OBJECTIVES: This study sought to identify alterations in electroencephalography (EEG) microstates among adolescents with first-episode and drug-naive major depressive disorder (MDD). Additionally, it aimed to explore the association of EEG microstates with clinical characteristics and patient response to antidepressant treatment over a period of 4 weeks. METHODS: A total of 81 first-episode and drug-naive adolescents with MDD and 60 healthy controls (HCs) were recruited. General demographic information and resting EEG data were collected from all participants. Depression symptoms were evaluated using the Hamilton Depression Scale (HAMD) at baseline and following 4 weeks of antidepressant treatment. The study employed EEG microstates and support vector machine (SVM) techniques for data interpretation. RESULTS: Adolescents with first-episode and drug-naive MDD exhibited a significant reduction in the duration of microstate D and an increase in the occurrence of microstate A compared to the HCs (p < 0.05).When comparing treatment responders and non-responders, treatment responders demonstrated an elevated occurrence and coverage of microstate A and transition probabilities of A-C. Conversely, treatment responders showed decreased occurrence and coverage of microstate B and transition probabilities of BD (all p < 0.05). Upon feature selection, five distinct micro-state parameters were utilized as features. Subsequently, the SVM model demonstrated its capability to distinguish between treatment responders and non-responders, achieving an average accuracy of 75.29 %. Notably, the model's peak performance was characterized by a classification accuracy of 82.35%, accompanied by an AUC of 0.819, a sensitivity of 75.00%, and a specificity of 88.89%. CONCLUSIONS: Microstate A may be associated with the severity of depressive symptoms, while microstate B might serve as a potent predictor of antidepressant response in adolescents with first-episode and drug-naive MDD.
Gliomas are highly heterogeneous brain tumors with metabolic and molecular alterations that drive their progression and aggressiveness. While genomic classifications have improved glioma diagnosis and prognosis prediction, the functional consequences of tumor progression at the protein and metabolite levels remain not fully explored. This study represents an advancement in glioma research by, for the first time, integrating LC-MS-based proteomics and metabolomics with GC-MS-based metabolomics to comprehensively characterize the molecular landscape of glioma tissues. By capturing key molecular changes occurring between these grades, we identify previously unreported alterations in fundamental pathways, offering a more complete perspective on tumor biology beyond the disturbances that have been only partially explored in earlier studies. Proteomic and metabolomic profiling using LC-MS and GC-MS identified alterations in mitochondrial function, metabolic stress responses, and cytoskeletal remodeling, alongside disruptions in amino acid metabolism, glycolysis, and lipid processing. While confirming known metabolic adaptations in gliomas, our findings also identified previously unreported proteins and metabolites, including plasmalogen alterations (LPC P-18:0, LPC O-18:0), and key metabolic enzymes like TKT and ME1. These insights broaden our understanding of glioma progression, highlighting novel biomarkers and potential therapeutic targets through comprehensive analysis of results from both methods.
BACKGROUND: Data regarding the safety and efficacy of balloon expandable valves (BEVs) for transcatheter aortic valve replacement (TAVR) in patients with Sievers type 0 bicuspid aortic valve (BAV) stenosis remain limited. AIMS: This study aims to evaluate the clinical outcomes of BEVs implantation in patients with Sievers type 0 BAV. METHODS: We conducted a multicenter, retrospective study across 28 centers in China between October 2020 and March 2023. Consecutive patients with Sievers type 0 BAV anatomy undergoing TAVR with the Edwards Sapien 3 BEV were enrolled. RESULTS: The study included 131 patients with Sievers type 0 BAV (mean age 69.8 ± 7.5 years; 52.7 % male). The lateral-lateral type predominated (86.3 %). Calcification distribution analysis identified the superior leaflet margin as the most primary site (62.6 %). All procedures utilized femoral artery access. High implantation depth (The ratio of the aortic side of the prosthetic valve to the outflow tract side is > 8:2) was achieved in 80.2 % of cases. Prosthetic valves smaller than 26 mm were implanted in nearly half of the patients (49.6 %). The 30-day all-cause mortality rate was 0.8 %, with no incidence of disabling stroke. The overall technical success rate was 98.5 %. CONCLUSION: The findings of this study demonstrate that BEVs implantation in patients with Sievers type 0 BAV is associated with favorable safety and efficacy outcomes. These results provide valuable insights for current TAVR practice in this specific patient population.
Structurally-engineered hollow carbon nanomaterials have emerged as frontier materials for advanced energy storage technologies, because of their inherent architectural merits, including expansive specific surface area and interconnected porosity, which enable efficient sodium ion storage mechanisms. Hollow carbon shells with flattened circular shapes were prepared using FeO as templates. By precisely tuning the N/S doping ratios, the electronic structure and surface properties of hollow carbon nanomaterials can be effectively modified. The regulatory mechanisms of nitrogen and sulfur synergistic doping on electron/ion transport, structural stability, and sodium ion diffusion kinetics were revealed. Specifically, it reveals that as a sodium-ion half-cell anode, the materials deliver 368.4 mAh g at 200 mA g. Importantly, the full cell battery (Mg-NaVO//NSC-21) achieves 348.9 mAh g at 500 mA g, demonstrating remarkable rate capability which sustains 101.7 mAh g even at 5000 mA g. Characterization studies attribute these improvements to an optimized N/S-doped ratio of 12 can substantially boost sodium storage capabilities via coordinated enhancements in charge transport efficiency, ionic mobility and electrode integrity. This study establishes fundamental guidelines for designing architecturally controlled N/S-coordinated carbon matrices, directly propelling the engineering of high-efficiency sodium-ion batteries (SIBs), opening up new avenues for the development of advanced energy storage systems.
This study synthesizes dual-modified graphitic carbon nitride (CN) through morphological engineering and Na doping, synergistically enhancing visible-light absorption and charge carrier dynamics. A coral-like Na-doped CN (NaCCN) was fabricated via one-step calcination method, leveraging the self-assembly of melamine and cyanuric acid in NaCl solution. This strategy simultaneously improved the electronic structure of the catalyst skeleton, increasing active sites and boosting electron transfer efficiency. Characterization revealed that NaCCN exhibits broadened visible-light utilization, lower photogenerated carrier coincidence rate, and higher electron transfer rate. NaCCN achieved complete tetracycline hydrochloride (TC) degradation in 18 min, with a rate constant of 0.224 min, which is 32 times faster than CN. It maintained high efficiency across TC concentrations (25-200 mg L) and pH (1.6-11), with universal efficacy against multiple antibiotics. Structural integrity and reactivity were preserved over 10 cycles. Additionally, NaCCN inactivated ∼100 % of Escherichia coli, Salmonella typhimurium, and Pseudomonas aeruginosa within 60 min. Mechanistic studies combining band structure analysis, reactive oxygen species (ROS) trapping, and Liquid Chromatograph Mass Spectrometer (LC-MS) identified superoxide radical and photoexcited hole as dominant species, with TC degradation proceeding through hydroxylation, demethylation, and ring-opening steps. The dual modification strategy provides a scalable approach to design robust g-CN-based photocatalysts for environmental remediation.
The microenvironment around the wounds of chronic disease patients often exhibits weakly alkaline conditions, primarily due to defects in the patients' blood glucose regulation, tissue hypoxia, accumulation of metabolic products, and bacterial infection and growth. To regulate the wound microenvironment across a broad pH range, a Fe-doped ZIF-8 nanozyme loaded with glucose oxidase (Fe-ZIF-8@GOx) was synthesized via a one-step in situ growth method. This nanozyme, with ZIF-8 serving both as a protective matrix and immobilization scaffold, enhances the enzyme's operational microenvironment and maintains functionality across a wide pH range. It exhibits the activities of cascade glucose oxidase (GOx), catalase-like (CAT-like), and peroxidase-like (POD-like) enzymes. When Fe-ZIF-8@GOx nanozymes encounter high glucose levels at the site of weakly alkaline chronic ulcers, the GOx particles catalyze the reduction of local pH, simultaneously triggering CAT-like enzyme activity to release O₂ and improve the wound microenvironment. The subsequent pH reduction induces the controlled release of iron ions, enabling Fe to react with endogenously produced hydrogen peroxide to generate reactive oxygen species (ROS), conferring a distinctive guest-carrier synergistic antibacterial effect. Both in vitro and in vivo studies confirm that this material effectively reduces inflammation, modulates macrophage polarization, enhances collagen deposition, and promotes angiogenesis, ultimately accelerating wound healing under chronic diabetic conditions. Thus, our work not only overcomes microenvironmental limitations in antibacterial therapy but also offers a promising strategy for treating chronic diabetic infections.
lithium (Li) metal has emerged as one of the most promising anode materials for next-generation batteries, attracting considerable interest owing to its exceptional high energy density and specific capacity. However, severe volume expansion and dendritic growth during cycling critically hinder the practical application of Li metal anodes. Herein, a hollow carbon sphere-encapsulating cobalt oxide (CoO) core (CoO/CS) framework was fabricated through a layer-by-layer assembly and controlled etching approach, which effectively suppresses dendrite formation in Li metal anodes. Density functional theory (DFT) calculations reveal that the CoO core exhibits significantly higher Li adsorption energy compared to the graphite shell, demonstrating its preferential role in guiding Li deposition. COMSOL Multiphysics simulations demonstrate that the CoO core effectively optimizes the local current density distribution. Consequently, the Li preferentially nucleates at the CoO core due to its lithiophilic character, sequentially filling the hollow carbon sphere's interior volume. The hollow architecture provides abundant nucleation sites and sufficient void space to accommodate deposited Li metal, effectively mitigating volume changes during cycling. The synergistic combination of the hollow carbon structure and lithiophilic CoO core enables exceptional stability (operation exceeding 1700 h). Finally, the full cell capacity of CoO/CS electrode shows significant improvement across various current densities.
Sulfide all-solid-state batteries (ASSBs) using high-capacity silicon (Si) anodes and high‑nickel ternary cathodes offer a promising route to realize high energy density and safety simultaneously. However, the low inherent electronic conductivity of Si constrains its further application in ASSBs. Importing element doping is an available strategy to improve intrinsic electronic conductivity of raw Si anodes. Herein, the effects of N-type (phosphorus doped) and P-type (boron doped) Si anodes were systematically studied in ASSBs. The doping type and doping contents determined the anodic performances. It is unraveled that the doping element with low content will migrate away from the Si matrices during the initial lithiation and amorphization process of the Si anode, forming low conductivity elemental phases. These low conductivity doping elements hinder internal Li migration through Si particles and deteriorate the electrochemical performance. In contrast, the high content element doping remains stable conductive ionic network inside the Si particles. In addition, the N-type Si with phosphorus formed conductive LiP help to increase the lithium utilizations. Therefore, after prelithiation, matching with Li(NiCoMn)O (NCM811) cathode, the capacity retention of the high content doped N-type Si ASSBs is 76.24 % after 100 cycles at 0.5C, whereas the capacity retention of the raw Si ASSBs is only 70.61 %.
氨硼烷(AB,NHBH)具有高储氢容量,使其成为各种储氢材料中的理想候选者。提高活性位点的光学性能和电子密度是通过光催化AB水解实现高效制氢的有效策略。本研究利用磷掺杂(P掺杂)的海胆状二氧化钛(TiO)作为负载铜钴(CuCo)双金属合金纳米颗粒的载体,从而开发出用于AB水解制氢(H)的CuCo/P-TiO光催化剂。在298K下,光照下的产氢速率测得为957mL min g,光照条件下的周转频率(TOF)为28.23min,这比在黑暗中观察到的高出1.45倍。实验表征表明,优异的光催化活性可归因于金属Cu的局域表面等离子体共振(LSPR)效应以及金属-载体(CuCo/P-TiO)相互作用。这些因素的协同作用提高了光学性能,优化了催化剂的电子结构,并有效地调节了Co活性位点的电子密度。这项工作提出了一种实现低成本高效催化AB水解制氢的直接方法。
This study successfully demonstrates a new concept of complementary electrostatic interactions between drugs and nanocarriers. Water-soluble modified chitosan (Na-CMC) has negatively charged carboxylate groups on its side chains and co-assembles with the positively charged anticancer agents rhodamine 6G (R6G) or doxorubicin (DOX). This concept represents a promising facile strategy for the development of efficient, multifunctional drug delivery systems to potentially enable safer, more effective chemotherapy. Due to electrostatic interactions, Na-CMC and R6G (or DOX) can form complexes in aqueous environments and subsequently co-assemble into nanogels. The resulting Na-CMC/R6G nanogels exhibit several excellent and unique physical properties, including high R6G-loading capacity, nearly uniform co-assembled morphology and size, stable intrinsic fluorescence, outstanding structural stability in biological media, sensitive acid-responsive behavior, and controllable pH-triggered drug release. Systematic cellular studies clearly confirmed that the Na-CMC/R6G nanogels were selectively internalized by HeLa cells via stable micropinocytosis and subsequently released R6G in the mildly acidic microenvironment, and thereby induced targeted apoptosis in cancer cells. In contrast, the Na-CMC/DOX nanogels self-aggregated and induced massive levels of necrotic cell death in both normal and cancer cells. Overall, this study clearly demonstrates that the combination of appropriate anticancer agents and stable electrostatic interactions in a bio-based drug delivery system can critically enhance selective internalization and induce programmed cancer cell death.
Simultaneously achieving sensitive detection and efficient degradation of organic pollutants remains a challenging task. Dual-functional MXene@FeO@Ag NPs nanosheets was fabricated via co-precipitation and electrostatic self-assembly techniques to enhance synergistic effect of SERS detction and photo-Fenton catalysis for organic pollutants degradation, respectively. The synergistic interplay of electromagnetic and chemical enhancement was responsible for excellent SERS sensitivity of MXene@FeO@Ag NPs, as confirmed by Finite-difference time-domain (FDTD) simulations. The limit of detection (LOD) of SERS substrates for crystal violet (CV) as low as 1.08 × 10 M. Notably, MXene@FeO@Ag NPs demonstrated high degradation capacity, the degradation rate of CV reached 91.5 % within 40 min, representing an enhancement of 1.77 times compared to FeO alone. The composite's magnetic properties also facilitated easy recovery and reuse, with the material maintaining its outstanding SERS sensitivity even after eight cycles, and sustaining strong photocatalytic performance after three cycles. The enhancement mechanism of SERS and the interpretation of catalytic phenomena provide promising guidance for providing a low-cost and stable composite SERS platform in the detection and treatment of emerging contaminants.

由于吡咯衍生物频繁出现在生物活性化合物中,它们在药物化学领域是一种具有优势的骨架结构。在此,我们报道了基于汉茨希吡咯合成法,采用混合-均分策略固相合成一个由211种吡咯衍生物组成的组合库。使用人淋巴母细胞系P493-6(一种受Myc调控生长的模型)对混合化合物进行细胞增殖测定评估。四个混合物表现出显著的抑制活性,随后对16种单个吡咯衍生物进行反卷积和合成,从而鉴定出几种具有强效抗增殖特性的化合物。
Based on findings from analyses with cross-lagged panel models, Gonçalves-Pereira et al. (2025) suggested causal effects of sense of coherence (SOC) on subjective burden, anxiety, and depression among family caregivers. Here, we simulated data to resemble the data used by Gonçalves-Pereira et al. We used triangulation and fitted complementary models to the simulated data and found contradicting increasing, decreasing, and null effects of initial sense of coherence on subsequent change in subjective burden and mental health. These divergent findings indicated that it is premature to assume causal effects of sense of coherence on subjective burden and mental health and the suggestions by Gonçalves-Pereira et al. in this regard can be challenged. It is important for researchers to be aware that correlations, including adjusted cross-lagged effects, do not prove causality in order not to overinterpret findings, something that appears to have happened to Gonçalves-Pereira et al. We recommend researchers to triangulate by fitting complementary models to their data in order to evaluate if analyzed data could be used to support contradicting conclusions, in which case the data should not be used to support any of those conclusions.
The hydrogenation of phenolic compounds to achieve high value-added conversion is an important reaction in industrial applications. Promoting the hydrogenation process by regulating the properties of H active species has great potential. In this paper, we achieved in-situ metal doping using the one-pot hydrothermal strategy to regulate the cleavage pathway of H on the surface of noble metals, thereby promoting the hydrogenation of phenol to form ketones. The results of catalytic performance, characterization and density functional theory (DFT) calculations confirmed that the Co doping regulated the surface properties of Pd metal, leading to easier heterolytic cleavage of H to form electron-rich highly active H species. Mechanistic studies showed that the modified metal surface was more favorable for the adsorption and activation of H, and the electron-rich H species could lower the hydrogenation barrier and promote the progress of the hydrogenation process. In addition, this strategy achieved the highly stable materials with core-shell via one-step synthesis, which showed good stability in continuous use. Our study presents a successful paradigm in biomass conversion, deepening the understanding of the regulation of hydrogenation processes.
BACKGROUND: Prenatal anxiety and depression have been linked to adverse childhood neurodevelopment, potentially through cortisol-induced epigenetic changes. Postpartum depression is also associated with neurodevelopmental delays, possibly via altered parental attachment. While prenatal and postpartum mental health may be correlated, their relative and independent impacts on offspring neurodevelopment remain unclear. This study examines the effects of prenatal and postpartum anxiety and/or depression on neurodevelopmental delay at 24 months. METHODS: In a nationwide prospective cohort from the "Assessing the Safety of Pregnancy in the Coronavirus Pandemic" study, prenatal anxiety (GAD-7), prenatal depression (PHQ-9), and six-week postpartum depression (EPDS) were assessed. Childhood neurodevelopment was measured using the Ages and Stages Questionnaire, 3rd edition (ASQ-3). Logistic regression tested associations between moderate-to-severe maternal anxiety/depression and neurodevelopmental delay, adjusting for participant age, education, household income, and residential density. Alcohol, nicotine, anxiety/depression medication use during pregnancy, and preterm birth were considered as moderators/mediators. RESULTS: Offspring of participants experiencing both prenatal and postpartum moderate-to-severe anxiety or depression (N = 62) had a higher risk of neurodevelopmental delay at 24 months compared to those who experienced neither (N = 1060) with an adjusted risk ratio of 1.88 (p < 0.001). While delay risk was higher in offspring of those with only prenatal (N = 218) or postpartum (N = 45) anxiety/depression, these were not statistically significant. CONCLUSION: Having both moderate-to-severe prenatal and postpartum anxiety or depression independently increased the risk of developmental delay at 24 months, even after adjusting for confounders. Further research is needed to explore underlying mechanisms linking maternal mental health and fetal neurodevelopment.
Ammonia decomposition is a promising strategy to address critical challenges in hydrogen storage and transportation, thereby facilitating the widespread adoption of fuel-cell technologies. However, conventional catalytic require harsh conditions (600 °C) for complete conversion. In this study, we report nanocluster Ru/CeO and Ni/CeO catalysts integrated with electric field-assisted catalysis to achieve efficient ammonia decomposition under significantly milder conditions (≤400 °C). With electric field, Ru/CeO and Ni/CeO achieve 100 % and 60 % conversion at 400 °C, and maintain 62 % and 15 % conversion even at 150 °C accompanied by substantial reductions in activation energy (79.5 % and 78.9 %, respectively). Long-term stability tests reveal minimal activity loss (<3 %) over 48 h. Mechanistic studies show that the electric field promotes the formation of Ru-O-Ce bonds, thereby enhancing the strong metal-support interaction (SMSI). This facilitates electron transfer from CeO to the metal site, enhancing NH adsorption and activation, while weakening the interaction between metal and N to promote N desorption. Additionally, electric field-induced proton hopping accelerates hydrogen spillover and suppresses hydrogen poisoning. This work provides a new approach for low temperature, high efficiency ammonia decomposition, offering a viable path for next-generation hydrogen energy infrastructure.
The practical implementation of wearable sensing devices for human health monitoring requires significant advancements in lightweight design and multifunctional integration. Fiber-shaped sensors have attracted considerable research attention due to their ability to maintain exceptional sensitivity and measurement accuracy under various mechanical deformations, including bending, stretching, and torsion. Nevertheless, the functional integration remains constrained, particularly as evidenced by sensitivity degradation and device failure under extreme high-temperature conditions, which severely hinders their practical applicability for real-time health monitoring applications in complex environmental scenarios. Herein, we developed a core-sheath aerogel fibrous multifunctional sensor via a one-step coaxial wet-spinning technique. This sensor integrates humidity sensing capabilities for respiratory monitoring and liquid molecule recognition, along with high-temperature-resistant pressure sensing performance. The fiber-based humidity sensor demonstrates rapid response and ultrahigh sensitivity (3144.74 %/% RH) with excellent repeatability. Beyond enabling real-time respiratory detection, the ANFs@MXene/PVA (AMP) humidity sensor responds effectively to non-contact humidity stimuli and discriminates diverse liquid molecules, showcasing its potential for both contact and non-contact environmental sensing in complex scenarios. Additionally, the aramid nanofiber-based sheath enhances the stability of the fiber sensor as a wearable electronic device under extreme conditions, ensuring its functionality in high-temperature environments. This intelligent core-sheath fiber architecture offers a robust solution for real-time health monitoring in harsh environments, demonstrating significant potential for applications in smart textiles.
BACKGROUND: Attention-Deficit/Hyperactivity Disorder (ADHD) is characterized by impairments in executive functioning, particularly response inhibition (RI). This study combines time-domain analysis and source analyses of event-related potentials (ERPs) to explore the underlying neuropsychological mechanisms of RI deficits in unmedicated youth with ADHD, and assesses ERP features as potential biomarkers to differentiate ADHD from healthy controls (HCs). METHODS: The study included 52 unmedicated youth with ADHD (ages 6-12) and 53 HCs. ERPs were recorded using an oddball paradigm, followed by within- and between-group comparisons. Source localization analysis examined regional brain activation during task performance. Significant ERP features were then used in a machine learning classification model. RESULTS: Compared to HCs, youth with ADHD exhibited prolonged mismatch negativity (MMN) latency at frontal (Fz) and posterior (Pz) electrodes, and reduced latency at the central (Cz) electrode. Source analysis indicated increased activation in the cuneus and superior temporal gyrus during the MMN-deviant condition, and enhanced activation in the superior parietal lobules, inferior frontal gyrus, and rectal gyrus during the MMN-novelty condition. Additionally, ADHD patients showed higher activation in the middle temporal and middle occipital gyri during the P300-target condition, and increased activation in the superior frontal gyrus and cuneus during the P300-non-target condition. Notably, the classification model achieved an area under curve (AUC) of 0.918 using MMN latency features. CONCLUSION: Abnormal ERP patterns in unmedicated youth with ADHD may reflect impaired RI and have potential as neurobiological markers for the disorder.
Advanced flexible CoSe@carbon fibers (CoSe@CNFs) were synthesized through electrospinning and sintering processes, with the aim of being applied to high rate and long cycle stability of sodium ion batteries (SIBs) and lithium‑sulfur batteries (LSBs). CNFs interconnect ultrafine CoSe particles to form a coating structure, and the fibers intertwine to create a self-standing three-dimensional network. This not only helps to store electrons in electrochemical reactions but also facilitates the adsorption and desorption of Na/S species. Therefore, when directly used as an anode for SIBs, the electrode has a reversible capacity of 202.1 mAh g after 3000 cycles at a current density of 10 Ag. The microstructure changes of CoSe during the charging and discharging process were investigated in detail by TEM, and the results showed that the crystal form of CoSe changed from long range-order transforms into short-range disorder after sodiated. In addition, the electrocatalytic advantages of flexible electrodes as catalysts for lithium polysulfides can be easily demonstrated through catalytic experiments. Leveraging the morphology and inherent advantages of CoSe, the flexible CoSe@CNFs electrode demonstrates a reversible capacity of 566.8 mAh g at 5 C after 1500 cycles. Most importantly, the morphology of CoSe after the electrochemical reaction was carefully investigated, demonstrating its consistency before and after the electrocatalytic reaction. Flexible CoSe@CNFs provide diversity for the development of high rate performance SIBs and long cycle stability LSBs, and promote a deeper understanding of their morphological evolution during electrochemical reactions.
INTRODUCTION: Little research has focused on adjustment disorder (AjD) in the UK military despite being a frequently reported psychological diagnosis. The study aimed to report prevalence estimates for probable AjD in UK serving and ex-serving personnel and explore associations between stressors and risk factors for probable AjD. METHODS: Data from the King's Centre for Military Health Research (KCMHR) Health and Wellbeing study was used. The KCMHR study investigated health and wellbeing outcomes for UK personnel deployed to Iraq/Afghanistan. Data from the third phase (2014-2016) were used (n = 4656); serving personnel (n = 1999) and ex-serving personnel (n = 2657). RESULTS: A probable AjD prevalence of 6.0 % for serving personnel (95 % CI: 4.9 % - 7.5 %) and 7.1 % for ex-serving personnel (95 % CI: 6.0 % - 8.3 %) was identified. Relationship dissatisfaction and financial difficulties had the strongest association with probable AjD. Being in a combat role and being single were positively associated with AjD, while senior rank was protective. Childhood adversities and externalising behaviours were associated with adult AjD. Risk factors differed depending on serving status. LIMITATIONS: Several established mental health measures were used to identify probable AjD opposed to the 'gold-standard' screening tool, of which the development was too late to include in the study. CONCLUSION: The findings provide foundational knowledge of AjD for the UK military. In addition to military-specific factors, non-military stressors and risk factors were identified, which mapped onto those seen in the general population. Further exploration is recommended to understand AjD differences between civilian and military populations.
炎症性肠病(IBD)是一种慢性免疫介导的疾病,其特征为肠道炎症,常进展为包括肠道狭窄、梗阻和穿孔在内的并发症。IBD 中持续的炎症负担和胃肠道出血最终导致全身性铁缺乏,使患者易患缺铁性贫血(IDA)。在此,我们报告一种经过合理设计的纳米酶,白芍多糖 - 铁复合物(PPFeCs),其设计目的是将超氧化物歧化酶/过氧化氢酶模拟抗氧化酶活性与可生物利用的铁递送相结合,以同时治疗 IBD 及其 IDA 合并症。实验结果表明,PPFeCs 减轻了葡聚糖硫酸钠诱导的结肠炎症,通过上调紧密连接蛋白增强上皮屏障完整性,并通过恢复血红蛋白水平改善全身性铁缺乏,从而证实了它们治疗 IBD - IDA 合并症的治疗潜力。从机制上讲,PPFeCs 通过磷酸肌醇 3 - 激酶/蛋白激酶 B(PI3K/Akt)途径调节,将糖酵解与氧化磷酸化之间的平衡转移,从而重新编程巨噬细胞葡萄糖代谢。这种代谢转换与核因子 - κB(NF - κB)信号抑制协同作用,驱动巨噬细胞从促炎性 M1 表型向抗炎性 M2 表型极化,从而打破炎症和氧化应激的恶性循环。我们的研究结果不仅阐明了 PPFeCs 的多方面治疗机制,也为开发用于治疗 IBD 及其相关并发症的多糖 - 金属基纳米酶奠定了基础。
背景:睡眠障碍,包括日间嗜睡(DS)、失眠和睡眠呼吸暂停(SA),已与衰老相关表型相关联,但其因果作用仍不清楚。本研究旨在使用孟德尔随机化(MR)方法研究这些睡眠特征对生物衰老的潜在因果效应。 方法:我们使用来自大规模全基因组关联研究(GWAS)的基因工具对DS、失眠和SA进行了两样本MR分析。逆方差加权(IVW)方法是主要分析方法,并进行了敏感性分析以进行验证。与衰老相关的结果包括内在表观遗传年龄加速(IEAA)、GrimAge、HannumAge、PhenoAge、端粒长度、面部衰老、衰弱指数和认知表现。对多重检验应用了错误发现率(FDR)校正。 结果:DS与衰弱指数增加显著相关(β = 0.33,95%CI:0.09 - 0.57,PFDR = 0.045)。失眠与IEAA(β = 1.57,95%CI:0.40 - 2.73,PFDR = 0.035)和衰弱指数(β = 0.42,95%CI:0.23 - 0.61,PFDR <0.001)均显著相关。SA与面部衰老(β = 0.03,95%CI:0.01 - 0.06,PFDR = 0.016)和衰弱指数(β = 0.09,95%CI:0.02 - 0.16,PFDR = 0.028)显著相关。未发现端粒长度、GrimAge、PhenoAge或认知表现有显著关联。 结论:这项MR研究支持失眠对表观遗传衰老和衰弱的潜在因果效应。DS和SA也与衰弱增加有关,并且SA还与面部衰老有关。这些发现强调了睡眠健康在减轻与年龄相关的生物衰退中的重要性。
Precise delivery of antitumor drugs has become a research focus in cancer treatment. Herein, we developed a bovine serum albumin (BSA) modified carbon dots (CDs) and berberine (BBR) composite for improved intravenous BBR delivery. The surface-negatively charged CDs can associate with positively charged BBR through electrostatic interactions, resulting in CDs and BBR composite (BBR@CDs). BBR@CDs can be further stabilized by modification with BSA, resulting in enlarged composite (BSA@BBR@CDs) with much better water solubility. In vitro, with BSA modification, BSA@BBR@CDs was more readily taken up by tumor cells than BBR@CDs. After entering cells, BSA@BBR@CDs could more efficiently target mitochondria, resulting in mitochondrial dysfunction and eventually showing a stronger pro-apoptotic effect on tumor cells than BBR. In vivo, BSA@BBR@CDs can well accumulate in tumors via intravenous injection and significantly inhibit the tumor growth without significant toxicity to other organs. Therefore, BSA@BBR@CDs holds potential as a promising nanomedicine for cancer therapy.
Reactive oxygen species (ROS) play a fundamental role in antibacterial therapeutic strategies. However, excessive ROS generation can disrupt redox homeostasis and induce a severe inflammatory response, causing immense stress on surrounding cells and tissues. Herein, an intelligent nanoheterojunction established with Prussian blue (PB) and manganese polyphthalocyanine (MnPPc), PB@MnPPc (PM), was established to achieve sequential antibacterial and anti-inflammatory functions via controllable ROS regulation. With spatiotemporal control of near-infrared (NIR, 808 nm) light, PM demonstrates the potential for on-demand generation and scavenging of ROS. When exposed to NIR irradiation, PM exhibits prominent bactericidal abilities, which result from its augmented singlet oxygen generation capacity and photothermal effects. These advantages originate from the narrow band gap as well as the enhanced electron-hole separation and transfer efficiency enabled by its unique heterostructure. Upon cessation of NIR irradiation, PM efficiently achieves ROS elimination and inflammation alleviation through its superior superoxide dismutase-like and catalase-like activities. In vivo studies in a mouse Staphylococcus aureus-infected skin wound model further confirmed the superior therapeutic effects of PM, which effectively eliminated bacteria, relieved inflammation, promoted collagen deposition, and angiogenesis. This work provides an attractive therapeutic modality for equipping nanoheterojunctions with antibacterial and anti-inflammatory properties through programmed ROS regulation.
Autologous tumor cells demonstrate considerable promise as individualized therapeutic vaccines owing to their endogenous neoantigen repertoire. Nevertheless, their suboptimal immunogenicity substantially impedes clinical translation. Herein, we engineered an innovative whole tumor cell vaccine platform utilizing photothermal CuSe nanoparticles, which encapsulate comprehensive tumor-associated antigens and intrinsic immunostimulatory molecules to elicit a polyvalent antitumor immune response. In this work, CuSe was applied to prepare the whole tumor cell vaccine for the first time. As a pyroptosis inducer, CuSe triggered the expression of damage-associated molecular patterns (DAMPs) as endogenous adjuvants in 4T1 cells (mouse breast cancer cells) under near-infrared (NIR) irradiation. Repeated freeze-thaw cycles inactivated and lysed CuSe-loaded 4T1 cells, releasing DAMPs for laser-activated CuSe-based whole tumor cell vaccine (LC-TCV) preparation. Mild photothermal therapy (PTT) at the vaccination site by NIR irradiation effectively suppressed tumor growth. This efficacy was primarily attributed to the synergistic effects of multiple natural antigens and adjuvants in LC-TCV, which promoted dendritic cells (DCs) maturation and subsequent immune activation. Consequently, it potentiates the recruitment of cytotoxic T lymphocytes, elicits immunogenic cell death (ICD), and consequently initiates a potent antigen-specific immune cascade. Collectively, this study presents an innovative approach to unleash the potential of personalized whole tumor cell vaccines in cancer therapy.
Lithium-ion batteries will inevitably undergo aging during long-term use. Especially under the condition of overcharged electrical abuse, the electrolyte decomposes to produce a series of aging products. In this paper, 2,5-dioxahexanedioic acid dimethyl ester (DMDOHC) is taken as an example to explore the relationship between the substance and the battery electrochemical aging process under overcharge conditions based on Raman spectroscopy. Firstly, establish a Raman detection platform and prepare electrolyte samples with different concentrations of DMDOHC. Select characteristic peaks through Raman detection for subsequent analysis. On this basis, a LiFePO battery simulation device is used as the experimental basis to conduct cycling experiments on lithium-ion batteries under different charge cut-off potentials and cycle periods. It is found that with the increase of the cut-off voltage, the content of DMDOHC increased (from 144.07 ppm at 3.8 V to 553.28 ppm at 4.4 V), and the capacity decay rate of the battery is accelerated. There is also a positive correlation between the content of DMDOHC and the number of battery cycles, and the DMDOHC content shows the most significant growth at 4.4 V. The experimental results show that the concentration of DMDOHC can be used as an indicator of the battery aging process, which provides a theoretical basis for further health status evaluation of lithium-ion batteries.
The rapid development of flexible electronics resulted in a surge in the generation of e-waste, which stimulated a strong demand for environmentally friendly polymer substrates. Developing mechanically robust and recyclable polymer substrates is a promising approach, but remains an ongoing challenge due to the conflict in intrinsic mechanisms of that the weak noncovalent bonds required for recyclability resulting in poor mechanical strength. Herein, we design a dynamic hard domains strategy to develop a cellulose/castor oil-derived fully bio-based thermoset elastomer with excellent mechanical robustness, recyclability, and biodegradation performance for flexible electronic substrates. The construction of the phase separated structure realizes high strength (25.6 MPa), and toughness (43.5 MJ/m), while the reconfigurability of the dynamic hard domains achieves excellent recyclability with a high mechanical strength retention rate of 88.2 %. Impressively, the bio-based thermoset elastomer can be completely degraded by being buried in the soil for 70 days. Given these features, the bio-based thermoset elastomers are employed as an environmentally friendly substrate for the preparation of printable capacitive sensors (PCSs). The PCSs exhibit robust capacitive sensing performance in both contact or non-contact modes for detecting multiple signals, including pressure, orientation, humidity, and respiration. This work promotes the development of environmentally friendly bio-based polymeric substrates for addressing the growing e-waste problem in flexible electronics.
极端温度条件常常会加速超级电容器材料的降解并提高电解质电阻,从而缩短器件的使用寿命和可靠性。进行有效的温度调节对于确保超级电容器能够在恶劣环境条件下稳定工作是必要的。为了克服这些挑战,我们引入了一种具有核壳结构且相变温度范围为双温区的相变纤维薄膜,它是采用先进的逐层同轴静电纺丝技术制备而成的。该薄膜在真空镀上金层后用作聚苯胺纳米阵列原位聚合的基底,以制备具有PVA/HSO凝胶电解质的柔性超级电容器。独特的针状聚苯胺纳米阵列增加了表面积和离子传输通道,使得器件在5 mV s的扫描速率下面积电容达到521.3 mF cm 。我们的相变纤维在0至10°C和40至50°C范围内具有62.4 J g的高潜热,可实现高效的温度调节。在两个相变区域内稳定的电容和内阻突出了该器件强大的热调节能力。这一进展代表了柔性超级电容器向前迈出的重要一步,为未来的储能应用提供了更好的热管理和巨大潜力。
本研究旨在揭示金疸化瘀颗粒对急性肝衰竭(ALF)拮抗作用的潜在调控机制。通过观察肝组织切片的苏木精-伊红染色以及检测大鼠血清中天冬氨酸转氨酶(AST)、丙氨酸转氨酶(ALT)和总胆红素(TBIL)水平,评估金疸化瘀颗粒的抗炎作用。采用无标记定量蛋白质组学和非靶向代谢组学技术,评估ALF大鼠在金疸化瘀颗粒治疗前后肝组织中的蛋白质和代谢物变化。对差异表达蛋白(DEPs)和代谢物(DEMs)进行鉴定并进行生物信息学分析。金疸化瘀颗粒可减轻肝组织的病理变化,降低ALF大鼠血清中ALT、AST和TBIL水平。蛋白质组学结果表明,模型组和金疸化瘀颗粒组共有303个DEPs,这些蛋白主要富集在磷脂酰肌醇-3激酶-蛋白激酶B(PI3K-Akt)信号通路、糖酵解和糖异生等通路中。代谢组学分析确定模型组和金疸化瘀颗粒组之间有31个DEMs。这些代谢物主要富集在糖酵解和糖异生等通路中。蛋白质组学和代谢组学的联合富集分析显示,DEPs和DEMs在糖酵解和糖异生等通路中显著富集。此外,平行反应监测验证了ALF肝脏中常见DEPs的平行变化,其表达变化与蛋白质组学分析一致。金疸化瘀颗粒对ALF的治疗作用可能涉及激活PI3K-AKT通路和抑制肝脏糖酵解,从而减轻肝脏炎症应激。
尽管铈基金属有机框架材料(MOFs)相较于MOF家族中的其他材料展现出卓越的光催化性能,但它们仍未达到必要标准。通过将改性策略与贵金属钯相结合,该材料的光催化性能得到显著增强,进一步提升了钯改性铈基金属有机框架的性能。在此,我们展示了一种新型的三维钯卟啉铈基金属有机框架(Pd-Ce PMOFs),其通过稳定的N-Pd配位键均匀地包裹钯。这种方法有效解决了钯改性光催化剂中常见的分散不均和稳定性问题。优化后的Pd-Ce PMOFs在二氧化碳还原方面表现出优异的光催化性能,CO产率达到191.24±3μmol g⁻¹ h⁻¹,是原始Ce PMOFs的3.81倍,选择性为98.13%。密度泛函理论(DFT)计算表明,钯作为二氧化碳吸附及其催化活化的双活性位点。这一过程将形成*COOH中间体的能垒降低至1.59 eV,并促进了有效的载流子迁移。这项工作不仅开创了一种稳定的三维Ce-Pd PMOFs结构,还推动了钯配位改性的应用,从而推进了基于MOF的高性能光催化剂用于可持续CO₂转化的合理设计。
已开发出一种选择性气相色谱-轨道阱方法,用于分析四类不同口服液体制剂中的乙二醇(EG)和二甘醇(DEG):西药(WM)、传统药物(TM)、保健品(HS)和中成药(CM)。在负离子模式下,使用甲烷气将这些二醇化学离子化,生成各自的去质子化离子,并通过靶向选择离子监测(t-SIM)进行分析,质量误差窗口保持在±5 ppm。使用浓度范围为5至100 μg/mL的基质辅助标准溶液进行内标校正,以1,4-丁二醇-2,2,3,3-D作为内标(IS)。两种二醇的检测限和定量限(分别为1.0 μg/mL和3.0 μg/mL)与使用气相色谱-串联三重四极杆质谱仪(GC-MS/MS)时分别获得的0.4 μg/mL和1.0 μg/mL相当。结果表明,大多数样品不含EG和DEG。检测到的痕量EG和/或DEG低于0.1% w/w的安全限值。该方法不仅解决了先前气相色谱-火焰离子化检测(GC-FID)中遇到的假阳性识别问题,而且如本研究所示,在不同样品基质(如口腔凝胶)中也具有更广泛的适用性。
开发用于氧还原反应(ORR)和析氧反应(OER)的高效双功能电催化剂是能量转换和存储技术的一个基本前提。这项工作通过密度泛函理论(DFT)方法系统地研究了负载在锑烯两个不同位点上的一系列过渡金属(TM = Mn、Fe、Co、Ni、Cu、Ru、Rh、Pd、Ag、Re、Os、Ir、Pt、Au)作为ORR/OER双功能电催化剂的潜力。对于ORR,计算结果表明I-Ag-Sb、II-Pt-Sb和II-Pd-Sb具有最佳的ORR活性,它们的过电位值分别为0.41、0.43和0.42V。对于OER,I-Pd-Sb的过电位值为0.38V,具有最佳的OER性能。值得注意的是,I-Pd-Sb的电位间隙值为0.92V,显示出无可挑剔的双功能催化活性。最后,电子结构分析也有效地证明了中间体的吸附行为会影响其催化活性。该研究为锑单原子催化剂作为双功能电催化剂提供了重要的理论指导。
二维共轭金属有机框架(2D c-MOFs)因其高孔隙率、优异的比表面积、高度可调的化学性质和出色的导电性,在神经形态领域具有巨大潜力。在此,采用逐层自组装方法制备了基于Cu(HHTP)薄膜的两终端光电突触。该器件展现出出色的突触功能,包括双脉冲易化(PPF)、脉冲宽度依赖可塑性(SWDP)和脉冲速率依赖可塑性(SRDP)。此外,Cu(HHTP)薄膜在可见光范围内的广泛吸收使该器件具有广泛的光谱响应,这对于实现颜色区分和联想记忆至关重要。最终,基于神经形态语音识别系统的模拟揭示了该器件实现高语音数字识别准确率的能力,即使在嘈杂环境下也能保持稳健性能。这些结果凸显了基于Cu(HHTP)的光电突触作为利用MOFs独特性质的下一代神经计算有前景平台的潜力。
甘草酸(GA)作为一种天然存在的皂苷生物表面活性剂,由于其分级自组装行为以及生物利用度、生物相容性和生物降解性等优点,已被广泛用于构建超分子功能材料。然而,其在溶液中刺激响应性自组装的潜在机制,这对于设计先进结构至关重要,仍不清楚。在本研究中,我们结合一系列显微镜技术、小角X射线散射、核磁共振、等温滴定量热法和分子动力学模拟,研究了GA在pH值为2至8的水溶液中的自组装行为。我们提出了一个GA组装的综合模型:(1)在pH值约为4时,一个羧基去质子化,GA形成纳米纤维,由三萜部分之间的横向疏水相互作用稳定,其中二葡糖醛酸单元形成外壳并提供有助于纤维稳定的静电排斥力;(2)在pH值低于4时,羧基的完全质子化使外壳中和,导致静电排斥力降低,GA纳米纤维的氢键聚集增强,形成更粗的纤维束;(3)在pH值高于5时,随着两个或三个羧基去质子化,GA纳米纤维解体并重新组装成球形聚集体。在这个阶段,静电排斥削弱了横向疏水相互作用,导致三萜核心松散堆积,二葡糖醛酸外壳暴露于水中。特别是在pH值高于8时,GA主要以单体形式存在。这些发现表明,GA自组装受氢键、疏水和静电相互作用的pH调节相互作用控制,通过其羧基解离程度进行调节。
临床研究表明,许多传统中药不仅具有抗病毒作用,而且在缓解2019冠状病毒病(COVID-19)临床症状方面也有疗效。然而,其抗COVID-19疗效的药理活性成分仍不清楚。本研究旨在建立一种从临床用于治疗COVID-19的草药中鉴定活性成分的新策略。开发了一种将数据挖掘与亲和超滤(AUF)相结合的综合方法。首先,采用数据挖掘策略,从临床用于治疗COVID-19的草药中筛选出高频草药。此外,利用AUF技术从高频草药中筛选潜在的生物活性成分。通过酶活性测定和分子对接评估活性化合物的抗COVID-19潜力,随后在细胞和动物模型中进行验证。数据挖掘显示,甘草、金银花和连翘是治疗COVID-19常用的高频草药。通过AUF从这三种草药中筛选出5种潜在的3-糜蛋白酶样蛋白酶(3CL)抑制剂,并使用高分辨率质谱进行鉴定。进一步的酶学和细胞试验表明,甘草查尔酮C(LCC)和连翘酯苷A(FTA)在微摩尔浓度下可抑制严重急性呼吸综合征冠状病毒2(SARS-CoV-2)的复制。值得注意的是,FTA治疗显著抑制了SARS-CoV-2核衣壳蛋白诱导的小鼠肺部参数和炎症介质的升高。总之,本研究提出了一种将数据挖掘与AUF相结合的新策略,以从中药中发现活性化合物。两种成分,LCC和FTA,被确定为体外SARS-CoV-2奥密克戎毒株复制的剂量依赖性抑制剂。
伤口敷料是保护伤口免受细菌污染和破坏所引发并发症的重要屏障。理想的伤口敷料应具备多种协同治疗特性,包括强大的抗菌活性、促进细胞迁移和增殖的能力,以及生物相容性和成本效益。在此,报道了一种高效的伤口敷料,它由聚离子液体基复合凝胶(ZA凝胶)制成,其中掺入了聚乙二醇包覆的氧化锌和金纳米颗粒(ZA-PEG)。在这种复合水凝胶中,ZA-PEG不仅通过产生活性氧(ROS)增强了离子液体水凝胶的抗菌功效,还通过提供电刺激来加速伤口愈合——这种效果归因于超声照射下氧化锌的压电特性。此外,所设计的复合水凝胶具有更大的孔结构,这增加了其肿胀能力以改善渗出液吸附,并加快释放的锌离子向伤口部位的输送,从而促进结缔组织形成和上皮再生。对小鼠全层皮肤缺损的测试进一步验证了ZA凝胶伤口敷料卓越的伤口愈合能力。这项工作拓宽了离子液体在伤口治疗中的潜在应用,展示了在对抗细菌感染和促进组织修复方面的广阔前景。
二羟基化维生素D(VD)的生物活性最强的形式是1α,25-二羟基维生素D(1α,25(OH)D),它参与各种生理过程和疾病发展。因此,准确量化1α,25(OH)D对于临床诊断、VD相关疾病管理和感染控制至关重要。然而,由于生物样品中1α,25(OH)D浓度低且受其他二羟基化VD代谢物干扰,对其进行量化具有挑战性。在本研究中,我们开发了一种用于1α,25(OH)D量化的新型检测方法,该方法基于液相色谱-串联质谱(LC-MS/MS),结合蛋白质沉淀、固相萃取(SPE)以及用14-(4-二甲基氨基苯基)-9-苯基-9,10-二氢-9,10-[1,2]环三氮唑蒽-13,15-二酮(DAP-PA)对VD代谢物进行衍生化。在衍生化过程中,以1:1比例获得的1α,25(OH)D的6R和6S异构体通过五氟苯基-十八烷基甲硅烷基混合模式柱进行定量分离和检测。该方法能够将1α,25(OH)D与其他二羟基化VD完全分离,包括1β,25-二羟基维生素D(1β,25(OH)D)、3-表-1α,25-二羟基维生素D(3-表-1α,25(OH)D)、2α,25-二羟基维生素D(2α,25(OH)D)、2β,25-二羟基维生素D(2β,25(OH)D)、4α,25-二羟基维生素D(4α,25(OH)D)和4β,25-二羟基维生素D(4β,25(OH)D)。为了证明这种优化方法的适用性,我们分析了人血清,并将结果与一种广泛使用的基于免疫亲和萃取的1α,25(OH)D的LC-MS/MS检测方法进行比较,结果显示定量值相当。优化后的LC-MS/MS方法运行时间为7.7分钟,使用100µL样品血清体积时定量下限为2.5 pg/mL。该方法具有高灵敏度、高精度且能够进行高通量分析,为准确量化1α,25(OH)D提供了一种强大的方法,同时有效分离干扰性二羟基化VD异构体。
由过氧化氢(H₂O₂)燃料驱动的微纳马达(MNMs)在有机污染物的灵敏比色检测和快速催化降解方面引起了广泛关注。然而,它们的实际应用仍然受到多种限制,包括对高浓度有毒H₂O₂的需求、缓慢的Fe²⁺/Fe³⁺氧化还原循环以及金属离子浸出带来的二次污染风险。在此,我们以木棉衍生的C微管为模板,通过多步制备合理开发了一种新型磁性管状FeCu@NC/MnO微马达。该微马达在0.5 M过碳酸钠(SPC)溶液和磁引导下表现出显著的推进力(126.47 μm s⁻¹),通过用固体SPC替代不稳定的液态H₂O₂实现了环保型燃料利用。得益于丰富的活性位点和氧空位(Ov),该微马达在SPC活化方面具有双重功能,既能进行灵敏的比色检测(检测限 = 0.214 μM),又能高效催化降解四环素(TC,90分钟内去除率达93.73%)。猝灭实验和电子顺磁共振(EPR)揭示了TC降解过程中涉及羟基自由基(•OH)和单线态氧(¹O₂)的自由基和非自由基途径。更重要的是,Ov介导的电子转移促进了Cu²⁺/Cu⁺、Fe³⁺/Fe²⁺和Mn⁴⁺/Mn²⁺的氧化还原循环,而Ov与溶解氧(DO)的协同相互作用促进了活性氧(ROS,•OH → ¹O₂ → ²O₂)的生成和转化。本研究为Ov和DO介导的ROS生成/转化机制提供了基本见解,并为环境修复中设计缺陷工程微马达提供了范例。
聚对苯二甲酸乙二酯(PET)塑料的广泛且无控制的处置带来了重大的环境挑战。在本研究中,我们提出了一种可持续的升级循环策略,通过一锅溶剂热法将废弃PET转化为高价值的双金属镍/钴-1,4-苯二甲酸金属有机框架(NiCo-BDC MOFs)。通过调节Ni/Co前驱体比例,所得NiCo-BDC的形态可控制地从堆叠纳米线转变为纳米棒,形成具有大比表面积和发达分级孔隙率的混合晶体-非晶结构。在合成材料中,NiCo-BDC表现出优异的电化学性能,在2 A g时的比电容为949 F g,在20 A g时保持820 F g。当与生物质衍生的纳米碳组装成不对称超级电容器时,该器件在1613 W kg的功率密度下实现了22 Wh kg的能量密度,在10 A g下5000次循环中电容保持率为83%。值得注意的是,这种升级循环方法对各种类型的PET废料都具有广泛的适应性,提供了一个将塑料增值与开发用于下一代储能系统的高性能电极材料相结合的通用平台。
设计特定的电活性位点并调节共价有机框架(COF)的局部微环境以实现电化学CO还原(ECR)已受到越来越多的关注。然而,活性位点电子态的调整所引起的分子内电子转移能力变化对氧化还原介导的催化过程的潜在影响仍未得到充分理解。在这项工作中,我们通过席夫碱缩合反应,以[四(4-甲酰基苯基)卟啉]钴(CoTFPP)和联苯胺(BD)作为前体,构建了一种基于金属卟啉的COF,它是代表性COF-367-Co的异构体,具有相同的化学成分,但亚胺连接方向相反,记为CoTFPP-BD-COF,以专门研究连接方向作为增强电子传输效率以实现ECR的单个变量。在600 mV的宽电位范围内,CoTFPP-BD-COF表现出令人印象深刻的高于90%的CO法拉第效率(FE),远高于基准COF-367-Co(低于50%)。实验和计算结果共同表明,与异构体COF-367-Co相比,CoTFPP-BD-COF中亚胺连接方向的反转不仅通过调整其电子构型增强了钴卟啉中活性中心的CO吸附能力,还通过抑制其电子供体效应促进了分子内定向电子转移,从而协同促进了ECR。这项研究专门证明了连接在COF远程电子调谐中的作用,并揭示了其相关的电合成机制。
玉米赤霉烯酮(ZEN)是一种具有雌激素样活性的有害霉菌毒素,可导致生殖和免疫系统紊乱。在本研究中,开发了一种三明治结构的光电化学(PEC)传感器用于超灵敏检测ZEN。该传感器利用Z型NiTiO/CdInS异质结作为光活性层,显著提高了光吸收、电荷分离效率和光稳定性。用ZEN特异性适配体修饰的NiFeO纳米颗粒用作识别探针,ZEN分子作为桥梁将探针连接到PEC底物上。未结合的NiFeO探针可以使用外部磁场快速、简单且有效地去除,而结合ZEN的探针则保持锚定在电极表面,导致光电流的浓度依赖性猝灭。这种磁辅助分离策略简化了实验过程,大大减少了由非标准洗涤操作引起的假阳性和假阴性。优化后的传感器线性检测范围为100 fg/mL至1 μg/mL,检测限低至2.6 fg/mL,具有出色的选择性、稳定性和重现性。总体而言,该平台为检测复杂食品和环境样品中的痕量ZEN提供了一种可靠、简单且高度灵敏的方法。
背景:本研究的目的是利用网络药理学和分子对接技术确定艾司西酞普兰介导的长QT综合征(LQTS)发生发展的潜在分子机制。 方法:从GeneCards、DisGeNET和OMIM数据库中获取与LQTS相关的靶点,而从PharmMapper、SwissTargetPrediction、SuperPred、GeneCards、DrugBank和SEA数据库中检索与艾司西酞普兰相关的靶点。使用生物信息学在线工具生成包含药物-疾病交集靶点的维恩图。利用STRING数据库构建蛋白质-蛋白质相互作用网络。使用Cytoscape筛选核心靶点,并使用DAVID对艾司西酞普兰-LQTS交集靶点进行基因本体(GO)和京都基因与基因组百科全书(KEGG)富集分析。用Cytoscape构建药物-疾病-靶点通路网络。使用AutoDock Vina和PyMOL软件进行分子对接分析。 结果:在分子对接分析中,艾司西酞普兰介导的LQTS的六个潜在靶点,包括TNF、IL-1β、INS、SRC、STAT3和GSK-3β,显示与艾司西酞普兰结合良好。KEGG富集分析表明,艾司西酞普兰通过调节催乳素和脂质水平、动脉粥样硬化以及钙信号通路引起不良的LQTS反应。 局限性:需要进一步的体外或分子生物学实验来验证本研究中确定的艾司西酞普兰诱导LQTS的机制。 结论:基于生物信息学分析,艾司西酞普兰可能影响LQTS相关的电解质平衡、动脉粥样硬化和离子通道,为后续研究提供理论线索。
背景:基于术后三维(3D)定量冠状动脉造影(QCA)的血管血流储备分数(vFFR)已显示出与有创FFR测量值有很强的相关性。然而,经皮冠状动脉介入治疗(PCI)后vFFR、vFFR衍生的压力回撤梯度(PPG)、临床结局以及PCI后生活质量(QoL)之间关于性别差异的关系仍未得到探索。 方法:这项单中心回顾性研究纳入了因稳定型或不稳定型心绞痛或非ST段抬高型心肌梗死(NSTEMI)接受PCI治疗的患者,这些患者有两个适合计算PCI术后vFFR和完整QoL评估的血管造影视图。使用欧洲五维健康量表(EQ-5D-5L)问卷和西雅图心绞痛问卷(SAQ)评估PCI术后QoL。局灶性病变定义为vFFR衍生的PPG≥0.74,弥漫性病变定义为PPG值<0.74。对QoL和临床结局进行了分析并在性别之间进行了比较。 结果:共分析了234例患者(286条血管),中位随访时间为4.21年。PCI术后vFFR的中位数为0.92(四分位间距0.90-0.95),vFFR衍生的PPG中位数为0.74(四分位间距0.65-0.84),性别之间无显著差异。在PCI术后vFFR较高(高于中位数0.92)的患者中,女性的EQ指数得分低于男性(p<0.001)。在PCI术后vFFR三分位数的中间部分(vFFR在0.88至0.93之间),女性的SAQ总结得分低于男性(p<0.001)。在局灶性和弥漫性病变患者中,女性的EQ指数和SAQ总结得分均显著低于男性,所有p值均<0.05。性别之间的临床结局无差异。 结论:这一发现表明vFFR可能与术后QoL相关,在我们的研究中,尽管PCI术后vFFR和vFFR衍生的PPG值相似,但女性的QoL低于男性,尽管在不同工具或领域中不一致,这需要在更大规模的前瞻性研究中得到证实。
以其成本效益和高工作电压为特征的钠铁硫酸盐(Alluaudite-type NaFe(SO))已成为钠离子电池(SIBs)一种有前景的正极材料。然而,较差的电子导电性和缓慢的反应动力学阻碍了其实际应用。在本研究中,我们采用可扩展的喷雾干燥法制备了一种低应变球形的NaFe(SO)@C@KB(NFS@C@KB)正极,其被包裹在高导电性的科琴黑(KB)中。原位X射线衍射分析表明,近乎零体积应变源于致密球形结构和珍珠状KB支链的协同效应,有效增强了结构稳定性并延长了循环寿命。此外,相互连接的KB网络建立了连续的电子传输路径,从而提高了电子导电性。优化后的NFS@C@KB正极在5C时的容量为75 mAh g,在4000次循环中表现出卓越的循环稳定性。即使在-20°C的极端条件下,它在1C倍率下仍保持63 mAh g的放电容量。因此,低应变结构与出色的电化学性能相结合有望推动对铁基硫酸盐正极的进一步探索,并促进用于储能应用的可充电钠离子电池的发展。
建立并验证了一种反相液相色谱 - 串联质谱法,用于定量测定9种主要用于非小细胞肺癌的新型口服靶向抗癌药物:阿达格拉西布、卡马替尼、恩扎替尼、恩曲替尼、拉罗替尼、洛拉替尼、普拉替尼、塞尔帕替尼和索托拉西布,以用于人体血浆中的治疗药物监测。色谱分离采用Acquity BEH C18色谱柱,流动相为含0.1%甲酸的水和乙腈 - 甲醇(50:50,v/v)的梯度洗脱,流速为0.5 mL/min。血浆样品通过乙腈沉淀进行预处理,并用含0.1%甲酸的水稀释。反相色谱与正离子模式的串联质谱联用。该方法在以下浓度范围内成功验证:阿达格拉西布、卡马替尼、恩曲替尼、普拉替尼、塞尔帕替尼为100 - 10,000 ng/mL;恩扎替尼为50 - 50,000 ng/mL;拉罗替尼、洛拉替尼为10 - 1000 ng/mL;索托拉西布为10 - 10,000 ng/mL。准确度和精密度符合预定标准。稳定性试验证实,除恩曲替尼在-20°C下可稳定35天外,所有分析物在-20°C下的血浆中最多可稳定157天。在室温下,分析物在血浆中至少稳定7天,然而,对于阿达格拉西布、恩曲替尼和索托拉西布,可证明其最多稳定3天。我们建议使用干冰或冷藏方式运送这些样品。验证后,在应用阶段测定了74份血浆样品,除一份结果外,所有结果均在验证范围内。该方法可同时定量测定9种新型靶向疗法,并支持治疗药物监测。