WO2003022955A1 - Dispositif electroluminescent organique comportant une couche de transport de trous contenant un polyimide - Google Patents

Dispositif electroluminescent organique comportant une couche de transport de trous contenant un polyimide Download PDF

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Publication number
WO2003022955A1
WO2003022955A1 PCT/KR2001/001531 KR0101531W WO03022955A1 WO 2003022955 A1 WO2003022955 A1 WO 2003022955A1 KR 0101531 W KR0101531 W KR 0101531W WO 03022955 A1 WO03022955 A1 WO 03022955A1
Authority
WO
WIPO (PCT)
Prior art keywords
bis
electroluminescent device
formula
dianhydride
polyimide
Prior art date
Application number
PCT/KR2001/001531
Other languages
English (en)
Inventor
Dong Keun Choi
Young Kyoo Kim
Ki Jong Han
Original Assignee
Nessdisplay Co., Ltd.
Priority date (The priority date is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the date listed.)
Filing date
Publication date
Application filed by Nessdisplay Co., Ltd. filed Critical Nessdisplay Co., Ltd.
Priority to PCT/KR2001/001531 priority Critical patent/WO2003022955A1/fr
Publication of WO2003022955A1 publication Critical patent/WO2003022955A1/fr

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Classifications

    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08G—MACROMOLECULAR COMPOUNDS OBTAINED OTHERWISE THAN BY REACTIONS ONLY INVOLVING UNSATURATED CARBON-TO-CARBON BONDS
    • C08G73/00—Macromolecular compounds obtained by reactions forming a linkage containing nitrogen with or without oxygen or carbon in the main chain of the macromolecule, not provided for in groups C08G12/00 - C08G71/00
    • C08G73/06—Polycondensates having nitrogen-containing heterocyclic rings in the main chain of the macromolecule
    • C08G73/10—Polyimides; Polyester-imides; Polyamide-imides; Polyamide acids or similar polyimide precursors
    • C08G73/1042—Copolyimides derived from at least two different tetracarboxylic compounds or two different diamino compounds
    • C—CHEMISTRY; METALLURGY
    • C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
    • C09K—MATERIALS FOR MISCELLANEOUS APPLICATIONS, NOT PROVIDED FOR ELSEWHERE
    • C09K11/00—Luminescent, e.g. electroluminescent, chemiluminescent materials
    • C09K11/06—Luminescent, e.g. electroluminescent, chemiluminescent materials containing organic luminescent materials
    • 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
    • H10K85/10—Organic polymers or oligomers
    • H10K85/111—Organic polymers or oligomers comprising aromatic, heteroaromatic, or aryl chains, e.g. polyaniline, polyphenylene or polyphenylene vinylene
    • 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
    • H10K85/10—Organic polymers or oligomers
    • H10K85/151—Copolymers
    • 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
    • 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
    • H10K85/631—Amine compounds having at least two aryl rest on at least one amine-nitrogen atom, e.g. triphenylamine

Definitions

  • the present invention is directed to an organic electroluminescent device having a polyimide hole transport layer; and, more particularly, to an organic electroluminescent device having an improved stability and prolonged lifetime, which contains a polyimide derived from a triphenyldiamine derivative having a hole transport capability.
  • an organic electroluminescent device has a laminated structure comprising a transparent electrode layer, a metallic electrode layer, and an organic interlayer including an organic luminescent layer arranged between the two electrodes.
  • the organic interlayer comprising an organic luminescent layer may further include a hole transport layer sandwiched between the transparent electrode layer and the organic luminescent layer, and may still further include an electron transport layer inserted between the metallic electrode layer and the organic luminescent layer, often in a multilayer configuration to increase luminous efficiency.
  • N,N'-diphenyl-N,N'-bis(3-methylphenyl)- 1 , 1 '-diphenyl-4,4'-diamine(TPD), N-phenylcarbazole and 4,4'-bis[N-(l-naphthyl)-N-phenylamino]biphenyl (NPB) have been used in forming a hole transport layer.
  • TPD N-phenylcarbazole
  • PBD 4,4'-bis[N-(l-naphthyl)-N-phenylamino]biphenyl
  • electroluminescent devices containing such hole transport agents have low heat stability and unsatisfactory durability.
  • a hole transport layer has been prepared by dispersing such a molecular hole transport agent as TPD in a polyimide having high heat stability.
  • the hole transport layer exhibits stability which is still inferior to a layer consisting of only a polyimide. Therefore, there has existed a need to develop a polyimide hole transport agent having improved stability and hole transport capability.
  • an organic electroluminescent device comprising a transparent electrode layer, a metallic electrode layer and an organic interlayer disposed between the electrode 0 layers, wherein the organic interlayer has a hole transport layer comprising a polyimide derived from a triphenyldiamine derivative of formula (I):
  • C, D and E are each independently phenyl, biphenyl or naphthyl groups optionally substituted with one or more C alkyl groups.
  • FIG. 2 DSC(Differential Scanning Calorimeter) thermograms of the poly(amic acid) and polyimide, respectively, derived from pyromellitic o dianhydride(PMDA) and N,N'-diphenyl-N,N'-bis(4-aminobiphenyl)- 1,1 '- diphenyl-4,4'-diamine(DBDDA)(Example 2);
  • FIG. 3 the variations of the current density(A/m 2 )(2-l) and brightness(cd/m 2 )(2-2) of the electroluminescent device prepared in Example 1 as function of the applied voltage(V);
  • FIG. 4 the variation of the luminous eff ⁇ ciency(lm/W) of the electroluminescent device prepared in Example 1 with the applied voltage(V);
  • FIG. 5 the change in light intensity(cd/m ) of the electroluminescent device prepared in Example 1 with time(hr);
  • FIGs. 6 and 7 the variations of the current density(A/m 2 ) and brightness(cd/m 2 ), respectively, of the electroluminescent device prepared in Example 3 with the applied voltage(V);
  • FIGs. 8 and 9 the dependencies of the brightness(cd/m 2 ) and electroluminous eff ⁇ ciency(c ⁇ VA), respectively, of the electroluminescent device prepared in Example 3 on the current density(A/m 2 ); and
  • FIG. 10 the change of the electroluminous eff ⁇ ciency(coVA) of the electroluminescent device prepared in Example 3 with the brightness(cd/m 2 ).
  • the organic interlayer of the organic electroluminescent device of the present invention has a hole transport layer comprising a polyimide having a moiety derived from the triphenyldiamine derivative of formula (I) which is capable of transporting holes.
  • the inventive electroluminescent device comprises an organic interlayer which may be of a multi-layer structure containing a hole transport layer and an organic luminescent layer.
  • the organic interlayer may further include an electron transport layer, inserted between the metallic electrode layer and the organic luminescent layer.
  • FIG. 1 An example of the organic electroluminescent device of the present invention is shown in Figure 1.
  • This device consists of a transparent substrate(l), a transparent electrode layer(2), a hole transport layer(3), an organic luminescent/electron transport layer(4) and a metallic electrode layer(5).
  • the electric power supply(6) may be either alternating current(AC) or direct current(DC).
  • Polyimides in accordance with the present invention may be prepared by the methods as shown in Reaction Schemes 1 and 2. Specifically, a polyimide having a repeat unit of formula (VI) may be prepared by polymerizing a dianhydride of formula (II)(Reaction Scheme 1) or a diacid chloride of formula
  • A is a moiety derived from the compound of formula (II) or (III); R is a ⁇ alkyl group; m and p are each independently integers of 1 or higher; and C, D and E have the same meanings as defined above.
  • the polyimide thus prepared has a glass transition temperature of 200 °C or higher and exhibits improved hole transporting characteristics, and, thus, it may be directly used in fabricating a hole transport layer.
  • triphenyldiamine derivatives of formula (I) which may be used in the present invention include
  • Exemplary dianhydrides of formula (II) which may be used in the present invention include pyromellitic dianhydride(PMDA), 3,3',4,4'-benzophenone tetracarboxylic dianhydride(BTDA), 3,4,3 ',4 '-biphenyltetracarboxylic dianhydride(BPD A), 4,4 ' -(hexafluoropropylidene)diphthalic anhydride(6F-D A),
  • 1,2,3,4-cyclopentane tetracarboxylic dianhydride bicyclo[2,2,2]oct-7-ene-2,3,5,6-tetracarboxylic dianhydride, naphthalene- 1 ,4,5 ,8-tetracarboxylic dianhydride,
  • Exemplary diacid chlorides of formula (III) which may be used in the present invention include 2,5-bis-chlorocarbonyl-terephthalic acid dimethylester, 2,5-bis-chlorocarbonyl-terephthalic acid diethylester and
  • PMDA-DBDDA polyimide having a repeat unit of formula (Via) is preferably employed in the present invention.
  • a polyimide copolymer having a repeat unit of formula (X), prepared as in Reaction Scheme 3 or 4, may be advantageously used as a hole transport agent.
  • the polymers having repeat units of formulae (VIII) and (IX), respectively, are polyimide prepolymers;
  • B is a moiety derived from a diamine compound; o and n are each independently integers of 1 or higher; and A, C, D, E, R, m and p have the same meanings as defined above.
  • diamines of formula (VII) which may be used in the present invention include 4,4'-oxydianiline(ODA), 3,4'-diaminodiphenylether, 4,4 ' -diaminodiphenylether(DDE), 3,3' -diaminodipheny lmethane,
  • a conventional hole transport agent e.g., N,N'-diphenyl-N,N'-bis(3-methylphenyl)- 1 , 1 '-diphenyl-4,4'-diamine(TPD) of formula (XI)
  • TPD triphenyl-4,4'-diamine
  • the polyimide having the repeat unit of formula (VI) or (X) is coated on an anode by either a conventional wet process such as spin coating or a conventional vapor deposition to form a polyimide hole transport layer.
  • a polyimide thin layer may be formed by vapor depositing stoichiometric amounts of a dianhydride or diacid chloride and a triphenyldiamine derivative on an ITO substrate at a rate ranging from 0.1 to 0.3 A/sec, followed by thermal imidization at 150 to 300 ° C for 1 to 2 hours.
  • a polyimide layer may be formed by prepolymerizing a dianhydride or diacid chloride compound and a triphenyldiamine derivative in an appropriate solvent to obtain a prepolymer solution, which is spin-coated on an ITO substrate at 2,000 to 3,000 rpm for at least 3 min. and thermally imidized at 150 to 300 °C for 1 to 2 hours.
  • the thickness of the polyimide hole transport layer thus formed ranges from 100 to 1,000 A.
  • a metallic electrode layer comprising one or more metals having a low work function, e.g., magnesium, aluminum, silver and copper, may be formed in a thickness ranging from 50 to 3,000 A by a conventional vapor deposition.
  • the organic electroluminescent device of the present invention has improved thermal and physical stabilities, and good durability.
  • ITO Indium-tin-oxide
  • PMDA and DBDDA were vaporized at 220 and 190 ° C, respectively, and vapor deposited on the anode layer at a rate of 0.3 and 0.1 A/sec, respectively, at 5x10 ⁇ 6 torr. Then, the deposited PMDA-DBDDA poly(amic acid) thin layer was heated to 200 ° C at a rate of 2 ° C/min and heat-treated at 200 ° C for 1 hour to form a polyimide hole transport layer having a thickness of 250 A.
  • Alq 3 was vapor deposited on the hole transport layer to a thickness of 200 A at a rate of 0.1 A/sec at 5xlO "6 torr to form a luminescent/electron transport layer. Subsequently, aluminum was vapor deposited on the luminescent/electron transport layer to a thickness of 2000 A at a rate of 10 A/sec at 2xl0 "5 torr to form a cathode layer.
  • the luminescence characteristics of the organic electroluminescent device thus prepared are shown in FIGs. 3 to 5.
  • FIG. 3 reproduces the variations of the current density(A/m 2 )(2-l) and brightness(cd/m )(2-2) of the electroluminescent device as function of the applied voltage(V).
  • the current injection starts at about 3V, turn on voltage is about 4 to
  • FIG. 4 illustrates the variation of the luminous efficiency(lm/W) of the electroluminescent device with the applied voltage(V).
  • the luminous efficiency is steady at 12.4 lm/W at an applied voltage of 9.5 V and beyond.
  • FIG. 5 exhibits the change in light intensity(cd/m 2 ) of the electroluminescent device with time(hr). The light intensity is constant up to 45 hours after operation.
  • Example 2
  • Example 1 The procedure of Example 1 was repeated except that an Alq 3 luminescent/electron transport layer was doped with 2 wt% of Qdl(Quinacridone), and aluminum and lithium were vapor codeposited to form a cathode layer, to prepare an organic electroluminescent device having a total thickness of 4,000 A.
  • the luminescence characteristics of the organic electroluminescent device thus prepared are shown in FIGs. 6 to 10.
  • FIGs. 6 and 7 show the variations of the current density(A/m 2 ) and brightness(cd/m 2 ), respectively, of the electroluminescent device with the applied voltage(V).
  • the brightness is about 80,000c ⁇ 7m 3 at 19V.
  • FIGs. 8 and 9 exhibit the dependencies of the brightness(cd/m 2 ) and electroluminous eff ⁇ ciency(c ⁇ VA), respectively, of the electroluminescent device on the current density(A/m ).
  • a log-log plot of the current density and brightness exhibits a linear correlation.
  • the electroluminous efficiency depends only slightly on the current density and its maximum is about 7cd/A.
  • FIG. 10 represents the change in the electroluminous eff ⁇ ciency(coVA) of the electroluminescent device with the brightness(cd/m ).

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  • Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Materials Engineering (AREA)
  • Organic Chemistry (AREA)
  • Health & Medical Sciences (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Medicinal Chemistry (AREA)
  • Polymers & Plastics (AREA)
  • Macromolecular Compounds Obtained By Forming Nitrogen-Containing Linkages In General (AREA)

Abstract

La présente invention se rapporte à un dispositif électroluminescent comportant une couche de transport de trous contenant un polyimide issu d'un dérivé triphényldiamine. Ce dispositif électroluminescent se caractérise par une stabilité et une durabilité améliorées.
PCT/KR2001/001531 2001-09-11 2001-09-11 Dispositif electroluminescent organique comportant une couche de transport de trous contenant un polyimide WO2003022955A1 (fr)

Priority Applications (1)

Application Number Priority Date Filing Date Title
PCT/KR2001/001531 WO2003022955A1 (fr) 2001-09-11 2001-09-11 Dispositif electroluminescent organique comportant une couche de transport de trous contenant un polyimide

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PCT/KR2001/001531 WO2003022955A1 (fr) 2001-09-11 2001-09-11 Dispositif electroluminescent organique comportant une couche de transport de trous contenant un polyimide

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Cited By (7)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
WO2008072914A1 (fr) * 2006-12-15 2008-06-19 Kolon Industries, Inc. Résine polyimide et couche d'alignement de cristaux liquides et film polyimide utilisant cette résine
CN103834009A (zh) * 2012-11-27 2014-06-04 财团法人工业技术研究院 透明电致变色聚酰亚胺与其形成方法与电致变色组件
US20140206135A1 (en) * 2006-05-24 2014-07-24 Nissan Chemical Industries, Ltd. Coating liquid for gate insulating film, gate insulating film and organic transistor
CN104861162A (zh) * 2015-05-20 2015-08-26 上海交通大学 含叔丁基和三苯胺结构的可溶性聚酰亚胺及其制备方法
WO2015176545A1 (fr) * 2014-05-23 2015-11-26 哈尔滨工业大学 Polyimide thermoplastique à mémoire de forme résistant à des températures élevées et son procédé de préparation
US10597463B2 (en) 2004-04-22 2020-03-24 Agensys, Inc. Antibodies and molecules derived therefrom that bind to STEAP-1 proteins
US11180571B2 (en) 2017-04-03 2021-11-23 Hoffmann-La Roche Inc. Antibodies binding to STEAP-1

Citations (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JPH03274693A (ja) * 1990-03-26 1991-12-05 Idemitsu Kosan Co Ltd 有機薄膜エレクトロルミネッセンス素子及びその製造方法
KR20010009172A (ko) * 1999-07-08 2001-02-05 김선욱 우수한 안정성을 가진 유기전기발광소자
KR20010047942A (ko) * 1999-11-24 2001-06-15 김덕중 전기적 활성을 갖는 유기복합박막을 포함하는유기전기발광소자

Patent Citations (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JPH03274693A (ja) * 1990-03-26 1991-12-05 Idemitsu Kosan Co Ltd 有機薄膜エレクトロルミネッセンス素子及びその製造方法
KR20010009172A (ko) * 1999-07-08 2001-02-05 김선욱 우수한 안정성을 가진 유기전기발광소자
KR20010047942A (ko) * 1999-11-24 2001-06-15 김덕중 전기적 활성을 갖는 유기복합박막을 포함하는유기전기발광소자

Cited By (13)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US11401347B2 (en) 2004-04-22 2022-08-02 Agensys, Inc. Antibodies and molecules derived therefrom that bind to STEAP-1 proteins
US10597463B2 (en) 2004-04-22 2020-03-24 Agensys, Inc. Antibodies and molecules derived therefrom that bind to STEAP-1 proteins
US10573834B2 (en) * 2006-05-24 2020-02-25 Nissan Chemical Industries, Ltd. Coating liquid for gate insulating film, gate insulating film and organic transistor
US20140206135A1 (en) * 2006-05-24 2014-07-24 Nissan Chemical Industries, Ltd. Coating liquid for gate insulating film, gate insulating film and organic transistor
WO2008072914A1 (fr) * 2006-12-15 2008-06-19 Kolon Industries, Inc. Résine polyimide et couche d'alignement de cristaux liquides et film polyimide utilisant cette résine
TWI468440B (zh) * 2012-11-27 2015-01-11 Ind Tech Res Inst 透明電致變色聚醯亞胺與其形成方法與電致變色元件
CN103834009B (zh) * 2012-11-27 2016-03-30 财团法人工业技术研究院 透明电致变色聚酰亚胺与其形成方法与电致变色组件
US9331280B2 (en) 2012-11-27 2016-05-03 Industrial Technology Research Institute Transparent electrochromic polyimide, method for manufacturing the same, and electrochromic device utilizing the same
CN103834009A (zh) * 2012-11-27 2014-06-04 财团法人工业技术研究院 透明电致变色聚酰亚胺与其形成方法与电致变色组件
WO2015176545A1 (fr) * 2014-05-23 2015-11-26 哈尔滨工业大学 Polyimide thermoplastique à mémoire de forme résistant à des températures élevées et son procédé de préparation
CN104861162A (zh) * 2015-05-20 2015-08-26 上海交通大学 含叔丁基和三苯胺结构的可溶性聚酰亚胺及其制备方法
US11180571B2 (en) 2017-04-03 2021-11-23 Hoffmann-La Roche Inc. Antibodies binding to STEAP-1
US11685790B2 (en) 2017-04-03 2023-06-27 Hoffmann-La Roche Inc. Antibodies binding to STEAP-1

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