A family of dual-anion-based sodium superionic conductors for all-solid-state sodium-ion batteries.

The sodium (Na) superionic conductor is a key component that could revolutionize the energy density and safety of conventional Na-ion batteries. However, existing Na superionic conductors are primarily based on a single-anion framework, each presenting inherent advantages and disadvantages. Here we introduce a family of amorphous Na-ion conductors (Na2O2-MCly, M = Hf, Zr and Ta) based on the dual-anion framework of oxychloride. Benefiting from a dual-anion chemistry and with the resulting distinctive structures, Na2O2-MCly electrolytes exhibit room-temperature ionic conductivities up to 2.0 mS cm-1, wide electrochemical stability windows and desirable mechanical properties. All-solid-state Na-ion batteries incorporating amorphous Na2O2-HfCl4 electrolyte and a Na0.85Mn0.5Ni0.4Fe0.1O2 cathode exhibit a superior rate capability and long-term cycle stability, with 78% capacity retention after 700 cycles under 0.2 C (1C = 120 mA g-1) at room temperature. The discoveries in this work could trigger a new wave of enthusiasm for exploring new superionic conductors beyond those based on a single-anion framework.

Amorphous Oxyhalide Matters for Achieving Lithium Superionic Conduction.

The recently surged halide-based solid electrolytes (SEs) are great candidates for high-performance all-solid-state batteries (ASSBs), due to their decent ionic conductivity, wide electrochemical stability window, and good compatibility with high-voltage oxide cathodes. In contrast to the crystalline phases in halide SEs, amorphous components are rarely understood but play an important role in Li-ion conduction. Here, we reveal that the presence of amorphous component is common in halide-based SEs that are prepared via mechanochemical method. The fast Li-ion migration is found to be associated with the local chemistry of the amorphous proportion. Taking Zr-based halide SEs as an example, the amorphization process can be regulated by incorporating O, resulting in the formation of corner-sharing Zr-O/Cl polyhedrons. This structural configuration has been confirmed through X-ray absorption spectroscopy, pair distribution function analyses, and Reverse Monte Carlo modeling. The unique structure significantly reduces the energy barriers for Li-ion transport. As a result, an enhanced ionic conductivity of (1.35 ± 0.07) × 10-3 S cm-1 at 25 °C can be achieved for amorphous Li3ZrCl4O1.5. In addition to the improved ionic conductivity, amorphization of Zr-based halide SEs via incorporation of O leads to good mechanical deformability and promising electrochemical performance. These findings provide deep insights into the rational design of desirable halide SEs for high-performance ASSBs.

A Visible-Light-Driven Self-Powered Nodularin-R Biosensing Platform Controlled by an Integrated Portable Photoelectrochemical Detection Device.

The presence of nodularin-R (NOD-R) in water has gained considerable attention because of its widespread distribution and high toxicity. In this study, an accurate and rapid visible-light-driven self-powered photoelectrochemical (PEC) biosensor was developed by integrating a portable paper-based electrode with a custom-built miniaturized PEC detection device. The newly designed system successfully achieved on-site detection of NOD-R in real water samples based on PEC technology. First, target recognition triggers the initiation of the hybridization chain reaction to generate double-stranded DNA. The thus-formed double-stranded DNA entrapped methylene blue (MB), and the dye molecules were irradiated with visible light for conversion to leuco-MB in the presence of ascorbic acid. The resulting leuco-MB species significantly amplified the PEC signal output of TiO2-MXene, enabling NOD-R detection. Under optimal conditions, the proposed PEC assay strategy demonstrated NOD-R detection within a concentration range from 20 fg mL-1 to 10 ng mL-1 with a detection limit of 19.6 fg mL-1. In addition, a custom-built miniaturized PEC detection device conveniently integrates the detection component with the light source, enabling the real-time collection of results via a wireless module. This innovative self-powered PEC platform provides significant advancements in smooth and intelligent detection compared to traditional PEC detection devices.

Identification of Optimal Parameters for Assessing Lymph Node Status of Patients with Esophageal Squamous Cell Carcinoma After Neoadjuvant Chemoradiotherapy.

BACKGROUND: This study aimed to compare the prognostic discrimination power of pretreatment pathologic N stage (prepN), lymph node tumor regression grade (LNTRG), and posttreatment pathologic N (ypN) category for esophageal squamous cell carcinoma (ESCC) patients who received neoadjuvant chemoradiotherapy (nCRT) plus surgery. METHODS: The study reviewed 187 ESCC patients from two medical centers who underwent nCRT plus surgery. Pathologic LNTRG was defined by the proportion of viable tumor area within the tumor bed in lymph nodes (LNs). An average LNTRG then was calculated by averaging the tumor regression grade (TRG) score of all resected LNs. Lymph nodes containing regression changes or vital tumor cells were used for interpretation of the prepN stage, which reflects the estimated number of originally involved LNs. RESULTS: The ypN, prepN, and LNTRG categories had significant prognostic stratification power (p < 0.001, log-rank test). Multivariable cox regression showed that all three categories were independent prognostic factors of disease-free survival (DFS) (p < 0.05). The LNTRG category showed a better prognostic value for DFS prediction than the ypN and prepN categories (Akaike information criterion [AIC]: LNTRG [933.69], ypN [937.56], prepN [937.45]). Additionally, the superior predictive capacity of the LNTRG category was demonstrated by decision curve analysis. Similar results were discovered for patients with remaining diseased LNs. CONCLUSIONS: The three staging categories had prognostic relevance for DFS, with the LNTRG category seeming to have better prognostic indication power. Comprehensive consideration of the ypN status, prepN status, and LN regression may allow for better prognostic stratification of patients.

Pulse buildup dynamics in a self-starting Mamyshev oscillator.

The Mamyshev oscillator (MO) can generate high-performance pulses. However, due to their non-resonant cavities, they usually are not self-starting, and there is almost no effort to reveal the pulse buildup dynamics of the MO. This paper investigates the dynamic of single pulse (SP) and multi-pulse formation in a self-starting MO. It indicated that both SP self-starting and multi-pulse self-starting can be obtained by adjusting the oscillator parameters. More importantly, increasing pump power could only result in bound state pulses (BSPs) if SP self-starting was formed. With the increase of the pump power, the pulse number in BSPs would increase. However, multiple pulses could not be formed only by increasing the pump power, and the BSPs obtained here underwent SP generated from noise, amplified, and then bounded, which is different from conventional passive mode-locked fiber lasers (CPMLFLs). On the other hand, if multiple pulses were self-initiated, BSPs, pulse bunch, and harmonic mode-locked pulses (HMLPs) could be obtained by adjusting the polarization state and pump power in the cavity. Furthermore, once any of the above states are formed, if the oscillator polarization state and filter interval are unchanged, only increasing the pump power from zero, the original state can still be obtained, which is consistent with the characteristics of the CPMLFLs. These findings will provide new insights into the pulse dynamics of self-starting MO, which will be significant for studying ultrafast laser technology and nonlinear optics.

Template-Free Synthesis of Boron-Doped Graphitic Carbon Nitride Porous Nanotubes for Enhanced Photocatalytic Hydrogen Evolution.

The photocatalytic activity of g-C3N4 can be enhanced by improving photoinduced carrier separation and exposing sufficient reactive sites. In this study, we synthesized B-doped porous tubular g-C3N4 (BCNT) using a H3BO3-assisted supramolecular self-template method, wherein H3BO3 helped in B-doping, building a porous structure, and maintaining one-dimensional nanotubes. The tubular structure had an ultrathin tube wall and large aspect ratio, which are conducive to the directional transmission and separation of photogenerated carriers; moreover, the abundant pore structure of the tube wall could fully expose the reactive sites. The introduction of B and the cyano group modulated the bandgap of g-C3N4 and elevated the position of the conduction band, thus enhancing the photoreduction ability and effectively improving the hydrogen evolution performance. Consequently, the hydrogen evolution of BCNT-2 (220.8, 53.2 µmol·h-1) was 1.82 and 1.54 times that of ultrathin g-C3N4 nanosheets (CNN, 121.3, 34.6 µmol·h-1) under simulated sunlight and LED lamp irradiation, respectively. Thus, this work provides in-depth insights into the rational design of one-dimensional g-C3N4 nanotubes with high hydrogen evolution activity under visible irradiation.

Chemical composition analysis of Qingyan dropping pills using ultra-high-performance liquid chromatography-quadrupole time-of-flight mass spectrometry.

RATIONALE: This study developed a method for the rapid classification and identification of the chemical composition of Qingyan dropping pills (QDP) to provide the theoretical basis and data foundation for further in-depth research on the pharmacological substance basis of the formula and the selection of quality control indexes. METHODS: Ultra-high performance liquid chromatography-quadrupole time-of-flight mass spectrometry (UHPLC-Q-TOF-MS) and data postprocessing technology were used to analyze the chemical composition of QDP. The fragmentation information on possible characteristic fragments and related neutral losses was summarized based on the literature and was compared with the MS data obtained from the assay, and thus a rapid classification and identification of chemical components in QDP could be achieved. RESULTS: A total of 73 compounds were identified, namely 24 flavonoids, 14 terpenoids, 30 organic acids and their esters, 3 alkaloids, and 2 phenylpropanoids. CONCLUSIONS: In this study, UHPLC-Q-TOF-MS and data postprocessing technology were used to realize the rapid classification and identification of the chemical constituents of QDP, which provided a comprehensive, efficient, and fast qualitative analysis method, a basis for further quality control and safe medication of QDP.

Th1/Th2 associated transcription factors and cytokines in pregnancies with systemic lupus erythematosus.

OBJECTIVES: Th1/Th2 shift occurs during pregnancy. Systemic lupus erythematosus (SLE) flares may induce the dysregulation of Th1 and Th2 cells. We aimed to investigate the dynamic changes of Th1/Th2 associated transcription factors and cytokines in patients with SLE during pregnancy. METHODS: Twenty-five pregnant patients with SLE and twenty-two healthy age-matched women served as controls from September 2021 to March 2022 were enrolled in the study. Real-time quantitative reverse transcription polymerase chain reaction analysis of peripheral blood mononuclear cells were performed to measure the expression of Th1 specific transcription factors T-bet, cytokine IFN-γ, and Th2 specific transcription factors GATA3, cytokine IL-4. The main statistical analysis methods were t test, Mann-Whitney U-test, Pearson correlation and Spearman rank correlation analysis. RESULTS: The mRNA level of IFN-γ and the relative expression of T-bet/GATA3 and IFN-γ/IL-4 in SLE patients were significantly higher than those in healthy individuals, whereas the GATA3 expression is lower in pregnant patients with SLE (p<0.001, p<0.05, p<0.05 and p<0.01 during the whole pregnancy, respectively; p<0.05, p<0.01, p<0.05 and p<0.05 specifically for the 3rd trimester, respectively). There were significant correlations between T-bet and IFN-γ (r=0.492, p<0.05), and between T-bet/GATA3 and IFN-γ/IL-4 (r=0.482, p<0.05). CONCLUSIONS: Our work indicates that in SLE patients Th1/Th2 shift is blocked with up-regulation of Th1 cell function and insufficient Th2 polarisation during pregnancy, which may be involved in adverse pregnancy outcomes.

Epsin1-mediated exosomal sorting of Dll4 modulates the tubular-macrophage crosstalk in diabetic nephropathy.

Tubular epithelial cells (TECs) play critical roles in the development of diabetic nephropathy (DN), and can activate macrophages through the secretion of exosomes. However, the mechanism(s) of TEC-exosomes in macrophage activation under DN remains unknown. By mass spectrometry, 1,644 differentially expressed proteins, especially Dll4, were detected in the urine exosomes of DN patients compared with controls, which was confirmed by western blot assay. Elevated Epsin1 and Dll4/N1ICD expression was observed in kidney tissues in both DN patients and db/db mice and was positively associated with tubulointerstitial damage. Exosomes from high glucose (HG)-treated tubular cells (HK-2) with Epsin1 knockdown (KD) ameliorated macrophage activation, TNF-α, and IL-6 expression, and tubulointerstitial damage in C57BL/6 mice in vivo. In an in vitro study, enriched Dll4 was confirmed in HK-2 cells stimulated with HG, which was captured by THP-1 cells and promoted M1 macrophage activation. In addition, Epsin1 modulated the content of Dll4 in TEC-exosomes stimulated with HG. TEC-exosomes with Epsin1-KD significantly inhibited N1ICD activation and iNOS expression in THP-1 cells compared with incubation with HG alone. These findings suggested that Epsin1 could modulate tubular-macrophage crosstalk in DN by mediating exosomal sorting of Dll4 and Notch1 activation.

Rapid classification and identification of chemical components in three different Zanthoxylum species by ultra-high-performance-liquid chromatography quadrupole-orbitrap-mass spectrometry.

Zanthoxylum, as a medicinal and edible herbal medicine, has a long history and complex chemical composition. There are many varieties of Zanthoxylum, and there are differences in composition between varieties. In this study, a rapid classification and identification method for the main components of Zanthoxylum was established using ultra-high-performance-liquid chromatography quadrupole-orbitrap-mass spectrometry. The components of Shandong Zanthoxylum bungeanum, Wudu Zanthoxylum bungeanum, and Zanthoxylum schinifolium were identified by studying the characteristic fragmentations and neutral losses of characteristic components. A total of 48 common components and 24 different components were identified and the fragmentation patterns of the main components, such as flavonoids, alkaloids, and organic acids were summarized. These findings provided a reference for the study of pharmacodynamic substance basis and quality control of different varieties of Zanthoxylum.