Zeolites play a crucial part in acid-base heterogeneous catalysis. Fundamental insight into their internal architecture is of great importance for understanding their structure-function relationships. Here, we report on a new approach correlating confocal fluorescence microscopy with focused ion beam-electron backscatter diffraction, transmission electron microscopy lamelling and diffraction, atomic force microscopy and X-ray photoelectron spectroscopy to study a wide range of coffin-shaped MFI-type zeolite crystals differing in their morphology and chemical composition. This powerful combination demonstrates a unified view on the morphology-dependent MFI-type intergrowth structures and provides evidence for the presence and nature of internal and outer-surface barriers for molecular diffusion. It has been found that internal-surface barriers originate not only from a 90 degrees mismatch in structure and pore alignment but also from small angle differences of 0.5 degrees-2 degrees for particular crystal morphologies. Furthermore, outer-surface barriers seem to be composed of a silicalite outer crust with a thickness varying from 10 to 200 nm.
A combination of atomic force microscopy (AFM), high-resolution scanning electron microscopy (HR-SEM), focused-ion-beam scanning electron microscopy (FIB-SEM), X-ray photoelectron spectroscopy (XPS), confocal fluorescence microscopy (CFM), and UV/Vis and synchrotron-based IR microspectroscopy was used to investigate the dealumination processes of zeolite ZSM-5 at the individual crystal level. It was shown that steaming has a significant impact on the porosity, acidity, and reactivity of the zeolite materials. The catalytic performance, tested by the styrene oligomerization and methanol-to-olefin reactions, led to the conclusion that mild steaming conditions resulted in greatly enhanced acidity and reactivity of dealuminated zeolite ZSM-5. Interestingly, only residual surface mesoporosity was generated in the mildly steamed ZSM-5 zeolite, leading to rapid crystal coloration and coking upon catalytic testing and indicating an enhanced deactivation of the zeolites. In contrast, harsh steaming conditions generated 5-50 nm mesopores, extensively improving the accessibility of the zeolites. However, severe dealumination decreased the strength of the Brønsted acid sites, causing a depletion of the overall acidity, which resulted in a major drop in catalytic activity.
Break on through: Steaming‐induced mesopores of individual ZSM‐5 crystals were studied by a combination of focused ion beam (FIB) and scanning electron microscopy (SEM) tomography (see picture). In this manner, quantitative insight into the width, length, morphology, and distribution of mesopores generated within zeolite crystals has been obtained.
When a current is passed through a non-magnetic metal with strong spin-orbit coupling, an orthogonal spin current is generated. This spin current can be used to switch the magnetization of an adjacent ferromagnetic layer or drive its magnetization into continuous precession. The interface, which is not necessarily sharp, and the crystallographic structure of the nonmagnetic metal can both affect the strength of current-induced spin-orbit torques. Here, we investigate the effects of interface intermixing and film microstructure on spin-orbit torques in perpendicularly magnetized Ta/Co40Fe40B20/MgO trilayers with different Ta layer thickness (5 nm, 10 nm, 15 nm), greater than the spin diffusion length. Effective spin-orbit torques are determined from harmonic Hall voltage measurements performed at temperatures ranging from 20 K to 300 K. We account for the temperature dependence of damping-like and field-like torques by including an additional contribution from the Ta/CoFeB interface in the spin diffusion model. Using this approach, the temperature variations of the spin Hall angle in the Ta underlayer and at the Ta/CoFeB interface are determined separately. Our results indicate an almost temperature-independent spin Hall angle of in Ta and a strongly temperature-dependent for the intermixed Ta/CoFeB interface.
Magnetization dynamics in W/CoFeB, CoFeB/Pt and W/CoFeB/Pt multilayers was investigated using spin-orbit-torque ferromagnetic resonance (SOT-FMR) technique. An analytical model based on magnetization dynamics due to SOT was used to fit heavy metal (HM) thickness dependence of symmetric and antisymmetric components of the SOT-FMR signal. The analysis resulted in a determination of the properties of HM layers, such as spin Hall angle and spin diffusion length. The spin Hall angle of -0.36 and 0.09 has been found in the W/CoFeB and CoFeB/Pt bilayers, respectively, which add up in the case of W/CoFeB/Pt trilayer. More importantly, we have determined effective interfacial spin-orbit fields at both W/CoFeB and CoFeB/Pt interfaces, which are shown to cancel Oersted field for particular thicknesses of the heavy metal layers, leading to pure spin-current-induced dynamics and indicating the possibility for a more efficient magnetization switching.
A combination of in situ UV-Vis and confocal fluorescence micro-spectroscopy was used to study the template decomposition process in large zeolite ZSM-5 crystals. Correlation of polarized light dependent UV-Vis absorption spectra with confocal fluorescence emission spectra in the 400-750 nm region allowed extracting localized information on the nature and amount of chemical species formed upon detemplation at the single particle level. It has been found by means of polarized light dependent UV-Vis absorption measurements that the progressive growth of molecules follows the orientation of the straight channels of ZSM-5 crystals. Oligomerizing template derivatives lead to the subsequent build-up of methyl-substituted benzenium cations and more extended coke-like species, which are thermally stable up to ∼740 K. Complementary confocal fluorescence emission spectra showed nearly equal distribution of these molecules within the entire volume of the thermally treated zeolite crystals. The strongest emission bands were appearing in the orange/red part of the visible spectrum, confirming the presence of large polyaromatic molecules.
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