• Thygesen Rye posted an update a month ago

    Significant orbital mixing is rare in lanthanide complexes because of the limited radial extent of the 4f orbitals, which results in a generally small stabilization due to 4f orbital interactions. Nevertheless, even a small amount of additional stabilization could enhance lanthanide separations. One lanthanide complex in which orbital mixing has been extensively studied both experimentally and computationally is cerocene, COT2Ce, where COT is cyclooctatetraene. This compound has a singlet ground state with a low-lying, triplet excited state. Previous fluorescence studies on trimethylsilyl-substituted cerocenes indicate the triplet state is 0.4 eV higher in energy than the singlet state. In addition, computational studies predict that the triplet is 0.3 to 1 eV higher in energy than the singlet. The synthesis of highly pure COT2Ce by Walter and Andersen allowed its physical properties to be accurately measured. Using these measurements, we evaluate the stabilization of the 4f orbitals using two, independent approaches. A Hubbard model is used to evaluate the stabilization of the ground state due to orbital mixing. This stabilization, which is also the singlet-triplet gap, is -0.29 eV using this model. selleckchem This gap was also from the temperature independent paramagnetism of COT2Ce, which yielded a value of -0.32 eV.Correction for ‘PLGA protein nanocarriers with tailor-made fluorescence/MRI/PET imaging modalities’ by Yajie Zhang et al., Nanoscale, 2020, 12, 4988-5002, DOI .Designing a Pt-alternative cocatalyst capable of dissociating HO-H bonds is of great significance yet challenging for the development of high-efficiency and cost-effective water splitting photocatalytic systems. In this study, we designed and constructed a 0D ultrafine ruthenium (U-Ru) quantum dot decorated 3D porous g-C3N4 (3DpCN) nanohybrid (U-Ru/3DpCN) for photocatalytic hydrogen evolution, in which the U-Ru quantum dots act as cocatalysts accelerating the surface proton reduction reaction, and the 3D porous architecture assembled by 2D ultrathin nanosheets inherits a short charge diffusion distance and has a large specific surface area. Owing to these structural and physicochemical merits, the optimal photocatalyst U-1Ru/3DpCN achieves a superior hydrogen evolution performance of 2945.47 μmol g-1 h-1 under visible light with a high apparent quantum efficiency (AQE) of 9.5% at 420 nm, which is close to Pt-cocatalyst/3DpCN and better than most reported co-catalysts/g-C3N4 photocatalytic systems. Experimental results indicate that the formed Schottky junction between U-Ru and 3DpCN contributes to efficient charge separation, and DFT calculations show that the Ru-cocatalyst/g-C3N4 system has an appropriate hydrogen adsorption Gibbs free energy (ΔGH*) of 0.24 eV, which are both responsible to improve the photocatalytic performance. This study provides a new way to develop excellent photocatalysts for hydrogen evolution by the integration of cost-effective Ru quantum dot cocatalysts with nanostructured semiconductors.The physicochemical properties of orally ingested metal nanoparticles can be influenced by the conditions prevailing in the digestive tract. In our work, we demonstrate the strong influence of the pH value on particle fate using a simplified digestion approach to analyze magnesium oxide, copper oxide and zinc oxide nanoparticles and show why a separate consideration of the digestion parameters is necessary.The Particle-in-Cell (PIC) method for plasmons provides a mechanical, single-particle picture of plasmon resonances by tracking in time the movement of all the individual conduction electrons. By applying it to gold nanorods, we demonstrate the usefulness of PIC for extracting time-domain information of plasmons such as plasmon decay times, the relative contribution of each plasmon damping channel, detailed electron movement, as well as radiation and hot electron-emission during damping. An analysis of the time-resolved velocity distribution of the conduction electrons shows that only a small offset in this distribution in each cycle constitutes the plasmon oscillation. We show how PIC can be used to separately analyse Landau damping and Drude damping, and how their decay times can be calculated. Electron-electron scattering and surface scattering are both shown to gradually increase the overall kinetic energy of the electrons and decrease their coherence.Two dimensional MXenes with fascinating characteristics of high electrical conductivity, high density and electroactivity show promising applications in various fields. However, the direct applications of MXenes have been limited due to their inferior mechanical properties and easy restacking. Herein, a kind of nacre-like composite film constructed with Ti3C2Tx, cellulose nanofiber (HCNF) and sodium lignosulfonate (Lig) obtained through the hydrothermal process, named Ti3C2Tx/HCNF@Lig, has been successfully synthesized. The hydrothermal cellulose nanofiber (HCNF) film shows an enhanced mechanical strength (114 MPa) compared to that of the CNF film (95 MPa). Wood-inspired HCNF@Lig composite films present an enhanced mechanical tensile strength of up to 133 MPa. Nacre-like deformable Ti3C2Tx/HCNF@Lig(3@1) composite films exhibit high conductivity (up to 1.75 × 105 S m-1) and mechanical properties (up to 258 MPa). The electrodes of Ti3C2Tx/HCNF@Lig(3@1)97/3 composite film assembled flexible solid-state supercapacitors possess an excellent volumetric specific capacitance of 748.96 F cm-3. The corresponding deformable supercapacitors show an excellent energy density of 16.2 W h L-1 and outstanding electrochemical cycling stability. The as-prepared nacre-like Ti3C2Tx/HCNF@Lig composite films with high mechanical properties and electrochemical performance are expected to be practically applied in flexible/wearable energy storage devices.Imogolite nanotubes are potentially promising co-photocatalysts because they are predicted to have curvature-induced, efficient electron-hole pair separation. This prediction has however not yet been experimentally proven. Here, we investigated the behavior upon irradiation of these inorganic nanotubes as a function of their water content to understand the fate of the generated electrons and holes. Two types of aluminosilicate nanotubes were studied one was hydrophilic on its external and internal surfaces (IMO-OH) and the other had a hydrophobic internal cavity due to Si-CH3 bonds (IMO-CH3), with the external surface remaining hydrophilic. Picosecond pulse radiolysis experiments demonstrated that the electrons are efficiently driven outward. For imogolite samples with very few external water molecules (around 1% of the total mass), quasi-free electrons were formed. They were able to attach to a water molecule, generating a water radical anion, which ultimately led to dihydrogen. When more external water molecules were present, solvated electrons, precursors of dihydrogen, were formed.

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