Latest ArticlesA novel biodegradable material, Se@PLA, was designed and prepared via the selenization reaction of polylactic acid using NaHSe as the selenization reagent. This material shows excellent antibacterial activity (EC50 = 13.38 µg/mL) against Xanthomonas oryzae pv. Oryzae, which is a highly destructive pathogen responsible for rice bacterial blight. Se@PLA induces oxidative stress in bacteria, leading to the rupture of bacterial cell membranes and eventual death. Moreover, Se@PLA can significantly inhibit the motility of bacteria and is low toxic to soil and aquatic organisms. This work provides an effective method for preventing and controlling rice bacterial blight, and reveals the great potential of using Se@PLA as an alternative next generation plant bactericide.
The adsorption of peroxymonosulfate (PMS) is crucial for PMS activation in the heterogeneous advanced oxidation processes. However, the investigation of PMS adsorption on the piezocatalysts still remains insufficient. In this work, bismuth oxychloride (BiOCl) nanosheets were prepared as the piezocatalysts for PMS activation under ultrasonic vibration to remove carbamazepine (CBZ) in aqueous solutions. Up to 92.5% of CBZ was degraded for 40 min in BiOCl piezo-activated PMS system with the reaction rate constant of 0.0741 min−1, being 1.63 times that of the sum of BiOCl piezocatalysis, BiOCl-activated PMS, and vibration-activated PMS. PMS adsorption on the surface of BiOCl was specifically studied by comparing the microscopic structure change of the fresh and used BiOCl. The results suggested that the piezoelectric field of BiOCl was able to promote the tight adsorption of PMS on the surface, thus facilitating the fast activation of PMS through electrons transfer to produce reactive species (HO•, SO4•−, O2•−, 1O2). This work presents an in-depth understanding for the role of piezoelectric effect on the adsorption and activation of PMS.
Reactive oxygen species (ROSs) in Fenton process are of great importance in treating contaminants in wastewater. It is crucial to understand their chemical properties, formation, and reaction mechanisms with contaminants. This review summarizes the reactive oxygen species in Fenton process, including hydroxyl radical (•OH), superoxide radical (O2•−), singlet oxygen (1O2), hydroperoxyl radical (HO2•), and high-valent iron. •OH shows a trend to react with chemistry groups with abundant electrons through H-atom abstraction, radical adduct formation and single electron transfer. Electron transfer is discovered to be an important pathway when 1O2 degrades organic pollutants. Ring-opening and β-scission are proposed to be the possible ways of 1O2 to certain contaminants. Proton abstraction, nucleophilic substitution, and single electron transfer are proposed to explain how O2•− degrade pollutants. As the conjugated acid of O2•−, radical adduct formation and H-atom abstraction are reported for the reaction mechanisms of hydroperoxyl radical. High-valent iron in Fenton, namely Fe(Ⅳ), reacts with certain pollutants via single- or two-electron transfer. This review is important for researchers to understand the ROSs produced in Fenton and how they react with pollutants.
Rhodium-catalyzed C4aryl−H activation and ring-retentive annulation of 2H-imidazoles with internal alkynes to build imidazo[5,1-a]isoquinolinium salts with high yields and broad scope has been disclosed. These novel salts serve as new full-color emissive fluorophores (433−633 nm), just by simply modifying the substituents on C3 and C4 positions of isoquinoline ring. Furthermore, these salts can undergo ring-opening C5aryl−H activation/annulation with a different alkyne to form non-symmetric and AIE-active 1,1′-biisoquinolines, where NH4OAc plays an indispensable role that accounts for Hofmann elimination and imine formation, leading to an unprecedented imine dance: cyclic imine → N-alkenyl imine → NH imine. The 15N labelling experiments indicate that the 2nd annulation includes two pathways: N-exchange (major) and N-retention (minor).
A novel and readily available binaphthyl-based fluorescent probe (S)-1 was designed and synthesized. (S)-1 can be used to not only chemoselectively discriminate 3 basic amino acids out of common amino acids, but also enantioselectively recognize histidine. Encouragingly, enantioselective imaging of histidine in cells was achieved for the first time by the probe (S)-1. These performances endowed it potential application in the chiral analysis of basic amino acids in asymmetric synthesis and cell imaging for diagnosis of diseases caused by racemization of histidine. Nuclear magnetic resonance (NMR) and mass spectrometry investigations suggested that different reaction extent of (S)-1 with l/d-histidine and different product structures generated the observed enantioselective fluorescent response. The molecular structures and thermodynamic stability of the complexes, formed from (S)-1 + Zn2+ and enantiomers of histidine, were calculated by Gaussian 16 based on density functional theory (DFT) to validate the above action mechanism.
The elimination of neonicotinoids (NEOs) from water has been a research priority due to their threats to human health and ecosystems. In this study, we established the heterogeneous peroxymonosulfate (PMS) activation system using manganese catalyst (Mn NC) and cobalt catalyst (Co NC) to trigger the nonradical oxidation and synergistic oxidation pathway, respectively to remove NEOs. The results showed that the nonradical oxidation system exhibited superior NEOs degradation capability. The composition of organic pollutants in wastewater significantly impacted subsequent degradation processes. The charge distribution and reaction sites of various NEOs were analyzed using density functional theory (DFT) calculations, and it demonstrated the electron distribution and activity of NEOs were significantly influenced by the type and number of substituents. Nitro group (–NO2) and cyanide group (–CN) were identified as strong electron-withdrawing groups and prone to be attacked by negatively charged radicals. The transformation of NEOs was analyzed, and result showed that the C and N sites adjacent to the nitro group and cyanide group were more susceptible to oxidation attacks. S and N atoms, which possess strong electronegativity and high electron cloud density, were identified as key active sites in the degradation pathway. The outcomes of this study provide valuable guidance for the oriented regulation of oxidation pathways towards efficient removal of NEOs in water.
Carbon monoxide (CO) is a vital intracellular gas messenger known for its cytoprotective and homeostatic properties. It plays a pivotal role in a myriad of biological processes. Therefore, the precise detection of CO is of paramount importance in unraveling the intricacies of pathological mechanisms and advancing the development of disease diagnosis. We herein introduce NFCOP, a state-of-the-art near-infrared (NIR) turn-on fluorescence (FL) probe that has been meticulously designed for highly sensitive, swift and selective imaging of CO. The NFCOP response occurred rapidly with CO, within just 10 s, and the calculated detection limit for CO was determined to be 0.32 µmol/L. Further investigations conducted at the cellular level and in vivo demonstrated that NFCOP possesses high sensitivity and selectivity for imaging CO.
Natural enzymes, such as horseradish peroxidase (HRP), are a class of important biocatalysts with the high specificity, but their catalytic efficiency is usually unsatisfactory. Thus, the higher catalytic efficiency induced by the confinement effect is promising in optical sensing systems. In this work, a dark-field light scattering sensing platform was fabricated by the confinement effect of HRP from hybridization chain reaction (HCR) and then released to solution by the toehold-mediated strand displacement reaction (TSDR). Then, HRP catalyzed the 3,3′, 5,5′-tetramethylbenzidine (TMB) to TMB2+ with the assistance of hydrogen peroxide, which etched the gold nanorods (AuNRs) with the weakened light scattering. The single-particle assay was established based on the decreased light scattering intensity of AuNRs under dark-field microscope. The proposed assay revealed excellent analytical performance within a linear range from 25 pmol/L to 600 pmol/L, and a low limit of detection of 3.12 pmol/L. Additionally, it also manifested satisfactory recovery of miRNA-21 in human serum samples. The high sensitivity, excellent specificity, and universal applicability make this sensing platform promising for disease diagnosis.
Nicotinamide phosphoribosyl transferase (NAMPT) is considered as a promising target for cancer therapy to its crucial role in cancer metabolism. Despite the therapeutic potential of NAMPT enzymatic inhibitors, their effectiveness is limited by dose-related toxicity and the inability to suppress nonenzymatic functions of extracellular NAMPT (eNAMPT). Herein, we designed and synthesized the first hydrophobic tagging NAMPT degraders. Among them, compound NH-11 selectively degraded NAMPT in leukemia cells through the ubiquitin-proteasome system. Compound NH-11 effectively induced apoptosis and showed low toxicity to normal cells, representing a promising anti-leukemia lead compound.
Aqueous zinc ion batteries (AZIBs) are promising energy storage devices. However, the formation of dendrites, hydrogen evolution, and corrosion reaction seriously affect their electrochemical performance. Herein, the synergistic effect of ion-migration regulation and interfacial engineering has been confirmed as the potential strategy by kaolin functionalized glass fiber separator (KL-GF) to alleviate these problems. The rapid and orderly Zn2+ migration was achieved to improve the transfer kinetics and induced uniform zinc deposition by more zinc-philic sites of KL-GF. Based on the interfacial engineering, the side reactions were effectively mitigated and crystal planes were regulated through KL-GF. The hydrophilicity of KL alleviated the corrosion and hydrogen evolution. Importantly, a preferential orientation of Zn (002) crystal plane by KL-GF was induced to further realize dendrite-free deposition by density functional theory (DFT) and X-ray diffraction (XRD) characterization. Hence, the Zn|KL-GF|MnO2 cell maintained a high discharge capacity of 96.8 mAh/g at 2 A/g after 1000 cycles. This work can provide guidance enabling high-performance zinc anode for AZIBs.
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