6 research outputs found

    Detecting Cage Crossing and Filling Clusters of Magnesium and Carbon Atoms in Zeolite SSZ-13 with Atom Probe Tomography

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    The conversion of methanol to valuable hydrocarbon molecules is of great commercial interest, as the process serves as a sustainable alternative for the production of, for instance, the base chemicals for plastics. The reaction is catalyzed by zeolite materials. By the introduction of magnesium as a cationic metal, the properties of the zeolite, and thereby the catalytic performance, are changed. With atom probe tomography (APT), nanoscale relations within zeolite materials can be revealed: i.e., crucial information for a fundamental mechanistic understanding. We show that magnesium forms clusters within the cages of zeolite SSZ-13, while the framework elements are homogeneously distributed. These clusters of just a few nanometers were analyzed and visualized in 3-D. Magnesium atoms seem to initially be directed to the aluminum sites, after which they aggregate and fill one or two cages in the zeolite SSZ-13 structure. The presence of magnesium in zeolite SSZ-13 increases the lifetime as well as the propylene selectivity. By using operando UV-vis spectroscopy and X-ray diffraction techniques, we are able to show that these findings are related to the suppression of aromatic intermediate products, while maintaining the formation of polyaromatic compounds. Further nanoscale analysis of the spent catalysts showed indications of magnesium redistribution after catalysis. Unlike zeolite H-SSZ-13, for which only a homogeneous distribution of carbon was found, carbon can be either homogeneously or heterogeneously distributed within zeolite Mg-SSZ-13 crystals as the magnesium decreases the coking rate. Carbon clusters were isolated, visualized, and analyzed and were assumed to be polyaromatic compounds. Small one-cage-filling polyaromatic compounds were identified; furthermore, large-cage-crossing aromatic molecules were found by isolating large coke clusters, demonstrating the unique coking mechanism in zeolite SSZ-13. Short-length-scale evidence for the formation of polyaromatic compounds at acid sites is discovered, as clear nanoscale relations between aluminum and carbon atoms exist

    Study of Spin-Orbit Interactions and Interlayer Ferromagnetic Coupling in Co/Pt/Co Trilayers in a Wide Range of Heavy-Metal Thickness

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    The spin-orbit torque, a torque induced by a charge current flowing through the heavy-metal-conducting layer with strong spin-orbit interactions, provides an efficient way to control the magnetization direction in heavy-metal/ferromagnet nanostructures, required for applications in the emergent magnetic technologies like random access memories, high-frequency nano-oscillators, or bioinspired neuromorphic computations. We study the interface properties, magnetization dynamics, magnetostatic features, and spin-orbit interactions within the multilayer system Ti(2)/Co(1)/Pt(0-4)/Co(1)/MgO(2)/Ti(2) (thicknesses in nanometers) patterned by optical lithography on micrometer-sized bars. In the investigated devices, Pt is used as a source of the spin current and as a nonmagnetic spacer with variable thickness, which enables the magnitude of the interlayer ferromagnetic exchange coupling to be effectively tuned. We also find the Pt thickness-dependent changes in magnetic anisotropies, magnetoresistances, effective Hall angles, and, eventually, spin-orbit torque fields at interfaces. The experimental findings are supported by the relevant interface structure-related simulations, micromagnetic, macrospin, as well as the spin drift-diffusion models. Finally, the contribution of the spin-orbital Edelstein-Rashba interfacial fields is also briefly discussed in the analysis.This work was supported by the National Science Centre, Poland, Grant No. 2016/23/B/ST3/01430 (SPINORBITRONICS). Numerical calculations were supported by PL-GRID infrastructure. As part of cooperation, the multilayer systems were deposited in the Institute of Molecular Physics Polish Academy of Sciences and nanofabrication was performed at the Academic Centre for Materials and Nanotechnology of the AGH University of Science and Technology. The authors would like to express their gratitude to Prof. F. Stobiecki for helpful discussions on data analysis. The authors also thank Jakub Mojsiejuk for his help with preparing numerical calculations. W.S. acknowledges National Science Centre Grant No. UMO-2015/17/D/ST3/00500, Poland

    Detecting Cage Crossing and Filling Clusters of Magnesium and Carbon Atoms in Zeolite SSZ-13 with Atom Probe Tomography

    No full text
    The conversion of methanol to valuable hydrocarbon molecules is of great commercial interest, as the process serves as a sustainable alternative for the production of, for instance, the base chemicals for plastics. The reaction is catalyzed by zeolite materials. By the introduction of magnesium as a cationic metal, the properties of the zeolite, and thereby the catalytic performance, are changed. With atom probe tomography (APT), nanoscale relations within zeolite materials can be revealed: i.e., crucial information for a fundamental mechanistic understanding. We show that magnesium forms clusters within the cages of zeolite SSZ-13, while the framework elements are homogeneously distributed. These clusters of just a few nanometers were analyzed and visualized in 3-D. Magnesium atoms seem to initially be directed to the aluminum sites, after which they aggregate and fill one or two cages in the zeolite SSZ-13 structure. The presence of magnesium in zeolite SSZ-13 increases the lifetime as well as the propylene selectivity. By using operando UV-vis spectroscopy and X-ray diffraction techniques, we are able to show that these findings are related to the suppression of aromatic intermediate products, while maintaining the formation of polyaromatic compounds. Further nanoscale analysis of the spent catalysts showed indications of magnesium redistribution after catalysis. Unlike zeolite H-SSZ-13, for which only a homogeneous distribution of carbon was found, carbon can be either homogeneously or heterogeneously distributed within zeolite Mg-SSZ-13 crystals as the magnesium decreases the coking rate. Carbon clusters were isolated, visualized, and analyzed and were assumed to be polyaromatic compounds. Small one-cage-filling polyaromatic compounds were identified; furthermore, large-cage-crossing aromatic molecules were found by isolating large coke clusters, demonstrating the unique coking mechanism in zeolite SSZ-13. Short-length-scale evidence for the formation of polyaromatic compounds at acid sites is discovered, as clear nanoscale relations between aluminum and carbon atoms exist
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