Many catalytic reactions under fixed conditions exhibit oscillatory behaviour. The oscillations are often attributed to dynamic changes in the catalyst surface. So far, however, such relationships were difficult to determine for catalysts consisting of supported nanoparticles. Here, we employ a nanoreactor to study the oscillatory CO oxidation catalysed by Pt nanoparticles using time-resolved high-resolution transmission electron microscopy, mass spectrometry and calorimetry. The observations reveal that periodic changes in the CO oxidation are synchronous with a periodic refacetting of the Pt nanoparticles. The oscillatory reaction is modelled using density functional theory and mass transport calculations, considering the CO adsorption energy and the oxidation rate as site-dependent. We find that to successfully explain the oscillations, the model must contain the phenomenon of refacetting. The nanoreactor approach can thus provide atomic-scale information that is specific to surface sites. This will improve the understanding of dynamic properties in catalysis and related fields.

Herein, we report the synthesis of a γ-Al 2 O 3 -supported NiCo catalyst for dry methane reforming (DMR) and study the catalyst using in situ scanning transmission X-ray microscopy (STXM) during the reduction (activation step) and under reaction conditions. During the reduction process, the NiCo alloy particles undergo elemental segregation with Co migrating toward the center of the catalyst particles and Ni migrating to the outer surfaces. Under DMR conditions, the segregated structure is maintained, thus hinting at the importance of this structure to optimal catalytic functions. Finally, the formation of Ni-rich branches on the surface of the particles is observed during DMR, suggesting that the loss of Ni from the outer shell may play a role in the reduced stability and hence catalyst deactivation. These findings provide insights into the morphological and electronic structural changes that occur in a NiCo-based catalyst during DMR. Further, this study emphasizes the need to study catalysts under operating conditions in order to elucidate material dynamics during the reaction.

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The porous nature of carbon nanotube (CNT) arrays allows for the unique opportunity to tailor their mechanical response by the infiltration and deposition of nano-scale conformal coatings. Here, we fabricate novel photo-lithographically defined CNT pillars that are conformally coated with amorphous silicon carbide (a-SiC) to strengthen the interlocking of individual CNTs at junctions using low pressure chemical vapour deposition (LPCVD). We further quantify the mechanical response by performing flat-punch nanoindentation measurements on coated CNT pillars with various high-aspect-ratios. We discovered new mechanical failure modes of coated CNT pillars, such as "bamboo" and brittle-like composite rupture as coating thickness increases. Furthermore, a significant increase in strength and modulus is achieved. For CNT pillars with high aspect ratio (1:10) and coating thickness of 21.4 nm, the compressive strength increases by an order of magnitude of 3, towards 1.8 GPa (from below 1 MPa for uncoated CNT pillars) and the elastic modulus increases towards 125 GPa. These results show that our coated CNT pillars, which can serve as vertical interconnects and 3D super-capacitors, can be transformed into robust high-aspectratio 3D-micro architectures with semiconductor device compatible processes.

In view of the integration of membrane resonators with more complex MEMS structures, we developed a general fabrication procedure for circular shape SiNx membranes using Deep Reactive Ion Etching (DRIE). Large area and high-stress SiNx membranes were fabricated and used as optomechanical resonators in a Michelson interferometer, where Q values up to 1.3 × 106 were measured at cryogenic temperatures, and in a Fabry-Pérot cavity, where an optical finesse up to 50000 has been observed