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[Display omitted] • A novel type of PILs has been fabricated. • PILs integrate the permanent pores of porous solids with the exceptional properties of ILs. • PILs possess high activity and selectivity for the DBT oxidation. • IL moiety serves as an extractant to enrich DBT and creates an electrostatic solvent effect. • UiO-66 moiety serves as a catalysis to handily catalyze the ODS reaction. Developing a highly efficient strategy for the stabilization of the solid-liquid interface is a persistent pursuit for researchers. Herein, porous ionic liquids based on UiO-66 (Zr) porous materials were synthesized and applied to the selective desulfurization catalysis, which integrates the permanent pores of porous solids with the exceptional properties of ionic liquids. Results show that porous ionic liquids possess high activity and selectivity for dibenzothiophene. Experimental analysis and density functional theory calculations revealed that the ionic liquids moiety served as an extractant to enrich dibenzothiophene into the porous ionic liquids phase through the π···π and C H···π interactions. Additionally, the electrostatic solvent effect in the porous ionic liquids contributes to the stabilization solid-liquid interface, which was favorable for UiO-66 moiety to catalytically activate hydrogen peroxide (H 2 O 2) to generate ·OH radicals, and subsequently oxidized dibenzothiophene to the corresponding sulfone. It is hoped that the development of porous ionic liquids could pave a new route to the stabilization of the solid-liquid interface for catalytic oxidation. [ABSTRACT FROM AUTHOR]

Background: Mechanical damage to plants triggers local and systemic electrical signals that are eventually decoded into plant defense responses. These responses are constantly affected by other environmental stimuli in nature, for instance, light fluctuation. In recent years, studies on decoding plant electrical signals powered by various machine learning models are increasing in a sense of early prediction or detection of different environmental stresses that threaten plant growth or crop yields. However, the main bottleneck is the low-throughput nature of plant electrical signals, making it challenging to obtain a substantial amount of training data. Consequently, training these models with small datasets often leads to unsatisfactory performance. Results: In the present work, we set out to decode wound-induced electrical signals (also termed slow wave potentials, SWPs) from plants that are deprived of light to different extents. Using non-invasive electrophysiology, we separately collected sets of local and distal SWPs from the treated plants. Then, we proposed a workflow based on few-shot learning to automatically identify SWPs. This workflow incorporates data preprocessing, feature extraction, data augmentation and classifier training. We established the integral and the first-order derivative as features for efficiently classifying SWPs. We then proposed an Adversarial Autoencoder (AAE) structure to augment the SWP samples. Combining them, the Random Forest classifier allowed remarkable classification accuracies of 0.99 for both local and systemic SWPs. In addition, in comparison to two other reported methods, our proposed AAE structure enabled better classification results using our tested features and classifiers. Conclusions: The results of this study establish new features for efficiently classifying wound-induced electrical signals, which allow for distinguishing dark-affected local and systemic plant wound responses. We also propose a new data augmentation structure to generate virtual plant electrical signals. The methods proposed in this study could be further applied to build models for crop plants using electrical signals as inputs, and also to process other small-scale signals. [ABSTRACT FROM AUTHOR]

Immune composition is commonly heterogeneous and varies among colorectal cancer (CRC) patients. A comprehensive immune classification may act as important characteristics to predict CRC prognosis. Thus, we aimed to identify novel immune specific subtypes to guide future therapies. Unsupervised clustering was used to classify CRC samples into different immune subtypes based on abundances of immune cell populations, during which TCGA and GSE17536 datasets were used as training and validation sets, respectively. The associations between the immune subtypes and patient prognosis were investigated. Further, we identified differentially expressed genes (DEGs) between immune high and low subtypes, followed by functional enrichment analyses of DEGs. The expression levels of 74 immunomodulators (IMs) across immune subtypes were analyzed. As a result, we clustered CRC samples into three distinct immune subtypes (immune high, moderate, and low). Patients with immune-high subtype showed the best prognosis, and patients with immune-low subtype had the worst survival in both TCGA and GSE17536 cohorts. A group of 2735 up-regulated DEGs were identified across immune high and low subtypes. The main DEGs were the members of complement components, chemokines, immunoglobulins, and immunosuppressive genes that are involved in immune modulation-related pathways (e.g., cytokine-cytokine receptor interaction) or GO terms (e.g., adaptive immune response and T cell activation). The expression levels of 63 IMs were significantly varied across immune subtypes. In conclusion, this study provides a conceptual framework and molecular characteristics of CRC immune subtypes, which may accurately predict prognosis and offer novel targets for personalized immunotherapy through modifying subtype-specific tumor immune microenvironment. [ABSTRACT FROM AUTHOR]

Objectives. Sepsis is characterized as a dysregulated host immune response to infection and has been known to be closely associated with the gut microbiome. This study was aimed at investigating the gut microbial profiles of Zhuang ethnic patients with sepsis. Method. Eleven Zhuang ethnic patients with sepsis and 20 healthy individuals (controls) were recruited at the Baise City People's Hospital, China. Their gut microbial community profiles were analyzed by 16S rRNA gene sequencing using the Illumina MiSeq system. Results. The gut microbial community of patients with sepsis was significantly altered compared to that of the healthy individuals based on the results of principal coordinate analysis and microbial ecological networks. Additionally, significantly lower microbial alpha diversity was observed in patients with sepsis than in healthy individuals. In particular, the enrichment of Bilophila, Burkholderia, Corynebacterium, and Porphyromonas, along with the reduced abundance of a large number of short-chain fatty acid-producing microbes, including Roseburia, Bifidobacterium, Faecalibacterium, Coprococcus, Blautia, Clostridium, Ruminococcus, and Anaerostipe was observed in patients with sepsis compared to the control group. Moreover, patients with sepsis could be effectively classified based on the abundance of these bacteria using a support vector machine algorithm. Conclusion. This study demonstrated significant differences in the gut microbiome between Zhuang ethnic patients with sepsis and healthy individuals. In the future, it is necessary to determine whether such alterations are the cause or consequence of sepsis. [ABSTRACT FROM AUTHOR]

The Earth Exploration Satellite Service (EESS) for passive sensing has a primary frequency allocation in the 1400–1427 MHz band. All emissions unauthorized in this band are called RFI (Radio Frequency Interference). The SMOS (Soil Moisture and Ocean Salinity) mission is greatly perturbed by RFI impeding ocean salinity retrieval, especially in coastal areas such as the SCS (South China Sea), where the observed data has been discarded massively. At present, there is no way to eliminate the RFI impact on the retrieved salinity, other than by detecting and shutting down the emissions from the sources. However, it may be effective in a scientific sense if RFI can be quantified and applied to the salinity retrieval process. Therefore, this study proposes an RFI measuring method that can investigate contamination in both prominent and moderate respects, aroused either by on-site emissions or nearby continents. Based on the proposed method, two levels of hierarchical RFI maps of the SCS region, including the separated one and the merged one, are presented and discussed, indicating more severe contamination in northern and western SCS. Moreover, to verify the generalization of the method on open oceans far from continents, an area in the middle central Pacific is selected and tested. The result shows few or no RFI in this unattended region, which is consistent with the authors' knowledge. This study presents the concept of the "RFI map" to describe the contamination, which will hopefully help researchers comprehend the RFI state intuitively and assist in ocean salinity retrieval statistically. [ABSTRACT FROM AUTHOR]

Constructing reasonable pore structures and elements doping are significant for applying porous carbon materials in supercapacitors. Black humic acid is widely distributed in soils, waters and sediments, which inherently contains oxygen functional groups. In this research, black humic acid is used as a carbon source, and H 2 O 2 oxidation is synergistically applied with KOH activation to promote the formation of mesopores and enhance oxygen content to prepare the oxygen-rich and mesopore-rich hierarchical porous carbon material (HPC OA). HPC OA has a high oxygen content of 26.39 atom%, an abundant mesopore ratio of 87.00%, and a high specific surface area of 1727 m2·g-1. In a 6 M KOH electrolyte, the electrode material of HPC OA as a supercapacitor exhibits a specific capacitance of 226 F⋅g-1 at 0.2 A⋅g-1. The symmetric electrodes exhibit an energy density of 11.28 Wh⋅kg−1 with a power density of 60.00 W⋅kg−1 and the capacitor retention are 98.53% after 6000 cycles. The research proposes a new strategy from hierarchical porous carbon materials to regulate the mesoporous formation and oxygen doping, providing carbon electrode materials for supercapacitors with excellent performance. [Display omitted] [ABSTRACT FROM AUTHOR]

Background: Reverse Transcription quantitative polymerase chain reaction (RT-qPCR) is a sensitive and reliable method for mRNA quantification and rapid analysis of gene expression from a large number of starting templates. It is based on the statistical significance of the beginning of exponential phase in real-time PCR kinetics, reflecting quantitative cycle of the initial target quantity and the efficiency of the PCR reaction (the fold increase of product per cycle). Results: We used the large clinical biomarker dataset and 94-replicates-4-dilutions set which was published previously as research tools, then proposed a new qPCR curve analysis method——CqMAN, to determine the position of quantitative cycle as well as the efficiency of the PCR reaction and applied in the calculations. To verify algorithm performance, 20 genes from biomarker and partial data with concentration gradients from 94-replicates-4-dilutions set of MYCN gene were used to compare our method with various publicly available methods and established a suitable evaluation index system. Conclusions: The results show that CqMAN method is comparable to other methods and can be a feasible method which applied to our self-developed qPCR data processing and analysis software, providing a simple tool for qPCR analysis. [ABSTRACT FROM AUTHOR]

• Dynamic loaded tooth contact analysis (DLTCA) for computing entrainment speed. • Accurate solution to elastohydrodynamic lubrication (EHL) governing equation. • Discrete convolution and fast Fourier transformation (DC-FFT) for flank elastic deformation. • A separation flow method for iteration of EHL governing equation. • Accurate entrainment effect-based EHL forecasting model for hypoid gears. In full consideration of time-varying meshing performance and oil film characteristics, entrainment effect on elastohydrodynamic lubrication (EHL) is developed for establishing accurate forecasting model of the complex hypoid gears. Firstly, dynamic loaded tooth contact analysis (DLTCA) is employed to determine the meshing interface kinematics, load distribution and entrainment speed under dynamic load condition. Then, entrainment speed is introduced into the EHL governing equation and accurate forecasting model is established. With accurate discretization of EHL governing equation, discrete convolution and fast Fourier transformation (DC-FFT) method is employed to compute the flank elastic deformation. Finally, a hypoid gear set in automotive industrial application is exercised to verify entrainment effect on EHL assessment in the proposed model. [ABSTRACT FROM AUTHOR]

This study proposes a compact structure of the three‐way Gysel power divider with arbitrary power dividing ratio, which has a significant difference from existing N‐way ones with a common node in the centre of the circuit. First, existing equations are reviewed, and new analytical closed‐form equations are derived according to the proposed structure. The frequency bandwidths, affected by the parameters of isolation networks are investigated in detail and optimised for performance balance. For verification, the proposed three‐way Gysel power dividers are calculated, optimised and fabricated at the centre frequency of 3.5GHz with different dividing ratios of 1:1:1 and 1:2:3, respectively. Moreover, the equations are derived to design the N‐way Gysel power divider. [ABSTRACT FROM AUTHOR]

Metal/oxide heterointerfaces are ubiquitous in functional materials, and their microstructures frequently govern the macroscopic properties. It has been believed that the interfacial interactions are very weak at incoherent interfaces with large mismatches. Combining atomic-resolution scanning transmission electron microscopy with density functional theory calculations, we investigated the interaction and bonding reconstruction at Pd/ZnO{0001} interfaces, which have large mismatches. Molecular beam epitaxy was employed to grow Pd films on clean Zn-terminated ZnO(0001) and O-terminated ZnO(000 1 ¯) polarized surfaces. Atomically sharp Zn-terminated interfaces formed on both substrates, and the large lattice misfits between them were not strongly accommodated, suggesting the formation of incoherent regions. The interfacial atoms were located almost at bulk lattice points in the stoichiometric Zn-terminated Pd(111)/ZnO(0001) structure, whereas the interfacial Pd and Zn atoms underwent relatively large relaxations on the interfacial plane in the nonstoichiometric Zn-terminated Pd(111)/ZnO(000 1 ¯ ) interface. Effective Pd–Zn chemical bonds were formed across both interfaces, but the bonding mechanisms were quite different, depending on the local atomic geometry. The Pd–Zn bonds exhibited site-dependent characteristics and gradually transitioned from covalent to ionic at the Pd(111)/ZnO(0001) interface, whereas most of Pd–Zn bonds exhibited strong covalent behavior at the Pd/ZnO(000 1 ¯ ) interface. The adhesive energies indicated that the Zn-terminated Pd/ZnO(000 1 ¯ ) interface is energetically preferable to the Zn-terminated Pd/ZnO(0001) interface. Thus, the interfacial interaction can be strong and direct metal–metal interactions can play a critical role in metal/oxide heterointerfaces with large mismatches, opening up a new avenue for understanding the origins of interface-related issues. Image 1 [ABSTRACT FROM AUTHOR]

The charge degree of freedom of A-site cation as well as B-site cation plays a significant role in determining the internal charge distribution and gives rise to fascinating physical properties in perovskite oxides. Here, we discuss the magnetic couplings and electronic structures of rare-earth Ce cation incorporated A-site-ordered quadruple perovskite CeMn 3 Mn 4 O 12 via first-principles calculations. This report demonstrates that the A site Ce is magnetic cation with quantity of 4 f electrons, which is quite different from the nonmagnetic Ce4+ usually found in isostructural compounds. As a result, not only the A′ and B site manganese sublattices but also the A site cerium sublattice is involved in the complex magnetic interactions. In the low-temperature phase, CeMn 3 Mn 4 O 12 is ferrimagnetic with the Ce(↓)-Mn1(↑)-Mn2(↓)-Mn3(↑)-Mn4(↑)-Mn5(↓) type, in which the effective magnetic couplings are generated from A-site Ce sublattice as well as the antiparallel arrangement within both the A and B site manganese sublattices. The analysis of electronic structure reveals the valence distribution is Ce3+Mn3+ 3 Mn3+ 4 O2- 12 where both the oxidation state of Ce and Mn is +3. Nevertheless, ferromagnet is the most favorable in energy with a large saturated magnetic moment at the high-temperature phase. Interestingly, the electronic structure undergoes a semiconducting to half-metallic transition accompanying with the phase transformation. The present results offer a new strategy to realizing the tunable charge distribution via variable valence A site cation in A-site-ordered quadruple perovskites and thus open an avenue to modulate these materials with exotic properties. [Display omitted] • CeMn 3 Mn 4 O 12 is ferrimagnetic with the Ce(↓)-Mn1(↑)-Mn2(↓)-Mn3(↑)-Mn4(↑)-Mn5(↓) type in the low-temperature phase. • Ferromagnet is the most favorable in energy with a large saturated magnetic moment at the high-temperature phase. • The A-site Ce sublattice is magnetic with a small quantity of 4f electrons within both phases. • A semiconducting to half-metal transition is realized accompanying with the temperature-induced phase transformation. [ABSTRACT FROM AUTHOR]

Graphical abstract The interlayer-expanded 1 T-MoSe 2 cocatalyst modified 2D-C 3 N 4 exhibits an ultra-high hydrogen evolution rate of 1672.6 μmol g−1 h−1 with AQE of 5.2% at 420 nm. The giant improved HER performance can be ascribed to the enhanced charge separation efficiency and favorable hydrogen evolution capacity of cocatalyst. Highlights • The interlayer-expanded 1T-MoSe 2 is for the first time utilized as cocatalyst in photocatalytic hydrogen evolution. • The MoSe 2 cocatalyst can effectively boost the HER performance of 2D-C 3 N 4 with AQE = 5.2% at 420 nm. • The interlayer-expanded 1T-phase structure leads to favorable hydrogen evolution capacity of MoSe 2 benifiting for HER. Abstract Visible-light-driven photocatalytic hydrogen evolution reaction (HER) is of far-reaching significance to address the energy and environmental issues. Owing to the seriously limited charge separation and surface catalytic conversion efficiency, cocatalyts especially noble-metals (e.g. Pt) are fundamentally required for this reaction. Transitional metal dichalcogenides (TMDs) represent a type of promising nonprecious cocatalysts, but they still lack effective strategies to optimize the performance. In this work, we report a rational design of MoSe 2 to form interlayer-expanded 1T-phase structure, to maximize the cocatalytic activity for photocatalytic HER by optimizing the surface activation ability for reaction molecule at both edge and basal sites. In a practical photocatalytic reaction, when intergrated with a semiconductor (two-dimensional carbon nitride, 2D-C 3 N 4), the hybrid exhibits a satisfactory hydrogen evolution rate (1672.6 μmol g−1 h−1, with external quantum efficiency of 5.2% at 420 nm) that greatly higher than the normal spacing 2H-MoSe 2 (186.7 μmol g−1 h−1) and most noble-metals (e.g. Au, Ag, Pd). The giant improved HER performance strongly demonstrates the superiority of the presented phase and interlayer engineering strategy. The formation mechanism of the specialized structure and the key factor affecting the performance are also discussed. This work may provide new avenues for the design of TMDs-based catalysts toward HER application. [ABSTRACT FROM AUTHOR]

Hydrogen peroxide (H 2 O 2 ) decomposition mechanism and its oxidative desulfurization activity on hexagonal boron nitride monolayer (h-BN) have been explored by density functional theory (DFT) at M06–2X/6-311 + G (d,p) level. A cluster model which contains seven rings has been constructed to simulate the h-BN surface. It is found that 7 possible species will be generated after the decomposition of H 2 O 2 . Among them, 2H*+O 2 * and 2H*+2O* are relatively unstable while other species, such as HOO*+H*, HO*+HO*, H*+HO + O*, H 2 O*+O* are relatively stable and may exist in the current system. In addition, 4 decomposition pathways have been explored. Results show that the H 2 O 2 * will first undergo an O-H bond break (HOO*+H*), then the HO-O bond decomposes into H*+HO*+O* (Pathway (b)). By considering the concentration and activation energy together, the H 2 O*+O* is proposed to be the most possible active species for oxidative desulfurization due to the relative higher concentration and lower activation energy. [ABSTRACT FROM AUTHOR]

CXCL8 is a typical CXC-type chemokine, which mediates the migration of immune cells from blood vessels to the site of inflammation or injury to clear pathogenic microorganisms and repair damaged tissues. In this study, Megalobrama amblycephala CXCL8 (MaCXCL8) gene was identified and characterized. Sequence analysis showed that the deduced MaCXCL8 protein possessed the typical structure of CXCL8 from other species, with the characteristic CXC cysteine residues in the N-terminal and accompanied by a DLR motif (Asp-Leu-Arg motif). Phylogenetic analysis revealed that MaCXCL8 was homologous to that of Ctenopharyngodon idella and other cyprinid fishes. MaCXCL8 gene was expressed in all detected healthy tissues, with the highest expression levels in the spleen, and its expression was significantly up-regulated upon the challenge of Aeromonas hydrophila and Lipopolysaccharide (LPS) both in juvenile M. amblycephala tissues and primary macrophages. The immunohistochemical assay showed that MaCXCL8 was mainly distributed in the nucleus and cytoplasm, and its expression levels increased observably with the prolongation of bacterial infection. In addition, recombinant MaCXCL8 protein exhibited significant chemotactic effects on neutrophils and macrophages. In conclusion, MaCXCL8 is involved in the immune response of M. amblycephala , and these findings will be helpful to understand the biological roles of MaCXCL8 and provide a theoretical basis for the prevention and control of fish bacterial diseases. • MaCXCL8 shared structural similarities with that of other teleosts, except DLR motif was in place of ELR-like motif. • The expression of MaCXCL8 was the most abundant in the spleen, which was dramatically increased upon bacterial infection. • LPS and Aeromonas hydrophila treatment significantly induced the up-regulation of MaCXCL8 expression in macrophages. • Recombinant MaCXCL8 protein exhibited chemotactic effects on neutrophils and macrophages. [ABSTRACT FROM AUTHOR]

To obtain the adsorption strength is the key point for materials design and parameters optimization in chemical engineering. Here we report a simple but accuracy method to estimate the adsorptive energies by counting the number of π-orbital involved atoms based on theoretical computations for hexagonal boron nitride (h-BN) and graphene. Computational results by density function theory (DFT) as well as spin-component scaled second-order Møller-Plesset perturbation theory (SCS-MP2) both confirm that the adsorptive energies correlate well with the number of π-orbital involved atoms for π-orbital contained molecules. The selected molecules (adsorbates) are commonly used in chemical industry, which contains C, N, S, O atoms. The predicted results for the proposed formulas agree well with the current and previous DFT calculated values both on h-BN and graphene surfaces. Further, it can be also used to predict the adsorptive energies for small π-orbital contained molecules on BN and carbon nanotubes. The interaction type for these adsorptions is typical π-π interaction. Further investigations show that the physical origin of these interactions source from the polar interactions between the adsorbents and adsorbates. Hence, for separation or removal of aromatic molecules, how to modify the aromaticity and polarity of both adsorbents and adsorbates will be the key points for experiments. [ABSTRACT FROM AUTHOR]

• Numerical loaded tooth contact analysis for meshing interface. • Meshing interface state evolution under TEHL condition. • Non-Newtonian fluid ETHL model considering entrainment angle. • Separation flow method for the friction coefficient determination. • Energy loss and mechanical efficiency forecasting model. Energy loss and mechanical efficiency directly affect the service performance and reliability of aero-engine bevel gear power transmission, but there is currently a lack of effective diagnosis in early design stage due to the complex tooth meshing interface state evolution under the thermal elastohydrodynamic lubrication (TEHL) condition. A new energy loss and mechanical efficiency prediction model is proposed by using the improved TEHL analysis considering the entrainment angle and non-Newtonian fluid effect. Firstly, numerical loaded tooth contact analysis (NLTCA) is developed to determine tooth meshing kinematic relating to the entrainment and sliding states. Then, the entrainment angle is taken into account the Non-Newtonian fluid TEHL model and separation flow method is applied for friction coefficient solution. Finally, new energy loss and mechanical efficiency model is established by simulating the complex tooth meshing interface TEHL. This model is enabling ever-higher levels of aero-engine bevel gear production efficiency and design sustainability. It can provide an important access to geometric and physical assessments that can improve the energy generation, conversion, transfer and utilization of the whole aero-engine power transmission system. [Display omitted]. [ABSTRACT FROM AUTHOR]

Deep eutectic solvents (DESs), as ionic liquid analogues for green solvents, have gained increasing attentions in chemistry. In this work, three typical kinds of DESs (ChCl/Gly, ChCl/AcOH and ChCl/Urea) were successfully synthesized and characterized by Fourier transform infrared spectroscopy (FTIR) and Raman. Then comprehensive and systematical analyses were performed by the methods of density functional theory (DFT). Two methods (B3LYP/6-311 + +G(2d,p) and dispersion-corrected B3LYP-D3/6-311 + +G(2d,p)) were employed to investigate the structures, vibrational frequencies and assign their ownership of vibrational modes for the DESs, respectively. Nearly all the experimental characteristic peaks of IR and Raman were identified according to the calculated results. By linear fitting of the combined calculated vs experimental vibration frequencies, it can be found that both of the two methods are excellent to reproduce the experimental results. Besides, hydrogen bonds were proved to exist in DESs by IR spectrum, structure analysis and RDG analysis. This work was aimed at predicting and understanding the vibrational spectra of the three typical DESs based on DFT methods. Moreover, by comparing experimental and theoretical results, it provides us a deep understanding of the formation mechanisms of DESs. [ABSTRACT FROM AUTHOR]

We perform a first-principles study of electronic structure and magnetic properties of V, Nb and Ta-doped WS 2 monolayers. Formation energy calculations reveal that all the doped systems are thermodynamically more preferred under S-rich condition than W-rich condition, and that under either condition the incorporation of 5d Ta dopant into monolayer is the most favorable, followed by the incorporation of 4d Nb and 3d V. Electronic structure analysis reveals that all the doped systems show p-type doping and metallic character, i.e. metallicity in the V-doped case, while half-metallicity in the Nb and Ta-doped cases. Furthermore, ferromagnetism is induced by the impurities, which mainly comes from the coupling between unpaired d orbitals of the dopants and the nearest neighbors of W 5d and S 3p states. These findings indicate that doping metals in WS 2 monolayers may act as a useful way to tailor the electronic structure of two-dimensional materials for many device applications. [ABSTRACT FROM AUTHOR]

Chemical doping represents one of the most effective ways in engineering electronic structures of anatase TiO2 for practical applications. Here, we investigate formation energies, geometrical structures, and electronic properties of Si-, F-doped and Si/F co-doped anatase TiO2 by using spin-polarized density functional theory calculation. We find that the co-doped TiO2 is thermodynamically more favorable than the Si- and F-doped TiO2- Structural analysis shows that atomic impurity varies crystal constants slightly. Moreover, all the three doped systems show a pronounced narrowing of band gap by 0.33 eV for the F-doped TiO2, 0.17 eV for the Si-doped TiO2, and 0.28 eV for the Si/F-co-doped TiO2, which could account for the experimentally observed redshift of optical absorption edge. Our calculations suggest that the Si/F-co-doping represents an effective way in tailoring electronic structure and optical properties of anatase TiO2. [ABSTRACT FROM AUTHOR]

In this work, interaction nature between a group of aromatic sulfur compounds and [BMIM] + [FeCl 4 ] − have been investigated by density functional theory (DFT). A coordination structure is found to be critical to the mechanism of extractive desulfurization. Interaction energy and extractive selectivity follow the order: thiophene (TH) < dibenzothiophene (DBT) ≈ benzothiophene (BT). Alkylation of TH or BT ( e.g. 3-methylthiophene, and 3-methylbenzothiophene) leads to a stronger interaction with ionic liquid, but steric hindrance effects of some alkylic derivatives ( e.g. 2,7-dimethylbenzothiophene) lead to a weaker interaction with ionic liquid. The mechanism of extractive desulfurization is attributed to the charge transfer effect. During extractive desulfurization, electrons on aromatic sulfur compounds transfer into the Lewis part of ionic liquid, namely, [FeCl 4 ] − . Furthermore, it is better to consider the Lewis acidity of Fe-containing ionic liquid by the whole unit (such as [FeCl 4 ] − and aromatic sulfur compounds (X)) rather than only Fe or S atom. [ABSTRACT FROM AUTHOR]

In the processing of 4H-SiC MOSFET devices, it is crucial to optimize the condition of wet oxidation based on the wafer surface orientation to obtain excellent electronic properties. However, the mechanism of surface oxidation and the effect of surface polarity remain unclear. The atomic structures of SiO 2 /4H-SiC (0001) [Si-face] and (000 1 ¯) [C-face] interfaces can be analyzed by aberration-corrected STEM and first-principles MD calculations. On the Si-face, interfacial O atoms on the amorphous SiO 2 layer show clear atomic ordering with a rigid O-Si bridge structure across the SiO 2 /4H-SiC interface, involving a slow oxidation rate. The C-face can be rapidly oxidized, resulting in dangling bonds, bond bending, rough interface, and residual carbon in the SiO 2. A key feature is the formation of a stable and flat oxidation front by O atom ordering and then the suppression of interface defects or residual C, which provides an approach for designing high-performance 4H-SiC MOSFET devices. In 4H-SiC MOSFET devices, initial stage of wet oxidation in SiO 2 /4H-SiC interface plays key role to obtain excellent device properties. STEM imaging and MD calculation reveal O-atom-ordering in the amorphous SiO 2 layer. This O-atom-ordering provides strong O-Si bridge structure with crystalline 4H-SiC and then the formation of atomically flat wide oxidation front without any defects, such as dangling bonds. [Display omitted] [ABSTRACT FROM AUTHOR]

[Display omitted] High entropy oxides are promising catalysts for numerous catalytic oxidation processes with oxygen as the oxidant. However, most of them often show bulk morphologies, which hinders the full exposure of active sites. In this work, a unique 26-faceted polyhedral high entropy oxide MnNiCuZnCoO x -1000 (P-HEO) with highly active site exposure is fabricated via a mechanochemistry-assisted strategy. By employing such a strategy, the supersaturation of P-HEO during the crystal growth process is effectively reduced to form high-index facets, which is proved to be beneficial to the formation of high-index facets. Characterization results indicate that more oxygen vacancies are generated in P-HEO compared with the bulk counterparts. Density functional theory calculations reveal that the high-index facets { −2 1 1} can facilitate adsorption and activation of O 2 because of the higher adsorption energy −2.23 eV compared with that of (1 1 1) surfaces (-1.79 eV), which induces significantly enhanced activity for organic sulfides oxidation. Interestingly, the synthesized P-HEO with high-index facets shows a 98.4% removal rate of dibenzothiophene from model oil within 8 h at 120 °C, which is much higher than that of the bulk counterparts (33.5%). [ABSTRACT FROM AUTHOR]

Abstract: We have investigated the electronic and magnetic properties of A-site-ordered perovskite CaFe3Ti4O12 using first-principles calculations. Our calculated results indicate that CaFe3Ti4O12 is mechanically stable and it is an antiferromagnetic insulator. Similar to its isostructural perovskite CaCu3Ti4O12, the primary magnetic coupling mechanism in CaFe3Ti4O12 is ascribed to the Fe–O–Ti–O–Fe superexchange interaction. From this fact we can clearly see that the empty 3d orbitals play an important role to realize the superexchange interaction. Moreover, comparing CaFe3Ti4O12 and CaCu3Ti4O12 in some details, we find that Fe (Cu)–O bond distance is one of the important parameters to determine the antiferromagnetic strength within this superexchange interaction. [Copyright &y& Elsevier]

Abstract: Three guanidinium-based ionic liquids (GBILs) including [1,1,3,3-tetramethylguanidinium][phenol] ([TMG][PHE]), [1,1,3,3-tetramethylguanidinium][2,2,2-trifluoroethanol] ([TMG][TE]) and [1,1,3,3-tetramethylguanidinium][imidazole] ([TMG][IM]) were synthesized and their absorption and desorption of sulfur dioxide were investigated, respectively. The saturated molar ratio of SO2 to GBILs varied from 2.24 to 3.16 at 40°C with high absorption rate. The absorption mechanism might be that SO2 reacts with the –NH2 group on the cation and then a new –SO2H group is formed. The new GBILs could absorb SO2 by both physical and chemical interactions while physical absorption does play an important role at the experimental conditions under investigation. [Copyright &y& Elsevier]

Polyacrylic acid (PAA) has high water absorbency but poor salt resistance. Humic acid (HA) extracted from lignite was introduced into the cross-linked copolymer systems of AA to improve the water absorbency and salt-tolerance. A polyacrylic acid-potassium humate (PAA-KHA) coated ammonium dihydrogen phosphate (ADP) fertilizer with water-preserving, salt-resistant and slow-release properties was prepared. The main properties of HA extracted from lignite oxidized by H2O2 were studied. Furthermore, the synthesis process, water absorbency of PAA-KHA in deionized water and in NaCl solution, morphologies of PAA-KHA, and the slow-release performance of the fertilizer (ADP@PAA-KHA) were investigated. The results showed PAA-KHA had a layered interpenetrating network, which can provide sufficient storage space for water and nutrients. The salty water absorbency of PAA-KHA increased by about 3 times compared to PAA. Both the PO43− and NH4+ cumulative release of ADP@PAA-KHA with a coating rate of 10% in deionized water, were less than 20% within 24 h, and were 55.71% and 28.04% after the 15th day, respectively. The weight change of ADP@PAA-KHA before and after absorbing water was about 53 times in deionized water and about 4 times in 1 wt% of NaCl salty water. The results show that ADP@PAA-KHA has excellent properties of water retention, salt resistance and slow-release. This will efficiently improve the utilization of fertilizer and reduce the irrigation water consumption at the same time. [ABSTRACT FROM AUTHOR]

• Carburizing-meshing coupling effect in loaded contact pattern area of aerospace spiral bevel gears. • Data-driven prediction of tooth flank heat treatment deformation considering coupling effect. • Adaptive tooth flank heat treatment deformation optimization model. • Sensitivity analysis strategy-based adaptive data-drive optimization of tooth flank heat treatment deformation. In the current tooth flank manufacturing of aerospace spiral bevel gears, accurate prediction and optimization of heat treatment deformation is of paramount significance to high accuracy improvement. In particular, the loaded elastic contact mechanical variation can directly affect tooth flank heat treatment geometric topography in micro-scale. An innovative adaptive data-driven prediction and optimization of tooth flank heat treatment deformation for spiral bevel gears by considering carburizing-meshing coupling effect is proposed in this work. At first, numerical loaded tooth contact analysis (NLTCA) based on data-driven tooth flank finite element modeling is integrated into tooth flank carburizing to get an accurate data-driven determination of carburizing-meshing coupling effect. Then, machine settings are used as the basic data to perform the data-driven tooth flank deformation prediction. The recent machine tool settings modification is extended to the case that the loaded contact deformation is predicted as the important tooth flank geometric accuracy. Finally, an adaptive data-driven optimization of tooth flank heat treatment deformation considering carburizing-meshing coupling effect is proposed for a high-accuracy tooth flank manufacturing. The given numerical instance can verify the proposed method. [ABSTRACT FROM AUTHOR]

The tautomeric equilibrium constant KC of ethyl acetoacetate (EAA) in CO2–n-pentane and CO2–ethanol was studied by UV–VIS spectroscopy at 308.2 K over the pressure range from 6.5 to 9.0 MPa. This work focuses on how the tautomeric equilibrium changes with pressure and composition of the mixed solvents in the near critical region. The results showed that the effect of pressure on KC was very limited at pressures much higher than the phase separation pressures. However, the KC increased sharply as the pressure approached the critical point or the bubble point of the mixed solvents. [Copyright &y& Elsevier]

• A novel 3D crosslinked solid polymer electrolyte containing phosphorus was successfully prepared. • IFR-SPE exhibited outstanding flame-retardant ability. • The Li/IFR-SPE/Li cell formed a LiF/Li 3 PO 4 -rich solid electrolyte interphase on the Li electrode. • The Li/IFR-SPE/LiFePO 4 cell showed acceptable rate and cycle performances. The solid polymer electrolyte (SPE) has been regarded as a promising candidate for the next-generation rechargeable Li metal battery with high-energy density. However, the current SPEs are still challenged by insufficient security owing to their flammability. Here, we reported a novel inherently flame-retardant SPE (IFR-SPE), which was fabricated via the one-step in situ crosslinking of two novel synthetic P-containing monomers with porous polyimide film as a supporting host. Compared with liquid and conventional solid polyethylene oxide electrolytes, the unique IFR-SPE exhibits outstanding flame-retardant ability. Furthermore, it demonstrates a high Li-ion conductivity (0.28 mS cm−1 at 25 °C), a stable electrochemical window up to 4.12 V, and effective Li dendrite suppression via a LiF/Li 3 PO 4 -rich solid electrolyte interphase formed on the Li anode. Consequently, the Li/IFR-SPE/LiFePO 4 cell shows acceptable electrochemical performances. We believe that this work offers a novel and effective strategy for establishing a promising Li metal battery system with high safety. [ABSTRACT FROM AUTHOR]

The deformation behavior and microstructural evolution of fine-grained 2050 alloys at elevated temperatures and slow strain rates were investigated. The results showed that significant dynamic anisotropic grain growth occurred at the primary stage of deformation. Insignificant dislocation activity, particle-free zones, and the complete progress of grain neighbor switching based on diffusion creep were observed during superplastic deformation. Quantitative calculation showed that diffusion creep was the dominant mechanism in the superplastic deformation process, and that grain boundary sliding was involved as a coordination mechanism. Surface studies indicated that the diffusional transport of materials was accomplished mostly through the grain boundary, and that the effect of the bulk diffusion was not significant. [ABSTRACT FROM AUTHOR]

Inspired by searching new forms of Boron Nitride (BN) compounds, the electronic structure and physicochemical property of a graphyne-like BN compound was explored by density functional theory with cluster models as well as periodic models. This graphyne-like BN compound is named Boron Nitridene in this work, based on geometry and bond order analysis as its B–N linking units take on double bond characteristics. Different cluster models of Boron Nitridene- x (x = 1–5) were constructed. Results show that the geometric parameters and molecular orbitals are similar for these models. The chemical stability of Boron Nitridene was estimated by the concept of heats of formation, vibrational frequency, and ab initio molecular dynamics. In addition, the IR and Raman spectra were predicted and the unique stretching modes were assigned to give a reference with experimental synthesis. Last, the adsorption strength of small molecules was calculated, and the results show the boron nitridene interacts stronger than hexagonal boron nitride (h-BN). Image 1 • Boron Nitridene as a new form of BN has been systematic studied. • Chemical stability of Boron Nitridene was estimated by the concept of heats of formation. • IR and Raman spectra were predicted and the unique stretching modes were assigned. • Adsorption strength of small molecules on boron nitridene was calculated. [ABSTRACT FROM AUTHOR]

With the increasingly strict limitations on emission standards of vehicles, deep desulfurization in fuel is indispensable for social development worldwide. In this study, a series of hybrid materials based on SiO2-supported polyoxometalate ionic liquid were successfully prepared via a facile ball milling method and employed as catalysts in the aerobic oxidative desulfurization process. The composition and structure of prepared samples were studied by various techniques, including FT-IR, UV-vis DRS, wide-angle XRD, BET, XPS, and SEM images. The experimental results indicated that the synthesized polyoxometalate ionic liquids were successfully loaded on SiO2 with a highly uniform dispersion. The prepared catalyst (C16PMoV/10SiO2) exhibited good desulfurization activity on different sulfur compounds. Moreover, the oxidation product and active species in the ODS process were respectively investigated via GC-MS and ESR analysis, indicating that the catalyst can activate oxygen to superoxide radicals during the reaction to convert DBT to its corresponding sulfone in the fuel. [ABSTRACT FROM AUTHOR]

Background: Early life microflora is an important determinant of immune and metabolic development and may have lasting consequences. However, the mode of delivery and the effect of povidone iodine disinfection on neonatal oral microflora colonization are still unclear. The objective of the study was to understand the effects of the use of polyvidone iodine on infant's oral microflora after transvaginal examination during delivery, provided data support for the establishment of neonatal oral microflora health.Methods: A total of 20 cases of full-term neonatal delivered in October 2017 in Shenzhen Bao'an Maternity and Child Health Hospital through vaginal delivery. These neonates were randomly divided into two groups, the conventional disinfection group and the non-disinfection group. Simultaneously, 10 infants with elective cesarean section were taken as comparison. With Illumina MiSeq platform, 16S rRNA V3-V4 sequencing method was used to analyze bacterial DNA of oral secretions.Results: At the phylum level, compared to the non-disinfection group, higher relative abundance of Bacteroidetes and Proteobacteria, and lower proportion of Firmicutes were observed in the cesarean section group and the disinfection group. As main composition of phylum Firmicutes, genus Lactobacillus presented extremely low in the cesarean section group and the disinfection group, whereas it was the absolute dominant bacteria in the non-disinfection group. Compared with the caesarean section group, only Lactobacillus increased in majority of the non-disinfection group. There was no increase in Lactobacillus in the disinfection group, but Prevotella, Escherichia-Shigella, Staphyloccus, and Klebsiella increased significantly. Through KEGG pathway analysis, we found that there were more harmful pathways such as staphylococcus aureus infection, viral myocarditis and sporulation in the disinfection group.Conclusions: The mode of delivery affects the infant's Lactobacillus obtained from the mother. Moreover, vulvar disinfection played an important part in the colonization of neonatal oral microbiota. And the impact of the first oral colonizers on infant health needs further follow-up investigations. [ABSTRACT FROM AUTHOR]

[Display omitted] • An OCNR method has been first proposed for the controllable synthesis of functionalized PPILs. • The protic ion pairs play a crucial role in the formation of PPILs with low viscosity. • The PPILs possess excellent extractive capacity due to the rapid mass transfer offering enough electrons for DBT. • The primary driving forces for the extraction of DBT are the interactions of C H·π in protic ion pairs sites and C H···O in HS sites. Porous ionic liquids (PILs) offer a distinctive combination of liquid-like fluidity and solid porosity, making them well-suited for various applications including separation, catalysis, and energy storage. Nevertheless, the design limitations and complex synthesis processes have hindered the development of PILs. Here, the one-step coupling neutralization reaction (OCNR) method has been first proposed for the controllable synthesis of functionalized protic porous ionic liquids (PPILs). Specifically, three types of PPILs have been synthesized based on tuning the position of the corona amino functional groups. The results indicate the crucial role of protic ion pairs in the formation of pure liquid PPILs with low viscosity. The extraction efficiency has obviously increased after introducing the porous materials from 38.5% to 51.9%. The results showed PPILs play good extraction-adsorption coupled desulfurization (EADS) performance. The density functional theory (DFT) results show that both the protic ion pairs and the porous structure have significant roles in EADS, with the former offering C H···π interactions, while the latter provides hydrogen bonding (C H···O) interactions. Ultimately, the strategy simplifies the synthesis process, providing a new idea for the directional design of low-viscosity PILs with specific functions. [ABSTRACT FROM AUTHOR]

Acidic deep eutectic solvents (DESs) have been considered desirable extractants and catalysts for desulfurization. However, their hydrogen bond donors (HBDs) are usually sole organic acids, which are not conducive to efficient green catalysis. Herein, a novel inorganic–organic dual-acid DES (DADES) was reported for efficient extractive and oxidative desulfurization. Benefiting from the physical interaction among the three components in a DADES, a transparent homogeneous liquid can be obtained even though inorganic acid (boric acid, BA) and organic acid (acetic acid, AA) can be immiscible. Furthermore, the dual-acid HBD can increase the acidity of the DADES and reduce its viscosity, accelerating its mass transfer efficiency and enhancing its catalytic activity. With 1-butyl-3-methylimidazolium chloride ([Bmim]Cl) as the hydrogen bond acceptor, [Bmim]Cl/BA/0.3AA effectively activated hydrogen peroxide and achieved sulfur removal of 96.6% at 40 °C. Furthermore, the universality of the synergistic effect in various DADESs was confirmed by the modulation of the types of organic acids. This study not only motivates the construction of more intriguing novel DESs based on the DADES concept but also highlights their potential in clean fuel production. [ABSTRACT FROM AUTHOR]

One of the crucial issues in rechargeable zinc-air batteries is to explore low-cost, highly efficient bifunctional electrocatalysts for the oxygen reduction/evolution reaction. Here, the unique NiCo alloy nanoparticles encapsulated in the multi-dimensional nitrogen-doped carbon architecture (NiCo/MNC) is reported as an effective bifunctional catalyst for rechargeable zinc-air batteries. The multi-dimensional nitrogen-doped carbon architecture was synthesized through the rapid calcination of two-dimensional graphitic carbon nitride (g-C 3 N 4) and one-dimensional multi-walled carbon nanotubes (MWCNTs). The g-C 3 N 4 serves as the nitrogen source and the precursor for N-doped carbon nanosheets (NCSs). Simultaneously, NCSs can intertwine with MWCNTs to further obtain the multi-dimensional architecture with a large specific surface area. The synergistic effect between multi-dimensional nitrogen-doped carbon architectures and NiCo alloy nanoparticles endowed the NiCo/MNC with a positive half-wave potential of 0.83 V (vs. RHE: Reversible Hydrogen Electrode) for oxygen reduction reaction and a low potential of 1.61 V (vs. RHE) at the current density of 10 mA cm−2 for oxygen evolution reaction. Moreover, the zinc-air battery assembled with NiCo/MNC as the air-cathode exhibited a high-power density of 135.2 mW cm−2, a specific capacity of 701.7 mAh g−1, and an excellent stability in charging/discharging cycle test (over 115 h). The prepared catalyst could potentially serve to take the place of precious metal catalysts in rechargeable zinc-air batteries. Image 1 • NiCo alloy nanoparticles encapsulated in the multi-dimensional N-doped carbon (MNC) architecture was designed. • The synergistic effect between MNC and NiCo alloy nanoparticles can facilitate ORR/OER activities. • NiCo/MNC serves as an efficient ORR/OER catalyst for rechargeable zinc−air batteries. [ABSTRACT FROM AUTHOR]

CNO-V 0.005 anode material prepared by simple molten salt method not only has faster lithium-ion diffusion kinetics and lower transfer internal resistance, but also has 276.9 mAh g−1 of high discharge capacity at current density of 2000 mA g−1 over 1000 cycles. [Display omitted] • CoNb 2 O 6 was prepared and was in-situ doped with V5+ ion by a molten-salt method. • The interstitial-doped CNO-V 0.005 exhibits long cycling stability at 2000 mA g−1 (≈ 8C). • The CNO-V 0.005 ||LiFePO 4 full cell has discharge capacity of 150.6 mAh g−1 after 200 cycles. Niobium-based bimetallic oxide, as a potential anode material for fast-charging lithium-ion batteries, has attracted much attention owing to its unique lithium intercalation channel. However, the poor conductivity and structural instability of such material severely limit its further application. In this paper, CoNb 2 O 6 was prepared by a molten-salt method and was in-situ doped with high-valence V5+ ion in different proportions. Different from conventional substitutional doping, a small amount of interstitial doping is more conducive to the entry of V5+ into the gap, which leads to lattice expansion. With the increase of doping amount, elemental Nb5+ was gradually replaced by V5+, which then hinders the Li+ intercalation/de-intercalation to a certain extent. Based on the DFT and electrochemical tests, the interstitial-doped CNO-V 0.005 nanoparticles has not only faster Li+ diffusion kinetics and lower energy barrier, but also delivers high discharge capacity with long cycling stability at high current density of 2000 mA g−1 (≈ 8C). After assembling the full cell with CNO-V 0.005 and commercial LiFePO 4 cathode material, the reversible capacity of 150.6 mAh g−1 could be achieved after 200 cycles at the current density of 1000 mA g−1, demonstrating its application potential in fast- charging lithium-ion batteries. [ABSTRACT FROM AUTHOR]

35159662 5 Shtansky D.V., Matveev A.T., Permyakova E.S., Leybo D.V., Konopatsky A.S., Sorokin P.B. Recent Progress in Fabrication and Application of BN Nanostructures and BN-Based Nanohybrids. Boron nitride (BN) materials, graphene-like materials, are known as one of the most promising inorganic materials of this century because of their unique structures and properties. Kim et al. used V-Cu/BN-Ti to remove residual NO SB X sb and NH SB 3 sb [[2]]. h-BN was dispersed in the catalyst to improve the content of vanadium and copper species on the surface. [Extracted from the article]

Graphical abstract Herein, we designed a strategy to successfully synthesize a novel bi-functional rambutan-like oxygen electrocatalysts comprising in situ -formed N-doped metal (metal: Fe, Co or Ni) encapsulated carbon nanotubes grown on hollow-mesoporous carbon sphere (denoted as Me@N-CNT/HMCS). Metal acetate can catalyze melamine to generate uniformly distributed N-CNTs nanotubes at the surface of hollow-mesoporous carbon sphere. The Me@N-CNT/HMCS oxygen electrocatalysts with very low metal content show unexpectedly high catalytic activities toward both ORR, which is superior to commercial Pt/C. Especially, the optimized performance of Fe@N-CNT/HMCS is achieved with more positive onset potential (E 0 = 1.012 V) and half-wave (E 1/2 = 0.833 V). Additionally, this result indicated that excellent performance is attributed to the synergistic effect involve chemical composition, good conductivity, high porosity and unique rambutan-like structure. Highlights • We firstly reported a simple strategy to successfully synthesize high-performance bi-functional electrocatalysts of the 1D-3D rambutan-like carbon materials. • The excellent electrocatalytic activity was assigned to the synergistic effect between N doping, metal loading and rambutan-like electrocatalyst morphology. • The theoretical calculation study suggests that metallic Fe cluster can promote the O 2 adsorption strength in such chemical environment. Abstract Electrocatalysis of oxygen reaction is a critical step in operation of fuel cells and metal-air batteries. For the practical applications, the inexpensive non-noble metals catalysts with highly activity and stable need to be explored and utilized. Herein, a strategy for the preparation of a bi-functional rambutan shaped oxygen electrocatalyst is presented. The novel electrocatalyst is formed in situ with N doped carbon nanotubes grown on metal encapsulated hollow-mesoporous carbon sphere (Me@N-CNT/HMCS). The Me@N-CNT/HMCS oxygen electrocatalysts show high catalytic activities towards ORR, comparable to commercial Pt/C catalyst. The optimized performance of Fe@N-CNT/HMCS was achieved with a positive onset potential of 1.012 V and half-wave potential of 0.833 V. It is emphasized that Me@N-CNT/HMCS shows high stability and enhanced tolerance against methanol in alkaline medium. The Fe@N-CNT/HMCS electrocatalyst possessed a high OER activity with a low overpotential of 0.35 V at 10 mA cm−2 current density. The excellent performance could be attributed to the synergistic effect involving chemical composition, high conductivity, good porosity and unique rambutan-like structure. In addition, the theoretical calculation study suggests that metallic Fe cluster can promote the O 2 adsorption strength in such chemical environment. [ABSTRACT FROM AUTHOR]

The catalyst of WO3 highly dispersed on mesoporous ZrO2 was prepared by hydrothermal treatment and calcination. Ionic liquid templates with different cations and various calcination temperatures were taken into account to investigate factors that affect the structure of the catalysts. Wide-angle XRD, Raman, low-angle XRD, N2 adsorption-desorption, SEM, EDS-mapping and TEM analyses were employed to characterize the composition, morphology and the dispersion of WO3. It was found that [C16H33N(CH3)3]4SiW12O40 and 700 °C were the optimal ionic liquid template and calcination temperature; the obtained catalyst, expressed as 700-C16-WO3/ZrO2, exhibited the best catalytic activity in oxidation desulfurization. Dibenzothiophene (DBT) in the model oil could be oxidized to DBT sulfone (DBTO2) completely, certified by GC-MS analysis, under optimum conditions. The oxidative desulfurization efficiencies of different substrates catalyze by 700-C16-WO3/ZrO2, and the cycle performance on the oxidation of DBT were studied. [ABSTRACT FROM AUTHOR]

Mannan oligosaccharides (MOS) are functional oligosaccharides with beneficial effects on the non-specific immunity of Megalobrama amblycephala, but systematic studies on the immunomodulatory mechanisms of MOS are still lacking. To investigate the protective mechanisms of three different levels of dietary MOS supplementation on the intestinal immunity of juvenile M. amblycephala, comparative digital gene expression (DGE) profiling was performed. In this study, 622 differentially expressed genes (DEGs) were identified, while the similar expression tendency of 34 genes by qRT-PCR validated the accuracy of the DGE analyses. Gene Ontology (GO) enrichment revealed that the DEGs were mainly enriched in two functional categories of biological process and molecular function. Kyoto Encyclopedia of Genes and Genomes (KEGG) analysis revealed that the DEGs were mainly related to complement and coagulation cascades, coagulation cascades, platelet activation, natural killer cell mediated cytotoxicity, Fc gamma R-mediated phagocytosis and antigen processing and presentation. In addition, the pro-inflammatory, apoptosis and tight junction-related genes were more significantly up-regulated upon infection in the dietary MOS groups to enhance host immune functions and maintain the stability of the intestinal barrier. These results will be helpful to clarify the regulatory mechanism of MOS on the intestinal immunity of M. amblycephala and lay the theoretical foundation for the prevention and protection of fish bacterial diseases. [ABSTRACT FROM AUTHOR]

Herein, functional molybdenum-containing ordered mesoporous silica (Mo-OMS) were successfully fabricated from imidazole and polyoxometalate-based ionic liquids, and employed for the removal of organosulfur compounds. The composition and structure of as-prepared materials were characterized in detail by FT-IR, Raman, DRS, low and wide-angle XRD, nitrogen adsorption–desorption and TEM. The hybrid materials exhibited a high dispersion of molybdenum species and good activity on removing organosulfur compounds without any organic solvents as extractants. Various effects such as the amount of samples, O/S molar ratio, temperature, types of sulfur-containing substrate on the sulfur removal were also investigated. Under optimal conditions, dibenzothiophene (DBT) could be completely removed in 50 min. Moreover, the sulfur removal of reaction system could still reach 91% after recycling for nine times. [ABSTRACT FROM AUTHOR]

CD68 is a highly glycosylated transmembrane glycoprotein that belongs to the lysosome-associated membrane glycoprotein family and is involved in various immune processes. In this study, Megalobrama amblycephala CD68 (MaCD68) was cloned and characterized, and its expression patterns and evolutionary characteristics were analyzed. The coding region of MaCD68 was 987 bp, encoding 328 amino acids, and the predicted protein molecular weight was 34.9 kDa. MaCD68 contained two transmembrane helical structures and 18 predicted N-glycosylation sites. Multiple sequence alignments showed that the MaCD68 protein had high homology with other fish, and their functional sites were also highly conserved. Phylogenetic analysis revealed that MaCD68 and other cypriniformes fish clustered into one branch. Adaptive evolution analysis identified several positively selected sites of teleost CD68 using site and branch-site models, indicating that it was under positive selection pressure during evolution. Quantitative real-time reverse transcription polymerase chain reaction analysis showed that MaCD68 was highly expressed in the head kidney, spleen, and heart. After Aeromonas hydrophila infection, MaCD68 was significantly upregulated in all tested tissues, peaking at 12 h post-infection (hpi) in the kidney and head kidney and at 120 hpi in the liver and spleen, suggesting that MaCD68 participated in the innate immune response of the host against bacterial infection. Immunohistochemical and immunofluorescence analyses also showed that positive signals derived from the MaCD68 protein were further enhanced after bacterial and lipopolysaccharide treatment, which suggested that MaCD68 is involved in the immune response and could be used as a macrophage marker. Biological activity analysis indicated that recombinant MaCD68 (rMaCD68) protein had no agglutination or bactericidal effects on A. hydrophila but did have these effects on Escherichia coli. In conclusion, these results suggest that MaCD68 plays a vital role in the immune response against pathogens, which is helpful in understanding the immune responses and mechanisms of M. amblycephala. [ABSTRACT FROM AUTHOR]

[Display omitted] • UiO-66-BAPILs were designed and fabricated for oxidative desulfurization. • The permanent cavity in UiO-66-BAPILs was validated by gas uptake experiments and molecular size simulations. • UiO-66-BAPILs exhibited higher catalytic activity than the two components. • The mechanism was in detail studied by experiments and theoretical calculations. Porous ionic liquids have been highlighted with special interest for their desirable catalytic activity and extraction properties. Herein, bifunctional porous ionic liquids (denoted UiO-66-BAPILs) were synthesized by dispersing UiO-66 into a pyridinium-based Brønsted acidic ionic liquid ([BSPy][CF 3 SO 3 ]) for oxidative desulfurization. The permanent cavity of UiO-66 moiety in UiO-66-BAPILs was validated as well-preserved by the SO 2 uptake experiments and molecular size simulations. Under the optimum reaction conditions, the sulfur removal could reach up to 99.5% with hydrogen peroxide as the oxidant. Additionally, bifunctional UiO-66-BAPILs were deemed as both extractants and catalysts during the reaction. A possible mechanism has been proposed that UiO-66-BAPILs extract the aromatic sulfur compounds via π···π interactions and C-H···π interactions and meanwhile oxidize them with peroxysulfonic acids and •OH radicals. These findings will open up new avenues to facilitate the catalytic oxidation performance by constructing bifunctional Brønsted acidic porous ionic liquids. [ABSTRACT FROM AUTHOR]

For hypoid gear transmission showing time-varying meshing characteristics, three always is a very complicated solid-liquid-thermo-mechanical coupling lubrication interface behavior. In full consideration of tooth flank roughness and non-Newton fluid effect for this thermal elastohydrodynamic lubrication (TEHL) interface, an innovative multi-field coupling lubrication interface heat transfer model is established. Firstly, dynamic loaded tooth contact analysis (DLTCA) is performed to determine the input parameters about lubrication interface behavior, such as meshing interface kinematics, load distribution and entrainment speed parameters. Then, considering tooth roughness setup and non-Newton fluid flow, accurate TEHL interface heat transfer model is developed by establishing three-dimensional (3D) energy equation. Moreover, heat transfer model is solved for time-varying TEHL assessments including oil film pressure, temperature and thickness. Where, a non-Newton fluid effect correction is used to get accurate discretization of oil film pressure flow. In accurate solution to non-Newton fluid effect, an improved Eyring rheological model is employed for accurate computation of comprehensive shear force, flow factor and equivalent viscosity. A column-by-column scanning method is applied to determine the temperature field in a given computational domain. Finally, the numerical instances are provided to verify the proposed model. • DLTCA for basic input parameters determination; • TEHL governing equation considering tooth flank roughness and non-Newton fluid effect; • Computation for roughness tooth flank non-Newton TEHL forecasting equation; • Roughness tooth flank non-Newton TEHL forecasting model; • Time-varying characteristics of TEHL assessments [ABSTRACT FROM AUTHOR]

Lignin is a vital organic constituent of plant biomass and it can be transformed into value-added chemicals through chemical processes. This study employs the Density Functional Theory (DFT) to investigate the mechanistic effects of various oxidants on the depolymerization of sodium lignosulfonate model compounds into vanillin. Under alkaline conditions, OH- ions participation in the hydrolysis of β-O-4 bonds has been predicted. The dehydration of dihydroconiferyl alcohol to form eugenol, with an energy barrier of 69.0 kcal/mol was identified as the major rate-determining step in the oxidation reaction. In the absence of an oxidant, the energy barrier for the oxidation of eugenol to vanillin was 77.8 kcal/mol. However, when using nitrobenzene or H 2 O 2 as oxidants, the energy barrier has significantly decreased to 12.6 kcal/mol and 21.4 kcal/mol, respectively. The effects of temperature and pressure on the rate-determining step of the reaction were analyzed using Statistical Product and Service Solutions (SPSS) software. These results have demonstrated that the energy barrier for the hydrolysis reaction's rate-determining step is positively correlated with temperature but negatively correlated with pressure. These theoretical findings would potentially help in designing the experiments and aid in enhancing the selectivity and yield of vanillin. [Display omitted] • OH- ions promote the breaking of β-O-4 bonds. • Using oxidants like nitrobenzene or H 2 O 2 reduces energy barrier. • Nitrobenzene oxidizes isoeugenol to vanillin with lower energy barrier. [ABSTRACT FROM AUTHOR]

Based on the acid–base neutralization, the (1-methylimidazolium)(tetrazol-1-yl)borane was successfully synthesized by taking advantage of the acidity of the tetrazole and the basicity of the 1-methylimidazole borane complex. Through HRMS, NMR, and FT−IR, the structure of synthetic compounds was characterized in detail. Concerning about the (1-methylimidazolium)(tetrazol-1-yl)borane, it had an ignition−delay time of about 25 ms and a density specific impulse over 351 s·g/cm3, making it a suitable candidate for green hypergolic fuels. Moreover, it also demonstrated that introducing tetrazole into the borane could be an appropriate strategy to adjust the performance of the energy of those borane compounds. [ABSTRACT FROM AUTHOR]

Single atom adsorbents (SAAs) are a novel class of materials that have great potential in various fields, especially in the field of adsorptive desulfurization. However, it is still challenging to gain a fundamental understanding of the complicated behaviors on SAAs for adsorbing thiophenic compounds, such as 1-Benzothiophene (BT), Dibenzothiophene (DBT), and 4,6-Dimethyldibenzothiophene (4,6-DMDBT). Herein, we investigated the mechanisms of adsorptive desulfurization over a single Ag atom supported on defective hexagonal boron nitride nanosheets via density functional theory calculations. The Ag atom can be anchored onto three typical sites on the pristine h-BN, including the monoatomic defect vacancy (B-vacancy and N-vacancy) and the boron-nitrogen diatomic defect vacancy (B-N-divacancy). These three Ag-doped hexagonal boron nitride nanosheets all exhibit enhanced adsorption capacity for thiophenic compounds primarily by the S-Ag bond with π-π interaction maintaining. Furthermore, from the perspective of interaction energy, all three SAAs show a high selectivity to 4,6-DMDBT with the strong interaction energy (−33.9 kcal mol−1, −29.1 kcal mol−1, and −39.2 kcal mol−1, respectively). Notably, a little charge transfer demonstrated that the dominant driving force of such S-Ag bond is electrostatic interaction rather than coordination effect. These findings may shed light on the principles for modeling and designing high-performance and selective SAAs for adsorptive desulfurization. [ABSTRACT FROM AUTHOR]