CN111244308B - Quantum dot light emitting layer and quantum dot light emitting diode - Google Patents
Quantum dot light emitting layer and quantum dot light emitting diode Download PDFInfo
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Abstract
The invention belongs to the technical field of display, and particularly relates to a quantum dot light-emitting layer and a quantum dot light-emitting diode. The material of the quantum dot light emitting layer includes quantum dots and one or more ionic liquid materials dispersed between the quantum dots. The quantum dot light-emitting layer can be used for various electronic devices, such as quantum dot light-emitting diodes, organic light-emitting diodes, photoelectric sensors, photoelectric detectors, lasers, thin film transistors, complementary metal oxide semiconductor devices and the like.
Description
Technical Field
The invention belongs to the technical field of display, and particularly relates to a quantum dot light-emitting layer and a quantum dot light-emitting diode.
Background
Quantum dot light-emitting diodes (QLEDs) are an emerging display device, and the principle and structure of the QLEDs are similar to Organic light-emitting diodes (OLEDs): namely a flat panel display device which is driven by an external direct current electric field, excitons of the quantum dots and the organic/inorganic semiconductor emit light in a combined manner. Compared with OLED and QLED, the QLED has the characteristic that the luminescent material is quantum dots prepared by a colloid method. The unique quantum size effect, macroscopic quantum tunneling effect, quantum size effect and surface effect of the quantum dots enable the quantum dots to show excellent physical properties, especially excellent optical performance; compared with organic fluorescent dye, the colloidal quantum dot has the advantages of adjustable spectrum, high luminous intensity, high color purity, capability of exciting multicolor fluorescence by a single light source and the like, is expected to become a next-generation display, and has wide development prospect.
In the QLED device, the quantum dots and the metal nanoparticle transmission layer material commonly used in the device are generally prepared by a solution method, so the suitable process for the industrialization of the QLED in the industry is generally considered as an ink-jet printing method in the solution method, the preparation process is simple, the material utilization rate is low, the preparation efficiency is high, and the QLED device is considered as a new technology with great potential for future flat panel display. Although the QLED has many advantages compared with the OLED, as Quantum Dots (QDs), partial transport layer materials and the like are solution phase nanoparticles, compared with the mature evaporation process of an OLED film layer, the film forming performance is not easy to control, and the film layer problems such as incomplete coverage or "pinholes" are easy to occur, which not only can generate leakage current to the device and reduce the light emitting performance of the device, but also most importantly, the service life of the device can be greatly influenced by the defect regions. According to the research progress in the industry, the device efficiency of the QLED reaches the marketization level, but the problem of short device lifetime is the biggest bottleneck restricting the commercialization of the QLED, and the problem is also the key breakthrough point which is consistently and strively solved in the industry. At present, the service life of the device is improved by improving a packaging method, introducing an insulating polymer modification layer into an ETL/Cathodode interface and the like, but the improvement effect is not obvious, and the introduction of the insulating polymer layer can reduce the mobility of carriers instead, so that the balance of the carriers and the improvement of the service life are obtained on the basis of sacrificing part of the device performance, and the methods have certain effects but cannot well improve the service life of the device.
Therefore, the prior art is still in need of further research and development.
Disclosure of Invention
The invention aims to overcome the defects in the prior art, and provides a quantum dot light-emitting layer and a quantum dot light-emitting diode, aiming at solving the technical problems that the conventional quantum dot light-emitting layer is not uniform, and a 'pinhole' phenomenon occurs, so that the service life of a device is shortened.
In order to achieve the purpose, the invention adopts the following technical scheme:
the invention provides a quantum dot light-emitting layer, wherein the material of the quantum dot light-emitting layer comprises quantum dots and one or more ionic liquid materials dispersed among the quantum dots.
The quantum dot light-emitting layer provided by the invention is composed of quantum dots and one or more ionic liquid materials, and the ionic liquid materials have the characteristics of stable chemical properties, large cohesiveness, strong water and oxygen blocking capacity and the like, so that the quantum dot materials in the quantum dot light-emitting layer can be uniformly coated and tightly cohered together, the quantum dots are not easy to agglomerate, a uniform, compact, balanced and smooth quantum dot light-emitting layer with excellent stability is formed, meanwhile, the ionic liquid materials can passivate the surface defects of the quantum dots, and the fluorescence scintillation phenomenon of the quantum dots is reduced; therefore, the quantum dot light emitting layer can be used in various electronic devices, such as quantum dot light emitting diodes, organic light emitting diodes, photosensors, photodetectors, lasers, thin film transistors, complementary metal oxide semiconductor devices, and the like.
The invention also provides a quantum dot light-emitting diode which comprises an anode, a cathode and a quantum dot light-emitting layer arranged between the anode and the cathode, wherein the quantum dot light-emitting layer is the quantum dot light-emitting layer.
The quantum dot light emitting layer in the quantum dot light emitting diode is the special quantum dot light emitting layer, has the characteristics of uniformity, compactness, balance, smoothness and good stability, can avoid the defects of serious device leakage current and rapid service life attenuation caused by uneven film layers, thereby prolonging the service life of the device, and meanwhile, the ionic liquid has strong conductivity and good design property, so that the transmission barrier of carriers in the device can be reduced, the utilization rate of the carriers is improved, and the effect of improving the light emitting performance of the device is achieved.
Drawings
Fig. 1 is a material structure diagram of a quantum dot light emitting layer according to an embodiment of the present invention;
FIG. 2 is a diagram of a quantum dot light emitting diode according to an embodiment of the present invention;
fig. 3 is a structural diagram of a quantum dot light emitting diode according to an embodiment of the invention.
Detailed Description
In order to make the technical problems, technical solutions and advantageous effects to be solved by the present invention more clearly apparent, the present invention is further described in detail below with reference to the following embodiments. It should be understood that the specific embodiments described herein are merely illustrative of the invention and are not intended to limit the invention.
In one aspect, the present invention provides a quantum dot light emitting layer, as shown in fig. 1, the material of the quantum dot light emitting layer includes quantum dots and one or more ionic liquid materials dispersed between the quantum dots.
The quantum dot light-emitting layer provided by the embodiment of the invention is composed of quantum dots and one or more ionic liquid materials, and the ionic liquid materials have the characteristics of stable chemical properties, high cohesiveness, strong water and oxygen blocking capacity and the like, so that the quantum dot materials in the quantum dot light-emitting layer can be uniformly coated and tightly cohered together, the quantum dots are not easy to agglomerate, a uniform, compact, balanced and smooth quantum dot light-emitting layer with excellent stability is formed, and meanwhile, the ionic liquid materials can passivate the surface defects of the quantum dots and reduce the fluorescence scintillation phenomenon of the quantum dots; the quantum dot light-emitting layer can be used for various electronic devices, such as quantum dot light-emitting diodes, organic light-emitting diodes, photoelectric sensors, photoelectric detectors, lasers, thin film transistors, complementary metal oxide semiconductor devices and the like.
Further, in the quantum dot light-emitting layer of the embodiment of the present invention, the ionic liquid material is a salt composed of an organic cation and an inorganic anion; wherein the organic cation is selected from alkyl quaternary ammonium ions [ NRxH4-x]+Alkyl quaternary phosphonium ion [ PRxH4-x]+Alkyl-substituted imidazolium [ R ]1R3im]+Alkyl-substituted pyridinium ion [ RPy]+Wherein the inorganic anion is selected from one of halogen ion and inorganic acid anion;
by way of example, the quaternary alkylammonium ion is selected from one of the cations N, N-diethyl-N-methyl-N- (N-propyl) ammonium and N, N-diethyl-N-methyl- (2-methoxyethyl) ammonium; the alkyl quaternary phosphonium ion is selected from one of tetradecyl tributylphosphonium cation, tetramethylolphosphonium cation, ethyltributylphosphonium cation and tetrabutylphosphonium cation; the alkyl-substituted imidazolium is selected from one of 1-butyl-3-methylimidazole cation, 1-ethyl-3-methylimidazole cation, 1-octyl-3-methylimidazole cation, 1-decyl-3-methylimidazole cation, 1-hexyl-3-methylimidazole cation and 1-methyl-3-n-octylimidazole cation; the alkyl-substituted pyridine ions are selected from one of N-ethyl pyridine cations, N-butyl pyridine cations, N-hexyl pyridine cations, N-octyl pyridine cations and N-methyl-N-propyl pyridine cations.
In the embodiment of the invention, the ionic liquid is salt which is in a liquid state at room temperature or close to room temperature and completely consists of anions and cations, and is also called as low-temperature molten salt, and the ionic liquid has the outstanding advantages of strong conductivity, stable property, high heat resistance, low vapor pressure, non-flammability, greenness, no pollution, capability of adjusting various performances of materials through anion and cation design and the like. Further, because the quaternary alkyl ammonium ionic liquid and the alkyl-substituted imidazole ionic liquid have better electrochemical stability, the preferred organic cations in the embodiment of the present invention are quaternary alkyl ammonium ions and alkyl-substituted imidazole ions. I.e. the organic cation is selected from the group consisting of the N, N-diethyl-N-methyl-N- (N-propyl) ammonium cation, the N, N-diethyl-N-methyl- (2-methoxyethyl) ammonium cation, the 1-butyl-3-methylimidazole cation, the 1-ethyl-3-methylimidazole cation, the 1-octyl-3-methylimidazole cation, the 1-decyl-3-methylimidazole cation, the 1-hexyl-3-methylimidazole cation and the 1-methyl-3-N-octylimidazole cation. And the halide ion is selected from F-、Cl-、Br-And I-At least one of; the inorganic acid anion is selected from BF4 -、PF6 -、CF3SO3 -、CF3COO-、(CF3SO2)3C-、(C2F5SO2)3C-、(CF3SO2)2N-、C3F7COO-、C4F9SO3 -、(C2F5SO2)2N-、SbF6 -、AsF6 -、CB11H12 -、NO2 -、NO3 -、ClO4 -And C8H17SO4 -At least one of (1), preferably BF4 -、PF6 -、CF3SO3 -、CF3COO-。
Further, in the ionic liquid material of the embodiment of the present invention, the organic cation is an asymmetric cation; and/or hydrogen bonds are formed between the organic cations and the inorganic anions.
The important index for evaluating the practicability of the ionic liquid is the melting point of the ionic liquid, and the structure of the ionic liquid and the melting point of the ionic liquid have a decisive relationship and are directly related to the use temperature range of the ionic liquid. Under the condition that the cations are the same, the melting point is gradually reduced along with the increase of the volume of the anions, and the influence of the cations on the melting point can be known by comparing the melting points of different chlorides. In the case of the same anion, the melting point gradually decreases with increasing volume of the cation. Also, in order to remain liquid at room temperature, the ionic liquid is preferably asymmetric. The lower the structural symmetry of the ionic liquid, the weaker the intermolecular forces, the more uniform the cationic or anionic charge distribution, and the lower the melting point of the ionic liquid.
The order of the melting points of the anion generating compounds from large to small is: cl->NO2 ->NO3 ->AlCl4 ->BF4 ->CF3SO3>CF3CO2 -。
The viscosity of the ionic liquid at normal temperature is dozens of times to hundreds of times of that of water. The structure of the anions and cations has a great influence on the viscosity of the ionic liquid: the carbon chain length of the substituent of the cation increases the viscosity of the ionic liquid, for example, the ionic liquid with the cation [ bmin ] has much higher viscosity than [ emin ]; the alkyl branching of the substituent group increases the viscosity of the ionic liquid, for example, the ionic liquid with cation [ ibmin ] has higher viscosity than [ bmin ]; in addition, the viscosity of the ionic liquid is mainly determined by Van der Waals force and hydrogen bond action, the volume of anions is reduced, the Van der Waals force is reduced, the electrostatic action is increased, and the viscosity is reduced; the anion has high alkalinity and low viscosity, such as the anion of [ emin ] F (HF) n has high alkalinity and the viscosity is minimum. Therefore, after the cation and the anion form hydrogen bonds, the viscosity of the ionic liquid is increased; the relationship between the viscosity and the temperature of the ionic liquid is expressed by a Vogel-Tammann-Fulchers equation.
In conclusion, the organic cation is asymmetric cation, and the ionic liquid material with hydrogen bond formed between the organic cation and the inorganic anion not only ensures low melting point, but also has good viscosity.
Preferably, ionic liquids of embodiments of the present invention include, but are not limited to, 1-butyl-3-methylimidazolium tetrafluoroborate ([ BMIM ]]BF4), 1-butyl-3-methylimidazolium hexafluorophosphate ([ BMIM)]PF6), 1-ethyl-3-methylimidazolium hexafluorophosphate ([ EMIM)]PF6), 1-ethyl-3-methylimidazolium bistrifluoromethylsulfonyl imide salt ([ EMIM ])]TFSI), 1-octyl-3-methylimidazolium hexafluorophosphate ([ OMIM)]PF6), 1-ethyl-3-methylimidazole chloride ([ EMIM)]Cl), 1-decyl-3-methylimidazolium hexafluorophosphate ([ DMIM)]PF6), 1-ethyl-3-methylimidazolium bis (pentafluoroethylsulfonyl) imide ([ EMIM)]BETI), 1-hexyl-3-methylimidazolium tetrafluoroborate ([ C6 MIM)]BF4), 1-methyl-3-n-octyl imidazole tetrafluoroborate ([ C8 MIM)]BF4), fluoromethylsulfamidophosphine ([ P14)][TF2N]) 1-Ethyl-3-methylimidazolium bistrifluoromethylsulfonyl imide salt ([ EMIM ]]TF2N), 1-ethyl-3-methylimidazolium dicyanamide ([ EMIM)]DCA), N-diethyl-N-methyl-N- (N-propyl) trifluoromethyl ammonium trifluoroborate ([ Et)2PrNMe]CF3BF3) 1-butyl-3-methylimidazolium trifluoromethanesulfonate ([ BMIM ]]OTF), N-diethyl-N-methyl-N- (2-methoxyethyl) ammonio bis (trifluoromethylsulfonyl) imide ([ DEME)]TFSI), N-diethyl-N-methyl-N- (2-methoxyethyl) quaternary ammonium tetrafluoroborate ([ DEME ]]BF4) One or more of (a).
Furthermore, in the quantum dot light-emitting layer provided by the embodiment of the invention, the mass ratio of the one or more ionic liquid materials to the quantum dots is 1 (3-250). Within the mass ratio range, the ionic liquid material has a better modification effect on the quantum dots, and most preferably, the mass ratio of the one or more ionic liquid materials to the quantum dots is 1 (5-50).
Further, the quantum dot light-emitting layer also comprises organic molecules for dispersion. The organic molecules enable the quantum dots and the ionic liquid material to be dispersed more uniformly, and a more uniform quantum dot light-emitting layer is formed. The organic molecule is selected from at least one of oleic acid, thioglycolic acid, octadecenoic acid, octadecylphosphonic acid, mercaptoundecanoic acid, thioglycolic acid, 3-mercaptopropionic acid, 3-mercaptobutyric acid, 6-mercaptohexanoic acid, 4-mercaptobenzoic acid, mercaptophenylacetic acid, nitrobenzenesulfonic acid, terephthalic acid, terephthaloic acid, aminobenzoic acid, 4- (diphenylphosphino) benzoic acid, 9-octadecenylamine, octadecylamine, phenylenediamine, mercaptoaniline, nitroaniline, sulfoaniline, mercaptoethylamine, mercaptopropylamine, 1, 2-ethylenediamine, 1, 3-propylenediamine, 1, 4-butanediamine, 1, 5-pentanediamine, 1, 6-hexanediamine, trioctylamine, oleylamine, and ethanolamine. The organic molecules are combined on the surfaces of the quantum dots through coordination, so that the dispersibility of the quantum dots is improved, and the ionic liquid and the quantum dots are well and uniformly dispersed. Preferably, the organic molecule is selected from organic molecules having coordination and certain acidity and alkalinity. Preferably, the mass of the organic molecule is 0.01 to 7 wt% of the total mass of the quantum dot and the ionic liquid material. More preferably, the mass of the organic molecule is 1-5 wt% of the total mass of the quantum dot and the ionic liquid material, so that the organic molecule has the best dispersion effect.
On the other hand, the embodiment of the invention provides a preparation method of a quantum dot light-emitting layer, which comprises the following steps:
s01: providing a substrate, and preparing a solution containing quantum dots and one or more ionic liquid materials;
s02: and depositing the solution on the substrate, and then carrying out annealing treatment to obtain the quantum dot light-emitting layer.
The preparation method of the quantum dot light-emitting layer provided by the embodiment of the invention has the advantages that the process is simple, the cost is low, and the prepared solution containing the quantum dots and the ionic liquid material is deposited on the substrate for annealing, so that the quantum dot light-emitting layer which is uniform, compact, balanced, smooth and excellent in stability can be obtained.
Further, in step S01, the substrate may be a substrate for preparing a quantum dot light emitting diode, and if the substrate is provided with an anode and a hole functional layer from bottom to top, the quantum dot light emitting layer is directly prepared on the hole functional layer, that is, the quantum dot light emitting layer; if the substrate is provided with the cathode and the electronic functional layer from bottom to top, the quantum dot light-emitting layer is directly prepared on the electronic functional layer, namely the quantum dot light-emitting layer.
Further, preparing the solution according to the mass ratio of the one or more ionic liquid materials to the quantum dots being 1 (3-250); more preferably, the solution is prepared according to the mass ratio of the one or more ionic liquid materials to the quantum dots being 1 (5-50); the quantum dot luminescent layer prepared in the proportion range has the best modification effect of the ionic liquid material on the quantum dots.
Further, the ionic liquid material is a salt composed of an organic cation and an inorganic anion; wherein the organic cation is at least one selected from alkyl quaternary ammonium ion, alkyl quaternary phosphonium ion, alkyl substituted imidazolium ion and alkyl substituted pyridinium ion, and the inorganic anion is at least one selected from halogen ion and inorganic acid anion; preferably, the quaternary alkyl ammonium ion is selected from at least one of N, N-diethyl-N-methyl-N- (N-propyl) ammonium cation and N, N-diethyl-N-methyl- (2-methoxyethyl) ammonium cation, the quaternary alkyl phosphonium ion is selected from one of tetradecyltributylphosphonium cation, tetramethylolphosphonium cation, ethyltributylphosphonium cation, tetrabutylphosphonium cation, the alkyl substituted imidazolium ion is selected from at least one of 1-butyl-3-methylimidazolium cation, 1-ethyl-3-methylimidazolium cation, 1-octyl-3-methylimidazolium cation, 1-decyl-3-methylimidazolium cation, the alkyl substituted pyridinium ion is selected from N-ethylpyridinium cation, N-diethylphosphonium cation, N-methyl- (2-methoxyethyl) ammonium cation, and N, N-diethyl-N-methyl- (2-methoxyethyl) ammonium cation, The selection of one of the ionic liquids N-butylpyridinium, N-hexylpyridinium, N-octylpyridinium, N-methyl-N-propylpyridinium cations has been described in detail above.
Further, in the above step S02, a solution containing the organic molecules for dispersion, the quantum dots, and the ionic liquid material is prepared, the solution is deposited on the substrate, and then an annealing treatment is performed. Wherein the organic molecule is selected from at least one of oleic acid, thioglycolic acid, octadecenoic acid, octadecylphosphonic acid, mercaptoundecanoic acid, thioglycolic acid, 3-mercaptopropionic acid, 3-mercaptobutyric acid, 6-mercaptohexanoic acid, 4-mercaptobenzoic acid, mercaptophenylacetic acid, nitrobenzenesulfonic acid, terephthalic acid, p-phenylenediacetic acid, aminobenzoic acid, 4- (diphenylphosphino) benzoic acid, 9-octadecylamine, phenylenediamine, mercaptoaniline, nitroaniline, sulfoaniline, mercaptoethylamine, mercaptopropylamine, 1, 2-ethylenediamine, 1, 3-propylenediamine, 1, 4-butylenediamine, 1, 5-pentylenediamine, 1, 6-hexylenediamine, trioctylamine, oleylamine, and ethanolamine. The organic molecule is preferably an organic molecule which has a coordination function and has certain acidity and alkalinity, the organic molecule is added into the organic molecule to prepare a solution, the pH value of the mixed solution is adjusted, and the uniform dispersion of the quantum dot material is maintained, so that the uniform dispersion of the quantum dot in the solution (or the quantum dot ink) can be improved. The mass of the organic molecule is 0.01-7 wt% of the total mass of the quantum dot and the ionic liquid material. More preferably, the mass of the organic molecule is 1-5 wt% of the total mass of the quantum dot and the ionic liquid material, so that the organic molecule has the best dispersion effect.
Furthermore, the temperature of the annealing treatment is 25-120 ℃; the annealing treatment time is 5-60 min. The purpose of the annealing treatment is to volatilize the solvent in the solution and promote uniform densification of the film. The annealing temperature is not too high, mainly considering the stability of the quantum dot material, if the temperature is higher than 120 ℃, ligands on the surface of the quantum dot are easy to fall off, so that the performance of a device is reduced, and for the added ionic liquid, generally, the ionic liquid is carbonized and decomposed only when the temperature exceeds 400 ℃, and because the ionic liquid has good thermal stability, the ionic liquid can stably exist in the temperature range which can be borne by the quantum dot material and cannot be changed, the annealing temperature range of 25-120 ℃ does not influence the quantum dot and the ionic liquid.
The preparation method of the quantum dot light-emitting layer pair of the embodiment of the invention may be a solution film-forming method, including but not limited to one or more of a spin coating method, a printing method, a blade coating method, a dip-draw method, a dipping method, a spray coating method, a roll coating method, a casting method, a slit coating method, and a strip coating method.
In the above preparation method according to the embodiment of the present invention, the solvent used for preparing the solution is an organic solvent, and includes, but is not limited to, one or a mixture of a plurality of saturated hydrocarbons, unsaturated hydrocarbons, aromatic hydrocarbons, alcohol solvents, ether solvents, ketone solvents, nitrile solvents, ester solvents, and derivatives thereof. Wherein the organic solvent includes, but is not limited to, hexane, cyclohexane, heptane, n-octane, isooctane, pentane, methylpentane, ethylpentane, cyclopentane, methylcyclopentane, ethylcyclopentane, benzene, toluene, xylene, ethylbenzene, dichloromethane, trichloromethane, carbon tetrachloride, dichloroethane, trichloroethane, chloropropane, dichloropropane, trichloropropane, chlorobutane, dibromomethane, tribromomethane, bromoethane, bromopropane, iodomethane, chlorobenzene, bromobenzene, benzyl chloride, benzyl bromide, trifluorotoluene, methanol, ethanol, propanol, isopropanol, butanol, isobutanol, sec-butanol, tert-butanol, pentanol, isopentanol, tert-pentanol, cyclohexanol, octanol, benzyl alcohol, ethylene glycol, phenol, o-cresol, diethyl ether, anisole, phenetole, diphenyl ether, tetrahydrofuran, ethylene glycol dimethyl ether, propylene glycol methyl ether, ethylene glycol diethyl ether, At least one of hydroxyethyl ether, propylene glycol monopropyl ether, propylene glycol monobutyl ether, acetaldehyde, benzaldehyde, acetone, butanone, cyclohexanone, acetophenone, formic acid, acetic acid, ethyl acetate, diethyl oxalate, diethyl malonate, propyl acetate, methyl propyl ester, butyl acetate, methyl amyl acetate, nitrobenzene, acetonitrile, diethylamine, triethylamine, aniline, pyridine, picoline, ethylenediamine, N-dimethylformamide, N-dimethylacetamide, N-methylpyrrolidone, dimethyl sulfoxide, hexamethylphosphoramide, carbon disulfide, methyl sulfide, ethyl sulfide, dimethyl sulfoxide, mercaptan, ethanethiol, and methoxytetrahydrofuran.
Finally, an embodiment of the present invention provides a quantum dot light emitting diode, which includes an anode, a cathode, and a quantum dot light emitting layer disposed between the anode and the cathode, where the quantum dot light emitting layer is the quantum dot light emitting layer according to the embodiment of the present invention.
The quantum dot light-emitting layer in the quantum dot light-emitting diode provided by the embodiment of the invention is the special quantum dot light-emitting layer, the quantum dot light-emitting layer has the characteristics of uniformity, compactness, balance, smoothness and good stability, and can avoid the defects of serious device leakage current and rapid service life attenuation caused by uneven film layers, so that the service life of the device is prolonged.
Furthermore, a hole injection layer and/or a hole transmission layer are/is arranged between the quantum dot light-emitting layer and the anode; an electron transmission layer is arranged between the quantum dot light-emitting layer and the cathode. Fig. 2 and fig. 3 are schematic structural diagrams of two different types of qd-led pairs according to embodiments of the present invention.
Wherein, the cathode includes but is not limited to one or more of metal material, carbon material and metal oxide. Wherein the metal material comprises one or more of Al, Ag, Cu, Mo, Au, Ba, Ca and Mg. The carbon material comprises one or more of graphite, carbon nanotubes, graphene and carbon fibers. The metal oxide can be doped or undoped metal oxide, including one or more of ITO, FTO, ATO, AZO, GZO, IZO, MZO and AMO, and also including a composite electrode sandwiching metal between doped or undoped transparent metal oxides, wherein the composite electrode includes AZO/Ag/AZO, AZO/Al/AZO, ITO/Ag/ITO, ITO/Al/ITO, ZnO/Ag/ZnO, ZnO/Al/ZnO, TiO/Al/ZnO2/Ag/TiO2、TiO2/Al/TiO2、ZnS/Ag/ZnS、ZnS/Al/ZnS、TiO2/Ag/TiO2、TiO2/Al/TiO2One or more of (a).
Wherein the electron transport layer is selected from inorganic material and/or organic material with electron transport capability, wherein the inorganic electron transport layer is selected from doped or undoped metal oxide, doped or undoped metal sulfideOne or more of them. Wherein the doped or undoped metal oxide comprises ZnO and TiO2、SnO2、Ta2O3、ZrO2One or more of NiO, TiLiO, ZnAlO, ZnMgO, ZnSnO, ZnLiO and InSnO. The doped or undoped metal sulfide comprises one or more of CdS, ZnS, MoS, WS and CuS.
The quantum dot material of the quantum dot light-emitting layer is one or more of II-VI compound, III-V compound, II-V compound, III-VI compound, IV-VI compound, I-III-VI compound, II-IV-VI compound or IV elementary substance. Specifically, the semiconductor materials used for the quantum dot light emitting layer include, but are not limited to, nanocrystals of II-VI semiconductors such as CdS, CdSe, CdTe, ZnS, ZnSe, ZnTe, HgS, HgSe, HgTe, PbS, PbSe, PbTe and other binary, ternary, quaternary II-VI compounds; nanocrystals of group III-V semiconductors such as GaP, GaAs, InP, InAs and other binary, ternary, quaternary III-V compounds; the semiconductor material for electroluminescence is not limited to group II-V compounds, group III-VI compounds, group IV-VI compounds, group I-III-VI compounds, group II-IV-VI compounds, group IV simple substance, and the like.
The quantum dot material of the quantum dot light-emitting layer can also be a doped or undoped inorganic perovskite type semiconductor and/or an organic-inorganic hybrid perovskite type semiconductor; specifically, the structural general formula of the inorganic perovskite type semiconductor is AMX3Wherein A is Cs+Ion, M is a divalent metal cation, including but not limited to Pb2+、Sn2+、Cu2+、Ni2+、Cd2+、Cr2+、Mn2+、Co2+、Fe2+、Ge2+、Yb2+、Eu2+X is a halide anion, including but not limited to Cl-、Br-、I-(ii) a The structural general formula of the organic-inorganic hybrid perovskite type semiconductor is BMX3Wherein B is an organic amine cation including but not limited to CH3(CH2)n-2NH3 +(n.gtoreq.2) or NH3(CH2)nNH3 2+(n.gtoreq.2). When n is 2, the inorganic metal halide octahedron MX6 4-The metal cations M are positioned in the center of a halogen octahedron through connection in a roof sharing mode, and the organic amine cations B are filled in gaps among the octahedrons to form an infinitely extending three-dimensional structure; inorganic metal halide octahedra MX linked in a coterminous manner when n > 26 4-The organic amine cation bilayer (protonated monoamine) or the organic amine cation monolayer (protonated diamine) is inserted between the layers, and the organic layer and the inorganic layer are overlapped with each other to form a stable two-dimensional layered structure; m is a divalent metal cation including, but not limited to, Pb2+、Sn2+、Cu2+、Ni2+、Cd2+、Cr2+、Mn2+、Co2+、Fe2+、Ge2+、Yb2+、Eu2 +(ii) a X is a halide anion, including but not limited to Cl-、Br-、I。
Wherein, the material of the hole transport layer and/or the hole injection layer comprises but is not limited to one or more of PEDOT, PSS, CuPc, F4-TCNQ, HATCN, transition metal oxide and transition metal chalcogenide compound. Wherein the transition metal oxide comprises one or more of NiOx, MoOx, WOx, CrOx and CuO. The metal sulfur compound comprises one or more of MoSx, MoSex, WSx, WSex and CuS. The hole transport layer materials include, but are not limited to, poly (9, 9-dioctylfluorene-CO-N- (4-butylphenyl) diphenylamine), polyvinylcarbazole, poly (N, N ' bis (4-butylphenyl) -N, N ' -bis (phenyl) benzidine), poly (9, 9-dioctylfluorene-CO-bis-N, N-phenyl-1, 4-phenylenediamine), 4', 4 ″ -tris (carbazol-9-yl) triphenylamine, 4' -bis (9-carbazol) biphenyl, N ' -diphenyl-N, N ' -bis (3-methylphenyl) -1,1 ' -biphenyl-4, 4' -diamine, 15N, N ' -diphenyl-N, at least one of N ' - (1-naphthyl) -1,1 ' -biphenyl-4, 4' -diamine, graphene and C60. As another embodiment, the hole transport layer is selected from inorganic materials having hole transport capability, including but not limited to at least one of NiOx, MoOx, WOx, CrOx, CuO, MoSx, MoSex, WSx, WSex, CuS.
Wherein, the anode comprises one or more of but not limited to metal materials, carbon materials, metal oxides and hole injection materials. Wherein the metal material comprises one or more of Al, Ag, Cu, Mo, Au, Ba, Ca and Mg. The carbon material comprises one or more of graphite, carbon nanotubes, graphene and carbon fibers. The metal oxide can be doped or undoped metal oxide, including one or more of ITO, FTO, ATO, AZO, GZO, IZO, MZO and AMO, and also including a composite electrode sandwiching metal between doped or undoped transparent metal oxides, wherein the composite electrode includes AZO/Ag/AZO, AZO/Al/AZO, ITO/Ag/ITO, ITO/Al/ITO, ZnO/Ag/ZnO, ZnO/Al/ZnO, TiO/Al/ZnO2/Ag/TiO2、TiO2/Al/TiO2、ZnS/Ag/ZnS、ZnS/Al/ZnS、TiO2/Ag/TiO2、TiO2/Al/TiO2One or more of (a). The hole injection material comprises but is not limited to one or more of PEDOT PSS, CuPc, F4-TCNQ, HATCN, transition metal oxide and transition metal chalcogenide compound. Wherein the transition metal oxide comprises one or more of NiOx, MoOx, WOx, CrOx and CuO. The metal sulfur compound comprises one or more of MoSx, MoSex, WSx, WSex and CuS.
Wherein the substrate is a rigid substrate or a flexible substrate, wherein the rigid substrate includes but is not limited to one or more of glass and metal foil; the flexible substrate includes, but is not limited to, one or more of polyethylene terephthalate (PET), polyethylene terephthalate (PEN), Polyetheretherketone (PEEK), Polystyrene (PS), Polyethersulfone (PES), Polycarbonate (PC), Polyarylate (PAT), Polyarylate (PAR), Polyimide (PI), polyvinyl chloride (PV), Polyethylene (PE), polyvinylpyrrolidone (PVP), and textile fibers.
Specifically, the preparation of the quantum dot light emitting diode of the embodiment of the invention comprises the following steps:
step S1: preparing a bottom electrode on a substrate;
step S2: preparing a first functional layer on the bottom electrode;
step S3: preparing an ionic liquid modified quantum dot light-emitting layer on the first functional layer;
step S4: preparing a second functional layer on the quantum dot light-emitting layer;
step S5: preparing a top electrode on the second functional layer;
the quantum dot light emitting diode comprises a substrate, a bottom electrode, a first functional layer, a quantum dot light emitting layer, a second functional layer and a top electrode which are sequentially arranged. For a positive-type structure device, the bottom electrode is an anode, the top electrode is a cathode, and the first functional layer is a hole injection layer and/or a hole transport layer; the second functional layer is an electron transport layer. For a device with an inversion structure, the bottom electrode is a cathode, the top electrode is an anode, and the first functional layer is an electron transport layer; the second functional layer is a hole transport layer and/or a hole injection layer. The quantum dot light emitting diode may be packaged partially, fully or not, and the embodiment of the present invention is not limited strictly.
Besides the above special description, the preparation method of each layer of the quantum dot light-emitting diode can be a chemical method or a physical method, wherein the chemical method includes but is not limited to one or more of a chemical vapor deposition method, a continuous ion layer adsorption and reaction method, an anodic oxidation method, an electrolytic deposition method and a coprecipitation method; physical methods include, but are not limited to, physical coating methods or solution methods, wherein solution methods include, but are not limited to, spin coating, printing, knife coating, dip-coating, dipping, spraying, roll coating, casting, slot coating, bar coating; physical coating methods include, but are not limited to, one or more of thermal evaporation coating, electron beam evaporation coating, magnetron sputtering, multi-arc ion coating, physical vapor deposition, atomic layer deposition, pulsed laser deposition.
Finally, the embodiment of the invention also provides a printed quantum dot display screen which comprises the quantum dot light-emitting diode.
The invention is described in further detail with reference to a part of the test results, which are described in detail below with reference to specific examples.
Example 1
A quantum dot light-emitting diode is prepared by the following steps:
first [ BMIM ]]BF4Adding into CdSe/ZnS quantum dot n-octane solution to prepare [ BMIM ]]BF4Mixed solution with CdSe/ZnS, wherein the concentration of CdSe/ZnS is 30mg/mL, [ BMIM ]]BF4The mass ratio of the CdSe @ ZnS to the CdSe @ ZnS is 1:27, and then the device is prepared according to the following steps:
spin-coating a PEDOT (PSS) hole injection layer on the ITO conductive glass;
spin-coating a TFB hole transport layer on a PEDOT/PSS hole injection layer;
will be described in [ BMIM]BF4Spin coating the mixed solution with CdSe/ZnS on the TFB hole transport layer at 3000rpm/s, and heating at 80 deg.C for 15min to obtain a dense layer of [ BMIM ]]BF4-a CdSe/ZnS ionic liquid modified quantum dot light emitting layer;
in [ BMIM ]]BF4A ZnO electron transmission layer is coated on the CdSe/ZnS ionic liquid modified quantum dot light-emitting layer in a spin coating mode;
and evaporating and plating an Al anode layer on the ZnO electron transmission layer to obtain the quantum dot light-emitting diode.
Example 2
A quantum dot light-emitting diode is prepared by the following steps:
first [ BMIM ]]BF4Adding into CdSe/ZnS quantum dot n-octane solution, adding oleylamine, and making into oleylamine, [ BMIM ]]BF4Mixed solution with CdSe/ZnS, wherein the concentration of CdSe/ZnS is 30mg/mL, [ BMIM ]]BF4The mass ratio of the metal oxide to CdSe @ ZnS is 1:27, the mass ratio of the added oleylamine is 0.5 wt%, and then the device is prepared according to the following steps:
spin-coating a PEDOT (PSS) hole injection layer on the ITO conductive glass;
spin-coating a TFB hole transport layer on a PEDOT/PSS hole injection layer;
mixing the above oleylamine, [ BMIM ]]BF4Mixed solution with CdSe/ZnS at 3000rpm/s spin coating on TFB hole transport layer, heating at 80 deg.C for 15min to obtain a compact [ BMIM ]]BF4-a CdSe/ZnS ionic liquid modified quantum dot light emitting layer;
spin-coating a ZnO electron transport layer on the [ BMIM ] BF4-CdSe/ZnS ionic liquid modified quantum dot light-emitting layer;
and evaporating and plating an Al anode layer on the ZnO electron transmission layer to obtain the quantum dot light-emitting diode. [
The above description is only for the purpose of illustrating the preferred embodiments of the present invention and is not to be construed as limiting the invention, and any modifications, equivalents and improvements made within the spirit and principle of the present invention are intended to be included within the scope of the present invention.
Claims (11)
1. A quantum dot light-emitting layer, wherein the material of the quantum dot light-emitting layer comprises quantum dots, one or more ionic liquid materials dispersed among the quantum dots, and organic molecules for dispersion; the mass ratio of the one or more ionic liquid materials to the quantum dots is 1 (3-250), the mass of the organic molecules is 0.01-7 wt% of the total mass of the quantum dots and the one or more ionic liquid materials, and the organic molecules are combined on the surfaces of the quantum dots through coordination.
2. The quantum dot light emitting layer of claim 1, wherein the ionic liquid material is a salt of an organic cation and an inorganic anion; wherein the content of the first and second substances,
the organic cation is selected from one of alkyl quaternary ammonium ion, alkyl quaternary phosphonium ion, alkyl substituted imidazolium ion and alkyl substituted pyridinium ion, and the inorganic anion is selected from one of halogen ion and inorganic acid anion.
3. The quantum dot light emitting layer of claim 2, wherein the alkyl quaternary ammonium ion is selected from one of a N, N-diethyl-N-methyl-N- (N-propyl) ammonium cation and a N, N-diethyl-N-methyl- (2-methoxyethyl) ammonium cation; alternatively, the first and second electrodes may be,
the alkyl quaternary phosphonium ion is selected from one of tetradecyl tributylphosphonium cation, tetramethylolphosphonium cation, ethyltributylphosphonium cation and tetrabutylphosphonium cation; alternatively, the first and second electrodes may be,
the alkyl-substituted imidazolium is selected from one of 1-butyl-3-methylimidazole cation, 1-ethyl-3-methylimidazole cation, 1-octyl-3-methylimidazole cation, 1-decyl-3-methylimidazole cation, 1-hexyl-3-methylimidazole cation and 1-methyl-3-n-octylimidazole cation; alternatively, the first and second electrodes may be,
the alkyl-substituted pyridinium ion is selected from one of N-ethyl pyridinium cation, N-butyl pyridinium cation, N-hexyl pyridinium cation, N-octyl pyridinium cation and N-methyl-N-propyl pyridinium cation.
4. The quantum dot light emitting layer of claim 2, wherein the halide ion is selected from F-、Cl-、Br-And I-One of (1); and/or
The inorganic acid anion is selected from BF4 -、PF6 -、CF3SO3 -、CF3COO-、(CF3SO2)3C-、(C2F5SO2)3C-、(CF3SO2)2N-、C3F7COO-、C4F9SO3 -、(C2F5SO2)2N-、SbF6 -、AsF6 -、CB11H12 -、NO2 -、NO3 -、ClO4 -And C8H17SO4 -One kind of (1).
5. The quantum dot light emitting layer of claim 2, wherein the organic cation is an asymmetric cation; and/or
Hydrogen bonds are formed between the organic cations and the inorganic anions.
6. The quantum dot light emitting layer of claim 2, wherein the organic cation is selected from one of alkyl quaternary ammonium ions and alkyl substituted imidazolium ions.
7. The quantum dot light emitting layer of claim 1, wherein the ionic liquid material is selected from the group consisting of 1-butyl-3-methylimidazolium tetrafluoroborate, 1-butyl-3-methylimidazolium hexafluorophosphate, 1-ethyl-3-methylimidazolium bistrifluoromethylsulfonyl imide, 1-octyl-3-methylimidazolium hexafluorophosphate, 1-ethyl-3-methylimidazolium chloride, 1-decyl-3-methylimidazolium hexafluorophosphate, 1-ethyl-3-methylimidazolium bis (pentafluoroethylsulfonyl) imide, 1-hexyl-3-methylimidazolium tetrafluoroborate, 1-methyl-3-n-octylimidazolium tetrafluoroborate, mixtures thereof, and mixtures thereof, 1-ethyl-3-methylimidazolidinedicyanamide, N-diethyl-N-methyl-N- (N-propyl) trifluoromethylammonium trifluoroborate, 1-butyl-3-methylimidazolium trifluoromethanesulfonate, N-diethyl-N-methyl-N- (2-methoxyethyl) ammoniumbis (trifluoromethanesulfonyl) imide and one of N, N-diethyl-N-methyl-N- (2-methoxyethyl) quaternary ammonium tetrafluoroborate.
8. The quantum dot light-emitting layer of claim 1, wherein the mass ratio of the one or more ionic liquid materials to the quantum dot is 1 (5-50).
9. The quantum dot light emitting layer of claim 1, wherein the organic molecule is selected from at least one of oleic acid, thioglycolic acid, octadecenoic acid, octadecylphosphonic acid, mercaptoundecanoic acid, 3-mercaptopropionic acid, 3-mercaptobutyric acid, 6-mercaptohexanoic acid, 4-mercaptobenzoic acid, mercaptophenylacetic acid, nitrobenzenesulfonic acid, terephthalic acid, terephthaloic acid, aminobenzoic acid, 4- (diphenylphosphino) benzoic acid, 9-octadecylamine, phenylenediamine, mercaptoaniline, nitroaniline, sulfoaniline, mercaptoethylamine, mercaptopropylamine, 1, 2-ethylenediamine, 1, 3-propylenediamine, 1, 4-butanediamine, 1, 5-pentanediamine, 1, 6-hexanediamine, trioctylamine, oleylamine, and ethanolamine.
10. The quantum dot light emitting layer of claim 1, wherein the mass of the organic molecule is 1 to 5 wt% of the total mass of the quantum dot and the ionic liquid material.
11. A quantum dot light emitting diode comprising an anode, a cathode and a quantum dot light emitting layer disposed between the anode and the cathode, wherein the quantum dot light emitting layer is the quantum dot light emitting layer of any one of claims 1-10.
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