X-ray absorption spectroscopy insights on the structure anisotropy and charge transfer in Chevrel Phase chalcogenides.

The electronic structure and local coordination of binary (Mo6T8) and ternary Chevrel Phases (MxMo6T8) are investigated for a range of metal intercalant and chalcogen compositions. We evaluate differences in the Mo L3-edge and K-edge X-ray absorption near edge structure across the suite of chalcogenides MxMo6T8 (M = Cu, Ni, x = 1-2, T = S, Se, Te), quantifying the effect of compositional and structural modification on electronic structure. Furthermore, we highlight the expansion, contraction, and anisotropy of Mo6 clusters within these Chevrel Phase frameworks through extended X-ray absorption fine structure analysis. Our results show that metal-to-cluster charge transfer upon intercalation is dominated by the chalcogen acceptors, evidenced by significant changes in their respective X-ray absorption spectra in comparison to relatively unaffected Mo cations. These results explain the effects of metal intercalation on the electronic and local structure of Chevrel Phases across various chalcogen compositions, and aid in rationalizing electron distribution within the structure.

Risk Factors for COVID-19 Morbidity and Mortality in Institutionalised Elderly People.

BACKGROUND: SARS-CoV-2 has caused a high mortality in institutionalised individuals. There are very few studies on the involvement and the real impact of COVID-19 in nursing homes. This study analysed factors related to morbidity and mortality of COVID-19 in institutionalised elderly people. METHODS: This cohort study included 842 individuals from 12 nursing homes in Sant Cugat del Vallès (Spain) from 15 March to 15 May 2020. We evaluated individual factors (demographic, dependence, clinical, and therapeutic) and those related to the nursing homes (size and staff) associated with infection and mortality by SARS-CoV-2. Infection was diagnosed by molecular biology test. RESULTS: Of the 842 residents included in the analysis, 784 underwent a Polymerase Chain Reaction (PCR) test; 74.2% were women, the mean age was 87.1 years, and 11.1% died. The PCR test was positive in 44%. A total of 33.4% of the residents presented symptoms compatible with COVID-19 and of these, 80.9% were PCR-positive for SARS-CoV-2. Infection by SARS-CoV-2 among residents was associated with the rate of staff infected in the homes. Mortality by SARS-CoV-2 was related to male sex and a greater grade of dependence measured with the Barthel index. CONCLUSIONS: SARS-Cov-2 infection in institutionalised people is associated with the infection rate in nursing home workers and mortality by SARS-Cov-2 with sex and greater dependency according to the Barthel index. Adequate management of nursing home staff and special attention to measures of infection control, especially of individuals with greater dependence, are keys for successful management of future pandemic situations.

Machine Learning Guided Synthesis of Multinary Chevrel Phase Chalcogenides.

The Chevrel phase (CP) is a class of molybdenum chalcogenides that exhibit compelling properties for next-generation battery materials, electrocatalysts, and other energy applications. Despite their promise, CPs are underexplored, with only ∼100 compounds synthesized to date due to the challenge of identifying synthesizable phases. We present an interpretable machine-learned descriptor (Hδ) that rapidly and accurately estimates decomposition enthalpy (ΔHd) to assess CP stability. To develop Hδ, we first used density functional theory to compute ΔHd for 438 CP compositions. We then generated >560 000 descriptors with the new machine learning method SIFT, which provides an easy-to-use approach for developing accurate and interpretable chemical models. From a set of >200 000 compositions, we identified 48 501 CPs that Hδ predicts are synthesizable based on the criterion that ΔHd < 65 meV/atom, which was obtained as a statistical boundary from 67 experimentally synthesized CPs. The set of candidate CPs includes 2307 CP tellurides, an underexplored CP subset with a predicted preference for channel site occupation by cation intercalants that is rare among CPs. We successfully synthesized five of five novel CP tellurides attempted from this set and confirmed their preference for channel site occupation. Our joint computational and experimental approach for developing and validating screening tools that enable the rapid identification of synthesizable materials within a sparse class is likely transferable to other materials families to accelerate their discovery.

Stabilizing Hydrogen Adsorption through Theory-Guided Chalcogen Substitution in Chevrel-Phase Mo6X8 (X=S, Se, Te) Electrocatalysts.

In this work, we implement a facile microwave-assisted synthesis method to yield three binary Chevrel-Phase chalcogenides (Mo6X8; X = S, Se, Te) and investigate the effect of increasing chalcogen electronegativity on hydrogen evolution catalytic activity. Density functional theory predictions indicate that increasing chalcogen electronegativity in these materials will yield a favorable electronic structure for proton reduction. This is confirmed experimentally via X-ray absorption spectroscopy as well as traditional electrochemical analysis. We have identified that increasing the electronegativity of X in Mo6X8 increases the hydrogen adsorption strength owing to a favorable shift in the p-band position as well as an increase in the Lewis basicity of the chalcogen, thereby improving hydrogen evolution reaction energetics. We find that Mo6S8 exhibits the highest hydrogen evolution activity of the Mo6X8 series of catalysts, requiring an overpotential of 321 mV to achieve a current density of 10 mA cm-2ECSA, a Tafel slope of 74 mV per decade, and an exchange current density of 6.01 × 10-4 mA cm-2ECSA. Agreement between theory and experiment in this work indicates that the compositionally tunable Chevrel-Phase chalcogenide family is a promising framework for which electronic structure can be predictably modified to improve catalytic small-molecule reduction reactivity.

Linear correlation models for the redox potential of organic molecules in aqueous solutions.

In this study, we use the molecular orbital energy approximation (MOEA) and the energy difference approximation (EDA) to build linear correlation models for the redox potentials of 53 organic compounds in aqueous solutions. The molecules evaluated include nitroxides, phenols, and amines. Both the MOEA and EDA methods yield similar correlation models, however, the MOEA method is less computationally expensive. Correlation coefficients (R2) below 0.3 and mean absolute errors above 0.25 V were found for correlation models built without solvent effects. When explicit water molecules and a continuum solvent model are added to the calculations, correlation coefficients close to 0.8 are reached, and mean absolute errors below 0.18 V are obtained. The incorporation of solvent effects is necessary for good correlation models, particularly for redox processes of charged molecules in aqueous solutions. A comparison of the correlation models from different methodologies is provided. Graphical abstract.

Estimació dels casos de mort tributàries de cures pal·liatives pediàtriques / Estimación de los casos de muerte tributarias de cuidados paliativos pediátricos / Estimation of the number of child deaths that are susceptible of benefitting from palliative care

Fonament: la mort ha estat, és i seguirà sent una realitat, per sort poc freqüent, en pediatria. La causa inicial o fonamental que pot causar la mort a un nen o una nena pot ser una malaltia aguda o crònica, que equival a una potencial mort imprevisible o previsible, respectivament. En els casos en què es pot preveure una mort abans d'arribar a l'edat adulta, independentment de les opcions curatives, estan indicades les cures pal·liatives pediàtriques (CPP). Objectiu: conèixer la situació i les causes de mortalitat de pacients entre 0 i 19 anys a Catalunya entre el període 2007-2011 i classificar les causes inicials o fonamentals en tributàries o no de CPP. Mètode.: revisió de l'estadística de mortalitat i de la causalitat d'aquesta segons fonts del Ministeri de Sanitat, Serveis Socials i Igualtat. Classificació de la causa inicial de mort entre tributàries o no de CPP, segons la classificació de Cochrane H et al. Resultats.: els primers anys de vida, la principal causa de mortalitat són les afeccions originades en el període perinatal i les malformacions congènites, en edats posteriors, els tumors i les causes externes. Més del 60% de morts en l'edat pediàtrica podrien ser tributàries de CPP a causa del caràcter amenaçant o limitant de la malaltia de base. Conclusions: l'etiologia de la mort varia en funció de l'edat. Conèixer les causes de mortalitat i les malalties tributàries de CPP permet estimar les necessitats de CPP (AU)

Fundamento. La muerte ha sido, es y seguirá siendo una realidad, por suerte poco frecuente, en pediatría. La causa inicial o fundamental que puede causar la muerte a un niño o una niña puede ser una enfermedad aguda o crónica, que equivale a una probable muerte imprevisible o previsible, respectivamente. En aquellos casos en los que se puede prever una muerte antes de llegar a la edad adulta, independientemente de las opciones curativas, están indicados los cuidados paliativos pediátricos (CPP). Objetivo. Conocer la situación y las causas de mortalidad de pacientes entre 0 y 19 años en Cataluña entre el periodo 2007-2011 y clasificar las causas iniciales o fundamentales en tributarias o no de CPP. Método. Revisión de la estadística de mortalidad y de la causalidad de ésta según fuentes del Ministerio de Sanidad, Servicios Sociales e Igualdad. Clasificación de la causa inicial de muerte entre tributarias o no de CPP, según la clasificación de Cochrane H et al. Resultados. En los primeros años de vida, la principal causa de mortalidad son las afecciones originadas en el período perinatal y las malformaciones congénitas, en edades posteriores, los tumores y las causas externas. Más del 60% de muertes en la edad 0-19 años podrían ser tributarias de CPP debido al carácter amenazante o limitante de la enfermedad de base. Conclusiones. La etiología de la muerte varía en función de la edad. Conocer las causas de mortalidad y las enfermedades tributarias de CPP permite estimar las necesidades de CPP (AU)

Background. Death has been, is, and will continue to be a reality, fortunately rare, in pediatrics. The main causes of death in children are acute or chronic diseases, which result in unexpected or foreseeable death, respectively. In those cases where death before adulthood can be foreseen there is an indication for paediatric palliative care (PPC), regardless of the curative options. Objective. To determine the status and cause of death in patients younger than 19 years in Catalonia between 2007 and 2011, and to classify the causes of death in terms of their potential for PPC services. Method. We reviewed the mortality statistics of the Spanish Ministry of Health, Social Services, and Equality, and we identified the main cause of death. We then categorized the causes of death between those who could have benefitted from PPC and those who could not, according to the Cochrane classification. Results. The main causes of death were congenital malformations or perinatal diseases in the younger age groups, and cancer and external causes in older children and adolescents. More than 60% of children who die are candidates for PPC, due to the life-threatening or life-limiting characteristics of the underlying disease. Conclusions. The cause of death varies with age. In those cases where death before adulthood could be foreseen, a comprehensive and multidisciplinary care involving the child and the family is necessary (AU)

Encuesta nacional sobre las urgencias pediátricas. Aspectos organizativos y funcionales / Structure and operational organization of pediatric emergency services: a Spanish national survey

Introducción: El conocimiento de la estructura y funcionamiento de los servicios de urgencias pediátricos hospitalarios es fundamental para diseñar y promover acciones de mejora. Objetivos: 1. Conocer aspectos sobre la organización y funcionamiento de las urgencias pediátricas de hospitales. 2. Determinar el grado de cumplimiento de los Indicadores Básicos de Calidad establecidos por la Sociedad Española de Urgencias Pediátricas(SEUP).Método: El Grupo de Calidad de la SEUP diseña una encuesta dirigida a responder los objetivos planteados que se remite a los responsables de 40 hospitales con miembros de la SEUP. Se recogen las respuestas recibidas en el período transcurrido del 09/2006al 01/2007.Resultados: Son 34 encuestas de centros repartidos por toda España. Veintitrés (68%)tienen un responsable específico de urgencias, 25 (74%) staff propio y 30 (88%) MIR. Durante las noches y fines de semana, la asistencia corre a cargo en muchos casos de personal no específico de urgencias. La libranza de guardias genera problemas asistenciales en 18 centros (53%). En cuanto a los indicadores destaca que: en los del Área de Patologías el cumplimiento del estándar varia entre el 56 y el 88%, en los del Área de Actividades 7 no disponen de triaje (21%), en los del Área de Documentación todos(100%) cumplimentan el informe de asistencia y 22 realizan codificación diagnóstica(65%), en los del Área de Trabajo 33 hospitales revisan el carro de paros (97%).Conclusiones: Se observan importantes oportunidades de mejora tanto a nivel estructural como funcional. La escasez de profesionales y/o responsables específicos es el factor principal que justifica los problemas detectados. El cumplimiento de los Indicadores presenta una evaluación correcta en el área de patologías pero se observan deficiencias debidas a sistemas informáticos insuficientes en las de actividades y documentación (AU)

Background: A good understanding of the structure and operational organization of pediatric emergency departments(EDs) is essential for the design and promotion of interventions that can lead to improvement. Objectives: 1) To describe the structure and operational organization of pediatric EDs in Spanish hospitals. 2) To determine the degree of fulfillment of the basic quality indicators established by the Spanish Society of Pediatric Emergency Medicine (SEUP).Methods: The SEUP Quality Group designed a questionnaire to measure the described objectives. Forty hopstial EDs with SEUP members were surveyed. Answers received between September 2006 and January 2007 were analyzed. Results: Thirty-four questionnaires were received. Twenty-three EDs had a chief of staff, 25 had emergency staff, and 30had residents in different years of training. On most nights and weekends, medical care is given by nonemergency staff. Eighteen EDs had problems when staff doctors were on leave. The EDs surveyed were compliant on 56% to 88% of the items related to the dimension “diseases”. Under the dimension “activities”, 7 (21%) did not have a triage system. Onitems related to documentation, all EDs (100%) completed care reports and 22 entered diagnostic codes. Under the dimension “workplace resources”, 33 (97%) performed a check of the crash cart. Conclusions: Important opportunities for improvement were identified at the levels of structural organization and functioning. The lack of an ED chief of staff and/or permanent staff was the main factor causing the detected problems. The analysis of quality indicators shows that compliance is acceptable in the area of diseases but was deficient in those of activities and documentation, probably due to inadequate computer systems (AU)