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Carbodicarbenes (CDCs) possess two lone pairs of electrons on their central carbone C atom (Ccarbone). Coordination to a transition metal via a σ bond leaves one pair of electrons with appropriate symmetry for π donation to the metal. However, the high energy of the latter also renders the CDC ligand potentially redox-active. Herein, we explore these alternatives in the redox series [Cr(L)2]n+ and [Co(L)2]n+ (n = 2-5), where L is a tridentate ligand comprised of a central CDC and two flanking pyridine donors. To this end, all members of both redox series were synthesized and their electronic structures were investigated by using a combination of 1H NMR, Evans' NMR, IR, UV-vis, and EPR spectroscopies, SQUID magnetometry, X-ray crystallography, and density functional theory studies. Whereas [CoII(L)2]2+ is a straightforward low-spin (S = 1/2) cobalt(II) complex, the corresponding chromium complex was found to feature an electronic structure that is intermediate between the two limiting resonance forms [CrIII(L•-)(L)]2+ and [CrII(L)2]2+. In the case of the tri-, tetra-, and pentacationic complexes, the qualitatively identical electronic structures [MIII(L)2]3+, [MIII(L•+)(L)]4+, and [MIII(L•+)2]5+ were observed for both metals. Thus, the metal ions retain a 3+ oxidation state throughout, and the higher redox states contain oxidized ligands. The majority of the unpaired spin on the cation radical ligands was calculated to be localized in π-symmetry orbitals on the coordinated Ccarbone atoms. Analogous behavior was previously reported for the corresponding iron redox series and, as such, redox noninnocence in oxidized CDC and, more broadly, carbone complexes is likely widely accessible.Transport of water, solutes, and contaminants through a thin film composite (TFC) membrane is governed by the intrinsic structure of its polyamide separation layer. https://www.selleckchem.com/products/VX-770.html In this work, we systematically characterized the nanoscale polyamide structure of four commercial TFC membranes to reveal the underlying structure-property relationship. For all the membranes, their polyamide layers have an intrinsic thickness in the range of 10-20 nm, which is an order of magnitude smaller than the more frequently reported apparent thickness of the roughness protuberances due to the ubiquitous presence of nanovoids within the rejection layers. Tracer filtration tests confirmed that these nanovoids are well connected to the pores in the substrates via the honeycomb-like opening of the backside of the polyamide layers such that the actual separation takes place at the frontside of the polyamide layer. Compared to SW30HR and BW30, loose membranes XLE and NF90 have thinner intrinsic thickness and greater effective filtration area (e.g., by the creation of secondary roughness features) for their polyamide layers, which correlates well to their significantly higher water permeability and lower salt rejection. With the aid of scanning electron microscopy, transmission electron microscopy, and tracer tests, the current study reveals the presence of nanosized defects in a polyamide film, which is possibly promoted by excessive interfacial degassing. The presence of such defects not only impairs the salt rejection but also has major implications for the removal of pathogens and micropollutants.Layered hybrid metal-halide perovskites with non-centrosymmetric crystal structure are predicted to show spin-selective band splitting from Rashba effects. Thus, fabrication of metal-halide perovskites with defined crystal symmetry is desired to control the spin-splitting in their electronic states. Here, we report the influence of halogen para-substituents on the crystal structure of benzylammonium lead iodide perovskites (4-XC6H4CH2NH3)2PbI4 (X = H, F, Cl, Br). Using X-ray diffraction and second-harmonic generation, we study structure and symmetry of single-crystal and thin-film samples. We report that introduction of a halogen atom lowers the crystal symmetry such that the chlorine- and bromine-substituted structures are non-centrosymmetric. The differences can be attributed to the nature of the intermolecular interactions between the organic molecules. We calculate electronic band structures and find good control of Rashba splittings. Our results present a facile approach to tailor hybrid layered metal halide perovskites with potential for spintronic and nonlinear optical applications.Thermoelectric (TE) materials have attracted extensive interest because of their ability to achieve direct heat-to-electricity conversion. They provide an appealing renewable energy source in a variety of applications by harvesting waste heat. The record-breaking figure of merit reported for single crystal SnSe has stimulated related research on its polycrystalline counterpart. Boosting the TE conversion efficiency requires increases in the power factor and decreases in thermal conductivity. It is still a big challenge, however, to optimize these parameters independently because of their complex interrelationships. Herein, we propose an innovative approach to decouple electrical and thermal transport by incorporating carbon fiber (CF) into polycrystalline SnSe. We show that the incorporation of highly conductive CF can successfully enhance the electrical conductivity, while greatly reducing the thermal conductivity of polycrystalline SnSe. As a result, a high TE figure-of-merit (zT) of 1.3 at 823 K is obtained in p-type SnSe/CF composite polycrystalline materials. Furthermore, SnSe samples incorporated with CFs exhibit superior mechanical properties, which are favorable for device fabrication applications. Our results indicate that the dispersion of CF can be a good way to greatly improve both TE and mechanical performance.Electrodeposition of conducting polymer-carbon composites from an electrolyte precursor solution is a facile one-step approach to fabricate device-ready electrodes for energy storage. A key challenge in this approach is the dispersion of the carbon nanomaterials with the aqueous precursor solution with previous approaches either heavily oxidizing the carbon nanomaterials or using high concentrations of anionic surfactants as dopants. However, the former reduces the electrical conductivity of carbon, while the latter reduces the ionic mobility of the conducting polymer due to the large anion size. Herein, for the first time we present a quaternary electrolyte formulation for the fabrication of pristine carbon and polypyrrole (PPy) composites that does not sacrifice either electron or ion mobility. The electrolyte uses lithium perchlorate (20 mM) as a supporting electrolyte and dopant, sodium dodecylbenzenesulfonate at a very low concentration (1.43 mM) as a surfactant, together with pristine carbon nanomaterials and pyrrole monomers.
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