Pyrolysis-Free Covalent Organic Polymers Directly for Oxygen Electrocatalysis.

ConspectusOxygen electrode catalysis is crucial for the efficient operation of clean energy devices, such as proton exchange membrane fuel cells (PEMFCs) and Zn-air batteries (ZABs). However, sluggish oxygen electrocatalysis kinetics in these infrastructures put forward impending requirements toward seeking efficient oxygen-electrode catalytic materials with a clear active-site configuration and geometrical morphology to study in depth the structure-property relationship of materials. Although transition-metal-nitrogen-carbon (M-N-C) electrocatalysts have shown great prospects currently and potential in oxygen electrocatalysis as promising platinum group metal-free catalysts, the universal pyrolysis operation in the preparation process often inevitably brings about randomness and diversity of active sites, for which it is difficult to determine the structure-activity relationship, understand the catalytic mechanism, and further improve facilities performance.Covalent organic polymers (COPs) are a class of molecular geometric constructs linked by irreversible kinetic covalent bonds through reticular chemistry. Unique structural tailorability, diverse design principles, and inherent well-defined construction in pristine COPs naturally provide a great platform to study the structure-property relationship of active sites and exhibit unique features for application. In this Account, we afford an overview of our recent attempts toward the utilization of COP materials as free-pyrolysis oxygen electrode catalysts, enabling accurate construction of oxygen electrodes with clear active site and geometrical morphology characteristics in PEMFC and ZAB devices yet without enduring any high-temperature pyrolysis treatments. Starting from the needs of modern electrocatalysis, we discussed the unique properties for the design and development of pyrolysis-free pristine COPs as high-performance oxygen electrode catalytic materials in terms of intrinsic electronic structure properties and membrane-electrode-assembly (MEA) application distinguished from pyrolysis M-N-C catalysts. First, the pyrolysis-free COP catalysts provide a viable molecular model catalyst platform, which is conducive to mechanism comprehension for the relationship between catalyst activity and structure. Second, the simple and low-energy consumption synthesis process for pyrolysis-free catalysts lays the foundation for the large-scale production of catalysts, oxygen electrodes, and even the entire stack assembly without considering numerous complicated factors as traditional pyrolytic catalysts. Besides, most traditional COPs are difficult to dissolve and solution process due to their cross-linked skeleton. Our newly developed COP materials with solution processability bring about new opportunities to the process and assemble oxygen electrodes into device. These properties are unparalleled and have not been systematically reviewed and analyzed by any research reports so far. Here, we have clarified the specific advantage and potential of pyrolysis-free COP materials as oxygen electrodes applied in PEMFC and ZAB devices in response to the latest progress and requirements of current electrocatalytic research.

Insight of neonicotinoid insecticides: Exploring exposure, mechanisms in non-target organisms, and removal technologies.

Neonicotinoid insecticides (NEOs) have garnered global attention due to their selective toxicity to insects and minimal impact on mammals. However, growing concerns about their extensive use and potential adverse effects on the ecological environment and non-target organisms necessitate further investigation. This study utilized bibliometric tools to analyze Web of Science data from 2003 to 2024, elucidating the current research landscape, identifying key research areas, and forecasting future trends related to NEOs. This paper provides an in-depth analysis of NEO exposure in non-target organisms, including risk assessments for various samples and maximum residue limits established by different countries. Additionally, it examines the impacts and mechanisms of NEOs on non-target organisms. Finally, it reviews the current methods for NEO removal and degradation. This comprehensive analysis provides valuable insights for regulating NEO usage and addressing associated exposure challenges.

Chemical Vapor Deposition Toward Efficient Bimetallic Atomically Dispersed Oxygen Reduction Catalysts.

Non-precious metal-based nitrogen-doped carbon (M-Nx/C) shows great potential as a substitute for precious metal Pt-based catalysts. However, the conventional pyrolytic methods for forming M-Nx/C active sites are prone to issues such as the lack of synergistic interactions among bimetallic atoms and the potential encasement of active sites, leading to compromised catalytic efficiency and hindered mass transfer. In this work, a highly active FeCo-N-C@U-AC electrocatalyst is developed with a high density of active sites, adequate exposure of catalytic sites, and robust mass transfer capability using the chemical vapor-phase deposition (CVD) technique. The resulting catalyst demonstrates impressive oxygen reduction reaction (ORR) catalytic performance and stability, with half-wave potentials of 0.820 V (0.1 M HClO4) and 0.911 V (0.1 M KOH), respectively. It also exhibits significantly enhanced stability, retaining 93.25% and 98.38% of current after continuous 50 000 s of durability testing, surpassing the retention rates of Pt/C (80.31% in HClO4 and 84.96% in KOH electrolytes). Notably, when employed as a cathode catalyst in proton exchange membrane fuel cells (PEMFCs) and zinc-air flow batteries (ZAFBs), the FeCo-N-C@U-AC catalyst delivers peak power densities of 859 and 162 mW·cm-2, respectively, showcasing competitive performance comparable to benchmark Pt/C.

Supramolecular salicylic acid combined with niacinamide in chloasma: A randomized controlled trial.

BACKGROUND: No trial of supramolecular salicylic acid (SSA) for chloasma is available yet. OBJECTIVE: The purpose of this study was to assess the efficacy and safety of Bole DA 30% supramolecular salicylic acid (SSA) combined with 10% niacinamide in treating chloasma. METHODS: This multicenter (n=15), randomized, double-blind, parallel placebo-controlled trial randomized the subjects (1:1) to Bole DA 30% SSA or placebo. The primary endpoint was the effective rate after 16 weeks using the modified melasma area severity index (mMASI) [(pretreatment-posttreatment)/pretreatment×100%]. RESULTS: This study randomized 300 subjects (150/group in the full analysis set, 144 and 147 in the per-protocol set). The total mMASI score, overall Griffiths 10 score, left Griffiths 10 score, and right Griffiths 10 score were significantly lower in the Bole DA 30% SSA group than in the placebo group (all P<0.001). One study drug-related AE and one study drug-unrelated adverse events (AE) were reported in the Bole DA 30% SSA group. No AE was reported in the placebo group. CONCLUSION: Bole DA 30% SSA combined with 10% niacinamide is effective and safe for treating chloasma. CLINICAL TRIAL REGISTRATION NUMBER: ChiCTR2200065346.

Expert consensus on perioperative integrated skincare for noninvasive energy-based device aesthetic procedures in clinical practice in China.

BACKGROUND: Noninvasive energy-based device (NI-EBD) aesthetic procedures has recently gained widespread usage for treating various skin conditions, enhancing skin texture and performing rejuvenation-related procedures. However, practically all NI-EBD procedures result in variable degrees of damage to the skin barrier, inducing pathological and physiological processes such as oxidative stress and inflammation, and only a small percentage of individuals possess the innate ability to restore it. OBJECTIVE: To introduce the concept of integrated skincare and establish standardized operational procedures for perioperative integrated skincare, and furnish a theoretical basis for clinical diagnosis and treatment performed by professional medical aestheticians. METHODS: The author leveraged domestic and international guidelines, clinical practice expertise and evidence-based research, adapting them to suit the specific circumstances in China. RESULTS: The consensus were provided four parts, including concept and essence of integrated skincare, integrated skincare significance during the perioperative phase of NI-EBD procedures, active ingredients and functions of effective skincare products, standardized perioperative skincare procedure for NI-EBD procedures and precautions. For the standardized perioperative skincare procedure, four recommendations were listed according to different stages during NI-EBD procedures. CONCLUSION: These recommendations create the 'Expert Consensus on Perioperative Integrated Skincare for Noninvasive Energy-Based Device Aesthetic Procedures in Clinical Practice in China'.

Efficacy and Safety of Drug-Coated Balloon in Elderly Patients with Intrastent Restenosis After Lower Extremity Arteriosclerotic Obliterans After Rotarex Thrombus Removal.

Objective: This study aims to compare the efficacy and safety of drug-coated balloon (DCB) and standard angioplasty balloon (SAB) in the treatment of intrastent restenosis (ISR) after lower extremity ASO following rotarex thrombus removal. Methods: 94 patients with ISR after lower extremity ASO were selected and divided into DCB group (47 cases) and SAB group (47 cases). After patients were treated with DCB and SAB methods, six months after discharge care, the therapeutic effect, lower extremity dorsal arterial blood flow, ankle-brachial index, lameness distance, hemorheology, endothelial function indexes, and lipid levels were measured. Results: DCB group showed significantly higher effective rate compared to SAB group (P < .05). After treatment, post-treatment improvements in dorsalis arterial blood flow, ankle-brachial index intermittent claudicity distance, high-density lipoprotein cholesterol (HDL-C) and nitric oxide (NO) contents were more pronounced in the DCB group than SAB group (P < .05).Indexes of hemorheology and the contents of total cholesterol (TC), triglyceride (TG), low-density lipoprotein cholesterol (LDL-C), and endothelin-1 (ET-1) levels significantly decreased after treatment, with greater reduction observed in DCB group (P < .05). In addition, No significant change in adverse reactions between groups, but DCB group had lower adverse drug reaction rate. Conclusions: Overall, DCB demonstrated superior efficacy in treating ISR after lower extremity ASO, offering a promising option for improving patient outcomes.

Abbreviated Versus Full-Protocol MRI for Breast Cancer Neoadjuvant Chemotherapy Response Assessment: Diagnostic Performance by General and Breast Radiologists.

BACKGROUND. Abbreviated protocols could allow wider adoption of MRI in patients undergoing breast cancer neoadjuvant chemotherapy (NAC). However, abbreviated MRI has been explored primarily in screening settings. OBJECTIVE. The purpose of this article was to compare diagnostic performance of abbreviated MRI and full-protocol MRI for evaluation of breast cancer NAC response, stratifying by radiologists' breast imaging expertise. METHODS. This retrospective study included 203 patients with breast cancer (mean age, 52.1 ± 11.2 [SD] years) from two hospitals who underwent MRI before NAC initiation and after NAC completion before surgical resection from March 2017 to April 2021. Abbreviated MRI was extracted from full-protocol MRI and included the axial T2-weighted sequence and precontrast and single early postcontrast T1-weighted sequences. Three general radiologists and three breast radiologists independently interpreted abbreviated and full-protocol MRI in separate sessions, identifying enhancing lesions to indicate residual tumor and measuring lesion size. The reference standard was presence and size of residual tumor on pathologic assessment of post-NAC surgical specimens. RESULTS. A total of 50 of 203 patients had pathologic complete response (pCR). Intraobserver and interobserver agreement for abbreviated and full-protocol MRI for general and breast radiologists ranged from substantial to nearly perfect (κ = 0.70-0.81). Abbreviated MRI compared with full-protocol MRI showed no significant difference for general radiologists in sensitivity (54.7% vs 57.3%, p > .99), specificity (92.8% vs 95.6%, p = .29), or accuracy (83.4% vs 86.2%, p = .30), nor for breast radiologists in sensitivity (60.0% vs 61.3%, p > .99), specificity (94.6% vs 97.4%, p = .22), or accuracy (86.0% vs 88.5%, p = .30). Sensitivity, specificity, and accuracy were not significantly different between protocols for any reader individually (p > .05). Mean difference in residual tumor size on MRI relative to pathology for abbreviated protocol ranged for general radiologists from -0.19 to 0.03 mm and for breast radiologists from -0.15 to -0.05 mm, and for full protocol ranged for general radiologists from 0.57 to 0.65 mm and for breast radiologists from 0.66 to 0.79 mm. CONCLUSION. Abbreviated compared with full-protocol MRI showed similar intraobserver and interobserver agreement and no significant difference in diagnostic performance. Full-protocol MRI but not abbreviated MRI slightly overestimated pathologic tumor sizes. CLINICAL IMPACT. Abbreviated protocols may facilitate use of MRI for post-NAC response assessment by general and breast radiologists.

Review of machine learning-based surrogate models of groundwater contaminant modeling.

Heavy computational load inhibits the application of groundwater contaminant numerical model to groundwater pollution source identification, remediation design, and uncertainty analysis, since a large number of model runs are required for these applications. Machine learning-based surrogate models are an effective approach to enhance the efficiency of the numerical models, and have recently attracted considerable attention in the field of groundwater contaminant modeling. Here, we review 120 research articles on machine learning-based surrogate models for groundwater contaminant modeling that were published between 1994 and 2022. We outline the state of the art method, identify the most significant research challenges, and suggest potential future directions. The six major applications of machine learning-based surrogate models are groundwater pollution source identification, groundwater remediation design, coastal aquifer management, uncertainty analysis of groundwater, groundwater monitoring network design, and groundwater transport parameters inversion. Together, these account for more than 90% of the studies we review. Latin hypercube sampling (LHS) is the most widely used sampling method, and artificial neural networks (ANNs) and Kriging are the two most widely used methods for constructing surrogate model. No method is universally superior, the advantages and disadvantages of different methods, as well as the applicability of these methods for different application purposes of groundwater contaminant modeling were analyzed. Some recommendations on the method selection for various application fields are given based on the reviews and experiences. Based on our review of the state-of-the-art, we suggest several future research directions to enhance the feasibility of the machine learning-based surrogate models of groundwater contaminant modeling: the alleviation of the curse of dimensionality, enhancing transferability, practical applications for real case studies, multi-source dada fusion, and real-time monitoring and prediction.

Prevalence, antimicrobial susceptibility, and antibiotic resistance gene transfer of Bacillus strains isolated from pasteurized milk.

Pasteurization is carried out in dairy industries to kill harmful bacteria present in raw milk. However, endospore-forming bacteria, such as Bacillus, cannot be completely eliminated by pasteurization. In this study, a total of 114 Bacillus strains were isolated from 133 pasteurized milk samples. Antibiotic susceptibility tests showed that the percentage of Bacillus with intrinsic resistance to ampicillin and penicillin were 80 and 86%, respectively. Meanwhile, some Bacillus isolates had acquired resistance, including trimethoprim-sulfamethoxazole resistance (10 isolates), clindamycin resistance (8 isolates), erythromycin resistance (2 isolates), and tetracycline resistance (1 isolate). To further locate these acquired resistance genes, the plasmids were investigated in these 16 Bacillus strains. The plasmid profile indicated that Bacillus cereus BA008, BA117, and BA119 harbored plasmids, respectively. Subsequently, the Illumina Novaseq PE150 was applied for the genomic and plasmid DNA sequencing. Notably, the gene tetL encoding tetracycline efflux protein was found to be located on plasmid pBC46-TL of B. cereus BA117. In vitro conjugative transfer indicated that pBC46-TL can be transferred into Bacillus invictae BA142, Bacillus safensis BA143, and Bacillus licheniformis BA130. The frequencies were of 1.5 × 10-7 to 1.7 × 10-5 transconjugants per donor cells. Therefore, Bacillus strains with acquired antibiotic resistance may represent a potential risk for the spread of antibiotic resistance between Bacillus and other clinical pathogens via horizontal gene transfer.

Extrafollicular PD-1highCXCR5-CD4+ T cells participate in local immunoglobulin production in nasal polyps.

BACKGROUND: Local immunoglobulin hyperproduction is observed in nasal polyps (NPs) with and without ectopic lymphoid tissues (eLTs). OBJECTIVE: Our aim was to identify the T-cell subsets involved in local immunoglobulin production independent of eLTs in NPs. METHODS: The localization, abundance, and phenotype of CD4+ T-cell subsets were studied by immunofluorescence, flow cytometry, and single-cell RNA sequencing. Purified nasal T-cell subsets were cultured with autologous peripheral naive B cells to explore their function. Programmed death ligand 1 and programmed death ligand 2 expression in NPs was investigated by immunofluorescence staining and flow cytometry. RESULTS: Accumulation of PD-1highCXCR5-CD4+ T cells outside lymphoid aggregates was found in NPs. Nasal PD-1highCXCR5-CD4+ T cells were characterized by a unique phenotype that was related to B-cell help and tissue residency and distinct from PD-1-/intCXCR5- and CXCR5+ CD4+ T cells in NPs as well as PD-1highCXCR5highCD4+ follicular helper T cells in tonsils. Compared with the frequencies of PD-1highCXCR5-CD4+ T cells and their IFN-γ+, IL-17A+, and IL-21+ subsets in the control inferior turbinate tissues, the frequencies of these cells and their subsets were increased in both eosinophilic and noneosinophilic NPs, whereas the frequencies of the IL-4+ and IL-4+IL-21+ subsets were increased only in eosinophilic NPs. Nasal PD-1highCXCR5-CD4+ T cells induced immunoglobulin production from B cells in a potency comparable to that induced by tonsillar follicular helper T cells. PD-1highCXCR5-CD4+ T-cell frequencies were correlated with IgE levels in eosinophilic NPs. PD-L1 and PD-L2 suppressed the function of PD-1highCXCR5-CD4+ T cells, and their levels were reduced in NPs. PD-1highCXCR5-CD4+ T-cell abundance was associated with the postsurgical relapse of NPs. CONCLUSION: PD-1highCXCR5-CD4+ T cells participate in local immunoglobulin production independent of eLTs in NPs.