Functional MXenes: Progress and Perspectives on Synthetic Strategies and Structure-Property Interplay for Next-Generation Technologies.

MXenes are a class of 2D materials that include layered transition metal carbides, nitrides, and carbonitrides. Since their inception in 2011, they have garnered significant attention due to their diverse compositions, unique structures, and extraordinary properties, such as high specific surface areas and excellent electrical conductivity. This versatility has opened up immense potential in various fields, catalyzing a surge in MXene research and leading to note worthy advancements. This review offers an in-depth overview of the evolution of MXenes over the past 5 years, with an emphasis on synthetic strategies, structure-property relationships, and technological prospects. A classification scheme for MXene structures based on entropy is presented and an updated summary of the elemental constituents of the MXene family is provided, as documented in recent literature. Delving into the microscopic structure and synthesis routes, the intricate structure-property relationships are explored at the nano/micro level that dictate the macroscopic applications of MXenes. Through an extensive review of the latest representative works, the utilization of MXenes in energy, environmental, electronic, and biomedical fields is showcased, offering a glimpse into the current technological bottlenecks, such asstability, scalability, and device integration. Moreover, potential pathways for advancing MXenes toward next-generation technologies are highlighted.

Artificial Photosynthetic System with Spatial Dual Reduction Site Enabling Enhanced Solar Hydrogen Production.

Although S-scheme artificial photosynthesis shows promise for photocatalytic hydrogen production, traditional methods often overly concentrate on a single reduction site. This limitation results in inadequate redox capability and inefficient charge separation, which hampers the efficiency of the photocatalytic hydrogen evolution reaction. To overcome this limitation, a double S-scheme system is proposed that leverages dual reduction sites, thereby preserving energetic photo-electrons and holes to enhance apparent quantum efficiency. The design features a double S-scheme junction consisting of CdS nanospheres decorated with anatase TiO2 nanoparticles coupled with graphitic C3 N4 . The as-prepared catalyst exhibits a hydrogen evolution rate of 26.84 mmol g-1  h-1 and an apparent quantum efficiency of 40.2% at 365 nm. This enhanced photocatalytic hydrogen evolution is ascribed to the efficient charge separation and transport induced by the double S-scheme. Both theoretical calculations and comprehensive spectroscopy tests (both in situ and ex situ) affirm the efficient charge transport across the catalyst interface. Moreover, substituting the reduction-type catalyst CdS with other similar sulfides like ZnIn2 S4 , ZnS, MoS2 and In2 S3 further confirms the feasibility of the proposed double S-scheme configuration. The findings provide a pathway to designing more effective double S-scheme artificial photosynthetic systems, opening up fresh perspectives in enhancing photocatalytic hydrogen evolution performance.

Enhancing Photocatalytic Hydrogen Evolution by Synergistic Benefits of MXene Cocatalysis and Homo-Interface Engineering.

Photocatalytic water splitting holds great promise as a sustainable and cost-effectiveness alternative for the production of hydrogen. Nevertheless, the practical implementation of this strategy is hindered by suboptimal visible light utilization and sluggish charge carrier dynamics, leading to low yield. MXene is a promising cocatalyst due to its high conductivity, abundance of active sites, tunable terminal functional groups, and great specific surface area. Homo-interface has perfect lattice matching and uniform composition, which are more conducive to photogenerated carriers' separation and migration. In this study, a novel ternary heterogeneous photocatalyst, a-TiO2 /H-TiO2 /Ti3 C2 MXene (MXTi), is presented using an electrostatic self-assembly method. Compared to commercial P25, pristine anatase, and rutile TiO2 , as-prepared MXTi exhibit exceptional photocatalytic hydrogen evolution performance, achieving a rate of 0.387 mmol h-1 . The significant improvement is attributable to the synergistic effect of homo-interface engineering and Ti3 C2 MXene, which leads to widened light absorption and efficient carrier transportation. The findings highlight the potential of interface engineering and MXene cocatalyst loading as a proactive approach to enhance the performance of photocatalytic water splitting, paving the way for more sustainable and efficient hydrogen production.

Rhodium(I)-Catalyzed Direct Enantioselective C-H Functionalization of Indoles.

A highly regiospecific vinylogous carbene insertion protocol for direct asymmetric C-H functionalization of indoles with arylvinyldiazoacetates has been developed. Under the catalysis of simple Rh(I)/chiral diene complexes, the reaction occurs solely at the vinylogous position of the vinylcarbenoid with exceptional E selectivity and enantiocontrol. It provides an efficient way to obtain an interesting class of chiral indole scaffolds bearing an α,ß-unsaturated ester unit and a gem-diaryl carbon stereocenter in good yields (≤99%) with excellent enantioselectivities (≤96%) at room temperature.

Design of a Coumarin-Based Fluorescent Probe for Efficient In Vivo Imaging of Amyloid-ß Plaques.

Amyloid-ß (Aß) is the core constituent protein of senile plaques, which is one of the key pathological hallmarks of Alzheimer's disease (AD). Here we describe the design, synthesis, and evaluation of coumarin-derived small molecule fluorophores for Aß imaging. By embedding the aromatic coumarin framework into π bridge of a push-pull chromophore, a novel fluorescence probe XCYC-3 applicable to efficient Aß recognition was discovered. XCYC-3 displays higher fluorescent enhancement for aggregated Aß than monomeric Aß, and possesses good blood-brain barrier permeability. In vitro staining and in vivo imaging studies demonstrated that XCYC-3 could efficiently recognize Aß plaques in the brain of AD transgenic mice. These results suggest that XCYC-3 is a promising fluorescence imaging agent for Aß, which might provide important clues for the future development of potent NIR fluorescent probes for Aß diagnosis.

Low Coordination State RhI -Complex as High Performance Catalyst for Asymmetric Intramolecular Cyclopropanation: Construction of penta-Substituted Cyclopropanes.

A simple, broad-scope rhodium(I)/chiral diene catalytic system for challenging asymmetric intramolecular cyclopropanation of various tri-substituted allylic diazoacetates was successfully developed. The low coordination state RhI -complex exhibits an extraordinarily high degree of tolerance to the variation in the extent of substitution of the allyl double bond, thus allowing the efficient construction of a wide range of penta-substituted, fused-ring cyclopropanes bearing three contiguous stereogenic centers, including two quaternary carbon stereocenters, in a highly enantioselective manner with ease at catalyst loading as low as 0.1 mol %. The stereoinduction mode of this RhI -carbene-directed asymmetric intramolecular cyclopropanation was investigated by DFT calculations, indicating that π-π stacking interactions between the aromatic rings of chiral diene ligand and diazo substrate play a key role in the control of the reaction enantioselectivity.

Enhanced sentiment analysis regarding COVID-19 news from global channels.

For a healthy society to exist, it is crucial for the media to focus on disease-related issues so that more people are widely aware of them and reduce health risks. Recently, deep neural networks have become a popular tool for textual sentiment analysis, which can provide valuable insights and real-time monitoring and analysis regarding health issues. In this paper, as part of an effort to develop an effective model that can elicit public sentiment on COVID-19 news, we propose a novel approach Cov-Att-BiLSTM for sentiment analysis of COVID-19 news headlines using deep neural networks. We integrate attention mechanisms, embedding techniques, and semantic level data labeling into the prediction process to enhance the accuracy. To evaluate the proposed approach, we compared it to several deep and machine learning classifiers using various metrics of categorization efficiency and prediction quality, and the experimental results demonstrate its superiority with 0.931 testing accuracy. Furthermore, 73,138 pandemic-related tweets posted on six global channels were analyzed by the proposed approach, which accurately reflects global coverage of COVID-19 news and vaccination.

NanoSNP: a progressive and haplotype-aware SNP caller on low-coverage nanopore sequencing data.

MOTIVATION: Oxford Nanopore sequencing has great potential and advantages in population-scale studies. Due to the cost of sequencing, the depth of whole-genome sequencing for per individual sample must be small. However, the existing single nucleotide polymorphism (SNP) callers are aimed at high-coverage Nanopore sequencing reads. Detecting the SNP variants on low-coverage Nanopore sequencing data is still a challenging problem. RESULTS: We developed a novel deep learning-based SNP calling method, NanoSNP, to identify the SNP sites (excluding short indels) based on low-coverage Nanopore sequencing reads. In this method, we design a multi-step, multi-scale and haplotype-aware SNP detection pipeline. First, the pileup model in NanoSNP utilizes the naive pileup feature to predict a subset of SNP sites with a Bi-long short-term memory (LSTM) network. These SNP sites are phased and used to divide the low-coverage Nanopore reads into different haplotypes. Finally, the long-range haplotype feature and short-range pileup feature are extracted from each haplotype. The haplotype model combines two features and predicts the genotype for the candidate site using a Bi-LSTM network. To evaluate the performance of NanoSNP, we compared NanoSNP with Clair, Clair3, Pepper-DeepVariant and NanoCaller on the low-coverage (∼16×) Nanopore sequencing reads. We also performed cross-genome testing on six human genomes HG002-HG007, respectively. Comprehensive experiments demonstrate that NanoSNP outperforms Clair, Pepper-DeepVariant and NanoCaller in identifying SNPs on low-coverage Nanopore sequencing data, including the difficult-to-map regions and major histocompatibility complex regions in the human genome. NanoSNP is comparable to Clair3 when the coverage exceeds 16×. AVAILABILITY AND IMPLEMENTATION: https://github.com/huangnengCSU/NanoSNP.git. SUPPLEMENTARY INFORMATION: Supplementary data are available at Bioinformatics online.

The color stability, water sorption, and solubility of ten composite resins.

OBJECTIVES: This study aims to evaluate the color stability and related properties including water sorption and solubility of ten light-cured composite resins in different solutions. METHODS: A total of 10 composite resins were BeautifilⅡ(B2) and Ceram. X One Universal (CXU), Charisma (CS), Charisma Diamond (CD), Denfil (DF), DX. Universal (DXU), Filtek Z250 (Z250), Filtek Z350 XT (Z350), FS-1 (FS), and Magnafill Putty (MP). Meanwhile, a total of 20 disk-shaped samples were fabricated and randomly divided into four groups (n=5), which were immersed in distilled water (control group), curry, coffee, and red wine for 28 days. The color (CIE L∗a∗b∗) was measured by a spectrophotometer at baseline and 1, 7, 14, 21, and 28 days after immersion, and the color differences were calculated. Water sorption and solubility values were measured ba-sed on ISO 4049: 2019. In addition, three-way ANOVA was used to evaluate the influence of resin materials, solutions, and immersion time on discoloration results, meanwhile, one-way ANOVA was used to compare the water sorption values and solubility values of different materials. RESULTS: All samples showed a certain degree of color change with time. Color differences were significantly influenced by materials, solutions, and immersion time (P<0.001). The color changes of the measured materials at any time point: curry>red wine>coffee>distilled water. Thus, all materials showed clinically unacceptable discoloration (ΔE>3.3) after immersing in staining curry, coffee, and red wine for 7 days. Therefore, when immersed in curry for 28 days, CS and DXU had the smallest and the largest color difference. In addition, when immersed in coffee for 28 days, FS showed the smallest color change and DXU showed the largest. Moreover, when immersed in red wine for 28 days, FS showed the smallest color change and Z350 showed the largest. Furthermore, MP and CXU had small color differences in all solutions. Meanwhile, Z350 had the highest water sorption and MP had the lowest. The solubility values of CS and CD were significantly higher than those of other materials. CONCLUSIONS: The color stability of light-cured composite resin is materials-depended and affected by pigment types and immersion time. Thus, MP and CXU have better color stability. MP has low water sorption.

Rhodium-Catalyzed Asymmetric 1,4-Addition of α/ß-(N-Indolyl) Acrylates.

A rhodium-catalyzed asymmetric 1,4-addition of α/ß-(N-indolyl) acrylates to access highly enantioenriched chiral N-alkylindoles promoted by chiral diene or sulfur-olefin ligands under mild reaction conditions has been developed, which provides an efficient and practical approach for constructing carbon stereocenters adjacent to the indole nitrogen. The reaction can be applied to various N-indolyl-substituted α,ß-unstaturated esters and arylboron reagents, providing access to a wide range of α- and ß-(N-indolyl) propionate derivatives in high yields with excellent enantioselectivities (≤99% ee).

Evaluation of the Color Stability, Water Sorption, and Solubility of Current Resin Composites.

This study aims to assess the color stability, water sorption, and solubility of 11 resin composites as commercially available dental products. Twenty samples (10 mm in diameter and 2 mm in thickness) of each material were fabricated using a customized silicone mold, followed by immersion in each of curry, coffee, wine, and distilled water for 28 days (n = 5). Baseline shade and color changes (ΔE) were measured using a reflection spectrophotometer. The CIE L*, a*, b* system was used to evaluate the color changes. Five samples of each resin composite were applied to test water sorption and solubility according to ISO 4049:2009. As a result, the ∆E values were significantly influenced by each of the three factors (composition of material, solution, time) and the interactions between them (p < 0.001). Highest resistance to discoloration was achieved by Ceram.X One Universal (CXU), followed by Magnafill Putty (MP). Generally, microhybrid composites showed fewer color changes than nanohybrid composites and giomers. DX. Universal and Filtek Z350 XT showed the highest ΔE values in all colorants. All materials tested in this study fulfilled the criteria of ISO 4049:2009; CXU and MP had the lowest water sorption and solubility. The Pearson test showed statistically significant positive correlations between water sorption and ΔE and between solubility and ΔE.

Media Bias and Factors Affecting the Impartiality of News Agencies during COVID-19.

When COVID-19 was raging around the world, people were more fearful and anxious. In this context, the media should uphold impartiality and shoulder the responsibility of eliminating misinformation. Therefore, our research adopted sentiment analysis technologies to analyze the impartiality of news agencies and analyzed the factors that affect the impartiality of COVID-19-related articles about various countries. The SentiWordNet3.0 and bidirectional encoder representations from transformers (BERT) models were employed to analyze the articles and visualize the data. The following conclusions were redrawn in our research. During the pandemic, articles of some news agencies were not objective; the impartiality of news agencies was related to the reliability of news agencies instead of the bias of news agencies; there were obvious differences in the coverage and positivity of international news agencies to report the performance of COVID-19 prevention and control in different countries.

Rhodium(I) Carbene-Promoted Enantioselective C-H Functionalization of Simple Unprotected Indoles, Pyrroles and Heteroanalogues: New Mechanistic Insights.

A rhodium(I)-diene catalyzed highly enantioselective C(sp2 )-H functionalization of simple unprotected indoles, pyrroles, and their common analogues such as furans, thiophenes, and benzofurans with arylvinyldiazoesters has been developed for the first time. This transformation features unusual site-selectivity exclusively at the vinyl terminus of arylvinylcarbene and enables a reliable and rapid synthetic protocol to access a distinctive class of diarylmethine-bearing α,ß-unsaturated esters containing a one or two heteroarene-attached tertiary carbon stereocenter in high yields and excellent enantioselectivities under mild reaction conditions. Mechanistic studies and DFT calculations suggest that, compared to the aniline substrate, the more electron-rich indole substrate lowers the C-C addition barrier and alters the rate-determining step to the reductive elimination, leading to different isotope effect.

Association of Killer Cell Immunoglobulin-like Receptor and Human Leukocyte antigen-C Genotype with HLA-B27 Associated Acute Anterior Uveitis and Idiopathic Acute Anterior Uveitis in a Chinese Han Population.

PURPOSE: whether killer cell immunoglobulin-like receptors (KIRs) and human leukocyte antigens C (HLA-C) are associated with HLA-B27 associated acute anterior uveitis (B27AAU) and idiopathic AAU (IAAU) remains unclear. METHODS: PCR with sequence-specific primers was used to analyze KIR genes and HLA-C alleles in a Chinese Han population of 196AAU patients and 210 control subjects. RESULTS: The higher frequencies of HLA-C2 and KIR2DL1/HLA-C2 (p = .009 and p = .044, respectively) and the lower frequencies of HLA-C1C1 and HLA-C1 (p = .034 and p = .009, respectively) were observed in B27AAU than control group. The higher frequencies of KIR2DL2 and KIR2DL2/HLA-C1 (p = .009 and p = .044, respectively) and the lower frequencies of KIR2DL3 and KIR2DL3/HLA-C1 (p = .000 and p = .001, respectively) were observed in IAAU than control group. CONCLUSIONS: HLA-C2 and KIR2DL1/HLA-C2, KIR2DL2, and KIR2DL2/HLA-C1 might be susceptible for B27AAU and IAAU, respectively. HLA-C1C1 and HLA-C1, KIR2DL3 and KIR2DL3/HLA-C1 might protect from B27AAU and IAAU, respectively.

Topics, Sentiments, and Emotions Triggered by COVID-19-Related Tweets from IRAN and Turkey Official News Agencies.

There is no doubt that the COVID-19 epidemic posed the most significant challenge to all governments globally since January 2020. People have to readapt after the epidemic to daily life with the absence of an effective vaccine for a long time. The epidemic has led to society division and uncertainty. With such issues, governments have to take efficient procedures to fight the epidemic. In this paper, we analyze and discuss two official news agencies' tweets of Iran and Turkey by using sentiment- and semantic analysis-based unsupervised learning approaches. The main topics, sentiments, and emotions that accompanied the agencies' tweets are identified and compared. The results are analyzed from the perspective of psychology, sociology, and communication.

Stereodivergent Synthesis of Enantioenriched 2,3-Disubstituted Dihydrobenzofurans via a One-Pot C-H Functionalization/Oxa-Michael Addition Cascade.

A one-pot rhodium-catalyzed C-H functionalization/organocatalyzed oxa-Michael addition cascade reaction has been developed. This methodology enables the stereodivergent synthesis of diverse 2,3-disubstituted dihydrobenzofurans with broad functional group compatibility in good yields with high levels of stereoselectivity under exceptionally mild conditions. The full complement of stereoisomers of chiral 2,3-disubstituted dihydrobenzofurans and 3,4-disubstituted isochromans could be accessed at will by appropriate permutations of the two chiral catalysts. The current work provides a rare example of two chiral catalysts independently controlling two contiguous stereogenic centers subsequently via a two-step reaction in a single operation.

Near-infrared fluorescent probe for evaluating the acetylcholinesterase effect in the aging process and dietary restriction via fluorescence imaging.

Dietary restriction (DR), as a natural intervention, not only benefits the neuroendocrine system, but also has an antiaging action. Acetylcholinesterase (AChE) is one of the most important bioactive substances and plays a major part in choline changes in the aging process. Thus, we aim to evaluate the effect of DR on AChE in the brains of aging animals. In this study, we synthesize a NIR fluorescent probe BD-AChE for the real-time and in situ monitoring of AChE level changes in living cells and living mice, notably in brains. In situ visualization with BD-AChE verified a decrease in the AchE level in the brains of mice aging models. Evidently, the prepared probe has the excellent capability of measuring AChE variation in the brains of aging mice with DR via NIR fluorescence bioimaging, indicating that long-term DR can effectively affect AChE levels in the brain. The attenuation of AChE level in the brain of aging mice after DR could be helpful in infering the advantageous impact of DR on age-related neurodegenerative disease, as a better treatment alternative in the future.

Regiospecific and Enantioselective Arylvinylcarbene Insertion of a C-H Bond of Aniline Derivatives Enabled by a Rh(I)-Diene Catalyst.

Asymmetric insertion of an arylvinylcarbenoid into the C-H bond for direct enantioselective C(sp2)-H functionalization of aniline derivatives catalyzed by a rhodium(I)-diene complex was developed for the first time. The reaction occurred exclusively at the uncommon vinyl terminus site with excellent E selectivity and enantioselectivities, providing various chiral γ,γ-gem-diarylsubstituted α,ß-unsaturated esters with broad functional group compatibility under simple and mild conditions. It provides a rare example of the asymmetric C-H insertion of arenes with selective vinylogous reactivity. Synthesis applications of this protocol were featured by several versatile product transformations. Systematic DFT calculations were also performed to elucidate the reaction mechanism and origin of the uncommon enantio- and regioselectivity of the Rh(I)-catalyzed C(sp2)-H functionalization reaction. The measured and computed inverse deuterium kinetic isotope effect supports the C-C bond-formation step as the rate-determining step. Attractive interactions between the chiral ligand and substrates were also proposed to control the enantioselectivity.

Water as a Direct Proton Source for Asymmetric Hydroarylation Catalyzed by a Rh(I)-Diene: Access to Nonproteinogenic ß2/γ2/δ2-Amino Acid Derivatives.

A highly enantioselective rhodium-catalyzed intermolecular hydroarylation of α-aminoalkyl acrylates using water as a direct proton source has been realized by employing a chiral bicyclo[3.3.0] diene ligand, allowing efficient access to a broad range of α-aryl-methyl-substituted ß2-, γ2-, and δ2-amino esters with excellent enantioselectivities (up to 98% ee) under exceptionally mild conditions. By utilizing this method, a series of structurally interesting benzo-fused heterocyclic molecules and the corresponding ß2-, γ2-, and δ2-amino acids are facilely constructed.

Clinical study of different doses of atorvastatin combined with febuxostat in patients with gout and carotid atherosclerosis.

OBJECTIVE: To evaluate the efficacy of atorvastatin combined with febuxostat in the treatment of gout patients with carotid atherosclerosis and to observe the effects on serum tumor necrosis factor-α (TNF-α), interleukin-1ß (IL-1ß), and C-reactive protein (CRP) levels, carotid plaques, and the adverse reactions. METHODS: Seventy patients with gout and carotid atherosclerosis admitted to Affiliated Hospital of Hebei University from January 2014 to June 2017 were randomly divided into a treatment group and a control group. The treatment group received oral febuxostat 40 mg/day combined with atorvastatin 40 mg/day. The control group was given 40 mg/day febuxostat combined with 20 mg/day atorvastatin for 90 days. The effects of treatment on TNF-α, IL-1ß, and CRP levels and carotid plaques of the patients were observed. RESULTS: After 90 days of treatment, serum TNF-α, IL-1ß, and CRP levels, as well as HUA and total cholesterol (TC), decreased in both groups after treatment. There were significant differences observed (p < 0.05). The carotid artery plaques in the two groups were significantly smaller after treatment (P<0.05). There was no significant difference in adverse reactions between the two groups (P > 0.05). CONCLUSION: Double doses of atorvastatin combined with febuxostat can effectively reduce uric acid to improve the inflammatory state in patients and reduce carotid plaques without increasing the incidence of adverse reactions.