Edge Graphitized Oxygen-Rich Carbon Based on Stainless Steel-Assisted High-energy Ball Milling for High-Capacity and Ultrafast Sodium Storage.

Oxygen doping is an effective strategy for constructing high-performance carbon anodes in Na ion batteries; however, current oxygen-doped carbons always exhibit low doping levels and high-defect surfaces, resulting in limited capacity improvement and low initial Coulombic efficiency (ICE). Herein, a stainless steel-assisted high-energy ball milling is exploited to achieve high-level oxygen doping (19.33%) in the carbon framework. The doped oxygen atoms exist dominantly in the form of carbon-oxygen double bonds, supplying sufficient Na storage sites through an addition reaction. More importantly, it is unexpected that the random carbon layers on the surface are reconstructed into a quasi-ordered arrangement by robust mechanical force, which is low-defect and favorable for suppressing the formation of thick solid electrolyte interfaces. As such, the obtained carbon presents a large reversible capacity of 363 mAh g-1 with a high ICE up to 83.1%. In addition, owing to the surface-dominated capacity contribution, an ultrafast Na storage is achieved that the capacity remains 139 mAh g-1 under a large current density of 100 A g-1 . Such good Na storage performance, especially outstanding rate capability, has rarely been achieved before.

Maximal Margin Support Vector Machine for Feature Representation and Classification.

High-dimensional small sample size data, which may lead to singularity in computation, are becoming increasingly common in the field of pattern recognition. Moreover, it is still an open problem how to extract the most suitable low-dimensional features for the support vector machine (SVM) and simultaneously avoid singularity so as to enhance the SVM's performance. To address these problems, this article designs a novel framework that integrates the discriminative feature extraction and sparse feature selection into the support vector framework to make full use of the classifiers' characteristics to find the optimal/maximal classification margin. As such, the extracted low-dimensional features from high-dimensional data are more suitable for SVM to obtain good performance. Thus, a novel algorithm, called the maximal margin SVM (MSVM), is proposed to achieve this goal. An alternatively iterative learning strategy is adopted in MSVM to learn the optimal discriminative sparse subspace and the corresponding support vectors. The mechanism and the essence of the designed MSVM are revealed. The computational complexity and convergence are also analyzed and validated. Experimental results on some well-known databases (including breastmnist, pneumoniamnist, colon-cancer, etc.) show the great potential of MSVM against classical discriminant analysis methods and SVM-related methods, and the codes can be available on https://www.scholat.com/laizhihui.

Effects of pyrolysis temperature on proton and cadmium binding properties onto biochar-derived dissolved organic matter: Roles of fluorophore and chromophore.

Understanding the environmental behavior of biochar-derived dissolved organic matter (BDOM) is crucial for promoting the extensive utilization of biochar and meeting the carbon neutrality targets. However, limited studies focused on the binding mechanism of protons and Cd with DOM released from biochar produced at different pyrolysis temperatures. By combining excitation-emission matrix spectroscopy and parallel factor analysis, we found that the humic-like fluorophores in BDOM had higher aromaticity, molecular weight, and contents of carboxylic and phenolic groups relative to the protein-like fluorophores. Conversely, the protein-like fluorophores exhibited a stronger binding affinity for Cd than humic-like fluorophores. With the pyrolysis temperature increased from 300 °C to 500 °C, the quenching effects of Cd on the protein-like components were enhanced significantly. Their fluorescence intensities could be quenched up to 51.64%. The results of ultraviolet-visible absorbance spectroscopy and differential absorbance spectroscopy showed that the carboxylic-like and phenolic-like chromophores were involved in the protons and Cd binding process of BDOM. The binding ability of phenolic-like chromophores with Cd was reduced as a function of increasing pyrolysis temperature. These findings implied that these carboxylic and phenolic groups were mainly contained in the non-fluorescent components. Besides, protons and Cd could also induce inter-chromophore interactions in BDOM, and the interaction was proportional to the pyrolysis temperature. These results clearly demonstrated the pyrolysis temperature-dependent changes in the protons and Cd binding properties of BDOM. More importantly, the possible risk of Cd mobility caused by the protein-like components in BDOM cannot be ignored when the biochar was applied in contaminated soils. This research extends our knowledge of the application potentiality of biochar in heavy metal polluted soil.

Comparative effectiveness of biologics and targeted therapies for psoriatic arthritis.

OBJECTIVE: To quantify comparative effectiveness of interleukin (IL)-12/23 antagonist (ustekinumab), IL-17A antagonists (secukinumab and ixekizumab), PDE4 inhibitor (apremilast) and tumour necrosis factor-alpha (TNF-α) inhibitors (infliximab, etanercept, adalimumab, certolizumab pegol and golimumab) for psoriatic arthritis (PsA). METHODS: We adapted a deidentified claims-based algorithm validated for inflammatory arthritis treatments to compare treatments among a retrospective cohort of commercially insured and Medicare Advantage beneficiaries with PsA from October 2013 to April 2019 in the OptumLabs Data Warehouse. Main outcomes include (1) treatment effectiveness, based on: adherence, adding or switching biologic or PDE4, addition of new non-biologic disease-modifying antirheumatic drug, increase in biologic or PDE4 dose or frequency and glucocorticoid use and (2) percentage of each group fulfilling the effectiveness algorithm. We used Poisson regression with robust variance stratified by prior PsA biologic exposure and adjusted for potential confounders. RESULTS: Of 2730 individuals with PsA, 327 received IL-12/23, 138 IL-17A's, 624 PDE4 and 1641 TNF-α's. Effectiveness criteria were fulfilled among 63 (19.3%) IL-12/23 recipients, 40 (29.0%) IL-17A recipients, 160 (25.6%) PDE4 recipients and 530 (32.3%) TNF-α recipients. Among biologic-naïve individuals, IL-12/23 was less effective than TNF-α's with fully adjusted relative risk (aRR) compared with TNF-α's of 0.63 (95% CI 0.45 to 0.89). Among biologic-experienced individuals, PDE4 recipients were less effective than TNF-α's (aRR 0.67, 95% CI 0.46 to 0.96). CONCLUSIONS: TNF-α's appeared more effective than IL-12/23's for biologic-naïve individuals, and PDE4's for biologic-experienced individuals. These results may help inform treatment choice for individuals with PsA.

Development of a Copper-Based Metal Organic Electrode for Nitrite Sensing.

BACKGROUND: Nitrite is naturally present in vegetables and added to processed meats to enhance their color and prolong their shelf life. It is of concern because it reacts to form nitrosamines, which have been linked to cancer. OBJECTIVE: To develop a quick, reliable, and inexpensive method for quantifying nitrite in foods. METHOD: A copper-based metal organic framework (Cu-MOF)/gold-platinum alloy nanoparticle(Au@Pt)-modified glassy carbon electrode (GCE) was developed via a simple wet chemical synthesis followed by electrochemical deposition of gold-platinum alloy nanoparticles onto the surface of a GCE. Morphological characterization and component analysis of the prepared nanomaterials were carried out by Fourier transform infrared spectroscopy and scanning electron microscopy. Cyclic voltammetry and electrochemical impedance spectroscopy were used to study the electrochemical behavior of the fabricated electrodes. RESULTS: The quantitative and specific detection of nitrite was obtained by the amperometric i-t method. At a pH of 7, temperature of 25°C, and ionic strength of 0.4 M, the electrode exhibited a linear range of 0.001-12.2 mM nitrite with a low detection limit of 72 nM (S/N = 3). CONCLUSIONS: The Cu-MOF/Au@Pt/GCE exhibited good repeatability, reproducibility, stability, and selectivity to provide a capable analysis method for food samples. HIGHLIGHTS: A Cu-MOF with a large surface area and high porosity was developed to provide an electrode with many active sites. The Au@Pt alloy nanoparticle improved the electrocatalytic activity toward nitrite. The synergistic action between the Cu-MOF and Au@Pt alloy nanoparticle enhanced the electrochemical performance of the sensor.

Recent advances in nanomaterial-based biosensors for the detection of exosomes.

Exosomes are a type of extracellular vesicle actively secreted by almost all eukaryotic cells. They are ideal candidates for reliable next-generation biomarkers in the early diagnosis and therapeutic response evaluation of cancer. Thus, the quantification of exosomes is crucial in facilitating clinical research and application. Compared with traditional materials, nanomaterials have better optical, magnetic, electrical, and catalytic properties due to their small size, high specific surface area, and variable structure. The incorporation of nanomaterials into sensing systems is an attractive approach towards improving sensitivity and can provide improved sensor selectivity and stability. In this paper, we summarize the progress in nanomaterial-based exosome detection methods, including electrochemical biosensors, photoelectrochemical biosensors, colorimetric biosensors, fluorescence biosensors, chemiluminescence biosensors, electrochemiluminescence biosensors, surface plasmon resonance biosensors, and surface-enhanced Raman spectroscopy biosensors. Moreover, future research directions and challenges in exosome detection methods are discussed. We hope that this article will offer an overview of nanomaterial-based exosome detection techniques and open new avenues in disease research.Graphical abstract.

Discovery of novel indazole-acylsulfonamide hybrids as selective Mcl-1 inhibitors.

Overexpressing myeloid cell leukemia sequence 1 (Mcl-1) protein is an important way to confer the resistance of cancer cells to conventional anti-cancer treatments. Therefore, developing Mcl-1 inhibitors has become an attractive strategy for cancer therapy. In the studies, a series of new indazole-acylsulfonamide hybrids were designed, synthesized and evaluated as potent Mcl-1 inhibitors. Among them, the most potent compound 17 (Ki = 0.43 µM) showed a little better inhibitory activity against Mcl-1 protein than positive control AT-101 (Ki = 0.45 µM). Pleasingly, it displayed > 40-fold selectivity over Bcl-2 (Ki = 18 µM) and Bcl-xL (no activity). Furthermore, compound 17 had good inhibitory activities against PC-3, MDA-MB-231 and K562 cells (IC50 = 12.3, 10.6 and 6.62 µM, respectively) and could effectively induce apoptosis and the activation of caspase-3 in a dose-dependent manner in K562 cells.

Binding characteristics of cadmium and zinc onto soil organic matter in different water managements and rhizosphere environments.

Soil organic matter (SOM) could immobilize most of metals, but it could promote the migration of a small part of metals in special environments. Heavy rainfall and drought makes wetlands affected by the alternation of drought and flood, altering the mobility of metals. Few studies have been conducted on the changes of binding characteristics of metals onto SOM which derived from different water conditions and rhizospheric environments. The objective of this paper was to explore the sequential differences of spectral variations of fluorescent groups and UV-Vis groups of metals onto SOM which derived from different water managements and rhizospheric environments. The method adopted was mainly two-dimensional correlation analysis (2DCOS). The results showed that flooding samples contained more aromatic substances compared to draining samples, which could promote metal binding. The binding characteristics were shown in the following: (1) Cd2+ and Zn2+ could react with aromatic substances, react with functional groups in SOM, and promote the formation of new groups such as carboxyl; (2) both Zn2+ and Cd2+ could bind with functional groups on proteins but relatively reductive environment can weaken the binding ability of Cd2+; (3) the protein-like or fulvic-like groups gave the fastest responses and then came the amide and carboxyl groups in nearly all flooding samples; (4) in flooding samples, Cd2+ was most easily to bind with fulvic-like groups, while Zn2+ was most easily to bind with protein-like groups. This work is conducive to the long-term management of heavy metal pollutants in wetlands.

Spectroscopic study of the effects of dissolved organic matter compositional changes on availability of cadmium in paddy soil under different water management practices.

It is well established that water management can influence the availability of Cd in paddy soil but the role of dissolved organic matter (DOM) characteristics in this process is still unclear. Here, we measured and compared the DOM quantity and quality between flooded and wetted treatments by spectroscopic and chemometric analysis and applied correlation analysis to relate DOM characteristics with availability concentrations of Cd. Ultraviolet-visible showed that aromaticity and hydrophobicity of DOM significantly decreased with time in wetted paddy soil (p < 0.05) but had no significant difference in flooded paddy soil (p > 0.05). According the results from two-dimensional correlation spectroscopy analytical method, humic- and protein-like substances had fast response during cultivation process. Two humic-like substances (C1, C2) and two protein-like substances (C3, C4) were identified from paddy soil-derived DOM by combining emission and excitation matrix spectroscopy with parallel factor. Compared to component C1, C3, and C4, component C2 has stronger aromaticity and hydrophobicity and higher molecular size (665-1000 Da). Its proportion declined markedly during the wetting periods but increased slightly during flooding. Pearson correlation analysis illustrated that flooding was more helpful in immobilizing Cd than wetting due to the aromatic, hydrophobic, and high molecular weight constituents remained in flooded treatments and the substantial decomposition of component C2 in wetted treatments. These results suggested that spectroscopic and chemometric methods are helping to further explain the impacts of DOM quality on Cd availability under different water management practices.

Hollow and porous nickel sulfide nanocubes prepared from a metal-organic framework as an efficient enzyme mimic for colorimetric detection of hydrogen peroxide.

Hollow, porous NiS nanocubes were prepared by a hydrothermal method starting from Ni-Co Prussian blue analogue nanocubes as the template. The morphology and structure of the NiS nanocubes were tuned by adjustment of the ion-exchange rate and the degree of chemical etching, and they were characterized by scanning electron microscopy, energy-dispersive X-ray spectroscopy, transmission electron microscopy, X-ray diffraction, and nitrogen sorption measurements. The NiS nanocubes are shown to act as a peroxidase mimic that can catalyze the oxidization of 3,3',5,5'-tetramethylbenzidine by hydrogen peroxide (H2O2), producing a visible color change, for which the absorbance is best measured at 652 nm. The outstanding activity may result from the unique structure of the NiS nanocubes. The catalytic oxidation follows Michaelis-Menten kinetics and shows a ping-pong mechanism of enzyme action. The findings were used to develop a rapid, sensitive, and selective colorimetric H2O2 assay with a response that is linear in the 4-40 µM range with a detection limit of 1.72 µM (signal-to-noise ratio of 3). Graphical abstarct ᅟ.

Prostate cancer patients' refusal of cancer-directed surgery: a statewide analysis.

Introduction. Prostate cancer is the most common cancer among men in USA. The surgical outcomes of prostate cancer remain inconsistent. Barriers such as socioeconomic factors may play a role in patients' decision of refusing recommended cancer-directed surgery. Methods. The Nebraska Cancer Registry data was used to calculate the proportion of prostate cancer patients recommended the cancer-directed surgery and the surgery refusal rate. Multivariate logistic regression was applied to analyze the socioeconomic indicators that were related to the refusal of surgery. Results. From 1995 to 2012, 14,876 prostate cancer patients were recommended to undergo the cancer-directed surgery in Nebraska, and 576 of them refused the surgery. The overall refusal rate of surgery was 3.9% over the 18 years. Patients with early-stage prostate cancer were more likely to refuse the surgery. Patients who were Black, single, or covered by Medicaid/Medicare had increased odds of refusing the surgery. Conclusion. Socioeconomic factors were related to the refusal of recommended surgical treatment for prostate cancer. Such barriers should be addressed to improve the utilization of surgical treatment and patients' well-being.