WO2023051538A1 - 量子点发光二极管器件及其制备方法与显示面板 - Google Patents

量子点发光二极管器件及其制备方法与显示面板 Download PDF

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WO2023051538A1
WO2023051538A1 PCT/CN2022/121786 CN2022121786W WO2023051538A1 WO 2023051538 A1 WO2023051538 A1 WO 2023051538A1 CN 2022121786 W CN2022121786 W CN 2022121786W WO 2023051538 A1 WO2023051538 A1 WO 2023051538A1
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layer
quantum dot
dot light
self
functional layer
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PCT/CN2022/121786
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French (fr)
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王劲
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Tcl科技集团股份有限公司
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Publication of WO2023051538A1 publication Critical patent/WO2023051538A1/zh

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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
    • H10K50/00—Organic light-emitting devices
    • H10K50/10—OLEDs or polymer light-emitting diodes [PLED]
    • H10K50/14—Carrier transporting layers
    • H10K50/15—Hole transporting layers
    • 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
    • H10K50/00—Organic light-emitting devices
    • H10K50/80—Constructional details
    • 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
    • H10K71/60—Forming conductive regions or layers, e.g. electrodes
    • H—ELECTRICITY
    • H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
    • H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
    • H10K85/00—Organic materials used in the body or electrodes of devices covered by this subclass
    • H10K85/40—Organosilicon compounds, e.g. TIPS pentacene
    • H—ELECTRICITY
    • H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
    • H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
    • H10K85/00—Organic materials used in the body or electrodes of devices covered by this subclass
    • H10K85/60—Organic compounds having low molecular weight
    • H10K85/611—Charge transfer complexes

Definitions

  • the present application relates to the field of display technology, in particular to a quantum dot light-emitting diode device, a preparation method thereof, and a display panel.
  • Quantum Dots Semiconductor quantum dots
  • QDs Semiconductor quantum dots
  • the electroluminescence device based on quantum dot technology - quantum dot light emitting diode (Quantumdot Light Emitting Diode, QLED), has the advantages of high stability, solution processability and high color saturation. Realize the leap from point light source to surface light source through self-illumination.
  • the QLED device is a "sandwich" thin film stack structure formed by two electrodes and various functional layers added between the electrodes and quantum dots. These functional layers include electron injection layer, electron transport layer, hole transport layer, Hole injection layer, etc., the film quality, interface bonding and material stability of each thin film layer will greatly affect the performance of the device. Most of the current QLED devices and related materials are prepared under low temperature conditions ( ⁇ 300°C), and the requirements for equipment are correspondingly reduced, which is conducive to simplifying the process and reducing costs.
  • the electron transport layer material prepared by the low temperature method it has many surface defects and low electron mobility, and it is prone to uneven film formation and pinholes during the film formation process.
  • Common organic hole transport materials are mainly biphenyls, poly/thiophenes, triarylamines, carbazoles, pyrazolines, butadiene, styrene, etc., which have poor environmental stability and are not resistant to high temperatures. , low hole mobility and other shortcomings.
  • the functional thin film layer and the quantum dot light-emitting layer will adhere to each other, but based on the material types and characteristics of organic hole transport materials, inorganic quantum dot materials, and inorganic electron transport materials, the difference between the functional thin film layer and the quantum dot light-emitting layer
  • the present application provides a quantum dot light-emitting diode device, a manufacturing method thereof, and a display panel, which can improve the bonding between the functional thin film layer and the quantum dot light-emitting layer.
  • the present application provides a quantum dot light-emitting diode device, including a first electrode, a hole functional layer, a quantum dot light-emitting layer, an electronic functional layer, and a second electrode that are sequentially stacked; the hole functional layer and A self-assembled molecular layer is provided between the quantum dot luminescent layer, or a self-assembled molecular layer is provided between the electronic functional layer and the quantum dot luminescent layer, or the hole functional layer and the quantum dot luminescent A self-assembled molecular layer is arranged between the layers, and a self-assembled molecular layer is arranged between the electronic functional layer and the quantum dot light-emitting layer.
  • the hole functional layer includes a hole injection layer and/or a hole transport layer;
  • the electron functional layer includes an electron injection layer and/or an electron transport layer.
  • the self-assembled molecular layer between the hole functional layer and the quantum dot light-emitting layer includes a compound of the general formula (R 1 ) 3 NR 2 X;
  • R 1 is methyl or ethyl, N is a positively charged quaternary nitrogen;
  • X is a halide anion or carboxylate;
  • R 2 is selected from hydrocarbon groups, containing aromatic One or more of hydroxyl group, mercapto group, ester, ether, amine, amide, phosphorus, phosphine or thioether hydrocarbon group, polyoxypropylene group, perfluoroalkyl group and polysiloxane group, R2 The number of carbon atoms is 4 to 20.
  • the R2 has van der Waals force or forms a hydrogen bond with the ligands of the quantum dots in the quantum dot light-emitting layer, or forms a coordination bond between the R2 and the quantum dots in the quantum dot light-emitting layer.
  • the compound represented by the general formula (R 1 ) 3 NR 2 X is selected from:
  • the self-assembled molecular layer between the hole functional layer and the quantum dot light-emitting layer includes compounds of the general formula R 3 -R 4 ;
  • R 3 is a phenol group or a catechol group
  • R 4 is selected from hydrocarbon groups, containing aryl, hydroxyl, mercapto, ester, ether, amine, amide, phosphorus, One or more of the hydrocarbon group of oxon or thioether, polyoxypropylene group, perfluoroalkyl group and polysiloxane group, and R4 has 4 to 20 carbon atoms.
  • the R3 forms a hydrogen bond with the surface of the hole functional layer, so that the self-assembled molecular layer is combined with the surface of the hole functional layer;
  • the compound with the structure represented by the general formula R 3 -R 4 is selected from:
  • the self-assembled molecular layer between the quantum dot light-emitting layer and the electronic functional layer includes compounds of the general formula R 5 -R 6 ;
  • R 5 is selected from one of amino, mercapto, carboxyl, hydroxyl, carbonyl, amido, phosphorus, oxonyl, organophosphorus, thioether and polysiloxane group or Multiple;
  • R 6 is selected from one or more of hydrocarbon groups, hydrocarbon groups containing aryl groups, ether groups, polyoxypropylene groups and perfluoroalkyl groups, and R 6 has 4 to 20 carbon atoms.
  • the R5 forms a coordination bond with the quantum dots of the quantum dot light-emitting layer, or the R5 forms a hydrogen bond with the surface ligands of the quantum dots of the quantum dot light-emitting layer, so that the The self-assembled molecular layer is combined with the surface of the quantum dot luminescent layer;
  • the R 6 has van der Waals force with the surface of the electronic functional layer, so that the self-assembled molecular layer is adsorbed on the surface of the electronic functional layer.
  • the compounds of the formulas R 5 -R 6 are selected from:
  • the self-assembled molecular layer has a thickness of 1-50 nm.
  • the functional layer includes a hole transport layer
  • the hole transport layer includes an organic hole transport material
  • the organic hole transport material includes biphenyls, poly/thiophenes, triarylamines, carba One or more of azoles, pyrazolines, butadienes and styrenes.
  • the functional layer includes an electron transport layer, and the electron transport layer includes inorganic nanoparticle materials; the inorganic nanoparticles include one or more of doped or non-doped metal oxides;
  • the doped or non-doped metal oxide includes one or more of ZnO, TiO 2 , SnO 2 , Ta 2 O 3 , ZrO 2 , TiLiO, ZnAlO, ZnMgO, ZnSnO, ZnLiO, InSnO .
  • the quantum dot light-emitting layer includes quantum dots; the quantum dots include one or more of II-VI group compounds and III-V group compounds; preferably, the quantum dots include CdS, CdSe, One or more of CdTe, ZnS, ZnSe, ZnTe, GaAs, GaP, GaSb, HgS, HgSe, HgTe, InAs, InP, InSb, AlAs, AlP, CuInS and CuInSe.
  • the present application provides a method for preparing a quantum dot light-emitting diode device, the preparation method comprising the following steps:
  • the preparation method comprises the steps of:
  • a self-assembled molecular layer is provided between the hole functional layer and the quantum dot light-emitting layer, or a self-assembled molecular layer is provided between the electronic functional layer and the quantum dot light-emitting layer, or the hole A self-assembled molecular layer is provided between the hole functional layer and the quantum dot light-emitting layer, and a self-assembled molecular layer is provided between the electronic functional layer and the quantum dot light-emitting layer.
  • the self-assembled molecular layer disposed between the hole functional layer and the quantum dot light-emitting layer includes compounds of the general formula R 3 -R 4 , where the general formula R 3 - In R 4 , R 3 is a phenol group or a catechol group; R 4 is selected from a hydrocarbon group, a hydrocarbon group containing an aryl group, a hydroxyl group, a mercapto group, an ester, an ether, an amine, an amide, phosphorus, phosphine or thioether, One or more of polyoxypropylene group, perfluoroalkyl group and polysiloxane group, R 4 has 4 to 20 carbon atoms.
  • R 5 is selected from one of amino, mercapto, carboxyl, hydroxyl, carbonyl, amido, phosphorus, oxonyl, organophosphorus, thioether and polysiloxane group or Multiple;
  • R 6 is selected from one or more of hydrocarbon groups, hydrocarbon groups containing aryl groups, ether groups, polyoxypropylene groups and perfluoroalkyl groups, and R 6 has 4 to 20 carbon atoms.
  • the present application provides a display panel.
  • the display panel includes a substrate and quantum dot light-emitting diode devices arranged on the surface of the substrate in the form of an array.
  • the quantum dot light-emitting diode devices include sequentially stacked first An electrode, a hole functional layer, a quantum dot luminescent layer, an electronic functional layer, and a second electrode; a self-assembled molecular layer is arranged between the hole functional layer and the quantum dot luminescent layer, or the electronic functional layer and the A self-assembled molecular layer is provided between the quantum dot light-emitting layer, or a self-assembled molecular layer is provided between the hole functional layer and the quantum dot light-emitting layer, and the electronic functional layer and the quantum dot light-emitting layer A self-assembled molecular layer is arranged between them.
  • the self-assembled molecular layer disposed between the hole functional layer and the quantum dot light-emitting layer includes compounds of the general formula R 3 -R 4 , where the general formula R 3 -R 4 Among them, R3 is a phenol group or a catechol group; R4 is selected from a hydrocarbon group, a hydrocarbon group containing an aryl group, a hydroxyl group, a mercapto group, an ester, an ether, an amine, an amide, phosphorus, phosphine or thioether, a polyoxygen group One or more of propenyl, perfluoroalkyl and polysiloxane, R 4 has 4 to 20 carbon atoms.
  • the self-assembled molecular layer disposed between the electronic functional layer and the quantum dot light-emitting layer includes compounds of the general formula R 5 -R 6 , in the general formula R 5 -R 6 , R 5 is selected from one or more of amino, mercapto, carboxyl, hydroxyl, carbonyl, amido, phosphorus, phosphine, organophosphorus, thioether and polysiloxane; R 6 is selected from hydrocarbon groups, containing aromatic One or more of hydrocarbon groups, ether groups, polyoxypropylene groups and perfluoroalkyl groups, and R6 has 4 to 20 carbon atoms.
  • the present invention provides a quantum dot light-emitting diode device (QLED).
  • QLED quantum dot light-emitting diode device
  • a self-assembled molecular layer is arranged between the functional layer and the quantum dot light-emitting layer, and the self-assembled molecular layer can effectively improve the hole function.
  • This application utilizes the interaction between the self-assembled molecular layer and the organic hole transport layer, the quantum dot light-emitting layer and the electron transport layer (such as van der Waals force, coordination bond and hydrogen bond, etc.), thereby effectively improving the stability of the upper film material in the process.
  • the problem of solvent erosion destroying the underlying film, as well as the degree of interfacial adhesion between the functional layer and the quantum dot light-emitting layer improves the mechanical reliability of the interface and improves the performance of organic hole transport materials, inorganic quantum dot materials and inorganic electron transport materials.
  • the problem of poor bonding between interfaces caused by differences in material types and characteristics.
  • FIG. 1 is a schematic structural diagram of a quantum dot light-emitting diode device provided in an embodiment of the present application
  • Fig. 2 is the structural schematic diagram II of the quantum dot light-emitting diode device provided by the embodiment of the present application;
  • FIG. 3 is a schematic structural diagram of a display panel provided by an embodiment of the present application.
  • Figure 4 is a schematic structural view of the quantum dot light-emitting diode device provided in Embodiment 1 and Embodiment 2 of the present application;
  • Fig. 5 is a schematic structural view of the quantum dot light-emitting diode device provided in Example 3 of the present application;
  • FIG. 6 is a schematic structural view of the quantum dot light-emitting diode device provided in Comparative Example 1 of the present application;
  • Fig. 7 is the current efficiency-current density characteristic curve figure in the application test example 1;
  • Fig. 8 is a schematic diagram of the fluorescent film structure in Test Example 2 of the present application.
  • Fig. 9 is the relative fluorescence intensity figure of the fluorescent film in the application test example 2.
  • Fig. 10 is the AFM figure in the application test example 2;
  • Figure 11 is a schematic diagram of the fluorescent film structure in Test Example 3 of the present application.
  • FIG. 12 is a diagram of the relative fluorescence intensity of the fluorescent film in Test Example 3 of the present application.
  • Embodiments of the present application provide a quantum dot light emitting diode device, a manufacturing method thereof, and a display panel. Each will be described in detail below. It should be noted that the description sequence of the following embodiments is not intended to limit the preferred sequence of the embodiments.
  • a description of a range from 1 to 6 should be considered to have specifically disclosed subranges, such as from 1 to 3, from 1 to 4, from 1 to 5, from 2 to 4, from 2 to 6, from 3 to 6, etc., and Single numbers within the stated ranges, eg 1, 2, 3, 4, 5 and 6, apply regardless of the range.
  • a numerical range is indicated herein, it is meant to include any cited numeral (fractional or integral) within the indicated range.
  • the term "and/or” is used to describe the relationship between associated objects, indicating that there may be three relationships, for example, "A and/or B" may indicate three situations: the first situation is that A exists alone ; The second case is the presence of A and B at the same time; the third case is the case of B alone, wherein A and B can be singular or plural respectively.
  • the term "at least one” means one or more, and “multiple” means two or more.
  • the terms “at least one”, “at least one of the following” or similar expressions refer to any combination of these items, including any combination of single or plural items.
  • “at least one (one) of a, b, or c” or “at least one (one) of a, b, and c” can be expressed as: a, b, c, a-b (that is, a and b ), a-c, b-c or a-b-c, wherein, a, b and c can be single or multiple respectively.
  • An embodiment of the present application provides a quantum dot light-emitting diode device, including a first electrode, a hole functional layer, a quantum dot light-emitting layer, an electronic functional layer, and a second electrode that are sequentially stacked; the hole functional layer and the quantum dot A self-assembled molecular layer is provided between the dot light-emitting layers and/or between the electronic functional layer and the quantum dot light-emitting layer. An interaction force can be generated between the self-assembled molecular layer and the hole functional layer and/or between the self-assembled molecular layer and the electronic functional layer to enhance the quantum dot light-emitting layer and the hole function layer.
  • the force is selected from one or more of van der Waals forces, coordination bonds and hydrogen bonds .
  • the self-assembled molecular layer may be a self-assembled monolayer (SAM), which is an ordered monomolecular film formed by spontaneous assembly of molecules with active groups on a solid surface.
  • SAM self-assembled monolayer
  • the hole functional layer includes a hole injection layer and/or a hole transport layer; the electron function layer includes an electron injection layer and/or an electron transport layer.
  • the quantum dot light-emitting diode device includes a first electrode, a hole transport layer, a quantum dot light-emitting layer, an electron transport layer and a second electrode that are sequentially stacked.
  • the quantum dot light emitting diode device includes a first electrode, a hole injection layer, a hole transport layer, a quantum dot light emitting layer, an electron transport layer, an electron injection layer and a second electrode which are stacked in sequence.
  • the self-assembled molecular layer is provided between the quantum dot light-emitting layer and the hole transport layer, and/or the self-assembled molecular layer is provided between the quantum dot light-emitting layer and the electron transport layer.
  • molecular layer is disposed between the quantum dot light-emitting layer and the hole transport layer, and/or the self-assembled molecular layer is disposed between the quantum dot light-emitting layer and the electron transport layer between.
  • the degree of adhesion between the hole transport layer and the quantum dot light-emitting layer and/or the electron transport layer and the quantum dot light-emitting layer can be effectively improved.
  • the degree of adhesion between the point-emitting layers improves the mechanical reliability of the interface.
  • the self-assembled molecular layer may have a thickness of 1-50 nm, for example, 1 nm, 3 nm, 5 nm, 10 nm, 15 nm, 20 nm, 25 nm, 30 nm, 35 nm, 40 nm, 45 nm or 50 nm.
  • the quantum dot light-emitting diode device 100 includes a hole transport layer 110, a quantum dot light-emitting layer 120 and an electron transport layer 130, and the hole transport layer 110 and the electron transport layer Layers 140 of self-assembled molecules are disposed between the layers 130 .
  • the self-assembled molecular layer 140 a is disposed between the hole transport layer 110 and the quantum dot light-emitting layer 120 .
  • the self-assembled molecular layer 140 b is disposed between the quantum dot light emitting layer 120 and the electron transport layer 130 .
  • the self-assembled molecular layer 140a is disposed between the hole transport layer 110 and the quantum dot light-emitting layer 120, and at the same time, the quantum dot light-emitting layer 120 is disposed between the electron transport layer 130 There is said self-assembled molecular layer 140b.
  • the self-assembled molecular layer has force with the hole transport layer and the electron transport layer respectively.
  • the material of the self-assembled molecular layer may be (R 1 ) 3 NR 2 X, R 3 -R 4 , R 5 -R 6 ; the applicant may select the material according to the specific position of the self-assembled molecular layer.
  • the selection of the self-assembled molecular layer can refer to the following.
  • the self-assembled molecular layer between the hole transport layer and the quantum dot light-emitting layer includes a structure represented by the general formula (R 1 ) 3 NR 2 X, wherein,
  • R 1 is methyl or ethyl, (R 1 ) 3 is three R 1 groups;
  • N is positively charged tetravalent nitrogen
  • X is a halide anion (F - , Cl - , Br - , I - ) or carboxylate (RCOO - ), wherein R in RCOO - is a hydrocarbon group;
  • R2 is selected from but not limited to hydrocarbon groups, hydrocarbon groups containing aryl groups, hydroxyl groups, mercapto groups, esters, ethers, amines (primary amines, secondary amines, tertiary amines), amides, phosphorus, phosphine, thioether, etc.
  • the order of the binding ability of the two is: coordination bond>hydrogen bond>van der Waals force.
  • the self-assembled molecular layer is electrostatically adsorbed on the surface of the hole transport layer by using positively charged quaternary nitrogen and unsaturated bonds (such as benzene rings, carbon-carbon double bonds) in the hole transport layer.
  • the self-assembled molecular layer is bound to the surface of the quantum dot luminescent layer through van der Waals force, coordination bond with quantum dots, or hydrogen bond with quantum dot surface ligands through R2 .
  • the R 2 is combined with the ligand of the quantum dot by van der Waals force or hydrogen bond, or the R 2 is combined with the quantum dot by a coordination bond.
  • the (R 1 ) 3 NR 2 X can be: acryloyloxyethyltrimethylammonium chloride (see structural formula 1) or methacryloyloxyethyltrimethylammonium chloride (see structural formula 2) .
  • the self-assembled molecular layer between the hole transport layer and the quantum dot light-emitting layer includes a structure represented by the general formula R 3 -R 4 , wherein,
  • R 3 is a phenol group or a catechol group
  • R is selected from but not limited to hydrocarbon groups, hydrocarbon groups containing aryl groups, hydroxyl groups, mercapto groups, esters, ethers, amines (primary amines, secondary amines, tertiary amines), amides, phosphorus, phosphine, thioether, etc.
  • the R 3 can form a hydrogen bond with the surface of the hole transport layer, so that the self-assembled molecular layer is combined with the surface of the hole transport layer.
  • R 3 -R 4 can use: 2-phenol ethoxy acrylate (see structural formula 3).
  • the self-assembled molecular layer between the quantum dot light-emitting layer and the electron transport layer includes a structure represented by the general formula R 5 -R 6 , wherein,
  • R is selected from but not limited to groups such as amino, mercapto, carboxyl, hydroxyl, carbonyl, amido, phosphorus, oxyphosphine, organophosphorus, thioether, polysiloxane;
  • R 6 is selected from but not limited to hydrocarbon groups, hydrocarbon groups containing aryl groups, ether groups, polyoxypropylene groups, perfluoroalkyl groups, etc.; preferably, the number of carbon atoms in R 6 is C 4 -C 20 .
  • the R 5 and the quantum dots in the light-emitting layer are combined with the surface of the quantum dot light-emitting layer through a coordination bond, or the R 5 and the surface ligands of the quantum dots are combined with the surface ligands of the quantum dots through hydrogen bonds.
  • the quantum dots are bound to the surface of the luminescent layer.
  • the R 6 is adsorbed on the surface of the electron transport layer by van der Waals force.
  • R 5 -R 6 can be: dodecyltrimethoxysilane (see structural formula 4).
  • the hole transport layer includes an organic hole transport material.
  • the organic hole transport materials include, but are not limited to: one or more of biphenyls, poly/thiophenes, triarylamines, carbazoles, pyrazolines, butadiene and styrenes .
  • the quantum dot light-emitting layer includes quantum dots.
  • the quantum dots include one or more of II-VI compounds and III-V compounds.
  • the II-VI group compounds such as CdS, CdSe, CdTe, ZnS, ZnSe, ZnTe, HgS, HgSe, HgTe, PbS, PbSe, PbTe and other binary, ternary, quaternary II-VI compounds ;
  • the III-V compound such as GaP, GaAs, InP, InAs and other binary, ternary, quaternary III-V compounds.
  • the quantum dots are quantum dot nanoparticle materials.
  • the quantum dots are selected from but not limited to CdS, CdSe, CdTe, ZnO, ZnS, ZnSe, ZnTe, GaAs, GaP, GaSb, HgS, HgSe, HgTe, InAs, InP, InSb, AlAs, AlP, CuInS and CuInSe One or more of them, and at least one of various core-shell quantum dots.
  • the electronic functional layer includes, but is not limited to, inorganic nanoparticle materials with electron transport capability.
  • the inorganic nanoparticles include one or more of doped or undoped metal oxides.
  • the doped or non-doped metal oxide includes but not limited to: one of ZnO, TiO 2 , SnO 2 , Ta 2 O 3 , ZrO 2 , TiLiO, ZnAlO, ZnMgO, ZnSnO, ZnLiO, InSnO one or more species.
  • the display panel 200 includes: a substrate 210 on which a plurality of the organic electroluminescent devices 100 are formed.
  • the substrate 210 can also be formed with a structure that has undergone several previous processes, for example, there may be an inorganic film layer, several film layers in the thin film transistor structure, or a complete thin film transistor and routing. Wire.
  • the display panel 200 also includes other known structures such as a packaging cover plate, which will not be repeated here.
  • An embodiment of the present application further provides a display device, including the above-mentioned display panel.
  • This embodiment provides a quantum dot light-emitting diode (QLED) device, please refer to Figure 4, including an anode, a hole injection layer, a hole transport layer, a self-assembled molecular layer, and a quantum dot light-emitting layer that are sequentially stacked on the substrate , electron transport layer and cathode.
  • the material of the self-assembled molecular layer is (R 1 ) 3 NR 2 X, specifically acryloyloxyethyltrimethylammonium chloride, and the structural formula is
  • the preparation method of the quantum dot light-emitting diode device comprises the following steps:
  • a cathode is formed on the electron transport layer.
  • quantum dot light-emitting diode device of this embodiment except for the substrate, anode and cathode, other functional layers are all deposited by printing.
  • This embodiment provides a quantum dot light-emitting diode (QLED) device, please refer to Figure 4, including an anode, a hole injection layer, a hole transport layer, a self-assembled molecular layer, and a quantum dot light-emitting layer that are sequentially stacked on the substrate , electron transport layer and cathode.
  • the material of the self-assembled molecular layer is R 3 -R 4 , specifically 2-phenol ethoxy acrylate, and the structural formula is
  • the preparation method of the quantum dot light-emitting diode device comprises the following steps:
  • a cathode is formed on the electron transport layer.
  • quantum dot light-emitting diode device of this embodiment except for the substrate, anode and cathode, other functional layers are deposited by printing.
  • This embodiment provides a quantum dot light-emitting diode (QLED) device, please refer to Figure 5, including an anode, a hole injection layer, a hole transport layer, a quantum dot light-emitting layer, and a self-assembled molecular layer that are sequentially stacked on the substrate , electron transport layer and cathode.
  • the material of the self-assembled molecular layer is R 5 -R 6 , specifically dodecyltrimethoxysilane is used, and the structural formula is
  • the preparation method of the quantum dot light-emitting diode device comprises the following steps:
  • a cathode is formed on the electron transport layer.
  • quantum dot light-emitting diode device of this embodiment except for the substrate, anode and cathode, other functional layers are deposited by printing.
  • This embodiment provides a quantum dot light-emitting diode (QLED) device, please refer to FIG. 6, including an anode, a hole injection layer, a hole transport layer, a quantum dot light-emitting layer, an electron transport layer and cathode.
  • QLED quantum dot light-emitting diode
  • the preparation method of the quantum dot light-emitting diode device comprises the following steps:
  • a cathode is formed on the electron transport layer.
  • quantum dot light-emitting diode device of this embodiment except for the substrate, anode and cathode, other functional layers are deposited by printing.
  • Examples 2-3 and Comparative Example 1 are not specifically limited, but the devices in Examples 2-3 and Comparative Example 1 are the same
  • the functional layer is the same in material and preparation process.
  • the performance results of the devices in Examples 2-3 are shown in FIG. 7 , wherein Comparative Example 1 is marked as Device A, Example 2 is marked as Device B, and Example 3 is marked as Device C.
  • Two kinds of fluorescent films are provided, one of which is fluorescent film A, which includes a hole injection layer and a hole transport layer sequentially stacked on a substrate (see A shown in Figure 8); another fluorescent film B , including a hole injection layer, a hole transport layer, and a self-assembled molecular layer (shown in B in FIG. 8 ) stacked sequentially on the substrate.
  • fluorescent film A which includes a hole injection layer and a hole transport layer sequentially stacked on a substrate (see A shown in Figure 8);
  • another fluorescent film B including a hole injection layer, a hole transport layer, and a self-assembled molecular layer (shown in B in FIG. 8 ) stacked sequentially on the substrate.
  • the fluorescence emission intensity was tested, as shown in FIG. 9 .
  • the surface roughness of the film was tested by AFM, and the AFM map was obtained to prove the improvement effect of the self-assembled monolayer on the upper layer of quantum dot solvent erosion of the lower hole transport film.
  • Two kinds of fluorescent films are provided, wherein one kind of fluorescent film C includes a substrate, a hole injection layer, a hole transport layer and a quantum dot light-emitting layer (see Figure 11 shown in C); A fluorescent film D, or a substrate, a hole injection layer, a hole transport layer, a quantum dot light-emitting layer and a self-assembled molecular layer (see D shown in Figure 11).
  • this application aims to improve the problem of poor bonding between the functional thin film layer and the quantum dot light-emitting layer due to the difference in material types and characteristics of organic hole transport materials, inorganic quantum dot materials, and inorganic electron transport materials.
  • using the positively charged quaternary nitrogen (N) and R3 in the self-assembled molecular layer can form strong electrostatic and hydrogen bonding with the organic hole transport layer; R2 and R4 can only form van der Waals with the hole transport layer Force adsorption but can combine with the quantum dot light-emitting layer by coordination bond or hydrogen bond; or use the self-assembled molecular layer R5 can form a coordination bond or hydrogen bond with the quantum dot light-emitting layer, R6 and quantum dot light emission
  • the layer can only form van der Waals force adsorption, thereby effectively improving the adhesion between the functional transport film layer and the quantum dot light-emitting layer, improving the mechanical reliability of the interface, and at the same time solving the solvent erosion of the upper film material during
  • a quantum dot light-emitting diode device and its preparation method and display panel provided by the embodiments of the present application have been introduced in detail above.
  • specific examples are used to illustrate the principles and implementation methods of the present application.
  • the description of the above embodiments It is only used to help understand the method of the present application and its core idea; at the same time, for those skilled in the art, according to the idea of the present application, there will be changes in the specific implementation and application scope. In summary, this The content of the description should not be understood as limiting the application.

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Abstract

本申请公开了一种量子点发光二极管器件及其制备方法与显示面板，所述量子点发光二极管器件包括功能层和量子点发光层，所述功能层与所述量子点发光层之间设置有自组装分子层，所述自组装分子层与功能层之间产生作用力以提高所述功能层与所述量子点发光层之间的结合力，提高了界面的机械可靠性。

Description

量子点发光二极管器件及其制备方法与显示面板
本申请要求于2021年09月30日在中国专利局提交的、申请号为202111164887.4、申请名称为“量子点发光二极管器件和显示面板”的中国专利申请的优先权，其全部内容通过引用结合在本申请中。
技术领域
本申请涉及显示技术领域，具体涉及一种量子点发光二极管器件及其制备方法与显示面板。
背景技术
半导体量子点(Quantum Dots，QDs)具有荧光量子效率高、可见光波段发光可调、色域覆盖度宽广等特点，在显示和固态照明领域受到极大关注。相比于传统显示技术，基于量子点技术的电致发光器件—量子点发光二极管器件(Quantumdot Light Emitting Diode,QLED)，具有高的稳定性、溶液可加工和高的色彩饱和度等优势，可以通过自发光实现关于从点光源到面光源的飞跃。
QLED器件，是由两个电极和在电极与量子点之间添加各种功能层形成的类似“三明治”的薄膜叠层结构，这些功能层包括电子注入层、电子传输层、空穴传输层、空穴注入层等，各薄膜层的成膜质量、界面结合和材料本身稳定性会极大程度地影响器件的各项性能。目前的QLED器件和相关材料大都是在低温条件下(≤300℃)制备，对设备的要求相应的降低，有利于简化工艺和降低成本。
技术问题
对于低温法制备的电子传输层材料，其表面缺陷多，电子迁移率低，且成膜过程中易出现成膜不均匀、存在针孔等现象。常见的有机空穴传输材料主要为联苯类、聚/并噻吩类、三芳胺类、咔唑类、砒唑啉类、丁二烯类、苯乙烯类等，具有环境稳定性差、不耐高温、空穴迁移率低等缺点。另外，功能薄膜层与量子点发光层之间会相互粘合，但基于有机空穴传输材料、无机量子点材料和无机电子传输材料的材料种类及特性差异，导致功能薄膜层与量子点发光 层之间结合力不佳的问题，尤其在基于溶液法制备QLED器件的制程中，存在上层薄膜层材料的溶剂对下层薄膜层的侵蚀破坏的问题，会对下层薄膜层的薄膜质量造成负面影响，并且不利于上层薄膜层与下层薄膜层之间的结合，从而严重降低器件性能。
因此，亟待提供一种量子点发光二极管器件，能够改善功能薄膜层与量子点发光层之间的结合性。
技术解决方案
鉴于此，本申请提供了一种量子点发光二极管器件及其制备方法与显示面板，能够改善功能薄膜层与量子点发光层之间的结合性。
第一方面，本申请提供了一种量子点发光二极管器件，包括依次层叠设置的第一电极、空穴功能层、量子点发光层、电子功能层和第二电极；所述空穴功能层与所述量子点发光层之间设置有自组装分子层，或者所述电子功能层与所述量子点发光层之间设置有自组装分子层，或者所述空穴功能层与所述量子点发光层之间设置有自组装分子层且所述电子功能层与所述量子点发光层之间设置有自组装分子层。
可选地，所述空穴功能层包括空穴注入层和/或空穴传输层；
所述电子功能层包括电子注入层和/或电子传输层。
可选地，所述空穴功能层与所述量子点发光层之间的自组装分子层包括通式(R 1) 3NR 2X所示结构的化合物；
在所述通式(R 1) 3NR 2X中，R 1为甲基或乙基，N为带正电荷的四价氮；X为卤素负离子或羧酸根；R 2选自烃基，含有芳基、羟基、巯基、酯、醚、胺、酰胺、磷、氧磷或硫醚的烃基，聚氧丙烯基，全氟烷基以及聚硅氧烷基中的一种或多种，R 2的碳原子数为4个至20个。
可选地，所述带正电荷的四价氮与所述空穴功能层中不饱和键之间具有静电吸附作用力；
所述R2与所述量子点发光层的量子点的配体之间具有范德华力或形成氢键，或所述R2与所述量子点发光层的量子点之间形成配位键。
可选地，所述通式(R 1) 3NR 2X所示结构的化合物选自：
Figure PCTCN2022121786-appb-000001
可选地，所述空穴功能层与所述量子点发光层之间的自组装分子层包括通式R 3-R 4所示结构的化合物；
在所述通式R 3-R 4中，R 3为苯酚基团或邻苯二酚基团；R 4选自烃基，含有芳基、羟基、巯基、酯、醚、胺、酰胺、磷、氧磷或硫醚的烃基，聚氧丙烯基，全氟烷基以及聚硅氧烷基中的一种或多种，R 4的碳原子数为4个至20个。
可选地，所述R 3与所述空穴功能层的表面形成氢键，使得所述自组装分子层与所述空穴功能层的表面结合；
所述R 4与所述量子点发光层的量子点的配体之间具有范德华力或形成氢键、或所述R 4与所述量子点发光层的量子点之间形成配位键，使得所述自组装分子层与所述量子点发光层的表面结合。
可选地，所述通式R 3-R 4所示结构的化合物选自：
Figure PCTCN2022121786-appb-000002
可选地，所述量子点发光层与所述电子功能层之间的自组装分子层包括通式R 5-R 6所示结构的化合物；
在所述通式R 5-R 6中，R 5选自氨基、巯基、羧基、羟基、羰基、酰胺基、磷、氧磷、有机磷、硫醚以及聚硅氧烷基中的一种或多种；R 6选自烃基，含有芳基、醚基的烃基，聚氧丙烯基以及全氟烷基中的一种或多种，R 6的碳原子数为4个至20个。
可选地，所述R 5与所述量子点发光层的量子点之间形成配位键、或所述R 5与所述量子点发光层的量子点的表面配体形成氢键，使所述自组装分子层与所述量子点发光层的表面结合；
所述R 6与所述电子功能层的表面具有范德华力，使所述自组装分子层吸附于所述电子功能层的表面。
可选地，所述式R 5-R 6所示结构的化合物选自：
Figure PCTCN2022121786-appb-000003
可选地，所述自组装分子层的厚度为1～50nm。
可选地，所述功能层包括空穴传输层，所述空穴传输层包括有机空穴传输材料，所述有机空穴传输材料包括联苯类、聚/并噻吩类、三芳胺类、咔唑类、砒唑啉类、丁二烯类以及苯乙烯类中的一种或多种。
可选地，所述功能层包括电子传输层，所述电子传输层包括无机纳米颗粒材料；所述无机纳米颗粒包括掺杂或非掺杂的金属氧化物中的一种或多种；
优选地，所述掺杂或非掺杂的金属氧化物包括ZnO、TiO 2、SnO 2、Ta 2O 3、ZrO 2、TiLiO、ZnAlO、ZnMgO、ZnSnO、ZnLiO、InSnO中的一种或多种。
可选地，所述量子点发光层包括量子点；所述量子点包括II-VI族化合物和III-V族化合物中的一种或多种；优选地，所述量子点包括CdS、CdSe、CdTe、ZnS、ZnSe、ZnTe、GaAs、GaP、GaSb、HgS、HgSe、HgTe、InAs、InP、InSb、AlAs、AlP、CuInS和CuInSe中的一种或多种。
第二方面，本申请提供了一种量子点发光二极管器件的制备方法，所述制备方法包括如下步骤：
提供一衬底，在所述衬底上形成第一电极；
在所述第一电极上形成空穴功能层；
在所述空穴功能层上形成量子点发光层；
在所述量子点发光层上形成电子功能层；以及
在所述电子功能层上形成第二电极；
或者，所述制备方法包括如下步骤：
提供一衬底，在所述衬底上形成第二电极；
在所述第二电极上形成电子功能层；
在所述电子功能层上形成量子点发光层；
在所述量子点发光层上形成空穴功能层；以及
在所述空穴功能层上形成第一电极；
其中，所述空穴功能层与所述量子点发光层之间设置有自组装分子层，或者所述电子功能层与所述量子点发光层之间设置有自组装分子层，或者所述空穴功能层与所述量子点发光层之间设置有自组装分子层且所述电子功能层与所述量子点发光层之间设置有自组装分子层。
可选地，设置于所述空穴功能层与所述量子点发光层之间的所述自组装分子层包括通式(R 1) 3NR 2X所示结构的化合物；
在所述通式(R 1) 3NR 2X中，R 1为甲基或乙基，N为带正电荷的四价氮；X为卤素负离子或羧酸根；R 2选自烃基，含有芳基、羟基、巯基、酯、醚、胺、酰胺、磷、氧磷或硫醚的烃基，聚氧丙烯基，全氟烷基以及聚硅氧烷基中的一种或多种，R 2的碳原子数为4个至20个。
可选地，设置于所述空穴功能层与所述量子点发光层之间的所述自组装分子层包括通式R 3-R 4所示结构的化合物，在所述通式R 3-R 4中，R 3为苯酚基团或邻苯二酚基团；R 4选自烃基，含有芳基、羟基、巯基、酯、醚、胺、酰胺、磷、氧磷或硫醚的烃基，聚氧丙烯基，全氟烷基以及聚硅氧烷基中的一种或多种，R 4的碳原子数为4个至20个。
可选地，设置于所述电子功能层与所述量子点发光层之间的所述自组装分子层包括通式R 5-R 6所示结构的化合物；
在所述通式R 5-R 6中，R 5选自氨基、巯基、羧基、羟基、羰基、酰胺基、磷、氧磷、有机磷、硫醚以及聚硅氧烷基中的一种或多种；R 6选自烃基，含有芳基、醚基的烃基，聚氧丙烯基以及全氟烷基中的一种或多种，R 6的碳原子数为4个至20个。
第三方面，本申请提供了一种显示面板，所述显示面板包括基板和以阵列的形式设置于所述基板表面的量子点发光二极管器件，所述量子点发光二极管器件包括依次层叠设置的第一电极、空穴功能层、量子点发光层、电子功能层和第二电极；所述空穴功能层与所述量子点发光层之间设置有自组装分子层，或者所述电子功能层与所述量子点发光层之间设置有自组装分子层，或者所述空穴功能层与所述量子点发光层之间设置有自组装分子层且所述电子功能层与所述量子点发光层之间设置有自组装分子层。
可选地，设置于所述空穴功能层与所述量子点发光层之间的所述自组装分 子层包括通式(R 1) 3NR 2X所示结构的化合物，在所述通式(R 1) 3NR 2X中，R 1为甲基或乙基，N为带正电荷的四价氮；X为卤素负离子或羧酸根；R 2选自烃基，含有芳基、羟基、巯基、酯、醚、胺、酰胺、磷、氧磷或硫醚的烃基，聚氧丙烯基，全氟烷基以及聚硅氧烷基中的一种或多种，R 2的碳原子数为4个至20个；
或者，设置于所述空穴功能层与所述量子点发光层之间的所述自组装分子层包括通式R 3-R 4所示结构的化合物，在所述通式R 3-R 4中，R 3为苯酚基团或邻苯二酚基团；R 4选自烃基，含有芳基、羟基、巯基、酯、醚、胺、酰胺、磷、氧磷或硫醚的烃基，聚氧丙烯基，全氟烷基以及聚硅氧烷基中的一种或多种，R 4的碳原子数为4个至20个。
可选地，设置于所述电子功能层与所述量子点发光层之间的自组装分子层包括通式R 5-R 6所示结构的化合物，在所述通式R 5-R 6中，R 5选自氨基、巯基、羧基、羟基、羰基、酰胺基、磷、氧磷、有机磷、硫醚以及聚硅氧烷基中的一种或多种；R 6选自烃基，含有芳基、醚基的烃基，聚氧丙烯基以及全氟烷基中的一种或多种，R 6的碳原子数为4个至20个。
有益效果
本发明提供了一种量子点发光二极管器件(QLED)，在所述QLED器件中，功能层与量子点发光层之间设置有自组装分子层，所述自组装分子层可有效提高空穴功能层与量子点发光层之间的粘合程度和/或电子功能层与量子点发光层与量子点发光层之间的粘合程度，从而提高了界面的机械可靠性。
本申请利用自组装分子层与有机空穴传输层、量子点发光层及电子传输层之间的作用力(例如范德华力、配位键和氢键等)，从而有效改善制程中上层薄膜材料的溶剂侵蚀破坏下层薄膜的问题，以及功能层与量子点发光层之间的界面粘合程度，提高了界面的机械可靠性，改善了因有机空穴传输材料、无机量子点材料和无机电子传输材料的材料种类及特性差异而导致的界面之间结合性不佳的问题。
附图说明
为了更清楚地说明本申请实施例中的技术方案，下面将对实施例描述中所 需要使用的附图作简单地介绍，显而易见地，下面描述中的附图仅仅是本申请的一些实施例，对于本领域技术人员来讲，在不付出创造性劳动的前提下，还可以根据这些附图获得其他的附图。
图1是本申请实施例提供的量子点发光二极管器件的结构示意图一；
图2是本申请实施例提供的量子点发光二极管器件的结构示意图二；
图3是本申请实施例提供的显示面板的结构示意；
图4是本申请实施例1和实施例2提供的量子点发光二极管器件的结构示意图；
图5是本申请实施例3提供的量子点发光二极管器件的结构示意图；
图6是本申请对比例1提供的量子点发光二极管器件的结构示意图；
图7是本申请试验例1中的电流效率-电流密度特性曲线图；
图8是本申请试验例2中的荧光薄膜结构示意图；
图9是本申请试验例2中的荧光薄膜的相对荧光强度图；
图10是本申请试验例2中的AFM图；
图11是本申请试验例3中的荧光薄膜结构示意图；
图12是本申请试验例3中的荧光薄膜的相对荧光强度图。
本申请的实施方式
下面将结合本申请实施例中的附图，对本申请实施例中的技术方案进行清楚、完整地描述，显然，所描述的实施例仅仅是本申请一部分实施例，而不是全部的实施例。基于本申请中的实施例，本领域技术人员在没有做出创造性劳动前提下所获得的所有其它实施例，都属于本申请保护的范围。
本申请实施例提供一种量子点发光二极管器件及其制备方法与显示面板。以下分别进行详细说明。需说明的是，以下实施例的描述顺序不作为对实施例优选顺序的限定。
另外，在本申请的描述中，术语“包括”是指“包括但不限于”。本申请的各种实施例可以以一个范围的型式存在；应当理解，以一范围型式的描述仅仅是因为方便及简洁，不应理解为对本申请范围的硬性限制；因此，应当认为所述的范围描述已经具体公开所有可能的子范围以及该范围内的单一数值。例如， 应当认为从1到6的范围描述已经具体公开子范围，例如从1到3，从1到4，从1到5，从2到4，从2到6，从3到6等，以及所述范围内的单一数字，例如1、2、3、4、5及6，此不管范围为何皆适用。每当在本文中指出数值范围，是指包括所指范围内的任何引用的数字(分数或整数)。
在本申请中，术语“和/或”用于描述关联对象的关联关系，表示可以存在三种关系，例如，“A和/或B”可以表示三种情况：第一种情况是单独存在A；第二种情况是同时存在A和B；第三种情况是单独存在B的情况，其中，A和B分别可以是单数或者复数。
在本申请中，术语“至少一种”是指一种或多种，“多种”是指两种或两种以上。术语“至少一个”、“以下至少一项(个)”或其类似表达，指的是这些项中的任意组合，包括单项(个)或复数项(个)的任意组合。例如，“a、b或c中的至少一项(个)”或“a,b和c中的至少一项(个)”均可表示为：a、b、c、a-b(即a和b)、a-c、b-c或a-b-c，其中，a,b和c分别可以是单个或多个。
本申请实施例提供一种量子点发光二极管器件，包括依次层叠设置的第一电极、空穴功能层、量子点发光层、电子功能层和第二电极；所述空穴功能层与所述量子点发光层之间和/或所述电子功能层与所述量子点发光层之间设置有自组装分子层。所述自组装分子层与所述空穴功能层之间和/或所述自组装分子层与所述电子功能层之间能够产生作用力，以增强所述量子点发光层与所述空穴功能层之间和/或所述量子点发光层与所述电子功能层之间的结合性；具体地，所述作用力选自范德华力、配位键和氢键中的一种或多种。进一步地，所述自组装分子层可以为自组装单分子层(SAM)，是一种由具有活性基团的分子在固体表面自发地组装形成的有序单分子薄膜。
所述空穴功能层包括空穴注入层和/或空穴传输层；所述电子功能层包括电子注入层和/或电子传输层。例如，所述量子点发光二极管器件包括依次层叠设置的第一电极、空穴传输层、量子点发光层、电子传输层和第二电极。在例如，所述量子点发光二极管器件包括依次层叠设置的第一电极、空穴注入层、空穴传输层、量子点发光层、电子传输层、电子注入层和第二电极。进一步地，所述量子点发光层与所述空穴传输层之间设置有所述自组装分子层，和/或所述量子点发光层与所述电子传输层之间设置有所述自组装分子层。例如，所述 自组装分子层设置于所述量子点发光层与所述空穴传输层之间，和/或所述自组装分子层设置于所述量子点发光层与所述电子传输层之间。通过在量子点发光二极管器件中设置所述自组装分子层，可以有效改善所述空穴传输层与所述量子点发光层之间的粘合程度和/或所述电子传输层与所述量子点发光层之间的粘合程度，从而提高了界面的机械可靠性。
进一步地，所述自组装分子层的厚度可以为1～50nm，例如，1nm、3nm、5nm、10nm、15nm、20nm、25nm、30nm、35nm、40nm、45nm或50nm。
进一步地，请参阅图1和图2，所述量子点发光二极管器件100包括空穴传输层110、量子点发光层120和电子传输层130，且所述空穴传输层110与所述电子传输层130之间设置有自组装分子层140。例如，请继续参阅图1，所述空穴传输层110与所述量子点发光层120之间设置有所述自组装分子层140a。例如，请继续参阅图2，所述量子点发光层120与所述电子传输层130之间设置有所述自组装分子层140b。可以想象，所述空穴传输层110与所述量子点发光层120之间设置有所述自组装分子层140a，同时，在所述量子点发光层120与所述电子传输层130之间设置有所述自组装分子层140b。所述自组装分子层分别与所述空穴传输层和所述电子传输层具有作用力。
进一步地，所述自组装分子层材料可以为(R 1) 3NR 2X、R 3-R 4、R 5-R 6；本申请可以根据自组装分子层设置的具体位置来选择材料。所述自组装分子层的选择可参考下述。
在一些实施例中，所述空穴传输层与所述量子点发光层之间的自组装分子层包括通式(R 1) 3NR 2X所示的结构，其中，
R 1为甲基或乙基，(R 1) 3为三个R 1基团；
N为带正电荷的四价氮；
X为卤素负离子(F -、Cl -、Br -、I -)或羧酸根(RCOO -)，其中RCOO -中的R为烃基；
R 2选自但不限于是烃基、含有芳基、羟基、巯基、酯、醚、胺(伯胺、仲胺、叔胺)、酰胺、磷、氧磷、硫醚等基团的烃基、聚氧丙烯基、全氟烷基、聚硅氧烷基等；优选地，R 2中碳原子数为C 4～C 20。进一步地，根据R 2基团和量子点配体种类的选择，两者结合能力大小排序为：配位键＞氢键＞范德华力。
本申请中，所述自组装分子层以带正电荷的四价氮与空穴传输层中不饱和键(如苯环、碳碳双键)通过静电方式吸附于空穴传输层表面。所述自组装分子层以R 2通过范德华力或与量子点通过配位键或与量子点表面配体通过氢键方式与量子点发光层表面结合。所述R 2与所述量子点的配体之间以范德华力或氢键方式结合，或所述R 2与所述量子点之间以配位键方式结合。
例如，所述(R 1) 3NR 2X可以采用：丙烯酰氧乙基三甲基氯化铵(见结构式1)或甲基丙烯酰氧乙基三甲基氯化铵(见结构式2)。
Figure PCTCN2022121786-appb-000004
在一些实施例中，所述空穴传输层与所述量子点发光层之间的自组装分子层包括通式R 3-R 4所示的结构，其中，
R 3为苯酚基团或邻苯二酚基团；
R 4选自但不限于是烃基、含有芳基、羟基、巯基、酯、醚、胺(伯胺、仲胺、叔胺)、酰胺、磷、氧磷、硫醚等基团的烃基、聚氧丙烯基、全氟烷基、聚硅氧烷基等；优选地，R 4中碳原子数为C 4～C 20。
本申请中，所述R 3与所述空穴传输层表面可形成氢键，使得所述自组装分子层与所述空穴传输层的表面结合。所述R 4与所述量子点之间具有范德华力或形成配位键、或所述R 4与所述量子点的表面配体之间形成氢键，使得所述自组装分子层与所述量子点发光层的表面结合。
例如，所述R 3-R 4可以采用：2-酚基乙氧基丙烯酸酯(见结构式3)。
Figure PCTCN2022121786-appb-000005
在一些实施例中，所述量子点发光层与所述电子传输层之间的自组装分子 层包括通式R 5-R 6所示的结构，其中，
R 5选自但不限于是氨基、巯基、羧基、羟基、羰基、酰胺基、磷、氧磷、有机磷、硫醚、聚硅氧烷基等基团；
R 6选自但不限于是烃基、含有芳基、醚等基团的烃基、聚氧丙烯基、全氟烷基等；优选地，R 6中碳原子数为C 4～C 20。
本申请中，所述R 5与发光层中量子点之间通过配位键与所述量子点发光层的表面结合，或所述R 5与所述量子点的表面配体通过氢键方式与所述量子点发光层的表面结合。所述R 6利用范德华力吸附于所述电子传输层的表面。
例如，所述R 5-R 6可以采用：十二烷基三甲氧基硅烷(见结构式4)。
Figure PCTCN2022121786-appb-000006
在一些实施例中，所述空穴传输层包括有机空穴传输材料。所述有机空穴传输材料包括但不限于：联苯类、聚/并噻吩类、三芳胺类、咔唑类、砒唑啉类、丁二烯类和苯乙烯类中的一种或多种。
在一些实施例中，所述量子点发光层包括量子点。所述量子点包括II-VI族化合物和III-V族化合物中的一种或多种。进一步地，所述II-VI族化合物，比如CdS、CdSe、CdTe、ZnS、ZnSe、ZnTe、HgS、HgSe、HgTe、PbS、PbSe、PbTe和其他二元、三元、四元的II-VI化合物；所述III-V族化合物，比如GaP、GaAs、InP、InAs和其他二元、三元、四元的III-V化合物。进一步地，所述量子点为量子点纳米颗粒材料。例如，所述量子点选自但不限于CdS、CdSe、CdTe、ZnO、ZnS、ZnSe、ZnTe、GaAs、GaP、GaSb、HgS、HgSe、HgTe、InAs、InP、InSb、AlAs、AlP、CuInS和CuInSe中的一种或或多种，以及各种核壳结构量子点中的至少一种。
在一些实施例中，所述电子功能层包括但不限于具有电子传输能力的无机纳米颗粒材料。所述无机纳米颗粒包括掺杂或非掺杂的金属氧化物中的一种或多种。进一步地，所述掺杂或非掺杂的金属氧化物包括但不限于：ZnO、TiO 2、SnO 2、Ta 2O 3、ZrO 2、TiLiO、ZnAlO、ZnMgO、ZnSnO、ZnLiO、InSnO中的 一种或多种。
本申请实施例还提供一种显示面板，包括上述的量子点发光二极管器件。如图3所示，所述显示面板200包括：一基板210，所述基板210上形成复数个所述有机电致发光器件100。本领域技术人员可以理解的是，所述基板210上还可以形成有经过前序若干工序的结构，例如可能有无机膜层、薄膜晶体管结构中的若干膜层或者已经形成完整的薄膜晶体管及走线。当然，所述显示面板200还包括其他诸如封装盖板之类的已知结构，在此不再赘述。
本申请实施例还提供一种显示装置，包括上述的显示面板。
本申请先后进行过多次试验，现举一部分试验结果作为参考对发明进行进一步详细描述，下面结合具体实施例进行详细说明。
实施例1
本实施例提供一种量子点发光二极管(QLED)器件，请参阅图4，包括依次层叠设置于衬底上的阳极、空穴注入层、空穴传输层、自组装分子层、量子点发光层、电子传输层和阴极。所述自组装分子层的材料为(R 1) 3NR 2X，具体采用丙烯酰氧乙基三甲基氯化铵，结构式为
Figure PCTCN2022121786-appb-000007
所述量子点发光二极管器件的制备方法，包括如下步骤：
提供一衬底，在所述衬底上形成阳极；
在所述阳极上形成空穴注入层；
在所述空穴注入层上形成空穴传输层；
在所述空穴传输层上形成自组装分子层，其中所述自组装分子层的材料为(R 1) 3NR 2X；
在所述自组装分子层上形成量子点发光层；
在所述量子点发光层上形成电子传输层；
在所述电子传输层上形成阴极。
本实施例的量子点发光二极管器件中，除衬底、阳极和阴极外，其他功能 层均通过打印方式实现薄膜沉积。
实施例2
本实施例提供一种量子点发光二极管(QLED)器件，请参阅图4，包括依次层叠设置于衬底上的阳极、空穴注入层、空穴传输层、自组装分子层、量子点发光层、电子传输层和阴极。所述自组装分子层的材料为R 3-R 4，具体采用2-酚基乙氧基丙烯酸酯，结构式为
Figure PCTCN2022121786-appb-000008
所述量子点发光二极管器件的制备方法，包括如下步骤：
提供一衬底，在所述衬底上形成阳极；
在所述阳极上形成空穴注入层；
在所述空穴注入层上形成空穴传输层；
在所述空穴传输层上形成自组装分子层，其中所述自组装分子层的材料为R 3-R 4；
在所述自组装分子层上形成量子点发光层；
在所述量子点发光层上形成电子传输层；
在所述电子传输层上形成阴极。
本实施例的量子点发光二极管器件中，除衬底、阳极和阴极外，其他功能层均通过打印方式实现薄膜沉积。
实施例3
本实施例提供一种量子点发光二极管(QLED)器件，请参阅图5，包括依次层叠设置于衬底上的阳极、空穴注入层、空穴传输层、量子点发光层、自组装分子层、电子传输层和阴极。所述自组装分子层的材料为R 5-R 6，具体采用十二烷基三甲氧基硅烷，结构式为
Figure PCTCN2022121786-appb-000009
所述量子点发光二极管器件的制备方法，包括如下步骤：
提供一衬底，在所述衬底上形成阳极；
在所述阳极上形成空穴注入层；
在所述空穴注入层上形成空穴传输层；
在所述空穴传输层上形成量子点发光层；
在所述量子点发光层上形成自组装分子层，其中所述自组装分子层的材料为R 5-R 6；
在所述自组装分子层上形成电子传输层；
在所述电子传输层上形成阴极。
本实施例的量子点发光二极管器件中，除衬底、阳极和阴极外，其他功能层均通过打印方式实现薄膜沉积。
对比例1
本实施例提供一种量子点发光二极管(QLED)器件，请参阅图6，包括依次层叠设置于衬底上的阳极、空穴注入层、空穴传输层、量子点发光层、电子传输层和阴极。
所述量子点发光二极管器件的制备方法，包括如下步骤：
提供一衬底，在所述衬底上形成阳极；
在所述阳极上形成空穴注入层；
在所述空穴注入层上形成空穴传输层；
在所述空穴传输层上形成量子点发光层；
在所述量子点发光层上形成电子传输层；
在所述电子传输层上形成阴极。
本实施例的量子点发光二极管器件中，除衬底、阳极和阴极外，其他功能层均通过打印方式实现薄膜沉积。
试验例1
本试验例将实施例2～3和对比例1中的QLED器件进行比较，以对比验证了本申请的自组装分子层对QLED器件性能的改善效果。
实施例2～3和对比例1中的空穴注入层、空穴传输层、量子点发光层和电 子传输层材料不做具体限定，但实施例2～3和对比例1中的器件的相同功能层是材料及制备工艺相同。实施例2～3中的器件的性能结果如图7所示，其中，对比例1记为器件A，实施例2记为器件B，实施例3记为器件C。
可以发现，器件A、器件B和器件C的最大电流效率分别为16.5cd/A，37.2cd/A，33.4cd/A。显然，本申请的实施例2和实施例3的器件电流效率显著高于对比例1，进而证明了本申请的自组装分子层可以明显提升器件效率。
试验例2
本试验例研究自组装分子层能否有效减弱量子点发光层薄膜材料的溶剂对空穴传输层薄膜的侵蚀破坏和提高界面结合程度。
方法：提供了二种荧光薄膜，其中一种荧光薄膜A，包括依次层叠设置于衬底上的空穴注入层和空穴传输层(参见图8中A所示)；另一种荧光薄膜B，包括依次层叠设置于衬底上的空穴注入层、空穴传输层和自组装分子层(参见图8中B所示)。
将制备的荧光薄膜A和荧光薄膜B分别用量子点发光层材料的溶剂浸泡处理10min后，测试荧光发射强度，如图9所示。如图10所示，AFM测试薄膜表面粗糙度，得到AFM图，用以证明自组装单分子层对上层量子点溶剂侵蚀下层空穴传输薄膜的改善效果。
结果发现，荧光薄膜A(未用溶剂浸泡处理)、荧光薄膜B(未用溶剂浸泡处理)、荧光薄膜A(溶剂浸泡处理10min)和荧光薄膜B(溶剂浸泡处理10min)的相对荧光强度分别为100％、95％、35％和86％，参见图9；并且，四种薄膜的表面粗糙度Rq分别为0.491nm、0.560nm、1.74nm和0.550nm，参见图10。可见自组装分子层能有效减弱量子点发光层薄膜材料的溶剂对空穴传输层薄膜的侵蚀破坏。
试验例3
本试验例研究自组装分子层能否有效减弱电子传输层薄膜材料的溶剂对量子点发光层薄膜的侵蚀破坏和提高界面结合程度。
方法：提供了二种荧光薄膜，其中一种荧光薄膜C，包括依次层叠设置的衬底、空穴注入层、空穴传输层和量子点发光层(参见图11中C所示)；另 一种荧光薄膜D，或衬底、空穴注入层、空穴传输层、量子点发光层和自组装分子层(参见图11中D所示)。
将制备得到的荧光薄膜C和荧光薄膜D分别用电子传输层材料的溶剂浸泡处理30min后，测试荧光发射强度，如图12所示。
结果发现，荧光薄膜C(未用溶剂浸泡处理)、荧光薄膜D(未用溶剂浸泡处理)、荧光薄膜C(溶剂浸泡处理30min)和荧光薄膜D(溶剂浸泡处理30min)的相对荧光强度分别为100％、100.1％、85％和96％。可见自组装分子层能有效减弱电子传输层薄膜材料的溶剂对量子点发光层薄膜的侵蚀破坏。
综上所述，本申请为改善因有机空穴传输材料、无机量子点材料和无机电子传输材料的材料种类及特性差异而导致的功能薄膜层与量子点发光层之间结合力不佳的问题，利用自组装分子层中带正电荷的四价氮(N)和R 3可与有机空穴传输层形成强烈的静电和氢键结合；R 2与R 4与空穴传输层仅能形成范德华力吸附但能与量子点发光层以配位键或氢键方式结合；或利用自组装分子层中R 5可与量子点发光层形成以配位键或氢键结合，R 6与量子点发光层仅能形成范德华力吸附，从而有效改善功能传输薄膜层与量子点发光层粘合程度，提高了界面的机械可靠性，同时解决了制程中上层薄膜材料的溶剂侵蚀破坏下层薄膜的问题。
在上述实施例中，对各个实施例的描述都各有侧重，某个实施例中没有详述的部分，可以参见其他实施例的相关描述。
以上对本申请实施例所提供的一种量子点发光二极管器件及其制备方法与显示面板进行了详细介绍，本文中应用了具体个例对本申请的原理及实施方式进行了阐述，以上实施例的说明只是用于帮助理解本申请的方法及其核心思想；同时，对于本领域的技术人员，依据本申请的思想，在具体实施方式及应用范围上均会有改变之处，综上所述，本说明书内容不应理解为对本申请的限制。

Claims (20)

  1. 一种量子点发光二极管器件，其中，包括依次层叠设置的第一电极、空穴功能层、量子点发光层、电子功能层和第二电极；所述空穴功能层与所述量子点发光层之间设置有自组装分子层，或者所述电子功能层与所述量子点发光层之间设置有自组装分子层，或者所述空穴功能层与所述量子点发光层之间设置有自组装分子层且所述电子功能层与所述量子点发光层之间设置有自组装分子层。
  2. 根据权利要求1所述的量子点发光二极管器件，其中，所述空穴功能层包括空穴注入层和/或空穴传输层；
    所述电子功能层包括电子注入层和/或电子传输层。
  3. 根据权利要求1或2所述的量子点发光二极管器件，其中，所述空穴功能层与所述量子点发光层之间的自组装分子层包括通式(R 1) 3NR 2X所示结构的化合物；
    在所述通式(R 1) 3NR 2X中，R 1为甲基或乙基，N为带正电荷的四价氮；X为卤素负离子或羧酸根；R 2选自烃基，含有芳基、羟基、巯基、酯、醚、胺、酰胺、磷、氧磷或硫醚的烃基，聚氧丙烯基，全氟烷基以及聚硅氧烷基中的一种或多种，R 2的碳原子数为4个至20个。
  4. 根据权利要求3所述的量子点发光二极管器件，其中，所述带正电荷的四价氮与所述空穴功能层中不饱和键之间具有静电吸附作用力；
    所述R 2与所述量子点发光层的量子点的配体之间具有范德华力或形成氢键，或所述R 2与所述量子点发光层的量子点之间形成配位键。
  5. 根据权利要求3或4所述的量子点发光二极管器件，其中，所述通式(R 1) 3NR 2X所示结构的化合物选自：
    Figure PCTCN2022121786-appb-100001
  6. 根据权利要求1或2所述的量子点发光二极管器件，其中，所述空穴 功能层与所述量子点发光层之间的自组装分子层包括通式R 3-R 4所示结构的化合物；
    在所述通式R 3-R 4中，R 3为苯酚基团或邻苯二酚基团；R 4选自烃基，含有芳基、羟基、巯基、酯、醚、胺、酰胺、磷、氧磷或硫醚的烃基，聚氧丙烯基，全氟烷基以及聚硅氧烷基中的一种或多种，R 4的碳原子数为4个至20个。
  7. 根据权利要求6所述的量子点发光二极管器件，其中，所述R 3与所述空穴功能层的表面形成氢键，使得所述自组装分子层与所述空穴功能层的表面结合；
    所述R 4与所述量子点发光层的量子点的配体之间具有范德华力或形成氢键、或所述R 4与所述量子点发光层的量子点之间形成配位键，使得所述自组装分子层与所述量子点发光层的表面结合。
  8. 根据权利要求6或7所述的量子点发光二极管器件，其中，所述通式R 3-R 4所示结构的化合物选自：
    Figure PCTCN2022121786-appb-100002
  9. 根据权利要求1至8任一项中所述的量子点发光二极管器件，其中，所述量子点发光层与所述电子功能层之间的自组装分子层包括通式R 5-R 6所示结构的化合物；
    在所述通式R 5-R 6中，R 5选自氨基、巯基、羧基、羟基、羰基、酰胺基、磷、氧磷、有机磷、硫醚以及聚硅氧烷基中的一种或多种；R 6选自烃基，含有芳基、醚基的烃基，聚氧丙烯基以及全氟烷基中的一种或多种，R 6的碳原子数为4个至20个。
  10. 根据权利要求9所述的量子点发光二极管器件，其中，所述R 5与所述量子点发光层的量子点之间形成配位键、或所述R 5与所述量子点发光层的量子点的表面配体形成氢键，使所述自组装分子层与所述量子点发光层的表面结合；
    所述R 6与所述电子功能层的表面具有范德华力，使所述自组装分子层吸附于所述电子功能层的表面。
  11. 根据权利要求9或10所述的量子点发光二极管器件，其中，所述式R 5-R 6所示结构的化合物选自：
    Figure PCTCN2022121786-appb-100003
  12. 根据权利要求1至11任一项中所述的量子点发光二极管器件，其中，所述自组装分子层的厚度为1～50nm。
  13. 根据权利要求1至12任一项中所述的量子点发光二极管器件，其中，所述功能层包括空穴传输层，所述空穴传输层包括有机空穴传输材料，所述有机空穴传输材料包括联苯类、聚/并噻吩类、三芳胺类、咔唑类、砒唑啉类、丁二烯类以及苯乙烯类中的一种或多种；
    所述功能层包括电子传输层，所述电子传输层包括无机纳米颗粒材料；所述无机纳米颗粒包括掺杂或非掺杂的金属氧化物中的一种或多种，优选地，所述掺杂或非掺杂的金属氧化物包括ZnO、TiO 2、SnO 2、Ta 2O 3、ZrO 2、TiLiO、ZnAlO、ZnMgO、ZnSnO、ZnLiO、InSnO中的一种或多种；
    所述量子点发光层包括量子点；所述量子点包括II-VI族化合物和III-V族化合物中的一种或多种；优选地，所述量子点包括CdS、CdSe、CdTe、ZnS、ZnSe、ZnTe、GaAs、GaP、GaSb、HgS、HgSe、HgTe、InAs、InP、InSb、AlAs、AlP、CuInS和CuInSe中的一种或多种。
  14. 一种量子点发光二极管器件的制备方法，其中，所述制备方法包括如下步骤：
    提供一衬底，在所述衬底上形成第一电极；
    在所述第一电极上形成空穴功能层；
    在所述空穴功能层上形成量子点发光层；
    在所述量子点发光层上形成电子功能层；以及
    在所述电子功能层上形成第二电极；
    或者，所述制备方法包括如下步骤：
    提供一衬底，在所述衬底上形成第二电极；
    在所述第二电极上形成电子功能层；
    在所述电子功能层上形成量子点发光层；
    在所述量子点发光层上形成空穴功能层；以及
    在所述空穴功能层上形成第一电极；
    其中，所述空穴功能层与所述量子点发光层之间设置有自组装分子层，或者所述电子功能层与所述量子点发光层之间设置有自组装分子层，或者所述空穴功能层与所述量子点发光层之间设置有自组装分子层且所述电子功能层与所述量子点发光层之间设置有自组装分子层。
  15. 根据权利要求14所述的制备方法，其中，设置于所述空穴功能层与所述量子点发光层之间的所述自组装分子层包括通式(R 1) 3NR 2X所示结构的化合物；
    在所述通式(R 1) 3NR 2X中，R 1为甲基或乙基，N为带正电荷的四价氮；X为卤素负离子或羧酸根；R 2选自烃基，含有芳基、羟基、巯基、酯、醚、胺、酰胺、磷、氧磷或硫醚的烃基，聚氧丙烯基，全氟烷基以及聚硅氧烷基中的一种或多种，R 2的碳原子数为4个至20个。
  16. 根据权利要求14或15所述的制备方法，其中，设置于所述空穴功能层与所述量子点发光层之间的所述自组装分子层包括通式R 3-R 4所示结构的化合物，在所述通式R 3-R 4中，R 3为苯酚基团或邻苯二酚基团；R 4选自烃基，含有芳基、羟基、巯基、酯、醚、胺、酰胺、磷、氧磷或硫醚的烃基，聚氧丙烯基，全氟烷基以及聚硅氧烷基中的一种或多种，R 4的碳原子数为4个至20个。
  17. 根据权利要求14至16任一项中所述的制备方法，其中，设置于所述电子功能层与所述量子点发光层之间的所述自组装分子层包括通式R 5-R 6所示结构的化合物；
    在所述通式R 5-R 6中，R 5选自氨基、巯基、羧基、羟基、羰基、酰胺基、磷、氧磷、有机磷、硫醚以及聚硅氧烷基中的一种或多种；R 6选自烃基，含有芳基、醚基的烃基，聚氧丙烯基以及全氟烷基中的一种或多种，R 6的碳原子数为4个至20个。
  18. 一种显示面板，其中，所述显示面板包括基板和以阵列的形式设置于所述基板表面的量子点发光二极管器件，所述量子点发光二极管器件包括依次 层叠设置的第一电极、空穴功能层、量子点发光层、电子功能层和第二电极；所述空穴功能层与所述量子点发光层之间设置有自组装分子层，或者所述电子功能层与所述量子点发光层之间设置有自组装分子层，或者所述空穴功能层与所述量子点发光层之间设置有自组装分子层且所述电子功能层与所述量子点发光层之间设置有自组装分子层。
  19. 根据权利要求18所述的显示面板，其中，设置于所述空穴功能层与所述量子点发光层之间的所述自组装分子层包括通式(R 1) 3NR 2X所示结构的化合物，在所述通式(R 1) 3NR 2X中，R 1为甲基或乙基，N为带正电荷的四价氮；X为卤素负离子或羧酸根；R 2选自烃基，含有芳基、羟基、巯基、酯、醚、胺、酰胺、磷、氧磷或硫醚的烃基，聚氧丙烯基，全氟烷基以及聚硅氧烷基中的一种或多种，R 2的碳原子数为4个至20个；
    或者，设置于所述空穴功能层与所述量子点发光层之间的所述自组装分子层包括通式R 3-R 4所示结构的化合物，在所述通式R 3-R 4中，R 3为苯酚基团或邻苯二酚基团；R 4选自烃基，含有芳基、羟基、巯基、酯、醚、胺、酰胺、磷、氧磷或硫醚的烃基，聚氧丙烯基，全氟烷基以及聚硅氧烷基中的一种或多种，R 4的碳原子数为4个至20个。
  20. 根据权利要求18或19所述的显示面板，其中，设置于所述电子功能层与所述量子点发光层之间的自组装分子层包括通式R 5-R 6所示结构的化合物，在所述通式R 5-R 6中，R 5选自氨基、巯基、羧基、羟基、羰基、酰胺基、磷、氧磷、有机磷、硫醚以及聚硅氧烷基中的一种或多种；R 6选自烃基，含有芳基、醚基的烃基，聚氧丙烯基以及全氟烷基中的一种或多种，R 6的碳原子数为4个至20个。
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CN112038497A (zh) * 2020-09-15 2020-12-04 京东方科技集团股份有限公司 量子点发光器件、其制作方法及量子点显示装置
KR20210048786A (ko) * 2019-10-24 2021-05-04 삼성전자주식회사 전계 발광 소자 및 이를 포함하는 표시 장치

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CN103441221A (zh) * 2013-09-16 2013-12-11 东南大学 基于石墨烯的柔性量子点发光二极管器件及其制备方法
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