Wildermclean8363

49 cd/A, 17 s, 3.95 lm/W and 6.37%, respectively. The investigation of crystallographic characteristics have shown that the LEC performance of these complexes depends on cationic-anionic interaction which has a significant influence on molecular stacking of the molecules. Because, complex 2bTFSI, with weak cationic-anionic interactions, shows strong π···π stacking interactions between the adjacent molecules, it is the best lighting application candidate among the complexes.Nitrogen-doped porous carbon spheres have attracted great interest in diversified fields owing to their unique physical and chemical properties. However, the synthesis of nitrogen-doped porous carbon spheres with hierarchical superstructures and refined micropore structures is still a challenge. Herein, we develop a molecular-scale silica templating strategy to prepare nitrogen-doped microporous carbon spheres (MCSSs) with high porosity and a well-defined micropore structure. Octa(aminophenyl) polyhedral oligomeric silsesquioxane is used as a building block in MCSS precursors to provide precise molecular-scale templating and nitrogen doping. The morphology of MCSSs can be easily tuned by choosing the proper solvent. The as-synthesized MCSS with a large surface area (2036 m2 g-1), narrow micropore size distribution, nitrogen doping, and hierarchical geometry can serve as an efficient selective adsorbent for CO2 and organic pollutants. Furthermore, the MCSS decorated with Fe-N-C active sites (MCSS-Fe) shows enhanced electrocatalytic ORR activity in alkaline solution. This novel approach may open a new avenue for controllable fabrication of porous carbon spheres with desired geometry and well-designed pore structure and show potential applications in selective adsorption and catalysis.Fluoridation of HfO2 was carried out with three commonly used solid-state fluoridation agents PVDF, PTFE, and NH4HF2. Clear and reproducible differences are observed in the reaction products of the fluoropolymer reagents and NH4HF2 with the latter more readily reacting in air. Strong evidence of distinct, previously unreported hafnium oxyfluoride phases is produced by both reactions, and efforts to isolate them were successful for the air-NH4HF2 reaction. Synchrotron XRD, 19F NMR, and elemental analysis were employed to characterize the phase-pure material which appears to be analogous to known Zr-O-F phases with anion-deficient α-UO3 structures such as Zr7O9F10. Comparison with the hydrolysis of β-HfF4 under identical conditions depicts that the NH4HF2 route produces the oxyfluoride with greater selectivity and at lower temperatures. Thermodynamic calculations were employed to explain this result. Potential reaction pathways for the NH4HF2 fluoridation of HfO2 are discussed.The use of cosmogenically produced sulfur-35 (T1/2 = 87 days) and sodium-22 (T1/2 = 2.6 years) as intrinsic tracers can provide valuable information on catchment hydrology, flow paths, and subsurface storage. A new and straightforward method was created to determine the activities of both 35S and 22Na in various water sources by pumping large volumes (up to 1000 L) of water through cation- and anion-exchange resin columns in the field to collect sodium and sulfate ions and simple chemistry in the lab. Samples are counted for 35S using liquid scintillation counting (LSC) and for 22Na via γ spectroscopy. Our novel in situ method provides faster sample throughput as well as better counting statistics and lower detection limits. Both methods were successfully applied at the Southern Sierra Critical Zone Observatory.The role of electrochemical interfaces in energy conversion and storage is unprecedented and more so the interlayers of two-dimensional (2D) heterostructures, where the physicochemical nature of these interlayers can be adjusted by cation intercalation. We demonstrate in situ intercalation of Ni2+ and Co2+ with similar ionic radii of ∼0.07 nm in the interlayer of 1T-WS2 while electrodepositing NiCo layered double hydroxide (NiCo-LDH) to create a 2D heterostructure. The extent of intercalation varies with the electrodeposition time. Electrodeposition for 90 s results in 22.4-nm-thick heterostructures, and charge transfer ensues from NiCo-LDH to 1T-WS2, which stabilizes the higher oxidation states of Ni and Co. Density functional theory calculations validate the intercalation principle where the intercalated Ni and Co d electrons contribute to the density of states at the Fermi level of 1T-WS2. Water electrolysis is taken as a representative redox process. The 90 s electrodeposited heterostructure needs the relatively lowest overpotentials of 134 ± 14 and 343 ± 4 mV for hydrogen and oxygen evolution reactions, respectively, to achieve a current density of ±10 mA/cm2 along with exceptional durability for 60 h in 1 M potassium hydroxide. The electrochemical parameters are found to correlate with enhanced mass diffusion through the cation and Cl--intercalated interlayer spacing of 1T-WS2 and the number of active sites. While 1T-WS2 is mostly celebrated as a HER catalyst in an acidic medium, with the help of intercalation chemistry, this work explores an unfound territory of this transition-metal dichalcogenide to catalyze both half-reactions of water electrolysis.Novel constrained Schiff-base ligands (inden) were developed based on the well-known salen ligands. click here Chromium complexes supported by the constrained inden ligands were successfully synthesized and used as catalysts for the synthesis of cyclic carbonates from epoxides and carbon dioxide (CO2). The catalyst having tert-butyl ( t Bu) groups as substituents in combination with tetrabutylammonium bromide (TBAB) as a cocatalyst exhibited very high catalytic activity with a turnover frequency of up to 14800 h-1 for the conversion of CO2 and propylene oxide into propylene carbonate exclusively at 100 °C and 300 psi of CO2 under solvent-free conditions. The catalyst was found to be highly active for various epoxide substrates to produce terminal cyclic carbonates in 100% selectivity.Antimony chalcogenides represent a family of materials of low toxicity and relative abundance, with a high potential for future sustainable solar energy conversion technology. However, solar cells based on antimony chalcogenides present open-circuit voltage losses that limit their efficiencies. These losses are attributed to several recombination mechanisms, with interfacial recombination being considered as one of the dominant processes. In this work, we exploit atomic layer deposition (ALD) to grow a series of ultrathin ZnS interfacial layers at the TiO2/Sb2S3 interface to mitigate interfacial recombination and to increase the carrier lifetime. ALD allows for very accurate control over the ZnS interlayer thickness on the ångström scale (0-1.5 nm) and to deposit highly pure Sb2S3. Our systematic study of the photovoltaic and optoelectronic properties of these devices by impedance spectroscopy and transient absorption concludes that the optimum ZnS interlayer thickness of 1.0 nm achieves the best balance between the beneficial effect of an increased recombination resistance at the interface and the deleterious barrier behavior of the wide-bandgap semiconductor ZnS. This optimization allows us to reach an overall power conversion efficiency of 5.09% in planar configuration.Epitaxial transition metal nitrides (TMNs) are an emerging class of crystalline thin film metals that can be heteroepitaxially integrated with common group III-nitride semiconductors such as GaN and AlN. Within a binary family of TMN compounds (i.e., Ta x N y ), several phases typically exist, many with similar crystal structures that are difficult to distinguish by conventional X-ray diffraction or other bulk characterization means. In this work, we demonstrate the combined power of high-resolution transmission and aberration-corrected scanning transmission electron microscopy for definitive phase identification of tantalum nitrides with different N-sublattice ordering. Analysis of molecular beam epitaxy-grown γ-Ta2N films on SiC substrates shows that the films are γ phase, threading dislocation-free, and Ta-deficient. The lack of Ta manifests as ordered Ta vacancy planar defects oriented in the plane perpendicular to the [0001] growth direction and accounts for the substoichiometry. Optimization of the growth parameters should reduce the Ta vacancy concentration, and alternatively, exploitation of the attractive nature of the Ta vacancies may enable novel planar structures. These findings serve as an important first step in applying this epitaxial TMN material for new electronic and superconducting device structures.A material-guided, regenerative approach to heal cranial defects requires a scaffold that cannot only achieve conformal fit into irregular geometries but also has bioactivity and suitable resorption rates. We have previously reported "self-fitting" shape-memory polymer (SMP) scaffolds based on poly(ε-caprolactone) diacrylate (PCL-DA) that shape recover to fill irregular defect geometries. However, PCL-DA scaffolds lack innate bioactivity and degrade very slowly. Polydimethylsiloxane (PDMS) has been shown to impart innate bioactivity and modify degradation rates when combined with organic cross-linked networks. Thus, this work reports the introduction of PDMS segments to form PCL/PDMS SMP scaffolds. These were prepared as co-matrices with three types of macromers to systematically alter PDMS content and cross-link density. Specifically, PCL90-DA was combined with linear-PDMS66-dimethacrylate (DMA) or 4-armed star-PDMS66-tetramethacrylate (TMA) macromers at 9010, 7525, and 6040 wt % ratios. Additionally, a triblock macromer (AcO-PCL45-b-PDMS66-b-PCL45-OAc), having a 6535 wt % ratio PCL/PDMS, was used. Scaffolds exhibited pore interconnectivity and uniform pore sizes and further maintained excellent shape-memory behavior. Degradation rates increased with PDMS content and reduced cross-link density, with phase separation contributing to this effect. Irrespective of PDMS content, all PCL/PDMS scaffolds exhibited the formation of carbonated hydroxyapatite (HAp) following exposure to simulated body fluid (SBF). While inclusion of PDMS expectedly reduced scaffold modulus and strength, mineralization increased these properties and, in some cases, to values exceeding or similar to the PCL-DA, which did not mineralize.Poly(3,4 ethylenedioxythiophene)poly(styrenesulfonate) (PEDOTPSS) is perhaps the most successful polymer material for thermoelectric (TE) applications. So far, treatments by high-boiling solvents, acid or base, or mixing with the carbon nanotube (CNT) are the main ways to improve its TE performance. Herein, we report the synergistically boosting TE properties of PEDOTPSS/single-walled CNT (SWCNT) composites by the ionic liquid (IL). The composites are prepared by physically mixing the SWCNT dispersion containing the IL with PEDOTPSS solution and subsequent vacuum filtration. The IL additive has two major functions, that is, inducing the phase separation of PEDOTPSS and a linear quinoid conformation of PEDOT and promoting the SWCNT dispersion. The maximum power factor at room temperature reaches 182.7 ± 9.2 μW m-1 K-2 (the corresponding electrical conductivity and Seebeck coefficient are 1602.6 ± 103.0 S cm-1 and 33.4 ± 0.4 μV K-1, respectively) for the free-standing flexible film of the PEDOTPSS/SWCNT composites with the IL, which is much higher than those of the pristine PEDOTPSS, the IL-free PEDOTPSS/SWCNT, and the SWCNT films.