The Incorporation of Sulfonated PAF Enhances the Proton Conductivity of Nafion Membranes at High Temperatures.

Nafion membranes are widely used as proton exchange membranes, but their proton conductivity deteriorates in high-temperature environments due to the loss of water molecules. To address this challenge, we propose the utilization of porous aromatic frameworks (PAFs) as a potential solution. PAFs exhibit remarkable characteristics, such as a high specific surface area and porosity, and their porous channels can be post-synthesized. Here, a novel approach was employed to synthesize a PAF material, designated as PAF-45D, which exhibits a specific surface area of 1571.9 m2·g-1 and possesses the added benefits of facile synthesis and a low cost. Subsequently, sulfonation treatment was applied to PAF-45D in order to introduce sulfonic acid groups into its pores, resulting in the formation of PAF-45DS. The successful incorporation of sulfonic groups was confirmed through TG, IR, and EDS analyses. Furthermore, a novel Nafion composite membrane was prepared by incorporating PAF-45DS. The Nyquist plot of the composite membranes demonstrates that the sulfonated PAF-45DS material can enhance the proton conductivity of Nafion membranes at high temperatures. Specifically, under identical film formation conditions, doping with a 4% mass fraction of PAF-45DS, the conductivity of the Nafion composite membrane increased remarkably from 2.25 × 10-3 S·cm-1 to 5.67 × 10-3 S·cm-1, nearly 2.5 times higher. Such promising and cost-effective materials could be envisioned for application in the field of Nafion composite membranes.

Burden of non-communicable diseases attributed to alcohol consumption in 2019 for the Brazilian Unified Health System.

OBJECTIVE: To estimate the health and economic burden of non-communicable diseases (NCDs) attributed to alcohol consumption in 2019 for the Brazilian Unified Health System (SUS) stratified by states. STUDY DESIGN: Observational, descriptive, and ecological study. METHODS: We used population attributable fractions (PAFs) of NCDs due to alcohol consumption from the Global Burden of Disease study. We applied the PAFs to the costs of hospitalizations and outpatient procedures of medium to high complexity paid by SUS for each outcome, obtained from official databases. We also calculated the disability-adjusted life years (DALYs) and mortality caused by alcohol-related NCDs. We converted the costs into international dollars (Int$) using the purchasing parity power in 2019. RESULTS: Alcohol-related NCDs accounted for 8.48% of deaths and 7.0% of DALYs among men, and 1.33% of deaths and 1.6% of DALYs among women. The main diseases were substance use, digestive, and neoplastic diseases. The SUS spent Int$202.0 million on alcohol-related NCDs, mostly on hospitalizations. The highest health burden was observed in the states of the Northeast region, and the highest expenses in the states from the South. The burden and cost values varied by sex, age group, and state. CONCLUSION: The study showed that alcohol consumption has a significant impact on Brazilian population morbidity and mortality and SUS expenditures, especially among men. These results can support policies for the prevention and control of alcohol consumption and health promotion at the subnational level, prioritizing strategies that are more appropriate to local realities.

Photoactivatable Fluorophores for Bioimaging Applications.

Photoactivatable fluorophores provide the opportunity to switch fluorescence on exclusively in a selected area within a sample of interest at a precise interval of time. Such a level of spatiotemporal fluorescence control enables the implementation of imaging schemes to monitor dynamic events in real time and visualize structural features with nanometer resolution. These transformative imaging methods are contributing fundamental insights on diverse cellular processes with profound implications in biology and medicine. Current photoactivatable fluorophores, however, become emissive only after the activation event, preventing the acquisition of fluorescence images and, hence, the visualization of the sample prior to activation. We developed a family of photoactivatable fluorophores capable of interconverting between emissive states with spectrally resolved fluorescence, instead of switching from a nonemissive state to an emissive one. We demonstrated that our compounds allow the real-time monitoring of molecules diffusing across the cellular blastoderm of developing embryos as well as of polymer beads translocating along the intestinal tract of live nematodes. Additionally, they also permit the tracking of single molecules in the lysosomal compartments of live cells and the visualization of these organelles with nanometer resolution. Indeed, our photoactivatable fluorophores may evolve into invaluable analytical tools for the investigation of the fundamental factors regulating the functions and structures of cells at the molecular level.

Ultrasound diagnosis of non-mass MRI-detected lesions.

Magnetic resonance imaging (MRI)-detected lesions are often category 2 or 3 lesions on initial ultrasound examination. In addition, in the case of new non-mass lesions detected on MRI, one would expect to find lesions with ductal dilatation with minimal secretory accumulation, single short lesions with ductal dilatation, cyst-like lesions less than 5 mm in size, mammary gland-like lesions less than 8 mm in size, and very indistinct lesions. Detection is expected to be even more difficult. Currently, there are no clear uniform criteria for the indication of second-look ultrasonography (US) for MRI-detected lesions, so it is not possible to make a general comparison, but recent studies have indicated that the ratio of mass to non-mass MRI-detected lesions is 7:3. And it has been pointed out that the percentage of malignancy is about 30% for each. Before about 2012, the US detection rate was about 70%, and MRI-guided biopsies of undetected lesions showed a small percentage of malignant lesions. Therefore, some observers believe that lesions not detected on US should be followed up, while others believe that MRI-guided biopsy should be performed. Recently, however, the use of surrounding anatomical structures as landmarks for second-look US has increased the detection rate to as high as 87-99%, and the percentage of malignancy remains the same. In addition, recent surveillance of high-risk breast cancer requires careful management of MRI-detected lesions. In this review, we will discuss the literature on MRI-detected lesions and describe ultrasound techniques to accurately detect small lesions and reliably reveal pale lesions based on their structural differences from their surroundings.

Resource predictability modulates spatial-use networks in an endangered scavenger species.

BACKGROUND: Changes in human-induced resource availability can alter the behaviour of free-living species and affect their foraging strategies. The future European Landfill Waste Directive and Circular Economy Action Plan will reduce the number of predictable anthropogenic food subsidies (PAFS), above all, by closing landfills to preclude negative effects on human health. Obligate avian scavengers, the most threatened group of birds worldwide, are the most likely group of species that will be forced to change their behaviour and use of space in response to landfill site closures. Here, we examine the possible consequences of these management decisions on the foraging patterns of Egyptian vultures (Neophron percnopterus) in an expanding population in the Iberian Peninsula. METHODS: We tracked 16 individuals in 2018-2021, including breeders and non-breeders, and, using a combination of spatial-use and spatial-network modelling, assessed landscape connectivity between key resources based on movement patterns. We then carried out simulations of future scenarios based on the loss of PAFS to predict likely changes in the movement patterns of both non-breeders and breeders. RESULTS: Our results show that foraging strategies in non-breeders and breeders differ significantly: non-breeders performed more dispersal movements than breeding birds across a spatial-use network. Non-breeding and breeding networks were found to be vulnerable to the removal of central foraging areas containing landfill sites, a highly predictable resource, while perturbation analysis showed dissimilar foraging responses to the gradual reduction of other predictable resources. Under a context of the non-availability of landfills for breeders and non-breeders, vultures will increase their use of extensive livestock as a trophic resource. CONCLUSIONS: Future environmental policies should thus extend the areas used by scavengers in which livestock carcasses are allowed to remain in the wild, a strategy that will also mitigate the lack of food caused by any reduction in available waste if landfills close. In general, our results emphasize the capabilities of a spatial network approaches to address questions on movement ecology. They can be used to infer the behavioural response of animal species and, also demonstrate the importance of applying such approaches to endangered species conservation within a context of changing humanized scenarios.

Recommendations for progression criteria during external randomised pilot trial design, conduct, analysis and reporting.

BACKGROUND: External randomised pilot trials aim to assess whether a future definitive Randomised Controlled Trial (RCT) is feasible. Prespecified progression criteria help guide the interpretation of pilot trial findings to decide whether, and how, a definitive RCT should be conducted. This commentary presents a set of proposed recommendations for progression criteria to guide researchers when (i) designing, (ii) conducting, (iii) analysing and (iv) reporting external randomised pilot trials. METHODS: Recommendations were developed following a mixed methods approach. This involved (i) a methodological review of pilot trial publications, (ii) a cross-sectional study of pilot trial research funding applications, (iii) qualitative interviews with pilot trial researchers and (iv) a survey of corresponding authors of identified pilot trial publications. Initial recommendations were refined following two consultation stakeholder workshops held in July 2022. Recommendations for progression criteria for external randomised pilot trials: i. DESIGN: consider progression criteria from the earliest opportunity; map progression criteria to feasibility objectives; consider quantitative and qualitative interpretations of feasibility; provide justification; develop guidelines rather than rules; seek input from relevant stakeholders. ii. Conduct: regularly monitor pilot trial data against progression criteria. iii. ANALYSIS: avoid considering each progression criterion in isolation; engage in discussion with relevant stakeholders; consider context and other factors external to the pilot trial; consider feasibility (can we?) and progression (will we?). iv. Reporting: we propose a reporting checklist in relation to progression criteria and recommend reporting in a table format for clarity. CONCLUSION: These recommendations provide a helpful resource for researchers to consider progression criteria at different stages of external randomised pilot trials. We have produced a simple infographic tool to summarise these recommendations for researchers to refer to. Further research is needed to evaluate whether these proposed recommendations should inform future development, or update, of established guidelines for the design, conduct, analysis and reporting of external randomised pilot trials.

Photoactivatable BODIPYs for Live-Cell PALM.

Photoactivated localization microscopy (PALM) relies on fluorescence photoactivation and single-molecule localization to overcome optical diffraction and reconstruct images of biological samples with spatial resolution at the nanoscale. The implementation of this subdiffraction imaging method, however, requires fluorescent probes with photochemical and photophysical properties specifically engineered to enable the localization of single photoactivated molecules with nanometer precision. The synthetic versatility and outstanding photophysical properties of the borondipyrromethene (BODIPY) chromophore are ideally suited to satisfy these stringent requirements. Specifically, synthetic manipulations of the BODIPY scaffold can be invoked to install photolabile functional groups and photoactivate fluorescence under photochemical control. Additionally, targeting ligands can be incorporated in the resulting photoactivatable fluorophores (PAFs) to label selected subcellular components in live cells. Indeed, photoactivatable BODIPYs have already allowed the sub-diffraction imaging of diverse cellular substructures in live cells using PALM and can evolve into invaluable analytical probes for bioimaging applications.

Gold Nanoparticles Immobilized in Porous Aromatic Frameworks with Abundant Metal Anchoring Sites as Heterogeneous Nanocatalysts.

Porous aromatic frameworks (PAFs) with rich metal coordination sites are highly effective support materials for gold nanoparticles (AuNPs), which would not only prevent AuNPs agglomeration but also facilitate mass transfer during the catalytic process. In this work, PAF-160, -161, and -162 bearing diphosphine units are synthesized via the Friedel-Crafts alkylation reaction to act as efficient platforms for AuNPs immobilization. These PAFs possess high surface areas (up to 655 m2 g-1) together with excellent stabilities, and the different linkage lengths between P centers allow more scattered and accessible sites for gold coordination. In the resultant Au-PAFs, AuNPs with uniform sizes are stabilized dispersedly. The catalytic performances of these Au-PAFs are monitored by the reduction of 4-nitrophenol (4-NP), and all materials exhibit excellent catalytic activities on the reduction of 4-NP, especially Au-PAF-162 with the apparent rate constant (kapp) up to 0.019 s-1. Additionally, the reductions of various nitroarenes with different functional groups are explored and all Au-PAFs can convert most nitroaromatic derivatives to the corresponding arylamines with high conversions of 99%, in which the reaction mechanism is also proposed. Furthermore, a continuous catalytic device with Au-PAF-160 catalyst is explored, and Au-PAF-160 can convert 1-chloro-4-nitrobenzene, 2,6-dichoronitrobenzene and 1-chloro-2,4-dinitrobenzene into the corresponding amines in sequence in the continuous flow catalytic experiments. This work has enriched the variety of porous materials for noble metal immobilization and promotes their applications in heterogeneous catalysis.

PafS Containing GGDEF-Domain Regulates Life Activities of Pseudomonas glycinae MS82.

Cyclic dimeric guanosine monophosphate (c-di-GMP) is synthesized by diguanylate cyclase (DGC) with the GGDEF domain. As a ubiquitous bacterial second messenger, it regulates diverse life-activity phenotypes in some bacteria. Although 38 genes encoding GGDEF-domain-containing proteins have been identified in the genome of the Pseudomonas glycinae strain MS82, whether c-di-GMP functions as a facilitator or repressor of life-activity phenotypes is poorly understood. In this study, one of the 38 genes containing a GGDEF domain in MS82, PafS was investigated to explore its regulatory function in bacterial life activities. The PafS-deletion mutant ΔPafS and reversion mutant PafS-comp were constructed by the method of biparental conjugation and homologous recombination. The life activities of the mutants, such as antifungal activity, biofilm formation ability, polysaccharide content, and motor behavior, were explored. The results showed that all life-activity phenotypes were significantly reduced after knocking out PafS, whereas all were significantly restored to a similar level to that of MS82 after the complementation of PafS. These results suggested that PafS plays an important role in the regulation of a range of cellular activities by c-di-GMP in P. glycinae MS82.

Sonogashira Synthesis of New Porous Aromatic Framework-Entrapped Palladium Nanoparticles as Heterogeneous Catalysts for Suzuki-Miyaura Cross-Coupling.

Palladium nanoparticles entrapped in porous aromatic frameworks (PAFs) or covalent organic frameworks may promote heterogeneous catalytic reactions. However, preparing such materials as active nanocatalysts usually requires additional steps for palladium entrapment and reduction. This paper reports as a new approach, a simple procedure leading to the self-entrapment of Pd nanoparticles within the PAF structure. Thus, the selected Sonogashira synthesis affords PAF-entrapped Pd nanoparticles that can catalyze the C-C Suzuki-Miyaura cross-coupling reactions. Following this new concept, PAFs were synthesized via Sonogashira cross-coupling of the tetraiodurated derivative of tetraphenyladamantane or spiro-9,9'-bifluorene with 1,6-diethynylpyrene, then characterized them using powder X-ray diffraction, diffuse reflectance infrared Fourier transform spectroscopy, X-ray photoelectron spectroscopy, high-resolution scanning transmission electron microscopy, and textural properties (i.e., adsorption-desorption isotherms). The PAF-entrapped Pd nanocatalysts showed high catalytic activity in Suzuki-Miyaura coupling reactions (demonstrated by preserving the turnover frequency values) and stability (demonstrated by palladium leaching and recycling experiments). This new approach presents a new class of PAFs with unique structural, topological, and compositional complexities as entrapped metal nanocatalysts or for other diverse applications.

GPS tracking reveals landfill closures induce higher foraging effort and habitat switching in gulls.

BACKGROUND: Landfills are a major subsidy for some animals, with implications for their life history and demography. Gulls feed extensively on food from landfills and closures are expected to have ecological consequences, but how this influences movement ecology is virtually unknown. METHODS: We used GPS-tracking to quantify foraging behaviour and habitat choice of lesser black-backed gulls (Larus fuscus) breeding at two colonies before and after closure of two nearby landfills. RESULTS: Following closure, gulls from both colonies travelled further and for longer to forage. Gulls also changed habitat selection, although this differed by colony - birds from one colony shifted to agricultural habitats, while at the other, increased their use of urban areas. These behavioural responses had no effect on adult body condition but hint at potential direct effects of higher foraging costs and indirect impacts by shifting to new habitats. CONCLUSIONS: Our results demonstrate how landfill availability influences gull foraging movements and habitat selection. We also emphasize the value of biologging to detect rapid behavioural responses in contrast to more conventional demographic approaches, which is especially important for animals that spend the majority of their lives away from direct observation.

An appraisal of allergic disorders in India and an urgent call for action.

India is the second most populous country in the world with a population of nearly 1.3 billion, comprising 20% of the global population. There are an estimated 37.5 million cases of asthma in India, and recent studies have reported a rise in prevalence of allergic rhinitis and asthma. Overall, 40-50% of paediatric asthma cases in India are uncontrolled or severe. Treatment of allergic rhinitis and asthma is sub-optimal in a significant proportion of cases due to multiple factors relating to unaffordability to buy medications, low national gross domestic product, religious beliefs, myths and stigma regarding chronic ailment, illiteracy, lack of allergy specialists, and lack of access to allergen-specific immunotherapy for allergic rhinitis and biologics for severe asthma. High quality allergen extracts for skin tests and adrenaline auto-injectors are currently not available in India. Higher postgraduate specialist training programmes in Allergy and Immunology are also not available. Another major challenge for the vast majority of the Indian population is an unacceptably high level of exposure to particulate matter (PM)2.5 generated from traffic pollution and use of fossil fuel and biomass fuel and burning of incense sticks and mosquito coils. This review provides an overview of the burden of allergic disorders in India. It appraises current evidence and justifies an urgent need for a strategic multipronged approach to enhance quality of care for allergic disorders. This may include creating an infrastructure for education and training of healthcare professionals and patients and involving regulatory authorities for making essential treatments accessible at subsidised prices. It calls for research into better phenotypic characterisation of allergic disorders, as evidence generated from high income western countries are not directly applicable to India, due to important confounders such as ethnicity, air pollution, high rates of parasitic infestation, and other infections.

Highly Porous Organic Polymers for Hydrogen Fuel Storage.

Hydrogen (H2) is one of the best candidates to replace current petroleum energy resources due to its rich abundance and clean combustion. However, the storage of H2 presents a major challenge. There are two methods for storing H2 fuel, chemical and physical, both of which have some advantages and disadvantages. In physical storage, highly porous organic polymers are of particular interest, since they are low cost, easy to scale up, metal-free, and environmentally friendly. In this review, highly porous polymers for H2 fuel storage are examined from five perspectives: (a) brief comparison of H2 storage in highly porous polymers and other storage media; (b) theoretical considerations of the physical storage of H2 molecules in porous polymers; (c) H2 storage in different classes of highly porous organic polymers; (d) characterization of microporosity in these polymers; and (e) future developments for highly porous organic polymers for H2 fuel storage. These topics will provide an introductory overview of highly porous organic polymers in H2 fuel storage.

The Impact of Risk Factors for Coronary Heart Disease on Related Disability in Older Irish Adults.

OBJECTIVE: The aim of this study is to examine the prevalence of coronary heart disease (CHD)-related disability (hereafter also "disability") and the impact of CHD risk factors on disability in older adults in the Republic of Ireland (ROI) and Northern Ireland (NI). METHOD: Population attributable fractions were calculated using risk factor relative risks and disability prevalence derived from The Irish Longitudinal Study on Ageing and the Northern Ireland Health Survey. RESULTS: Disability was significantly lower in ROI (4.1% vs. 8.8%). Smoking and diabetes prevalence rates, and the fraction of disability that could be attributed to smoking (ROI: 6.6%; NI: 6.1%), obesity (ROI: 13.8%; NI: 11.3%), and diabetes (ROI: 6.2%; NI: 7.2%), were comparable in both countries. Physical inactivity (31.3% vs. 54.8%) and depression (10.2% vs. 17.6%) were lower in ROI. Disability attributable to depression (ROI: 16.3%; NI: 25.2%) and physical inactivity (ROI: 27.5%; NI: 39.9%) was lower in ROI. DISCUSSION: Country-specific similarities and differences in the prevalence of disability and associated risk factors will inform public health and social care policy in both countries.