Bimetallic platinum-nickel (Pt-Ni) nanostructures represent an emerging class of electrocatalysts for oxygen reduction reaction (ORR) in fuel cells, but practical applications have been limited by catalytic activity and durability. We surface-doped Pt3Ni octahedra supported on carbon with transition metals, termed M-Pt3Ni/C, where M is vanadium, chromium, manganese, iron, cobalt, molybdenum (Mo), tungsten, or rhenium. The Mo-Pt3Ni/C showed the best ORR performance, with a specific activity of 10.3 mA/cm(2) and mass activity of 6.98 A/mg(Pt), which are 81- and 73-fold enhancements compared with the commercial Pt/C catalyst (0.127 mA/cm(2) and 0.096 A/mg(Pt)). Theoretical calculations suggest that Mo prefers subsurface positions near the particle edges in vacuum and surface vertex/edge sites in oxidizing conditions, where it enhances both the performance and the stability of the Pt3Ni catalyst.
Most of recent research on layered chalcogenides is understandably focused on single atomic layers. However, it is unclear if single-layer units are the most ideal structures for enhanced gas-solid interactions. To probe this issue further, we have prepared large-area MoS2 sheets ranging from single to multiple layers on 300 nm SiO2/Si substrates using the micromechanical exfoliation method. The thickness and layering of the sheets were identified by optical microscope, invoking recently reported specific optical color contrast, and further confirmed by AFM and Raman spectroscopy. The MoS2 transistors with different thicknesses were assessed for gas-sensing performances with exposure to NO2, NH3, and humidity in different conditions such as gate bias and light irradiation. The results show that, compared to the single-layer counterpart, transistors of few MoS2 layers exhibit excellent sensitivity, recovery, and ability to be manipulated by gate bias and green light. Further, our ab initio DFT calculations on single-layer and bilayer MoS2 show that the charge transfer is the reason for the decrease in resistance in the presence of applied field.
Moiré superlattices provide a powerful tool to engineer novel quantum phenomena in twodimensional (2D) heterostructures, where the interactions between the atomically thin layers qualitatively change the electronic band structure of the superlattice. For example, mini-Dirac points, tunable Mott insulator states, and the Hofstadter butterfly can emerge in different types of graphene/boron nitride moiré superlattices, while correlated insulating states and superconductivity have been reported in twisted bilayer graphene moiré superlattices 1-12 . In addition to their dramatic effects on the single particle states, moiré superlattices were recently predicted to host novel excited states, such as moiré exciton bands [13][14][15] . Here we report the first observation of moiré superlattice exciton states in nearly aligned WSe 2 /WS 2 heterostructures.These moiré exciton states manifest as multiple emergent peaks around the original WSe 2 A exciton resonance in the absorption spectra, and they exhibit gate dependences that are distinctly different from that of the A exciton in WSe 2 monolayers and in large-twist-angle WSe 2 /WS 2 heterostructures. The observed phenomena can be described by a theoretical model where the periodic moiré potential is much stronger than the exciton kinetic energy and creates multiple flat exciton minibands. The moiré exciton bands provide an attractive platform to explore and control novel excited state of matter, such as topological excitons and a correlated exciton Hubbard model, in transition metal dichalcogenides.
Room-temperature, bottom-gate, field-effect transistor characteristics of 2D ultrathin layer GaS and GaSe prepared from the bulk crystals using a micromechanical cleavage technique are reported. The transistors based on active GaS and GaSe ultrathin layers demonstrate typical n-and p-type conductance transistor operation along with a good ON/OFF ratio and electron differential mobility.
The Cu(I)-catalyzed azide-alkyne cycloaddition (CuAAC) is the standard method for bioorthogonal conjugation. However, current Cu(I) catalyst formulations are toxic, hindering their use in living systems. Here we report that BTTES, a tris(triazolylmethyl)amine-based ligand for Cu(I), promotes the cycloaddition reaction rapidly in living systems without apparent toxicity. This catalyst allows, for the first time, noninvasive imaging of fucosylated glycans during zebrafish early embryogenesis. We microinjected embryos with alkyne-bearing GDP-fucose at the one-cell stage and detected the metabolically incorporated unnatural sugars using the biocompatible click chemistry. Labeled glycans could be imaged in the enveloping layer of zebrafish embryos between blastula and early larval stages. This new method paves the way for rapid, noninvasive imaging of biomolecules in living organisms.
In oxide semiconductors, such as those based on indium zinc oxide (IXZO), a strong oxygen binding metal ion ("oxygen getter"), X, functions to control O vacancies and enhance lattice formation, hence tune carrier concentration and transport properties. Here we systematically study, in the IXZO series, the role of X = Ga(3+) versus the progression X = Sc(3+) → Y(3+) → La(3+), having similar chemical characteristics but increasing ionic radii. IXZO films are prepared from solution over broad composition ranges for the first time via low-temperature combustion synthesis. The films are characterized via thermal analysis of the precursor solutions, grazing incidence angle X-ray diffraction (GIAXRD), atomic force microscopy (AFM), X-ray photoelectron spectroscopy (XPS), and scanning transmission electron microscopy (STEM) with high angle annular dark field (HAADF) imaging. Excellent thin-film transistor (TFT) performance is achieved for all X, with optimal compositions after 300 °C processing exhibiting electron mobilities of 5.4, 2.6, 2.4, and 1.8 cm(2) V(-1) s(-1) for Ga(3+), Sc(3+), Y(3+), and La(3+), respectively, and with I(on)/I(off) = 10(7)-10(8). Analysis of the IXZO TFT positive bias stress response shows X = Ga(3+) to be superior with mobilities (μ) retaining >95% of the prestress values and threshold voltage shifts (ΔV(T)) of <1.6 V, versus <85% μ retention and ΔV(T) ≈ 20 V for the other trivalent ions. Detailed microstructural analysis indicates that Ga(3+) most effectively promotes oxide lattice formation. We conclude that the metal oxide lattice formation enthalpy (ΔH(L)) and metal ionic radius are the best predictors of IXZO oxygen getter efficacy.
Monolayer molybdenum disulfide (MoS2) is a promising two-dimensional direct-bandgap semiconductor with potential applications in atomically thin and flexible electronics. An attractive insulating substrate or mate for MoS2 (and related materials such as graphene) is hexagonal boron nitride (h-BN). Stacked heterostructures of MoS2 and h-BN have been produced by manual transfer methods, but a more efficient and scalable assembly method is needed. Here we demonstrate the direct growth of single- and few-layer MoS2 on h-BN by chemical vapor deposition (CVD) method, which is scalable with suitably structured substrates. The growth mechanisms for single-layer and few-layer samples are found to be distinct, and for single-layer samples low relative rotation angles (<5°) between the MoS2 and h-BN lattices prevail. Moreover, MoS2 directly grown on h-BN maintains its intrinsic 1.89 eV bandgap. Our CVD synthesis method presents an important advancement toward controllable and scalable MoS2-based electronic devices.
Aerogels are used in a broad range of scientific and industrial applications due to their large surface areas, ultrafine pore sizes, and extremely low densities. Recently, a large number of reports have described graphene aerogels based on the reduction of graphene oxide (GO). Though these GO-based aerogels represent a considerable advance relative to traditional carbon aerogels, they remain significantly inferior to individual graphene sheets due to their poor crystallinity. Here, we report a straightforward method to synthesize highly crystalline GO-based graphene aerogels via high-temperature processing common in commercial graphite production. The crystallization of the graphene aerogels versus annealing temperature is characterized using Raman and X-ray absorption spectroscopy, X-ray diffraction, and electron microscopy. Nitrogen porosimetry shows that the highly crystalline graphene macrostructure maintains a high surface area and ultrafine pore size. Because of their enhanced crystallinity, these graphene aerogels exhibit a ∼ 200 °C improvement in oxidation temperature and an order of magnitude increase in electrical conductivity.
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