From biomineralization to synthesis, organic additives provide an effective means of controlling crystallization processes. There is growing evidence that these additives are often occluded within ...the crystal lattice. This promises an elegant means of creating nanocomposites and tuning physical properties. Here we use the incorporation of sulfonated fluorescent dyes to gain new understanding of additive occlusion in calcite (CaCO
), and to link morphological changes to occlusion mechanisms. We demonstrate that these additives are incorporated within specific zones, as defined by the growth conditions, and show how occlusion can govern changes in crystal shape. Fluorescence spectroscopy and lifetime imaging microscopy also show that the dyes experience unique local environments within different zones. Our strategy is then extended to simultaneously incorporate mixtures of dyes, whose fluorescence cascade creates calcite nanoparticles that fluoresce white. This offers a simple strategy for generating biocompatible and stable fluorescent nanoparticles whose output can be tuned as required.
NH3-Selective Catalytic Reduction (NH3-SCR) is a widely used technology for NO x reduction in the emission control systems of heavy duty diesel vehicles. Copper-based ion exchanged zeolites and in ...particular Cu-SSZ-13 (CHA framework) catalysts show both exceptional activity and hydrothermal stability for this reaction. In this work, we have studied the origin of the SCR activity of Cu-SSZ-13 as evidenced from a combination of synchrotron-based and laboratory techniques. Synchrotron-based in situ XAFS/XRD measurements were used to provide complementary information on the local copper environment under realistic NH3-SCR conditions. Crucial then to the catalytic activity of Cu-SSZ-13 is the local environment of the copper species, particularly in the zeolite. Cu-SSZ-13 contains mononuclear Cu2+ species, located in the face of the double-6-ring subunit of the zeolite after calcination where it remains under reaction conditions. At lower temperatures (with low activity), XAFS and XRD data revealed a conformational change in the local geometry of the copper from a planar form toward a distorted tetrahedron as a result of a preferential interaction with NH3. This process appears necessary for activity, but results in a stymieing of activity at low temperatures. At higher temperatures, the Cu2+ possess a local coordination state akin to that seen after calcination.
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IJS, KILJ, NUK, PNG, UL, UM
The purinergic receptor subtype 7 (P2X7R) represents a novel molecular target for imaging neuroinflammation via PET. GSK1482160, a potent P2X7R antagonist, has high receptor affinity, high ...blood-brain barrier penetration, and the ability to be radiolabeled with 11C. We report the initial physical and biologic characterization of this novel ligand. Methods:11C-GSK1482160 was synthesized according to published methods. Cell density studies were performed on human embryonic kidney cell lines expressing human P2X7R (HEK293-hP2X7R) and underwent Western blotting, an immunofluorescence assay, and radioimmunohistochemistry analysis using P2X7R polyclonal antibodies. Receptor density and binding potential were determined by saturation and association-disassociation kinetics, respectively. Peak immune response to lipopolysaccharide treatment in mice was determined in time course studies and analyzed via Iba1 and P2X7R Western blotting and Iba1 immunohistochemistry. Whole-animal biodistribution studies were performed on saline- or lipopolysaccharide-treated mice at 15, 30, and 60 min after radiotracer administration. Dynamic in vivo PET/CT was performed on the mice at 72 h after administration of saline, lipopolysaccharide, or lipopolysaccharide + blocking, and 2-compartment, 5-parameter tracer kinetic modeling of brain regions was performed. Results: P2X7R changed linearly with concentrations or cell numbers. For high-specific-activity 11C-GSK1482160, receptor density and Kd were 1.15 ± 0.12 nM and 3.03 ± 0.10 pmol/mg, respectively, in HEK293-hP2X7R membranes. Association constant kon, dissociation constant koff, and binding potential (kon/koff) in HEK293-hP2X7R cells were 0.2312 ± 0.01542 min-1⋅nM-1, 0.2547 ± 0.0155 min-1, and 1.0277 ± 0.207, respectively. Whole-brain Iba1 expression in lipopolysaccharide-treated mice peaked by 72 h on immunohistochemistry, and Western blot analysis of P2X7R for saline- and lipopolysaccharide-treated brain sections showed a respective 1.8- and 1.7-fold increase in signal enhancement at 72 h. Biodistribution of 11C-GSK1482160 in saline- and lipopolysaccharide-treated mice at 72 h was statistically significant across all tissues studied. In vivo dynamic 11C-GSK1482160 PET/CT of mice at 72 h after administration of saline, lipopolysaccharide, or lipopolysaccharide + blocking showed a 3.2-fold increase and 97% blocking by 30 min. The total distribution volumes for multiple cortical regions and the hippocampus showed statistically significant increases and were blocked by an excess of authentic standard GSK1482160. Conclusion: The current study provides compelling data that support the suitability of 11C-GSK1482160 as a radioligand targeting P2X7R, a biomarker of neuroinflammation.
Since 2010, UK social policy has been dominated by austerity and welfare reform. These policy platforms sit on a wider set of shifts in policy framings, in terms of both understanding the issue of ...poverty and the most effective solutions to it. The resulting strategies employed have had significant impacts on children and their household incomes. Within the context of the changing nature of state welfare and the drive for more privatised (non-state) provision, this paper focuses on the effects of this on assistance to children in particular, employing charitable food banks as a case study. Empirical data from the UK's largest food bank organisation (the Trussell Trust Foodbank Network) are explored to chart the rise of this provision as an example of the increasingly important role charitable organisations are playing in caring for children in the face of a reduced welfare state. The results show that both in mean and absolute terms, provision of food parcels to children by charitable foodbanks has grown considerably since the impacts of austerity, welfare reform and rising costs of living kicked in (2012/13). The results indicate that foodbanks are playing a bigger role in the provision of care to children generally in this context, but particularly where childhood deprivation is high. This paper furthers geographical discussions about the changing nature of care for those in or at risk of poverty, focusing on the increased vulnerability of children that has resulted from recent social policy shifts. Food banks form a particularly high-profile example of the rising prominence of charitable care in the context of an increasingly reduced welfare state. By discussing some of the key challenges of this provision, the paper also facilitates critical thinking about the issues that the contemporary shift away from universal social security and public care services might raise.
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BFBNIB, DOBA, FSPLJ, FZAB, GIS, IJS, IZUM, KILJ, NLZOH, NMLJ, NUK, OILJ, PILJ, PNG, SAZU, SBCE, SBMB, UILJ, UKNU, UL, UM, UPUK
Quantitative real-time PCR (qPCR) assays that target the human-associated HF183 bacterial cluster within members of the genus Bacteroides are among the most widely used methods for the ...characterization of human fecal pollution in ambient surface waters. In this study, we show that a current TaqMan HF183 qPCR assay (HF183/BFDrev) routinely forms nonspecific amplification products and introduce a modified TaqMan assay (HF183/BacR287) that alleviates this problem. The performance of each qPCR assay was compared in head-to-head experiments investigating limits of detection, analytical precision, predicted hybridization to 16S rRNA gene sequences from a reference database, and relative marker concentrations in fecal and sewage samples. The performance of the modified HF183/BacR287 assay is equal to or improves upon that of the original HF183/BFDrev assay. In addition, a qPCR chemistry designed to combat amplification inhibition and a multiplexed internal amplification control are included. In light of the expanding use of PCR-based methods that rely on the detection of extremely low concentrations of DNA template, such as qPCR and digital PCR, the new TaqMan HF183/BacR287 assay should provide more accurate estimations of human-derived fecal contaminants in ambient surface waters.
Population-level estimates of species' distributions can reveal fundamental ecological processes and facilitate conservation. However, these may be difficult to obtain for mobile species, especially ...colonial central-place foragers (CCPFs; e.g., bats, corvids, social insects), because it is often impractical to determine the provenance of individuals observed beyond breeding sites. Moreover, some CCPFs, especially in the marine realm (e.g., pinnipeds, turtles, and seabirds) are difficult to observe because they range tens to ten thousands of kilometers from their colonies. It is hypothesized that the distribution of CCPFs depends largely on habitat availability and intraspecific competition. Modeling these effects may therefore allow distributions to be estimated from samples of individual spatial usage. Such data can be obtained for an increasing number of species using tracking technology. However, techniques for estimating population-level distributions using the telemetry data are poorly developed. This is of concern because many marine CCPFs, such as seabirds, are threatened by anthropogenic activities. Here, we aim to estimate the distribution at sea of four seabird species, foraging from approximately 5,500 breeding sites in Britain and Ireland. To do so, we GPS-tracked a sample of 230 European Shags Phalacrocorax aristotelis, 464 Black-legged Kittiwakes Rissa tridactyla, 178 Common Murres Uria aalge, and 281 Razorbills Alca torda from 13, 20, 12, and 14 colonies, respectively. Using Poisson point process habitat use models, we show that distribution at sea is dependent on (1) density-dependent competition among sympatric conspecifics (all species) and parapatric conspecifics (Kittiwakes and Murres); (2) habitat accessibility and coastal geometry, such that birds travel further from colonies with limited access to the sea; and (3) regional habitat availability. Using these models, we predict space use by birds from unobserved colonies and thereby map the distribution at sea of each species at both the colony and regional level. Space use by all four species' British breeding populations is concentrated in the coastal waters of Scotland, highlighting the need for robust conservation measures in this area. The techniques we present are applicable to any CCPF.
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BFBNIB, FZAB, GIS, IJS, INZLJ, KILJ, NLZOH, NMLJ, NUK, OILJ, PNG, SAZU, SBCE, SBMB, UL, UM, UPUK, ZRSKP
Prevalence of alcohol-related harms in England are among the highest in Europe and represents an important policy issue. Understanding how alcohol-related trends vary by demographic factors is ...important for informing policy debates. The aim of our study was to examine trends in alcohol-related admissions to hospital in England, with a focus on variations by sex, age and socioeconomic deprivation.
We used data on hospital admissions for England for the financial years 2002/03 to 2013/14. Our four main outcome variables were acute and chronic conditions wholly and partially attributable to alcohol consumption. We also looked at four specific conditions wholly attributable to alcohol. Socioeconomic deprivation was measured using the English Indices of Deprivation of a patient's residence (categorised by quintile). We calculated crude rates, age-specific rates (visualised by Lexis plots) and directly standardised rates by deprivation category, separately for males and females.
Total admissions for all alcohol-attributable admissions increased from 201,398 in 2002/03 to 303,716 in 2013/14. The relative increase of these admissions was larger than compared to non-alcohol attributable admissions. Acute admissions wholly attributable to alcohol had the largest relative increase of our outcome measures, and displayed a bimodal distribution with higher rates in adolescence/young adults and middle age. Chronic conditions wholly attributable to alcohol were concentrated in middle age (particularly males). While admission rates were generally higher for males, females had higher rates of hospitalisations due to 'Intentional self-poisoning due to alcohol'. We also found evidence of wide social inequalities by level of deprivation, which were wider for men than compared to women across all of our outcome measures other than 'Intentional self-poisoning due to alcohol'.
Our study expands the evidence base to help understand population level trends in alcohol-related admissions by age, sex and socioeconomic deprivation. There have been increasing hospital admissions attributable to alcohol between 2002/03 and 2013/14, particularly concentrated in middle aged males and deprived areas. However, the increase in young females being admitted for 'Intentional self-poisoning due to alcohol' raises additional concerns.
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DOBA, IZUM, KILJ, NUK, PILJ, PNG, SAZU, SIK, UILJ, UKNU, UL, UM, UPUK
Supplemental bone grafting is regularly required before dental implant placement in patients with cleft lip and palate (CLP).
The study purpose was to measure and compare implant osseointegration and ...changes in graft dimensions following lateral incisor onlay cortical bone grafting in CLP and non-CLP patients.
Retrospective cohort study composed of patients who presented to Boston Children's Hospital and underwent autogenous onlay cortical block bone grafting at lateral incisor sites from 2015 through 2023. Patients were excluded if the cone beam computed tomography (CBCT) quality was insufficient for accurate measurements.
The predictor variable was CLP status coded as CLP or non-CLP.
The primary outcome variable was successful implant osseointegration confirmed by a torque of 35 N/cm or more after 3 months of implant healing. Secondary outcomes were change in bone width between preoperative and postoperative CBCT scans at lateral incisor sites and the need for additional bone augmentation prior to or during implant placement.
Covariates were age, sex, cleft location, and time from bone graft to postoperative CBCT and implant placement.
Data analyses were performed using t-tests, Fisher's exact tests, Mann-Whitney U tests, and Pearson's correlation. P < .05 was considered statistically significant.
A total of 22 subjects (16 with CLP) were evaluated. The mean age at the time of graft was 19.3 ± 2.4 years with 52.6% males. Implants were osseointegrated at 20 of 22 lateral incisor sites (1 CLP failure, 1 non-CLP failure). There was significant change in bone width after grafting for patients with CLP (P < .001). Patients with CLP experienced a 3.32 (± 1.80) mm and 2.99 (± 1.61) mm increase in bone width at 2 different levels. Patients with CLP achieved greater boney changes near the alveolar crest than noncleft patients (P = .008) but the change was not significantly different more apically (P = .86). One subject with CLP required additional grafting during implant placement.
Cortical block onlay bone grafting is a predictable technique to augment lateral incisor sites in patients with CLP for placement of a dental implant.
Health geographers have been long concerned with understanding how the accessibility of individuals to certain environmental features may influence health and wellbeing. Such insights are ...increasingly being adopted by policy makers for designing healthy neighbourhoods. To support and inform decision making, there is a need for small area national level data. This paper details the creation of a suite of open access health indicators, including a novel multidimensional index summarising 14 health-related features of neighbourhoods for Great Britain. We find no association of our overall index with physical health measures, but a significant association to mental wellbeing.
•There is greater need for open data on health-related features of neighbourhoods.•Designing multi-dimensional indices can help to describe environments.•The overall index is associated with mental wellbeing, but not physical health.•The domains of AHAH are consistently associated to our health outcomes.•All data are openly available at http://maps.cdrc.ac.uk.
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GEOZS, IJS, IMTLJ, KILJ, KISLJ, NLZOH, NUK, OILJ, PNG, SAZU, SBCE, SBJE, UL, UM, UPCLJ, UPUK, ZRSKP
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