Electrodeposition of Ni/Cu Bimetallic Conductive Metal-Organic Frameworks Electrocatalysts with Boosted Oxygen Reduction Activity for Zinc-Air Batteries.

Zinc-air batteries employing non-Pt cathodes hold significant promise for advancing cathodic oxygen reduction reaction (ORR). However, poor intrinsic electrical conductivity and aggregation tendency hinder the application of metal-organic frameworks (MOFs) as active ORR cathodes. Conductive MOFs possess various atomically dispersed metal centers and well-aligned inherent topologies, eliminating the additional carbonization processes for achieving high conductivity. Here, a novel room-temperature electrochemical cathodic electrodeposition method is introduced for fabricating uniform and continuous layered 2D bimetallic conductive MOF films cathodes without polymeric binders, employing the organic ligand 2,3,6,7,10,11-hexaiminotriphenylene (HITP) and varying the Ni/Cu ratio. The influence of metal centers on modulating the ORR performance is investigated by density functional theory (DFT), demonstrating the performance of bimetallic conductive MOFs can be effectively tuned by the unpaired 3d electrons and the Jahn-Teller effect in the doped Cu. The resulting bimetallic Ni2.1Cu0.9(HITP)2 exhibits superior ORR performance, boasting a high onset potential of 0.93 V. Moreover, the assembled aqueous zinc-air battery demonstrates high specific capacity of 706.2 mA h g-1, and exceptional long-term charge/discharge stability exceeding 1250 cycles.

Direct Synthesis of α-Ketoamides via Copper-Catalyzed Reductive Amidation of Nitroarenes with α-Oxocarboxylic Acids.

Nitroarenes are known for their stability, low toxicity, easy availability, and cost-effectiveness, making them one of the most fundamental chemical feedstocks. The direct utilization of nitroarenes as nitrogen sources in amidation reactions offers significant advantages over using arylamines. Herein, we disclose a streamlined method for constructing α-ketoamides through the direct coupling of nitroarenes with α-oxocarboxylic acids. This transformation obviates the need for preparing, isolating, and purifying arylamines, leading to improved efficiency, cost-effectiveness, and time savings.

Contributions of Visuo-oculomotor Abilities to Interceptive Skills in Sports.

PURPOSE: Monitoring and intercepting a fast approaching object is a critical skill for many sports. Athletes might be distinguished from nonathletes based on their ability to access various visual abilities to accomplish interceptive actions. Here, we examined whether interceptive visuomotor skills of athletes and nonathletes are differently correlated to a hierarchy of visuo-oculomotor abilities related to the perception of motion in depth. METHODS: Eighty-six athletes in interceptive sports, as well as 60 nonathletes, were recruited based on their sport performance and prior experiences. Their basic visual abilities (dominant eye acuity, contrast sensitivity, visual span, and visual memory) and complex visuo-oculomotor abilities (dynamic acuity, accommodative facility, near point of convergence, and near/far phoria) were analyzed in relation to critical visuomotor skills (manual interception, visually guided locomotion, and depth judgment). RESULTS: Discriminant analysis revealed that athletes and nonathletes can be accurately differentiated based on measured visuomotor skills (91.3% accuracy, p < 0.0001). Near point of convergence, accommodative facility, and dynamic acuity were moderately effective in identifying athletes (71.3%, p = 0.002) and in predicting the three visuomotor skills (all r(2) ≥ 0.096, all p ≤ 0.022). Dominant eye acuity and contrast sensitivity also identified athletes (61.4%, p = 0.021) and contributed to complex visuo-oculomotor abilities (all r(2) ≥ 0.046, all p ≤ 0.039). The correlations among measured abilities were more significant for athletes than nonathletes. CONCLUSIONS: Athletes in interceptive sports are superior to nonathletes in their visuomotor skills. They also have broader access to various visual and complex visuo-oculomotor abilities than nonathletes. This likely allows athletes to more effectively coordinate visual and oculomotor abilities under demanding conditions when some visual cues are degraded. The present findings are consistent with a pyramid of sports vision and suggest a top-down process for athlete screening and training.

[Physical exercise and mental health: cognition, anxiety, depression and self-concept].

This review focuses on the benefits of regular physical activity participation have mainly focused on cognitive functioning, anxiety and depression, and self-concept. It is well documented that ex- ercise can enhance cognitive functioning, improve executive function at old age, and improve mental abil- ity of children labeled as educational subnormal or disability. Regular exercise has been used to reduce stress and ward off anxiety and feelings of depression. In addition, exercise can improve self-esteem and positive outlook in life. Studies in these three main areas were reviewed and issues and future directions were highlighted.

A comparison of the physical activity levels of 3-to-6-year-old children with autism spectrum disorder and children with typical development.

Background: Physical activity during early development is closely related to health. Differences in physical activity between young children with autism spectrum disorder and those with typical development are unclear. The purpose of this study was to compare the physical activity levels in children with autism spectrum disorder and typically developing children from the same area, including their sedentary physical activity, light physical activity, moderate-to-vigorous physical activity, and number of days in which the moderate-to-vigorous physical activity guideline recommendation of 60 min per day was met. Methods: A total of 77 participants aged 3-6 years were included: 41 children with autism spectrum disorder (mean age = 61.41 ± 10.69 months) and 36 children with typical development (mean age = 60.36 ± 10.16 months). The physical activity of the children was measured using an ActiGraph GT3x accelerometer. Results: There were no significant differences in daily sedentary physical activity (439.70 ± 54.98 vs. 450.42 ± 53.67) or moderate-to-vigorous physical activity (46.62 ± 18.93 vs. 47.47 ± 18.26) between the two groups. The average daily moderate-to-vigorous physical activity of the two groups did not reach 60 min, and they had similar proportions of participants who reached 60 min a given number of times (24.4% vs. 25%). Daily light physical activity was significantly higher in the autism spectrum disorder group (263.96 ± 43.17 vs. 242.32 ± 37.91, p < 0.05). The moderate-to-vigorous physical activity of both groups was similar and lower than the recommended minimum physical activity. Conclusion: Targeted interventions should be considered in early intervention programs for children with autism spectrum disorder to increase their moderate-to-vigorous physical activity.

Designing ultrathin Fe doped Ta2O5-x nanobelts for highly enhanced ammonia photosynthesis.

Solar-light photosynthesis of ammonia form N2 reduction in ultrapure water over the artificial photocatalysts is attractive but still challenging compared with Haber-Bosch process. In this work, ultrathin Fe-Ta2O5-x nanobelts were fabricated via the controllable solvothermal process for ammonia photosynthesis. The formed oxygen vacancies and Fe doping narrowed their bandgap energies and promoted the carriers' separation and transfer for Fe-Ta2O5-x nanobelts. In addition, Fe doping also resulted in the reduced working functions of the samples, indicating a weaker electron binding restriction and stronger separation and transfer of photo-induced carriers. The experimental results showed that Fe-Ta2O5-x nanobelts showed remarkably enhanced photocatalytic ammonia production performance under simulated sunlight irradiation, and the relevant ammonia production rate reached approximately 3030.86 µM g-1 h-1, which was 9.63 times of pristine Ta2O5-x and 491.0 times of commercial Ta2O5, and a relatively stable photocatalytic ammonia production performance under simulated sunlight irradiation for Fe-Ta2O5-x nanobelts. Meanwhile, it was also found that Fe doping has great influences on the photocatalytic performance under visible light and simulated sunlight irradiation, mainly because of their suitable bandgap energies and enhanced solar-light harvesting capacity. Current work indicates the great potentials of ultrathin tantalum-based functional materials for high-efficiency ammonia photosynthesis.

The relationship between inflammatory cytokines and in-hospital complications of acute pancreatitis.

OBJECTIVE: Acute necrotic collection (ANC), acute peripancreatic fluid collection (APFC), pleural effusion, and ascites are common early complications of acute pancreatitis. This study aimed to investigate the relationship between 12 serum cytokines and the early complications and severity of acute pancreatitis (AP). METHODS: We retrospectively analyzed the clinical data of 307 patients with AP, and divided them into severe group and mild-to-moderate group according to the revised Atlanta classification. Propensity score matching was used to control for confounding factors. Binary logistic regression analysis was used to explore the relationship between cytokine levels and early complications of AP. RESULTS: Serum levels of interleukin (IL)-1ß, IL-5, IL-6, IL-8, IL-10, IL-17, and tumor necrosis factor-α were significantly higher in the severe acute pancreatitis (SAP) group than in the non-SAP group (p < .05). After adjusting for confounding factors, the upper quartiles of IL-6, IL-8, and IL-10 were associated with an increased risk of ANC compared with those in the lowest quartile (IL-6: quartile 3, odds ratio [OR] = 3.99, 95% confidence interval [CI] = 1.95-8.16; IL-8: quartile 4, OR = 2.47, 95% CI = 1.27-4.84; IL-10: quartile 2, OR = 2.22, 95% CI = 1.09-4.56). APFC was associated with high serum levels of IL-6 (quartile 3, OR = 1.32, 95% CI = 1.02-1.72), pleural effusions were associated with high serum levels of IL-1ß, IL-6, IL-8, and IL-10 (IL-1ß: quartile 4, OR = 2.36, 95% CI = 1.21-4.58; IL-6: quartile 3, OR = 4.67, 95% CI = 2.27-9.61; IL-8: quartile 3, OR = 2.95, 95% CI = 1.51-5.79; IL-10: quartile 4, OR = 3.20, 95% CI = 1.61-6.36), and high serum levels of IL-6 and IL-10 were associated with an increased risk of ascites (IL-6: quartile 3, OR = 3.01, 95% CI = 1.42-6.37; IL-10: quartile 3, OR = 2.57, 95% CI = 1.23-5.37). CONCLUSION: Serum cytokine levels, including IL-1ß, IL-6, IL-8, and IL-10 may be associated with the occurrence of early complications of AP. In daily clinical practice, IL-6 may be the most worthwhile cytokine to be detected.

Enhanced degradation of phenolic pollutants by a novel cold-adapted laccase from Peribacillus simplex.

Laccase (EC 1.10.3.2), as eco-friendly biocatalysts, holds immense potential for sustainable applications across various environmental and industrial sectors. Despite the growing interest, the exploration of cold-adapted laccases, especially their unique properties and applicability, remains limited. In this study, we have isolated, cloned, expressed, and purified a novel laccase from Peribacillus simplex (GenBank: PP430751), which was derived from permafrost layer. The recombinant laccase (PsLac) exhibited optimal activity at 30 °C and a pH optimum of 3.5. Remarkably, PsLac exhibited remarkable stability in the presence of organic solvents, with its enzyme activity increasing by 20 % after being incubated in a 30 % trichloromethane solution for 12 h, compared to its initial activity. Furthermore, the enzyme preserved 100 % of its activity after undergoing eight freeze-thaw cycles. Notably, the catalytic center of PsLac contains Zn2+ instead of the typically observed Cu2+ found in other laccases, and metal-ion substitution experiments raised the catalytic efficiency to 3-fold when Zn2+ was replaced with Fe2+. Additionally, PsLac has demonstrated a proficient ability to degrade phenolic pollutants, such as hydroquinone, even at a low temperature of 16 °C, positioning it as a promising candidate for environmental bioremediation and contributing to cleaner production processes.

Dual role of nitroarenes as electrophiles and arylamine surrogates in Buchwald-Hartwig-type coupling for C-N bond construction.

One of the most widely utilized methods for the construction of C(sp2)-N bonds is the transition-metal-catalyzed cross-coupling of aryl halides/boronic acids with amines, known as Ullmann condensation, Buchwald-Hartwig amination, and Chan-Lam coupling. However, aryl halides/boronic acids often require multi-step preparation while generating a large amount of corrosive and toxic waste, making the reaction less attractive. Herein, we present an unprecedented method for the C(sp2)-N formation via Buchwald-Hartwig-type reactions using synthetically upstream nitroarenes as the sole starting materials, thus eliminating the need for arylhalides and pre-formed arylamines. A diverse range of symmetrical di- and triarylamines were obtained in a single step from nitroarenes, and more importantly, various unsymmetrical di- and triarylamines were also highly selectively synthesized in a one-pot/two-step process. Furthermore, the success of the scale-up experiments, the late-stage functionalization of a drug intermediate, and the rapid preparation of hole-transporting material TCTA showcased the utility and practicality of this protocol in synthetic chemistry. Mechanistic studies indicate that this transformation may proceed via an arylamine intermediate generated in situ from the reduction of nitroarenes, which is followed by a denitrative Buchwald-Hartwig-type reaction with another nitroarene to form a C-N bond.

Synergistic enhancement of oxygen vacancy enrichment and morphology regulation in CeO2-NiCo2O4 heterostructure catalysts for high-performance cathodes in direct borohydride-hydrogen peroxide fuel cells.

Hydrogen peroxide (H2O2) emerges as a viable oxidant for fuel cells, necessitating the development of an efficient and cost-effective electrocatalyst for the hydrogen peroxide reduction reaction (HPRR). In this study, we synthesized a self-supporting, highly active HPRR electrocatalyst comprising two morphologically distinct components: CeO2-NiCo2O4 nanowires and CeO2-NiCo2O4 metal organic framework derivatives, via a two-step hydrothermal process followed by air calcination. X-ray diffraction and transmission electron microscopy analysis confirmed the presence of CeO2 and NiCo2O4, revealing the amalgamated interface between them. CeO2 exhibits multifunctionality in regulating the surface electronic configuration of NiCo2O4, fostering synergistic connections, and introducing oxygen deficiencies to enhance the catalytic efficacy in HPRR. Electrochemical measurements demonstrate a reduction current density of 789.9 mA·cm-2 at -0.8 V vs. Ag/AgCl. The assembly of direct borohydride-hydrogen peroxide fuel cell (DBHPFC) exhibits a peak power density of 45.2 mW·cm-2, demonstrating durable stability over a continuous operation period of 120 h. This investigation providing evidence that the fabrication of heterostructured catalysts based on CeO2 for HPRR is a viable approach for the development of high-efficiency electrocatalysts in fuel cell technology.

Association of Collagen Changes in Distal Anastomotic Margin and Anastomotic Stenosis after Neoadjuvant Chemoradiotherapy for Rectal Cancer.

BACKGROUND: Neoadjuvant chemoradiotherapy (nCRT) for rectal cancer can lead to structural changes in collagen in the tumor microenvironment and increase the risk of postoperative anastomotic stenosis (AS). However, the quantitative relationship between AS and collagen has not been defined. This study is to quantitatively analyze the collagen features in rectal cancer and explore the relationship between the changes of collagen and postoperative anastomotic stenosis after nCRT. STUDY DESIGN: This is a retrospective study. A total of 371 patients with rectal cancer were included. Collagen features in the resection margin of rectal cancer anastomosis was extracted by multiphoton imaging. The least absolute shrinkage operator logistic regression was performed to select features related to AS and the collagen score (CS) was constructed. Area under the receiver operating curve (AUROC) and decision curve analysis were performed to evaluate the discrimination and clinical benefit of the nomogram. RESULTS: The probability of AS was 23% in the training cohort and 15.9% in the validation cohort. In the training cohort, the distance between tumor and resection margin, anastomotic leakage and CS were independent risk factors for postoperative AS in univariate and multivariate analyses. A nomogram was constructed based on these results. The prediction nomogram showed good discrimination (AUROC 0.864; 95% CI 0.776 to 0.952) and was validated in the validation cohort (AUROC 0.918; 95% CI 0.851 to 0.985). CONCLUSIONS: CS is an independent risk factor for AS in rectal cancer after nCRT. The predictive model based on CS can predict the occurrence of postoperative AS.

Effects of pleiotrophin (PTN) on the FAK inhibitor Y15 in breast cancer cells.

Overexpression of PTN (Pleiotrophin) in breast cancer cells stimulates breast cell proliferation and anti-apoptosis via the FAK/Src signaling pathway.1,2,4,5-Benzenetetramine tetrahydrochloride (C6H14Cl4N4) known as Y15 is an inhibitor that specifically blocks phosphorylation of Y397-FAK and total FAK phosphorylation. The exogenous PTN protein was induced to be expressed by a prokaryotic expression strain. The addition of PTN protein decreased the sensitivity of breast cancer cells to Y15, as shown by both MTT and flow cytometry assays. Breast cancer cells transfected with sh-RNA knockdown PTN were analyzed by real-time fluorescence quantitative PCR reaction (RT-PCR) and protein immunoblotting 24 h after transfection. MTT assay data showed a significant increase in the IC50 value of Y15 against breast cancer cells in the presence of PTN protein. Flow cytometry data confirmed the dose-dependent anti-apoptotic effect of PTN protein in Y15-treated breast cancer cells. After transfection with sh-RNA, Y15 further inhibited the FAK pathway, greatly reducing cell survival and promoting apoptosis. Western blotting analysis showed that knockdown of PTN protein with sh-RNA resulted in increased apoptosis and elevated levels of apoptotic proteins, such as cleaved PARP and cleaved caspase-3 in Y15-induced breast cancer cells. Finally, it was hypothesized that PTN and Y15 were associated with a significant increase in the IC50 value of PTN and Y15 in breast cancer cells by western blotting analysis. It was hypothesized that PTN and Y15 regulate the proliferation and apoptosis of breast cancer cells through the AKT/PI3K pathway. The results demonstrated that PTN affects the sensitivity of the kinase inhibitor Y15, and PTN silencing and Y15 may inhibit the survival of breast cancer cells through the AKT/PI3K pathway, which lays the foundation for subsequent in-depth research on the clinical treatment of breast cancer.

Palladium-Catalyzed Denitrative α-Arylation of Heteroarenes with Nitroarenes via C-H and C-NO2 Bond Activations.

A general approach for the α-arylation of heteroarenes with nitroarenes via denitrative coupling is reported for the first time. Various heteroarenes, including derivatives of furan, benzofuran, pyrrole, indole, thiophene, and benzothiophene, can be arylated at the α-position in moderate to good yields. Mechanistic studies demonstrate that the reaction proceeds via a CMD pathway, with C-H bond activation as the rate-determining step. Furthermore, the scalability and applicability in the synthesis of a drug molecule exemplify the utility of this protocol.

Reconfigurable Five-In-One Carbon Nanotube Optoelectronic Transistor for Intelligent Computing and Communication.

Advances in artificial general intelligence (AGI) necessitate the integration of diverse functionalities to address complex tasks. Carbon nanotubes (CNTs), with their unique physical properties, have broad applications in emerging research fields, providing a foundation for next-generation devices that could overcome the limits of Moore's Law. This work demonstrates a novel intelligent device that integrates five functions─sensors, memory, neuromorphic computing, logic, and communication─using CNT field-effect transistors (CNFETs) compatible with CMOS processes. Through passivation and annealing techniques, we have significantly enhanced the optoelectronic performance of CNFETs, leading to the development of multifunctional optoelectronic synaptic transistors. These optimized CNFETs enable dual-mode weight-tunable synaptic functions, including long-term plasticity and multilevel storage. Additionally, a CNT-based neural network has achieved high recognition accuracy on the MNIST data set, showcasing the potential of in-memory computing. This research also innovates by integrating logic functions with optoelectronic communication capabilities, paving the way for next-generation intelligent computing and communication integrated systems.

Athletes' self-compassion and emotional resilience to failure: the mediating role of vagal reactivity.

Whether athletes' self-compassion predicts their emotional resilience to failure has yet to be empirically tested. Moreover, as an important physiological process of stress regulation, vagal reactivity is a plausible physiological mechanism for this relationship. Through a laboratory-based observational study of 90 college athletes, this research explores the influence of athletes' trait self-compassion on their emotional resilience when recalling failure, and examines whether vagal reactivity plays a mediating role. The results show that self-compassion did not significantly predict athletes' positive emotions but did significantly predict better recovery from negative emotions after recalling failure events. Furthermore, vagal reactivity was a significant mediator between self-compassion and recovery from negative emotions.

Wild­type KRAS inhibits the migration and invasion of pancreatic cancer through the Wnt/ß­catenin pathway.

Kirsten rat sarcoma virus (KRAS) mutation is considered to be the event that leads to the initiation of pancreatic ductal adenocarcinoma (PDAC), the mutation frequency of the KRAS gene in PDAC is 90­95%. Studies have shown that wild­type KRAS (KRASWT) has a survival advantage in PDAC and can antagonize the effect of mutated KRAS G12D (KRASG12D), leading to a low cell transformation efficiency. The present study focused on the differences in biological behavior between KRASWT and KRASG12D and explored the mechanism in pancreatic cancer. Overexpressed KRASWT and KRASG12D was transfected into cells through lentiviral transfection. The differences and mechanisms were explored using cell counting kit­8 (CCK­8), clone formation, wound healing and Transwell assays, as well as western blotting, immunohistochemistry and tumor formation in nude mice. In vitro, the proliferation of KRASWT group was reduced compared with PANC­1 group, while the proliferation of KRASG12D group was not significantly changed. In vivo, the proliferation of KRASWT group was reduced and that of KRASG12D group was enhanced compared with that in the PANC­1 group. The invasion and migration of KRASWT group were decreased, while the invasion and migration of KRASG12D group were increased. Western blotting showed that the expression of E­cadherin, α­E­catenin, MMP­3, MMP­9, STAT3 and phosphorylated STAT3 in KRASWT group was increased, while no significant difference was observed in KRASG12D group. The results of immunohistochemistry were consistent with those of western blotting. KRASWT group can inhibit the proliferation of pancreatic cancer in vitro and in vivo, while KRASG12D group can significantly promote proliferation in vivo, but not significantly in vitro. Wild­type KRAS may inhibit the invasion and migration of pancreatic cancer through the Wnt/ß­catenin pathway.

Potential applications of prognostic and immunological marker transmembrane serine proteinase 2 in prediction, prevention and personalized treatment of lung cancer.

Transmembrane serine proteinase 2 (TMPRSS2), which is an essential serine protease for priming spike protein of SARS-CoV-2, was found in low expression in many cancer tissue including lung cancer. However, the mechanism of severely downregulated in lung adenocarcinoma (LUAD) and lung squamous cell carcinoma (LUSC) was not reported yet; the correlation between TMPRSS2 and prognosis in LUAD and LUSC is also not clear. In our present research, we found that TMPRSS2 was severely downregulated in LUAD and LUSC, and the expression of TMPRSS2 in LUAD is much lower than that of LUSC. Low TMPRSS2 expression was an independent prognostic factor for poor OS in LUAD, but not in LUSC patients. Promoter hypermethylation is one of the results of TMPRSS2 downregulated in LUAD and LUSC, whereas copy-number alteration is another reason for TMPRSS2 downregulated in LUAD but not LUSC. Then, low TMPRSS2 expression has higher prognostic value in LUAD and may be due to different immune environments and different enriched immune cells subgroups.

Recent Advances in Strategies to Combat Bacterial Drug Resistance: Antimicrobial Materials and Drug Delivery Systems.

Bacterial infection is a common clinical disease. Antibiotics have saved countless lives since their discovery and are a powerful weapon in the fight against bacteria. However, with the widespread use of antibiotics, the problem of drug resistance now poses a great threat to human health. In recent years, studies have investigated approaches to combat bacterial resistance. Several antimicrobial materials and drug delivery systems have emerged as promising strategies. Nano-drug delivery systems for antibiotics can reduce the resistance to antibiotics and extend the lifespan of novel antibiotics, and they allow targeting drug delivery compared to conventional antibiotics. This review highlights the mechanistic insights of using different strategies to combat drug-resistant bacteria and summarizes the recent advancements in antimicrobial materials and drug delivery systems for different carriers. Furthermore, the fundamental properties of combating antimicrobial resistance are discussed, and the current challenges and future perspectives in this field are proposed.

Hierarchical CoNiO2 Microflowers Assembled by Mesoporous Nanosheets as Efficient Electrocatalysts for Hydrogen Evolution Reaction.

In order to alleviate the energy crisis and propel a low-carbon economy, hydrogen (H2) plays an important role as a renewable cleaning resource. To break the hydrogen evolution reaction (HER) bottleneck, we need high-efficiency electrocatalysts. Based on the synergistic effect between bimetallic oxides, hierarchical mesoporous CoNiO2 nanosheets can be fabricated. Combining physical representations with electrochemical measurements, the resultant CoNiO2 catalysts present the hierarchical microflowers morphology assembled by mesoporous nanosheets. The ultrathin two-dimensional nanosheets and porous surface characteristics provide the vast channels for electrolyte injection, thus endowing CoNiO2 the outstanding HER performance. The excellent performance with a fewer onset potential of 94 mV, a smaller overpotential at 10 mA cm-2, a lower Tafel slope of 109 mV dec-1 and better stability after 1000 cycles makes CoNiO2 better than that of metallic Co and metallic Ni.