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The first heterodinuclear ruthenium(II) complexes of the 1,6,7,12-tetraazaperylene (tape) bridging ligand with iron(II), cobalt(II), and nickel(II) were synthesized and characterized. The metal coordination sphere in this complexes is filled by the tetradentate N,N-dimethyl-2,11-diaza[3.3](2,6)-pyridinophane (L-N4Me2) ligand, yielding complexes of the general formula [(L-N4Me2)Ru(mu-tape)M(L-N4Me2)](ClO4)(2)(PF6)(2) with M = Fe {[2](ClO4)(2)(PF6)(2)}, Co {[3](ClO4)(2)(PF6)(2)}, and Ni {[4](ClO4)(2)(PF6)(2)}. Furthermore, the heterodinuclear tape ruthenium(II) complexes with palladium(II)- and platinum(II)-dichloride [(bpy)(2)Ru(-tape)PdCl2](PF6)(2) {[5](PF6)(2)} and [(dmbpy)(2)Ru(-tape)PtCl2](PF6)(2) {[6](PF6)(2)}, respectively were also prepared. The molecular structures of the complex cations [2](4+) and [4](4+) were discussed on the basis of the X-ray structures of [2](ClO4)(4)MeCN and [4](ClO4)(4)MeCN. The electrochemical behavior and the UV/Vis absorption spectra of the heterodinuclear tape ruthenium(II) complexes were explored and compared with the data of the analogous mono- and homodinuclear ruthenium(II) complexes of the tape bridging ligand.
Complementary to the well-established zwitterionic monomer 3-((3-methacrylamidopropyl) dimethylammonio) propane-1-sulfonate (SPP), the closely related monomers 2-hydroxy-3-((3-methacrylamidopropyl) dimethylammonio) propane-1-sulfonate (SHPP) and 4-((3-methacrylamidopropyl) dimethylammonio)butane- 1-sulfonate (SBP) were synthesised and polymerised by reversible addition-fragmentation chain transfer (RAFT) polymerisation, using a fluorophore labeled RAFT agent. The polyzwitterions of systematically varied molar masses were characterised with respect to their solubility in water and aqueous salt solutions. Both poly(sulfobetaine)s show thermoresponsive behaviour in water, exhibiting phase separation at low temperatures and upper critical solution temperatures (UCST). For both polySHPP and polySBP, cloud points depend notably on the molar mass, and are much higher in D2O than in H2O. Also, the cloud points are effectively modulated by the addition of salts. The individual effects can be in parts correlated to the Hofmeister series for the anions studied. Still, they depend in a complex way on the concentration and the nature of the added electrolytes, on the one hand, and on the detailed nature of the spacer group separating the anionic and the cationic charges of the betaine moiety, on the other hand. As anticipated, the cloud points of polySBP are much higher than the ones of the analogous polySPP of identical molar mass. Surprisingly, the cloud points of polySHPP are also somewhat higher than the ones of their polySPP analogues, despite the additional hydrophilic hydroxyl group present in the spacer separating the ammonium and the sulfonate moieties. These findings point to a complicated interplay of the various hydrophilic components in polyzwitterions with respect to their overall hydrophilicity. Thus, the spacer group in the betaine moiety proves to be an effective additional molecular design parameter, apparently small variations of which strongly influence the phase behaviour of the polyzwitterions in specific aqueous environments.
A unique fabrication process of low molar mass, crystalline polypeptoid fibers is described. Thermoresponsive fiber mats are prepared by electrospinning a homogeneous blend of semicrystalline poly(N-(n-propyl) glycine) (PPGly; 4.1 kDa) with high molar mass poly(ethylene oxide) (PEO). Annealing of these fibers at approximate to 100 degrees C selectively removes the PEO and produces stable crystalline fiber mats of pure PPGly, which are insoluble in aqueous solution but can be redissolved in methanol or ethanol. The formation of water-stable polypeptoid fiber mats is an important step toward their utilization in biomedical applications such as tissue engineering or wound dressing.
Warming and eutrophication are two of the most important global change stressors for natural ecosystems, but their interaction is poorly understood. We used a dynamic model of complex, size-structured food webs to assess interactive effects on diversity and network structure. We found antagonistic impacts: Warming increases diversity in eutrophic systems and decreases it in oligotrophic systems. These effects interact with the community size structure: Communities of similarly sized species such as parasitoid-host systems are stabilized by warming and destabilized by eutrophication, whereas the diversity of size-structured predator-prey networks decreases strongly with warming, but decreases only weakly with eutrophication. Nonrandom extinction risks for generalists and specialists lead to higher connectance in networks without size structure and lower connectance in size-structured communities. Overall, our results unravel interactive impacts of warming and eutrophication and suggest that size structure may serve as an important proxy for predicting the community sensitivity to these global change stressors.
Skipping a grade, one specific form of acceleration, is an intervention used for gifted students. Quantitative research has shown acceleration to be a highly successful intervention regarding academic achievement, but less is known about the social–emotional outcomes of grade-skipping. In the present study, the authors used the grounded theory approach to examine the experiences of seven gifted students aged 8 to 16 years who skipped a grade. The interviewees perceived their “feeling of being in the wrong place” before the grade-skipping as strongly influenced by their teachers, who generally did not respond adequately to their needs. We observed a close interrelationship between the gifted students’ intellectual fit and their social situation in class. Findings showed that the grade-skipping in most of the cases bettered the situation in school intellectually as well as socially, but soon further interventions, for instance, a specialized and demanding class- or subject-specific acceleration were added to provide sufficiently challenging learning opportunities.
1. Plant-plant interactions may critically modify the impact of climate change on plant communities. However, the magnitude and even direction of potential future interactions remains highly debated, especially for water-limited ecosystems. Predictions range from increasing facilitation to increasing competition with future aridification. 2. The different methodologies used for assessing plant-plant interactions under changing environmental conditions may affect the outcome but they are not equally represented in the literature. Mechanistic experimental manipulations are rare compared with correlative approaches that infer future patterns from current observations along spatial climatic gradients. 3. Here, we utilize a unique climatic gradient in combination with a large-scale, long-term experiment to test whether predictions about plant-plant interactions yield similar results when using experimental manipulations, spatial gradients or temporal variation. We assessed shrub-annual interactions in three different sites along a natural rainfall gradient (spatial) during 9 years of varying rainfall (temporal) and 8 years of dry and wet manipulations of ambient rainfall (experimental) that closely mimicked regional climate scenarios. 4. The results were fundamentally different among all three approaches. Experimental water manipulations hardly altered shrub effects on annual plant communities for the assessed fitness parameters biomass and survival. Along the spatial gradient, shrub effects shifted from clearly negative to mildly facilitative towards drier sites, whereas temporal variation showed the opposite trend: more negative shrub effects in drier years. 5. Based on our experimental approach, we conclude that shrub-annual interaction will remain similar under climate change. In contrast, the commonly applied space-for-time approach based on spatial gradients would have suggested increasing facilitative effects with climate change. We discuss potential mechanisms governing the differences among the three approaches. 6. Our study highlights the critical importance of long-term experimental manipulations for evaluating climate change impacts. Correlative approaches, for example along spatial or temporal gradients, may be misleading and overestimate the response of plant-plant interactions to climate change.
In nature, plants often encounter chronic or recurring stressful conditions. Recent results indicate that plants can remember a past exposure to stress to be better prepared for a future stress incident. However, the molecular basis of this is poorly understood. Here, we report the involvement of chromatin modifications in the maintenance of acquired thermotolerance (heat stress [HS] memory). HS memory is associated with the accumulation of histone H3 lysine 4 di- and trimethylation at memory-related loci. This accumulation outlasts their transcriptional activity and marks them as recently transcriptionally active. High accumulation of H3K4 methylation is associated with hyper-induction of gene expression upon a recurring HS. This transcriptional memory and the sustained accumulation of H3K4 methylation depend on HSFA2, a transcription factor that is required for HS memory, but not initial heat responses. Interestingly, HSFA2 associates with memory-related loci transiently during the early stages following HS. In summary, we show that transcriptional memory after HS is associated with sustained H3K4 hyper-methylation and depends on a hit-and-run transcription factor, thus providing a molecular framework for HS memory.
The competitive extraction of Cr(III) onto Nauclea diderrichii seed epicarp doped with MnO2 nanoparticles (MnO2 nano-bioextractant (MNB)) in a single and binary batch system was studied. For validity of experimental data, chi square test, root mean square error, sum of the square errors, hybrid fractional error function, Marquart’s percent standard deviation and standard absolute error were used. Among the kinetic models used, pseudo-second-order and Langmuir equations gave the best fits for the experimental data, with qe (mg g) for the uptake of Cr(III) in single metal system onto MNB, then Cr(III) with Cd(II), Pb(II), Hg(II), KCl and CaCl2 in binary metal systems onto MNB were 2.611, then 1.989, 1.016, 2.208, 1.249 and 1.868 from kinetic standpoint, respectively. The initial sorption rates, h (mg/g/min), and half lives, t1/2 (min), for the uptake of Cr(III) in single metal system onto MNB, then Cr(III) with Cd(II), Pb(II), Hg(II), KCl and CaCl2 in binary metal system onto MNB were 3.497, then 2.311, 2.274, 0.242, 2.956, 45.568 and 0.747, then 5.769, 1.766, 12.144, 1.762, and 2.415, respectively. Physicochemical surface analyses such as pH of point of zero charge, Brunauer–Emmett–Teller single point and multi-point techniques for surface area analyses, scanning electron microscopy and transmission electron microscopy were done on MNB and MnO2 nanoparticles in order to understand their surface microstructures. Desorption study showed that MNB can be recycled and used for future study. Hence, MNB showed good potential to remediate Cr(III) from wastewaters and polluted water.
Mediated bioelectrochemical system for biosensing the cell viability of Staphylococcus aureus
(2016)
Staphylococcus aureus is one of the most dangerous human pathogens and is the cause of numerous illnesses ranging from moderate skin infections to life-threatening diseases. Despite advances made in identifying microorganisms, rapid detection methods for the viability of bacteria are still missing. Here, we report a rapid electrochemical assay for cell viability combining the use of double redox mediators and multiwall carbon nanotubes-screen printed electrodes (MWCNTs-SPE), ferricyanide (FCN) and 2,6-dichlorophenolindophenol (DCIP), which served as electron shuttle to enable the bacterial-electrode communications. The current originating from the metabolically active cells was recorded for probing the activity of the intracellular redox centers. Blocking of the respiratory chain pathways with electron transfer inhibitors demonstrated the involvement of the electron transport chain in the reaction. A good correlation between the number of the metabolically active cells and the current was obtained. The proposed assay has been exploited for monitoring cell proliferation of S. aureus during the growth. The sensitivity of the detection method reached 0.1 OD600. Therefore, the technique described is promising for estimating the cell number, measuring the cell viability, and probing intracellular redox center(s).
Previous work on spatial-numerical association (SNAs) included either spatially distributed stimuli or responses. This raises the possibility that the inferred spatial nature of number concepts was a methodological artifact. We present results from a novel task that involves two categories (spatially oriented objects and number magnitudes) and dissociates spatial classification from number classification. The results reveal SNAs without inferential limitations of previous work and point to a working memory mechanism that transfers spatial coding across categories.