Formic acid (HCOOH) has great potential as an in situ source of hydrogen for fuel cells, because it offers high energy density, is non-toxic and can be safely handled in aqueous solution. So far, there has been a lack of solid catalysts that are sufficiently active and/or selective for hydrogen production from formic acid at room temperature. Here, we report that Ag nanoparticles coated with a thin layer of Pd atoms can significantly enhance the production of H₂ from formic acid at ambient temperature. Atom probe tomography confirmed that the nanoparticles have a core-shell configuration, with the shell containing between 1 and 10 layers of Pd atoms. The Pd shell contains terrace sites and is electronically promoted by the Ag core, leading to significantly enhanced catalytic properties. Our nanocatalysts could be used in the development of micro polymer electrolyte membrane fuel cells for portable devices and could also be applied in the promotion of other catalytic reactions under mild conditions.
Abstract-Precipitation of the Al 3 Sc (L1 2 ) phase in aluminum alloys, containing 0.1, 0.2 or 0.3 wt% Sc, is studied with conventional transmission and high-resolution (HREM) electron microscopies. The exact morphologies of the Al 3 Sc precipitates were determined for the first time by HREM, in Al-0.1 wt% Sc and Al-0.3 wt% Sc alloys. The experimentally determined equilibrium shape of the Al 3 Sc precipitates, at 300°C and 0.3 wt% Sc, has 26 facets, which are the 6 {100} (cube), 12 {110} (rhombic dodecahedron), and 8 {111} (octahedron) planes, a Great Rhombicuboctahedron. This equilibrium morphology had been predicted by first principles calculations of the pertinent interfacial energies. The coarsening kinetics obey the (time) 1/3 kinetic law of Lifshitz-Slyozov-Wagner theory and they yield an activation energy for diffusion, 164±9 kJ/mol, that is in agreement with the values obtained from tracer diffusion measurements of Sc in Al and first principles calculations, which implies diffusion-controlled coarsening.
Summary
Atom‐probe tomography analysis of complex multilayer structures is a promising avenue for studying interfacial properties. However, significant artefacts in the three‐dimensional reconstructed data arise due to the field evaporation process. To clarify the origin and impact of these artefacts for a FeCoB/FeCo/MgO/FeCo/IrMn multilayer, tip shapes were observed by transmission electron microscopy and compared to those obtained by finite difference modelling of electric fields and evaporation processes. It was found that the emitter shape is not spherical and its surface morphology evolves during successive evaporation of the different layers. This evolving morphology contributes to the artefacts generally observed in the reconstructed atom‐probe data for multilayer structures because algorithms for three‐dimensional reconstruction are based on the assumption that the shape of the emitter during field evaporation is spherical. Some proposed improvements to data reconstruction are proposed.
With the significant improvement in high temperature creep properties and resistance to radiation damage by addition of nanoscale oxide features, oxide-dispersion strengthened (ODS) ferritic/martensitic alloys are potential candidates for structural applications in nuclear fusion reactors. The structure of the oxygen-rich nanofeatures was analyzed by atom-probe tomography in three ODS alloys: MA957, ODS Fe–12wt%Cr, and ODS Eurofer-97. Although field evaporation and reconstruction of the precipitates suffer from artefacts, a core/shell structure is found even for very small precipitates. Precipitate cores are Y rich while shell regions are enriched in Ti, Cr, or V depending on alloy composition.
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