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1.
Nat Commun ; 15(1): 192, 2024 Jan 02.
Artigo em Inglês | MEDLINE | ID: mdl-38167422

RESUMO

High-rate production of multicarbon chemicals via the electrochemical CO2 reduction can be achieved by efficient CO2 mass transport. A key challenge for C-C coupling in high-current-density CO2 reduction is how to promote *CO formation and dimerization. Here, we report molecularly enhanced CO2-to-*CO conversion and *CO dimerization for high-rate ethylene production. Nanoconfinement of ascorbic acid by graphene quantum dots enables immobilization and redox reversibility of ascorbic acid in heterogeneous electrocatalysts. Cu nanowire with ascorbic acid nanoconfined by graphene quantum dots (cAA-CuNW) demonstrates high-rate ethylene production with a Faradaic efficiency of 60.7% and a partial current density of 539 mA/cm2, a 2.9-fold improvement over that of pristine CuNW. Furthermore, under low CO2 ratio of 33%, cAA-CuNW still exhibits efficient ethylene production with a Faradaic efficiency of 41.8%. We find that cAA-CuNW increases *CO coverage and optimizes the *CO binding mode ensemble between atop and bridge for efficient C-C coupling. A mechanistic study reveals that ascorbic acid can facilitate *CO formation and dimerization by favorable electron and proton transfer with strong hydrogen bonding.

2.
ACS Appl Mater Interfaces ; 15(38): 45167-45176, 2023 Sep 27.
Artigo em Inglês | MEDLINE | ID: mdl-37699415

RESUMO

Cross-linkable hole transport materials (HTMs) are ideal for improving the performance of solution-processed quantum dot light-emitting diodes (QLEDs) and phosphorescent light-emitting diodes (OLEDs). However, previously developed cross-linkable HTMs possessed poor hole transport properties, high cross-linking temperatures, and long curing times. To achieve efficient cross-linkable HTMs with high mobility, low cross-linking temperature, and short curing time, we designed and synthesized a series of low-temperature cross-linkable HTMs comprising dibenzofuran (DBF) and 4-divinyltriphenylamine (TPA) segments for highly efficient solution-processed QLEDs and OLEDs. The introduction of divinyl-functionalized TPA in various positions of the DBF core remarkably affected their chemical, physical, and electrochemical properties. In particular, cross-linked 4-(dibenzo[b,d]furan-3-yl)-N,N-bis(4-vinylphenyl)aniline (3-CDTPA) exhibited a deep highest occupied molecular orbital energy level (5.50 eV), high hole mobility (2.44 × 10-4 cm2 V-1 s-1), low cross-linking temperature (150 °C), and short curing time (30 min). Furthermore, a green QLED with 3-CDTPA as the hole transport layer (HTL) exhibited a notable maximum external quantum efficiency (EQEmax) of 18.59% with a remarkable maximum current efficiency (CEmax) of 78.48 cd A-1. In addition, solution-processed green OLEDs with 3-CDTPA showed excellent device performance with an EQEmax of 15.61%, a CEmax of 52.51 cd A-1, and outstanding CIE(x, y) color coordinates of (0.29, 0.61). This is one of the highest reported EQEs and CEs with high color purity for green solution-processed QLEDs and OLEDs using a divinyl-functionalized cross-linked HTM as the HTL. We believe that this study provides a new strategy for designing and synthesizing practical cross-linakable HTMs with enhanced performance for highly efficient solution-processed QLEDs and OLEDs.

3.
ACS Appl Mater Interfaces ; 14(4): 5807-5814, 2022 Feb 02.
Artigo em Inglês | MEDLINE | ID: mdl-35041372

RESUMO

Copper nanowires (CuNWs) possess key characteristics for realizing flexible transparent electronics. High-quality CuNW micropatterns with high resolution and uniform thickness are required to realize integrated transparent electronic devices. However, patterning high-aspect-ratio CuNWs is challenging because of their long length, exceeding the target pattern dimension. This work reports a novel reverse-offset printing technology that enables the sub-10 µm high-resolution micropatterning of CuNW transparent conducting electrodes (TCEs). The CuNW ink for reverse-offset printing was formulated to control viscoelasticity, cohesive force, and adhesion by adjusting the ligands, solvents, surface energy modifiers, and leveling additives. An inexpensive commercial adhesive handroller achieved a simple, fast, and scalable micropatterning of CuNW TCEs. Easy production of high-quality CuNW micropatterns with various curvatures and shapes was possible, regardless of the printing direction. The reverse-offset-printed CuNW micropatterns exhibited a minimum of 7 µm line width and excellent pattern qualities such as fine line spacing, sharp edge definition, and outstanding pattern uniformity. In addition, they exhibited excellent sheet resistance, high optical transparency, outstanding mechanical durability, and long-term stability. Flexible light-emitting diode (LED) circuits, transparent heaters, and organic LEDs (OLEDs) can be fabricated using high-resolution reverse-offset-printed CuNW micropatterns for applications in flexible transparent electronic devices.

4.
ACS Appl Mater Interfaces ; 14(47): 53250-53260, 2022 Nov 30.
Artigo em Inglês | MEDLINE | ID: mdl-36382782

RESUMO

With the advent of 5G wireless and Internet of Things technologies, flexible and stretchable printed circuit boards (PCBs) should be designed to address all the specifications necessary to receive signal transmissions, maintaining the signal integrity, and providing electrical connections. Here, we propose a silver nanoparticle (AgNP)/silver nanowire (AgNW) hybrid conductor and high-quality microprinting technology for fabricating flexible and stretchable PCBs in high-performance 5G wireless communication. A simple and low-cost reverse offset printing technique using a commercial adhesive hand-roller was adapted to ensure high-resolution and excellent pattern quality. The AgNP/AgNW micropatterns were fabricated in various line widths, from 5 µm to 5 mm. They exhibited excellent pattern qualities, such as fine line spacing, clear edge definition and outstanding pattern uniformity. After annealing via intense pulsed light irradiation, they showed outstanding electrical resistivity (15.7 µΩ cm). Moreover, they could withstand stretching up to a strain of 90% with a small change in resistance. As a demonstration of their practical application, the AgNP/AgNW micropatterns were used to fabricate 5G communication antennas that exhibited excellent wireless signal processing at operating frequencies in the C-band (4-8 GHz). Finally, a wearable sensor fabricated with these AgNP/AgNW micropatterns could successfully detected fine finger movements in real time with excellent sensitivity.

5.
Chem Sci ; 12(42): 14083-14097, 2021 Nov 03.
Artigo em Inglês | MEDLINE | ID: mdl-34760192

RESUMO

The concurrent enhancement of short-circuit current (J SC) and open-circuit voltage (V OC) is a key problem in the preparation of efficient organic solar cells (OSCs). In this paper, we report efficient and stable OSCs based on an asymmetric non-fullerene acceptor (NFA) IPC-BEH-IC2F. The NFA consists of a weak electron-donor core dithienothiophen[3,2-b]-pyrrolobenzothiadiazole (BEH) and two kinds of strong electron-acceptor (A) units [9H-indeno[1,2-b]pyrazine-2,3-dicarbonitrile (IPC) with a tricyclic fused system and 2-(5,6-difluoro-3-oxo-2,3-dihydro-1H-inden-1-ylidene)malononitrile (IC2F)]. For comparison, the symmetric NFAs IPC-BEH-IPC and IC2F-BEH-IC2F were characterised. The kind of flanking A unit significantly affects the light absorption features and electronic structures of the NFAs. The asymmetric IPC-BEH-IC2F has the highest extinction coefficient among the three NFAs owing to its strong dipole moment and highly crystalline feature. Its highest occupied molecular orbital (HOMO) and lowest unoccupied molecular orbital (LUMO) levels lie between those of the IPC-BEH-IPC and IC2F-BEH-IC2F molecules. The IPC group also promotes molecular packing through the tricyclic π-conjugated system and achieves increased crystallinity compared to that of the IC2F group. Inverted-type photovoltaic devices based on p-type polymer:NFA blends with PBDB-T and PM6 polymers as p-type polymers were fabricated. Among all these devices, the PBDB-T:IPC-BEH-IC2F blend device displayed the best photovoltaic properties because the IPC unit provides balanced electronic and morphological characteristics. More importantly, the PBDB-T:IPC-BEH-IC2F-based device exhibited the best long-term stability owing to the strongly interacting IPC moiety and the densely packed PBDB-T:IPC-BEH-IC2F film. These results demonstrate that asymmetric structural modifications of NFAs are an effective way for simultaneously improving the photovoltaic performance and stability of OSCs.

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