Latest ArticlesThe implementation of multiple pathogen testing is essential for a rapid response to future outbreaks and for reducing disease transmission. This study introduces a 96-channel microfluidic chip, fabricated through a molding process, which enables the batch detection of pathogens. It explores the rapid lysis and elution processes of pathogens within the microfluidic chips to ensure that nucleic acid extraction, elution, and amplification are completed entirely within the chip. This chip can extract nucleic acids from samples in just 10 min, achieving an extraction efficiency comparable to that of traditional in-tube methods. An oil phase is pre-loaded into the chip to effectively prevent aerosol contamination. This approach allows for the simultaneous detection of 21 common respiratory pathogens, with a detection limit of 10 copies per reaction. Furthermore, applications involving clinical samples demonstrate significant practicality. Compared to many traditional in-tube pathogen detection methods and molecular biology technologies that utilize microfluidic chips, this detection chip not only enables simultaneous detection of multiple pathogens but also demonstrates high sensitivity.
Constructing nanofibers with specific therapeutic effects against cancer is a challenge. Here, we present the synthesis approach and application prospects of supramolecular nanofibers, which are based on cucurbit[8]uril (CB[8]) as the host and terpyridine lanthanum ions metal complex as the guest, constructed by layer-by-layer self-assembly through supramolecular interaction. Moreover, nanofibers with lanthanide luminescence properties exhibit surprising pH-responsive deformation properties and antibacterial behavior. In the tumor micro-environment, the dramatic reduction in the size of the nanofibers enables specific and hierarchical release of anticancer drugs in tumor cells to exert an advanced therapeutic effect. In addition, the synergistic therapeutic efficacy was achieved by reducing the excess of Gram-positive and Gram-negative bacteria surrounding tumor cells. The novel supramolecular nanofibers with sequential drug release and combined therapeutic mode provide new guidance for the synthesis of drug carrier materials and direction for the promotion of nanomaterial-mediated cancer therapy.
Asplactones A–E (1–5), five unique diphenyl ether hybrids, along with two rare spiro-diphenyl ethers, aspviolaceols A (6) and B (7), were isolated and characterized from Aspergillus sp. F1–8A, an endophytic fungus associated with the parotoid glands of Bufo gargarizans Cantor. Compounds 1–5 represent the first examples of diphenyl ether hybrids fused with unusual moieties, including conjugated γ-butyrolactone and cyclopentenone. Compounds 6 and 7 are the first known natural spiro-diphenyl ethers, with 6 featuring an uncommon 6/6/6/6-membered carbon skeleton, and 7 possessing a distinct 6/6/6/6/6/6-membered diphenyl ether spiro-heterodimer carbon framework. Structural elucidation was performed using a combination of spectroscopic techniques, X-ray crystallography, and quantum-chemical calculations, and plausible biosynthetic pathways were proposed. Biologically, compounds 1, 2, 4, 6, and 7 exhibited antioxidant activity comparable to or surpassing that of vitamin C in 1,1-diphenyl-2-picrylhydrazyl (DPPH) and 2,2′-azino-bis(3-ethylbenzothiazoline-6-sulfonate) (ABTS), and ferric reducing power assays. They also significantly improved cell viability in H2O2-induced oxidative injury assays using A549 cells.
Successfully generating reactive oxygen species (ROS) in a targeted and efficient manner for the detoxification of chlorinated organic pollutants (CPs) is a significant and demanding challenge. Herein, we present an in-situ photoreduction strategy to fabricate a composite of palladium (Pd) nanoparticles anchored few-layer carbon nitride nanosheets (Pd-CN). This innovative Pd-CN is then leveraged to activate peroxymonosulfate (PMS) in pursuit of our objective. The incorporation of Pd nanoparticles enhances PMS absorption and targets its terminal oxygen, thereby aiding in the cleavage of the O-O bond. This process generates crucial intermediates, including adsorbed hydroxyl radicals (*OH) and adsorbed atomic oxygen (O*), which are essential for the production of 1O2. Consequently, the Pd-CN catalyst demonstrates strong preference for 1O2 generation during the PMS activation process, successfully degrading over 95% of pollutants such as 4-chlorophenol (4-CP), 2,4-dichlorophenol (2,4-DCP), and 2,4,6-trichlorophenol (2,4,6-TCP) within just 20 min. Additionally, the catalyst exhibits total organic carbon (TOC) removal rates ranging from 49.4% to 31.4%, while the rates for de-chlorination fall between 68.6% and 72.7%. A subsequent continuous-flow treatment experiment has confirmed the application potential of this system, demonstrating consistent catalytic activity for up to 8 h. This promising technique presents an efficient strategy for addressing the high toxicity of chlorinated organic pollutants in contaminated water.
Chiral benzylic amines are important motifs in medicines. A dicationic nickel complex of chiral diphosphine (R)-Ph-BPE promotes highly enantioselective reductive amination of aryl alkyl ketones with arylamines using isopropanol as hydrogen source. The reaction is easily scaled up in a gram-scale synthesis using 1 mol% nickel catalyst and it is applied to an asymmetric synthesis of (S)-rivastigmine. Building on this success, we achieved rare examples of asymmetric hydrogen borrowing reactions with arylamines using an Earth-abundant 3d metal, nickel.
Understanding the photoluminescence (PL) mechanism of metal nanoclusters from both molecular and supramolecular perspectives is crucial for developing highly emissive cluster-based nanomaterials. In this study, we synthesized two structurally similar Ag14 nanoclusters with different phosphine stabilizers, which demonstrated opposite PL behaviors in solution and crystalline states. The Ag14 nanocluster stabilized by P(Ph-OMe)3 ligands exhibited a higher PL intensity compared to the one stabilized by P(Ph-F)3 ligands, which was attributed to the stronger electron-donating ability of the P(Ph-OMe)3 ligand that improved ligand-to-metal charge transfer efficiency. In contrast, the P(Ph-F)3 stabilized Ag14 crystals displayed greater PL intensity than the Ag14 cluster crystal with a -OMe surface, which was due to stronger intermolecular interactions within the cluster lattice of the former that limited non-radiative energy loss and thus enhanced PL. Overall, this work aims to promote a comprehensive understanding of the fluorescence in cluster-based nanomaterials, which will be beneficial for their downstream applications.
Sulfoxides and sulfide compounds have broad-spectrum biological properties and have received considerable attention in the past few decades. Herein we reported two metal and oxidant-free, practical and efficient methods for the synthesis of highly synthetically useful and structurally diverse ortho-aminoaryl sulfoxides and 3,4,5-trisubstituted oxazolones from readily accessible N-arylhydroxylamines and N-thiophthalimides. This rapid transformation occurred smoothly to achieve chemo- and regioselective cascade rearrangements due to the differences of the protecting-groups of the nitrogen atom of N-arylhydroxyamines. DFT studies suggested that the competing S-O and S-C bond formations via SN2 nucleophilic substitution are crucial for the observed protecting-group-dependent chemoselectivity. Subsequent applications have shown that these two protocols might be powerful tools for the construction of sulfur-containing complex molecules under simple conditions.
Freshwater scarcity is exacerbated by uneven distribution of limited freshwater resources and high energy costs of desalination technologies. Atmospheric water vapor, a vast and geographically unrestricted reservoir, could become a sustainable alternative. Sorption-based atmospheric water harvesting (SAWH) has emerged as an available solution, yet conventional desorption methods relying on energy-intensive electrical heating hinder its scalability. Herein, a photothermal hygroscopic sponge has been developed for solar-driven atmospheric water harvesting. The composites combine a malleable melamine sponge skeleton, lithium chloride as a hygroscopic agent, and hydrangea-like molybdenum disulfide as a photothermal component, forming a multiscale "pore-film" cross-linked structure by an eco-friendly immersion-freeze-drying method. The optimized sample achieves exceptional hygroscopic capacity (3.92 g/g at 90% RH) and freshwater production efficiency (87.77%), which is attributed to synergistic effects of porous skeleton based crosslinked structures and "pore-film" structures, and outstanding photothermal conversion efficiency of MoS2. The unique structure could stabilize LiCl to prevent leakage, increase mass transfer effectiveness of whole SWAH process, and enable flexibility for diverse applications. We carried out outdoor experiments to demonstrate a solar-driven water production rate of 4.22 L m-2 d-1 without external energy input. This work provides insights into sustainable freshwater generation and promotes green energy utilization in addressing global water scarcity.
The coexistence of emerging containments, such as antibiotic resistant bacteria (ARB), antibiotic-resistant genes (ARGs) and antibiotics, potentially influence elimination efficiencies in UV light-emitting diode (UV-LED) alone and UV-LED/H2O2 system as their complex interactions. Tetracycline (TC) degradation efficiency (kF) correlated closely with its UV molar absorbance (R2 = 0.831) in UV-LED alone system and with •OH yield (R2 = 0.999) in UV-LED/H2O2 system across studied wavelengths (265, 280 and 310 nm). The kF values for intracellular DNA (i-ARGs) also exhibited a high correlation with UV-LED wavelengths in both systems (R2 = 0.997–0.999). The coexistence of TC and ARB/ARGs resulted in a mutual inhibition of their degradation efficiencies due to competition for photons and •OH, along with the consequent reduction in intracellular ROS within ARB, with their degradation efficiencies exhibiting marked dependence on wavelength in both systems. Notably, the UV-LED/H2O2 system at 265 nm effectively achieved the simultaneous removal of TC, ARB and ARGs with minimal energy consumption, and successfully fragmented ARGs. The degradation pathway of TC was analyzed, and the biotoxicity of its degradation intermediates demonstrated the environmental friendliness and safety of UV-LED/H2O2 technology. This study elucidated the competitive interactions between antibiotics and ARB/ARGs within UV-LED/H2O2 system, providing a promising approach for their simultaneous removal while ensuring energy efficiency.
Hard carbon (HC) in sodium-ion batteries is searched by numerous investigations, which can offer the excellent performance of reversible Na+ insertion and extraction. The covalent heteroatom doping in HC is recently worth concentrating, which can dilate the interlayer spacing of graphite to adjust the electrochemical storage performance in carbon anodes. However, the reported doping strategies of the modified HC have only resulted in limited improvement, especially unobvious effects on tuning porous structure. In this study, tannin extract and K2SO4 are respectively utilized as carbon source and sulfur source for the fabrication of HC, in which K2SO4 can contribute to the heteroatom doping, and the pore forming as well. The tannin-derived sulfur-doped carbon anode shows the excellent cycle stability, achieving a high reversible capacity of 520.5 mAh/g at a current density of 100 mA/g. Even after 500 cycles at a current density of 3 A/g, a high specific capacity of 236.7 mAh/g and a capacity retention rate of 92.6% can be reserved. Compared with the initial carbon, the adsorption energy of Na+ is multifold times higher, whereas Na+ diffusion energy barriers manyfold decrease. Moreover, the full battery assembled with Na3V2(PO4)3/tannin-based HC demonstrates a stable cycling performance. This work can manifest the potentiality of the tannin-based electrode as anode for a high-performance sodium-ion batteries (SIBs), which could especially offer an explanation of Na+ storage and solid-electrolyte interface (SEI) stability to the electrochemical performance.
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