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1.
ACS Appl Mater Interfaces ; 16(38): 51201-51211, 2024 Sep 25.
Artigo em Inglês | MEDLINE | ID: mdl-39279143

RESUMO

Organic light-emitting diodes (OLEDs) have been extensively investigated in full-color displays and energy-saving lighting owing to their unique advantages. However, deep-blue OLEDs based on nondoped emitting layers with a satisfactory external quantum efficiency (EQE) are still rare for applications. In this work, six hot exciton materials, PPIM-12F, PPIM-22F, PPIM-13F, PPIM-23F, PPIM-1CN, and PPIM-2CN, are designed and synthesized via an isomer engineering design strategy and their photophysical properties and OLED performance are systematically investigated. These emitters all possess wide band gaps (3.53-3.69 eV), hybrid local and charge transfer (HLCT) characteristics, and good thermal stabilities. The C2 series compounds, PPIM-22F, PPIM-23F, and PPIM-2CN, all show redder emission peaks than the N1 series counterparts of PPIM-12F, PPIM-13F, and PPIM-1CN. In addition, the LUMO energy levels decrease consecutively in the sequence of PPIM-22F < PPIM-23F < PPIM-2CN and are all lower than their respective N1 series position isomers of PPIM-12F, PPIM-13F, and PPIM-1CN. The CV measurements indicate that such a design strategy renders the fine-tuning of LUMO energy levels, and the incorporation of electron acceptors at the extended C2 position of the PI unit is a better choice to improve the electron injection ability. Theoretical simulations indicate that they may harvest the triplet exciton through an upper-level reverse intersystem crossing process, which decreases the gathering of triplet excitons and allows the OLEDs to be fabricated by nondoping technology. Among them, PPIM-22F with a difluorobenzene substituent at the C2 position manifests the best performance in OLEDs, which exhibits the maximum EQE of 7.87% and Commission Internationale de lEclairage (CIE) coordinates of (0.16, 0.10). This work demonstrates an effective strategy for considerable improvement in device performance by a subtle change in the molecular structure through isomer engineering.

2.
Chem Sci ; 13(39): 11614-11622, 2022 Oct 12.
Artigo em Inglês | MEDLINE | ID: mdl-36320387

RESUMO

All-organic symmetric lithium-ion batteries (LIBs) show promising prospects in sustainable energy storage systems, due to their environmental friendliness, structural diversity and low cost. Nevertheless, it remains a great challenge to explore suitable electrode materials and achieve excellent battery performance for all-organic symmetric LIBs. Herein, a squaraine-anthraquinone polymer (PSQ) electrode material was designed through rational molecular engineering. The well-designed extended π-conjugated system, donor-acceptor structure, abundant redox-active sites and rational manipulation of weak inter-/intramolecular interactions endow the PSQ electrode with outstanding electrochemical performance. The capacity of the PSQ cathode can be optimized to 311.5 mA h g-1 by in situ carbon-template polymerization. Impressively, PSQ-based all-organic symmetric LIBs displayed high reversible capacity (170.8 mA h g-1 at 50 mA g-1), excellent rate performance (64.9% capacity retention at 4000 mA g-1 vs. 50 mA g-1), ultralong cycle life up to 30 000 cycles at 2000 mA g-1 and 97% capacity retention after 2500 cycles at 500 mA g-1, which is one of the best comprehensive battery performances among the all-organic LIBs reported thus far.

3.
Front Chem ; 9: 668336, 2021.
Artigo em Inglês | MEDLINE | ID: mdl-33859976

RESUMO

Carbon nanomaterials with high electrical conductivity, good chemical, and mechanical stability have attracted increasing attentions and shown wide applications in recent years. In particularly, hollow carbon nanomaterials, which possess ultrahigh specific surface area, large surface-to-volume ratios, and controllable pore size distribution, will benefit to provide abundant active sites, and mass loading vacancy, accelerate electron/ion transfer as well as contribute to the specific density of energy storage systems. In this mini-review, we summarize the recent progresses of hollow carbon nanomaterials by focusing on the synthesis approaches and corresponding nanostructures, including template-free and hard-template carbon hollow structures, metal organic framework-based hollow carbon structures, bowl-like and cage-like structures, as well as hollow fibers. The design and synthesis strategies of these hollow carbon nanomaterials have been systematically discussed. Finally, the emerging challenges and future prospective for developing advanced hollow carbon structures were outlined.

4.
ACS Appl Mater Interfaces ; 12(14): 16715-16725, 2020 Apr 08.
Artigo em Inglês | MEDLINE | ID: mdl-32180398

RESUMO

A family of pyrene[4,5-d]imidazole derivatives, PyPA, PyPPA, PyPPAC, and PyPAC, with different excited states are successfully developed. Among them, PyPPA and PyPPAC possess hybridized local and charge-transfer (HLCT) state, endowing them with pure blue fluorescence as well as high quantum yields. The nondoped organic light-emitting diode (OLED) based on PyPPA displays Commission Internationale de L'Eclairage coordinates of (0.14, 0.13) and achieves a maximum external quantum efficiency (EQE) of 8.47%, which are among the highest value reported to date for nondoped blue HLCT OLEDs. The nondoped OLED based on PyPPAC exhibits a maximum luminance of 50,046 cd m-2 located in the blue region with CIE coordinates of (0.15, 0.21) and an EQE of 6.74% even when the luminance reached over 10,000 cd m-2. In addition, they both reveal ultimate exciton utilizing efficiencies of nearly 100%. The potential of a blue emitter of PyPPA with an HLCT character for application in white OLED (WOLED) is further tested. The efficient two-color hybrid warm WOLED is successfully achieved, which provides the total EQE, power efficiency, and current efficiency of up to 21.19%, 61.46 lm W-1, and 62.13 cd A-1, respectively. The nondoped blue OLEDs and hybrid WOLEDs present good color stabilities with low efficiency roll-offs. Our results prove that taking advantage of the HLCT state, nondoped blue OLEDs as well as hybrid WOLEDs with high performance could be realized, which have a promising prospect for the displays and lightings in the future.

5.
Chem Asian J ; 15(1): 163-168, 2020 Jan 02.
Artigo em Inglês | MEDLINE | ID: mdl-31774941

RESUMO

Organic light-emitting diodes (OLEDs) have been greatly developed in recent years owing to their abundant advantages for full-color displays and general-purpose lightings. Blue emitters not only provide one of the primary colors of the RGB (red, green and blue) display system to reduce the power consumption of OLEDs, but are able able to generate light of all colors, including blue, green, red, and white by energy transfer processes in devices. However, it remains a challenge to achieve high-performance blue electroluminescence, especially for nondoped devices. In this paper, we report a blue light emitting molecule, DPAC-AnPCN, which consists of 9,9-diphenyl-9,10-dihydroacridine and p-benzonitrile substituted anthracene moieties. The asymmetrically decoration on anthracene with different groups on its 9 and 10 positions combines the merits of the respective constructing units and endows DPAC-AnPCN with pure blue emission, high solid-state efficiency, good thermal stability and appropriate HOMO and LUMO energy levels. Furthermore, DPAC-AnPCN can be applied in a nondoped device to effectively reduce the fabrication complexity and cost. The nondoped device exhibits pure blue electroluminescence (EL) locating at 464 nm with CIE coordinates of (0.15, 0.15). Moreover, it maintains high efficiency at relatively high luminescence. The maximum external quantum efficiency (EQE) reaches 6.04 % and still remains 5.31 % at the luminance of 1000 cd m-2 showing a very small efficiency roll-off.

6.
Chem Asian J ; 14(7): 1004-1012, 2019 Apr 01.
Artigo em Inglês | MEDLINE | ID: mdl-30680943

RESUMO

The development of efficient blue materials has been a continuous research topic in the field of organic light-emitting diodes (OLEDs). In this paper, three aggregation-induced emission enhancement active blue emitters, PIAnTPE, TPAAnTPE and CzAnTPE, are successfully synthesized by attaching a triphenylethylene unit and phenanthroimidazole/triphenylamine/carbazole moieties to the 9,10-positions of anthracene, respectively. The three compounds exhibit good thermal stabilities, appropriate for the highest occupied molecular orbital (HOMO) and the lowest unoccupied molecular orbital (LUMO) energy levels and display high photoluminescence quantum yields (PLQYs) of 65, 70 and 46 % in the solid state. Non-doped blue devices using PIAnTPE, TPAAnTPE and CzAnTPE as the emitting layers show good electroluminescent performances, with the maximum external quantum efficiencies (EQEs) of 4.46, 4.13 and 4.04 %, respectively. More importantly, EQEs of all the three devices can be still retained when the luminescence reaches 1000 cd m-2 , exhibiting quite small efficiency roll-offs in the non-doped OLEDs.

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