The assembly-disassembly-organization-reassembly mechanism for 3D-2D-3D transformation of germanosilicate IWW zeolite

J.Č. thanks the Czech Science Foundation for the support of this research (P106/12/G015). R.E.M. thanks the Royal Society for provision of an industry fellowship and the E.P.S.R.C. for funding (EP/K025112/1). A.B.P. acknowledges the support of the European Community under a Marie Curie Intra‐European Fellowship.Hydrolysis of germanosilicate zeolites with the IWW structure shows two different outcomes depending on the composition of the starting materials. Ge-rich IWW (Si/Ge=3.1) is disassembled into a layered material (IPC-5P), which can be reassembled into an almost pure silica IWW on treatment with diethoxydimethylsilane. Ge-poor IWW (Si/Ge=6.4) is not completely disassembled on hydrolysis, but retains some 3D connectivity. This structure can be reassembled into IWW by incorporation of Al to fill the defects left when the Ge is removed.Publisher PDFPeer reviewe

Synthesis and structural characterization of Zn-containing DAF-1

A study exploring the use of ionic liquid reactions based on imidazolium halides in molecular sieve synthesis has produced a novel zincoaluminophosphate material with an open DFO-type framework structure. This framework structure had only been observed previously in the magnesioaluminophosphate system (Mg-DAF-1) where decamethonium was used as the structure directing agent. The new Zn-DAF-1 material has been characterized using chemical and thermogravimetric analysis and ^(13)C, ^(19)F, ^(27)Al and ^(31)P MAS NMR techniques. Structure analysis (P6/mcc, a = 22.2244(1) Å, c = 42.3293(3) Å) using synchrotron powder diffraction data not only confirmed the framework structure, but also revealed the locations of the Al, P and Zn atoms in the framework, the N,N′-di-isopropyl-imidazolium (DIPI) ions in the pores, some fluoride ions associated with double 4-rings, and some water molecules and anions filling the remaining space. This level of structural detail had not been possible in the Mg-DAF-1 material. Four different locations for the DIPI cation were found in the two 12-ring channels and Zn was found to substitute for only one of the six crystallographically distinct Al sites to yield the approximate crystal chemical formula |(DIPI)_(17)(OH,F)_(11)(H2O)_(23)|[Zn_6Al_(126)P_(132)O_(528)]-DFO

Inhibitory Effect of Azamacrocyclic Ligands on Polyphenol Oxidase in Model and Food Systems

This document is the unedited Author's version of a Submitted Work that was subsequently accepted for publication in Journal of Agricultural and Food Chemistry, copyright © American Chemical Society after peer review. To access the final edited and published work see https://pubs.acs.org/doi/10.1021/acs.jafc.0c02407[EN] Enzymatic browning is one of the main problems faced by the food industry due to the enzyme polyphenol oxidase (PPO) provoking an undesirable color change in the presence of oxygen. Here, we report the evaluation of 10 different azamacrocyclic compounds with diverse morphologies as potential inhibitors against the activity of PPO, both in model and real systems. An initial screening of 10 ligands shows that all azamacrocyclic compounds inhibit to some extent the enzymatic browning, but the molecular structure plays a crucial role on the power of inhibition. Kinetic studies of the most active ligand (L2) reveal a S-parabolic I-parabolic noncompetitive inhibition mechanism and a remarkable inhibition at micromolar concentration (IC50 = 10 mu M). Furthermore, L2 action has been proven on apple juice to significantly reduce the enzymatic browning.Financial support by the Spanish Ministerio de Ciencia, Innovacion y Universidades (project RTI2018-100910-B-C44), Ministerio de Economia y Competitividad (projects CTQ2016-78499-C6-1-R, Unidad de Excelencia MDM 2015-0038 and CTQ2017-90852-REDC), and Generalitat Valenciana (Project PROMETEOII2015-002) is gratefully acknowledged.Muñoz-Pina, S.; Ros-Lis, JV.; Delgado-Pinar, E.; Martínez-Camarena, Á.; Verdejo, B.; García-España, E.; Argüelles Foix, AL.... (2020). Inhibitory Effect of Azamacrocyclic Ligands on Polyphenol Oxidase in Model and Food Systems. Journal of Agricultural and Food Chemistry. 68(30):7964-7973. https://doi.org/10.1021/acs.jafc.0c02407796479736830Simpson, B. K. (Ed.). (2012). 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Journal of Agricultural and Food Chemistry, 58(18), 10076-10084. doi:10.1021/jf1015347Massini, L., Rico, D., & Martin-Diana, A. B. (2018). Quality Attributes of Apple Juice. Fruit Juices, 45-57. doi:10.1016/b978-0-12-802230-6.00004-7McEvily, A. J., Iyengar, R., & Otwell, W. S. (1992). Inhibition of enzymatic browning in foods and beverages. Critical Reviews in Food Science and Nutrition, 32(3), 253-273. doi:10.1080/10408399209527599Iyengar, R., & McEvily, A. J. (1992). Anti-browning agents: alternatives to the use of sulfites in foods. Trends in Food Science & Technology, 3, 60-64. doi:10.1016/0924-2244(92)90131-fMuñoz-Pina, S., Ros-Lis, J. V., Argüelles, Á., Coll, C., Martínez-Máñez, R., & Andrés, A. (2018). Full inhibition of enzymatic browning in the presence of thiol-functionalised silica nanomaterial. Food Chemistry, 241, 199-205. doi:10.1016/j.foodchem.2017.08.059Muñoz-Pina, S., Ros-Lis, J. V., Argüelles, Á., Martínez-Máñez, R., & Andrés, A. (2020). Influence of the functionalisation of mesoporous silica material UVM-7 on polyphenol oxidase enzyme capture and enzymatic browning. Food Chemistry, 310, 125741. doi:10.1016/j.foodchem.2019.125741Castillo, C. E., Máñez, M. A., Basallote, M. G., Clares, M. P., Blasco, S., & García-España, E. (2012). Copper(ii) complexes of quinoline polyazamacrocyclic scorpiand-type ligands: X-ray, equilibrium and kinetic studies. Dalton Transactions, 41(18), 5617. doi:10.1039/c2dt30223cSantra, S., Mukherjee, S., Bej, S., Saha, S., & Ghosh, P. (2015). Amino-ether macrocycle that forms CuII templated threaded heteroleptic complexes: a detailed selectivity, structural and theoretical investigations. Dalton Transactions, 44(34), 15198-15211. doi:10.1039/c5dt00596eFan, R., Serrano-Plana, J., Oloo, W. N., Draksharapu, A., Delgado-Pinar, E., Company, A., … Münck, E. (2018). Spectroscopic and DFT Characterization of a Highly Reactive Nonheme FeV–Oxo Intermediate. Journal of the American Chemical Society, 140(11), 3916-3928. doi:10.1021/jacs.7b11400Martínez-Camarena, Á., Liberato, A., Delgado-Pinar, E., Algarra, A. G., Pitarch-Jarque, J., Llinares, J. M., … García-España, E. (2018). Coordination Chemistry of Cu2+ Complexes of Small N-Alkylated Tetra-azacyclophanes with SOD Activity. Inorganic Chemistry, 57(17), 10961-10973. doi:10.1021/acs.inorgchem.8b01492Algarra, A. G., Basallote, M. G., Belda, R., Blasco, S., Castillo, C. E., Llinares, J. M., … Verdejo, B. (2009). Synthesis, Protonation and CuIIComplexes of Two Novel Isomeric Pentaazacyclophane Ligands: Potentiometric, DFT, Kinetic and AMP Recognition Studies. European Journal of Inorganic Chemistry, 2009(1), 62-75. doi:10.1002/ejic.200800576Díaz, P., Basallote, M. G., Máñez, M. A., García-España, E., Gil, L., Latorre, J., … Luis, S. V. (2003). Thermodynamic and kinetic studies on the Cu2+ coordination chemistry of a novel binucleating pyridinophane ligandElectronic supplementary information (ESI) available: Table S1: observed rate constants for the acid-promoted decomposition of Cu2+ complexes with ligand L. Table S2: observed rate constants for the acid-promoted decomposition of Cu2+ complexes with macrocycle L1. Fig. S1: Variation of some selected 13C chemical shifts as a function of pH. See http://www.rsc.org/suppdata/dt/b2/b209013a/. Dalton Transactions, (6), 1186-1193. doi:10.1039/b209013aBasallote, M. G., Doménech, A., Ferrer, A., García-España, E., Llinares, J. M., Máñez, M. A., … Verdejo, B. (2006). Synthesis and Cu(II) coordination of two new hexaamines containing alternated propylenic and ethylenic chains: Kinetic studies on pH-driven metal ion slippage movements. 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Characterization of polyphenoloxidase (PPO) and total phenolic contents in medlar (Mespilus germanica L.) fruit during ripening and over ripening. Food Chemistry, 106(1), 291-298. doi:10.1016/j.foodchem.2007.05.096Qin, X.-Y., Lee, J., Zheng, L., Yang, J.-M., Gong, Y., & Park, Y.-D. (2018). Inhibition of α-glucosidase by 2-thiobarbituric acid: Molecular dynamics simulation integrating parabolic noncompetitive inhibition kinetics. Process Biochemistry, 65, 62-70. doi:10.1016/j.procbio.2017.10.016Chakrabarty, S. P., Ramapanicker, R., Mishra, R., Chandrasekaran, S., & Balaram, H. (2009). Development and characterization of lysine based tripeptide analogues as inhibitors of Sir2 activity. Bioorganic & Medicinal Chemistry, 17(23), 8060-8072. doi:10.1016/j.bmc.2009.10.003Gou, L., Lee, J., Yang, J.-M., Park, Y.-D., Zhou, H.-M., Zhan, Y., & Lü, Z.-R. (2017). Inhibition of tyrosinase by fumaric acid: Integration of inhibition kinetics with computational docking simulations. 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Synthesis and structural characterization of Zn-containing DAF-1

A study exploring the use of ionic liquid reactions based on imidazolium halides in molecular sieve synthesis has produced a novel zincoaluminophosphate material with an open DFO-type framework structure. This framework structure had only been observed previously in the magnesioaluminophosphate system (Mg-DAF-1) where decamethonium was used as the structure directing agent. The new Zn-DAF-1 material has been characterized using chemical and thermogravimetric analysis and ^(13)C, ^(19)F, ^(27)Al and ^(31)P MAS NMR techniques. Structure analysis (P6/mcc, a = 22.2244(1) Å, c = 42.3293(3) Å) using synchrotron powder diffraction data not only confirmed the framework structure, but also revealed the locations of the Al, P and Zn atoms in the framework, the N,N′-di-isopropyl-imidazolium (DIPI) ions in the pores, some fluoride ions associated with double 4-rings, and some water molecules and anions filling the remaining space. This level of structural detail had not been possible in the Mg-DAF-1 material. Four different locations for the DIPI cation were found in the two 12-ring channels and Zn was found to substitute for only one of the six crystallographically distinct Al sites to yield the approximate crystal chemical formula |(DIPI)_(17)(OH,F)_(11)(H2O)_(23)|[Zn_6Al_(126)P_(132)O_(528)]-DFO

Имитация распределенной обработки информации в вычислительных системах и локальных вычислительных сетях

Предложено использовать для анализа вариантов организации распределенной обработки информации в вычислительных системах и локальных вычислительных сетях вероятностный граф реализации вычислительного процесса с явными связями типа вероятностных сетевых графиков.Запропоновано використовувати для аналізу варіантів організації розподіленої обробки інформації в обчислювальних системах і в локальних обчислювальних мережах імовірнісний граф реалізації обчислювального процесу з явними зв’язками типу імовірнісних сіткових графіків.It іs оffered to use for analyzing variants of organization of distributed information processing in computing systems and local computing networks a probabilistic graph for realizing a computing process with evident relationships of the type probabilistic network diagrams

Evaluation of individual and ensemble probabilistic forecasts of COVID-19 mortality in the United States

Short-term probabilistic forecasts of the trajectory of the COVID-19 pandemic in the United States have served as a visible and important communication channel between the scientific modeling community and both the general public and decision-makers. Forecasting models provide specific, quantitative, and evaluable predictions that inform short-term decisions such as healthcare staffing needs, school closures, and allocation of medical supplies. Starting in April 2020, the US COVID-19 Forecast Hub (https://covid19forecasthub.org/) collected, disseminated, and synthesized tens of millions of specific predictions from more than 90 different academic, industry, and independent research groups. A multimodel ensemble forecast that combined predictions from dozens of groups every week provided the most consistently accurate probabilistic forecasts of incident deaths due to COVID-19 at the state and national level from April 2020 through October 2021. The performance of 27 individual models that submitted complete forecasts of COVID-19 deaths consistently throughout this year showed high variability in forecast skill across time, geospatial units, and forecast horizons. Two-thirds of the models evaluated showed better accuracy than a naïve baseline model. Forecast accuracy degraded as models made predictions further into the future, with probabilistic error at a 20-wk horizon three to five times larger than when predicting at a 1-wk horizon. This project underscores the role that collaboration and active coordination between governmental public-health agencies, academic modeling teams, and industry partners can play in developing modern modeling capabilities to support local, state, and federal response to outbreaks

Peri-operative red blood cell transfusion in neonates and infants: NEonate and Children audiT of Anaesthesia pRactice IN Europe: A prospective European multicentre observational study

BACKGROUND: Little is known about current clinical practice concerning peri-operative red blood cell transfusion in neonates and small infants. Guidelines suggest transfusions based on haemoglobin thresholds ranging from 8.5 to 12 g dl-1, distinguishing between children from birth to day 7 (week 1), from day 8 to day 14 (week 2) or from day 15 (≥week 3) onwards. OBJECTIVE: To observe peri-operative red blood cell transfusion practice according to guidelines in relation to patient outcome. DESIGN: A multicentre observational study. SETTING: The NEonate-Children sTudy of Anaesthesia pRactice IN Europe (NECTARINE) trial recruited patients up to 60 weeks' postmenstrual age undergoing anaesthesia for surgical or diagnostic procedures from 165 centres in 31 European countries between March 2016 and January 2017. PATIENTS: The data included 5609 patients undergoing 6542 procedures. Inclusion criteria was a peri-operative red blood cell transfusion. MAIN OUTCOME MEASURES: The primary endpoint was the haemoglobin level triggering a transfusion for neonates in week 1, week 2 and week 3. Secondary endpoints were transfusion volumes, 'delta haemoglobin' (preprocedure - transfusion-triggering) and 30-day and 90-day morbidity and mortality. RESULTS: Peri-operative red blood cell transfusions were recorded during 447 procedures (6.9%). The median haemoglobin levels triggering a transfusion were 9.6 [IQR 8.7 to 10.9] g dl-1 for neonates in week 1, 9.6 [7.7 to 10.4] g dl-1 in week 2 and 8.0 [7.3 to 9.0] g dl-1 in week 3. The median transfusion volume was 17.1 [11.1 to 26.4] ml kg-1 with a median delta haemoglobin of 1.8 [0.0 to 3.6] g dl-1. Thirty-day morbidity was 47.8% with an overall mortality of 11.3%. CONCLUSIONS: Results indicate lower transfusion-triggering haemoglobin thresholds in clinical practice than suggested by current guidelines. The high morbidity and mortality of this NECTARINE sub-cohort calls for investigative action and evidence-based guidelines addressing peri-operative red blood cell transfusions strategies. TRIAL REGISTRATION: ClinicalTrials.gov, identifier: NCT02350348

The United States COVID-19 Forecast Hub dataset

Academic researchers, government agencies, industry groups, and individuals have produced forecasts at an unprecedented scale during the COVID-19 pandemic. To leverage these forecasts, the United States Centers for Disease Control and Prevention (CDC) partnered with an academic research lab at the University of Massachusetts Amherst to create the US COVID-19 Forecast Hub. Launched in April 2020, the Forecast Hub is a dataset with point and probabilistic forecasts of incident cases, incident hospitalizations, incident deaths, and cumulative deaths due to COVID-19 at county, state, and national, levels in the United States. Included forecasts represent a variety of modeling approaches, data sources, and assumptions regarding the spread of COVID-19. The goal of this dataset is to establish a standardized and comparable set of short-term forecasts from modeling teams. These data can be used to develop ensemble models, communicate forecasts to the public, create visualizations, compare models, and inform policies regarding COVID-19 mitigation. These open-source data are available via download from GitHub, through an online API, and through R packages

A global experiment on motivating social distancing during the COVID-19 pandemic

Finding communication strategies that effectively motivate social distancing continues to be a global public health priority during the COVID-19 pandemic. This cross-country, preregistered experiment (n = 25,718 from 89 countries) tested hypotheses concerning generalizable positive and negative outcomes of social distancing messages that promoted personal agency and reflective choices (i.e., an autonomy-supportive message) or were restrictive and shaming (i.e., a controlling message) compared with no message at all. Results partially supported experimental hypotheses in that the controlling message increased controlled motivation (a poorly internalized form of motivation relying on shame, guilt, and fear of social consequences) relative to no message. On the other hand, the autonomy-supportive message lowered feelings of defiance compared with the controlling message, but the controlling message did not differ from receiving no message at all. Unexpectedly, messages did not influence autonomous motivation (a highly internalized form of motivation relying on one’s core values) or behavioral intentions. Results supported hypothesized associations between people’s existing autonomous and controlled motivations and self-reported behavioral intentions to engage in social distancing. Controlled motivation was associated with more defiance and less long-term behavioral intention to engage in social distancing, whereas autonomous motivation was associated with less defiance and more short- and long-term intentions to social distance. Overall, this work highlights the potential harm of using shaming and pressuring language in public health communication, with implications for the current and future global health challenges

Non-affirmative Theory of Education as a Foundation for Curriculum Studies, Didaktik and Educational Leadership

This chapter presents non-affirmative theory of education as the foundation for a new research program in education, allowing us to bridge educational leadership, curriculum studies and Didaktik. We demonstrate the strengths of this framework by analyzing literature from educational leadership and curriculum theory/didaktik. In contrast to both socialization-oriented explanations locating curriculum and leadership within existing society, and transformation-oriented models viewing education as revolutionary or super-ordinate to society, non-affirmative theory explains the relation between education and politics, economy and culture, respectively, as non-hierarchical. Here critical deliberation and discursive practices mediate between politics, culture, economy and education, driven by individual agency in historically developed cultural and societal institutions. While transformative and socialization models typically result in instrumental notions of leadership and teaching, non-affirmative education theory, previously developed within German and Nordic education, instead views leadership and teaching as relational and hermeneutic, drawing on ontological core concepts of modern education: recognition; summoning to self-activity and Bildsamkeit. Understanding educational leadership, school development and teaching then requires a comparative multi-level approach informed by discursive institutionalism and organization theory, in addition to theorizing leadership and teaching as cultural-historical and critical-hermeneutic activity. Globalisation and contemporary challenges to deliberative democracy also call for rethinking modern nation-state based theorizing of education in a cosmopolitan light. Non-affirmative education theory allows us to understand and promote recognition based democratic citizenship (political, economical and cultural) that respects cultural, ethical and epistemological variations in a globopolitan era. We hope an American-European-Asian comparative dialogue is enhanced by theorizing education with a non-affirmative approach