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A series of new poly-1,3,4-oxadiazoles has been synthesized by polycondensation reaction of hydrazine sulfate with a mixture of a dicarboxylic acid containing unsaturated bonds and a dicarboxylic acid containing silicon, by using methanesulfonic acid/phosphorus pentoxide as a reaction medium. These polymers were highly thermostable but they were only soluble in strong inorganic acids such as sulfuric or methanesulfonic ones. An alternative way was followed by using the corresponding dihydrazides containing unsaturated bonds and the corresponding diacid chloride containing silicon that reacted in N-methylpyrrolidinone (NMP) to give soluble silicon-containing unsaturated polyhydrazides, which were cyclodehydrated either by thermal or chemical treatment to give the corresponding polyoxadiazoles. Very thin coatings of polyhydrazides and polyoxadiazoles were deposited onto silicon wafers and they showed a very smooth surface, free of pinholes, when studied by atomic force microscopy (AFM). Some polyoxadiazole films showed strong blue photoluminescence.
SpiderMAEn
(2019)
A growing energy demand requires new and preferably renewable energy sources. The infinite availability of solar radiation makes its conversion into storable and transportable energy forms attractive for research as well as for the industry. One promising example of a transportable fuel is hydrogen (H-2), making research into eco-friendly hydrogen production meaningful. Here, a hybrid system was developed using newly designed recombinant spider silk protein variants as a template for mineralization with inorganic titanium dioxide and gold. These bioinspired organic/inorganic hybrid materials allow for hydrogen production upon light irradiation. To begin with, recombinant spider silk proteins bearing titanium dioxide and gold-binding moieties were created and processed into structured films. These films were modified with gold and titanium dioxide in order to produce a photocatalyst. Subsequent testing revealed hydrogen production as a result of light-induced hydrolysis of water. Therefore, the novel setup presented here provides access to a new principle of generating advanced hybrid materials for sustainable hydrogen production and depicts a promising platform for further studies on photocatalytic production of hydrogen, the most promising future fuel.
Many biochemical processes are involved in regulating the consecutive transition of different phases of dormancy in sweet cherry buds. An evaluation based on a metabolic approach has, as yet, only been partly addressed. The aim of this work, therefore, was to determine which plant metabolites could serve as biomarkers for the different transitions in sweet cherry buds. The focus here was on those metabolites involved in oxidation-reduction processes during bud dormancy, as determined by targeted and untargeted mass spectrometry-based methods. The metabolites addressed included phenolic compounds, ascorbate/dehydroascorbate, reducing sugars, carotenoids and chlorophylls. The results demonstrate that the content of phenolic compounds decrease until the end of endodormancy. After a long period of constancy until the end of ecodormancy, a final phase of further decrease followed up to the phenophase open cluster. The main phenolic compounds were caffeoylquinic acids, coumaroylquinic acids and catechins, as well as quercetin and kaempferol derivatives. The data also support the protective role of ascorbate and glutathione in the para- and endodormancy phases. Consistent trends in the content of reducing sugars can be elucidated for the different phenophases of dormancy, too. The untargeted approach with principle component analysis (PCA) clearly differentiates the different timings of dormancy giving further valuable information.
We measure valence-to-core x-ray emission spectra of compressed crystalline GeO₂ up to 56 GPa and of amorphous GeO₂ up to 100 GPa. In a novel approach, we extract the Ge coordination number and mean Ge-O distances from the emission energy and the intensity of the Kβ'' emission line. The spectra of high-pressure polymorphs are calculated using the Bethe-Salpeter equation. Trends observed in the experimental and calculated spectra are found to match only when utilizing an octahedral model. The results reveal persistent octahedral Ge coordination with increasing distortion, similar to the compaction mechanism in the sequence of octahedrally coordinated crystalline GeO₂ high-pressure polymorphs.
Many biochemical processes are involved in regulating the consecutive transition of different phases of dormancy in sweet cherry buds. An evaluation based on a metabolic approach has, as yet, only been partly addressed. The aim of this work, therefore, was to determine which plant metabolites could serve as biomarkers for the different transitions in sweet cherry buds. The focus here was on those metabolites involved in oxidation-reduction processes during bud dormancy, as determined by targeted and untargeted mass spectrometry-based methods. The metabolites addressed included phenolic compounds, ascorbate/dehydroascorbate, reducing sugars, carotenoids and chlorophylls. The results demonstrate that the content of phenolic compounds decrease until the end of endodormancy. After a long period of constancy until the end of ecodormancy, a final phase of further decrease followed up to the phenophase open cluster. The main phenolic compounds were caffeoylquinic acids, coumaroylquinic acids and catechins, as well as quercetin and kaempferol derivatives. The data also support the protective role of ascorbate and glutathione in the para- and endodormancy phases. Consistent trends in the content of reducing sugars can be elucidated for the different phenophases of dormancy, too. The untargeted approach with principle component analysis (PCA) clearly differentiates the different timings of dormancy giving further valuable information.
We measure valence-to-core x-ray emission spectra of compressed crystalline GeO₂ up to 56 GPa and of amorphous GeO₂ up to 100 GPa. In a novel approach, we extract the Ge coordination number and mean Ge-O distances from the emission energy and the intensity of the Kβ'' emission line. The spectra of high-pressure polymorphs are calculated using the Bethe-Salpeter equation. Trends observed in the experimental and calculated spectra are found to match only when utilizing an octahedral model. The results reveal persistent octahedral Ge coordination with increasing distortion, similar to the compaction mechanism in the sequence of octahedrally coordinated crystalline GeO₂ high-pressure polymorphs.
The Great Nebula in Carina provides an exceptional view into the violent massive star formation and feedback that typifies giant H II regions and starburst galaxies. We have mapped the Carina star-forming complex in X-rays, using archival Chandra data and a mosaic of 20 new 60 ks pointings using the Chandra X-ray Observatory's Advanced CCD Imaging Spectrometer, as a testbed for understanding recent and ongoing star formation and to probe Carina's regions of bright diffuse X-ray emission. This study has yielded a catalog of properties of > 14,000 X-ray point sources;> 9800 of them have multiwavelength counterparts. Using Chandra's unsurpassed X-ray spatial resolution, we have separated these point sources from the extensive, spatially-complex diffuse emission that pervades the region; X-ray properties of this diffuse emission suggest that it traces feedback from Carina's massive stars. In this introductory paper, we motivate the survey design, describe the Chandra observations, and present some simple results, providing a foundation for the 15 papers that follow in this special issue and that present detailed catalogs, methods, and science results.
Understanding animal movement is essential to elucidate how animals interact, survive, and thrive in a changing world. Recent technological advances in data collection and management have transformed our understanding of animal "movement ecology" (the integrated study of organismal movement), creating a big-data discipline that benefits from rapid, cost-effective generation of large amounts of data on movements of animals in the wild. These high-throughput wildlife tracking systems now allow more thorough investigation of variation among individuals and species across space and time, the nature of biological interactions, and behavioral responses to the environment. Movement ecology is rapidly expanding scientific frontiers through large interdisciplinary and collaborative frameworks, providing improved opportunities for conservation and insights into the movements of wild animals, and their causes and consequences.
Writing a history of a scientific theory is always difficult because it requires to focus on some key contributors and to "reconstruct" some supposed influences. In the 1970s, a new way of performing science under the name "chaos" emerged, combining the mathematics from the nonlinear dynamical systems theory and numerical simulations. To provide a direct testimony of how contributors can be influenced by other scientists or works, we here collected some writings about the early times of a few contributors to chaos theory. The purpose is to exhibit the diversity in the paths and to bring some elements-which were never published-illustrating the atmosphere of this period. Some peculiarities of chaos theory are also discussed.
Background
Proficiency in fundamental movement skills (FMS) lays the foundation for being physically active and developing more complex motor skills. Improving these motor skills may provide enhanced opportunities for the development of a variety of perceptual, social, and cognitive skills.
Objective
The objective of this systematic review and meta-analysis was to assess the effects of FMS interventions on actual FMS, targeting typically developing young children.
Method
Searches in seven databases (CINAHL, Embase, MEDLINE, PsycINFO, PubMed, Scopus, Web of Science) up to August 2015 were completed. Trials with children (aged 2-6 years) in childcare or kindergarten settings that applied FMS-enhancing intervention programs of at least 4 weeks and meeting the inclusion criteria were included. Standardized data extraction forms were used. Risk of bias was assessed using a standard scoring scheme (Effective Public Health Practice Project-Quality Assessment Tool for Quantitative Studies [EPHPP]). We calculated effects on overall FMS, object control and locomotor subscales (OCS and LMS) by weighted standardized mean differences (SMDbetween) using random-effects models. Certainty in training effects was evaluated using GRADE (Grading of Recommendations Assessment, Development, and Evaluation System).
Results
Thirty trials (15 randomized controlled trials and 15 controlled trials) involving 6126 preschoolers (aged 3.3-5.5 years) revealed significant differences among groups in favor of the intervention group (INT) with small-to-large effects on overall FMS (SMDbetween 0.46), OCS (SMDbetween 1.36), and LMS (SMDbetween 0.94). Our certainty in the treatment estimates based on GRADE is very low.
Conclusions
Although there is relevant effectiveness of programs to improve FMS proficiency in healthy young children, they need to be interpreted with care as they are based on low-quality evidence and immediate post-intervention effects without long-term follow-up.
Homotherium was a genus of large-bodied scimitar-toothed cats, morphologically distinct from any extant felid species, that went extinct at the end of the Pleistocene [1-4]. They possessed large, saber-form serrated canine teeth, powerful forelimbs, a sloping back, and an enlarged optic bulb, all of which were key characteristics for predation on Pleistocene megafauna [5]. Previous mitochondrial DNA phylogenies suggested that it was a highly divergent sister lineage to all extant cat species [6-8]. However, mitochondrial phylogenies can be misled by hybridization [9], incomplete lineage sorting (ILS), or sex-biased dispersal patterns [10], which might be especially relevant for Homotherium since widespread mito-nuclear discrepancies have been uncovered in modern cats [10]. To examine the evolutionary history of Homotherium, we generated a -7x nuclear genome and a similar to 38x exome from H. latidens using shotgun and target-capture sequencing approaches. Phylogenetic analyses reveal Homotherium as highly divergent (similar to 22.5 Ma) from living cat species, with no detectable signs of gene flow. Comparative genomic analyses found signatures of positive selection in several genes, including those involved in vision, cognitive function, and energy consumption, putatively consistent with diurnal activity, well-developed social behavior, and cursorial hunting [5]. Finally, we uncover relatively high levels of genetic diversity, suggesting that Homotherium may have been more abundant than the limited fossil record suggests [3, 4, 11-14]. Our findings complement and extend previous inferences from both the fossil record and initial molecular studies, enhancing our understanding of the evolution and ecology of this remarkable lineage.
Background Proficiency in fundamental movement skills (FMS) lays the foundation for being physically active and developing more complex motor skills. Improving these motor skills may provide enhanced opportunities for the development of a variety of perceptual, social, and cognitive skills. Objective The objective of this systematic review and meta-analysis was to assess the effects of FMS interventions on actual FMS, targeting typically developing young children. Method Searches in seven databases (CINAHL, Embase, MEDLINE, PsycINFO, PubMed, Scopus, Web of Science) up to August 2015 were completed. Trials with children (aged 2-6 years) in childcare or kindergarten settings that applied FMS-enhancing intervention programs of at least 4 weeks and meeting the inclusion criteria were included. Standardized data extraction forms were used. Risk of bias was assessed using a standard scoring scheme (Effective Public Health Practice Project-Quality Assessment Tool for Quantitative Studies [EPHPP]). We calculated effects on overall FMS, object control and locomotor subscales (OCS and LMS) by weighted standardized mean differences (SMDbetween) using random-effects models. Certainty in training effects was evaluated using GRADE (Grading of Recommendations Assessment, Development, and Evaluation System). Results Thirty trials (15 randomized controlled trials and 15 controlled trials) involving 6126 preschoolers (aged 3.3-5.5 years) revealed significant differences among groups in favor of the intervention group (INT) with small-to-large effects on overall FMS (SMDbetween 0.46), OCS (SMDbetween 1.36), and LMS (SMDbetween 0.94). Our certainty in the treatment estimates based on GRADE is very low. Conclusions Although there is relevant effectiveness of programs to improve FMS proficiency in healthy young children, they need to be interpreted with care as they are based on low-quality evidence and immediate post-intervention effects without long-term follow-up.
OBJECTIVE: Higher plasma vitamin C levels are associated with lower type 2 diabetes risk, but whether this association is causal is uncertain. To investigate this, we studied the association of genetically predicted plasma vitamin C with type 2 diabetes.
RESEARCH DESIGN AND METHODS: We conducted genome-wide association studies of plasma vitamin C among 52,018 individuals of European ancestry to discover novel genetic variants. We performed Mendelian randomization analyses to estimate the association of genetically predicted differences in plasma vitamin C with type 2 diabetes in up to 80,983 case participants and 842,909 noncase participants. We compared this estimate with the observational association between plasma vitamin C and incident type 2 diabetes, including 8,133 case participants and 11,073 noncase participants.
RESULTS: We identified 11 genomic regions associated with plasma vitamin C (P < 5 x 10(-8)), with the strongest signal at SLC23A1, and 10 novel genetic loci including SLC23A3, CHPT1, BCAS3, SNRPF, RER1, MAF, GSTA5, RGS14, AKT1, and FADS1. Plasma vitamin C was inversely associated with type 2 diabetes (hazard ratio per SD 0.88; 95% CI 0.82, 0.94), but there was no association between genetically predicted plasma vitamin C (excluding FADS1 variant due to its apparent pleiotropic effect) and type 2 diabetes (1.03; 95% CI 0.96, 1.10).
CONCLUSIONS: These findings indicate discordance between biochemically measured and genetically predicted plasma vitamin C levels in the association with type 2 diabetes among European populations. The null Mendelian randomization findings provide no strong evidence to suggest the use of vitamin C supplementation for type 2 diabetes prevention.
Materials for polymer electronics applications semiconducting polymer thin films and nanoparticles
(2004)
The paper presents two different approaches to nanostructured semiconducting polymer materials: (i) the generation of aqueous semiconducting polymer dispersions (semiconducting polymer nanospheres SPNs) and their processing into dense films and layers, and (ii) the synthesis of novel semiconducting polyfluorene-block-polyaniline (PF-b-PANI) block copolymers composed of conjugated blocks of different redox potentials which form nanosized morphologies in the solid state
We demonstrate a recycling system for synthetic nicotinamide cofactor analogues using a soluble hydrogenase with turnover number of >1000 for reduction of the cofactor analogues by H-2.
Coupling this system to an ene reductase, we show quantitative conversion of N-ethylmaleimide to N-ethylsuccinimide.
The biocatalyst system retained >50% activity after 7 h.
Permafrost is a distinct feature of the terrestrial Arctic and is vulnerable to climate warming. Permafrost degrades in different ways, including deepening of a seasonally unfrozen surface and localized but rapid development of deep thaw features. Pleistocene ice-rich permafrost with syngenetic ice-wedges, termed Yedoma deposits, are widespread in Siberia, Alaska, and Yukon, Canada and may be especially prone to rapid-thaw processes. Freeze-locked organic matter in such deposits can be re-mobilized on short time-scales and contribute to a carbon-cycle climate feedback. Here we synthesize the characteristics and vulnerability of Yedoma deposits by synthesizing studies on the Yedoma origin and the associated organic carbon pool. We suggest that Yedoma deposits accumulated under periglacial weathering, transport, and deposition dynamics in non-glaciated regions during the late Pleistocene until the beginning of late glacial warming. The deposits formed due to a combination of aeolian, colluvial, nival, and alluvial deposition and simultaneous ground ice accumulation. We found up to 130 gigatons organic carbon in Yedoma, parts of which are well-preserved and available for fast decomposition after thaw. Based on incubation experiments, up to 10% of the Yedoma carbon is considered especially decomposable and may be released upon thaw. The substantial amount of ground ice in Yedoma makes it highly vulnerable to disturbances such as thermokarst and thermo-erosion processes. Mobilization of permafrost carbon is expected to increase under future climate warming. Our synthesis results underline the need of accounting for Yedoma carbon stocks in next generation Earth-System-Models for a more complete representation of the permafrost-carbon feedback.
Permafrost warming has the potential to amplify global climate change, because when frozen sediments thaw it unlocks soil organic carbon. Yet to date, no globally consistent assessment of permafrost temperature change has been compiled. Here we use a global data set of permafrost temperature time series from the Global Terrestrial Network for Permafrost to evaluate temperature change across permafrost regions for the period since the International Polar Year (2007–2009). During the reference decade between 2007 and 2016, ground temperature near the depth of zero annual amplitude in the continuous permafrost zone increased by 0.39 ± 0.15 °C. Over the same period, discontinuous permafrost warmed by 0.20 ± 0.10 °C. Permafrost in mountains warmed by 0.19 ± 0.05 °C and in Antarctica by 0.37 ± 0.10 °C. Globally, permafrost temperature increased by 0.29 ± 0.12 °C. The observed trend follows the Arctic amplification of air temperature increase in the Northern Hemisphere. In the discontinuous zone, however, ground warming occurred due to increased snow thickness while air temperature remained statistically unchanged.