Electrolyte design for Li-ion batteries under extreme operating conditions.

The ideal electrolyte for the widely used LiNi0.8Mn0.1Co0.1O2 (NMC811)||graphite lithium-ion batteries is expected to have the capability of supporting higher voltages (≥4.5 volts), fast charging (≤15 minutes), charging/discharging over a wide temperature range (±60 degrees Celsius) without lithium plating, and non-flammability1-4. No existing electrolyte simultaneously meets all these requirements and electrolyte design is hindered by the absence of an effective guiding principle that addresses the relationships between battery performance, solvation structure and solid-electrolyte-interphase chemistry5. Here we report and validate an electrolyte design strategy based on a group of soft solvents that strikes a balance between weak Li+-solvent interactions, sufficient salt dissociation and desired electrochemistry to fulfil all the aforementioned requirements. Remarkably, the 4.5-volt NMC811||graphite coin cells with areal capacities of more than 2.5 milliampere hours per square centimetre retain 75 per cent (54 per cent) of their room-temperature capacity when these cells are charged and discharged at -50 degrees Celsius (-60 degrees Celsius) at a C rate of 0.1C, and the NMC811||graphite pouch cells with lean electrolyte (2.5 grams per ampere hour) achieve stable cycling with an average Coulombic efficiency of more than 99.9 per cent at -30 degrees Celsius. The comprehensive analysis further reveals an impedance matching between the NMC811 cathode and the graphite anode owing to the formation of similar lithium-fluoride-rich interphases, thus effectively avoiding lithium plating at low temperatures. This electrolyte design principle can be extended to other alkali-metal-ion batteries operating under extreme conditions.

Generation of advanced cerebellar organoids for neurogenesis and neuronal network development.

Neurons within the cerebellum form temporal-spatial connections through the cerebellum, and the entire brain. Organoid models provide an opportunity to model the early differentiation of the developing human cerebellum, which is difficult to study in vivo, and affords the opportunity to study neurodegenerative and neurodevelopmental diseases of the cerebellum. Previous cerebellar organoid models focused on early neuron generation and single cell activity. Here, we modify previous protocols to generate more mature cerebellar organoids that allow for the establishment of several classes of mature neurons during cerebellar differentiation and development, including the establishment of neural networks during whole-organoid maturation. This will provide a means to study the generation of several more mature cerebellar cell types, including Purkinje cells, granule cells and interneurons expression as well as neuronal communication for biomedical, clinical and pharmaceutical applications.

An Accurate and Fast 31P qNMR Assay Method for Oligonucleotide Therapeutics.

Chemically modified nucleic acid molecules have been developed as oligonucleotide therapeutics, and its assay is critical in quality assurance. The common DNA/RNA quantification method using UV-260 nm can lack accuracy because of structure modifications and the possible formation of higher-order structure (HOS). Additionally, process-associated water and counterions affect the accuracy in gravimetric analysis. Thus, to improve accuracy, efficiency, and flexibility, in this work a fast (<1 h) externally referenced 31P quantitative-NMR (qNMR) method was developed. The qNMR assay results agreed within 1-5% of the UV-260 nm results for the single-stranded DNA standards, confirming the method accuracy. Next, an NMR and UV comparison study was performed on intact oligonucleotide drug products. The 31P qNMR method showed 7 ± 2%, 8 ± 1%, and 12 ± 1% lower concentration values compared with drug product labels for eteplirsen, inotersen, and inclisiran, respectively. Meanwhile the UV-260 nm results showed 28 ± 3%, 10 ± 3%, and 10 ± 1% lower concentrations than the label for the same three drugs. The agreement between NMR and UV for phosphorothioate (PS)-based inotersen and mostly phosphodiester (PO)-based inclisiran suggest that the labeled concentration may have been obtained using different extinction coefficients. The underestimate of UV results for eteplirsen, which has a phosphorodiamidate morpholino oligomer (PMO) structure, suggests that the UV-260 nm extinction coefficient may need to be re-established for the PMO based oligonucleotide. Therefore, the 31P qNMR method could be a primary assay method for the oligonucleotide drug and reference standard.

Multislip-enabled morphing of all-inorganic perovskites.

All-inorganic lead halide perovskites (CsPbX3, X = Cl, Br or I) are becoming increasingly important for energy conversion and optoelectronics because of their outstanding performance and enhanced environmental stability. Morphing perovskites into specific shapes and geometries without damaging their intrinsic functional properties is attractive for designing devices and manufacturing. However, inorganic semiconductors are often intrinsically brittle at room temperature, except for some recently reported layered or van der Waals semiconductors. Here, by in situ compression, we demonstrate that single-crystal CsPbX3 micropillars can be substantially morphed into distinct shapes (cubic, L and Z shapes, rectangular arches and so on) without localized cleavage or cracks. Such exceptional plasticity is enabled by successive slips of partial dislocations on multiple [Formula: see text] systems, as evidenced by atomic-resolution transmission electron microscopy and first-principles and atomistic simulations. The optoelectronic performance and bandgap of the devices were unchanged. Thus, our results suggest that CsPbX3 perovskites, as potential deformable inorganic semiconductors, may have profound implications for the manufacture of advanced optoelectronics and energy systems.

Organophotocatalytic Remote Thiocyanation Reaction via Ring-Opening Functionalization of Cycloalkanols.

The remote C(sp3)-SCN bond formation via ring-opening functionalization of cycloalkanols with N-thiocyanatosaccharin as the precursor of SCN radicals and pyrylium salt as the organic photocatalyst under visible light has been developed. Thus, various terminal keto thiocyanates were prepared without transition metals and oxidants in moderate to good yields. The simplicity, wide substrate scope and mild conditions feature its synthetic application capability.

Insoluble Acyclic Cucurbit[n]uril-Type Receptors Capture Iodine from the Vapor Phase.

Nuclear energy makes large contributions toward meeting global energy needs, but societal concerns remain high given the impacts of the intended release of radioactive materials including 129I and 131I. In this paper we explore the use of a homologous series of acyclic CB[n] type hosts (H1 - H4) as adsorbents of iodine from the vapor phase. We find that H2 - H4, but not H1 - perform well in this application with uptake capacities of 2.2 g g-1, 1.5 g g-1, and 1.9 g g-1, respectively. The chemisorptive uptake process involves partial oxidation of catechol walled H2 to quinone walled host and capture of I3- and I5-. Solid H2 can be regenerated by treatment with Na2S2O4 and reused at least five times. The x-ray crystal structure of H2 is also reported.

Me3SiBr-promoted cascade electrophilic thiocyanation/cyclization of ortho-alkynylanilines to synthesize indole derivatives.

A Lewis acid-promoted electrophilic thiocyanation/cyclization of ortho-alkynylanilines for the synthesis of indole derivatives has been developed. The reaction utilizes Me3SiBr as the Lewis acid and N-thiocyanatosuccinimide as the thiocyanation reagent. A series of 2-aryl-3-thiocyanato indoles were prepared in moderate to high yields under mild conditions without metals and oxidants. It provides an efficient protocol for the construction of the indole skeleton and C-SCN and C-N bonds in one step as well.

Immune-stealth VP28-conjugated heparin nanoparticles for enhanced and reversible anticoagulation.

Heparins are a family of sulfated linear negatively charged polysaccharides that have been widely used for their anticoagulant, antithrombotic, antitumor, anti-inflammatory, and antiviral properties. Additionally, it has been used for acute cerebral infarction relief as well as other pharmacological actions. However, heparin's self-aggregated macrocomplex may reduce blood circulation time and induce life-threatening thrombocytopenia (HIT) complicating the use of heparins. Nonetheless, the conjugation of heparin to immuno-stealth biomolecules may overcome these obstacles. An immunostealth recombinant viral capsid protein (VP28) was expressed and conjugated with heparin to form a novel nanoparticle (VP28-heparin). VP28-heparin was characterized and tested to determine its immunogenicity, anticoagulation properties, effects on total platelet count, and risk of inducing HIT in animal models. The synthesized VP28-heparin trimeric nanoparticle was non-immunogenic, possessed an average hydrodynamic size (8.81 ± 0.58 nm) optimal for the evasion renal filtration and reticuloendothelial system uptake (hence prolonging circulating half-life). Additionally, VP28-heparin did not induce mouse death or reduce blood platelet count when administered at a high dosein vivo(hence reducing HIT risks). The VP28-heparin nanoparticle also exhibited superior anticoagulation properties (2.2× higher prothrombin time) and comparable activated partial thromboplastin time, but longer anticoagulation period when compared to unfractionated heparin. The anticoagulative effects of the VP28-heparin can also be reversed using protamine sulfate. Thus, VP28-heparin may be an effective and safe heparin derivative for therapeutic use.

Dual-band terahertz chiral metasurface absorber with enhanced circular dichroism based on temperature-tunable InSb for sensing applications.

Circular dichroism (CD) in terahertz (THz) regions has been widely used in biomonitoring, analytical chemistry, communication sensing, and other fields. Herein, we present a simple design for a dual-band THz chiral metasurface absorber (CMA) with a stronger CD effect based on temperature-tunable InSb for enhanced sensing applications. The proposed dual-band CMA consisted of a periodic array of the evolved C-shaped InSb adhered to a copper substrate. The designed CMA at 305 K achieved a right-handed circular polarization (RCP)-selective absorbance of 98.86% and 97.43% at 1.65 THz and 1.89 THz, respectively, and left-handed circular polarization (LCP) absorbance of 9.98% and 22.46%, respectively, and exhibited stronger CD values of 0.89 and 0.75. In addition, the CD properties of the designed CMA can be adjusted by changing the geometrical parameters of the unit-cell structure. The simulated electric field and power follow distributions indicate that this dual-band chiral-selective absorption of the designed CMA is due to the different plasma resonance mode excitations for the incident circular polarization (CP) wave. In addition, the CD properties of the designed CMA can be adjusted by changing the geometrical parameters of the unit-cell structure. Furthermore, CD spectra can be dynamically adjusted by varying the outside temperature and refraction index (RI) of the filled analytes. The designed dual-band CMA can function as a high-performance temperature sensor with sensitivities of 4.68 GHz K-1 and 5.52 GHz K-1 and also as an RI sensor with sensitivities of 1080 GHz RIU-1 and 860 GHz RIU-1, respectively. Our proposed tunable dual-band CMA with its exquisite performance has the potential to be widely applied in diverse areas such as detection, sensing, and other related optoelectronic fields.

Isolation of bacteria from Grifola frondosa cultivation on wood logs to find mycelial growth-promoting bacteria.

This study aimed to isolate bacteria that coexist with the edible mushroom Grifola frondosa when it is cultured on wood, and to determine their interactions; in turn, the aim was to find bacteria that stimulate mycelial growth so as to decrease the time required for spawn preparation on potato dextrose agar (PDA). Some Pseudomonas, Dyella, Bacillus, and Priestia spp. isolated from the cultivation surroundings of G. frondosa had a positive effect on the mycelial growth of the fungus in PDA. However, some isolated bacteria had a severe negative effect on the mycelial growth, especially Burkholderia spp. Thus, both mycelial-promoting bacteria and potentially pathogenic bacteria coexist with G. frondosa in cultivation. Enzyme activity assays indicated that some wood-degrading bacteria inhabit the cultivation surroundings of G. frondosa, and these bacteria probably help the fungus to degrade wood (especially cellulose).

Intersecting planetary health: Exploring the impacts of environmental stressors on wildlife and human health.

This comprehensive review articulates critical insights into the nexus of environmental stressors and their health impacts across diverse species, underscoring significant findings that reveal profound effects on both wildlife and human health systems. Central to our examination is the role of pollutants, climate variables, and pathogens in contributing to complex disease dynamics and physiological disruptions, with particular emphasis on immune and endocrine functions. This research brings to light emerging evidence on the severe implications of environmental pressures on a variety of taxa, including predatory mammals, raptorial birds, seabirds, fish, and humans, which are pivotal as indicators of broader ecosystem health and stability. We delve into the nuanced interplay between environmental degradation and zoonotic diseases, highlighting novel intersections that pose significant risks to biodiversity and human populations. The review critically evaluates current methodologies and advances in understanding the morphological, histopathological, and biochemical responses of these organisms to environmental stressors. We discuss the implications of our findings for conservation strategies, advocating for a more integrated approach that incorporates the dynamics of zoonoses and pollution control. This synthesis not only contributes to the academic discourse but also aims to influence policy by aligning with the Global Goals for Sustainable Development. It underscores the urgent need for sustainable interactions between humans and their environments, which are critical for preserving biodiversity and ensuring global health security. By presenting a detailed analysis of the interdependencies between environmental stressors and biological health, this review highlights significant gaps in current research and provides a foundation for future studies aimed at mitigating these pressing issues. Our study is significant as it proposes integrative and actionable strategies to address the challenges at the intersection of environmental change and public health, marking a crucial step forward in planetary health science.

Breathing in danger: Understanding the multifaceted impact of air pollution on health impacts.

Air pollution, a pervasive environmental threat that spans urban and rural landscapes alike, poses significant risks to human health, exacerbating respiratory conditions, triggering cardiovascular problems, and contributing to a myriad of other health complications across diverse populations worldwide. This article delves into the multifarious impacts of air pollution, utilizing cutting-edge research methodologies and big data analytics to offer a comprehensive overview. It highlights the emergence of new pollutants, their sources, and characteristics, thereby broadening our understanding of contemporary air quality challenges. The detrimental health effects of air pollution are examined thoroughly, emphasizing both short-term and long-term impacts. Particularly vulnerable populations are identified, underscoring the need for targeted health risk assessments and interventions. The article presents an in-depth analysis of the global disease burden attributable to air pollution, offering a comparative perspective that illuminates the varying impacts across different regions. Furthermore, it addresses the economic ramifications of air pollution, quantifying health and economic losses, and discusses the implications for public policy and health care systems. Innovative air pollution intervention measures are explored, including case studies demonstrating their effectiveness. The paper also brings to light recent discoveries and insights in the field, setting the stage for future research directions. It calls for international cooperation in tackling air pollution and underscores the crucial role of public awareness and education in mitigating its impacts. This comprehensive exploration serves not only as a scientific discourse but also as a clarion call for action against the invisible but insidious threat of air pollution, making it a vital read for researchers, policymakers, and the general public.

Interaction of titanium dioxide nanoparticles with PVC-microplastics and chromium counteracts oxidative injuries in Trachyspermum ammi L. by modulating antioxidants and gene expression.

The emergence of polyvinyl chloride (PVC) microplastics (MPs) as pollutants in agricultural soils is increasingly alarming, presenting significant toxic threats to soil ecosystems. Ajwain (Trachyspermum ammi L.), a plant of significant medicinal and culinary value, is increasingly subjected to environmental stressors that threaten its growth and productivity. This situation is particularly acute given the well-documented toxicity of chromium (Cr), which has been shown to adversely affect plant biomass and escalate risks to the productivity of such economically and therapeutically important species. The present study was conducted to investigate the individual effects of different levels of PVC-MPs (0, 2, and 4 mg L-1) and Cr (0, 150, and 300 mg kg-1) on various aspects of plant growth. Specifically, we examined growth and biomass, photosynthetic pigments, gas exchange attributes, oxidative stress responses, antioxidant compound activity (both enzymatic and nonenzymatic), gene expression, sugar content, nutritional status, organic acid exudation, and Cr accumulation in different parts of Ajwain (Trachyspermum ammi L.) seedlings, which were also exposed to varying levels of titanium dioxide (TiO2) nanoparticles (NPs) (0, 25, and 50 µg mL-1). Results from the present study showed that the increasing levels of Cr and PVC-MPs in soils significantly decreased plant growth and biomass, photosynthetic pigments, gas exchange attributes, sugars, and nutritional contents from the roots and shoots of the plants. Conversely, increasing levels of Cr and PVC-MPs in the soil increased oxidative stress indicators in term of malondialdehyde, hydrogen peroxide, and electrolyte leakage, and also increased organic acid exudation pattern in the roots of T. ammi seedlings. Interestingly, the application of TiO2-NPs counteracted the toxicity of Cr and PVC-MPs in T. ammi seedlings, leading to greater growth and biomass. This protective effect is facilitated by the NPs' ability to sequester reactive oxygen species, thereby reducing oxidative stress and lowering Cr concentrations in both the roots and shoots of the plants. Our research findings indicated that the application of TiO2-NPs has been shown to enhance the resilience of T. ammi seedlings to Cr and PVC-MPs toxicity, leading to not only improved biomass but also a healthier physiological state of the plants. This was demonstrated by a more balanced exudation of organic acids, which is a critical response mechanism to metal stress.

Multinuclear 1H/13C/15N chemical shift assignment of therapeutic octreotide acetate performed at natural abundance.

Octreotide acetate, the active pharmaceutical ingredient in the long-acting release (LAR) drug product Sandostatin®, is a cyclic octapeptide that mimics the naturally occurring somatostatin peptide hormone. Modern NMR can be a robust analytical method to identify and quantify octreotide molecules. Previous 1H chemical shift assignments were mostly performed in organic solvents, and no assignments for heteronuclear 13C, 15N, and aromatic 1H nuclei are available. Here, using state-of-the-art 1D and 2D homo- and heteronuclear NMR experiments, octreotide was fully assigned, including water exchangeable amide protons, in aqueous buffer except for 13CO and 15NH of F1, 15NH of C2, and 15NζHζ of K5 that were not observed because of water exchange or conformational exchange. The solution NMR spectra were then directly compared with 1D 1H/13C/15N solid-state NMR (SSNMR) spectra showing the potential applicability of 13C/15N SSNMR for octreotide drug product characterization.

Associations between an open-response situational judgment test and performance on OSCEs and fieldwork: implications for admissions decisions and matriculant diversity in an occupational therapy program.

BACKGROUND: Casper, an online open-response situational judgement test that assesses social intelligence and professionalism [1], is used in admissions to health professions programs. METHOD: This study (1) explored the incremental validity of Casper over grade point average (GPA) for predicting student performance on objective structured clinical examinations (OSCEs) and fieldwork placements within an occupational therapy program, (2) examined optimal weighting of Casper in GPA in admissions decisions using non-linear optimization and regression tree analysis to find the weights associated with the highest average competency scores, and (3) investigated whether Casper could be used to impact the diversity of a cohort selected for admission to the program. RESULTS: Multiple regression analysis results indicate that Casper improves the prediction of OSCE and fieldwork performance over and above GPA (change in Adj. R2 = 3.2%). Non-linear optimization and regression tree analysis indicate the optimal weights of GPA and Casper for predicting performance across fieldwork placements are 0.16 and 0.84, respectively. Furthermore, the findings suggest that students with a slightly lower GPA (e.g., 3.5-3.6) could be successful in the program as assessed by fieldwork, which is considered to be the strongest indicator of success as an entry-level clinician. In terms of diversity, no statistically significant differences were found between those actually admitted and those who would have been admitted using Casper. CONCLUSION: These results constitute preliminary validity evidence supporting the integration of Casper into applicant selection in an occupational therapy graduate program.

High-Resolution Metalens Imaging with Sequential Artificial Intelligence Models.

An analysis of the optical response of a GaN-based metalens was conducted alongside the utilization of two sequential artificial intelligence (AI) models in addressing the occasional issues of blurriness and color cast in captured images. The optical loss of the metalens in the blue spectral range was found to have resulted in the color cast of images. Autoencoder and CodeFormer sequential models were employed in order to correct the color cast and reconstruct image details, respectively. Said sequential models successfully addressed the color cast and reconstructed details for all of the allocated face image categories. Subsequently, the CIE 1931 chromaticity diagrams and peak signal-to-noise ratio analysis provided numerical evidence of the AI models' effectiveness in image reconstruction. Furthermore, the AI models can still repair the image without blue information. Overall, the integration of metalens and artificial intelligence models marks a breakthrough in enhancing the performance of full-color metalens-based imaging systems.

Directly Unveiling the Energy Transfer Dynamics between Alq3 Molecules and Si by Ultrafast Optical Pump-Probe Spectroscopy.

The energy transfer (ET) between organic molecules and semiconductors is a crucial mechanism for enhancing the performance of semiconductor-based optoelectronic devices, but it remains undiscovered. Here, ultrafast optical pump-probe spectroscopy was utilized to directly reveal the ET between organic Alq3 molecules and Si semiconductors. Ultrathin SiO2 dielectric layers with a thickness of 3.2-10.8 nm were inserted between Alq3 and Si to prevent charge transfer. By means of the ET from Alq3 to Si, the SiO2 thickness-dependent relaxation dynamics of photoexcited carriers in Si have been unambiguously observed on the transient reflectivity change (ΔR/R) spectra, especially for the relaxation process on a time scale of 200-350 ps. In addition, these findings also agree with the results of our calculation in a model of long-range dipole-dipole interactions, which provides critical information for developing future optoelectronic devices.

Effectiveness of the lay health advisor program on oral function and quality of life in aboriginal older adults: A randomized controlled trial.

BACKGROUND: Aboriginal older adults residing in remote areas have poor oral function due to inadequate access to healthcare services. Lay health advisor (LHA) strategies can fill capacity shortages of healthcare professionals in rural communities and increase population acceptance of health care or healthy behaviours. OBJECTIVE(S): To evaluate the effectiveness the LHA program on oral function and oral health-related quality of life (OHRQoL) among older adults in aboriginal community. METHODS: Participants were randomly assigned to an experimental group (EG; n = 122) and a control group (CG; n = 118). All participants performed oral exercises, and the EG received additional one-on-one 30-min lessons by an LHA over 4 weeks. Data were collected through face-to-face interview and oral examination. The generalized estimating equation model was used to analyse changes in outcomes over time. RESULTS: The EG exhibited significantly greater improvement in swallowing (ß = .63) at the 6-month follow-up and in masticatory performance (ß = .52) and pronunciation of the syllable/pa/ (ß = 2.65) at the 2-week follow-up than the CG did. The EG had a significantly lower plaque control record (ß = -.14) and plaque index (ß = -.30) at the 3-month follow-up than the CG did. Moreover, the OHRQoL was significantly increased at 6-months follow-up in the EG (p = .010). CONCLUSION: The LHA program had positive effects on chewing, swallowing and plaque control in aboriginal older adults. LHA group also experienced positive long-term effect on OHRQoL after intervention.

A single-nucleus transcriptomic atlas characterizes cell types and their molecular features in the ovary of adult Nile tilapia.

In fish species, there is limited analysis of signature transcriptome profiles at the single-cell level in gonadal cells. Here, the molecular signatures of distinct ovarian cell categories in adult Nile tilapia (Oreochromis niloticus) were analysed using single-nucleus RNA sequencing (snRNA-seq). We identified four cell types (oogonia, oocytes, granulosa cell, and thecal cell) based on their specifically expressed genes and biological functions. Similarly, we found some key pathways involved in ovarian development that may affect germline-somatic interactions. A cell-to-cell communication network between the distinct cell types was constructed. We found that the bidirectional communication is mandatory for the development of germ cells and somatic cells in fish ovaries, and the granulosa cells and thecal cells play a central regulating role in the cell network in fish ovary. Additionally, we identified some novel candidate marker genes for various types of ovarian cells and also validated them using in situ hybridization. Our work reveals an ovarian atlas at the cellular and molecular levels and contributes to providing insights into oogenesis and gonad development in fish.

Enhanced remediation of PFAS-metal co-contaminated soil by ceramsite supported Fe3O4-MoS2 heterojunction as a high-performance piezocatalyst.

In this study, a novel piezoremediation system was developed to remediate an actual soil co-polluted by high contents of per- and polyfluoroalkyl substances (PFAS, 5725 µg/kg soil) and heavy metals (6455 mg/kg soil). Two piezocatalysts, MoS2/ceramsite (MC) and Fe3O4-MoS2/ceramsite (FMC), were synthesized using a facile hydrothermal-coprecipitation method. These two materials were employed to treat the co-contaminated soil in soil slurry environment under sonication. FMC exhibited significantly higher piezoremediation performance than MC, wherein 91.6% of PFAS, 97.8% of Cr6+ ions and 81% of total metals (Cr, Cu, Zn and Ni) were removed from the soil after 50 min of the FMC piezoremediation process. FMC also exhibited the advantages of easy separation from the slurry phase and excellent reusability. In comparison with MC, the Fe3O4-MoS2 heterojunction in FMC can stabilize MoS2 particles on the surface of ceramsite granules, promote the separation of electron/hole pairs, accelerate charge transfer, therefore enhancing piezocatalytic performance. The electron spin resonance analysis and free radical quenching tests show that •OH was the dominant oxidative radical responsible for PFAS degradation. The count of bacteria and the bacterial community structure in the treated soil can be basically restored to the initial states after 30 days of incubation under nutrient stimulation. Overall, this study not only provides a deep insight on soil remediation process, but also offers an efficient and reliable technique for simultaneous decontamination of organic and metal pollutants in soil.