Atomically isolated Sb(CN)3 on sp2-c-COFs with balanced hydrophilic and oleophilic sites for photocatalytic C-H activation.

Activation of carbon-hydrogen (C-H) bonds is of utmost importance for the synthesis of vital molecules. Toward achieving efficient photocatalytic C-H activation, our investigation revealed that incorporating hydrophilic C≡N-Sb(CN)3 sites into hydrophobic sp2 carbon-conjugated covalent organic frameworks (sp2-c-COFs) had a dual effect: It simultaneously enhanced charge separation and improved generation of polar reactive oxygen species. Detailed spectroscopy measurements and simulations showed that C≡N-Sb(CN)3 primarily functioned as water capture sites, which were not directly involved in photocatalysis. However, the potent interaction between water molecules and the Sb(CN)3-modified framework notably enhanced charge dynamics in hydrophobic sp2-c-COFs. The reactive species ·O2- and ·OH (ad) subsequently combined with benzyl radical, leading to the formation of benzaldehyde, benzyl alcohol, and lastly benzyl benzoate. Notably, the Sb(CN)3-modified sp2-c-COFs exhibited a 54-fold improvement in reaction rate as compared to pristine sp2-c-COFs, which achieved a remarkable 68% conversion rate for toluene and an 80% selectivity for benzyl benzoate.

Research landscape and hotspots of selective catalytic reduction (SCR) for NOx removal: insights from a comprehensive bibliometric analysis.

Selective catalytic reduction (SCR) has been one of the most efficient and widely used technologies to remove nitrogen oxides (NOx). SCR research has developed rapidly in recent years, which can be reflected by the dramatic increase of related academic publications. Herein, based on the 10,627 documents from 2001 to 2020 in Web of Science, the global research landscape and hotspots in SCR are investigated based on a comprehensive bibliometric analysis. The results show that SCR research has developed positively; the annul number of articles increase sharply from 246 in 2001 to 1092 in 2020. People's Republic of China and Chinese Academy of Sciences are the most productive country and institution, respectively. The global collaboration is extensive and frequent, while People's Republic of China and USA have the most frequent research cooperation. Applied Catalysis B-Environmental is the leading publication source with 711 records. Five major research areas on SCR are identified and elaborated, including catalyst, reductant, deactivation, mechanism, and others. Zeolite is the most widely studied SCR catalyst, while copper, silver, platinum, and iron are the most popular metal elements in catalyst. Ammonia (NH3) is dominated among various SCR reductants, while hydrocarbon reductant has gained more attention. Sulfur dioxide (SO2) and vapor are the two most concerned factors leading to catalyst deactivation, and catalyst regeneration is also an important research topic. Density functional theory (DFT), in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS), Fourier transform infrared spectroscopy (FTIR), X-ray photoelectron spectroscopy (XPS), and kinetics are the most widely used methods to conduct mechanism study. The studies on "low temperature," "atomic-scale insight," "elemental mercury," "situ DIRFTS investigation," "arsenic poisoning," "SPOA-34," "Cu-CHA catalyst," "TiO2 catalyst," and "Ce catalyst" have been the hotspots in recent years.

The Incidence and Characteristics of Perinatal Stroke in Beijing: A Multicenter Study.

Objective: To assess the incidence, risk factors, and clinical characteristics of perinatal stroke in Beijing. Methods: This multicenter prospective study included all the live births from 17 representative maternal delivery hospitals in Beijing from March 1, 2019 to February 29, 2020. Neonates with a stroke were assigned to the study group. Clinical data, including general information, clinical manifestations, and risk factors, were collected. Up until 18 months after birth, neonates were routinely assessed according to the Ages and Stages Questionnaire (ASQ) and/or the Bayley scale. Statistical analysis was done using the chi-squared, t-tests, and logistic regression analysis using SPSS version 26.0. Outcomes: In total, 27 cases were identified and the incidence of perinatal stroke in Beijing was 1/2,660 live births, including 1/5,985 for ischemic stroke and 1/4,788 for hemorrhagic stroke. Seventeen cases (62.96%) of acute symptomatic stroke and convulsions within 72 h (10 cases, 37.04%) were the most common presentations. Ten patients showed no neurological symptoms and were found to have had a stroke through routine cranial ultrasonography after being hospitalized for non-neurological diseases. The risk factors include primiparity, placental or uterine abruption/acute chorioamnionitis, intrauterine distress, asphyxia, and severe infection. In the study group, 11.1% (3/27) of patients had adverse neurodevelopmental outcomes. The patients in the study group had lower scores for the ASQ than those in the control group in the communication, gross, and fine motor dimensions. Conclusion: The incidence of perinatal stroke in Beijing was consistent with that in other countries. Routine neuroimaging of infants with risk factors may enable identification of asymptomatic strokes in more patients. Patients who have suffered from a stroke may have neurological sequelae; therefore, early detection, treatment, and regular follow-ups are beneficial for improving their recovery outcomes.

Effects of Cu doping on electrochemical NOx removal by La0.8Sr0.2MnO3 perovskites.

Electrochemical removal of nitrogen oxides (NOx) by perovskite electrodes is a promising method due to its low cost, simple operation and no secondary pollution. In this study, a series of La0.8Sr0.2Mn1-xCuxO3 (x = 0, 0.05, 0.1 and 0.15) perovskites are fabricated as the improved electrodes of solid electrolyte cells (SECs) for NOx removal and the effects of Cu doping are investigated systematacially. Multiple characterization methods are carried out to analyze the physicochemical properties of perovskites firstly. Then the performances of cells based on various perovskites are evaluated by the measurements of electrochemical properties and NOx conversions. The results show that the Cu-doped electrode has more surface oxygen vacancies and a better redox property, thus having a higher NOx conversion and smaller polarization resistance. The electrode based on La0.8Sr0.2Mn0.9Cu0.1O3 has the maximum 70.8% NOx conversion and the lowest 36.3 Ω cm2 Rp value in the atmosphere of 1000 ppm NO at 700 °C. First-principle calculation reveals that the Cu-doped electrode is easier to form surface oxygen vacancy, while the surface oxygen vacancy plays an important role on electron transfer between electrode and NOx molecule. This study not only provides a new strategy to enhance the electrode performance for NOx removal in SECs but reveals the fundamental effect of Cu doping on the properties of La0.8Sr0.2MnO3 perovskites.

Electrochemical removal of NOx by La0.8Sr0.2Mn1-xNixO3 electrodes in solid electrolyte cells: Role of Ni substitution.

Electrochemical removal of nitrogen oxides (NOx) by solid electrolyte cells (SECs) is a promising technology due to no required reductant. Herein, a series of La0.8Sr0.2Mn1-xNixO3 (0 ≤ x ≤ 0.5) perovskites were first synthesized and utilized as the electrode materials of SECs. The role of Ni substitution in electrode performance and NOx reduction mechanism were revealed by various experimental characterization and first-principle calculations. The results indicate that the moderate Ni substitution (x ≤ 0.3) increased the NOx conversion of electrodes while reduced the polarization resistance. The further investigation shows that this improvement was attributed to the more surface oxygen vacancies, better reducibility and higher Mn4+ proportion of the Ni-substituted perovskites. The electrochemical impedance spectroscopy (EIS) shows that these changes facilitated the NOx adsorption and dissociation processes on the electrode. According to first-principle calculations, the Ni-substituted perovskite had a lower formation energy of surface oxygen vacancy, while the NO molecule adsorbed on defect surface gained more electrons thus was easier to be reduced and dissociated. Finally, the electrode performance at different operating temperatures and the operational stability were verified.

Facile Synthesis of Thiol-Functionalized Magnetic Activated Carbon and Application for the Removal of Mercury(II) from Aqueous Solution.

To improve the adsorption capacity, reduce the disposal cost, and enhance the separation efficiency of common activated carbon as an adsorbent in wastewater treatment, a novel thiol-modified magnetic activated carbon adsorbent of NiFe2O4-PAC-SH was successfully synthesized with a facile and safe hydrothermal method without any toxic and harmful reaction media. The as-prepared NiFe2O4-PAC-SH can effectively remove mercury(II) ions from aqueous solution. The maximal adsorption capacities from the experiment and Langmuir fitting achieve 298.8 and 366.3 mg/g at pH 7, respectively, exceeding most of adsorptive materials. The as-prepared NiFe2O4-PAC-SH has an outstanding regeneration performance, remarkable hydrothermal stability, and efficient separation efficiency. The data of kinetics, isotherms, and thermodynamics show that the adsorption of mercury(II) ions is spontaneous and exothermic. Ion exchange and electrostatic attraction are the main adsorption factors. The experimental results exhibit that the NiFe2O4-PAC-SH can be a prominent substitute for conventional activated carbon as an adsorbent.

Facile Synthesis of Polypyrrole-Functionalized CoFe2O4@SiO2 for Removal for Hg(II).

In order to avoid using toxic or harmful operational conditions, shorten synthesis time, enhance adsorption capacity, and reduce operational cost, a novel magnetic nano-adsorbent of CoFe2O4@SiO2 with core⁻shell structure was successfully functionalized with polypyrrole (Ppy). The physical and chemical properties of CoFe2O4@SiO2-Ppy are examined by various means. The as-prepared CoFe2O4@SiO2-Ppy nanomaterial was used to adsorb Hg2+ from water. During the process, some key effect factors were studied. The adsorption process of Hg2+ onto CoFe2O4@SiO2-Ppy was consistent with the pseudo-second-order kinetic and Langmuir models. The Langmuir capacity reached 680.2 mg/g, exceeding those of many adsorbents. The as-prepared material had excellent regeneration ability, dispersibility, and stability. The fitting of kinetics, isotherms, and thermodynamics indicated the removal was endothermic and spontaneous, and involved some chemical reactions. The application evaluation of electroplating wastewater also shows that CoFe2O4@SiO2-Ppy is an excellent adsorbent for Hg2+ ions from water.

A Mild and Facile Synthesis of Amino Functionalized CoFe2O4@SiO2 for Hg(II) Removal.

To avoid the dangerous operational conditions, shorten the preparation time, and improve the adsorption performance of amino-functionalized nanomagnetic materials with a core⁻shell structure, a magnetic nanocomposite of CoFe2O4@SiO2 was successfully functionalized with amino group (-NH2) through a mild and facile hydrothermal method without the use of any toxic or harmful solvents at a relatively low temperature. The preparation time of the key steps of amino functionalization was shortened from 30 h to about 10 h. The core-shell structure and successful grafting were confirmed by various means. The amino-functionalized CoFe2O4@SiO2 was used for the removal mercury (Hg(II)), a heavy metal, and exhibited excellent magnetic properties and a high Langmuir adsorption capacity of 149.3 mg Hg(II)/g. The adsorption of Hg(II) onto CoFe2O4@SiO2⁻NH2 followed the pseudo-second-order kinetic equation and Langmuir model. The thermodynamic data showed that the Hg(II) adsorption process was achieved through spontaneous exothermic and monolayer adsorption with electrostatic adsorption and chemisorption. In addition, the as-prepared CoFe2O4@SiO2⁻NH2 nanoparticles had a good reusable value, good application performance and stability, and can provide a mild and facile way to remove heavy metals from aqueous solution.