CN112786799A - Inverted light emitting device, manufacturing method thereof, display device and solid-state lighting device - Google Patents
Inverted light emitting device, manufacturing method thereof, display device and solid-state lighting device Download PDFInfo
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- H10K71/00—Manufacture or treatment specially adapted for the organic devices covered by this subclass
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- H10K71/12—Deposition of organic active material using liquid deposition, e.g. spin coating
- H10K71/13—Deposition of organic active material using liquid deposition, e.g. spin coating using printing techniques, e.g. ink-jet printing or screen printing
- H10K71/135—Deposition of organic active material using liquid deposition, e.g. spin coating using printing techniques, e.g. ink-jet printing or screen printing using ink-jet printing
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- 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
- H10K50/165—Electron transporting layers comprising dopants
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- H10K50/00—Organic light-emitting devices
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- H10K50/166—Electron transporting layers comprising a multilayered structure
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Abstract
The invention discloses an inverted light-emitting device and a preparation method thereof, a display device and a solid-state lighting device, wherein the inverted light-emitting device comprises a cathode, an electron transport layer and a light-emitting layer which are sequentially arranged, the electron transport layer comprises a first structural layer and a second structural layer which are arranged in a stacked mode, the first structural layer is arranged close to the cathode, the second structural layer is arranged close to the light-emitting layer, the first structural layer comprises a first electron transport material, the second structural layer comprises a second electron transport material and a semiconductor two-dimensional material, and energy bands of the semiconductor two-dimensional material and the second electron transport material are in interactive matching and are loaded on the surface of the second electron transport material. The novel electronic transmission layer structure provided by the invention improves the problem of unbalanced current carriers of the device, and improves the stability and the service life of the device.
Description
Technical Field
The invention relates to the technical field of display devices, in particular to the technical field of light-emitting devices, and specifically relates to an inverted light-emitting device and a preparation method thereof, a display device and a solid-state lighting device.
Background
The light emitting device generally comprises an upright device and an inverted device, wherein the inverted device only needs to prepare an electron transport layer and a light emitting layer on an ITO (indium tin oxide) cathode, and other hole transport layers, hole injection layers, anode layers and the like can be prepared under mature evaporation conditions, so that the preparation process of the inverted device is simpler and more convenient, and the inverted device has great commercial prospect. However, in the electron transport layer of the conventional inverted light emitting device, due to the defects of the electron transport material, carriers are easily trapped by the defects, the carrier transport of the device is affected, carrier injection is unbalanced, and excessive holes or electrons cause side reactions to the carrier transport, so that the stability and the service life of the device are affected.
Disclosure of Invention
The invention mainly aims to provide an inverted light-emitting device, a preparation method thereof, a display device and a solid-state lighting device, aiming at solving the problem of unbalanced current carriers in the light-emitting device so as to improve the stability and the service life of the device.
In order to achieve the above object, the present invention provides an inverted light emitting device, which includes a cathode, an electron transport layer, and a light emitting layer sequentially disposed, where the electron transport layer includes a first structural layer and a second structural layer disposed in a stacked manner, the first structural layer is disposed near the cathode, and the second structural layer is disposed near the light emitting layer, where a material of the first structural layer includes a first electron transport material, a material of the second structural layer includes a second electron transport material and a semiconductor two-dimensional material, and energy bands of the semiconductor two-dimensional material and the second electron transport material are interactively matched and loaded on a surface of the second electron transport material.
Optionally, the first electron transport material comprises titanium oxide and the second electron transport material comprises zinc oxide; and/or the presence of a gas in the gas,
the semiconductor two-dimensional material comprises any one of carbon nitride, boron nitride, molybdenum carbide and black phosphorus; and/or the presence of a gas in the gas,
optionally, the titanium oxide is titanium oxide particles with a truncated octahedral crystal phase, and the zinc oxide is zinc oxide nano rods with the length-diameter ratio of 1000-3000; and/or the presence of a gas in the gas,
the semiconductor two-dimensional material comprises carbon nitride.
Optionally, the mass of the semiconductor two-dimensional material is 5-10% of the mass of the second electron transport material; and/or the presence of a gas in the gas,
the thickness of the first structural layer is 5-10 nm; and/or the presence of a gas in the gas,
the total thickness of the first structural layer and the second structural layer is 30-150 nm.
Optionally, the inverted light emitting device is a quantum dot light emitting diode.
The invention also provides a preparation method of the inverted light-emitting device, which comprises the following steps:
preparing a first electron transport material into a film to form a first structural layer;
and arranging a second electron transmission material on the first structural layer, and loading a semiconductor two-dimensional material on the second electron transmission material to form a second structural layer which is arranged in a laminating manner with the first structural layer, so as to obtain the electron transmission layer.
Optionally, the step of disposing a second electron transport material on the first structural layer and loading a semiconductor two-dimensional material on the second electron transport material to form a second structural layer disposed in a stacked manner with the first structural layer to obtain the electron transport layer includes:
preparing a zinc oxide nanorod with the length-diameter ratio of 1000-3000 nm on the first structural layer through an electrochemical reaction;
and depositing a semiconductor two-dimensional material on the zinc oxide nano rod by using a thermal polycondensation mode to form a second structural layer which is stacked with the first structural layer, so as to prepare the electron transmission layer.
Optionally, the step of depositing a semiconductor two-dimensional material on the zinc oxide nanorods by thermal condensation to form a second structural layer stacked on the first structural layer to obtain an electron transport layer includes:
the heating rate of the thermal polycondensation is 4-6 ℃, the polycondensation reaction temperature is 500-600 ℃, and the reaction time is 20-40 min.
The present invention also proposes a display apparatus comprising an inverted light emitting device as described above or an inverted light emitting device made by the method as described above.
The present invention also proposes a solid state lighting apparatus comprising an inverted light emitting device as described above or made by a method as described above.
In the technical scheme provided by the invention, by designing the electron transmission layer in the inverted light-emitting device into two layers, two different electron transport materials with energy bands which are mutually matched are selected as main raw materials, namely a first electron transport material and a second electron transport material, and a semiconductor two-dimensional material is loaded on the surface of the second electron transport material, correspondingly preparing a first structural layer and a second structural layer, the second structural layer is arranged close to the light-emitting layer of the inverted light-emitting device, the first structural layer is arranged close to the cathode of the inverted device, and thus, through the matching of the first electron transmission material and the second electron transmission material and the mode of loading the semiconductor two-dimensional material on the second electron transmission material, the transmission of current carriers is improved, the current carrier balance of a device can be promoted, and the stability and the service life of the device are improved.
Drawings
In order to more clearly illustrate the embodiments of the present invention or the technical solutions in the prior art, the drawings used in the description of the embodiments or the prior art will be briefly described below, it is obvious that the drawings in the following description are only some embodiments of the present invention, and for those skilled in the art, other related drawings can be obtained according to the drawings without creative efforts.
Fig. 1 is a schematic structural diagram of an inverted light emitting device according to an embodiment of the present invention.
The reference numbers illustrate:
| 100 | resulting in a |
40 | |
| 10 | |
50 | |
| 20 | |
60 | |
| 30 | |
70 | |
| 31 | First |
80 | |
| 32 | The second structural layer |
The implementation, functional features and advantages of the objects of the present invention will be further explained with reference to the accompanying drawings.
Detailed Description
In order to make the objects, technical solutions and advantages of the embodiments of the present invention clearer, the technical solutions in the embodiments of the present invention will be clearly and completely described below. The examples, in which specific conditions are not specified, were conducted under conventional conditions or conditions recommended by the manufacturer. The reagents or instruments used are not indicated by the manufacturer, and are all conventional products available commercially. In addition, the meaning of "and/or" appearing throughout includes three juxtapositions, exemplified by "A and/or B" including either A or B or both A and B. In addition, technical solutions between various embodiments may be combined with each other, but must be realized by a person skilled in the art, and when the technical solutions are contradictory or cannot be realized, such a combination should not be considered to exist, and is not within the protection scope of the present invention. All other embodiments, which can be derived by a person skilled in the art from the embodiments given herein without making any creative effort, shall fall within the protection scope of the present invention.
The electronic transmission layer of the traditional inverted light-emitting device has some defects due to the existence of electronic transmission materials, so that current carriers are easily captured by the defects, the current carrier transmission of the device is influenced, the current carrier injection is unbalanced, excessive holes or electrons can cause side reactions to the current carrier transmission, and the stability and the service life of the device are influenced. In view of this, the present invention provides an inverted light emitting device, in which an electron transport layer is improved to improve the problem of carrier imbalance in the device, and fig. 1 is a specific embodiment of the inverted light emitting device provided in the present invention.
Referring to fig. 1, in an embodiment of the inverted light emitting device provided by the present invention, the inverted light emitting device 100 includes a substrate 10, a cathode 20, an electron transport layer 30, a light emitting layer 40, a hole transport layer 50, a hole injection layer 60, an anode 70, and an encapsulation layer 80, which are sequentially disposed, the electron transport layer 30 includes a first structural layer 31 and a second structural layer 32 disposed in a stacked manner, the second structural layer 32 is disposed adjacent to the light emitting layer 40, and the first structural layer 31 is disposed adjacent to the cathode 20, since the invention of the present invention mainly focuses on the improvement of the electron transport layer 30 in the device, a detailed description will be given below on a specific scheme of the electron transport layer 30.
The material of the first structural layer 31 comprises a first electron transport material, the material of the second structural layer 32 comprises a second electron transport material and a semiconductor two-dimensional material, the energy band of the semiconductor two-dimensional material is matched with the energy band of the second electron transport material, the semiconductor two-dimensional material is loaded on the surface of the second electron transport material, and further preferably, the band gap widths of the first electron transport material and the second electron transport material are-3.0-7.7 eV.
In the solution provided by the present invention, by designing the electron transport layer 30 in the inverted light emitting device 100 into two layers, two different electron transport materials with energy bands which are mutually matched are selected as main raw materials, namely a first electron transport material and a second electron transport material, and a semiconductor two-dimensional material is loaded on the surface of the second electron transport material, correspondingly prepared as a first structural layer 31 and a second structural layer 32, the second structural layer 32 is disposed adjacent to the light-emitting layer 40 of the inverted light-emitting device 100, the first structural layer 31 is disposed adjacent to the cathode 20 of the inverted device, and thus, through the matching of the first electron transmission material and the second electron transmission material and the mode of loading the semiconductor two-dimensional material on the second electron transmission material, the transmission of current carriers is improved, the current carrier balance of a device can be promoted, and the stability and the service life of the device are improved.
The inverted light emitting device 100 includes but is not limited to an Organic Light Emitting Diode (OLED) or a quantum dot light emitting diode (QLED), preferably, a QLED, that is, the light emitting layer 40 in the inverted light emitting device 100 is a quantum dot light emitting layer prepared by using a quantum dot material, and the quantum dot material is used as the light emitting layer material in the inverted light emitting device 100, so that the inverted light emitting device has the advantages of high color purity, high light emitting efficiency, adjustable light emitting color, good device stability and the like, and the QLED has a wide application prospect in the fields of display devices, solid state lighting and the like.
The specific substances of the first electron transport material and the second electron transport material are not limited, and any two different electron transport materials with band gap widths ranging from-3.0 to-7.7 eV can be selected for matching. The zinc oxide is a commonly used electron transport material in the field, has the advantages of high electron transport efficiency, good stability, convenient preparation and the like, and is used as the second electron transport material, so that the device performance of the inverted light-emitting device 100 is ensured. The cathode in the inverted light emitting device 100 is usually an ITO thin film, titanium oxide having a band gap width and an energy band position similar to zinc oxide is selected as the first electron transport material, and the prepared first structural layer 31 can be used for modifying an ITO electrode layer and extracting electrons of the ITO electrode layer, so that defects and roughness of an interface between the electron transport layer 30 and the ITO electrode are reduced, meanwhile, a contact area between the electron transport layer 30 and the ITO electrode interface is increased, resistance of electron transport is reduced, injection and transport of electrons are improved, the problem that the ITO thin film is difficult to extract and inject into an electron injection layer when being used as the cathode due to an extremely high work function is solved, the problem of carrier imbalance is further improved, and stability and service life of the device are further improved.
Further, in the embodiment of the present invention, the titanium oxide is preferably titanium oxide particles of a truncated octahedral crystal phase, which has a large specific surface area, and since the crystal plane contacts are all plane contacts, the contact resistance and the crystal plane voids are reduced, and the titanium oxide particles are suitable for carrier extraction. In addition, the zinc oxide is preferably a zinc oxide nanorod with an aspect ratio of 1000 to 3000, and the zinc oxide nanorod can be grown on the first structural layer 31 by an electrochemical reaction, and a specific preparation process is described in detail below with reference to specific examples. And a zinc oxide nano rod with the length-diameter ratio of 1000-3000 is selected as the second electron transmission material, so that the electron transmission is improved, the load of the semiconductor two-dimensional material is facilitated, and the transmission of current carriers and electrons is further improved.
After the semiconductor two-dimensional material is loaded on the surface of the second electron transport material, the carrier transport is improved, and meanwhile, a semiconductor heterojunction is generated, so that the recombination of holes and electrons at the interface of the electron transport layer 30 can be controlled, and the problem of carrier imbalance is solved. The second semiconductorThe specific substance of the dimension material is not limited as long as the energy band interaction matching of the semiconductor two-dimensional material and the second electron transport material is satisfied, and the semiconductor two-dimensional material is loaded on the surface of the second electron transport material and then fills the surface defects of the second electron transport material, so that the electron transport is facilitated, the recombination of holes, electrons and carriers is inhibited, and the formation of non-radiative recombination is reduced. In the specific embodiment provided by the present invention, the semiconductor two-dimensional material includes, but is not limited to, any one of carbon nitride, boron nitride, molybdenum carbide and black phosphorus, and is preferably carbon nitride. Carbon nitride (C)3N4) The semiconductor heterojunction can be formed by interaction of a conduction band of 1.57eV, a valence band of-1.12 eV and an energy band of 3.1eV of zinc oxide, and carrier recombination is inhibited.
Furthermore, the loading amount of the semiconductor two-dimensional material is preferably 5-10 wt%, that is, the mass of the semiconductor two-dimensional material is 5-10% of the mass of the second electron transport material. In the load range, the load of the semiconductor two-dimensional material is proper, the surface defects of the zinc oxide nano rod can be well filled, and the problems that the load of the semiconductor two-dimensional material is too low or too high, the improvement effect on carrier transmission is not good and the like can be solved.
The thicknesses of the first structural layer 31 and the second structural layer 32 are not limited, and may be set according to actual production requirements, and the total thickness of the electron transport layer 30 is usually set to be 30 to 150nm, that is, the total thickness of the first structural layer 31 and the second structural layer 32 is 30 to 150 nm. The thickness of the first structure layer 31 is preferably set to be 5-10 nm, which can promote sufficient contact between the electron transport layer 30 and an electrode interface, improve extraction and transport of electrons, promote carrier balance, and finally improve stability and lifetime of the device.
In addition, besides the electron transport layer 30, the material selection, thickness setting, and preparation process of other layer structures of the inverted light emitting device 100 may be conventional in the art, and the following specifically provides some material choices: the cathode 20 includes but is not limited toAn ITO thin film; the light-emitting layer 40 is a quantum dot light-emitting layer prepared from quantum dot materials, and the quantum dot materials include but are not limited to core-shell quantum dots such as CdSe/ZnS, CdS/ZnSe, CdSn/ZnSe and the like or quantum dot materials based on a gradient shell; the hole transport material of the hole transport layer 50 includes at least one of an organic transport material including, but not limited to, at least one of poly-TPD and TFB, and an inorganic transport material including, but not limited to, NiO and MoO3At least one of (a); materials of the hole injection layer 60 include, but are not limited to, PEDOT and MoO3At least one of; the anode 70 may be Ag or Al.
Based on the above-mentioned inverted light emitting device 100, the present invention also provides a method for manufacturing the inverted light emitting device 100, and since the improvement of the inverted light emitting device 100 of the present invention is mainly focused on the electron transport layer 30, the detailed description is first provided for the preparation of the electron transport layer 30. Specifically, the method for manufacturing the inverted light emitting device 100 includes the steps of:
step S10, preparing the first electron transport material into a thin film to form a first structural layer 31;
the light emitting device provided by the present invention is an inverted device, so the first structural layer is directly prepared on the cathode 20 of the inverted light emitting device 100, and specifically includes: the titanium oxide with the truncated octahedral crystalline phase is configured into ink, and a titanium oxide film is prepared on the cathode 20 by adopting an ink-jet printing mode, so that the first structural layer 31 is prepared. In addition, before the titanium oxide with the truncated octahedral crystalline phase is configured into ink, the titanium oxide with the truncated octahedral crystalline phase can be prepared by self, and the specific preparation steps comprise: dissolving titanate as a water-soluble titanium precursor, dissolving titanate in deionized water, adding 0.2mol of ammonium fluoride, stirring for 5-10 min, and in the process, adsorbing F atoms in the ammonium fluoride on a titanium oxide crystal face to reduce the surface energy of the top crystal face; and then transferring the stirred solution into a polytetrafluoroethylene container, reacting for 24 hours at 200 ℃, and finally separating solid matters in a reaction product by a solid-liquid separation mode such as centrifugation, so as to obtain the titanium oxide with the truncated octahedral crystalline phase.
Step S20 is to provide a second electron transport material on the first structure layer 31, and to load a semiconductor two-dimensional material on the second electron transport material, thereby forming a second structure layer 32 laminated with the first structure layer 31, and obtaining the electron transport layer 30.
After the first structural layer 31 is prepared, the second structural layer 32 is prepared on the basis of the first structural layer 31, and thus the preparation of the electron transport layer 30 can be completed. Specifically, in this embodiment, the preparation process of the second structural layer 32 includes:
step S21, preparing a zinc oxide nanorod with the length-diameter ratio of 1000-3000 nm on the first structural layer 31 through electrochemical reaction;
step S22, depositing a semiconductor two-dimensional material on the zinc oxide nanorods by thermal condensation to form a second structure layer 32 stacked on the first structure layer 31, thereby obtaining the electron transport layer 30.
The zinc oxide nano rod is prepared by adopting an electrochemical reaction mode, a zinc oxide film layer is more uniform, and the transmission of electrons can be improved, and specifically, the method for preparing the zinc oxide nano rod by adopting the electrochemical reaction comprises the following steps: and placing the substrate with the first structural layer 31 in an electrolyte, wherein the electrolyte contains 5mmol of zinc oxide and 0.1mol of HCl, reacting for 1000-3000 s at a voltage of 1V and a temperature of 60-85 ℃, ensuring that the length-diameter ratio of the zinc oxide grows to 1000-3000, taking out the substrate, and washing to obtain the zinc oxide nanorod.
Then, a semiconductor two-dimensional material is deposited on the zinc oxide nano-rods by means of thermal polycondensation, for example, the semiconductor two-dimensional material is carbon nitride (C)3N4) In the process, melamine can be used as a raw material, and C is loaded on the zinc oxide nano rod through thermal polycondensation reaction3N4When the semiconductor two-dimensional material is boron nitride, BCl2 can be selected as a raw material, and BN is loaded on the zinc oxide nano-rod through a thermal polycondensation reaction. Specifically, the thermal polycondensation method comprises the following steps: will correspond toThe raw material is placed on a first structural layer 31 on which the zinc oxide nanorod grows, then the temperature is heated to 500-600 ℃ in a microwave heating mode at a heating rate of 4-6 ℃/min, and the temperature is kept for 20-40 min, so that the zinc oxide nanorod loaded with the corresponding semiconductor two-dimensional material is obtained, namely, a second structural layer 32 which is stacked with the first structural layer 31 is formed, and the electronic transmission layer 30 is prepared.
In the preparation method of the inverted light-emitting device 100 provided by the invention, the electronic transmission layer 30 is prepared into the zinc oxide nanorod loaded with carbon nitride by using an electrochemical and microwave heating polycondensation mode during preparation, so that the electronic transmission is improved, heterojunction can be generated, and the recombination of current carriers in a non-light-emitting region is inhibited, and the inverted device with the structure of the electronic transmission layer 30 is more favorable for the injection and transmission of electrons, improves the balance of current carriers, and obviously improves the efficiency and the service life of the device. In addition, the preparation methods of the cathode 20, the light emitting layer 40, the hole transport layer 50, the hole injection layer 60, the anode 70 and the encapsulation layer 80 can refer to the prior art in the field, for example, the substrate 10 can be directly a glass substrate with an ITO thin film plated on the surface, the ITO thin film layer constitutes the cathode 20, the light emitting layer 40 can be prepared by ink jet printing or the like, the hole transport layer 50 and the hole injection layer 60 can be prepared by printing or evaporation, the anode 70 can be prepared by evaporation, and the evaporation speed is 0.1-0.3 nm/s. The fabrication method and structure of the inverted light emitting device 100 will be described in more detail with reference to specific embodiments.
The present invention further provides a display apparatus including, but not limited to, a computer, a television, a mobile phone, a flat panel display, etc., the display apparatus including the inverted light emitting device 100, and a specific structure or a manufacturing method of the inverted light emitting device 100 is described with reference to the above embodiments. It can be understood that, since the display device of the present invention adopts all the technical solutions of all the embodiments, at least all the beneficial effects brought by the technical solutions of the embodiments are achieved, and are not described in detail herein.
The present invention further provides a solid-state lighting apparatus including the inverted light emitting device 100, and the specific structure or manufacturing method of the inverted light emitting device 100 refers to the above embodiments. It can be understood that, since the solid-state lighting device of the present invention adopts all the technical solutions of all the embodiments, at least all the advantages brought by the technical solutions of the embodiments are provided, and no further description is provided herein.
The technical solutions of the present invention are further described in detail below with reference to specific examples and drawings, it should be understood that the following examples are merely illustrative of the present invention and are not intended to limit the present invention.
Example 1
(1) The structure of the inverted light-emitting device comprises a substrate, ITO (15nm), Ag (140nm) + ITO (15nm), titanium oxide (5nm) + load C which are sequentially stacked3N4The zinc oxide nano rod (50nm), the quantum dot luminescent layer (20nm), the poly-TPD (30nm), the PEDOT (20nm), the Ag (20nm) and the packaging layer (100 nm).
(2) The preparation method of the inverted light-emitting device comprises the following steps:
cleaning and drying an ITO substrate according to a standard method, preparing titanium oxide particles with the octahedral crystalline phase removed into 5mg/mL ink, printing 8 drops of the ink to deposit on the ITO substrate, and drying the ink to form a film to form a titanium oxide film; then placing the substrate with the titanium oxide film in a container filled with electrolyte (the electrolyte contains 5mmol of zinc oxide and 0.1mol of HCl), adding 1V of voltage, and reacting for 1000s at 85 ℃ to obtain a zinc oxide nanorod with the length-diameter ratio of 1000; then 0.3mg of melamine is added on the zinc oxide nano rod, the microwave is used for heating to 500 ℃ at the heating rate of 5 ℃/min, and the reaction is carried out for 30min to obtain the load C3N4Preparing an electron transport layer by using the zinc oxide nano rod (the load is 8%); and then, sequentially preparing functional layers with corresponding thicknesses on the electron transmission layer by adopting methods such as printing or evaporation and the like to prepare the inverted light-emitting device.
Example 2
(1) The structure of the inverted light-emitting device comprises a substrate, ITO (20nm), titanium oxide (10nm) and a load C which are sequentially stacked3N4The zinc oxide nano rod (50nm), the quantum dot luminescent layer (20nm), the poly-TPD (30nm), the PEDOT (20nm), the Ag (70nm) and the packaging layer (100 nm).
(2) The preparation method of the inverted light-emitting device comprises the following steps:
cleaning and drying an ITO substrate according to a standard method, preparing the titanium oxide particles with the octahedral crystalline phase removed into 5mg/mL ink, printing 16 drops of the ink to deposit on the ITO substrate, and drying the ink to form a film to form a titanium oxide film; then placing the substrate with the titanium oxide film in a container filled with electrolyte (the electrolyte contains 5mmol of zinc oxide and 0.1mol of HCl), adding 1V of voltage, and reacting for 1000s at 85 ℃ to obtain a zinc oxide nanorod with the length-diameter ratio of 1000; then 0.2mg of melamine is added on the zinc oxide nano rod, microwave heating is carried out at the heating rate of 5 ℃/min until the temperature reaches 500 ℃, and reaction is carried out for 30min to obtain the load C3N4Preparing the zinc oxide nano rod (the load is 6%) to obtain an electron transport layer; and then, sequentially preparing functional layers with corresponding thicknesses on the electron transmission layer by adopting methods such as printing or evaporation and the like to prepare the inverted light-emitting device.
Example 3
(1) The structure of the inverted light-emitting device comprises a substrate, ITO (15nm), Ag (140nm) + ITO (15nm), titanium oxide (10nm) + load C which are sequentially stacked3N4The zinc oxide nano rod (50nm), the quantum dot luminescent layer (20nm), the poly-TPD (30nm), the PEDOT (20nm), the Ag (20nm) and the packaging layer (100 nm).
(2) The preparation method of the inverted light-emitting device comprises the following steps:
cleaning and drying an ITO substrate according to a standard method, preparing the titanium oxide particles with the octahedral crystalline phase removed into 5mg/mL ink, printing 16 drops of the ink to deposit on the ITO substrate, and drying the ink to form a film to form a titanium oxide film; then placing the substrate with the titanium oxide film in a container filled with electrolyte (the electrolyte contains 5mmol of zinc oxide and 0.1mol of HCl), adding 1V of voltage, and reacting for 3000s at 85 ℃ to obtain a zinc oxide nano rod with the length-diameter ratio of 3000; then 0.2mg of BCl is added on the zinc oxide nano-rod2Microwave heating to 600 deg.C at a heating rate of 5 deg.C/min in ammonia atmosphere,reacting for 30min to obtain a BN-loaded zinc oxide nano rod (the load is 6%), and preparing an electron transport layer; and then, sequentially preparing functional layers with corresponding thicknesses on the electron transmission layer by adopting methods such as printing or evaporation and the like to prepare the inverted light-emitting device.
Example 4
(1) The structure of the inverted light-emitting device comprises a substrate, ITO (20nm), titanium oxide (8nm) and a load C which are sequentially stacked3N4The zinc oxide nano rod (50nm), the quantum dot luminescent layer (20nm), the poly-TPD (30nm), the PEDOT (20nm), the Ag (70nm) and the packaging layer (100 nm).
(2) The preparation method of the inverted light-emitting device comprises the following steps:
cleaning and drying an ITO substrate according to a standard method, preparing titanium oxide particles with the octahedral crystalline phase removed into 5mg/mL ink, printing 13 drops of the ink to deposit on the ITO substrate, and drying the ink to form a film to form a titanium oxide film; then placing the substrate with the titanium oxide film in a container filled with electrolyte (the electrolyte contains 5mmol of zinc oxide and 0.1mol of HCl), adding 1V of voltage, and reacting at 70 ℃ for 2000s to obtain a zinc oxide nanorod with the length-diameter ratio of 2000; then 0.4mg of melamine is added on the zinc oxide nano rod, microwave heating is carried out at the heating rate of 5 ℃/min until the temperature reaches 500 ℃, and reaction is carried out for 30min to obtain the load C3N4Preparing the zinc oxide nano rod (the load is 10%) to obtain an electron transport layer; and then, sequentially preparing functional layers with corresponding thicknesses on the electron transmission layer by adopting methods such as printing or evaporation and the like to prepare the inverted light-emitting device.
Example 5
(1) The structure of the inverted light-emitting device comprises a substrate, ITO (20nm), titanium oxide (10nm) and a load C which are sequentially stacked3N4The zinc oxide nano rod (140nm), the quantum dot luminescent layer (20nm), the poly-TPD (30nm), the PEDOT (20nm), the Ag (70nm) and the packaging layer (100 nm).
(2) The preparation method of the inverted light-emitting device comprises the following steps:
cleaning and drying an ITO substrate according to a standard method, preparing the titanium oxide particles with the octahedral crystal phase removed into 5mg/mL ink, and printing 16 drops of the ink to be deposited on the ITO substrateDrying the substrate to form a film and form a titanium oxide film; then placing the substrate with the titanium oxide film in a container filled with electrolyte (the electrolyte contains 5mmol of zinc oxide and 0.1mol of HCl), adding 1V of voltage, and reacting for 1000s at 75 ℃ to obtain a zinc oxide nanorod with the length-diameter ratio of 1000; then 0.2mg of melamine is added on the zinc oxide nano rod, microwave heating is carried out at the heating rate of 4 ℃/min until the temperature reaches 550 ℃, and the reaction is carried out for 20min to obtain the load C3N4Preparing the zinc oxide nano rod (the load is 6%) to obtain an electron transport layer; and then, sequentially preparing functional layers with corresponding thicknesses on the electron transmission layer by adopting methods such as printing or evaporation and the like to prepare the inverted light-emitting device.
Example 6
(1) The structure of the inverted light-emitting device comprises a substrate, ITO (20nm), titanium oxide (5nm) and a load C which are sequentially stacked3N4The zinc oxide nano rod (25nm), the quantum dot luminescent layer (20nm), the poly-TPD (30nm), the PEDOT (20nm), the Ag (70nm) and the packaging layer (100 nm).
(2) The preparation method of the inverted light-emitting device comprises the following steps:
cleaning and drying an ITO substrate according to a standard method, preparing titanium oxide particles with the octahedral crystalline phase removed into 5mg/mL ink, printing 8 drops of the ink to deposit on the ITO substrate, and drying the ink to form a film to form a titanium oxide film; then placing the substrate with the titanium oxide film in a container filled with electrolyte (the electrolyte contains 5mmol of zinc oxide and 0.1mol of HCl), adding 1V of voltage, and reacting for 1000s at 65 ℃ to obtain a zinc oxide nanorod with the length-diameter ratio of 1000; then 0.15mg of melamine is added on the zinc oxide nano rod, microwave heating is carried out at the heating rate of 6 ℃/min until the temperature reaches 500 ℃, and reaction is carried out for 40min to obtain the load C3N4Preparing an electron transport layer from the zinc oxide nanorod (the load is 5%); and then, sequentially preparing functional layers with corresponding thicknesses on the electron transmission layer by adopting methods such as printing or evaporation and the like to prepare the inverted light-emitting device.
Comparative example 1
The structure of the inverted light emitting device was the same as in example 1, except that the electron transport layer was a zinc oxide film, which was prepared by printing or evaporation.
The inverted light emitting devices prepared in the above-described examples and comparative examples were tested for performance, and the test results are shown in table 1 below.
TABLE 1
As can be seen from comparison between the embodiments in table 1 and the comparative examples, the efficiency of the inverted light emitting device prepared in the embodiments of the present invention is significantly improved due to the double-layer structure of the novel electron transport layer provided in the present invention, which is because electrons are more easily injected and transported and carriers are more easily recombined in the light emitting region due to the double-layer structure of the electron transport layer provided in the present invention, so that the light emitting efficiency of the device is improved, the light emitting efficiency is improved, and the lifetime of the device can also be improved.
The above is only a preferred embodiment of the present invention, and it is not intended to limit the scope of the invention, and various modifications and changes will occur to those skilled in the art. Any modification, equivalent replacement, or improvement made within the spirit and principle of the present invention shall be included in the scope of the present invention.
Claims (10)
1. The utility model provides an inverted light-emitting device, its characterized in that, is including the negative pole, electron transport layer and the luminescent layer that set gradually, electron transport layer is including being range upon range of first structural layer and the second structural layer that sets up, first structural layer is close to the negative pole sets up, the second structural layer is close to the luminescent layer sets up, wherein, the material of first structural layer includes first electron transport material, the material of second structural layer includes second electron transport material and semiconductor two-dimensional material, semiconductor two-dimensional material with the mutual matching of energy band of second electron transport material and load in the surface of second electron transport material.
2. The inverted light emitting device of claim 1, wherein the first electron transport material comprises titanium oxide, the second electron transport material comprises zinc oxide; and/or the presence of a gas in the gas,
the semiconductor two-dimensional material comprises any one of carbon nitride, boron nitride, molybdenum carbide and black phosphorus.
3. The inverted light emitting device according to claim 2, wherein the titanium oxide is titanium oxide particles of a truncated octahedral crystalline phase, and the zinc oxide is zinc oxide nanorods having an aspect ratio of 1000 to 3000; and/or the presence of a gas in the gas,
the semiconductor two-dimensional material comprises carbon nitride.
4. The inverted light emitting device of claim 1, wherein the mass of the semiconductor two-dimensional material is 5-10% of the mass of the second electron transporting material; and/or the presence of a gas in the gas,
the thickness of the first structural layer is 5-10 nm; and/or the presence of a gas in the gas,
the total thickness of the first structural layer and the second structural layer is 30-150 nm.
5. The inverted light emitting device of claim 1, wherein the inverted light emitting device is a quantum dot light emitting diode.
6. A method for preparing an inverted light emitting device is characterized by comprising the following steps:
preparing a first electron transport material into a film to form a first structural layer;
and arranging a second electron transmission material on the first structural layer, and loading a semiconductor two-dimensional material on the second electron transmission material to form a second structural layer which is arranged in a laminating manner with the first structural layer, so as to obtain the electron transmission layer.
7. The method of manufacturing an inverted light emitting device according to claim 6, wherein the step of forming a second structural layer disposed to be laminated with the first structural layer by disposing a second electron transporting material on the first structural layer and supporting a semiconductor two-dimensional material on the second electron transporting material to obtain the electron transporting layer comprises:
preparing a zinc oxide nanorod with the length-diameter ratio of 1000-3000 nm on the first structural layer through an electrochemical reaction;
and depositing a semiconductor two-dimensional material on the zinc oxide nano rod by using a thermal polycondensation mode to form a second structural layer which is stacked with the first structural layer, so as to prepare the electron transmission layer.
8. The method for preparing an inverted light emitting device according to claim 7, wherein the step of depositing a semiconductor two-dimensional material on the zinc oxide nanorods by thermal condensation to form a second structure layer stacked on the first structure layer to obtain an electron transport layer comprises:
the heating rate of the thermal polycondensation is 4-6 ℃, the polycondensation reaction temperature is 500-600 ℃, and the reaction time is 20-40 min.
9. A display device comprising the inverted light emitting device according to any one of claims 1 to 5 or the inverted light emitting device produced by the method according to any one of claims 6 to 8.
10. A solid state lighting device comprising the inverted light emitting device of any of claims 1 to 5 or made by the method of any of claims 6 to 8.
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