Latest ArticlesElectrocatalysis for nitrate (NO3–) removal from wastewater faces the challenge of merging efficient reduction and high selectivity to nitrogen (N2) with economic viability in a durable catalyst. In this study, bimetallic PdCu/TiOx composite catalysts were synthesized with varying Pd and Cu ratios through electrochemical deposition on defective TiOx nanotube arrays. Denitrification experiments demonstrated that the Pd1Cu1/TiOx catalyst exhibited the highest NO3– removal rate (81.2%) and N2 selectivity (67.2%) among all tested catalysts. Leveraging the exceptional light-responsive property of TiOx, the introduction of light energy as an assisting factor in electrocatalysis further augmented the NO3– treatment rate, resulting in a higher NO3– removal rate of 95.1% and N2 selectivity of approximately 90%. Compared to individual electrocatalysis and photocatalysis systems, the overpotential for the catalytic interface active *H formation in the photo-assisted electrocatalysis system was remarkably reduced, thus accelerating electron migration and promoting NO3– reduction kinetics. Economic analysis revealed an energy consumption of 2.74 kWh/mol and a corresponding energy consumption per order (EEO) of 0.79 kWh/m3 for the Pd1Cu1/TiOx catalyst to reduce 25.2 mg/L of NO3–-N in water to N2, showcasing remarkable competitiveness and economic advantages over other water treatment technologies. This study developed the PdCu/TiOx electrocatalysts with high NO3– removal rates and N2 selectivity, particularly when combined with light energy, the efficiency and selectivity were significantly enhanced, offering a competitive and economically viable solution for wastewater treatment.
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.
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.
A 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.
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.
Quantum dots (QDs), a type of nanoscale semiconductor material with unique optical and electrical properties like adjustable emission and high photoluminescence quantum yields, are suitable for applications in optoelectronics. However, QDs are typically degraded under humid and high-temperature circumstances, greatly limiting their practical value. Coating the QD surface with an inorganic silica layer is a feasible method for improving stability and endurance in a variety of applications. This paper comprehensively reviews silica coating methodologies on QD surfaces and explores their applications in optoelectronic domains. Firstly, the paper provides mainstream silica coating approaches, which can be divided into two categories: in-situ hydrolysis of silylating reagents on QD surfaces and template techniques for encapsulation QDs. Subsequently, the recent applications of the silica-coated QDs on optoelectronic fields including light-emitting diodes, solar cells, photodetectors were discussed. Finally, it reviews recent advances in silica-coated QD technology and prospects for future applications.
The transition metal-catalyzed C-H activation have been considered as increasingly useful approach for installing new functional groups onto organic small molecules due to their high step- and atom-economy, the abundance of hydrocarbon compounds, and the potential for late-stage functionalization of complex organic molecules. The ortho- and meta-C-H activation and functionalization of aromatic compounds have been widely explored in recent years, however the distal para-C-H activation and functionalization has remained a significant challenge because of the difficulty in forming energetically favorable metallacyclic transition states. The utilization of appropriate directing groups or templates as well as the meticulous design of catalysts and ligands has proven to be effective in transition-metal-catalyzed remote para-C-H bonds activation and functionalization of aromatic compounds. This review aims to summarize the strategies for controlling para-selective C-H functionalization using the directing group, template engineering, and catalyst/ligand design under transition metals catalysis in recent years.
Selective catalytic transfer hydrogenation (CTH) of carbonyl compounds to obtain specific alcohols holds significant importance across various fields. Achieving multiple selectivity in CTH is particularly crucial, but full of great challenge. Herein, a cationic In-captured Zr-porphyrin framework (1) with nanosized pores/cages was successfully constructed and showed high structure stability. Catalytic investigations revealed that 1 displayed highly multi-selective CTH of aldehydes and ketones containing both chemo- and size selectivity for the first time. The CTH of aldehydes and ketones exhibited remarkable reductive selectivity of 99% towards CO bonds into CHOH in the presence of -NO2, -CN and CC groups. Through tuning the reaction conditions, 1 also exhibited highly selective reduction of 97% for -CHO groups in the simultaneous presence of -CHO and -COCH3 groups in intra- and intermolecular settings. Remarkably, reductive selectivity towards -CHO group remained prominent among five concurrent unsaturated groups mentioned above. Additionally, the definite pore size of 1 facilitated volume control of substrates, enabling size selectivity. 1 as a heterogeneous catalyst was further confirmed by leaching tests, and maintained high activity even after being used for at least six cycles. Mechanistic studies have revealed that Zr6O8 clusters served as the catalytic centers and the observed chemoselectivity mainly results from the synergistic effect of distinct metal sites within 1. The heightened selectivity towards -CHO over -COCH3 can be attributed to the easier realization of transfer hydrogenation processes for -CHO compared to -COCH3.
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