Steffensenrice1814

This study offers some new insights into tuning the crystal and electronic structures of LDHs by lattice doping to achieve high-efficiency electrocatalysis for OER.The direct and indirect photochemical degradation of rotenone (ROT) and deguelin (DEG), the primary reduced nicotinamide adenine dinucleotide-inhibiting rotenoid components of the piscicide CFT Legumine, were investigated under simulated sunlight conditions relevant to their dissipation from high-latitude surface waters. Photochemical degradation dominated the elimination of ROT and DEG from surface waters with half-lives ranging from 1.17 to 2.32 and 4.18 to 20.12 h for DEG and ROT, respectively, when the rotenoids were applied in the formulation CFT Legumine. We assessed enhanced degradation processes using argon-purged and cesium chloride-amended water, which demonstrated the rotenoids to rapidly decompose from excited triplet states. We further assessed the influence of reactive oxygen species by hydroxyl radical quenching and thermal generation of singlet oxygen. The studied reactive oxygen species did not significantly contribute; however, alcohols such as isopropanol may inhibit degradation by quenching ROT excited states or preventing intersystem crossing. Finally, we compared photochemical degradation in water collected from Hope Lake, Alaska, to a solution of Suwanee River fulvic acids, which demonstrated that dissolved organic matter (DOM) quality is a major factor that modulates ROT attenuation through a combination of shielding (light attenuation) and excited-state quenching mechanisms and is temperature-dependent. Molecular-level characterizations of DOM may help account for the site-specific degradation of these rotenoids in the environment.Ion exchange is a predominant and flexible route to tailor the composition and crystal structure of various materials. In situ monitoring of the ion exchange process at the single-particle level is critical to better understand the reaction mechanism and engineer high-performance materials. We report herein a dark-field imaging approach to in situ investigate the anion exchange reactions between individual Cu2O microparticles and S2- or Cl- assisted by the hydrolysis of Sn4+, which are visualized by directly observing the color change of single Cu2O microparticles. The variation of the scattering intensity is applied for quantitative analysis of anion exchange kinetics, revealing that this reaction process is dependent on the morphology, size, environmental pH, and reactant concentration. We directly observe that the corners of Cu2O are the preferential exchange sites, and the reaction activity is surface dependent. Moreover, the reaction rate constant and diffusion coefficient are estimated to be 1.1 × 10-2 s-1 and 9.4 × 10-11 cm2/s. Furthermore, a single-particle colorimetric assay is also fabricated for visual detection of S2-.Although ceria-based catalysts serve as an appealing alternative to traditional V2O5-based catalysts for selective catalytic reduction (SCR) of NOx with NH3, the inevitable deactivation caused by SO2 at low temperatures severely hampers the ceria-based catalysts to efficiently control NOx emissions from SO2-containing stack gases. Here, we rationally design a strong sulfur-resistant ceria-based catalyst by tuning the electronic structures of ceria highly dispersed on acidic MoO3 surfaces. By using Ce L3-edge X-ray absorption near edge structure spectra in conjunction with various surface and bulk structural characterizations, we report that the sulfur resistance of the catalysts is closely associated with the electronic states of ceria, particularly expressed by the Ce3+/Ce4+ ratio related to the size of the ceria particles. As the Ce3+/Ce4+ ratio increases up to or over 50%, corresponding to CeO2/MoO3(x %, x ≤ 2.1) with the particle size of approximately 4 nm or less, the non-bulk electronic states of ceria appear, where the catalysts start to show strong sulfur resistance. This work could provide a new strategy for designing sulfur-resistant ceria-based SCR catalysts for controlling NOx emissions at low temperatures.Lipid droplets (LDs) are intracellular lipid-rich organelles, which not only serve as neutral lipid reservoirs but also involve in many physiological processes and are associated with a variety of metabolic diseases and cancers. Long-term tracking of the state and behavior of LDs is of great significance but challenging. The difficulty is largely due to the lack of low cytotoxicity, high photobleaching resistance, and long intracellular retention probes that are capable of long-term tracking LDs. Herein, we report the discovery of two amphiphilic LD-targeting carbon nanoparticles (CNPs, i.e., CPDs and CDs) prepared by one-step room-temperature and hydrothermal methods. Their high lipid-water partition coefficient (log P > 2.13) and strong positive solvatochromism property ensure the quality of LD imaging. Especially, CDs exhibit favorable biocompatibility (2 mg mL-1, cell viability >90%), excellent photostability (after continuous laser irradiation on a confocal microscope for 2 h, relative FL intensity >85%), and superior intracellular retention ability, thereby enabling long-term tracking of LDs in hepatocytes for up to six passages. Based on the excellent long-term tracking ability, CDs are successfully applied to observe autophagy in a typical catabolic process and to evaluate the effect of a commonly used lipid-lowering drug atorvastatin on hepatocyte lipid uptake.Spontaneous processes triggered in a sample by free electrons, such as cathodoluminescence, are commonly regarded and detected as stochastic events. Here, we supplement this picture by showing through first-principles theory that light and free-electron pulses can interfere when interacting with a nanostructure, giving rise to a modulation in the spectral distribution of the cathodoluminescence light emission that is strongly dependent on the electron wave function. Specifically, for a temporally focused electron, cathodoluminescence can be canceled upon illumination with a spectrally modulated dimmed laser that is phase-locked relative to the electron density profile. We illustrate this idea with realistic simulations under attainable conditions in currently available ultrafast electron microscopes. We further argue that the interference between excitations produced by light and free electrons enables the manipulation of the ultrafast materials response by combining the spectral and temporal selectivity of the light with the atomic resolution of electron beams.Ethylenedinitramine (H2EDN, 1) was prepared in a simple manner and with a high overall yield by direct nitration of 2-imidazolidinone using 100% HNO3 at 0 °C and subsequent hydrolysis in water at 100 °C. The versatility of 1 allows its application as starting material for a broad range of different materials. It was used for the preparation of both various salts and cocrystalline materials incorporating varying amounts of the TATOT moiety. Furthermore, H2EDN was successfully applied in the concept of energetic coordination compounds (ECCs) resulting in five copper(II) and two silver(I) complexes. A reaction path for the direct precipitation or slow crystallization of 17 different salts, including several alkali, alkaline earth, silver, and nitrogen-rich samples, is presented. The substances were extensively characterized by low-temperature single-crystal X-ray diffraction, elemental analysis (EA), IR spectroscopy, differential thermal analysis (DTA), and thermogravimetric analysis (TGA), proving their high thermal stability, especially of the alkali salts. In addition, 1 and all salts were characterized by 1H, 13C, and 14N NMR, whereas 1 was also investigated using the beneficial 1H-15N HMBC NMR spectroscopy. The sensitivities toward various mechanical stimuli according to BAM standard methods, as well as ball drop impact and electrostatic discharge (ESD) were determined using the BAM 1-out-6 method. Hot plate and hot needle tests were performed, followed by further characterization of the copper(II)-based ECCs through laser ignition experiments and UV-vis spectroscopy, offering new candidates for nontoxic, less sensitive laser-ignitable materials. Several detonation parameters were calculated using EXPLO5 (V6.05.02).Purposively designing environmental advanced materials and elucidating the underlying reactivity mechanism at the atomic level allows for the further optimization of the removal performance for contaminants. Herein, using well facet-controlled I-Cu2WS4 single crystals as a model transition metal chalcogenide sorbent, we investigated the adsorption performance of the exposed facets toward gaseous elemental mercury (Hg0). We discovered that the decahedron exhibited not only facet-dependent adsorption properties for Hg0 but also recrystallization along the preferential [001] growth direction from a metastable state to the steady state. Besides, the metastable crystals with a predominant exposure of 101 facets dominated the promising adsorption efficiency (about 99% at 75 °C) while the saturated adsorption capacity was evaluated to be 2.35 mg·g-1. Subsequently, comprehensive characterizations and X-ray adsorption fine structure (XAFS), accompanied by density functional theory (DFT) calculations, revealed that it might be owing to the coordinatively unsaturated local environment of W atoms with S defects and the surface relative stability of different facets, which could be affected by the change in surface atom configuration. Hence, the new insight into the facet-dependent adsorption property of transition metal chalcogenide for Hg0 may have important implications, and the atomic-level study directly provides instructions for development and design of highly efficient functional materials.The wearable and self-powered sensors with multiple functions are urgently needed for energy saving devices, economical convenience, and artificial human skins. It is a meaningful idea to convert excess heat sources into power supplies for wearable sensors. In this report, we have fabricated a series of free-standing self-powered temperature-strain dual sensors based on poly(3,4-ethylenedioxythiophene) polystyrenesulfonate (PEDOTPSS)/carbon nanocoils (CNCs)-poly(vinyl) alcohol composite films by a simple drop casting method. The Seebeck coefficients of the composite films were measured to be 19 μV/K. The sensor, with the addition of CNCs, showed a superior sensing performance to that without CNCs. PEDOTPSS is used to provide a thermoelectric power to detect temperature changes and strain deformations. read more The minimum detect limit for the temperature difference was 0.3 K. Under a constant temperature gradient of 30 K, strains from 1 to 10% were detected without any external power supply. The films can be easily made into an array to detect the temperature of the fingers and motions of the wrist by attaching it to the human wrist directly. For the first time, due to the independent action of the thermoelectric material and strain sensing material, the thermoelectric voltage which is generated by a constant temperature difference is maintained under different strains. This kind of free-standing self-powered multifunctional sensors has great application prospects in the fields of healthcare and artificial intelligence in the future.