colloidal Quantum Dots and Graphene, it is characterized in that: metal alloy electrodes is Mg and Ag alloy.
According to claim 1 a kind of be the solar cell of light anode based on Colloidal Quantum Dots and Graphene, it is characterized in that: between based on the light anode of Colloidal Quantum Dots and Graphene and organic polymer active layer, add one deck hole transmission layer, and between organic polymer active layer and electrode, add one deck electron transfer layer.
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