Suarezstroud9481

This work proposes a general strategy to enhance PE responses of Schottky contacts, which may advance the design of LSPR-related PE systems.In spite of the recent progress made in organic electrode materials, high-performance candidates are still lacking, especially when taking affordability into account. Herein, we report a novel polymeric lithium salt, namely dilithium salt of poly(2,5-dihydroxy-1,4-benzoquinone-3,6-methylene) (Li2PDBM), which can be easily synthesized by phenol-formaldehyde condensation, followed by lithiation in LiOH solution to eliminate the negative effect of phenol groups in PDBM. Benefiting from a high theoretical capacity (327 mA h g-1), structure stability, insolubility, and redox reversibility, Li2PDBM exhibits superior electrochemical performance as a cathode for rechargeable lithium batteries, including a high reversible capacity (256 mA h g-1), a high rate capability (79% @ 2000 mA g-1), and a high cycling stability (77% @ 2000th cycle). Besides the cost-effective electrode material synthesis approach, this work also provides an important mechanistic understanding of the structure-performance relationship of carbonyl-based electrode materials, especially those with -OH or -OM (M = Li, Na, and K) substituents.The polarization of photoluminescence emitted from anisotropic nanocrystals directly reflects the symmetry of the eigenstates involved in the recombination process and can thus be considered as a characteristic feature of a nanocrystal. We performed polarization resolved magneto-photoluminescence spectroscopy on single colloidal Mn2+CdSe/CdS core-shell quantum dots of wurtzite crystal symmetry. At zero magnetic field, a distinct linear polarization pattern is observed, while applying a magnetic field enforces circularly polarized emission with a characteristic saturation value below 100%. These polarization features are shown to act as a specific fingerprint of each individual nanocrystal. mTOR inhibitor A model considering the orientation of the crystal c⃗ axis with respect to the optical axis and the magnetic field and taking into account the impact of magnetic doping is introduced and quantitatively explains our findings. We demonstrate that a careful analysis of the polarization state of single nanocrystal emission using the full set of Stokes parameters allows for identification of the complete three-dimensional orientation of the crystal anisotropy axis of an individual nanoobject in lab coordinates.Polymeric fiber molecular sieves (PFMs) with ultrahigh surface areas, well-defined Murray's-law hierarchical nanoporous structures, and superior self-standing properties are of great interest for molecular-level separation applications. However, creating such PFMs has been proven extremely challenging. Herein, we report a cross-scale pore-forming strategy to create intriguing sponge fiber molecular sieves with hierarchical, tailorable, and molecularly defined nanoporosity by nanospace-confined chain-packing modulation at the molecular level. Robust secondary ultramicropores ( less then 7 Å) and micropores ( less then 2 nm) are in situ constructed in the macro/mesoporous skeletons of sponge fibers to realize a tunable pore size distribution. link2 The resultant PFMs exhibit the integrated properties of ultrahigh surface area (860 m2 g-1), large pore volume (0.6 cm3 g-1), self-standing properties, and excellent molecular sieving performance and are widely applied in acetophenone/phenyl ethanol separation, hydrogen peroxide purification, ethyl acetate separation, and CO2 adsorption fields. The fabrication of such PFMs provides a feasible way for the design and development of polymeric fibrous sieves for molecular separation in large-scale chemical, energy, and environmental operation processes.Fluorescence imaging is a critical tool to understand the spatial distribution of biomacromolecules in cells and in vivo, providing information on molecular dynamics and interactions. Numerous valuable insights into biological systems have been provided by the specific detection of various molecular species. However, molecule-selective detection is often hampered by background fluorescence, such as cell autofluorescence and fluorescence leakage from molecules stained by other dyes. Here we describe a method for all-optical selective imaging of fluorescent nanodiamonds containing nitrogen-vacancy centers (NVCs) for wide-field fluorescence bioimaging. The method is based on the fact that the fluorescence intensity of NVCs strictly depends on the configuration of ground-state electron spins, which can be controlled by changing the pulse recurrence intervals of microsecond excitation laser pulses. Therefore, by using regulated laser pulses, we can oscillate the fluorescence from NVCs in a nanodiamond, while oscillating other optical signals in the opposite phase to NVCs. As a result, we can reconstruct a selective image of a nanodiamond by using a series of oscillated fluorescence images. We demonstrate application of the method to the selective imaging of nanodiamonds in live cells, in microanimals, and on a hippocampal slice culture obtained from a rat. Our approach potentially enables us to achieve high-contrast images of nanodiamond-labeled biomolecules with a signal-to-background ratio improved by up to 100-fold over the standard fluorescence image, thereby providing a more powerful tool for the investigation of molecular dynamics in cells and in vivo.Iron carboxylates are widely used as iron precursors in the thermal decomposition process or considered as in situ formed intermediate precursors. Their molecular and three-dimensional (3D)-structural nature has been shown to affect the shape, size, and composition of the resulting iron oxide nanoparticles (NPs). Among carboxylate precursors, stearates are particularly attractive because of their higher stability to aging and hydration and they are used as additives in many applications. Despite the huge interest of iron stearates, very few studies aimed up to now at deciphering their full metal-ligand structures and the mechanisms allowing us to achieve in a controlled manner the bottom-up NP formation. In this work, we have thus investigated the molecular structure and composition of two iron stearate precursors, synthesized by introducing either two (FeSt2) or three (FeSt3) stearate (St) chains. Interestingly, both iron stearates consist of lamellar structures with planes of iron polynuclear complexes (polycations) separated with stearate chains in all-trans conformation. The iron content in polycations was found very different between both iron stearates. Their detailed characterizations indicate that FeSt2 is mainly composed of [Fe3-(μ3-O)St6·xH2O]Cl, with no (or few) free stearate, whereas FeSt3 is a mixture of mainly [Fe7(μ3-O(H))6(μ2-OH)xSt12-2x]St with some [Fe3(μ3-O)St6·xH2O]St and free stearic acid. The formation of bigger polynuclear complexes with FeSt3 was related to higher hydrolysis and condensation rates within the iron(III) chloride solution compared to the iron(II) chloride solution. These data suggested a nucleation mechanism based on the condensation of polycation radicals generated by the catalytic departure of two stearate chains from an iron polycation-based molecule.Biocompatible hydrogels for tissue regeneration/replacement and drug release with specific architectures can be obtained by three-dimensional bioprinting techniques. The preservation of the higher order structure of the proteins embedded in the hydrogels as drugs or modulators is critical for their biological activity. Solution nuclear magnetic resonance (NMR) experiments are currently used to investigate the higher order structure of biotherapeutics in comparability, similarity, and stability studies. However, the size of pores in the gel, protein-matrix interactions, and the size of the embedded proteins often prevent the use of this methodology. The recent advancements of solid-state NMR allow for the comparison of the higher order structure of the matrix-embedded and free isotopically enriched proteins, allowing for the evaluation of the functionality of the material in several steps of hydrogel development. Moreover, the structural information at atomic detail on the matrix-protein interactions paves the way for a structure-based design of these biomaterials.The self-labeling protein tags (SLPs) HaloTag7, SNAP-tag, and CLIP-tag allow the covalent labeling of fusion proteins with synthetic molecules for applications in bioimaging and biotechnology. To guide the selection of an SLP-substrate pair and provide guidelines for the design of substrates, we report a systematic and comparative study of the labeling kinetics and substrate specificities of HaloTag7, SNAP-tag, and CLIP-tag. HaloTag7 reaches almost diffusion-limited labeling rate constants with certain rhodamine substrates, which are more than 2 orders of magnitude higher than those of SNAP-tag for the corresponding substrates. SNAP-tag labeling rate constants, however, are less affected by the structure of the label than those of HaloTag7, which vary over 6 orders of magnitude for commonly employed substrates. Determining the crystal structures of HaloTag7 and SNAP-tag labeled with fluorescent substrates allowed us to rationalize their substrate preferences. We also demonstrate how these insights can be exploited to design substrates with improved labeling kinetics.A series of complexes of metal halides with unreduced quinone-type ligands have been synthesized and characterized in detail. The 3,6-di-tert-butyl-o-benzoquinone (1) and 4,6-di-tert-butyl-N-aryl-substituted o-iminobenzoquinones (2-5) (aryl is 2,6-dimethylphenyl in 2, 2-methyl-6-ethylphenyl in 3, 2,6-diethylphenyl in 4, and 2,6-diisopropylphenyl in 5) were used to obtain the molecular complexes with metal 12 group halides as well as with indium(III) iodide. The molecular structures of five complexes, bearing an unreduced form of redox-active ligand, have been established by single-crystal X-ray analysis. The spectral data, electrochemical measurements, and DFT calculations indicate the significant transformations of the molecular orbitals of 1-5 upon complexation with Lewis acids. The reduction potentials of o-(imino)quinones in complexes with metal halides shift into the anodic region versus uncoordinated ones. The choice of metal halide allows varying the shift magnitude up to 1.7 V in 2·CdI2. The change of the oxidizing ability of the 1-5 upon coordination with Lewis acids enables the oxidation of mercury and ferrocene, infeasible for free ligands.In the context of environmental plastic pollution, it is still under debate if and how the "plastisphere", a plastic-specific microbial community, emerges. In this study, we tested the hypothesis that the first conditioning film of dissolved organic matter (DOM) sorbs selectively to polymer substrates and that microbial attachment is governed in a substrate-dependent manner. We investigated the adsorption of stream water-derived DOM to polyethylene terephthalate (PET), polystyrene (PS), and glass (as control) including UV-weathered surfaces by Fourier-transform ion cyclotron mass spectrometry. Generally, the saturated, high-molecular mass and thus more hydrophobic fraction of the original stream water DOM preferentially adsorbed to the substrates. The UV-weathered polymers adsorbed more polar, hydrophilic OM as compared to the dark controls. link3 The amplicon sequencing data of the initial microbial colonization process revealed a tendency of substrate specificity for biofilm attachment after 24 h and a clear convergence of the communities after 72 h of incubation.