Latest ArticlesThe construction of triplet-to-singlet Förster resonance energy transfer (TS-FRET) systems has significantly contributed to the advancement of high-performance optoelectronic materials, particularly in the development of metal-free organic environmental afterglow materials. Despite these notable advancements, achieving highly efficient energy transfer between luminescent donor and acceptor molecules remains a formidable challenge. In this study, we present the utilization of cation-π interactions as an effective strategy to enhance TS-FRET efficiency, with the ultimate objective of further advancing fluorescence afterglow materials. Our results demonstrate that the cation-π interaction in 1D supramolecular nanorods (1D-SNRs) enhances the dipole-dipole coupling, a crucial parameter for regulating TS-FRET between the triplet state phosphorescent donor and singlet state fluorescent acceptor. As a result, we achieved an outstanding TS-FRET efficiency of up to 97%. Furthermore, the 1D-SNRs exhibit a long-lifetime afterglow property, which suggests their potential application as a cost-effective and secure medium for information encryption. Thus, our findings highlight the promising prospects of cation-π interactions in enhancing TS-FRET efficiency and advancing the field of organic photo-functional materials.
Selective separation of phenanthrene (PHE) from aromatic isomer mixtures poses a significant challenge in industry due to the similar physical properties of PHE and its isomer anthracene (ANT). Herein, we report the self-assembly of a water-soluble Pd2L2 cage 1 with a large hydrophobic cavity, formed from novel macrocyclic ligands (L) and cis-Pd(Ⅱ). Cage 1 can selectively encapsulate PHE instead of ANT. Based on host-guest recognition followed by extraction, we achieve a remarkable 99% purity of PHE separation from an equimolar mixture of PHE and ANT using cage 1 in aqueous solution. Importantly, the separation performance of PHE using cage 1 remains unaffected even after five extraction cycles, demonstrating its robustness. This work highlights the potential of supramolecular cages for efficient and cost-effective PHE separation from the isomer ANT in aqueous solutions using such promising host-guest strategy.
For nano-collision, regulating the interaction between nanoparticles (NPs) and electrode interfaces is crucial for the precise analysis of individual NPs. However, existing ultramicroelectrodes (UMEs) suffer from narrow electrochemical window and poor electrode interface adhesion, severely hindering the application of precise single NP analysis. Here, we propose a simple and effective interface modification strategy. By electrochemically self-assembling poly(diallyldimethylammonium chloride) (PC) on the surface of carbon nanocone electrodes (CNCEs), we successfully prepared PC-modified CNCEs (PC‑CNCEs). These electrodes not only possess sufficiently wide electrochemical window but also exhibit strong adhesion to negatively charged Ag NPs on their surfaces. Surface physical analysis and electrochemical molecule detection validated the high-density loading of PC on the modified electrodes. Furthermore, the working principle of PC‑CNCEs for single Ag NP collision detection was further verified through the techniques of nano-collision and double-potential steps. Leveraging these significant advantages, PC‑CNCEs not only achieved precise measurements of single or mixed-sized Ag NPs but also detected Ag NP solutions at concentrations as low as fmol/L levels. This advancement offers a new strategy for the rapid and precise analysis of NP colloids.
Aromatic nitro compounds present substantial health and environmental concerns due to their toxic nature and potential explosive properties. Consequently, the development of host–guest molecular recognition systems for these compounds serves a dual-purpose: enabling the fabrication of high-performance sensors for detection and guiding the design of efficient adsorbents for environmental remediation. This study investigated the host–guest recognition behavior of perethylated pillar[n]arenes toward two aromatic nitro molecules, 1-chloro-2,4-dinitrobenzene and picric acid. Various techniques including 1H NMR, 2D NOESY NMR, and UV-vis spectroscopy were employed to explore the binding behavior between pillararenes and aromatic nitro guests in solution. Moreover, valuable single crystal structures were obtained to elucidate the distinct solid-state assembly behaviors of these guests with different pillararenes. The assembled solid-state supramolecular structures observed encompassed a 1:1 host–guest inclusion complex, an external binding complex, and an exo-wall tessellation complex. Furthermore, based on the findings from these systems, a pillararene-based test paper was developed for efficient picric acid detection, and the removal of picric acid from solution was also achieved using pillararenes powder. This research provides novel insights into the development of diverse host–guest systems toward hazardous compounds, offering potential applications in environmental protection and explosive detection domains.
The rapid emergence of drug-resistant bacterial strains undermines the efficacy of conventional antibiotics, necessitating the development of alternative therapies. Antimicrobial photodynamic therapy (PDT) is a promising approach, but its effectiveness is often limited by the suboptimal photocatalytic activity of photosensitizers. In this study, we introduce a novel photoresponsive carbon-based antibacterial agent, Ce6/g-C3N4, which combines the photocatalytic properties of graphite-phase carbon nitride (g-C3N4) with the photodynamic attributes of chlorin e6 (Ce6). This agent, with an average particle size of 250.7 nm, demonstrates significantly enhanced photocatalytic activity. Additionally, the strong affinity of Ce6/g-C3N4 for bacteria and efficient delivery of Ce6 result in an inhibition rate exceeding 99% against Gram-positive bacteria and excellent biofilm eradication under light irradiation. In vivo experiments reveal that Ce6/g-C3N4 effectively inhibits bacterial growth on wounds, and promotes wound healing post-light treatment, while maintaining good biocompatibility. Overall, the Ce6/g-C3N4 antibacterial agent synergizes photodynamic and photocatalytic mechanisms, offering a new avenue for the photo-mediated, multi-strategic treatment of bacterial infections and wound healing.
Liquid-liquid phase separation (LLPS) of proteins and nucleic acids is a common phenomenon in cells that underlies the formation of membraneless organelles. Although the macroscopic behavior of biomolecular coacervates has been elucidated by microscopy, the detailed dynamic properties of proteins/peptides during the LLPS process remain poorly characterized. Here, site-directed spin labeling-electron paramagnetic resonance (SDSL-EPR) spectroscopy was employed to characterize the dynamic properties of a minimal model LLPS system consisting of positively charged peptides and RNA. The degree of phase separation, indicated by broadening of the EPR spectrum of the spin-labeled peptide due to slow molecular tumbling, was monitored by EPR. In addition, three distinct populations with varying molecular motion during LLPS, featuring different spectral lineshapes, were identified. These populations included a fast motion component (Ⅰ), a slower motion component (Ⅱ) associated with peptides in the dispersed phase and an immobile component (Ⅲ) observed in the dense phase. With gradual titration of the peptides to RNA, the EPR spectrum gradually shifted, reflecting changes in the populations of the components. Together, SDSL-EPR method not only provides new insights into the dynamic behavior of biomolecules during LLPS, but also offers a sensitive method for biomolecular phase separation processes at the molecular level.
Two thioamino acids and four fluorinated amino acids were employed to substitute either partially or entirely the Ile2, Ser3, Ile6, and Ser7 residues of Leu10-teixobactin to prepare ten analogues and the bioactivity of them was investigated. The SAR studies revealed that Ile6 was tolerable for both thioamidation and fluoridation, while Ser7 was identified as the most tolerable site for thioamidation. Analogue 1a demonstrated comparable or slightly improved antibacterial activity, superior protease stability compared to Leu10-teixobactin, while not exhibiting obvious cytotoxicity against mammalian cells.
In this work, we put forward a new and universal approach, i.e., cyanine ketone method, for fabricating meso–aryl heptamethine indocyanines, which is so simple that the treatment of the easy-to-get cyanine ketones with various aromatic lithium (ArLi), followed by acidification, could straightforwardly give rise to the products in one-pot way. Importantly, due to the strong nucleophilicity of ArLi, a series of bulky hydrophilic aromatic groups can be facilely integrated into the meso–position of heptamethine indocyanines, not only effectively inhibiting the undesired dye self-aggregation but also largely improving the water-solubility. Using one of anti-aggregation meso–aryl heptamethine indocyanines, we fabricated a dye-antibody conjugate for in vivo imaging tumor in a mouse model and achieved a high tumor-to-normal tissue ratio. The work laid a chemical foundation for constructing various meso–aryl heptamethine indocyanines, facilitating the advanced imaging and therapeutic applications in future.
Mo2N has been identified as a highly promising carrier for electrocatalysis. However, its complex synthesis method, use of toxic gases, and serious effects on supported noble metals catalyst during high-temperature sintering processes have seriously affected its hydrogen evolution reaction (HER) activity and stability. Here, we report an efficient strategy for synthesizing Mo2N using the high temperature shock (HTS) method in just 1.67 s, while also uniformly loading Ru onto Mo2N nanosheets. The HTS enables the homogeneous dispersion of the noble metal Ru, leading to an increased electrocatalytic activity, along with a strong charge transfer between Mo2N and Ru. Ru/Mo2N exhibited an overpotential of 66 mV at 10 mA/cm2 in 1 mol/L KOH. In the evaluation of catalytic activity, Ru/Mo2N demonstrates superiority over commercial Pt/C catalysts in terms of mass activity (1.71 A/mgRu vs. 0.91 A/mgPt at 200 mV) and turnover frequency (1.41 s−1 vs. 0.18 s−1 at 100 mV). This result provides a rational and effective pathway for the preparation of efficient electrocatalysts.
Established evidence has unveiled two strategies for treating cancer: depleting tumor-associated macrophages (TAMs) and reprogramming M2-like TAMs into an antitumor M1 phenotype. Here, we designed novel pH-sensitive biomimetic hybrid nanovesicles (EDHPA) loaded with doxorubicin (DOX). DOX@EDHPA can specifically target TAMs by activating macrophage-derived exosomes (M1-Exos) and anisamide (AA) as cancer-specific targeting ligands. In vitro and in vivo studies demonstrated that DOX@EDHPA could efficiently be delivered to the tumor site and taken up by cells. Meanwhile, it synergistically enhanced immunogenic cell death (ICD) and induced a subsequent antigen-specific T cell immune response. The tumor inhibitory rate of the DOX@EDHPA group was 1.42 times that of the free DOX group. Further analysis showed that the excellent antitumor effects of DOX@EDHPA should ascribe to the homing effect of M1-Exos on macrophages and the repolarization to antitumor M1 TAMs, which induced the elevated secretion of pro-inflammatory factors. Therefore, the hybrid EDHPA targeting TAMs to reshape the tumor microenvironment constituted a novel immunochemotherapy strategy to inhibit tumor growth.
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