CN114649479A - Composite cathode electrode layer for positive organic solar cell and preparation method thereof - Google Patents

Composite cathode electrode layer for positive organic solar cell and preparation method thereof Download PDF

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CN114649479A
CN114649479A CN202210235990.1A CN202210235990A CN114649479A CN 114649479 A CN114649479 A CN 114649479A CN 202210235990 A CN202210235990 A CN 202210235990A CN 114649479 A CN114649479 A CN 114649479A
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solar cell
organic solar
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杨曦
张曲
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Guangzhou Zhuoguang Technology Co ltd
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Abstract

The invention relates to a composite cathode electrode layer for a forward organic solar cell and a preparation method thereof. The composite cathode electrode layer is a double-layer metal Yb and Ag; one surface of the Yb layer is an Ag layer, and the other surface is an active layer of the positive organic solar cell. Further, the Yb thickness is 0.5nm to 20nm, and the Ag thickness is 5nm to 500 nm. The Yb and Ag double-layer electrode can reduce the work function of the electrode, is more matched with the LUMO energy level of a common organic active layer acceptor material, enables the organic active layer and the metal cathode to form ohmic contact, and improves the device performance of the organic solar cell. The method for preparing the composite cathode electrode layer adopts a vacuum thermal evaporation coating method. Compared with the prior art, the invention has the following remarkable advantages: and a cathode interface layer is not used, so that the preparation steps are reduced, and the industrial production cost is reduced.

Description

Composite cathode electrode layer for positive organic solar cell and preparation method thereof
Technical Field
The invention relates to an organic solar cell device, in particular to a composite cathode electrode layer for a forward organic solar cell and a preparation method thereof.
Background
Organic Solar Cells (OSC) have been intensively studied for many years and have been tried to be applied in the market due to their translucency, flexibility, rollability, lightness in weight, portability, and designability of color and shape. The solar cell has the working principle that a photovoltaic device is utilized to convert light energy into electric energy, sunlight irradiates an organic material in the conversion process, photons are absorbed, excitons, namely electron-hole pairs are generated, the electron-hole pairs are separated under the action of an internal electric field and move towards corresponding electrodes respectively, and are finally collected by the electrodes on two sides to generate electromotive force, and if the two ends are connected into an external circuit, the photo-generated electromotive force can form current, so that the conversion from light to electricity is completed. The OSC is generally a sandwich structure comprising a cathode, an anode and an organic photoactive layer sandwiched therebetween. Conventional OSC devices, i.e. a forward OSC anode, function to collect holes and a cathode to collect electrons. The most commonly used cathode material for forward OSC is silver (Ag), aluminum (Al), etc., and ohmic contact is formed on the metal surface of the active layer to improve the collection efficiency of electrons. However, such metal cathodes have a relatively high work function of about-4.3 eV. In order to reduce the work function of the cathode, reduce the series resistance and charge recombination loss, and form a good ohmic contact between the active layer and the electrode, a cathode interface layer needs to be inserted between the cathode and the active layer to facilitate the electron transport and the electron collection of the cathode.
Common cathode interface materials mainly comprise solution-prepared organic polymers PFN (adv. Mater.2011,23,4636-4643) and derivatives PFN-Br thereof, but these organic polymers have the disadvantages of difficult synthesis route, high production cost, and low material utilization rate of solution coating method in the process of preparing components, which is not favorable for the industrial preparation of organic solar cells.
Disclosure of Invention
The invention aims to provide a composite cathode electrode layer for a forward organic solar cell and a preparation method thereof.
In order to realize the purpose of the invention, the specific technical solution is as follows:
a composite cathode electrode layer for a positive organic solar cell is a double-layer metal of ytterbium Yb and silver Ag; wherein one surface of the Yb layer is an Ag layer, and the other surface is an active layer of the positive organic solar cell.
Further, the Yb thickness is 0.5nm to 20nm, and the Ag thickness is 5nm to 500 nm. In a more preferred embodiment, the Yb layer has a thickness of 0.5nm to 20nm, the Ag layer has a thickness of 5nm to 500nm, and the Yb layer has a purity of 99.9% or more.
A method for preparing a composite cathode electrode layer adopts a vacuum thermal evaporation coating method.
Further, the vacuum degree of the vacuum thermal evaporation coating method is 1 x 10-5～1×10-8Torr, the coating rate of Yb layer is
Figure BDA0003542200630000021
The coating rate of the Ag layer is
Figure BDA0003542200630000022
Preferably, the degree of vacuum is 5X 10-6～1×10-7Torr, the coating rate of Yb layer is
Figure BDA0003542200630000023
The coating rate of the Ag layer is
Figure BDA0003542200630000024
The principle of the invention is as follows: the double-layer metal of Yb and Ag is used as the cathode layer of the forward OSC device, the work function of Yb is-2.4-2.6 eV, the work function of Ag is-4.26-4.4 eV, and the double-layer electrode of Yb and Ag can reduce the work function and is more matched with the LUMO energy level (generally-4.0-4.3 eV) of a common organic active layer acceptor material. Ohmic contact is formed between the organic active layer and the metal cathode, and the device performance of the organic solar cell is improved.
Compared with the prior art, the invention has the following remarkable advantages:
1. the composite cathode layer provided by the invention is preferably subjected to a vacuum thermal evaporation coating method, metal Yb is directly evaporated on the substrate, a cathode interface layer is not used, the metal Yb does not need to be synthesized and can be obtained by purchasing, the preparation steps are reduced, and the preparation link of a device is optimized;
2. the composite cathode layer provided by the invention is prepared by a preferable vacuum thermal evaporation coating method, Yb and Ag are heated and evaporated to be gasified and deposited on the surface of the active layer, the required raw materials are less, the waste of the materials in the using process can be reduced, the production cost is reduced, and the industrial preparation of the organic solar cell is facilitated;
3. the composite cathode layer provided by the invention is applied to a forward organic solar cell device, and compared with a device with a cathode interface layer (PFN-Br), the performance is slightly excellent, the energy conversion rate is improved by 2.8%, and the filling factor is improved by 2.5%.
Drawings
FIG. 1 is a schematic structural view of a forward organic solar cell device of the present invention;
in the figure: 101 a substrate; 102 an anode; 103 a Hole Transport Layer (HTL); 104 an active layer; 105 cathode.
Detailed Description
The present invention will be described in further detail with reference to specific examples, but the present invention is not limited thereto. The measurement methods not described in detail in the present invention are all conventional in the art.
The following four parameters are the most direct criteria for measuring the battery performance, specifically as follows:
1. short-circuit current density (Jsc):
the current (A) output by the two ends of the photovoltaic device when the OSC is in the working current under the short-circuit condition, namely the external circuit voltage → 0;
2. open-circuit voltage (Voc)
Voltage (V) output across the photovoltaic device at the output voltage of the OSC under open circuit conditions, i.e., external circuit voltage → ∞;
3. fill Factor (Fill Factor, FF)
The ratio of the maximum output work Pm of the photovoltaic device to the product of Jsc and Voc:
Figure BDA0003542200630000031
4. photoelectric conversion efficiency PCE
The ratio of the output electric energy to the input light energy is the most direct reaction to the quality of the battery.
Figure BDA0003542200630000032
Wherein Pin is incident light power per unit area (W), and L is effective area of photovoltaic device (m)2)。
The forward organic solar cell may include a double-layer structure solar cell, a bulk heterojunction solar cell, a PMHJ (planar-mixed heterojunction) structure solar cell, a tandem cell structure (tandem cell). Preferably, the forward organic solar cell structure includes, as shown in fig. 1: a substrate (101), an anode (102), a hole transport layer (103), an active layer (104), and a cathode (105). Wherein, the cathode is the composite cathode electrode layer provided by the invention. Wherein:
the substrate (101) is transparent. Organic solar cells require a transparent bottom to absorb incident light. The substrate may be rigid or flexible. The substrate may be plastic or glass. Preferably, the substrate has a smooth surface. A substrate free of surface defects is a particularly desirable choice. In a preferred embodiment, the substrate is flexible, and may be selected from polymeric films or plastics having a glass transition temperature Tg of 150 deg.C or greater, preferably greater than 200 deg.C, more preferably greater than 250 deg.C, and most preferably greater than 300 deg.C. Examples of suitable flexible substrates are poly (ethylene terephthalate) (PET) and polyethylene glycol (2, 6-naphthalene) (PEN).
The anode (102) may comprise a conductive metal or metal oxide, or a conductive polymer. The anode may easily receive holes output from a Hole Transport Layer (HTL) or an active layer. In one embodiment, the absolute value of the difference between the work function of the anode and the HOMO level or valence band level of the donor in the active layer or the p-type semiconductor material as HTL is less than 0.5eV, preferably less than 0.3eV, most preferably less than 0.2 eV. Examples of anode materials include, but are not limited to: al, Cu, Au, Ag, Mg, Fe, Co, Ni, Mn, Pd, Pt, ITO (oxidized tin), aluminum-doped zinc oxide (AZO), and the like. Other suitable anode materials are known and can be readily selected for use by one of ordinary skill in the art. The anode material may be deposited using any suitable technique, such as a suitable physical vapor deposition method including radio frequency magnetron sputtering, vacuum thermal evaporation, electron beam (e-beam), and the like. In certain embodiments, the anode is pattern structured. Patterned ITO conductive substrates are commercially available and can be used to prepare devices according to the present invention.
The hole transport layer (103) is a material that receives holes from the active layer and transports the holes to the anode, and is a suitable hole transport material for a material having a high hole mobility. By way of specific example, suitable organic HTM materials may be selected from compounds containing structural units selected from the group consisting of phthalocyanines, porphyrins, amines, aromatic amines, triphenylamines of the biphenyl type, thiophenes, bithiophenes such as dithienothiophene and bithiophenes, pyrroles, anilines, carbazoles, azaindenoazafluorenes and derivatives thereof. In addition, suitable HTMs also include fluorocarbon containing polymers, polymers containing conductive dopants, conductive polymers, such as PEDOT: PSS.
The active layer (104) is preferably a material that can absorb sunlight, generate excitons, and separate the excitons into electrons and holes, and has a wide spectral absorption range. The material can be formed by mixing one or more materials, a more typical example is a material for an active layer which is formed by combining a thiophene polymer or a derivative thereof and fullerene or a derivative thereof and is combined with an acceptor, and a material which comprises a donor material PM6(adv. Mater.2015,27, 4655-4660) and an acceptor material Y6(Joule 3,1140-1151, April 17,2019) is more typical and commonly used at present.
The cathode (105) may include a conductive metal or metal oxide. The cathode can easily accept electrons output from the active layer or ETL. The cathode material may be deposited using any suitable technique, such as a suitable physical vapor deposition method, including radio frequency magnetron sputtering, vacuum thermal evaporation, electron beam (e-beam), and the like.
Devices of the following examples and comparative examples were prepared using a commercial hole transport layer, PEDOT, PSS, donor polymer, PM6, acceptor small molecule Y6, and electron transport layer, PFN-Br materials:
Figure BDA0003542200630000051
example 1
Anode ITO/hole transport layer PEDOT PSS/active layer PM 6Y 6/cathode Yb/Ag
Cleaning the conductive glass substrate plated with 170nm ITO by using a plurality of solvents, sequentially cleaning deionized water, acetone and isopropanol, and then carrying out ultraviolet ozone plasma treatment; PSS (PEDOT: PSS) filtered by a 0.22um filter membrane is coated on ITO in a spinning mode at the speed of 3500rpm, the coating thickness is about 40nm, then annealing is carried out for 15 minutes at 150 ℃, and the ITO is transferred into a glove box; spin-coating a PM6: Y6 blended active layer solution (the mass ratio is 1:1.2, the concentration of Y6 is 1.2g/ml, the solvent is chloroform, the additive is chloronaphthalene, the volume ratio of the chloronaphthalene is 0.5%) with the thickness of about 200nm on PEDOT: PSS, and annealing at 110 ℃ for 10 minutes; placing the prepared sheet in a vapor deposition chamber under vacuum degree of 2 × 10-7Torr to
Figure BDA0003542200630000052
Is evaporated at a rate of Yb with a thickness of 5nm and then
Figure BDA0003542200630000053
Ag was deposited at a rate of 50 nm.
Example 2
Anode ITO/hole transport layer PEDOT PSS/active layer PM 6Y 6/cathode Yb/Ag
Example 1 was repeated with the same procedure as described, but in the deposition chamber, the degree of vacuum was 2X 10-6Torr to
Figure BDA0003542200630000061
Is evaporated at a rate of Yb with a thickness of 10nm and then
Figure BDA0003542200630000062
The thickness of Ag is 100 nm.
Example 3
Anode ITO/hole transport layer PEDOT PSS/active layer PM 6Y 6/cathode Yb/Ag
Example 1 was repeated with the same procedure as described, butIn a vapor deposition chamber, the vacuum degree is 5X 10-6Torr to
Figure BDA0003542200630000063
Is evaporated at a rate of Yb, the thickness is 15nm, and then
Figure BDA0003542200630000064
The thickness of Ag is 200 nm.
Example 4
Anode ITO/hole transport layer PEDOT PSS/active layer PM 6Y 6/cathode Yb/Ag
Example 1 was repeated with the same procedure as described, but with a vacuum of 3X 10 in the deposition chamber-7Torr to
Figure BDA0003542200630000065
Is evaporated at a rate of Yb with a thickness of 20nm and then
Figure BDA0003542200630000066
The thickness of Ag is 200 nm.
Example 5
Anode ITO/hole transport layer PEDOT PSS/active layer PM 6Y 6/cathode Yb/Ag
Example 1 was repeated with the same procedure as described, but with a vacuum of 1X 10 in the deposition chamber-6Torr to
Figure BDA0003542200630000067
Is evaporated at a rate of Yb with a thickness of 20nm and then
Figure BDA0003542200630000068
The thickness of Ag is 300 nm.
Example 6
Anode ITO/hole transport layer PEDOT PSS/active layer PM 6Y 6/cathode Yb/Ag
Example 1 was repeated with the same procedure as described, but in the deposition chamber, the degree of vacuum was 1X 10-7Torr to
Figure BDA0003542200630000069
Is evaporated at a rate of Yb with a thickness of 20nm and then
Figure BDA00035422006300000610
The Ag is evaporated at a rate of 500 nm.
Comparative example
Anode ITO/hole transport layer PEDOT PSS/active layer PM 6Y 6/cathode buffer layer PFN-Br/cathode Ag
Cleaning a conductive glass substrate plated with 170nm ITO by using a plurality of solvents, sequentially cleaning deionized water, acetone and isopropanol, and then carrying out ultraviolet ozone plasma treatment; PSS (PEDOT: PSS) filtered by a 0.22um filter membrane is coated on ITO in a spinning mode at the speed of 3500rpm, the coating thickness is about 40nm, then annealing is carried out for 15 minutes at 150 ℃, and the ITO is transferred into a glove box; spin-coating a PM6: Y6 blended active layer solution (the mass ratio is 1:1.2, the concentration of Y6 is 1.2g/ml, the solvent is chloroform, the additive is chloronaphthalene, the volume ratio of the chloronaphthalene is 0.5%) with the thickness of about 200nm on PEDOT: PSS, and annealing at 110 ℃ for 10 minutes; PFN-Br (solvent: methanol, concentration: 0.5mg/ml) was spin-coated at 3000 rmp; placing the prepared sheet in a vapor deposition chamber, and then
Figure BDA0003542200630000071
The thickness of Ag is 100 nm.
And (3) performing performance test on the prepared organic solar cell device, testing a cell current-voltage curve under the irradiation of standard light of a solar simulator (SS-F5-3A) AM1.5G, and calculating the photoelectric conversion efficiency.
Figure BDA0003542200630000072
The cell performance of examples 1-5 was comparable to the comparative example, with a 2.8% improvement in photoelectric conversion efficiency and a 2.5% improvement in fill factor.

Claims (5)

1. A composite cathode electrode layer for a forward organic solar cell, characterized by: the composite cathode electrode layer is a double-layer metal of ytterbium Yb and silver Ag; one surface of the Yb layer is an Ag layer, and the other surface of the Yb layer is an active layer of the forward organic solar cell.
2. A composite cathode electrode layer for a forward organic solar cell according to claim 1, wherein: the Yb thickness is 0.5nm-20nm and the Ag thickness is 5nm-500 nm.
3. A composite cathode electrode layer for a forward organic solar cell according to claim 2, wherein: the Yb thickness was 10nm and the Ag thickness was 100 nm.
4. A method of preparing a composite cathode electrode layer according to any one of claims 1 to 3, characterized in that: the preparation of the composite cathode electrode layer adopts a vacuum thermal evaporation coating method.
5. The method of claim 4, wherein: the vacuum degree of the vacuum thermal evaporation coating method is 1 multiplied by 10-5～1×10-8Torr, a coating rate of the Yb layer is
Figure FDA0003542200620000011
The coating rate of the Ag layer is
Figure FDA0003542200620000012
CN202210235990.1A 2022-03-11 2022-03-11 Composite cathode electrode layer for positive organic solar cell and preparation method thereof Pending CN114649479A (en)

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Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN116234334A (en) * 2023-02-16 2023-06-06 武汉大学 Tin-lead mixed perovskite solar cell based on double-layer metal electrode and preparation method thereof

Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN116234334A (en) * 2023-02-16 2023-06-06 武汉大学 Tin-lead mixed perovskite solar cell based on double-layer metal electrode and preparation method thereof

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