CN109560201B - Metal transparent electrode, preparation method thereof and organic solar cell formed by metal transparent electrode - Google Patents
Metal transparent electrode, preparation method thereof and organic solar cell formed by metal transparent electrode Download PDFInfo
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Abstract
The invention discloses a metal transparent electrode, a preparation method thereof and an organic solar cell formed by the metal transparent electrode. The metal transparent electrode comprises a seed crystal layer, a molecular self-assembly layer and a conducting layer, wherein the conducting layer is a composite film of an Ag film and cluster Ag, and the thickness of the conducting layer is 1-20 nm; and a cathode buffer layer, an active layer, an anode buffer layer and a back electrode are sequentially arranged on the metal transparent electrode to form the organic solar cell. The metal transparent electrode not only has better conductivity and flexibility, but also can adjust the optical field distribution in the device by utilizing the optical microcavity effect generated by the Ag film and the plasma enhancement effect (or scattering effect) generated by the cluster Ag, improve the absorption and utilization rate of the device to sunlight and prepare a high-performance flexible organic solar cell device.
Description
Technical Field
The invention relates to the field of solar cells, in particular to a metal transparent electrode, a preparation method thereof and an organic solar cell.
Technical Field
Indium Tin Oxide (ITO) is a transparent electrode material widely used in organic solar cells at present due to its good conductivity and high transmittance. However, ITO also has some disadvantages, such as the rising price of indium, which is the raw material, and the rising preparation cost; in addition, the flexibility of the ITO is poor, the conductivity is greatly reduced after the ITO is bent, and the preparation of a high-performance flexible solar cell device is not facilitated. Therefore, the development of a novel transparent electrode material that can replace ITO is a very important research topic. Scientists have developed conductive polymers, carbon nanotubes, graphene films, metal nanowires, ultra-thin metal films, and other materials as transparent electrodes. Compared with other materials, the metal thin film has the characteristics of high conductivity, high stability, good ductility and the like, so that the metal thin film is the most promising material for replacing ITO.
Disclosure of Invention
The invention aims to overcome the defects of the prior art and provides a metal transparent electrode, a preparation method thereof and an organic solar cell formed by the metal transparent electrode.
The technical scheme of the invention is as follows:
a metal transparent electrode:
the self-assembly type solar cell comprises a seed crystal layer, a molecular self-assembly layer and a conducting layer from bottom to top in sequence, wherein the conducting layer is a composite film of an Ag thin film and cluster Ag, and the thickness of the conducting layer is 1-20 nm.
The molecular self-assembly layer is a composite film of 11-mercaptoundecanoic acid and acetonitrile terephthalate, and the weight ratio of the 11-mercaptoundecanoic acid to the acetonitrile terephthalate is 1-1000: 1, the thickness of the molecular self-assembly layer is 1-5 nm.
The seed crystal layer is a ZnO film with the thickness of 10-100 nm.
Secondly, a preparation method of the metal transparent electrode, which comprises the following steps:
carrying out ultrasonic cleaning on the glass substrate by using a detergent, isopropanol, ethanol and acetone in sequence, and drying by using nitrogen after cleaning; preparing a ZnO seed crystal layer with the thickness of 10-100nm on the surface of the glass substrate by a spin coating method, and annealing the formed film, wherein the annealing temperature is 200 ℃, and the annealing time is 2 hours; then spin-coating a self-assembled layer of 11-mercaptoundecanoic acid and acetonitrile terephthalate molecules on the ZnO seed crystal layer, wherein the weight ratio of the 11-mercaptoundecanoic acid to the acetonitrile terephthalate is 1-1000: 1; depositing Ag with the thickness of 1-20nm as a conductive layer by a vacuum thermal evaporation method to form a metal transparent electrode.
Thirdly, an organic solar cell composed of a metal transparent electrode:
the light-emitting diode comprises a substrate, a metal transparent electrode, a cathode buffer layer, a light activity layer, an anode buffer layer and a back electrode in sequence from bottom to top, wherein the metal transparent electrode comprises a seed crystal layer, a molecule self-assembly layer and a conducting layer, the conducting layer is a composite film of an Ag film and a cluster Ag, and the thickness of the conducting layer is 1-20 nm.
The molecular self-assembly layer is a composite film of 11-mercaptoundecanoic acid and acetonitrile terephthalate, and the weight ratio of the 11-mercaptoundecanoic acid to the acetonitrile terephthalate is (1-1000): 1, the thickness of the molecular self-assembly layer is 1-5 nm.
The seed crystal layer is a ZnO film with the thickness of 10-100 nm.
The substrate material is glass or a polyester film; the cathode buffer layer is made of ZnO; the photoactive layer is PTB7-Th and PC 71 Mixed film of BM; the anode buffer layer is made of MoO 3 (ii) a The back electrode material is Ag.
Advantageous effects
The metallic transparent electrode designed by the invention can control the growth process of Ag through the seed crystal layer and the molecular self-assembly layer. Because the terminal functional groups of the two molecular self-assembly materials of the 11-mercapto undecanoic acid and the acetonitrile terephthalate are different, the 11-mercapto undecanoic acid can form a continuous and smooth Ag film, and the acetonitrile benzoate forms a cluster Ag, so that an Ag film/cluster Ag composite conducting layer can be formed on the ZnO seed crystal layer. Compared with the traditional ITO electrode, the metal transparent electrode not only has better conductivity and flexibility, but also can adjust the optical field distribution in the device by utilizing the optical microcavity effect generated by the Ag film and the plasma enhancement effect (or scattering effect) generated by the cluster Ag, improve the utilization rate of light and prepare a high-performance flexible organic solar cell device.
Drawings
Fig. 1 is a schematic structural diagram of an organic solar cell device according to the present invention.
FIG. 2 is an I-V curve diagram of an organic solar cell device of example 7 of the present invention.
Detailed Description
The present invention will be described in further detail with reference to specific examples.
As shown in figure 1, the metal transparent electrode comprises a seed crystal layer, a molecular self-assembly layer and a conductive layer, wherein the conductive layer is a composite film of an Ag thin film and cluster Ag, and the thickness of the conductive layer is 1-20 nm.
The preferable molecular self-assembly layer is a composite film of 11-mercaptoundecanoic acid and acetonitrile terephthalate, and the weight ratio of the 11-mercaptoundecanoic acid to the acetonitrile terephthalate is 1-1000: 1, the thickness of the molecular self-assembly layer is 1-5 nm.
The seed crystal layer is preferably ZnO film with thickness of 10-100 nm.
The organic solar cell comprises a substrate, a metal transparent electrode, a cathode buffer layer, a photoactive layer, an anode buffer layer and a back electrode, wherein the metal transparent electrode comprises a seed crystal layer, a molecular self-assembly layer and a conducting layer, the conducting layer is a composite film of an Ag thin film and cluster Ag, and the thickness of the conducting layer is 1-20 nm.
The preferable molecular self-assembly layer is a composite film of 11-mercaptoundecanoic acid and acetonitrile terephthalate, and the weight ratio of the 11-mercaptoundecanoic acid to the acetonitrile terephthalate is 1: 1-1000: 1, the thickness of the molecular self-assembly layer is 1-5 nm.
The seed crystal layer is preferably ZnO film with thickness of 10-100 nm.
The preferred substrate material is glass or mylar; the preferable cathode buffer layer material is ZnO; preferred photoactive layers are PTB7-Th and PC 71 A mixed film of BM; the preferred anode buffer layer material is MoO 3 (ii) a The preferred back electrode material is Ag.
The metal transparent electrode is applied to an organic solar cell. The structure comprises a seed crystal layer, a molecular self-assembly layer and a conducting layer, wherein the conducting layer is a composite film of an Ag film and cluster Ag. The invention can control the growth process of Ag through the seed crystal layer and the molecular self-assembly layer, change the appearance of Ag and form an Ag film and cluster Ag composite film. The continuous and flat Ag film can ensure that the transparent electrode has better conductivity and forms an optical resonance microcavity effect, and the plasma effect (or scattering effect) generated by the cluster Ag can effectively change the distribution of an optical field in the device, increase the absorption and utilization rate of the active layer to light, and achieve the purpose of improving the short-circuit current density of the device.
The examples of the invention are as follows:
example 1:
carrying out ultrasonic cleaning on the glass substrate by using a detergent, isopropanol, ethanol and acetone in sequence, and drying by using nitrogen after cleaning; preparing a ZnO seed crystal layer with the thickness of 10nm on the surface of the glass substrate by a spin coating method, and annealing the formed film, wherein the annealing temperature is 200 ℃, and the annealing time is 2 hours; then spin-coating a self-assembled layer of 11-mercaptoundecanoic acid and acetonitrile terephthalate on the surface, wherein the weight ratio of the 11-mercaptoundecanoic acid to the acetonitrile terephthalate is 10: 1; a metal transparent electrode was formed by depositing Ag of 10nm as a conductive layer by a vacuum thermal evaporation method.
Spin coating a ZnO cathode buffer layer with the thickness of 30 nm; followed by spin coating of 90nm PTB 7-Th: PC (personal computer) 71 A BM active layer; finally, 8nm of MoO is deposited 3 (anode buffer layer) and 100nm Ag (back electrode) to obtain an organic solar cell as shown in fig. 1, whose photoelectric conversion efficiency was 7.3%.
Example 2:
carrying out ultrasonic cleaning on the glass substrate by using a detergent, isopropanol, ethanol and acetone in sequence, and drying by using nitrogen after cleaning; preparing a 40nm ZnO seed crystal layer on the surface of the glass substrate by a spin coating method, and annealing the formed film, wherein the annealing temperature is 200 ℃, and the annealing time is 2 hours; then spin-coating a self-assembled layer of 11-mercaptoundecanoic acid and acetonitrile terephthalate molecules on the surface, wherein the weight ratio of the 11-mercaptoundecanoic acid to the acetonitrile terephthalate is 10: 1; a metal transparent electrode was formed by depositing Ag of 10nm as a conductive layer by a vacuum thermal evaporation method.
Spin coating a ZnO cathode buffer layer with the thickness of 30 nm; followed by spin coating of 90nm PTB 7-Th: PC (personal computer) 71 A BM active layer; finally, 8nm of MoO is deposited 3 (anode buffer layer) and 100nm Ag (back electrode) to obtain an organic solar cell as shown in fig. 1, whose photoelectric conversion efficiency was 8.3%.
Example 3:
carrying out ultrasonic cleaning on the glass substrate by using a detergent, isopropanol, ethanol and acetone in sequence, and drying by using nitrogen after cleaning; preparing a 100nm ZnO seed crystal layer on the surface of the glass substrate by a spin coating method, and annealing the formed film, wherein the annealing temperature is 200 ℃, and the annealing time is 2 hours; then spin-coating a self-assembled layer of 11-mercaptoundecanoic acid and acetonitrile terephthalate molecules on the surface, wherein the weight ratio of the 11-mercaptoundecanoic acid to the acetonitrile terephthalate is 10: 1; a metal transparent electrode was formed by depositing Ag of 10nm as a conductive layer by a vacuum thermal evaporation method.
Spin-coating a 30nm ZnO cathode buffer layer; followed by spin coating of 90nm PTB 7-Th: PC (personal computer) 71 A BM active layer; final deposition of 8nMoO of m 3 (anode buffer layer) and 100nm Ag (back electrode) to obtain an organic solar cell as shown in fig. 1, whose photoelectric conversion efficiency was 7.5%.
Example 4:
carrying out ultrasonic cleaning on the glass substrate by using a detergent, isopropanol, ethanol and acetone in sequence, and drying by using nitrogen after cleaning; preparing a 40nm ZnO seed crystal layer on the surface of the glass substrate by a spin coating method, and annealing the formed film, wherein the annealing temperature is 200 ℃, and the annealing time is 2 hours; and then spin-coating a self-assembled layer of 11-mercaptoundecanoic acid and acetonitrile terephthalate molecules on the surface, wherein the weight ratio of the 11-mercaptoundecanoic acid to the acetonitrile terephthalate is 1: 1; a metal transparent electrode was formed by depositing Ag of 10nm as a conductive layer by a vacuum thermal evaporation method.
Spin coating a ZnO cathode buffer layer with the thickness of 30 nm; followed by spin coating of 90nm PTB 7-Th: PC (personal computer) 71 A BM active layer; finally, 8nm of MoO is deposited 3 (anode buffer layer) and 100nm Ag (back electrode) to obtain an organic solar cell as shown in fig. 1, whose photoelectric conversion efficiency was 6.8%.
Example 5:
carrying out ultrasonic cleaning on the glass substrate by using a detergent, isopropanol, ethanol and acetone in sequence, and drying by using nitrogen after cleaning; preparing a 40nm ZnO seed crystal layer on the surface of the glass substrate by a spin coating method, and annealing the formed film, wherein the annealing temperature is 200 ℃, and the annealing time is 2 hours; then spin-coating a self-assembled layer of 11-mercaptoundecanoic acid and acetonitrile terephthalate molecules on the surface, wherein the weight ratio of the 11-mercaptoundecanoic acid to the acetonitrile terephthalate is 100: 1; a metal transparent electrode was formed by depositing Ag of 10nm as a conductive layer by a vacuum thermal evaporation method.
Spin coating a ZnO cathode buffer layer with the thickness of 30 nm; followed by spin coating of 90nm PTB 7-Th: PC (personal computer) 71 A BM active layer; finally, 8nm of MoO is deposited 3 (anode buffer layer) and 100nm Ag (back electrode) to obtain the organic solar cell shown in fig. 1, which has a photoelectric conversion efficiency of 8.2%.
Example 6:
sequentially carrying out ultrasonic cleaning on the glass substrate by using a detergent, isopropanol, ethanol and acetone, and drying by using nitrogen after cleaning; preparing a 40nm ZnO seed crystal layer on the surface of the glass substrate by a spin coating method, and annealing the formed film, wherein the annealing temperature is 200 ℃, and the annealing time is 2 hours; and then spin-coating a self-assembled layer of 11-mercaptoundecanoic acid and acetonitrile terephthalate molecules on the surface, wherein the weight ratio of the 11-mercaptoundecanoic acid to the acetonitrile terephthalate is 20: 1; a metal transparent electrode was formed by depositing 1nm Ag as a conductive layer by a vacuum thermal evaporation method.
Spin coating a ZnO cathode buffer layer with the thickness of 30 nm; followed by spin coating of 90nm PTB 7-Th: PC (personal computer) 71 A BM active layer; finally, 8nm of MoO is deposited 3 (anode buffer layer) and 100nm Ag (back electrode) to obtain an organic solar cell as shown in fig. 1, whose photoelectric conversion efficiency was 2.7%.
Example 7:
sequentially carrying out ultrasonic cleaning on the glass substrate by using a detergent, isopropanol, ethanol and acetone, and drying by using nitrogen after cleaning; preparing a 40nm ZnO seed crystal layer on the surface of the glass substrate by a spin coating method, and annealing the formed film, wherein the annealing temperature is 200 ℃, and the annealing time is 2 hours; and then spin-coating a self-assembled layer of 11-mercaptoundecanoic acid and acetonitrile terephthalate molecules on the surface, wherein the weight ratio of the 11-mercaptoundecanoic acid to the acetonitrile terephthalate is 20: 1; a metal transparent electrode was formed by depositing Ag of 10nm as a conductive layer by a vacuum thermal evaporation method.
Spin coating a ZnO cathode buffer layer with the thickness of 30 nm; followed by spin coating of 90nm PTB 7-Th: PC (personal computer) 71 A BM active layer; finally, 8nm of MoO is deposited 3 (anode buffer layer) and 100nm Ag (back electrode) to obtain the organic solar cell shown in figure 1, wherein the photoelectric conversion efficiency of the organic solar cell is 8.9%; fig. 2 is an I-V graph of the organic solar cell device of the present embodiment.
Example 8:
carrying out ultrasonic cleaning on the glass substrate by using a detergent, isopropanol, ethanol and acetone in sequence, and drying by using nitrogen after cleaning; preparing a ZnO seed crystal layer with the thickness of 10nm on the surface of the glass substrate by a spin coating method, and annealing the formed film, wherein the annealing temperature is 200 ℃, and the annealing time is 2 hours; and then spin-coating a self-assembled layer of 11-mercaptoundecanoic acid and acetonitrile terephthalate molecules on the surface, wherein the weight ratio of the 11-mercaptoundecanoic acid to the acetonitrile terephthalate is 20: 1; and depositing 20nm of Ag by a vacuum thermal evaporation method to form a metal transparent electrode.
Spin coating a ZnO cathode buffer layer with the thickness of 30 nm; followed by spin coating of 90nm PTB 7-Th: PC (personal computer) 71 A BM active layer; finally, 8nm of MoO is deposited 3 (anode buffer layer) and 100nm Ag (back electrode) to obtain an organic solar cell as shown in fig. 1, whose photoelectric conversion efficiency was 7.1%.
Example 9:
carrying out ultrasonic cleaning on the glass substrate by using a detergent, isopropanol, ethanol and acetone in sequence, and drying by using nitrogen after cleaning; preparing a 40nm ZnO seed crystal layer on the surface of the glass substrate by a spin coating method, and annealing the formed film, wherein the annealing temperature is 200 ℃, and the annealing time is 2 hours; then spin-coating a self-assembled layer of 11-mercaptoundecanoic acid and acetonitrile terephthalate on the surface, wherein the weight ratio of 11-mercaptoundecanoic acid to acetonitrile terephthalate is 1000: 1; a metal transparent electrode was formed by depositing Ag of 10nm as a conductive layer by a vacuum thermal evaporation method.
Spin-coating a 30nm ZnO cathode buffer layer; followed by spin coating of 90nm PTB 7-Th: PC (personal computer) 71 A BM active layer; finally, 8nm of MoO is deposited 3 (anode buffer layer) and 100nm Ag (back electrode) to obtain an organic solar cell as shown in fig. 1, whose photoelectric conversion efficiency was 8.6%.
The above examples of the present invention are merely illustrative of the present invention and are not intended to limit the embodiments of the present invention. It will be apparent to those skilled in the art that other variations and modifications may be made in the foregoing disclosure, and it is not intended to be exhaustive or to limit all embodiments to the precise form disclosed. All obvious changes and modifications of the present invention are within the scope of the present invention.
Claims (4)
1. A metal transparent electrode, characterized by: the self-assembly molecular seed crystal layer sequentially comprises a seed crystal layer, a molecular self-assembly layer and a conducting layer from bottom to top;
the conducting layer is a composite film of an Ag film and cluster Ag, and the thickness of the conducting layer is 1-20 nm;
the molecular self-assembly layer is a composite film of 11-mercaptoundecanoic acid and acetonitrile terephthalate, and the weight ratio of the 11-mercaptoundecanoic acid to the acetonitrile terephthalate is (1-1000): 1, the thickness of the molecular self-assembly layer is 1-5 nm;
the seed crystal layer is a ZnO film with the thickness of 10-100 nm.
2. The method of claim 1, wherein the step of preparing the transparent metal electrode comprises: the method specifically comprises the following steps:
carrying out ultrasonic cleaning on the glass substrate by using a detergent, isopropanol, ethanol and acetone in sequence, and drying by using nitrogen after cleaning; preparing a ZnO seed crystal layer with the thickness of 10-100nm on the surface of the glass substrate by a spin coating method, and annealing the formed film, wherein the annealing temperature is 200 ℃, and the annealing time is 2 hours; and then spin-coating a self-assembled layer of 11-mercaptoundecanoic acid and acetonitrile terephthalate molecules on the ZnO seed crystal layer, wherein the weight ratio of the 11-mercaptoundecanoic acid to the acetonitrile terephthalate is (1-1000): 1; depositing Ag with the thickness of 1-20nm as a conductive layer by a vacuum thermal evaporation method to form a metal transparent electrode.
3. An organic solar cell comprising the metal transparent electrode of claim 1, wherein: from the bottom up includes substrate, transparent electrode of metal, negative pole buffer layer, light activity layer, positive pole buffer layer, back electrode in proper order, and transparent electrode of metal includes seed crystal layer, molecule self-assembly layer, conducting layer.
4. The organic solar cell of claim 3, wherein the organic solar cell comprises a metal transparent electrode, and the metal transparent electrode comprises: the substrate material is glass or a polyester film; the cathode buffer layer is made of ZnO; the photoactive layer is PTB7-Th and PC 71 Mixed film of BM; the anode buffer layer is made of MoO 3 (ii) a The back electrode material is Ag.
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