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Rapid Colorimetric Detection of Pseudomonas aeruginosa in Clinical Isolates Using a Magnetic Nanoparticle Biosensor
A rapid, sensitive, and specific colorimetric biosensor based on the use of magnetic nanoparticles (MNPs) was designed for the detection of Pseudomonas aeruginosa in clinical samples. The biosensing platform was based on the measurement of P. aeruginosa proteolytic activity using a specific protease substrate. At the N-terminus, this substrate was covalently bound to MNPs and was linked to a gold sensor surface via cystine at the C-terminus of the substrates. The golden sensor appears black to naked eyes because of the coverage of the MNPs. However, upon proteolysis, the cleaved peptide–MNP moieties will be attracted by an external magnet, revealing the golden color of the sensor surface, which can be observed by the naked eye. In vitro, the biosensor was able to detect specifically and quantitatively the presence of P. aeruginosa with a detection limit of 102 cfu/mL in less than 1 min. The colorimetric biosensor was used to test its ability to detect in situ P. aeruginosa in clinical isolates from patients. This biochip is anticipated to be useful as a rapid point-of-care device for the diagnosis of P. aeruginosa-related infections.
Structural and mechanical characterization of heterogeneities in a CuZr-based bulk metallic glass processed by high pressure torsion
Cu45Zr45Al5Ag5 bulk metallic glass samples, processed by high pressure torsion (HPT) under various conditions, were characterized using synchrotron X-ray diffraction, nanoindentation, differential scanning calorimetry, atomic force and transmission electron microscopy. The experimental results clearly show that HPT modifies the amorphous structure by increasing the mean atomic volume. The level of rejuvenation, correlated with the excess mean atomic volume, is enhanced at higher shear strains as inferred from relaxation enthalpies. By mapping of structural and mechanical quantities, the strain-induced rejuvenated state is characterized on cross-sectional HPT samples on a local scale. A clear correlation both between elastic and plastic softening and between softening and excess mean atomic volume is obtained. But also the heterogeneity of the HPT induced rejuvenation is revealed, resulting in the formation of highly strain-softened regions next to less-deformed ones. A hardness drop of up to 20% is associated with an estimated increase of the mean atomic volume of up to 0.75%. Based on synchrotron X-ray diffraction and nanoindentation measurements it is concluded that elastic fluctuations are enhanced in the rejuvenated material on different length scales down to atomic scale. Furthermore, the calculated flexibility volume and the corresponding average mean square atomic displacement is increased. The plastic response during nanoindentation indicates that HPT processing promotes a more homogeneous-like deformation.
Actively Tunable Collective Localized Surface Plasmons by Responsive Hydrogel Membrane
Collective (lattice) localized surface plasmons (cLSP) with actively tunable and extremely narrow spectral characteristics are reported. They are supported by periodic arrays of gold nanoparticles attached to a stimuli-responsive hydrogel membrane, which can on demand swell and collapse to reversibly modulate arrays period and surrounding refractive index. In addition, it features a refractive index-symmetrical geometry that promotes the generation of cLSPs and leads to strong suppression of radiative losses, narrowing the spectral width of the resonance, and increasing of the electromagnetic field intensity. Narrowing of the cLSP spectral band down to 13 nm and its reversible shifting by up to 151 nm is observed in the near infrared part of the spectrum by varying temperature and by solvent exchange for systems with a poly(N-isopropylacrylamide)-based hydrogel membrane that is allowed to reversibly swell and collapse in either one or in three dimensions. The reported structures with embedded periodic gold nanoparticle arrays are particularly attractive for biosensing applications as the open hydrogel structure can be efficiently post-modified with functional moieties, such as specific ligands, and since biomolecules can rapidly diffuse through swollen polymer networks. © 2019 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim
Nitrous oxide emissions from winter oilseed rape cultivation
Winter oilseed rape (Brassica napus L., WOSR) is the major oil crop cultivated in Europe. Rapeseed oil is predominantly used for production of biodiesel. The framework of the European Renewable Energy Directive requires that use of biofuels achieves GHG savings of at least 50% compared to use of fossil fuel starting in 2018. However, N2O field emissions are estimated using emission factors that are not specific for the crop and associated with strong uncertainty. N2O field emissions are controlled by N fertilization and dominate the GHG balance of WOSR cropping due to the high global warming potential of N2O. Thus, field experiments were conducted to increase the data basis and subsequently derive a new WOSR-specific emission factor. N2O emissions and crop yields were monitored for three years over a range of N fertilization intensities at five study sites representative of German WOSR production. N2O fluxes exhibited the typical high spatial and temporal variability in dependence on soil texture, weather and nitrogen availability. The annual N2O emissions ranged between 0.24 kg and 5.48 kg N2O-N ha−1 a−1. N fertilization increased N2O emissions, particularly with the highest N treatment (240 kg N ha−1). Oil yield increased up to a fertilizer amount of 120 kg N ha−1, higher N-doses increased grain yield but decreased oil concentrations in the seeds. Consequently oil yield remained constant at higher N fertilization. Since, yield-related emission also increased exponentially with N surpluses, there is potential for reduction of the N fertilizer rate, which offers perspectives for the mitigation of GHG emissions. Our measurements double the published data basis of annual N2O flux measurements in WOSR. Based on this extended dataset we modeled the relationship between N2O emissions and fertilizer N input using an exponential model. The corresponding new N2O emission factor was 0.6% of applied fertilizer N for a common N fertilizer amount under best management practice in WOSR production (200 kg N ha−1 a−1). This factor is substantially lower than the linear IPCC Tier 1 factor (EF1) of 1.0% and other models that have been proposed. © 2017
Fe3O4 Nanoparticles Grown on Cellulose/GO Hydrogels as Advanced Catalytic Materials for the Heterogeneous Fenton-like Reaction
Cellulose/graphene oxide (GO)/iron oxide (Fe3O4) composites were prepared by coprecipitating iron salts onto cellulose/GO hydrogels in a basic solution. X-ray photoelectron spectroscopy (XPS), Fourier-transform infrared, and X-ray diffraction characterization showed that Fe3O4 was successfully coated on GO sheets and cellulose. Cellulose/GO/Fe3O4 composites showed excellent catalytic activity by maintaining almost 98% of the removal of acid orange 7 (AO7) and showed stability over 20 consecutive cycles. This performance is attributable to the synergistic effect of Fe3O4 and GO during the heterogeneous Fenton-like reaction. Especially, the cellulose/GO/Fe3O4 composites preserve their activity by keeping the ratio of Fe3+/Fe2+ at 2 even after 20 catalysis cycles, which is supported by XPS analysis.
Plasmonic Hepatitis B Biosensor for the Analysis of Clinical Saliva
A biosensor for the detection of hepatitis B antibodies in clinical saliva was developed. Compared to conventional analysis of blood serum, it offers the advantage of noninvasive collection of samples. Detection of biomarkers in saliva imposes two major challenges associated with the low analyte concentration and increased surface fouling. The detection of minute amounts of hepatitis B antibodies was performed by plasmonically amplified fluorescence sandwich immunoassay. To have access to specific detection, we prevented the nonspecific adsorption of biomolecules present in saliva by brushes of poly[(N-(2-hydroxypropyl) methacrylamide)-co-(carboxybetaine methacrylamide)] grafted from the gold sensor surface and post modified with hepatitis B surface antigen. Obtained results were validated against the response measured with ELISA at a certified laboratory using serum from the same patients. © 2017
Benchmark of Simplified Time-Dependent Density Functional Theory for UV–Vis Spectral Properties of Porphyrinoids
Time-dependent density functional theory is thoroughly benchmarked for the predictive calculation of UV–vis spectra of porphyrin derivatives. With the aim to provide an approach that is computationally feasible for large-scale applications such as biological systems or molecular framework materials, albeit performing with high accuracy for the Q-bands, the results given by various computational protocols, including basis sets, density-functionals (including gradient corrected local functionals, hybrids, double hybrids and range-separated functionals), and various variants of time-dependent density functional theory, including the simplified Tamm–Dancoff approximation, are compared. An excellent choice for these calculations is the range-separated functional CAM-B3LYP in combination with the simplified Tamm–Dancoff approximation and a basis set of double-ζ quality def2-SVP (mean absolute error [MAE] of ≈0.05 eV). This is not surpassed by more expensive approaches, not even by double hybrid functionals, and solely systematic excitation energy scaling slightly improves the results (MAE ≈0.04 eV).
Devulcanization of Waste Rubber and Generation of Active Sites for Silica Reinforcement
Each year, hundreds of millions of tires are produced and ultimately disposed into nature. To address this serious environmental issue, devulcanization could be one of the sustainable solutions that still remains as one of the biggest challenges across the globe. In this work, sulfur-vulcanized natural rubber (NR) is mechanochemically devulcanized utilizing a silane-based tetrasulfide as a devulcanizing agent, and subsequently, silica (SiO2)-based rubber composites are prepared. This method not only breaks the sulfur–sulfur cross-links but also produces reactive poly(isoprene) chains to interact with silica. The silica natural rubber composites are prepared by replacing 30% fresh NR by devulcanized NR with varying contents of silica. The composites exhibit excellent mechanical properties, tear strength, abrasion resistance, and dynamic mechanical properties as compared with the fresh natural rubber silica composites. The tensile strength of devulcanized rubber-based silica composites is ∼20 MPa, and the maximum elongation strain is ∼921%. The devulcanized composites are studied in detail by chemical, mechanical, and morphological analyses. Thus, the value added by the devulcanized rubber could attract the attention of recycling community for its sustainable applications.
Anti-Stokes Stress Sensing: Mechanochemical Activation of Triplet-Triplet Annihilation Photon Upconversion
The development of methods to detect damage in macromolecular materials is of paramount importance to understand their mechanical failure and the structure–property relationships of polymers. Mechanofluorophores are useful and sensitive molecular motifs for this purpose. However, to date, tailoring of their optical properties remains challenging and correlating emission intensity to force induced material damage and the respective events on the molecular level is complicated by intrinsic limitations of fluorescence and its detection techniques. Now, this is tackled by developing the first stress-sensing motif that relies on photon upconversion. By combining the Diels–Alder adduct of a π-extended anthracene with the porphyrin-based triplet sensitizer PtOEP in polymers, triplet–triplet annihilation photon upconversion of green to blue light is mechanochemically activated in solution as well as in the solid state. © 2019 The Authors. Published by Wiley-VCH Verlag GmbH & Co. KGaA.
High-resolution vertical velocities and their power spectrum observed with the MAARSY radar – Part 1: frequency spectrum
The Middle Atmosphere Alomar Radar System (MAARSY) installed at the island of Andøya has been run for continuous probing of atmospheric winds in the upper troposphere and lower stratosphere (UTLS) region. In the current study, we present high-resolution wind measurements during the period between 2010 and 2013 with MAARSY. The spectral analysis applying the Lomb–Scargle periodogram method has been carried out to determine the frequency spectra of vertical wind velocity. From a total of 522 days of observations, the statistics of the spectral slope have been derived and show a dependence on the background wind conditions. It is a general feature that the observed spectra of vertical velocity during active periods (with wind velocity > 10 m s−1) are much steeper than during quiet periods (with wind velocity < 10 m s−1). The distribution of spectral slopes is roughly symmetric with a maximum at −5/3 during active periods, whereas a very asymmetric distribution with a maximum at around −1 is observed during quiet periods. The slope profiles along altitudes reveal a significant height dependence for both conditions, i.e., the spectra become shallower with increasing altitudes in the upper troposphere and maintain roughly a constant slope in the lower stratosphere. With both wind conditions considered together the general spectra are obtained and their slopes are compared with the background horizontal winds. The comparisons show that the observed spectra become steeper with increasing wind velocities under quiet conditions, approach a spectral slope of −5/3 at a wind velocity of 10 m s−1 and then roughly maintain this slope (−5/3) for even stronger winds. Our findings show an overall agreement with previous studies; furthermore, they provide a more complete climatology of frequency spectra of vertical wind velocities under different wind conditions.