A Modified Vancomycin Molecule Confers Potent Inhibitory Efficacy against Resistant Bacteria Mediated by Metallo-β-Lactamases

Multidrug-resistant bacterial infections mediated by metallo-β-lactamases (MβLs) have grown into an emergent health threat, and development of novel antimicrobials is an ideal strategy to combat the infections. Herein, a novel vancomycin derivative V_b was constructed by conjugation of triazolylthioacetamide and vancomycin molecules, characterized by reverse-phase high performance liquid chromatography (HPLC) and confirmed by matrix-assisted laser desorption/ionization-time of flight mass spectrometry (MALDI-TOF MS). The biological assays revealed that V_b effectively inhibited S. aureus and methicillin-resistant S. aureus (MRSA), gradually increased the antimicrobial effect of β-lactam antibiotics (cefazolin, meropenem and penicillin G) and exhibited a dose-dependent synergistic antibacterial effect against eight resistant strains tested, which was confirmed by the time-kill curves determination. Most importantly, V_b increased the antimicrobial effect of meropenem against the clinical isolates EC08 and EC10 and E. coli producing ImiS and CcrA, resulting in a 4- and 8-fold reduction in MIC values, respectively, at a dose up to 32 μg/mL. This work offers a promising scaffold for the development of MβLs inhibitors, specifically antimicrobials for clinically drug-resistant isolates.     

Protective Effect of Flavonoids against Methylglyoxal-Induced Oxidative Stress in PC-12 Neuroblastoma Cells and Its Structure–Activity Relationships

Methylglyoxal-induced oxidative stress and cytotoxicity are the main factors causing neuronal death-related, diabetically induced memory impairment. Antioxidant and anti-apoptotic therapy are potential intervention strategies. In this study, 25 flavonoids with different substructures were assayed for protecting PC-12 cells from methylglyoxal-induced damage. A structure–activity relationship (SAR) analysis indicated that the absence of the double bond at C-2 and C-3, substitutions of the gallate group at the 3 position, the pyrogallol group at the B-ring, and the R configuration of the 3 position enhanced the protection of flavan-3-ols, and a hydroxyl substitution at the 4′ and meta-positions were important for the protection of flavonol. These SARs were further confirmed by molecular docking using the active site of the Keap1–Nrf2 complex as the receptor. The mechanistic study demonstrated that EGCG with the lowest EC₅₀ protected the PC-12 cells from methylglyoxal-induced damage by reducing oxidative stress via the Nrf2/Keap1/HO-1 and Bcl-2/Bax signaling pathways. These results suggested that flavan-3-ols might be a potential dietary supplement for protection against diabetic encephalopathy.     

Aggregation-Induced Intermolecular Charge Transfer Emission for Solution-Processable Bipolar Host Material via Adjusting the Length of Alkyl Chain

Molecules with donor–spacer–acceptor configuration have been developed rapidly given their peculiar properties. How to utilize intermolecular interactions and charge transfers for solution-processed organic light-emitting diodes (OLEDs) greatly relies on molecular design strategy. Herein, soluble luminophores with D-spacer-A motif were constructed via shortening the alkyl chain from nonane to propane, where the alkyl chain was utilized as a spatial linker between the donor and acceptor. The alkyl chain blocks the molecular conjugation and induces the existence of aggregation-induced intermolecular CT emission, as well as the improved solubility and morphology in a solid-state film. In addition, the length of the alkyl chain affects the glass transition temperature, carrier transport and balance properties. The mCP-3C-TRZ with nonane as the spacer shows better thermal stability and bipolar carrier transport ability, so the corresponding solution-processable phosphorescent organic light-emitting diodes exhibit superior external quantum efficiency of 9.8% when using mCP-3C-TRZ as a host material. This work offers a promising strategy to establish a bipolar host via utilizing intermolecular charge transfer process in an aggregated state.     

Analysis of Components and Properties of Extractives from Alnus cremastogyne Pods from Different Provenances

Chemical components with anti-oxidant, anti-inflammatory, and anti-cancer properties extracted from Alnus bark and leaves have been extensively studied. However, less attention has been paid to extractives from Alnus pods, which are mostly treated as waste. Here, extractives of Alnus cremastogyne pods from 12 provenances in Sichuan Province were studied for high value-added utilization of Alnus waste. The extractives were analyzed by Gas Chromatography-Mass Spectrometer (GC-MS), Ultraviolet-visible spectroscopy (UV-Vis spectra), and 1,1-diphenyl-2-picrylhydrazyl (DPPH) scavenging activity. A total of 58, 49, and 51 chemical components were found when the organic solvents of ethanol, petroleum ether, and ethyl acetate were used to collect extractives, respectively. These chemical components including Phytol, CIS-5,8,11,14,17-eicosapentaenoic acid, Germacrene D, Lupeol, and β-sitosterol, etc., have wide applications in the fields of pharmacy and cosmetics. Moreover, it was also found that extractives in ethanol and ethyl acetate had impressive UV resistance, especially for UV-C and UV-B blocking. The results showed that the maximum block ratio towards UV-C and UV-B could reach 99%. In addition, the ethanol extract showed good anti-oxidant activity with a maximum free radical scavenging rate of 96.19%. This comprehensive and systematic study on extractives from Alnus cremastogyne pods promotes the development of high-value utilization of Alnus components.     

Contact-Piezoelectric Bi-Catalysis of an Electrospun ZnO@PVDF Composite Membrane for Dye Decomposition

The treatment of organic pollutants in wastewater is becoming a great challenge for social development. Herein, a novel contact-piezoelectric bi-catalysis of a ZnO@ PVDF composite membrane was prepared by electrospinning technology. The obtained ZnO@PVDF composite membranes is superior to the pure PVDF membrane in decomposing methyl orange (MO) under ultrasonication at room temperature, which is mainly attributed to the synergy effect of the contact-electro-catalysis of dielectric PVDF, as well as the piezoelectric catalysis of tetrapodal ZnO and the β-phase of PVDF. The heterostructure of the piezoelectric-ZnO@dielectric-PVDF composite is beneficial in reducing the electron/hole pair recombination. As compared to the pure PVDF membrane, the catalytic degradation efficiency of the ZnO@PVDF composite membrane was improved by 444.23% under ultrasonication. Moreover, the reusability and stability of the composite membrane are comparable to those of the traditional powdered catalyst. This work offers a promising strategy for improving the pollutant degradation by combining contact-electro-catalysis with piezoelectric catalysis.     

By-Product of the Red Ginseng Manufacturing Process as Potential Material for Use as Cosmetics: Chemical Profiling and In Vitro Antioxidant and Whitening Activities

Red ginseng (RG), which is obtained from heated Panax ginseng and is produced by steaming followed by drying, is a valuable herb in Asian countries. Steamed ginseng dew (SGD) is a by-product produced in processing red ginseng. In the present study, phytochemical profiling of extracts of red ginseng and steamed ginseng dew was carried out using gas chromatography-mass spectrometry (GC-MS) and rapid resolution liquid chromatography coupled with quadrupole-time-of-flight mass spectrometry (RRLC-Q-TOF-MS) analysis. Additionally, antioxidant activities (DPPH, ·OH, and ABTS scavenging ability) and whitening activities (tyrosinase and elastase inhibitory activity) were analyzed. Phytochemical profiling revealed the presence of 66 and 28 compounds that were non-saponin components in chloroform extracts of red ginseng and steamed ginseng dew (RG-CE and SGD-CE), respectively. Meanwhile, there were 20 ginsenosides identified in n-butanol extracts of red ginseng and steamed ginseng dew (RG-NBE and SGD-NBE). By comparing the different polar extracts of red ginseng and steamed ginseng dew, it was found that the ethyl acetate extract of red ginseng (RG-EAE) had the best antioxidant capacity and whitening effect, the water extract of steamed ginseng dew (SGD-WE) had stronger antioxidant capacity, and the SGD-NBE and SGD-CE had a better whitening effect. This study shows that RG and SGD have tremendous potential to be used in the cosmetic industries.     

Urea Synthesis from Isocyanides and O-Benzoyl Hydroxylamines Catalyzed by a Copper Salt

In the presence of CuOAc, a series of unsymmetric ureas can be generated in moderate to good yields under mild reaction conditions (10 mol% of CuOAc, 2 equiv t-BuONa or PhONa, 30 °C), using aryl isocyanides and O-benzoyl hydroxylamines as the readily accessible starting materials. The reactions might undergo a cascade process involving isocyanide insertion into the N-O bond and Mumm-type rearrangement. This work represents a rare example of isocyanide insertion into N-O bonds, which would extend isocyanide insertion chemistry.     

Pseudo-mono-axial ligand fields that support high energy barriers in triangular dodecahedral Dy(iii) single-ion magnets

The synthesis of air-stable, high-performance single-molecule magnets (SMMs) is of great significance for their practical applications. Indeed, Ln complexes with high coordination numbers are satisfactorily air stable. However, such geometries easily produce spherical ligand fields that minimize magnetic anisotropy. Herein, we report the preparation of three air-stable eight-coordinate mononuclear Dy(iii) complexes with triangular dodecahedral geometries, namely, [Dy(BPA-TPA)Cl](BPh₄)₂ (1) and [Dy(BPA-TPA)(X)](BPh₄)₂·nCH₂Cl₂ (X = CH₃O⁻ and n = 1 for 2; L = PhO⁻ and n = 2 for 3), using a novel design concept in which the bulky heptadentate [2,6-bis[bis(2-pyridylmethyl)amino]methyl]-pyridine (BPA-TPA) ligand enwraps the Dy(iii) ion through weak coordinate bonds leaving only a small vacancy for a negatively charged (Cl⁻), methoxy (CH₃O⁻) or phenoxy (PhO⁻) moiety to occupy. Magnetic measurements reveal that the single-molecule magnet (SMM) property of complex 1 is actually poor, as there is almost no energy barrier. However, complexes 2 and 3 exhibit fascinating SMM behavior with high energy barriers (U_eff = 686 K for 2; 469 K for 3) and magnetic hysteresis temperatures up to 8 K, which is attributed to the pseudolinear ligand field generated by one strong, highly electrostatic Dy–O bond. Ab initio calculations were used to show the apparent difference in the magnetic dynamics of the three complexes, confirming that the pseudo-mono-axial ligand field has an important effect on high-performance SMMs compared with the local symmetry. This study not only presents the highest energy barrier for a triangular dodecahedral SMM but also highlights the enormous potential of the pseudolinear Dy–L ligand field for constructing promising SMMs.

Air-stable triangular dodecahedral Dy(iii) single-ion magnets with pseudo-mono-axial linear ligand fields exhibit high energy barrier exceeding 600 K, which represent the highest energy barrier for mononuclear SMMs with triangular dodecahedron.     

A smelting–rolling strategy for ZnIn bulk phase alloy anodes

Reversibility and stability are considered as the key indicators for Zn metal anodes in aqueous Zn-ion batteries, yet they are severely hindered by uncontrolled Zn stripping/plating and side reactions. Herein, we fabricate a bulk phase ZnIn alloy anode containing trace indium by a typical smelting–rolling process. A uniformly dispersed bulk phase of the whole Zn anode is constructed rather than only a protective layer on the surface. The Zn deposition can be regarded as instantaneous nucleation due to the adsorption of the evenly dispersed indium, and formation of the exclusion zone for further nucleation can be prevented at the same time. Owing to the bulk phase structure of ZnIn alloy, the indium not only plays a crucial role in Zn deposition, but also improves the Zn stripping. Consequently, the as-designed ZnIn alloy anode can sustain stable Zn stripping/plating for over 2500 h at 4.4 mA cm⁻² with nearly 6 times smaller voltage hysteresis than that of pure Zn. Moreover, it enables a substantially stable ZnIn//NH₄V₄O₁₀ battery with 96.44% capacity retention after 1000 cycles at 5 A g⁻¹. This method of regulating the Zn nucleation by preparing a Zn-based alloy provides a potential solution to the critical problem of Zn dendrite growth and by-product generation fundamentally.

A ZnIn alloy anode with trace indium is obtained by smelting–rolling method. The Zn deposition could be regarded as instantaneous nucleation that can alleviate the effect of deposition layer for the diffusion zone and suppresses dendrite growth.