Latest ArticlesA pair of asymmetric rigid carbazole-benzonitrile-based emitters were synthesized by strategically alternating donor and acceptor groups along the molecular edges. The spin-flip process is accelerated by both the formation of localized and delocalized charge transfer states due to linearly positioned donors and strong spin-orbital coupling between different excitation feature of the lowest singlet and triplet excited states. This molecular architecture results in a remarkable short delayed lifespan of around 100 ns. The application of the two emitters in organic light-emitting diodes (OLEDs) achieves the highest external quantum efficiencies of 13.0% for the green emitter and 9.1% for the sky-blue emitter. Impressively, these devices maintain their high efficiency even at high luminance levels. The sustained efficiency is ascribed to the effective suppression of exciton quenching by substantially shortening delayed lifespan. These findings underscore the practical utility of the molecular design strategy that incorporates alternate donor and acceptor groups at the molecular periphery for shortening delayed fluorescence lifetime, and hold great promise for the development of high-performance OLEDs.
Electromagnetic wave-absorbing materials (EWAMs) are susceptible to failure in complex chemical environments. It is urgent to develop composites with high-efficiency electromagnetic wave (EMW) absorption and strong corrosion resistance. In the work, polyaniline (PANI) is in-situ polymerized on the surface of oxidized carbon nanohorns (ox-CNHs) to create a core-shell composite of ox-CNHs@PANI. By adjusting the thickness of the PANI shell and effectively regulating the electromagnetic parameters of the composite material, excellent impedance matching and efficient EMW absorption are achieved. At a thickness of 2.22 mm, the composite exhibits a reflection loss peak (RLmin) and a maximum effective absorption broadband (EAB) of −66.7 dB and 5.68 GHz, respectively. Additionally, the dense PANI shell effectively prevents contact between the corrosive medium and ox-CNHs, which significantly reduces the possibility of corrosion. Due to the formation of the ox-CNHs/PANI interface, the ox-CNHs@PANI composite exhibits strong corrosion resistance under acidic, alkaline, and neutral conditions. The ox-CNHs@PANI composite exhibits excellent EMW absorption and strong corrosion resistance, offering a new approach to developing advanced bifunctional materials.
Molecular catalysts can effectively steer the electrocatalytic acetylene semihydrogenation into ethylene, but realizing high Faradaic efficiency (FE) at industrial current densities remains a challenge. Herein, we report a ligand engineering strategy that utilizes polymeric N-heterocyclic carbene (NHC) as a hydrophobic ligand to modulate the microenvironment of Cu sites. This polymeric NHC imparts appropriate hydrophobic properties for the chelated Cu sites, thereby moderating the H2O transport and enabling easy access of acetylene. Consequently, the polymeric NHC chelated Cu exhibits an FEethylene of ~97% at a current density of 500 mA/cm2 in a flow cell. Particularly in a zero-gap reactor, the FEethylene consistently exceeds 86% across current densities from 100 mA/cm2 to 400 mA/cm2, reaching an optimal FEethylene of 98% at 200 mA/cm2 and achieving durable operation for 155 h at 100 mA/cm2. This work provides a promising paradigm to regulate the microenvironment of molecular catalysts for improving electrocatalytic performances under industrial current densities.
Recently, CsPbBr3 perovskite solar cells (PSCs) have garnered attention due to cost-effectiveness and reliability. However, hole transport limitations lead to charge recombination and lower power conversion efficiency (PCE). Defects in the CsPbBr3 layer, poor hole transport at the interface with carbon electrodes, and energy level differences hinder performance. Optimizing the perovskite layer using electron-donating organic molecules containing -NH2 groups enhances efficiency and stability by passivating defects and modulating lattice structure. In this work, tetra(4-aminophenyl)ethylene (TPE) and tetra(4-aminobiphenyl)ethylene (TPE-Ph) were employed to optimize the CsPbBr3/carbon electrode interface. Their strong electron-donating properties and amino groups facilitate hole transfer and defect passivation, boosting PCE to 9.38% and enhancing stability.
Enhancing the corrosion resistance of carriers within Fenton-like systems and inhibiting the migration and aggregation of single atoms in reaction environments are essential for maintaining both high activity and stability at catalytic sites, thus meeting fundamental requirements for practical application. The Fenton-like process of activating various strong oxidants by silicon-based single atom catalysts (SACs) prepared based on silicon-based materials (mesoporous silica, silicon-based minerals, and organosilicon materials) has unique advantages such as structural stability (especially important under strong oxidation conditions) and environmental protection. In this paper, the preparation strategies for the silicon-based SACs were assessed first, and the structural characteristics of various silicon-based SACs are systematically discussed, their application process and mechanism in Fenton-like process to achieve water purification are investigated, and the progress of Fenton-like process in density functional theory (DFT) of silicon-based derived single atom catalysts is summarized. In this paper, the preparation strategies and applications of silicon-based derived SACs are analyzed in depth, and their oxidation activities and pathways to different pollutants in water are reviewed. In addition, this paper also summarizes the device design and application of silicon-based derived SACs, and prospects the future development of silicon-based SACs in Fenton-like applications.
Epoxy resin is widely used in electronic packaging due to its exceptional performance, particularly the low-temperature curable thiol/epoxy system, which effectively minimizes thermal damage to sensitive electronic components. However, the majority of commercial thiol curing agents contain hydrolysable ester bonds and lack rigid structures, which induces most of thiol/epoxy systems still suffering from unsatisfactory heat resistance and hygrothermal resistance, significantly hindering their application in electronic packaging. In this study, we synthesized a tetrafunctional thiol compound, bis[3-(3-sulfanylpropyl)-4-(3-sulfanylpropoxy)phenyl]sulfone (TMBPS) with rigid and ester-free structures to replace traditional commercial thiol curing agents, pentaerythritol tetra(3-mercaptopropionate) (PETMP). Compared to the PETMP/epoxy system, the TMBPS/epoxy system exhibited superior comprehensive properties. The rigid structures of bisphenol S-type tetrathiol enhanced the heat resistance and mechanical properties of TMBPS/epoxy resin cured products, outperforming those of PETMP/epoxy resin cured products. Notably, the glass transition temperature of TMBPS/epoxy resin cured products was 74.2 ℃ which was 11.8 ℃ higher than that of PETMP cured products. Moreover, the ester-free structure in TMBPS contributed to its enhanced resistance to chemicals and hygrothermal conditions. After undergoing 1000 h of high-temperature and high-humidity aging, the tensile strength and adhesion strength of TMBPS-cured products were 73.33 MPa and 3.39 MPa, respectively exceeding 100% and 40% of their initial values, while PETMP-cured products exhibited a complete loss of both tensile strength and adhesion strength. This study provides a strategy for obtaining thermosetting polymers that can be cured at low temperatures and exhibit excellent comprehensive properties.
Organic semiconductor materials have demonstrated extensive potential in the field of gas sensors due to the advantages including designable chemical structure, tunable physical and chemical properties. Through density functional theory (DFT) calculations, researchers can investigate gas sensing mechanisms, optimize, and predict the electronic structures and response characteristics of these materials, and thereby identify candidate materials with promising gas sensing applications for targeted design. This review concentrates on three primary applications of DFT technology in the realm of organic semiconductor-based gas sensors: (1) Investigating the sensing mechanisms by analyzing the interactions between gas molecules and sensing materials through DFT, (2) simulating the dynamic responses of gas molecules, which involves the behavior on the sensing interface using DFT combined with other computational methods to explore adsorption and diffusion processes, and (3) exploring and designing sensitive materials by employing DFT for screening and predicting chemical structures, thereby developing new sensing materials with exceptional performance. Furthermore, this review examines current research outcomes and anticipates the extensive application prospects of DFT technology in the domain of organic semiconductor-based gas sensors. These efforts are expected to provide valuable insights for further in-depth exploration of DFT applications in sensor technology, thereby fostering significant advancements and innovations in the field.
Bacterial pneumonia is one of the most common infectious diseases, a great threat to the health of children and the elderly. In the clinic, due to the extensive use of antibiotics, multi-drug-resistant bacteria have increased in large numbers, seriously affects the treatment of patients with bacterial pneumonia. With the development of nanomedicine, it shows great potential in the treatment of bacterial pneumonia. In this review, it initially comprehensively describes the pathological process of bacterial pneumonia and the current status of its clinical treatment. Then it summarizes the strategies of nanomedicine for the treatment of bacterial pneumonia, including inorganic nanomaterials, polymer nanoparticles, natural source nanomaterials and artificial antimicrobial peptides, with a focus on novel nanomaterials for the treatment of bacterial pneumonia (biomimetic nanomaterials, nanovaccines and genetically engineered nanomaterials). Finally, the prospect of nanomedicine for bacterial pneumonia therapy is discussed in the hope of providing new ideas for the clinical treatment of bacterial pneumonia.