CN113594377A - Quantum dot light-emitting diode and preparation method thereof - Google Patents
Quantum dot light-emitting diode and preparation method thereof Download PDFInfo
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- H—ELECTRICITY
- H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
- H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
- H10K50/00—Organic light-emitting devices
- H10K50/10—OLEDs or polymer light-emitting diodes [PLED]
- H10K50/11—OLEDs or polymer light-emitting diodes [PLED] characterised by the electroluminescent [EL] layers
- H10K50/115—OLEDs or polymer light-emitting diodes [PLED] characterised by the electroluminescent [EL] layers comprising active inorganic nanostructures, e.g. luminescent quantum dots
-
- H—ELECTRICITY
- H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
- H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
- H10K30/00—Organic devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation
- H10K30/80—Constructional details
- H10K30/865—Intermediate layers comprising a mixture of materials of the adjoining active layers
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- H—ELECTRICITY
- H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
- H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
- H10K50/00—Organic light-emitting devices
- H10K50/10—OLEDs or polymer light-emitting diodes [PLED]
- H10K50/14—Carrier transporting layers
- H10K50/16—Electron transporting layers
-
- H—ELECTRICITY
- H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
- H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
- H10K71/00—Manufacture or treatment specially adapted for the organic devices covered by this subclass
Abstract
The invention belongs to the technical field of display, and relates to a quantum dot light-emitting diode and a preparation method thereof. The quantum dot light emitting diode includes: an anode and a cathode disposed opposite to each other; a quantum dot light emitting layer disposed between the anode and the cathode; an electron transport layer disposed between the quantum dot light emitting layer and the cathode; a polymer modification layer disposed between the electron transport layer and the quantum dot light emitting layer; wherein, the polymer in the polymer modification layer is selected from polymers containing amino functional groups. The quantum dot light-emitting diode provided by the invention has the advantages that the light-emitting efficiency is improved, and the service life is prolonged.
Description
Technical Field
The invention belongs to the technical field of display, and particularly relates to a quantum dot light-emitting diode and a preparation method thereof.
Background
The quantum dot electroluminescent display technology has the advantages of adjustable wavelength, high color saturation, high material stability, low preparation cost and the like, and becomes an optimal candidate for the next generation display technology. With the development of nearly twenty years, the external quantum efficiency of quantum dot light emitting diodes has been promoted to over 20% via 0.01%, and quantum dot light emitting diodes (QLEDs) have come quite close to Organic Light Emitting Diodes (OLEDs) in terms of device efficiency. However, despite the advantages of quantum dot devices, the performance of the devices has not yet fully reached the requirements of industrialization, especially for blue QLED devices.
The structure of the device of the QLED is similar to that of the OLED at present, a sandwich structure similar to a p-i-n junction is formed by a hole injection layer, a hole transport layer, a light emitting layer, an electron transport layer and the like, and the light emitting effect is achieved by balancing the injection of electrons and holes. Because the band gap of the blue quantum dot is wider than that of the red and green quantum dot, electron holes are more difficult to inject, the starting voltage is further increased, the interface charge accumulation is more serious, and the service life and the efficiency of the device are greatly influenced. Particularly, when the electron transport layer is made of zinc oxide, a charge transfer phenomenon exists between the zinc oxide and the quantum dot interface, and the electron binding capacity of the quantum dot is lower than that of the quantum dot, so that the serious charge transfer phenomenon occurs at the zinc oxide and quantum dot interface, and the charge transfer is more serious along with the improvement of the conduction band energy level of the blue quantum dot. The transfer of excited electrons between interfaces not only causes the charge accumulation at the interfaces, but also greatly improves the probability of nonradiative Auger recombination, and seriously influences the luminous efficiency and the service life of the device.
Disclosure of Invention
The invention aims to provide a quantum dot light-emitting diode and a preparation method thereof, and aims to solve the problem that the luminous efficiency and the service life of a device are influenced due to charge accumulation existing in an electron transmission layer and a quantum dot interface in the conventional quantum dot light-emitting diode.
In order to achieve the purpose, the invention adopts the following technical scheme:
the present invention provides, in a first aspect, a quantum dot light emitting diode comprising:
an anode and a cathode disposed opposite to each other;
a quantum dot light emitting layer disposed between the anode and the cathode;
an electron transport layer disposed between the quantum dot light emitting layer and the cathode;
a polymer modification layer disposed between the electron transport layer and the quantum dot light emitting layer;
wherein, the polymer in the polymer modification layer is selected from polymers containing amino functional groups.
The invention provides a preparation method of a quantum dot light-emitting diode in a second aspect, which comprises the following steps:
sequentially stacking a first electrode and a first functional layer on one side surface of the substrate;
depositing a polymer solution on the surface of the first functional layer on the side far away from the first electrode to prepare a polymer modification layer;
sequentially stacking a second functional layer and a second electrode on the surface of one side, away from the first functional layer, of the polymer modification layer;
the first electrode is an anode, the first functional layer is a quantum dot light-emitting layer, the second functional layer is an electron transport layer, and the second electrode is a cathode; or
The first electrode is a cathode, the first functional layer is an electron transport layer, the second functional layer is a quantum dot light emitting layer, and the second electrode is an anode.
According to the quantum dot light-emitting diode provided by the invention, the polymer modification layer capable of improving the energy level of the electron transport material is arranged between the electron transport layer and the quantum dot light-emitting layer. The polymer modification layer reduces the work function of the electron transmission layer through the amino dipole and the interface dipole, so that the energy level of the electron transmission layer is shifted upwards, the charge transfer between the quantum dots and the electron transmission material is inhibited, the electron injection efficiency is improved, and the transfer of electrons from the electron transmission layer to the quantum dot light emitting layer is promoted. Meanwhile, hole transmission on the side far away from the quantum dots is not affected, and the energy level is kept at the original level.
The preparation method of the quantum dot light-emitting diode provided by the invention only needs to introduce the polymer modification layer between the electron transmission layer and the quantum dot light-emitting layer. The method has the advantages of simple process, strong operability, solution processing mode and easy realization of industrial production.
Drawings
In order to more clearly illustrate the technical solutions in the embodiments of the present invention, the drawings needed to be used in the embodiments or the prior art descriptions will be briefly described below, and it is obvious that the drawings in the following description are only some embodiments of the present invention, and it is obvious for those skilled in the art to obtain other drawings based on these drawings without inventive exercise.
Fig. 1 is a schematic structural diagram of a quantum dot light-emitting diode provided in an embodiment of the present invention;
fig. 2 is a flow chart of a manufacturing process of a quantum dot light emitting diode according to an embodiment of the present invention.
Detailed Description
In order to make the technical problems, technical solutions and advantageous effects to be solved by the present invention more clearly apparent, the present invention is further described in detail below with reference to the following embodiments. It should be understood that the specific embodiments described herein are merely illustrative of the invention and are not intended to limit the invention.
In the description of the present invention, it is to be understood that the terms "first", "second" and the like are used for descriptive purposes only and are not to be construed as indicating or implying relative importance or implying any number of technical features indicated. Thus, a feature defined as "first" or "second" may explicitly or implicitly include one or more of that feature. In the description of the present invention, "a plurality" means two or more unless specifically defined otherwise.
The weight of the related components mentioned in the description of the embodiments of the present invention may not only refer to the specific content of each component, but also represent the proportional relationship of the weight among the components, and therefore, the content of the related components is scaled up or down within the scope disclosed in the description of the embodiments of the present invention as long as it is in accordance with the description of the embodiments of the present invention. Specifically, the weight in the description of the embodiment of the present invention may be a unit of mass known in the chemical industry field such as μ g, mg, g, kg, etc.
A first aspect of an embodiment of the present invention provides a quantum dot light emitting diode, including:
an anode and a cathode disposed opposite to each other;
a quantum dot light emitting layer disposed between the anode and the cathode;
an electron transport layer disposed between the quantum dot light emitting layer and the cathode;
the polymer modification layer is arranged between the electron transmission layer and the quantum dot light-emitting layer;
wherein, the polymer in the polymer modification layer is selected from polymers containing amino functional groups.
According to the quantum dot light-emitting diode provided by the embodiment of the invention, the polymer modification layer capable of improving the energy level of the electron transport material is arranged between the electron transport layer and the quantum dot light-emitting layer. The polymer modification layer reduces the work function of the electron transmission layer through the amino dipole and the interface dipole, so that the energy level of the electron transmission layer shifts upwards, the charge transfer between the quantum dots and the electron transmission material is inhibited, the electron injection efficiency is improved, and the transfer of electrons from the electron transmission layer to the quantum dot light emitting layer is promoted. Meanwhile, hole transmission on the side far away from the quantum dots is not affected, and the energy level is kept at the original level.
According to the embodiment of the invention, the polymer modification layer containing the amino functional group is arranged between the electron transmission layer and the quantum dot light emitting layer of the quantum dot light emitting diode, so that the energy level of the electron transmission layer material is improved on the basis of not influencing hole transmission, the quantum dot light emitting diode forms a more reasonable level gradient, and electrons are promoted to be injected into the quantum dot light emitting layer from the electron transmission layer. In some embodiments, the polymer modification layer is made of one polymer. Namely, the polymer modification layer is a single-layer film, and the material in the single-layer film is the same polymer. In some embodiments, the polymer modification layer is made of a hybrid material formed of two or more polymers. Namely, the polymer modification layer is a single-layer film, and the material in the single-layer film is a mixed material formed by two or more polymers. It should be understood that the polymers in the polymer modification layers of the embodiments of the present invention are all selected from polymers that can increase the energy level of the electron transport layer material.
More specifically, the quantum dot light emitting diode may further include a substrate on which the anode is disposed.
It is understood that the device structure is an inverted structure commonly used in the quantum dot light emitting diode, and if the device structure is inverted layer by layer into an inverted structure, the purpose of the present invention is not violated. For example, a cathode, an electron transport layer, a polymer modification layer, a quantum dot light emitting layer, and an anode are sequentially stacked on a substrate.
The present invention only takes the front-mounted structure as an example to illustrate the electroluminescent diode device provided in the above embodiments, and the materials and functions of the layers of the inverted structure are not different.
Based on the above embodiments, in some embodiments, the substrate may include a rigid substrate such as glass, metal foil, etc., or a flexible substrate such as Polyimide (PI), Polycarbonate (PC), Polystyrene (PS), Polyethylene (PE), polyvinyl chloride (PV), polyvinylpyrrolidone (PVP), polyethylene terephthalate (PET), etc., which mainly plays a role of support.
In some embodiments, the polymer in the polymer modification layer is selected from: at least one of Polyethyleneimine (PEI), ethoxylated Polyethyleneimine (PEIE) and Poly [ (9,9-bis (3'- (N, N-dimethylamino) propyl) -2,7-fluorene) -2,7- (9, 9-dioctylfluorene ] (Poly [ (9,9-bis (3' - (N, N-dimethyllamino) propyl) -2, 7-fluoroene) -alt-2,7- (9, 9-dioctylfluoroene) ], abbreviated as PFN), wherein, the structures of Polyethyleneimine (PEI), ethoxylated Polyethyleneimine (PEIE) and poly [ (9,9-bis (3' - (N, N-dimethylamino) propyl) -2,7-fluorene) -2,7- (9, 9-dioctylfluorene ] (PFN) are shown below.
In some embodiments, the polymer modification layer is made of one of polyethyleneimine, ethoxylated polyethyleneimine, and poly [ (9,9-bis (3'- (N, N-dimethylamino) propyl) -2,7-fluorene) -2,7- (9, 9-dioctylfluorene ] in some embodiments, the polymer modification layer is made of a mixed material of two or more polymers, more particularly, the polymer modification layer is made of a mixed material of polyethyleneimine and ethoxylated polyethyleneimine, the polymer modification layer is made of a mixed material of ethoxylated polyethyleneimine and poly [ (9,9-bis (3' - (N, N-dimethylamino) propyl) -2,7-fluorene) -2,7- (9, 9-dioctylfluorene ], the polymer modification layer is made of a mixed material formed by polyethyleneimine and poly [ (9,9-bis (3'- (N, N-dimethylamino) propyl) -2,7-fluorene) -2,7- (9, 9-dioctyl fluorene ], or the polymer modification layer is made of a mixed material formed by polyethyleneimine, ethoxylated polyethyleneimine and poly [ (9,9-bis (3' - (N, N-dimethylamino) propyl) -2,7-fluorene) -2,7- (9, 9-dioctyl fluorene ].
The modification layer made of the polymer interacts with the surface of an electron transport layer material (such as zinc oxide) when the modification layer is arranged between the quantum dot light-emitting layer and the electron transport layer, and due to the action of an interface dipole formed by combining the polymer and the electron transport layer material and a self-carried dipole of the polymer, the energy level of the electron transport layer material shifts upwards, the work function is reduced, and the electron transport layer material is matched with the conduction band energy level of the quantum dot light-emitting layer, so that the charge transfer between the quantum dot and the electron transport layer interface is reduced, the electron injection efficiency is improved, the light-emitting efficiency of the quantum dot light-emitting diode device is improved finally, and the service life of the quantum dot light-emitting diode device is prolonged.
In some embodiments, the polymer modification layer has a thickness of 2 to 10 nm. The thickness of the polymer modification layer is within the range, the energy level structure of the electron transport layer material can be effectively adjusted, and the electron transport layer material is enabled to be matched with the conduction band energy level of the quantum dot light emitting layer, so that the charge transfer between the quantum dot and the electron transport material interface is reduced, the electron injection efficiency is improved, the light emitting efficiency of the quantum dot light emitting diode device is finally improved, and the service life of the quantum dot light emitting diode device is finally prolonged. If the thickness of the polymer modification layer is too thin, the work function of the electron transport material cannot be effectively reduced, so that the energy level of the electron transport layer material cannot be effectively improved; if the thickness of the polymer modification layer is too thick, the intrinsic insulation property of the polymer material can reduce the conductivity of the device, and even the quantum dots and the electron transmission material are insulated, so that the quantum dot light-emitting diode loses the photoelectric property.
In the embodiment of the present application, the anode may be made of a common anode material and thickness, and the embodiment of the present application is not limited. For example, the anode material may be Indium Tin Oxide (ITO), Indium Zinc Oxide (IZO) conductive glass, or indium tin oxide, indium zinc oxide electrode, or may be other metal materials such as gold, silver, aluminum, and the like.
The electron transport layer is selected from common electron transport layer materials. In some embodiments, the material of the electron transport layer is selected from: at least one of nano zinc oxide, magnesium-doped zinc oxide and aluminum-doped zinc oxide.
In the embodiments of the present application, the cathode may be made of a common cathode material and thickness, and the embodiments of the present application are not limited. The cathode may be an Indium Tin Oxide (ITO), Indium Zinc Oxide (IZO) conductive glass, or an indium tin oxide, indium zinc oxide electrode, or may be other metal materials such as aluminum, silver, magnesium, and an alloy of at least two of aluminum, silver, and magnesium, or may be a conductive carbon material such as graphite, carbon nanotube, graphene, carbon fiber, or the like.
The material of the quantum dot light-emitting layer can be selected from conventional quantum dot materials according to conventional quantum dot types. For example, the quantum dots of the quantum dot light-emitting layer can be one of red quantum dots, green quantum dots, blue quantum dots and yellow quantum dots; the quantum dot material may or may not contain cadmium; the quantum dots can be oil-soluble quantum dots comprising binary phase, ternary phase and quaternary phase quantum dots. In some embodiments, the quantum dot material may be selected from at least one of semiconductor nanocrystals of CdS, CdSe, CdTe, ZnSe, ZnTe, GaAs, GaP, GaSb, HgS, HgSe, HgTe, InAs, InP, InSb, AlAs, AlP, CuInS, CuInSe, AgS, PbS, and PbSe, and core-shell structured quantum dots or alloy structured quantum dots formed of the above materials; in some embodiments, the quantum dot material may be selected from ZnXCd1-XS、CuXIn1-XS、ZnXCd1-XSe、ZnXSe1-XS、ZnXCd1-XTe、PbSeXS1-XHalf ofThe material comprises a conductor nanocrystal and at least one of core-shell structure quantum dots or alloy structure quantum dots formed by the material. In some embodiments, the quantum dot material may be selected from ZnXCd1-XS/ZnSe、CuXIn1-XS/ZnS、ZnXCd1-XSe/ZnS、CuInSeS、ZnXCd1-XTe/ZnS、PbSeXS1-XThe nano-crystalline material comprises/ZnS semiconductor nano-crystalline and at least one of core-shell structure quantum dots or alloy structure quantum dots formed by the material.
On the basis of the above embodiments, in some embodiments, a hole function layer is arranged between the anode and the quantum dot light-emitting layer; in some embodiments, an electron injection layer is disposed between the cathode and the electron transport layer; in some embodiments, a hole-functional layer is disposed between the anode and the quantum dot light-emitting layer, and an electron-injection layer is disposed between the cathode and the electron-transport layer. The hole function layer comprises at least one of a hole injection layer, a hole transport layer and an electron blocking layer.
The material of the hole injection layer can be made of a hole injection material which is conventional in the art, and can be PEODT: PSS, CuPc, HATCN, WoOx、MoOx、CrOx、NiO、CuO、VOx、CuS、MoS2、MoSe2、WS2、WSe2But is not limited thereto. The thickness of the hole injection layer is 30nm-100 nm.
The hole transport layer can be made of hole transport material conventional in the art, and can be TFB, PVK, PFB, TPD, TCTA, TAPC, Poly-TBP, Poly-TPD, NPB, CBP, MoO3、WoO3、NiO、CuO、V2O5And CuS, but not limited thereto. The thickness of the hole transport layer is 30nm-100 nm.
In some embodiments, the quantum dot light emitting diode comprises an anode and a cathode which are oppositely arranged, a quantum dot light emitting layer arranged between the anode and the cathode, an electron transport layer arranged between the quantum dot light emitting layer and the cathode, and a polymer modification layer arranged between the electron transport layer and the quantum dot light emitting layer, wherein the polymer in the polymer modification layer is polyethyleneimine and/or ethoxylated polyethyleneimine; the thickness of the polymer modification layer is 2nm to 10 nm. On the basis, the material of the electron transport layer is selected from the following group: at least one of nano zinc oxide, magnesium-doped zinc oxide and aluminum-doped zinc oxide.
As shown in fig. 1, in some embodiments, a quantum dot light emitting diode includes an anode and a cathode disposed opposite to each other, a quantum dot light emitting layer disposed between the anode and the cathode, an electron transporting layer disposed between the quantum dot light emitting layer and the cathode, a hole injecting layer disposed between the anode and the quantum dot light emitting layer, a hole transporting layer disposed between the hole injecting layer and the quantum dot light emitting layer, and a polymer modifying layer disposed between the electron transporting layer and the quantum dot light emitting layer, wherein the anode is disposed on a substrate, and a polymer in the polymer modifying layer is polyethyleneimine and/or ethoxylated polyethyleneimine; the thickness of the polymer modification layer is 2nm to 10 nm; the material of the electron transport layer is selected from: at least one of nano zinc oxide, magnesium-doped zinc oxide and aluminum-doped zinc oxide.
The quantum dot light-emitting diode provided by the embodiment of the invention can be prepared by the following method.
As shown in fig. 2, a second aspect of the embodiments of the present invention provides a method for manufacturing a quantum dot light emitting diode, including the following steps:
s01, sequentially stacking a first electrode and a first functional layer on one side surface of a substrate;
s02, depositing a polymer solution on the surface of one side, far away from the first electrode, of the first functional layer to prepare a polymer modification layer;
s03, sequentially stacking a second functional layer and a second electrode on the surface of one side, away from the first functional layer, of the polymer modification layer;
the first electrode is an anode, the first functional layer is a quantum dot light-emitting layer, the second functional layer is an electron transport layer, and the second electrode is a cathode; or
The first electrode is a cathode, the first functional layer is an electron transmission layer, the second functional layer is a quantum dot light-emitting layer, and the second electrode is an anode.
The preparation method of the quantum dot light-emitting diode provided by the embodiment of the invention only needs to introduce the polymer modification layer between the electron transmission layer and the quantum dot light-emitting layer. The method has the advantages of simple process, strong operability, solution processing mode and easy realization of industrial production.
Specifically, in step S01, the first electrode and the first functional layer are sequentially stacked on one surface of the substrate. In one embodiment, the first electrode is an anode and the first functional layer is a quantum dot light emitting layer. In some embodiments, a hole function layer is disposed between the quantum dot light emitting layer and the anode, and the hole function layer includes at least one of a hole injection layer, a hole transport layer, and an electron blocking layer. In another embodiment, the first electrode is a cathode and the first functional layer is an electron transport layer. In some embodiments, a hole injection layer is disposed between the electron transport layer and the cathode.
In the step S02, a polymer solution is provided, and the polymer solution is an organic solution of a polymer. Specifically, the preparation method of the polymer solution comprises the following steps: the polymer is dissolved in an organic solvent to obtain a polymer solution. Wherein the polymer in the polymer solution is selected from polymers capable of improving the energy level of the electron transport layer material; the organic solvent used to dissolve the polymer is preferably an organic alcohol, including but not limited to ethanol. In some embodiments, the polymer solution includes a polymer and an alcohol solvent.
In some embodiments, the polymer is selected from: at least one of polyethyleneimine, ethoxylated polyethyleneimine and poly [ (9,9-bis (3' - (N, N-dimethylamino) propyl) -2,7-fluorene) -2,7- (9, 9-dioctylfluorene ], a modification layer made of the above polymer interacts with the surface of an electron transport layer material such as zinc oxide when the modification layer is placed between the quantum dot light emitting layer and the electron transport layer, due to the action of an interface dipole and a polymer self-carried dipole formed by combining the polymer and an electron transport layer material such as zinc oxide, the energy level of the electron transport layer material such as zinc oxide shifts upwards, the work function is reduced, the electron transport layer material is more matched with the energy level of a conduction band of the quantum dot light-emitting layer, therefore, charge transfer between the quantum dot and the interface of the electron transport material is reduced, the electron injection efficiency is improved, and finally, the luminous efficiency and the service life of the quantum dot light-emitting diode device are improved.
In some embodiments, the concentration of the polymer in the polymer solution is 0.5 to 2 mg/ml. In this case, a polymer film having an appropriate thickness can be obtained by film formation by a solution processing method. Specifically, the concentration of the polymer in the polymer solution is controlled to be 0.5-2 mg/ml, so that a film with the thickness of 2-10 nm is obtained. The thickness of the polymer modification layer is within the range, the energy level structure of the electron transport layer material can be effectively adjusted, and the electron transport layer material is enabled to be matched with the conduction band energy level of the quantum dot light emitting layer, so that the charge transfer between the quantum dot and the electron transport material interface is reduced, the electron injection efficiency is improved, the light emitting efficiency of the quantum dot light emitting diode device is finally improved, and the service life of the quantum dot light emitting diode device is finally prolonged. If the thickness of the polymer modification layer is too thin, the work function of the electron transport material cannot be effectively reduced, so that the energy level of the electron transport layer material cannot be effectively improved; if the thickness of the polymer modification layer is too thick, the intrinsic insulation property of the polymer material can reduce the conductivity of the device, and even the quantum dots and the electron transmission material are insulated, so that the quantum dot light-emitting diode loses the photoelectric property.
The deposition of the polymer solution on the surface of the first functional layer remote from the first electrode can be achieved by solution processing methods including, but not limited to, ink jet printing, spin coating, doctor blading, and the like. It is worth noting that after the polymer solution is deposited on the surface of the first functional layer away from the first electrode, no heating treatment is performed, so that the polymer modification layer and the second functional layer can be well fused.
In some embodiments, the polymeric modifying layer is prepared using a spin-on process. Wherein the concentration of the polymer solution is 0.5-2 mg/ml, the spin coating rotation speed is 4000-6000 revolutions per second, and the thickness of the polymer modification layer is 2-10 nm.
In step S03, a second functional layer is formed on the surface of the polymer modified layer away from the first functional layer. In some embodiments, the step of preparing the second functional layer on the polymer modification layer comprises: providing a second functional material solution, and depositing the second functional material solution on the surface of one side, away from the first functional layer, of the polymer modification layer by a solution processing method to prepare a second functional layer; wherein the solvent in the second functional material solution is the same as or miscible with the solvent in the polymer solution. In this case, the polymer modification layer and the second functional layer are in closer contact, and the effect is more remarkable.
After the second functional layer is deposited, annealing treatment is carried out, so that the solvents in the polymer modification layer and the second functional layer are fully volatilized, meanwhile, the polymer and the second functional layer are tightly combined at the interface, and the compact polymer modification layer and the second functional layer are prepared. In some embodiments, the temperature of the annealing treatment is 80 ℃ to 100 ℃, and the time of the annealing treatment is 15min to 30 min.
Further, a second electrode is prepared on the second functional layer.
When it is understood that the second functional layer and the second electrode correspond to the first functional layer and the first electrode, when the first electrode is an anode and the first functional layer is a quantum dot light emitting layer, the second electrode is a cathode, and the second functional layer is an electron transport layer. In some embodiments, before depositing the second electrode, further comprising preparing an electron injection layer on the second functional layer.
When the first electrode is a cathode and the first functional layer is an electron transport layer, the second electrode is an anode and the second functional layer is a quantum dot light emitting layer. In some embodiments, before depositing the second electrode, further comprising preparing a hole functional layer on the second functional layer, and the hole functional layer comprises at least one of a hole injection layer, a hole transport layer, and an electron blocking layer.
The following description will be given with reference to specific examples.
Example 1
A preparation method of a quantum dot light-emitting diode comprises the following steps:
(1) depositing 40nm ITO on a transparent glass substrate to serve as an anode, cleaning the ITO surface for 15 minutes by adopting ultraviolet ozone (UVO), and simultaneously changing the wettability of the surface;
(2) preparing a hole injection layer by spin-coating PEDOT: PSS (poly (3, 4-ethylenedioxythiophene): poly (styrenesulfonic acid)) on ITO; wherein the spin coating speed is 5000 revolutions per minute and the spin coating time is 40 s; then annealing at 150 ℃ for 15min, wherein the whole step is carried out in the air;
(3) dissolving TFB (poly [ (9, 9-di-N-octylfluorenyl-2, 7-diyl) -alt- (4,4' - (N- (4-N-butyl) phenyl) -diphenylamine) ]) in chlorobenzene to prepare a TFB solution with a concentration of 8 mg/ml; spin-coating TFB solution on PEDOT (PSS) to prepare a hole transport layer; wherein the spin-coating speed is 3000 rpm, and the spin-coating time is 30 s; then heating at 150 deg.C for 30min, which is carried out in a glove box;
(4) dissolving quantum dots in n-octane to prepare a quantum dot solution with the concentration of 20 mg/ml; spin-coating a quantum dot solution on the TFB to prepare a quantum dot light-emitting layer; wherein, the rotating speed is 2000 rpm, and the spin coating is carried out for 30 s; then heating at 100 deg.C for 20min, which is carried out in a glove box;
(5) dissolving polyethyleneimine in ethanol to prepare a polyethyleneimine solution with the concentration of 2 mg/ml; spin-coating a polyethyleneimine solution on the quantum dot light-emitting layer to prepare a polyethyleneimine modification layer; wherein the spin coating speed is 5000 revolutions per minute, the spin coating is carried out for 40s, and the step is carried out in a glove box;
(6) dissolving zinc oxide colloid in ethanol, and setting the concentration of the zinc oxide colloid solution to be 30 mg/ml; directly spin-coating a zinc oxide colloid solution to prepare a zinc oxide layer without heating after the polyethylene imine modification layer is spin-coated; wherein the spin-coating speed is 3000 rpm, and the spin-coating time is 30 s; then heating at 100 deg.C for 30min, which is carried out in a glove box;
(7) and evaporating Al on the zinc oxide layer to prepare a cathode, wherein the thickness of the cathode is 80 nm.
Example 2
A preparation method of a quantum dot light-emitting diode comprises the following steps:
(1) depositing 40nm ITO on a transparent glass substrate to serve as an anode, cleaning the ITO surface for 15 minutes by adopting ultraviolet ozone (UVO), and simultaneously changing the wettability of the surface;
(2) PSS is used for preparing a hole injection layer; wherein the spin coating speed is 5000 revolutions per minute and the spin coating time is 40 s; then annealing at 150 ℃ for 15min, wherein the whole step is carried out in the air;
(3) dissolving TFB in chlorobenzene to prepare TFB solution with the concentration of 8 mg/ml; spin-coating TFB solution on PEDOT (PSS) to prepare a hole transport layer; wherein the spin-coating speed is 3000 rpm, and the spin-coating time is 30 s; then heating at 150 deg.C for 30min, which is carried out in a glove box;
(4) dissolving quantum dots in n-octane to prepare a quantum dot solution with the concentration of 20 mg/ml; spin-coating a quantum dot solution on the TFB to prepare a quantum dot light-emitting layer; wherein, the rotating speed is 2000 rpm, and the spin coating is carried out for 30 s; then heating at 100 deg.C for 20min, which is carried out in a glove box;
(5) dissolving poly [ (9,9-bis (3' - (N, N-dimethylamino) propyl) -2,7-fluorene) -2,7- (9, 9-dioctylfluorene ] in chlorobenzene, preparing poly [ (9,9-bis (3' - (N, N-dimethylamino) propyl) -2,7-fluorene) -2,7- (9, 9-dioctylfluorene ] solution with concentration of 2mg/ml, spin-coating poly [ (9,9-bis (3' - (N, N-dimethylamino) propyl) -2,7-fluorene) -2,7- (9, 9-dioctylfluorene ] solution on the quantum dot light-emitting layer to prepare the polyethyleneimine modifying layer, wherein the spin-coating rotation speed is 5000 revolutions per minute and 40 seconds, this step is carried out in a glove box;
(6) dissolving zinc oxide colloid in ethanol, and setting the concentration of the zinc oxide colloid solution to be 30 mg/ml; directly spin-coating a zinc oxide colloidal solution to prepare a zinc oxide layer without heating after spin-coating a poly [ (9,9-bis (3' - (N, N-dimethylamino) propyl) -2,7-fluorene) -2,7- (9, 9-dioctylfluorene ] modification layer, wherein the spin-coating speed is 3000 r/min, the spin-coating time is 30s, and then heating is carried out for 30min at 100 ℃, and the step is carried out in a glove box;
(7) and evaporating Al on the zinc oxide layer to prepare a cathode, wherein the thickness of the cathode is 80 nm.
Comparative example
A preparation method of a quantum dot light-emitting diode comprises the following steps:
(1) depositing ITO (indium tin oxide) with the thickness of 40nm on a transparent glass substrate to be used as an anode, cleaning the surface for 15 minutes by ultraviolet ozone (UVO), and cleaning the surface while changing the wettability of the surface;
(2) PSS is used as a hole injection layer, the spin coating speed is 5000 rpm, the spin coating is 40s, then the annealing is carried out for 15min at 150 ℃, and the whole step is carried out in the air;
(3) spin-coating a TFB layer on PEDOT (PSS) to form a hole transport layer, dissolving the TFB layer in chlorobenzene at a concentration of 8mg/ml, at a spin-coating speed of 3000 rpm for 30s, and heating at 150 ℃ for 30min, wherein the step is carried out in a glove box;
(4) spin-coating a quantum dot light-emitting layer on a TFB, dissolving quantum dots in n-octane at a concentration of 20mg/ml and a rotation speed of 2000 rpm for 30s, and then heating at 100 ℃ for 20min, wherein the step is carried out in a glove box;
(5) a zinc oxide layer is spin-coated on the quantum dot light-emitting layer, zinc oxide colloid is dissolved in ethanol, the concentration is 30mg/ml, the spin-coating rotating speed is 3000 r/min, the spin-coating time is 30s, then the heating is carried out for 30min at 100 ℃, and the step is carried out in a glove box;
(7) and a layer of Al is evaporated on the zinc oxide layer to be used as a cathode, and the thickness is 80 nm.
The quantum dot light-emitting diodes prepared in the above examples 1 to 2 and the quantum dot light-emitting diode prepared in the comparative example 1 were subjected to performance tests, and the test indexes and the test method were as follows:
(1) external Quantum Efficiency (EQE): measured using an EQE optical test instrument. Note: a QLED device with external quantum efficiency test; (2) service life: the standard of the life test is unified as the time for the attenuation to 95 percent under 1000cd/A, and the life test is measured by adopting a light-emitting diode life test device. Note: life test QLED device. The test results are shown in table 1 below.
TABLE 1
| Group of | External Quantum Efficiency (EQE)/(%) | Life/(h) |
| Example 1 | 17.7％ | 580h |
| Example 2 | 16.1％ | 760h |
| Comparative example 1 | 10.5％ | 300h |
As can be seen from table 1, in the quantum dot light emitting diode provided in embodiments 1 to 2 of the present application, since the polymer modification layer is introduced between the electron transport layer and the quantum dot light emitting layer, both the external quantum efficiency and the service life are significantly improved.
The above description is only for the purpose of illustrating the preferred embodiments of the present invention and is not to be construed as limiting the invention, and any modifications, equivalents and improvements made within the spirit and principle of the present invention are intended to be included within the scope of the present invention.
Claims (10)
1. A quantum dot light emitting diode, comprising:
an anode and a cathode disposed opposite to each other;
a quantum dot light emitting layer disposed between the anode and the cathode;
an electron transport layer disposed between the quantum dot light emitting layer and the cathode;
a polymer modification layer disposed between the electron transport layer and the quantum dot light emitting layer;
wherein, the polymer in the polymer modification layer is selected from polymers containing amino functional groups.
2. The quantum dot light-emitting diode of claim 1, wherein the polymer modification layer is made of a polymer; or
The polymer modification layer is made of a mixed material formed by two or more polymers.
3. The quantum dot light-emitting diode of claim 1, wherein the polymer is selected from the group consisting of: at least one of polyethyleneimine, ethoxylated polyethyleneimine and poly [ (9,9-bis (3' - (N, N-dimethylamino) propyl) -2,7-fluorene) -2,7- (9, 9-dioctylfluorene ].
4. The quantum dot light-emitting diode of claim 1, wherein the polymer modification layer has a thickness of 2 to 10 nm.
5. The qd-led of any one of claims 1 to 4, wherein the electron transport layer is made of a material selected from the group consisting of: at least one of nano zinc oxide, magnesium-doped zinc oxide and aluminum-doped zinc oxide.
6. The qd-led of any one of claims 1 to 4, wherein a hole functional layer is disposed between the anode and the qd-light emitting layer; and/or
An electron injection layer is arranged between the cathode and the electron transport layer.
7. A preparation method of a quantum dot light-emitting diode is characterized by comprising the following steps:
sequentially laminating a first electrode and a first functional layer on one side surface of the substrate;
depositing a polymer solution on the surface of the first functional layer on the side far away from the first electrode to prepare a polymer modification layer;
sequentially stacking a second functional layer and a second electrode on the surface of one side, away from the first functional layer, of the polymer modification layer;
the first electrode is an anode, the first functional layer is a quantum dot light-emitting layer, the second functional layer is an electron transport layer, and the second electrode is a cathode; or
The first electrode is a cathode, the first functional layer is an electron transport layer, the second functional layer is a quantum dot light emitting layer, and the second electrode is an anode.
8. The method for preparing a quantum dot light-emitting diode according to claim 7, wherein the concentration of the polymer in the polymer solution is 0.5-2 mg/ml; and/or
The polymer is selected from: at least one of polyethyleneimine, ethoxylated polyethyleneimine and poly [ (9,9-bis (3' - (N, N-dimethylamino) propyl) -2,7-fluorene) -2,7- (9, 9-dioctylfluorene ].
9. The method of claim 8, wherein the polymer solution comprises the polymer and an alcohol solvent.
10. The method of any one of claims 7 to 9, wherein the step of preparing a second functional layer on the polymer modification layer comprises:
providing a second functional material solution, and depositing the second functional material solution on the polymer modification layer through a solution processing method to prepare a second functional layer;
wherein the solvent in the second functional material solution is the same as the solvent in the polymer solution.
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