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In Europe, systematic national surveillance of antimicrobial resistance (AMR) in food-producing animals has been conducted for decades; however, geographic distribution within countries remains unknown. To determine distribution within Europe, we combined 33,802 country-level AMR prevalence estimates with 2,849 local AMR prevalence estimates from 209 point prevalence surveys across 31 countries. We produced geospatial models of AMR prevalence in Escherichia coli, nontyphoidal Salmonella, and Campylobacter for cattle, pigs, and poultry. We summarized AMR trends by using the proportion of tested antimicrobial compounds with resistance >50% and generated predictive maps at 10 × 10 km resolution that disaggregated AMR prevalence. For E. coli, predicted prevalence rates were highest in southern Romania and southern/eastern Italy; for Salmonella, southern Hungary and central Poland; and for Campylobacter, throughout Spain. Our findings suggest that AMR distribution is heterogeneous within countries and that surveillance data from below the country level could help with prioritizing resources to reduce AMR.
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Campylobacter , Escherichia coli , Animais , Bovinos , Suínos , Antibacterianos/farmacologia , Farmacorresistência Bacteriana , Europa (Continente)/epidemiologia , SalmonellaRESUMO
Nitric oxide (NO), a key element in the regulation of essential biological mechanisms, presents huge potential as therapeutic agent in the treatment and prevention of chronic diseases. Metal-organic frameworks (MOFs) with open metal sites are promising carriers for NO therapies but delivering it over an extended period in biological media remains a great challenge due to i) a fast degradation of the material in body fluids and/or ii) a rapid replacement of NO by water molecules onto the Lewis acid sites. Here, a new ultra-narrow pores Fe bisphosphonate MOF, denoted MIP-210(Fe) or Fe(H2O)(Hmbpa) (H4mbpa = p-xylenediphosphonic acid) is described that adsorbs NO due to an unprecedented sorption mechanism: coordination of NO through the Fe(III) sites is unusually preferred, replacing bound water, and creating a stable interaction with the free H2O and P-OH groups delimiting the ultra-narrow pores. This, associated with the high chemical stability of the MOF in body fluids, enables an unprecedented slow replacement of NO by water molecules in biological media, achieving an extraordinarily extended NO delivery time over at least 70 h, exceeding by far the NO kinetics release reported with others porous materials, paving the way for the development of safe and successful gas therapies.
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Yersinia enterocolitica (Y. enterocolitica) is the most frequent etiological agent of yersiniosis and has been responsible for several national outbreaks in Norway and elsewhere. A standardized high-resolution method, such as core genome Multilocus Sequence Typing (cgMLST), is needed for pathogen traceability at the national and international levels. In this study, we developed and implemented a cgMLST scheme for Y. enterocolitica. We designed a cgMLST scheme in SeqSphere + using high-quality genomes from different Y. enterocolitica biotype sublineages. The scheme was validated if more than 95% of targets were found across all tested Y. enterocolitica: 563 Norwegian genomes collected between 2012 and 2022 and 327 genomes from public data sets. We applied the scheme to known outbreaks to establish a threshold for identifying major complex types (CTs) based on the number of allelic differences. The final cgMLST scheme included 2,582 genes with a median of 97.9% (interquartile range 97.6%-98.8%) targets found across all tested genomes. Analysis of outbreaks identified all outbreak strains using single linkage clustering at four allelic differences. This threshold identified 311 unique CTs in Norway, of which CT18, CT12, and CT5 were identified as the most frequently associated with outbreaks. The cgMLST scheme showed a very good performance in typing Y. enterocolitica using diverse data sources and was able to identify outbreak clusters. We recommend the implementation of this scheme nationally and internationally to facilitate Y. enterocolitica surveillance and improve outbreak response in national and cross-border outbreaks.
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Surtos de Doenças , Genoma Bacteriano , Tipagem de Sequências Multilocus , Yersiniose , Yersinia enterocolitica , Yersinia enterocolitica/genética , Yersinia enterocolitica/classificação , Yersinia enterocolitica/isolamento & purificação , Tipagem de Sequências Multilocus/métodos , Humanos , Yersiniose/epidemiologia , Yersiniose/microbiologia , Yersiniose/diagnóstico , Noruega/epidemiologia , Genoma Bacteriano/genética , Monitoramento Epidemiológico , Epidemiologia Molecular/métodos , Genótipo , Técnicas de Tipagem Bacteriana/métodosRESUMO
Two new porous three-dimensional cadmium(II) metal-organic frameworks (MOFs) containing thiophene-appended carboxylate acid ligands, formulated as [Cd(L1)(4,4'-Bipy)]n.2n(DMF) (1) and [Cd(L2)(4,4'-Bipy)]n.2n(DMF) (2) [where L1 = 5-{(thiophen-2-ylmethyl)amino}isophthalate, L2 = 5-{(thiophen-3-ylmethyl)amino}isophthalate, 4,4'-Bipy = 4,4'-bipyridine, and DMF = N,N'-dimethylformamide] have been synthesized and structurally characterized. The gas adsorption analysis of the activated MOFs shows that they specifically capture CO2 (uptake amount 4.36 mmol/g under 1 bar at 195 K) over N2 and CH4. Moreover, both MOFs show a gate-opening-closing phenomenon, which features the S-shaped isotherms with impressive hysteretic desorption during the CO2 adsorption-desorption process at 195 K. Ideal adsorbed solution theory (IAST) calculations of these MOFs displayed that the obtained selectivity values for CO2/CH4 (50:50) and CO2/N2 (15:85) are approximately 8.6-23 and 93-565, respectively. Configurational bias Monte Carlo simulation was performed to understand the mechanism behind the better CO2 adsorption by these MOFs. Catalytic activity of the MOFs for the CO2 fixation reactions with different epoxides to form cyclic carbonates were tested. These MOFs demonstrated a significantly high conversion (94-99%) of epichlorohydrin to the corresponding cyclic carbonate within 8 h of reaction time at 1 bar of CO2 pressure, at 70 °C, and they can be reused up to five cycles without losing considerably their activity.
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The aim of this updated systematic review was to offer an overview of the effectiveness of environmental surveillance (ES) of SARS-CoV-2 as a potential early-warning system (EWS) for COVID-19 and new variants of concerns (VOCs) during the second year of the pandemic. An updated literature search was conducted to evaluate the added value of ES of SARS-CoV-2 for public health decisions. The search for studies published between June 2021 and July 2022 resulted in 1,588 publications, identifying 331 articles for full-text screening. A total of 151 publications met our inclusion criteria for the assessment of the effectiveness of ES as an EWS and early detection of SARS-CoV-2 variants. We identified a further 30 publications among the grey literature. ES confirms its usefulness as an EWS for detecting new waves of SARS-CoV-2 infection with an average lead time of 1-2 weeks for most of the publication. ES could function as an EWS for new VOCs in areas with no registered cases or limited clinical capacity. Challenges in data harmonization and variant detection require standardized approaches and innovations for improved public health decision-making. ES confirms its potential to support public health decision-making and resource allocation in future outbreaks.
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COVID-19 , SARS-CoV-2 , Humanos , COVID-19/epidemiologia , COVID-19/prevenção & controle , Pandemias/prevenção & controle , Monitoramento AmbientalRESUMO
Biopharmaceuticals have established an indisputable presence in the pharmaceutical pipeline, enabling highly specific new therapies. However, manufacturing, isolating, and delivering these highly complex molecules to patients present multiple challenges, including the short shelf-life of biologically derived products. Administration of biopharmaceuticals through inhalation has been gaining attention as an alternative to overcome the burdens associated with intravenous administration. Although most of the inhaled biopharmaceuticals in clinical trials are being administered through nebulization, dry powder inhalers (DPIs) are considered a viable alternative to liquid solutions due to enhanced stability. While freeze drying (FD) and spray drying (SD) are currently seen as the most viable solutions for drying biopharmaceuticals, spray freeze drying (SFD) has recently started gaining attention as an alternative to these technologies as it enables unique powder properties which favor this family of drug products. The present review focus on the application of SFD to produce dry powders of biopharmaceuticals, with special focus on inhalation delivery. Thus, it provides an overview of the critical quality attributes (CQAs) of these dry powders. Then, a detailed explanation of the SFD fundamental principles as well as the different existing variants is presented, together with a discussion regarding the opportunities and challenges of SFD as an enabling technology for inhalation-based biopharmaceuticals. Finally, a review of the main formulation strategies and their impact on the stability and performance of inhalable biopharmaceuticals produced via SDF is performed. Overall, this review presents a comprehensive assessment of the current and future applications of SFD in biopharmaceuticals for inhalation delivery.
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Produtos Biológicos , Secagem por Atomização , Humanos , Administração por Inalação , Liofilização , Inaladores de Pó Seco , Pós , Tamanho da Partícula , AerossóisRESUMO
BACKGROUND: Despite advances in surgical techniques, cataract remains the leading cause of preventable blindness, and massive surgeries have been adopted as a strategy to change this situation. Monitoring the results of cataract surgeries has become imperative to ensure their quality. Therefore, this study aims to assess the cataract surgery outcomes performed at the Central Hospital of Nampula Mozambique. METHODS: This is a prospective and longitudinal study in which translation, cultural adaptation and validation of the visual function (VF) and quality of life (QoL) questionnaire were performed. The appearance, content, construct, criterion, internal consistency and responsiveness were validated using the most common methods and indicators. Visual acuity (VA), VF and QoL were evaluated on 447 patients before and after surgery by t-test and effect sizes. RESULTS: VF and QoL questionnaires showed one-dimension, good values of TLI (0.973, 0.951) and SRMR (0.057, 0.054), and for each item, weights > 0.7, H2 > 0.5, ranges > 5.8 and the RMSEA < 0.08. Correlations for criterion validity were high and for responsiveness were high for QoL and moderate for VF one and the ordinal Cronbach's alpha coefficients were greater than 0.97. Difference between VA, VF and QoL before and after surgery was statistically significant (p < 0.001). After surgery, 74.3% of patients had good, 23.5% had borderline and 2.2% had poor VA. CONCLUSIONS: The cataract surgery outcomes are outside the WHO recommendations regarding VA, but they have had a great impact on improving VF and QoL. The questionnaires showed excellent psychometric properties and should be used in daily clinical practice to evaluate the results of cataract surgeries.
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Extração de Catarata , Catarata , Humanos , Qualidade de Vida , Estudos Longitudinais , Estudos Prospectivos , Moçambique , Acuidade Visual , Catarata/complicações , Inquéritos e QuestionáriosRESUMO
BACKGROUND: During the COVID-19 pandemic, wastewater-based surveillance gained great international interest as an additional tool to monitor SARS-CoV-2. In autumn 2021, the Norwegian Institute of Public Health decided to pilot a national wastewater surveillance (WWS) system for SARS-CoV-2 and its variants between June 2022 and March 2023. We evaluated the system to assess if it met its objectives and its attribute-based performance. METHODS: We adapted the available guidelines for evaluation of surveillance systems. The evaluation was carried out as a descriptive analysis and consisted of the following three steps: (i) description of the WWS system, (ii) identification of users and stakeholders, and (iii) analysis of the system's attributes and performance including sensitivity, specificity, timeliness, usefulness, representativeness, simplicity, flexibility, stability, and communication. Cross-correlation analysis was performed to assess the system's ability to provide early warning signal of new wave of infections. RESULTS: The pilot WWS system was a national surveillance system using existing wastewater infrastructures from the largest Norwegian municipalities. We found that the system was sensitive, timely, useful, representative, simple, flexible, acceptable, and stable to follow the general trend of infection. Preliminary results indicate that the system could provide an early signal of changes in variant distribution. However, challenges may arise with: (i) specificity due to temporary fluctuations of RNA levels in wastewater, (ii) representativeness when downscaling, and (iii) flexibility and acceptability when upscaling the system due to limited resources and/or capacity. CONCLUSIONS: Our results showed that the pilot WWS system met most of its surveillance objectives. The system was able to provide an early warning signal of 1-2 weeks, and the system was useful to monitor infections at population level and complement routine surveillance when individual testing activity was low. However, temporary fluctuations of WWS values need to be carefully interpreted. To improve quality and efficiency, we recommend to standardise and validate methods for assessing trends of new waves of infection and variants, evaluate the WWS system using a longer operational period particularly for new variants, and conduct prevalence studies in the population to calibrate the system and improve data interpretation.
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COVID-19 , SARS-CoV-2 , Humanos , COVID-19/epidemiologia , Águas Residuárias , Vigilância Epidemiológica Baseada em Águas Residuárias , Pandemias , Noruega/epidemiologiaRESUMO
Glycerin, a low-valued waste from biodiesel production, and dopamine were used as precursors for adsorbent materials. The study is centered on the preparation and application of microporous activated carbon as adsorbent materials in the separation of ethane/ethylene and of gases that are natural gas or landfill gas components (ethane/methane and carbon dioxide/methane). The activated carbons were produced by the following sequence reactions: facile carbonization of a glycerin/dopamine mixture and chemical activation. Dopamine allowed the introduction of nitrogenated groups that improved the selectivity of the separations. The activating agent was KOH, but its mass ratio was kept lower than one to improve the sustainability of the final materials. The solids were characterized by N2 adsorption/desorption isotherms, SEM, FTIR spectroscopy, elemental analysis, and point of zero charges (pHPZC). The order for adsorption of the different adsorbates (in mmolg-1) on the most well performing material-Gdop0.75-is methane (2.5) < carbon dioxide (5.0) < ethylene (8.6) < ethane (8.9).
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BACKGROUND: Next-generation sequencing has considerably increased the number of genomes available in the public domain. However, efforts to use these genomes for surveillance of antimicrobial resistance have thus far been limited and geographically heterogeneous. We inferred global resistance trends in Escherichia coli in food animals using genomes from public databases. METHODS: We retrieved 7632 E. coli genomes from public databases (NCBI, PATRIC and EnteroBase) and screened for antimicrobial resistance genes (ARGs) using ResFinder. Selection bias towards resistance, virulence or specific strains was accounted for by screening BioProject descriptions. Temporal trends for MDR, resistance to antimicrobial classes and ARG prevalence were inferred using generalized linear models for all genomes, including those not subjected to selection bias. RESULTS: MDR increased by 1.6 times between 1980 and 2018, as genomes carried, on average, ARGs conferring resistance to 2.65 antimicrobials in swine, 2.22 in poultry and 1.58 in bovines. Highest resistance levels were observed for tetracyclines (42.2%-69.1%), penicillins (19.4%-47.5%) and streptomycin (28.6%-56.6%). Resistance trends were consistent after accounting for selection bias, although lower mean absolute resistance estimates were associated with genomes not subjected to selection bias (difference of 3.16%±3.58% across years, hosts and antimicrobial classes). We observed an increase in extended-spectrum cephalosporin ARG blaCMY-2 and a progressive substitution of tetB by tetA. Estimates of resistance prevalence inferred from genomes in the public domain were in good agreement with reports from systematic phenotypic surveillance. CONCLUSIONS: Our analysis illustrates the potential of using the growing volume of genomes in public databases to track AMR trends globally.
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Infecções por Escherichia coli , Escherichia coli , Animais , Antibacterianos/farmacologia , Bovinos , Farmacorresistência Bacteriana , Escherichia coli/genética , Infecções por Escherichia coli/epidemiologia , Infecções por Escherichia coli/veterinária , Aves Domésticas , SuínosRESUMO
Thailand is undergoing rapid intensification of livestock production where small subsistence farms and medium sized commercial farms coexist. In medium farms, antimicrobials are prescribed by a veterinarian, whereas in small farms antimicrobial use remains largely unsupervised. The impact of these differences as well as other farming practices on the emergence and composition of antimicrobial resistance genes (ARGs) remains largely unknown. We analyzed 363 genomes of extended-spectrum ß-lactamase producing (ESBL) and/or AmpC producing Escherichia coli recovered from humans and pigs at small and medium farms from the Khon Kaen province, Thailand. We tested for genome-wide associations to identify links between ARGs, host, and farm size. Pig isolates from small farms were associated with mcr and qnr genes conferring resistance to colistin and fluoroquinolones, respectively. In contrast, pig isolates from medium farms were associated with ARGs conferring resistance to drugs commonly used on medium farms (i.e., streptomycin). ESBL plasmids from small farms co-carried ARGs conferring resistance to critically important antimicrobials more frequently compared to plasmid from medium farms. Frequent ARG combinations included blaCTX-M-55 + qnrS1 (29.8% vs 17.5% in small and medium farms, respectively), blaCTX-M-55 + qnrS1 + mcr-3.19 (5% vs 0%), blaCTX-M-14 + qnrS1 (9.3% vs 6.2%), and blaCTX-M-14 + qnrS1 + mcr-1.1 (3.1% vs 0%). The co-location on plasmids of ARGs conferring resistance to critically important antimicrobials as defined by the World Health Organization is concerning, and actions to curb their spread are urgently needed. Legislation on limiting antimicrobial sales and initiatives to better inform farmers and veterinarians on appropriate antimicrobial usage and farm biosecurity could help reduce antimicrobial use on farms.
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Anti-Infecciosos , Infecções por Escherichia coli , Proteínas de Escherichia coli , Humanos , Suínos , Animais , Escherichia coli/genética , Fazendas , Colistina/farmacologia , beta-Lactamases/genética , Tailândia , Infecções por Escherichia coli/veterinária , Plasmídeos/genética , Antibacterianos/farmacologia , Fluoroquinolonas , Estreptomicina , Proteínas de Escherichia coli/genéticaRESUMO
BACKGROUND: Malaria is one of the main causes of death in Angola, particularly among children under 5 years of age. An essential means to improve the situation is with strong malaria case management; this includes diagnosing suspected patients with a confirmatory test, either with a rapid diagnostic test (RDT) or microscopy, prompt and correct treatment with artemisinin-based combination therapy (ACT), and proper case registration (track). In 2011, the United States President's Malaria Initiative (PMI) launched a country-wide programme to improve malaria case management through the provision of regular training and supervision at different levels of health care provision. An evaluation of malaria testing, treatment and registration practices in eight provinces, and at health facilities of various capacities, across Angola was conducted to assess progress of the national programme implementation. METHODS: A retrospective assessment analysed data collected during supervision visits to health facilities conducted between 2012 and 2016 in 8 provinces in Angola. The supervision tool used data collected for malaria knowledge, testing, treatment and case registration practices among health workers as well as health facilities stock outs from different levels of health care delivery. Contingency tables with Pearson chi-squared (χ2) tests were used to identify factors associated with "knowledge", "test", "treat" and "track." Multivariable logistic regression models were used to assess factors associated with the defined outcomes. RESULTS: A total of 7156 supervisions were conducted between September 2012 and July 2016. The overall knowledge, testing, treatment and tracking practices among health care workers (HCWs) increased significantly from 2013 to 2016. Health care workers in 2016 were 3.3 times (95% CI: 2.7-3.9) as likely to have a higher knowledge about malaria case management as in 2013 (p < 0.01), 7.4 (95% CI: 6.1-9.0) times as likely to test more suspected cases (p < 0.01), 10.9 (95% CI: 8.6-13.6) times as likely to treat more confirmed cases (p < 0.01) and 3.7 (95% CI: 3.2-4.4) times as likely to report more accurately in the same period (p < 0.01). DISCUSSION: Improvements demonstrated in knowledge about malaria case management, testing with RDT and treatment with artemisinin-based combinations among HCWs is likely associated with malaria case management trainings and supportive supervisions. Gaps in testing and treatment practices are associated with RDT and ACT medicines stock outs in health facilities. Tracking of malaria cases still poses a major challenge, despite training and supervision. Hospitals consistently performed better compared to other health facilities against all parameters assessed; likely due to a better profile of HCWs. CONCLUSION: Significant progress in malaria case management in eight provinces Angola was achieved in the period of 2013-2016. Continued training and supportive supervision is essential to sustain gains and close existing gaps in malaria case management and reporting in Angola.
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Administração de Caso/estatística & dados numéricos , Controle de Doenças Transmissíveis/estatística & dados numéricos , Atenção à Saúde/estatística & dados numéricos , Testes Diagnósticos de Rotina/estatística & dados numéricos , Malária , Angola , Busca de Comunicante/estatística & dados numéricos , Instalações de Saúde/estatística & dados numéricos , Humanos , Malária/diagnóstico , Malária/prevenção & controle , Estudos RetrospectivosRESUMO
The development of solid materials that deliver nitric oxide (NO) are of interest for several therapeutic applications. Nevertheless, due to NO's reactive nature, rapid diffusion and short half-life, reporting their NO delivery characteristics is rather complex. The full knowledge of this parameter is fundamental to discuss the therapeutic utility of these materials, and thus, the NO quantification strategy must be carefully considered according to the NO-releasing scaffold type, to the expected NO-releasing amounts and to the medium of quantification. In this work, we explore and discuss three different ways of quantifying the release of NO in different biological fluids: haemoglobin assay, Griess assay and NO electrochemical detection. For these measurements, different porous materials, namely zeolites and titanosilicates were used as models for NO-releasing platforms. The oxyhaemoglobin assay offers great sensitivity (nanomolar levels), but it is only possible to monitor the NO release while oxyhaemoglobin is not fully converted. On the other hand, Griess assay has low sensitivity in complex biological media, namely in blood, and interferences with media make NO measurements questionable. Nevertheless, this method can measure micromolar amounts of NO and may be useful for an initial screening for long-term release performance. The electrochemical sensor enabled real-time measurements in a variety of biological settings. However, measured NO is critically low in oxygenated and complex media, giving transient signals, which makes long-term quantification impossible. Despite the disadvantages of each method, the combination of all the results provided a more comprehensive NO release profile for these materials, which will help to determine which formulations are most promising for specific therapeutic applications. This study highlights the importance of using appropriate NO quantification tools to provide accurate reports.
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Óxido Nítrico/análise , Silicatos/química , Zeolitas/química , Estrutura Molecular , Óxido Nítrico/metabolismo , Oxiemoglobinas/química , Porosidade , Titânio/químicaRESUMO
Materials for the controlled release of nitric oxide (NO) are of interest for therapeutic applications. However, to date, many suffer from toxicity and stability issues, as well as poor performance. Herein, we propose a new NO adsorption/release mechanism through the formation of nitrites on the skeleton of a titanium-based metal-organic framework (MOF) that we named MIP-177, featuring a suitable set of properties for such an application: (i) high NO storage capacity (3â µmol mg-1solid ), (ii) excellent biocompatibility at therapeutic relevant concentrations (no cytotoxicity at 90â µg mL-1 for wound healing) due to its high stability in biological media (<9 % degradation in 72â hours) and (iii) slow NO release in biological media (≈2â hours for 90 % release). The prospective application of MIP-177 is demonstrated through NO-driven control of mitochondrial respiration in cells and stimulation of cell migration, paving the way for the design of new NO delivery systems for wound healing therapy.
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Materiais Biocompatíveis/química , Preparações de Ação Retardada/química , Portadores de Fármacos/química , Estruturas Metalorgânicas/química , Óxido Nítrico/química , Óxido Nítrico/farmacologia , Titânio/química , Adsorção , Fenômenos Fisiológicos Celulares/efeitos dos fármacos , Liberação Controlada de Fármacos , Porosidade , Cicatrização/efeitos dos fármacosRESUMO
Nitric oxide (NO) presents innumerable biological roles, and its exogenous supplementation for therapeutic purposes has become a necessity. Some nanoporous materials proved to be potential vehicles for NO with high storage capacity. However, there is still a lack of information about their efficiency to release controlled NO and if they are biocompatible and biologically stable. In this work, we address this knowledge gap starting by evaluating the NO release and stability under biological conditions and their toxicity with primary keratinocyte cells. Titanosilicates (ETS-4 and ETS-10 types) and clay-based materials were the materials under study, which have shown in previous studies suitable NO gas adsorption/release rates. ETS-4 proved to be the most promising material, combining good biocompatibility at 180⯵g/mL, stability and slower NO release. ETS-10 and ETAS-10 showed the best biocompatibility at the same concentration and, in the case of clay-based materials, CoOS is the least toxic of those tested and the one that releases the highest NO amount. The potentiality of these new NO donors to regulate biological functions was assessed next by controlling the mitochondrial respiration and the cell migration. NO-loaded ETS-4 regulates O2 consumption and cell migration in a dose-dependent manner. For cell migration, a biphasic effect was observed in a narrow range of ETS-4 concentration, with a stimulatory effect becoming inhibitory just by doubling ETS-4 concentration. For the other materials, no effective regulation was achieved, which highlights the relevance of the new assessment presented in this work for nanoporous NO carriers that will pave the way for further developments.
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Materiais Biocompatíveis/metabolismo , Queratinócitos/metabolismo , Mitocôndrias/metabolismo , Óxido Nítrico/metabolismo , Porosidade , Adsorção , Materiais Biocompatíveis/química , Movimento Celular , Células Cultivadas , Células HeLa , Humanos , Queratinócitos/química , Mitocôndrias/química , Óxido Nítrico/química , Tamanho da Partícula , Propriedades de SuperfícieRESUMO
In this paper, we present a comparative study of the adsorption behavior of short chain alcohols (pure and in aqueous solution) into silicalite-1 (MFI-type zeolite) and silicalite-2 (MEL-type zeolite). For quite some time, silicalite-1 has been the reference material to address the problem of adsorptive-based separation, mostly for hydrocarbon mixtures. Interestingly, being structurally close to silicalite-1, adsorption studies using silicalite-2 are scarce and to the best of our knowledge, a comparative study of their behavior for alcohol-water mixtures has not been published to date. We have here resorted to molecular simulation techniques to analyze the adsorption and diffusion phenomena in both zeolites at 25 and 50 °C for pure methanol, ethanol, 1-butanol, and water, and for some relevant compositions of alcohol/water mixtures. In addition to the dilute regime in the mixture, our study ranges from intermediate alcohol concentrations to alcohol-rich phases, relevant to alcohol purification processes. Besides, we have performed volumetric and calorimetric measurements of single-component adsorption of alcohols in pure silica MEL zeolite, which were used to validate the model potentials used in the simulations. We observe that the zigzag channels of MFI zeolite are most likely responsible for its somewhat higher affinity for alcohols. This leads to higher adsorption selectivities when compared to those of MEL zeolite. We have also found that the choice of water model strongly conditions water coadsorption into the zeolites and subsequently the predictions of the adsorbent's selectivity in alcohol/water systems. Despite considerable differences for adsorbed pure components, diffusivities of alcohol and water adsorbed from mixtures are relatively similar, as a consequence of the strong hydrogen bonds between hydroxyl groups and water.
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Two-dimensional (2D) solid-state nuclear magnetic resonance (SSNMR) experiments on samples loaded with 13C-labeled CO2, "under controlled partial pressures", have been performed in this work, revealing unprecedented structural details about the formation of CO2 adducts from its reaction with various amine-functionalized SBA-15 containing amines having distinct steric hindrances (e.g., primary, secondary) and similar loadings. Three chemisorbed CO2 species were identified by NMR from distinct carbonyl environments resonating at δC ≈ 153, 160, and 164 ppm. The newly reported chemisorbed CO2 species at δC ≈ 153 ppm was found to be extremely moisture dependent. A comprehensive 1H-based SSNMR study [1D 1H and 2D 1H-X heteronuclear correlation (HETCOR, X = 13C, 29Si) experiments] was performed on samples subjected to different treatments. It was found that all chemisorbed CO2 species are involved in hydrogen bonds (HBs) with either surface silanols or neighboring alkylamines. 1H chemical shifts up to 11.8 ppm revealed that certain chemisorbed CO2 species are engaged in very strong HBs. We effectively demonstrate that NMR may help in discriminating among free and hydrogen-bonded functional groups. 13C{14N} dipolar-recoupling NMR showed that the formation of carbonate or bicarbonate is excluded. Density functional theory calculations on models of alkylamines grafted into the silica surface assisted the 1H/13C assignments and validated various HB arrangements that may occur upon formation of carbamic acid. This work extends the understanding of the chemisorbed CO2 structures that are formed upon bonding of CO2 with surface amines and readily released from the surface by pressure swing.
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We characterized the genetic environment of mcr-1 in colistin-resistant Escherichia coli strains isolated in Switzerland during 2014 to 2016 from humans (n = 3) and chicken meat (n = 6). Whole-genome and plasmid sequencing identified the mcr-1 gene integrated in IncX4 (of which, one strain carried the mcr-1.2 variant), IncI2, IncHI2, and novel IncK2 plasmids (overall, n = 7), as well as in the bacterial chromosome (n = 2) in single or duplicate copies. Our study supports the easy mobilization of mcr-1 across diverse genetic locations.
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Antibacterianos/farmacologia , Colistina/farmacologia , Proteínas de Escherichia coli/genética , Escherichia coli/efeitos dos fármacos , Escherichia coli/genética , Animais , Galinhas/microbiologia , Farmacorresistência Bacteriana/genética , Escherichia coli/isolamento & purificação , Infecções por Escherichia coli/microbiologia , Microbiologia de Alimentos , Humanos , Plasmídeos/efeitos dos fármacos , Plasmídeos/genética , SuíçaRESUMO
Reticulated foam shaped adsorbents are more efficient for the removal of volatile organic compounds (VOCs), particularly from low VOC-concentration indoor air streams. In this study composite structure of zeolite and metal organic frameworks (MOFs), referred as ZMF, has been fabricated by immobilization of fine MOF-199 powder on foam shaped Zeolite Socony Mobil-5 (ZSM-5) Zeolitic structure, referred as ZF. The ZMF possess a uniform and well-dispersed coating of MOF-199 on the porous framework of ZF. It shows higher surface area, pore volume, and VOCs adsorption capacity, as compared to ZF-structure. Post-fabrication changes in selective adsorption properties of ZMF were studied with three common indoor VOCs (benzene, n-hexane, and cyclohexane), using gravimetric adsorption technique. The adsorption capacity of ZMF with different VOCs follow the order of benzene>n-hexane>cyclohexane. In comparison with MOF-199 and ZF, the composite structure ZMF shows improvement in selectivity for benzene from other two VOCs. Further, improvement in efficiency and stability of prepared ZMF was found to be associated with its high MOF loading capacity and unique morphological and structural properties. The developed composite structure with improved VOCs removal and recyclability could be a promising material for small to limited scale air pollution treatment units.
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Poluentes Atmosféricos/análise , Poluição do Ar em Ambientes Fechados/análise , Metais/química , Compostos Orgânicos Voláteis/química , Zeolitas/química , Adsorção , Poluição do Ar , Recuperação e Remediação Ambiental/métodos , Metais/análise , Compostos Orgânicos Voláteis/análiseRESUMO
A carbapenem-resistant sequence type 512 (ST512) Klebsiella pneumoniae carbapenemase 3 (KPC-3)-producing K. pneumoniae strain showing a novel variant plasmid content was isolated in Palermo, Italy, in 2014. ST512 is a worldwide successful clone associated with the spread of bla(KPC) genes located on the IncFIIk pKpQIL plasmid. In our ST512 strain, the bla(KPC-3) gene was unusually located on an IncX3 plasmid, whose complete sequence was determined. Two copies of bla(KPC-3)::Tn4401a caused by intramolecular transposition events were detected in the plasmid.