Griffinwebb6421

Taking CO oxidations on Pt(111) and Pt(100) as examples, we demonstrate that the FSR approach can properly reproduce the results of an equivalent first-principles microkinetic model simulation with more reasonable reaction rates. The improved kMC simulation based on the FSR method can accurately incorporate the effect of the fast diffusion of species on the surface and provide several orders of magnitude of acceleration compared to the standard kMC simulation.A halide perovskite based photocatalyst has been demonstrated for the first time to simultaneously achieve efficient photocatalytic CO2 reduction and methanol oxidation, exhibiting an exciting yield of 1835 μmol g-1 for photocatalytic CO2-to-CO conversion. Moreover, almost stoichiometric value-added formic acid can be produced from methanol oxidation.Copper sulfides have attracted great attention recently in the thermoelectric community due to the liquid-like behavior of Cu ions. Among the numerous copper sulfides, digenite Cu1.80S has a poorer thermoelectric performance but better stability than the state-of-the-art binary copper sulfide Cu1.97S. In this study, good stability and high thermoelectric performance were simultaneously obtained in Fe-doped Cu1.80S. Because Fe ions will not form a concentration gradient under an external field to change the critical voltage, Fe-doped Cu1.80S samples inherit the good stability of the pristine Cu1.80S. The critical voltage for Cu1.80Fe0.064S is 0.16 V at 750 K, which has been the largest value reported so far. Likewise, the Fe dopants can significantly improve the thermoelectric performance by suppressing the too high electrical conductivity of Cu1.80S. The peak dimensionless figure of merit (zT) for Cu1.80Fe0.064S is around 0.8 at 750 K, about four times that of Cu1.80S. The average zT for Cu1.80Fe0.064S is 0.40 in 300-750 K, which is amongst the highest values in reported thermoelectric sulfides. Combining the good stability and high thermoelectric performance, the present Cu1.80Fe0.064S has great potential to be used in the application of waste heat harvesting in the middle temperature range.In this work, a disposable molecularly imprinted electrochemical sensor was developed towards the highly sensitive and selective detection of the organophosphorus insecticide phosalone (PAS), employing a home-made carbon paste microelectrode (CPME) modified with a Zr-based metal-organic framework catalyst (Pt-UiO-66) and a mesoporous structured conductive molecularly imprinted polymer (MIP). Pt-UiO-66 octahedra with isolated dispersed Pt nanoparticle active sites were firstly incorporated into the CPME to provide a remarkably amplified signal for voltammetric determination. The mesoporous MIP was then synthesized onto the Pt-UiO-66/CPME via electropolymerization and a subsequent sol-gel process, which could bind the PAS template molecules through hydrogen bond, coordinate bonding, hydrophobic interaction, and π-π stacking interaction. Morphological, structural, and electrochemical characterization studies revealed that this nano-sized MIP provided excellent features for PAS detection, including high porosity, large surface area, enhanced electron-transport ability, greatly improved diffusion capacity, and strong recognition specificity. BTK signaling pathway inhibitors Therefore, the resulting sensor exhibited an outstanding linearly proportional concentration domain of 0.50 nM-20 μM, low detection limit of 0.078 nM, marked selectivity over certain interferences with similar configurations, considerable repeatability, reproducibility, and stability for the analysis of PAS. Moreover, the sensor was successfully applied for the determination of PAS in agricultural products and environmental samples with results in good compatibility with a chromatographic method, indicative of the high reliability and practicability. Such an electrochemical sensor might open a novel window for the investigation of selective sensing of small organic species from their analogues coupled with the molecular imprinting technique.The development of a universal coating strategy for the construction of functional surfaces and modulation of surface properties is of great research interest. Tannic acid (TA) could serve as a sole precursor for the deposition of colorless coatings on substrate surfaces. However, the deposition of TA requires a high salt concentration (0.6 M), which may limit its practical application. Herein, primary amine moieties were introduced on the gallic acid groups in TA. The resultant amine-containing TA derivative (TAA) can self-polymerize under mild conditions (10 mM, Tris buffer), and form uniform and colorless coatings in a material-independent manner. In comparison with the TA coating under the same preparation conditions, the TAA coating exhibits an increased thickness as measured by ellipsometry. The TAA coating is adapted for secondary surface functionalization. The hydrophilic mPEG brushes can be grafted on the TAA coating to inhibit non-specific protein adsorption. A biotin probe can be immobilized on the TAA coating to promote specific binding with avidin. In addition, the TAA coating can be utilized for in situ reduction of silver ions to AgNPs. The resulting AgNP-loaded TAA coating can inhibit bacterial adhesion and prevent biofilm formation.Dry reforming of methane (DRM) is an attractive reaction that consumes two major greenhouse gases while producing the industrially important components of syngas. In this study, various semiconductors were examined as light-harvesting support materials to promote catalytic DRM reaction under mild conditions. Among the metal-loaded catalysts, rhodium-loaded tantalum oxynitride (Rh/TaON) drove the DRM reaction even under visible light irradiation (>400 nm), and its activity exceeded the thermal catalyst limit. According to our spectroscopic analysis and the surface temperature measurement, the bandgap excitation of TaON dominantly promotes the DRM reaction in addition to its photo-thermal effect.A novel transformation for the construction of Csp3-Csp bonds was achieved via a photo-induced copper-catalysed C-C bond cleavage. This approach was applied to prepare a series of highly functionalized alkynyl nitriles using readily available cyclobutanones and terminal alkynes. Mechanistic exploration showed that the in situ generated copper acetylide complex is an effective photosensitive catalyst to promote the C-C bond cleavage of cycloketoxime esters through a radical process.