Latest ArticlesA visible light-promoted fast photochemical Wolff rearrangement was developed toward synthesis of α-substituted amides in continuous flow with the use of a photochemical oscillatory flow reactor (POFR). The control experiment indicates that a fast process of the Wolff rearrangement (<40 s) is involved. Notably, this protocol does not require excess use of any reactants, and the resulting α-substituted amides could be isolated by recrystallization in good to excellent yields.
Wearable flexible sensor devices have the characteristics of lightweight and miniaturization. Currently, power supply and detection components limit the portability of wearable flexible sensor devices. Meanwhile, conventional liquid electrolytes are unsuitable for the integration of sensing devices. To address these constraints, wearable biofuel cells and flexible electrochromic displays have been introduced, which can improve integration with other devices, safety, and color-coded display data. Meanwhile, electrode chips prepared through screen printing technology can further improve portability. In this work, a wearable sensor device with screen-printed chips was constructed and used for non-invasive detection of glucose. Agarose gel electrolytes doped with PDA-CNTs were prepared, and the mechanical strength and moisture retention were significantly improved compared with traditional gel electrolytes. Glucose in interstitial fluid was non-invasive extracted to the skin surface using reverse iontophoresis. As a biofuel for wearable biofuel cells, glucose drives self-powered sensor and electrochromic display to produce color change, allowing for visually measurement of glucose levels in body fluids. Accurate detection results can be visualized by reading the RGB value with a cell phone.
Atomically dispersed Cu-based single-metal-site catalysts (Cu-N-C) have emerged as a frontier for electrocatalytic oxygen reduction reactions (ORR) because they can effectively optimize the d-band center of the Cu active site and provide appropriate adsorption/desorption energy for oxygen-containing intermediates. Metal-organic frameworks (MOFs) show excellent prospects in many fields because of their structural regularity and designability, but their direct use for electrocatalysis has been rarely reported due to the low intrinsic conductivity. Here, a MOF material (Cu-TCNQ) with highly regular single-atom copper active centers was successfully prepared using a solution chemical reaction method. Subsequently, Cu-TCNQ and graphene oxide (GO) were directly self-assembled to form a Cu-TCNQ/GO composite, which improved the conductivity of the catalyst while maintained the atomically precise controllability. The resistivity of the Cu-TCNQ/GO decreased by three orders of magnitude (1663.6–2.7 W/cm) compared with pure Cu-TCNQ. The half-wave potential was as high as 0.92 V in 0.1 mol/L KOH, even better than that of commercial 20% Pt/C. In alkaline polymer electrolyte fuel cells (APEFCs), the open-circuit voltage and power density of Cu-TCNQ/GO electrode reached 0.95 V and 320 mW/cm2, respectively, which suggests that Cu-TCNQ/GO has a good potential for application as a cathode ORR catalyst.
Sensitization of metal-centered forbidden transitions is of great significance. Solid MnⅡ-based phosphors with d-d forbidden transition sensitized by CeⅢ with d-f allowed transition are promising light conversion materials, but the energy transfer mechanism in CeⅢ-MnⅡ is still in dispute for the uncertainty of distances between metal centers. Herein, for the first time, we explored the energy transfer mechanism in two well-designed luminescent heteronuclear complexes with clear crystal structures, i.e., Ce-N8-Mn and Ce-N2O6-Mn (N8 = 1,4,7,10,13,16,21,24-octaazabicyclo[8.8.8]hexacosane; N2O6 = 4,7,13,16,21,24-hexaoxa-1,10-diazabicyclo[8.8.8]hexacosane). Short distances between metal centers facilitate efficient energy transfer from CeⅢ to MnⅡ in both complexes, resulting in high photoluminescence quantum yield up to unity. After systematic study of the two heteronuclear complexes as well as two reference complexes Ce(N8)Br3 and Ce(N2O6)Br3, we concluded that dipole-quadrupole interaction is the dominant energy transfer mechanism in the heteronuclear complexes.
A series of heteronuclear yttrium-nickel monoxide carbonyl complexes YNiO(CO)n− (n = 1–5) were generated in a pulsed-laser vaporization source and characterized by mass-selected photoelectron velocity-map spectroscopy combined with theoretical calculations. CO ligand-mediated reactivity in CO oxidation of yttrium-nickel monoxide carbonyl complexes was experimentally and theoretically identified. During the consecutive CO adsorption, a μ2-O linear structure was most favorable for YNiO(CO)n− (n = 1, 2), then a structure in which the terminal O was bonded to the Y atom became favored for YNiO(CO)3−, and finally a structure bearing a CO2 moiety was most favorable for YNiO(CO)n− (n = 4, 5). Theoretical calculations indicated that the Ni atom acted as an electron acceptor and accumulated electron density at n ≤ 3, and then served as an electron donor along with the Y atom to contribute electron density in the rearrangement that accompanied CO oxidation at n > 3.
The considerable hazard posed by periprosthetic joint infections underlines the urgent need for the rapid advancement of in-situ drug delivery systems within joint materials. However, the pursuit of sustained antibacterial efficacy remains a formidable challenge. In this context, we proposed a novel strategy that leverages swelling and erosion mechanisms to facilitate drug release of drug-loaded ultrahigh molecular weight polyethylene (UHMWPE), thereby ensuring its long-lasting antibacterial performance. Polyethylene oxide (PEO), a hydrophilic polymer with fast hydrating ability and high swelling capacity, was incorporated in UHMWPE alongside the antibacterial tea polyphenol (epigallocatechin gallate, EGCG as representative). The swelling of PEO enhanced water infiltration into the matrix, while the erosion of PEO balanced the release of the encapsulated EGCG, resulting in a steady release. The behavior was supported by the EGCG release profiles and the corresponding fitted release kinetic models. As demonstrated by segmented antibacterial assessments, the antibacterial efficiency was enhanced 2 to 3 times in the PEO/EGCG/UHMWPE composite compared to that of EGCG/UHMWPE. Additionally, the PEO/EGCG/UHMWPE composite exhibited favorable biocompatibility and mechanical performance, making it a potential candidate for the development of drug-releasing joint implants to combat prosthetic bacterial infections.
Accurate determination of lung cancer margins at the molecular level is of great significance to determine the optimal extent of resection during surgical operation and reduce the risk of postoperative recurrence. In this study, internal extractive electrospray ionization mass spectrometry (iEESI-MS) was used to trace potential molecular tumor margins in lung cancer tissue. Molecular differential model for the determination of lung cancer tumor margin was established via partial least-squares discriminant analysis (PLS-DA) of iEESI-MS data collected from lung tissue pieces within cancer tumor area and iEESI-MS data collected from lung tissue pieces outside cancer tumor area. Proof-of-concept data demonstrate that the developed molecular differential model yields ca. 1–2 mm wider potential molecular tumor margin of a lung cancer compared to the conventional histological analysis, showing promising potential of iEESI-MS to increase the accuracy of tumor margins determination and lower risk of lung cancer postoperative recurrence. Furthermore, our results revealed that creatine and taurine showed positive correlations with lung cancer.
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