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Journal of Materials Chemistry C · 2021 ·Vol. 9 ·期 13 ·4496-4504 · IF 7.393

Cellulose-based flexible organic light-emitting diodes with enhanced stability and external quantum efficiency

Qinghong Zheng,Huixin Li,Yiling Zheng,Yinan Li,Xi Liu,Shuangxi Nie,Xinhua Ouyang,Lihui Chen,Yonghao Ni

A cellulose-based flexible organic light-emitting diode (OLED) with enhanced stability and light extraction efficiency was prepared by using a PEDOT:PSS PH1000 transparent conductive electrode coated on regenerated cellulose film (RCF). The PH1000/RCF transparent conductive electrode exhibits extra-high bending stability as compared to the traditional ITO/RCF electrode, which can be attributed to the highly flexible nature of PH1000 and the strong interaction between PH1000 and cellulose. Finite-difference-time-domain simulations show that, due to the smaller refractive index mismatch between PH1000 and RCF, a small proportion of photons are confined in the optical waveguide. The external quantum efficiency of the PH1000/RCF OLED (3.65%) is enhanced by nearly 36.2%, as compared to the ITO/RCF OLED device (2.68%). The ITO-free cellulose-based flexible OLED with enhanced stability and external quantum efficiency would be attractive in a wide range of applications, such as flexible displays, wearable devices and so on.

研究领域: 材料科学 · 光学工程
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PROGRESS IN ORGANIC COATINGS · 2022 · IF 6.206

Transparent and flame-retardant hybrid protective coating with high surface hardness, yet foldability

Chaohua Peng,An Huang,Xinjie Ma,Jiahui Zhong,Guorong Chen,Weiang Luo,Birong Zeng,Conghui Yuan,Yiting Xu,Lizong Dai

With the rapid development of flexible OLED display technology, Poly(ethylene terephthalate) (PET) has also received extensive attention as a protective film. However, it is still a challenge to endow PET with abrasion resistance and flame retardancy while maintaining transparency and flexibility. Here, we developed an epoxy-amine curing hybrid coating based on phosphorus-containing organic amine (DPNP) and ladderlike epoxy-oligosiloxane (AEOS). The ratio of DPNP and AEOS was changed to study the effect of phosphorus and silicon content on the performance of hybrid coatings. All the coatings were transparent. The PET/AE-DP3 sample achieved the limiting oxygen index of 28 % and exhibited self-extinguishing in vertical burning test. In microscale combustion calorimeter (MCC) test, the minimum peak heat release rate was 236.4 W/g with a reduction of 29.5 %, compared with pure PET. In addition, the AE-DP3 coating could withstand the abrasion of copper mesh and cheese cotton with a pencil hardness of 8H, and showed good foldability with a bending diameter of 5 mm. At the same time, the coating exhibited satisfactory adhesion without plasma treatment and good UV resistance. These results indicated the hybrid coating overcome the inherited weakness of PET film such as poor scratch-resistance and flammability , promoting the wider application of PET.

研究领域: 材料科学 · 化学工程
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SURFACE REVIEW AND LETTERS · 2019 · IF 0.748

A NEW STRUCTURE OF FLEXIBLE OLED WITH COPPER NANOWIRE ANODE AND GRAPHERE OXIDE/PEDOT: PSS ANODE BUFFER LAYER

PING LIU,JIANGHAO WANG,JIE CHENG,LIMING LIU,HONGHANG WANG,BAOQING ZENG,FENG CHI

A flexible organic light-emitting device (OLED) was produced using copper nanowire (CuNW) film as anode and Graphene oxide (GO)/poly(3,4-ethylenedioxythiophene):poly(styrene sulfonate) (PEDOT:PSS) film as anode buffer layer. Compared with other transparent conductive films (TCFs), CuNWs are low cost, easy to fabricate, and compatible with flexible substrates over a large area. Due to these advantages, CuNWs are showing greater and greater promise for the next generation of TCF. Modified by PEDOT:PSS, the conductivity and work function of the CuNW film can be dramatically enhanced. However, PEDOT:PSS is highly acidic and easy to corrode the CuNW film, which will reduce maximum luminous brightness and current efficiency of the OLED. In this paper, GO/PEDOT:PSS was used as anode buffer layer to modify the CuNW anode and the composite transparent electrode exhibited excellent optoelectrical properties. The driving voltage of the OLED with CuNW/PEDOT:PSS is 6.2 V, and the maximum luminous brightness is 2737.2 cd/m 2 . The driving voltage of the OLED with CuNW/GO/PEDOT:PSS anode was reduced to 5.1 V, and the maximum luminous brightness was improved to 3007.4 cd/m 2 .

研究领域: 材料科学 · 光电技术
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ACS Applied Materials & Interfaces · 2024 · IF 8.3

Unravelling the Electrical Field Induced Ion Migration in Flexible OLEDs with PEDOT:PSS Electrodes

Chenxi Liu,Mengze Li,Yifan Wang,Zijie Hou,Jian Chen,Kun Cao,Lihui Liu,Shufen Chen

The development of flexible organic light-emitting didoes (FOLEDs) has spurred the research on flexible transparent electrodes (FTEs). Poly(3,4-ethylenedioxythiophene):polystyrenesulfonate (PEDOT:PSS) is one of the most attractive FTEs due to its adjustable conductivity and compatibility with low-cost and large-scale solution processing techniques. Significantly, highly efficient FOLEDs have been achieved with modified PEDOT:PSS FTEs. However, the intrinsic mechanisms that contribute to device degradation of FOLEDs utilizing PEDOT:PSS FTEs have not yet been fully elucidated. In this work, three ionic liquids (ILs) are used to enhance the electrical conductivity and mechanical flexibility of PEDOT:PSS FTEs. Simultaneously, the influence of the electric field induced ion migration from PEDOT:PSS FTEs on the operational stability of FOLEDs is unraveled. We find that the ILs with larger ionic radii and higher steric hindrance are beneficial to suppressing the electrical field induced ion migration and improving the operational stability of FOLEDs. Finally, large-area and high-performance FOLEDs are achieved based on the IL of 1-ethyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide modified PEDOT:PSS FTEs, which demonstrate a high current efficiency of 98.1 cd/A and a longer lifetime of 66.7 min. This finding may promote the practical application of PEDOT:PSS FTEs in flexible optoelectronics.

研究领域: 材料科学 · 电子工程
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Surfaces and Interfaces · 2024 · IF 5.7

Eco-friendly transparent conductive films formed by silver nanowires embedded with conductive polymers in HPMC for flexible OLEDs

Peng-Fei Qian,Wen-Hao Geng,Ze-Long Bao,Li-Chao Jing,Di Zhang,Hong-Zhang Geng

In this study, gentianic acid (GtA) was first doped into poly (3,4-ethylenedioxythiophene): poly (styrene-sulfonic) (PEDOT:PSS), and the doped PEDOT:PSS (GP) was spin-coated as a hydrophilic layer on the surface of relatively hydrophobic polyethylene terephthalate (PET) films. After that, silver nanowires (AgNWs) aqueous dispersion and hydroxypropyl methyl cellulose (HPMC) solution were coated over the surface of PET films. Finally, the GP/AgNWs/HPMC flexible conductive films were stripped from the PET surface, achieving a high visible light transmittance (81.5 % at 550 nm) with low sheet resistance (4.2 Ω/□). By embedding AgNWs on the surface of the HPMC film, the surface roughness ( R q) of this flexible transparent conductive film (TCF) was as low as 3.2 nm, meeting the requirements for the fabrication of organic light-emitting diode (OLED) devices. The OLED device fabricated via using this TCF as the anode achieved a maximum brightness ( L max ) of 13,740 cd/m 2 , a maximum current efficiency ( C.E. max ) of 10.6 cd/A, a maximum power efficiency ( P.E. max ) of 5.5 lm/W and a maximum external quantum efficiency ( EQE max ) of 2.9 %. Furthermore, HPMC demonstrated solubility in water at ambient temperature, facilitating the recycling of AgNWS and mitigating environmental pollution. These findings provide a new scope for the application of TCF in recyclable flexible electronic devices.

研究领域: 材料科学 · 电子工程 · 环境科学
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Surfaces and Interfaces · 2024 · IF 5.7

Preparation of PEDOT flexible transparent conductive film by Solution shear method for OLEDs

Shi-Wei Wang,Peng-Fei Qian,Di Zhang,Wen-Hao Geng,Yi-Song Zhang,Xuan-Chen Liu,Lu-Yao Tian,Qingxia Zhu,Hong-Zhang Geng

In this work, the large-area poly 3,4-ethylenedioxythiophene (PEDOT: PSS) transparent conductive films (TCFs) were prepared by the solution shear method. These films exhibited excellent bendability , strong adhesion , superior uniformity, and high-light transmission. The optimum photoelectric figure of merit (FoM) of the films was 195.5, and the optimum photoelectric performance at a low sheet resistance (< 50 Ω/sq) was observed in the three-layer films, which was prepared at a dilution ratio of 2:1 and a shear rate of 1 mm/s, showing a thin-layer resistance of 34.7 Ω/sq, a transmittance of 93.2 %, an FoM of 151.9 and electrical conductivity of 2398.6 S/cm. The prepared films were used as the organic light-emitting diode (OLED) anode, and the large-area flexible green OLED device with good uniformity was obtained. The maximum current efficiency of the prepared large-area flexible OLED was 2.16 cd/A, reflecting the great potential of this solution-shear film in the field of flexible devices.

CAS / MDL: 7789-24-4
研究领域: 材料科学 · 光电技术 · 柔性电子
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EUROPEAN POLYMER JOURNAL · 2021 · IF 4.598

Ultrahigh thermal-stability polyimides with low CTE and required flexibility by formation of hydrogen bonds between poly(amic acid)s

Zhenghui Yang,Pingchuan Ma,Furong Li,Haiquan Guo,Chuanqing Kang,Lianxun Gao

The flexibility of organic light-emitting diode (OLED) displays highly depends on the properties of the flexible substrates. In this paper, a series of aromatic polyimides have been fabricated via the copolycondensation of pyromellitic dianhydride (PMDA), the two different rigid heterocyclic diamines, 2,5-bis(4-aminophenyl)pyrimidine (PRM) or 2,5-bis(4-aminophenyl)pyridine (PRD), and another flexible diamine, 4,4′-oxydianiline (ODA). The performance of the polyimide films could be systematically tailored by means of adjusting the main-chain rigidity, as well as the close packing and orientation of polymer chains by the formation of the intermolecular hydrogen bonds between poly(amic acid)s. The optimal results (PIb-4, PIb-5, PIc-2) showed that the polyimides were endowed with ultra-high glass transition temperature (T g ) exceeding 450 °C, low coefficient of thermal expansion (CTE) at 0–5 ppm K −1 and excellent thermal stability (T d5%  = 570–590 °C). Meanwhile, all of them exhibited sufficient flexibility, the elongation at break at of 40–60%, extremely high tensile strength of 250–380 MPa and modulus of 4.1–6.1 GPa. Hence, the polyimide films should be the promising candidates for application as the polymer substrates for flexible OLED displays.

研究领域: 材料科学 · 显示技术
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Polymer Chemistry · 2021 ·Vol. 12 ·期 37 ·5364-5376 · IF 5.582

Synthesis and characterization of amide-bridged colorless polyimide films with low CTE and high optical performance for flexible OLED displays

Zhenghui Yang,Haiquan Guo,Chuanqing Kang,Lianxun Gao

Three novel dianhydride monomers involving amide groups were synthesized and further polymerized with various diamines to afford a series of colorless polyimides (cPI). The resultant cPI films present outstanding optical performance, exceedingly good dimensional stability at high temperature, great film ductility and solution-processability. In particular, chemically imidized AMDA/TFDB has an ultra-low coefficient of thermal expansion value of 5.2 ppm K−A, a relatively high Tg value of 333 °C and large elongation at break of 29%, resulting from its rigid-rod backbone and the formation of hydrogen bonding (–CO⋯NH–) between adjacent molecular chains. Concurrently, it exhibits a high optical transmittance of 87% at a wavelength of 550 nm, a small haze value of 0.71 and low yellow index of 4.29 by reason that the incorporation of bulky trifluoromethyl and cyclohexyl preclude the formation of a charge transfer complex effectively. The high overall performance of the amide-containing cPI films suggests its potential application in the field of flexible OLED displays.

CAS / MDL: 88-95-9 110-86-1
研究领域: 材料科学 · 显示技术
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COMPOSITES PART A-APPLIED SCIENCE AND MANUFACTURING · 2023 · IF 8.7

Transparent shape memory polyimide enables OLED for smart deformation

Xinzuo Huang,Rongxiang Hu,Fenghua Zhang,Yanju Liu,Jinsong Leng

An innovative process for producing flexible transparent graphene electrodes has been proposed. The electrochemically polished copper-foil was used as the metal substrate to prepare high-quality monolayer graphene. Monolayer graphene was transferred from copper-foil to transparent shape memory polyimide (TSMPI) intactly by novel flow-casting transfer technology, and the smart, ultra-clean and smooth flexible graphene electrode (pG@TSMPI) was fabricated. The light transmittance of pG@TSMPI at 550 nm is 86%, the average sheet resistance is 310 Ω/sq, and the surface roughness (Ra) is 18 nm. Smart white OLED was manufactured using pG@TSMPI as transparent anode, and its luminescence performance was comparable to that of ITO-based device. Depending on the shape memory effect of TSMPI substrate, the smart OLED has the superiorities of variable stiffness and reconfigurable shape, which can transform from 2D structure into complex 3D structure.

CAS / MDL: 341-58-2 38103-06-9
研究领域: 材料科学 · 光电技术
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NEW JOURNAL OF CHEMISTRY · 2021 ·Vol. 45 ·期 29 ·12945-12956 · IF 3.591

Enhanced gas barrier properties of polymer substrates for flexible OLEDs by adjusting the backbone rigidity and incorporating 2D nanosheets

Zhenghui Yang,Haiquan Guo,Chuanqing Kang,Lianxun Gao

A series of polymer substrates based on the polyimides (PIs) containing diphenylpyridine for flexible OLED displays were successfully fabricated by the incorporation of graphene oxide (GO) and organically modified layered double hydroxide (OLDH) nanosheets. In comparison with pristine PI, the OTR and WVTR of PI nanocomposite films at a loading of 3% OLDH were reduced by 78% and 25.7%, respectively, whereas by incorporation of 0.3% GO, the OTR and WVTR of PI nanocomposite films declined by 85.5% and 31.8%, respectively. The results revealed that GO nanosheets could have a great advantage over OLDH from the aspect of improving the gas barrier performance. Moreover, compared with the pristine PI films (CTE: 4.73 ppm K−1), the incorporation of GO and OLDH nanosheets was of great benefit in reducing the CTE value, such as 1.57 ppm K−1 for PIL-3.0 and 3.33 ppm K−1 for PIG-0.3, while maintaining high Tg values exceeding 450 °C and excellent thermal stability. The resulting PI nanocomposite films showed improved barrier properties without sacrificing the thermal and mechanical performance, and could serve as a promising candidate for substrate materials of flexible OLED displays.

研究领域: 材料科学 · 高分子化学
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ACS Applied Materials & Interfaces · 2023 · IF 9.5

Ultralow Coefficient of Thermal Expansion and a High Colorless Transparent Polyimide Film Realized Through a Reinforced Hydrogen-Bond Network by In Situ Polymerization of Aromatic Polyamide in Colorless Polyimide

Xueshuang Jiang,Kaijin Chen,Chuying Li,Yubo Long,Siwei Liu,Zhenguo Chi,Jiarui Xu,Yi Zhang

Colorless polyimides (CPIs) are a key substrate material for flexible organic light-emitting diode (OLED) displays and have attracted worldwide attention. Here, in this paper, the dispersion and interfacial interaction of aromatic polyamide (PA) in CPI (synthesized from 4,4′-(hexafluoroisopropylidene) diphthalic anhydride (6FDA) and 2,2′-bis(trifluoromethyl)benzidine (TFMB)) were significantly improved by in situ polymerization, and colorless transparent macromolecular polyimide composites (CPI-PAx) were successfully prepared by PA and CPI. By adjusting the ratio of PA to CPI, a high-performance engineering plastic with excellent film-forming properties was obtained. Molecular simulations confirmed the uniform distribution of PA in CPI and its interaction in polymers. In CPI-PAx, the CPI was locked by the PA chain, and numerous molecular chains were mutually entangled to form a hydrogen-bond network structure. Due to the strong interaction between the chains imparted by the hydrogen bonds of the PA, they do not slide under external forces and heating. In addition, the additive PA has excellent dimensional stability, thermal, and mechanical properties, and CPI has outstanding optical properties, so the synthesized CPI-PAx combines the comprehensive properties of PA and CPI. The CPI-PAx has excellent thermal and mechanical properties, with a thermal decomposition temperature of 499 °C, a glass transition temperature of 385 °C, a coefficient of thermal expansion of 0.8 ppm K–1, a tensile strength of 50.9 MPa, and an elastic modulus of 3.9 GPa. Particularly, CPI-PAx has a 90% transmittance in the visible region. These data prove that the strategy of combining PA and CPI by in situ polymerization is an effective method to circumvent the bottleneck of CPI in the current flexible window application, and this design strategy is universal.

CAS / MDL: 127-19-5
研究领域: 材料科学 · 高分子化学
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ACS Applied Materials & Interfaces · 2022 · IF 10.383

Highly Foldable, Super-Sensitive, and Transparent Nanocellulose/Ceramic/Polymer Cover Windows for Flexible OLED Displays

Jingyi Xie,Dongmei Jia,Mahmut Dirican,Yi Xia,Chunxing Li,Yi Liu,Meng Cui,Chaoyi Yan,Jiayu Wan,Hao Liu,Gang Chen,Xiangwu Zhang,Jinsong Tao

Polymer cover windows are important components of flexible OLED displays but they easily generate wrinkles because of their weak folding resistance. Increasing the polymer thickness can improve the folding resistance but it decreases the touch sensitivity. Thus, fabricating highly foldable and supersensitive polymer cover windows is still challenging. Here, by incorporating cellulose nanocrystals (CNCs) and zirconia (ZrO2) into colorless polyimide (CPI), we developed a highly foldable and supersensitive hybrid cover window. Inspired by the theory of elasticity, we added rigid CNCs into CPI to improve the elastic modulus and hence the foldability. ZrO2 was introduced to improve dielectric properties, which leads to improved touch sensitivity. After these modifications, the elastic modulus of the cover windows was increased from 1432 to 2221 MPa, whereas its dielectric constant was increased from 2.95 to 3.46 (@1 × 106 Hz), resulting in significantly enhanced foldability and sensitivity. Meanwhile, because of the nano size of CNCs and ZrO2, the hybrid cover windows exhibit excellent optical properties with the transmittance of ∼88.1%@550 nm and haze of 2.39%. With improved and balanced mechanical, dielectric, and optical properties, these hybrid cover windows overcome current cover windows’ defects and could be widely used in next-generation flexible displays.

CAS / MDL: 13520-92-8
研究领域: 材料科学 · 光学工程 · 电子工程
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