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Halloysites as tubular alumosilicates are introduced as inexpensive natural nanoparticles to form and stabilize oil-water emulsions. This stabilized emulsion is shown to enable efficient interfacial catalytic reactions. Yield, selectivity, and product separation can be tremendously enhanced, e.g., for the hydroformylation reaction of dodecene to tridecanal. In perspective, this type of formulation may be used for oil spill dispersions. The key elements of the described formulations are clay nanotubes (halloysites) which are highly anisometric, can be filled by helper molecules, and are abundantly available in thousands of tons, making this technology scalable for industrial applications.
Advances in nanotechnology lead to an increasing interest in how nanoparticles interact with biomembranes. Nanoparticles are wrapped spontaneously by biomembranes if the adhesive interactions between the particles and membranes compensate for the cost of membrane bending. In the last years, the cooperative wrapping of spherical nanoparticles in membrane tubules has been observed in experiments and simulations. For spherical nanoparticles, the stability of the particle-filled membrane tubules strongly depends on the range of the adhesive particle-membrane interactions. In this article, it is shown via modeling and energy minimization that elongated and patchy particles are wrapped cooperatively in membrane tubules that are highly stable for all ranges of the particle-membrane interactions, compared to individual wrapping of the particles. The cooperative wrapping of linear chains of elongated or patchy particles in membrane tubules may thus provide an efficient route to induce membrane tubulation, or to store such particles in membranes.
pH-sensitive nanoparticles have a great potential for dermal and transfollicular drug delivery. In this study, pH-sensitive, dexamethasone-loaded Eudragit (R) L 100, Eudragit (R) L 100-55, Eudragit (R) S 100, HPMCP-50, HPMCP-55 and cellulose acetate phthalate nanoparticles were prepared by nanoprecipitation and characterized. The pH-dependent swelling, erosion, dissolution and drug release kinetics were investigated in vitro using dynamic light scattering and Franz diffusion cells, respectively. Their toxicity potential was assessed by the ROS and MTT assays. 100-700 nm nanoparticles with high drug loading and entrapment efficiency were obtained. The nanoparticles bear no toxicity potential. Cellulose phthalates nanoparticles were more sensitive to pH than acrylates nanoparticles. They dissolved in 10 mM pH 7.5 buffer and released > 80% of the drug within 7 h. The acrylate nanoparticles dissolved in 40 mM pH 7.5 buffer and released 65-70% of the drug within 7 h. The nanoparticles remained intact in 10 and 40 mM pH 6.0 buffers (HPMCP nanoparticles dissolved in 40 mM pH 6.0 buffer) and released slowly. The nanoparticles properties could be modulated by blending the different polymers. In conclusion, various pH-sensitive nanoparticles that could release differently on the skin surface and dissolve and release in the hair follicles were obtained.
A variety of azobenzenes were synthesized to study the behavior of their E and Z isomers upon electrochemical reduction. Our results show that the radical anion of the Z isomer is able to rapidly isomerize to the corresponding E configured counterpart with a dramatically enhanced rate as compared to the neutral species. Due to a subsequent electron transfer from the formed E radical anion to the neutral Z starting material the overall transformation is catalytic in electrons; i.e., a substoichiometric amount of reduced species can isomerize the entire mixture. This pathway greatly increases the efficiency of (photo)switching while also allowing one to reach photostationary state compositions that are not restricted to the spectral separation of the individual azobenzene isomers and their quantum yields. In addition, activating this radical isomerization pathway with photoelectron transfer agents allows us to override the intrinsic properties of an azobenzene species by triggering the reverse isomerization direction (Z -> E) by the same wavelength of light, which normally triggers E -> Z isomerization. The behavior we report appears to be general, implying that the metastable isomer of a photoswitch can be isomerized to the more stable one catalytically upon reduction, permitting the optimization of azobenzene switching in new as well as indirect ways.
We investigate both analytically and by computer simulations the ensemble- and time-averaged, nonergodic, and aging properties of massive particles diffusing in a medium with a time dependent diffusivity. We call this stochastic diffusion process the (aging) underdamped scaled Brownian motion (UDSBM). We demonstrate how the mean squared displacement (MSD) and the time-averaged MSD of UDSBM are affected by the inertial term in the Langevin equation, both at short, intermediate, and even long diffusion times. In particular, we quantify the ballistic regime for the MSD and the time-averaged MSD as well as the spread of individual time-averaged MSD trajectories. One of the main effects we observe is that, both for the MSD and the time-averaged MSD, for superdiffusive UDSBM the ballistic regime is much shorter than for ordinary Brownian motion. In contrast, for subdiffusive UDSBM, the ballistic region extends to much longer diffusion times. Therefore, particular care needs to be taken under what conditions the overdamped limit indeed provides a correct description, even in the long time limit. We also analyze to what extent ergodicity in the Boltzmann-Khinchin sense in this nonstationary system is broken, both for subdiffusive and superdiffusive UDSBM. Finally, the limiting case of ultraslow UDSBM is considered, with a mixed logarithmic and power-law dependence of the ensemble-and time-averaged MSDs of the particles. In the limit of strong aging, remarkably, the ordinary UDSBM and the ultraslow UDSBM behave similarly in the short time ballistic limit. The approaches developed here open ways for considering other stochastic processes under physically important conditions when a finite particle mass and aging in the system cannot be neglected.
We study a theoretical model for the toxin-antitoxin (hok/sok) mechanism for plasmid maintenance in bacteria. Toxin-antitoxin systems enforce the maintenance of a plasmid through post-segregational killing of cells that have lost the plasmid. Key to their function is the tight regulation of expression of a protein toxin by an sRNA antitoxin. Here, we focus on the nonlinear nature of the regulatory circuit dynamics of the toxin-antitoxin mechanism. The mechanism relies on a transient increase in protein concentration rather than on the steady state of the genetic circuit. Through a systematic analysis of the parameter dependence of this transient increase, we confirm some known design features of this system and identify new ones: for an efficient toxin-antitoxin mechanism, the synthesis rate of the toxin’s mRNA template should be lower that of the sRNA antitoxin, the mRNA template should be more stable than the sRNA antitoxin, and the mRNA-sRNA complex should be more stable than the sRNA antitoxin. Moreover, a short half-life of the protein toxin is also beneficial to the function of the toxin-antitoxin system. In addition, we study a therapeutic scenario in which a competitor mRNA is introduced to sequester the sRNA antitoxin, causing the toxic protein to be expressed.
Recently, Kocyan & Wiland-Szymańska (2016) have published a thorough research article on one of the outstanding members of the family Hypoxidaceae on the Seychelles, which resulted in the raise of a new genus (Friedmannia Kocyan & Wiland-Szymańska 2016: 60) to accommodate the former Curculigo seychellensis Bojer ex Baker (1877: 368). However, it has turned out that the name Friedmannia Chantanachat & Bold (1962: 45) already exists in literature for a green alga, which renders the new hypoxid genus illegitimate (Melbourne Code; McNeill et al. 2012). Therefore, we assign a new generic epithet to Curculigo seychellensis.
Macrocycles based on L-cystine were synthesized by ring-closing metathesis (RCM) and subsequently polymerized by entropy-driven ring-opening metathesis polymerization (ED-ROMP). Monomer conversion reached similar to 80% in equilibrium and the produced poly (ester-amine-disulfide-alkene)s exhibited apparent molar masses (M-w(app)) of up to 80 kDa and dispersities (D) of similar to 2. The polymers can be further functionalized with acid anhydrides and degraded by reductive cleavage of the main-chain disulfide.
I can see clearly now
(2017)
Past research has revealed that narcissists lack forgiveness. However, little is known about factors that might either buffer or, more critically, enhance the link between narcissism and lack of forgiveness. To address this gap in the literature, the present studies focused on the moderating role of clarity of transgression-related motivations. In an original and a replication study (Ns = 509 and 532, respectively), participants rated their levels of narcissistic admiration and rivalry and recalled a personal episode in which someone had hurt them. Subsequently, participants reported on their lack of forgiveness toward their transgressor. Response speed to these ratings served as an indirect clarity measure, with faster responses indicating greater clarity. In both studies, narcissistic rivalry (but not admiration) was positively related to lack of forgiveness and this relationship was stronger among individuals who were clear about their transgression-related motivations. Results inform our understanding of socio-emotional factors that contribute to narcissists' lack of forgiveness following interpersonal hurt.
Fragmentation of landscapes creates a transition zone in between natural habitats or different kinds of land use. In forested and agricultural landscapes with transition zones, microclimate and matter cycling are markedly altered. This probably accelerates and is intensified by global warming. However, there is no consensus on defining transition zones and quantifying relevant variables for microclimate and matter cycling across disciplines. This article is an attempt to a) revise definitions and offer a framework for quantitative ecologists, b) review the literature on microclimate and matter cycling in transition zones and c) summarise this information using meta-analysis to better understand bio-geochemical and bio-geophysical processes and their spatial extent in transition zones. We expect altered conditions in soils of transition zones to be 10-20 m with a maximum of 50 m, and 25-50 m for above-ground space with a maximum of 125 m.
Near edge X-ray absorption fine structure (NEXAFS) simulations based on the conventional configuration interaction singles (CIS) lead to excitation energies, which are systematically blue shifted. Using a (restricted) open shell core hole reference instead of the Hartree Fock (HF) ground state orbitals improves (Decleva et al., Chem. Phys., 1992, 168, 51) excitation energies and the shape of the spectra significantly. In this work, we systematically vary the underlying SCF approaches, that is, based on HF or density functional theory, to identify best suited reference orbitals using a series of small test molecules. We compare the energies of the K edges and NEXAFS spectra to experimental data. The main improvement compared to conventional CIS, that is, using HF ground state orbitals, is due to the electrostatic influence of the core hole. Different SCF approaches, density functionals, or the use of fractional occupations lead only to comparably small changes. Furthermore, to account for bigger systems, we adapt the core-valence separation for our approach. We demonstrate that the good quality of the spectrum is not influenced by this approximation when used together with the non-separated ground state wave function. Simultaneously, the computational demands are reduced remarkably. (C) 2016 Wiley Periodicals, Inc.
Complexation with dissolved humic matter can be crucial in controlling the mobility of toxic or radioactive contaminant metals. For speciation and transport modelling, a dynamic equilibrium process is commonly assumed, where association and dissociation run permanently. This is, however, questionable in view of reported observations of a growing resistance to dissociation over time. In this study, the isotope exchange principle was employed to gain direct insight into the dynamics of the complexation equilibrium, including kinetic inertisation phenomena. Terbium(III), an analogue of trivalent actinides, was used as a representative of higher-valent metals. Isotherms of binding to (flocculated) humic acid, determined by means of Tb-160 as a radiotracer, were found to be identical regardless of whether the radioisotope was introduced together with the bulk of stable Tb-159 or subsequently after pre-equilibration for up to 3 months. Consequently, there is a permanent exchange of free and humic-bound Tb since all available binding sites are occupied in the plateau region of the isotherm. The existence of a dynamic equilibrium was thus evidenced. There was no indication of an inertisation under these experimental conditions. If the small amount of Tb-160 was introduced prior to saturation with Tb-159, the expected partial desorption of Tb-160 occurred at much lower rates than observed for the equilibration process in the reverse procedure. In addition, the rates decreased with time of pre-equilibration. Inertisation phenomena are thus confined to the stronger sites of humic molecules (occupied at low metal concentrations). Analysing the time-dependent course of isotope exchange according to first-order kinetics indicated that up to 3 years are needed to attain equilibrium. Since, however, metal-humic interaction remains reversible, exchange of metals between humic carriers and mineral surfaces cannot be neglected on the long time scale to be considered in predictive transport models.
We present a high-resolution study of the upper mantle structure of Central Europe, including the western part of the East European Platform, based on S-receiver functions of 345 stations. A distinct contrast is found between Phanerozoic Europe and the East European Craton across the Trans-European Suture Zone. To the west, a pronounced velocity reduction with depth interpreted as lithosphere-asthenosphere boundary (LAB) is found at an average depth of 90 km. Beneath the craton, no strong and continuous LAB conversion is observed. Instead we find a distinct velocity reduction within the lithosphere, at 80-120 km depth. This mid-lithospheric discontinuity (MLD) is attributed to a compositional boundary between depleted and more fertile lithosphere created by late Proterozoic metasomatism. A potential LAB phase beneath the craton is very weak and varies in depth between 180 and 250 km, consistent with a reduced velocity contrast between the lower lithosphere and the asthenosphere. Within the Trans-European Suture Zone, lithospheric structure is characterized by strong heterogeneity. A dipping or step-wise increase to LAB depth of 150 km is imaged from Phanerozoic Europe to 20-22 degrees E, whereas no direct connection to the cratonic LAB or MLD to the east is apparent. At larger depths, a positive conversion associated with the lower boundary of the asthenosphere is imaged at 210-250 km depth beneath Phanerozoic Europe, continuing down to 300 km depth beneath the craton. Conversions from both 410 km and 660 km discontinuities are found at their nominal depth beneath Phanerozoic Europe, and the discontinuity at 410 km depth can also be traced into the craton. A potential negative conversion on top of the 410 km discontinuity found in migrated images is analyzed by modeling and attributed to interference with other converted phases.
The Kenya rift revisited
(2017)
We present three-dimensional (3-D) models that describe the present-day thermal and rheological state of the lithosphere of the greater Kenya rift region aiming at a better understanding of the rift evolution, with a particular focus on plume-lithosphere interactions. The key methodology applied is the 3-D integration of diverse geological and geophysical observations using gravity modelling. Accordingly, the resulting lithospheric-scale 3-D density model is consistent with (i) reviewed descriptions of lithological variations in the sedimentary and volcanic cover, (ii) known trends in crust and mantle seismic velocities as revealed by seismic and seismological data and (iii) the observed gravity field. This data-based model is the first to image a 3-D density configuration of the crystalline crust for the entire region of Kenya and northern Tanzania. An upper and a basal crustal layer are differentiated, each composed of several domains of different average densities. We interpret these domains to trace back to the Precambrian terrane amalgamation associated with the East African Orogeny and to magmatic processes during Mesozoic and Cenozoic rifting phases. In combination with seismic velocities, the densities of these crustal domains indicate compositional differences. The derived lithological trends have been used to parameterise steady-state thermal and rheological models. These models indicate that crustal and mantle temperatures decrease from the Kenya rift in the west to eastern Kenya, while the integrated strength of the lithosphere increases. Thereby, the detailed strength configuration appears strongly controlled by the complex inherited crustal structure, which may have been decisive for the onset, localisation and propagation of rifting.
Moderate to large earthquakes can increase the amount of water feeding stream flows, mobilizing excess water from deep groundwater, shallow groundwater, or the vadose zone. Here we examine the regional pattern of streamflow response to the Maule M8.8 earthquake across Chile's diverse topographic and hydro-climatic gradients. We combine streamflow analyses with groundwater flow modeling and a random forest classifier, and find that, after the earthquake, at least 85 streams had a change in flow. Discharge mostly increased () shortly after the earthquake, liberating an excess water volume of >1.1 km3, which is the largest ever reported following an earthquake. Several catchments had increased discharge of >50 mm, locally exceeding seasonal streamflow discharge under undisturbed conditions. Our modeling results favor enhanced vertical permeability induced by dynamic strain as the most probable process explaining the observed changes at the regional scale. Supporting this interpretation, our random forest classification identifies peak ground velocity and elevation extremes as most important for predicting streamflow response. Given the mean recurrence interval of ∼25 yr for >M8.0 earthquakes along the Peru–Chile Trench, our observations highlight the role of earthquakes in the regional water cycle, especially in arid environments.
Temporal and spatial stability of the vegetation climate relationship is a basic ecological assumption for pollen-based quantitative inferences of past climate change and for predicting future vegetation. We explore this assumption for the Holocene in eastern continental Asia (China, Mongolia). Boosted regression trees (BRT) between fossil pollen taxa percentages (Abies, Artemisia, Betula, Chenopodiaceae, Cyperaceae, Ephedra, Picea, Pinus, Poaceae and Quercus) and climate model outputs of mean annual precipitation (P-ann) and mean temperature of the warmest month (Mt(wa)) for 9 and 6 ka (ka = thousand years before present) were set up and results compared to those obtained from relating modern pollen to modern climate. Overall, our results reveal only slight temporal differences in the pollen climate relationships. Our analyses suggest that the importance of P-ann compared with Mt(wa) for taxa distribution is higher today than it was at 6 ka and 9 ka. In particular, the relevance of P-ann for Picea and Pinus increases and has become the main determinant. This change in the climate tree pollen relationship parallels a widespread tree pollen decrease in north-central China and the eastern Tibetan Plateau. We assume that this is at least partly related to vegetation climate disequilibrium originating from human impact. Increased atmospheric CO2 concentration may have permitted the expansion of moisture-loving herb taxa (Cyperaceae and Poaceae) during the late Holocene into arid/semi-arid areas. We furthermore find that the pollen climate relationship between north-central China and the eastern Tibetan Plateau is generally similar, but that regional differences are larger than temporal differences. In summary, vegetation climate relationships in China are generally stable in space and time, and pollen-based climate reconstructions can be applied to the Holocene. Regional differences imply the calibration-set should be restricted spatially.
Intensive land use is a major cause of biodiversity loss, but most studies comparing the response of multiple taxa rely on simple diversity measures while analyses of other community attributes are only recently gaining attention. Species-abundance distributions (SADs) are a community attribute that can be used to study changes in the overall abundance structure of species groups, and whether these changes are driven by abundant or rare species. We evaluated the effect of grassland management intensity for three land-use modes (fertilization, mowing, grazing) and their combination on species richness and SADs for three belowground (arbuscular mycorrhizal fungi, prokaryotes and insect larvae) and seven aboveground groups (vascular plants, bryophytes and lichens; arthropod herbivores; arthropod pollinators; bats and birds). Three descriptors of SADs were evaluated: general shape (abundance decay rate), proportion of rare species (rarity) and proportional abundance of the commonest species (dominance). Across groups, taxonomic richness was largely unaffected by land-use intensity and only decreased with increasing mowing intensity. Of the three SAD descriptors, abundance decay rate became steeper with increasing combined land-use intensity across groups. This reflected a decrease in rarity among plants, herbivores and vertebrates. Effects of fertilization on the three descriptors were similar to the combined land-use intensity effects. Mowing intensity only affected the SAD descriptors of insect larvae and vertebrates, while grazing intensity produced a range of effects on different descriptors in distinct groups. Overall, belowground groups had more even abundance distribtitions than aboveground groups. Strong differences among aboveground groups and between above- and belowground groups indicate that no single taxonomic group can serve as an indicator for effects in other groups. In the past, the use of SADs has been hampered by concerns over theoretical models underlying specific forms of SADs. Our study shows that SAD descriptors that are not connected to a particular model are suitable to assess the effect of land use on community structure.
Landscape evolution models (LEMs) allow the study of earth surface responses to changing climatic and tectonic forcings. While much effort has been devoted to the development of LEMs that simulate a wide range of processes, the numerical accuracy of these models has received less attention. Most LEMs use first-order accurate numerical methods that suffer from substantial numerical diffusion. Numerical diffusion particularly affects the solution of the advection equation and thus the simulation of retreating landforms such as cliffs and river knickpoints. This has potential consequences for the integrated response of the simulated landscape. Here we test a higher-order flux-limiting finite volume method that is total variation diminishing (TVD-FVM) to solve the partial differential equations of river incision and tectonic displacement. We show that using the TVD-FVM to simulate river incision significantly influences the evolution of simulated landscapes and the spatial and temporal variability of catchment-wide erosion rates. Furthermore, a two-dimensional TVD-FVM accurately simulates the evolution of landscapes affected by lateral tectonic displacement, a process whose simulation was hitherto largely limited to LEMs with flexible spatial discretization. We implement the scheme in TTLEM (TopoToolbox Landscape Evolution Model), a spatially explicit, raster-based LEM for the study of fluvially eroding landscapes in TopoToolbox 2.
The dynamics of fragmentation and vibration of molecular systems with a large number of coupled degrees of freedom are key aspects for understanding chemical reactivity and properties. Here we present a resonant inelastic X-ray scattering (RIXS) study to show how it is possible to break down such a complex multidimensional problem into elementary components. Local multimode nuclear wave packets created by X-ray excitation to different core-excited potential energy surfaces (PESs) will act as spatial gates to selectively probe the particular ground-state vibrational modes and, hence, the PES along these modes. We demonstrate this principle by combining ultra-high resolution RIXS measurements for gas-phase water with state-of-the-art simulations.
We report on a study in which plasmid DNA in water was irradiated with 30 keV electrons generated by a scanning electron microscope and passed through a 100 nm thick Si3N4 membrane. The corresponding Monte Carlo simulations suggest that the kinetic energy spectrum of the electrons throughout the water is dominated by low energy electrons (<100 eV). The DNA radiation damage, single-strand breaks (SSBs) and double-strand breaks (DSBs), was determined by gel electrophoresis. The median lethal dose of D-1/2 = 1.7 +/- 0.3 Gy was found to be much smaller as compared to partially or fully hydrated DNA irradiated under vacuum conditions. The ratio of the DSBs to SSBs was found to be 1 : 12 as compared to 1 : 88 found for hydrated DNA. Our method enables quantitative measurements of radiation damage to biomolecules (DNA, proteins) in solutions under varying conditions (pH, salinity, co-solutes) for an electron energy range which is difficult to probe by standard methods.