Latest ArticlesSi coordination structures have been proven to greatly influence the ammonia-selective catalytic reduction (NH3-SCR) catalytic properties and the hydrothermal stability of Cu-based silicoaluminophosphate-form catalysts. However, the role of various Si coordination structures in the NH3-SCR reaction over Cu-SAPO-34 catalyst remains unknown. Herein, a batch of Cu-SAPO-34 samples with various Si contents was synthesized via a one-pot method to study the role of Si coordination structures in the NH3-SCR catalytic properties and hydrothermal stability. Cu/34–2 with the highest proportion of Si(xOAl) (x = 1~3) structures exhibits remarkable durability with 90% NO reduction efficiency within 200~450 ℃ even after a hydrothermal aging treatment at 850 ℃. In contrast, Cu/34–1 and Cu/34–4 with the highest proportions of Si(4OAl) and Si(0OAl) structures, respectively, are significantly deactivated by the same hydrothermal treatment. To better understand this phenomenon, the relationship between the Si coordination structures and SCR performance is established using characterization techniques and kinetics measurements. Results reveal that a high content of Si(4OAl) and Si(0OAl) is detrimental to the hydrothermal stability of Cu-SAPO-34 catalyst. However, Si(xOAl) (x = 1~3) structures are conducive to the stabilization of isolated Cu2+, thus enhancing the stability to severe hydrothermal treatment.
Chiral covalent organic frameworks (CCOFs) featuring chirality, stability, and good porosity have attracted a considerable amount of attention due to their important applications, such as asymmetric catalysis, chiral separation, and chiral recognition. In this study, a β-cyclodextrin (β-CD) covalent organic framework (β-CD-COF) diluted with polysiloxane OV-1701 was explored as a novel chiral stationary phase (CSP) for gas chromatography (GC) separation of racemates. The β-CD-COF coated capillary column had excellent selectivity, not only for the separation of linear alkanes, linear alcohols, fatty acid methyl esters mixture, the Grob mixture and positional isomers, but also for the resolution of chiral compounds, including chiral alcohols, aldehydes, ethers, and amino acid derivatives. In addition, the β-CD-COF-coated capillary column presented good repeatability and reproducibility. This work indicated the great potential of the CCOFs coated capillary column for the chromatographic separation of enantiomers.
In this work, the nano-g-C3N4/UiO-66-NH2 composite was prepared by one-step solvothermal method. The as-prepared composite was characterized by scanning electron microscopy, Brunner-Emmet-Teller measurement, energy dispersive spectrometer, X-ray diffraction, and Fourier transform infrared spectroscopy. By using nano-g-C3N4/UiO-66-NH2 composite as sorbent, a dispersive solid-phase extraction coupled with high-performance liquid chromatography was developed to sensitive analysis of food colorants including tartrazine, amaranth, carmine, sunset yellow, allura red and bright blue. The experiment parameters including the amount of sorbent, adsorption time, the pH of adsorption solution, desorption time, desorption solvent, the pH of desorption solution as well as the proportion between desorption solvent and buffer solvent were investigated. Under the optimized conditions, the limits of detection (S/N = 3) and limits of quantitation (S/N = 10) were determined in the ranges of 0.08–0.8 and 0.2–2.0 ng/mL, respectively. With the developed sample pretreatment method, carmine and brilliant blue were determined from blueberry juice by HPLC-DAD. The contents were calculated as 1.53 µg/mL and 0.17 µg/mL, respectively.
To address the challenge of treating complex pollutants containing heavy metals and organic compounds, a phenanthroline/TiO2 nanocomposite with rich oxygen vacancy defects was synthesized to integrate the functions of pollutant detection, adsorption, and photocatalytic degradation. The results showed that the nanocomposite could adsorb Cr3+ and the process could be transduced into a colorimetric signal for qualitative and quantitative detection. The adsorbed heavy metal also exhibited a synergistically enhanced photocatalytic degradation of a model organic pollutant under visible light. The simultaneous adsorption, detection, and photocatalysis could reduce the multifarious operations and high cost of traditional environmental remediation methods, indicating a strong application potential for the nanocomposite.
Pomalidomide is an immunomodulatory agent (IMiD) that has been approved by the US Food and Drug Administration (FDA) for clinical treatment of patients with multiple myeloma. In this work, we developed a sensitive and validated LC-MS/MS method for high-throughput determination of pomalidomide over the range of 1.006–100.6 ng/mL (R2 = 0.9991) in human plasma and pharmacokinetic studies. A liquid-liquid extraction method using ethyl acetate was applied to extract pomalidomide and afatinib (as an internal standard, IS) from human plasma. Chromatographic separation was performed on a Hedera ODS column (150 mm × 2.1 mm, 5 µm) with security guard C18 column (4 mm × 2.0 mm) at 40 ℃. Methanol and 10 mmol/L aqueous solution of ammonium acetate containing 0.1% formic acid were used as a gradient elution mobile phase, and the flow rate was 0.4 mL/min. A triple quadruple tandem mass spectrometer using multiplex reaction monitoring mode (MRM) with electrospray ionization (ESI) positive ionization was employed. The precursor to product ion transitions for the quantitative analysis of pomalidomide and the IS were m/z 274.2→163.1 and m/z 486.1 → 371.1, respectively. This established method has been validated according to regulatory guideline, and the results were all within the acceptance criteria. The validated LC-MS/MS method was successfully applied to analyze samples obtained from clinical pharmacokinetics study after oral administration of pomalidomide (4 mg) capsules in human.
The electro-Fenton process, with its capacity for in-situ H2O2 formation and Fe2+ regeneration, is a striking alternative to the traditional chemical-Fenton process. However, the frequent requirement of extra binders for electrode fabrication leads to low catalyst utilization, a complex fabrication process, and weak conductivity. Herein, a three-dimensional (3D) porous electrode was fabricated in-situ on a Ni foam (NF) substrate integrated with nitrogen-doped carbon nanotubes (N@C) derived from carbonization of zeolitic imidazolate framework-8 (ZIF-8) without any binder. The resulting 900/N@C-NF cathode (synthesized at 900 ℃) was high in surface area, N content, and degree of graphitization, achieved high performance of H2O2 production (2.58 mg L−1 h-1 H2O2/mg catalyst) at -0.7 V (vs. SCE), and enabled prompt regeneration of Fe2+. The electro-Fenton system equipped with the 900/N@C-NF cathode was effective in removing a diverse range of organic pollutants, including rhodamine B (RhB), phenol, bisphenol A (BPA), nitrobenzene (NB), and Cu-ethylenediaminetetraacetic acid (EDTA), and significantly attenuating the concentration of chemical oxygen demand (COD) in the real acid wastewater, exhibiting superior activity and stability. This binder-free and self-supporting electro-Fenton cathode was thus shown to be an attractive candidate for application to wastewater treatment, particularly those rich in organics, acids, and Fe3+/Fe2+.
In this work, hierarchical NiS@ZnIn2S4 heterostructure was developed by constructing ultra-thin ZnIn2S4 (ZIS) nanosheets on hollow NiS nanospheres for hydrogen production from photocatalytic water splitting. The NiS@ZIS displayed a strong optical absorption ability in the visible region and a high specific surface area of 33.14 m2/g. The Type-I band alignment in NiS@ZIS heterostructure was determined by the combination of UV–vis absorption spectroscopy and Mott-Schottky curves. The photocatalytic hydrogen production of NiS@ZIS (1.24 mmol g-1 h-1) was nearly 5.6 times higher than that of ZIS under visible light, in the absence of any co-catalyst and sacrificial agent. The separation and migration of charge in NiS@ZIS were characterized by a series of spectroscopy and photo/electrochemical tests, which verified the efficient charge transfer from ZIS to NiS.
As an antibiotic, sulfadiazine has posed a serious threat to humans and ecosystems due to its chronic toxicity. The advanced oxidation processes (AOPs) via heterogeneous catalytic activation of peroxymonosulfate (PMS) have significant potential for the degradation of antibiotics. However, there are multiple restrictions including non-specifically binding to target contaminants, which would deplete oxidation capacity, and lacking energy effectiveness due to inefficient utilization of reactive oxygen species (ROS). To overcome these obstacles, we adopted the "bait-hook & destroy" strategy in this study. Herein, we synthesized a novel micrometer-sized NiOOH hierarchical spheres assembled from nanosheets, which have relatively large specific surface areas and yield specified cavities to "bait-hook" sulfadiazine and PMS onto the surface cavities. This process was further conductive to effective generation of ROS and subsequently "destruction" of sulfadiazine with elevated mass transformation rate. 20.4% of sulfadiazine can adsorb to NiOOH surface in less than 30 min (0.0051 min−1), and then sulfadiazine was completely degraded in 90 min intervals in the NiOOH/PMS system. The degradation rate constant (k = 0.0537 min−1) was about 5.3, 2.5 and 2.2 times higher than that in Ni2O3/PMS, NiO/PMS and Ni(OH)2/PMS system, respectively. This was ascribed to the synergistic catalytic oxidation and adsorption process occurred on the surface of NiOOH. Appreciably, there were both non-radicals (1O2) and radicals (O2•− and SO4•−) involved in the NiOOH/PMS system, and 1O2 was distinguished as the dominated ROS for degradation of sulfadiazine. This study provides a novel strategy via synergistic adsorption and catalytic oxidation, and indicates that the micrometer-sized NiOOH hierarchical sphere as heterogeneous catalyst is an attractive candidate for potential application of the SR-AOPs technology in water treatment.
CeO2/TiO2 (denoted as CeTi) catalysts obtained by solid-phase impregnation behaved better in low-temperature selective catalytic reduction of NO with NH3 (NH3-SCR) than that by conventional wet impregnation. To explore the main factors for activity distinction, the texture property, CeO2 dispersion and structure changes of TiO2 were comprehensively analyzed. It was found that surface changes of TiO2 had a significant impact on the improved activity. From results of inductively coupled plasma atomic emission spectrometer (ICP-AES), diffuse reflectance UV–vis spectroscopy (UV–vis-DRS) and Raman, it was inferred that Ce ions were partially incorporated into TiO2 lattice, accompanied with the formation of defects and vacancies during solid-phase impregnation. Accordingly, CeTi catalysts from solid-phase impregnation exhibited superiority in adsorption and activation of reactants. Further result from monitoring the preparation process indicated that the evolved NO played an important role in promoting Ce doping through depriving oxygen atoms on TiO2 surface. The interaction between Ce and Ti was enhanced. The catalyst performed better in NH3-SCR, especially at low temperature, which testified the solid-phase impregnation could be an effective method to modulate interface structure for designing efficient catalyst.
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