Molecular level nucleation mechanisms of hierarchical MFI and MOR zeolite structures via non-stochastic pathways

Nanoscale ◽  
2020 ◽  
Vol 12 (30) ◽  
pp. 16292-16304
Author(s):  
Volkan Şahin ◽  
Abdulkerim Karabakan

Non-stochastic nucleation mechanisms were constructed for a precursor silicate structure with 1D molecular order which could crystallize into the 3D unit cells of MFI and MOR frameworks through different 2D nucleation stages.

2021 ◽  
Vol 7 (3) ◽  
pp. eabd9954 ◽  
Author(s):  
Chenxi Li ◽  
Jan Krohn ◽  
Martina Lippe ◽  
Ruth Signorell

Gas phase nucleation is a ubiquitous phenomenon in planetary atmospheres and technical processes, yet our understanding of it is far from complete. In particular, the enhancement of nucleation by the addition of a more volatile, weakly interacting gaseous species to a nucleating vapor has escaped molecular-level experimental investigation. Here, we use a specially designed experiment to directly measure the chemical composition and the concentration of nucleating clusters in various binary CO2-containing vapors. Our analysis suggests that CO2 essentially catalyzes nucleation of the low vapor pressure component through the formation of transient, hetero-molecular clusters and thus provides alternative pathways for nucleation to proceed more efficiently. This work opens up new avenues for the quantitative assessment of nucleation mechanisms involving transient species in multicomponent vapors.


Author(s):  
F.J. Sjostrand

In the 1940's and 1950's electron microscopy conferences were attended with everybody interested in learning about the latest technical developments for one very obvious reason. There was the electron microscope with its outstanding performance but nobody could make very much use of it because we were lacking proper techniques to prepare biological specimens. The development of the thin sectioning technique with its perfectioning in 1952 changed the situation and systematic analysis of the structure of cells could now be pursued. Since then electron microscopists have in general become satisfied with the level of resolution at which cellular structures can be analyzed when applying this technique. There has been little interest in trying to push the limit of resolution closer to that determined by the resolving power of the electron microscope.


Author(s):  
R.M. Glaeser ◽  
S.B. Hayward

Highly ordered or crystalline biological macromolecules become severely damaged and structurally disordered after a brief electron exposure. Evidence that damage and structural disorder are occurring is clearly given by the fading and eventual disappearance of the specimen's electron diffraction pattern. The fading and disappearance of sharp diffraction spots implies a corresponding disappearance of periodic structural features in the specimen. By the same token, there is a oneto- one correspondence between the disappearance of the crystalline diffraction pattern and the disappearance of reproducible structural information that can be observed in the images of identical unit cells of the object structure. The electron exposures that result in a significant decrease in the diffraction intensity will depend somewhat upon the resolution (Bragg spacing) involved, and can vary considerably with the chemical makeup and composition of the specimen material.


Author(s):  
P.P.K. Smith

Grains of pigeonite, a calcium-poor silicate mineral of the pyroxene group, from the Whin Sill dolerite have been ion-thinned and examined by TEM. The pigeonite is strongly zoned chemically from the composition Wo8En64FS28 in the core to Wo13En34FS53 at the rim. Two phase transformations have occurred during the cooling of this pigeonite:- exsolution of augite, a more calcic pyroxene, and inversion of the pigeonite from the high- temperature C face-centred form to the low-temperature primitive form, with the formation of antiphase boundaries (APB's). Different sequences of these exsolution and inversion reactions, together with different nucleation mechanisms of the augite, have created three distinct microstructures depending on the position in the grain.In the core of the grains small platelets of augite about 0.02μm thick have farmed parallel to the (001) plane (Fig. 1). These are thought to have exsolved by homogeneous nucleation. Subsequently the inversion of the pigeonite has led to the creation of APB's.


Author(s):  
E. Loren Buhle ◽  
Pamela Rew ◽  
Ueli Aebi

While DNA-dependent RNA polymerase represents one of the key enzymes involved in transcription and ultimately in gene expression in procaryotic and eucaryotic cells, little progress has been made towards elucidation of its 3-D structure at the molecular level over the past few years. This is mainly because to date no 3-D crystals suitable for X-ray diffraction analysis have been obtained with this rather large (MW ~500 kd) multi-subunit (α2ββ'ζ). As an alternative, we have been trying to form ordered arrays of RNA polymerase from E. coli suitable for structural analysis in the electron microscope combined with image processing. Here we report about helical polymers induced from holoenzyme (α2ββ'ζ) at low ionic strength with 5-7 mM MnCl2 (see Fig. 1a). The presence of the ζ-subunit (MW 86 kd) is required to form these polymers, since the core enzyme (α2ββ') does fail to assemble into such structures under these conditions.


Author(s):  
T. Schober

Nb, Ta and V are prototype substances for the study of the endothermic reactions of H with metals. Such metal-hydrogen reactions have gained increased importance due to the application of metal-hydrides in hydrogen- und heat storage devices. Electron microscopy and diffraction were demonstrated to be excellent methods in the study of hydride morphologies and structures (1). - Figures 1 and 2 show the NbH and TaH phase diagrams (2,3,4). EM techniques have contributed substantially to the elucidation of the structures and domain configurations of phases β, ζ and ε (1,4). Precision length measurement techniques of distances in reciprocal space (5) recently led to a detailed understanding of the distortions of the unit cells of phases ζ and ε (4). In the same work (4) the existence of the new phase η was shown. It is stable near -68 °C. The sequence of transitions is thus below 70 %.


Author(s):  
John H. Luft

With information processing devices such as radio telescopes, microscopes or hi-fi systems, the quality of the output often is limited by distortion or noise introduced at the input stage of the device. This analogy can be extended usefully to specimen preparation for the electron microscope; fixation, which initiates the processing sequence, is the single most important step and, unfortunately, is the least well understood. Although there is an abundance of fixation mixtures recommended in the light microscopy literature, osmium tetroxide and glutaraldehyde are favored for electron microscopy. These fixatives react vigorously with proteins at the molecular level. There is clear evidence for the cross-linking of proteins both by osmium tetroxide and glutaraldehyde and cross-linking may be a necessary if not sufficient condition to define fixatives as a class.


Author(s):  
A. F. Marshall ◽  
J. W. Steeds ◽  
D. Bouchet ◽  
S. L. Shinde ◽  
R. G. Walmsley

Convergent beam electron diffraction is a powerful technique for determining the crystal structure of a material in TEM. In this paper we have applied it to the study of the intermetallic phases in the Cu-rich end of the Cu-Zr system. These phases are highly ordered. Their composition and structure has been previously studied by microprobe and x-ray diffraction with sometimes conflicting results.The crystalline phases were obtained by annealing amorphous sputter-deposited Cu-Zr. Specimens were thinned for TEM by ion milling and observed in a Philips EM 400. Due to the large unit cells involved, a small convergence angle of diffraction was used; however, the three-dimensional lattice and symmetry information of convergent beam microdiffraction patterns is still present. The results are as follows:1) 21 at% Zr in Cu: annealed at 500°C for 5 hours. An intermetallic phase, Cu3.6Zr (21.7% Zr), space group P6/m has been proposed near this composition (2). The major phase of our annealed material was hexagonal with a point group determined as 6/m.


Author(s):  
J.A. Panitz

The first few atomic layers of a solid can form a barrier between its interior and an often hostile environment. Although adsorption at the vacuum-solid interface has been studied in great detail, little is known about adsorption at the liquid-solid interface. Adsorption at a liquid-solid interface is of intrinsic interest, and is of technological importance because it provides a way to coat a surface with monolayer or multilayer structures. A pinhole free monolayer (with a reasonable dielectric constant) could lead to the development of nanoscale capacitors with unique characteristics and lithographic resists that surpass the resolution of their conventional counterparts. Chemically selective adsorption is of particular interest because it can be used to passivate a surface from external modification or change the wear and the lubrication properties of a surface to reflect new and useful properties. Immunochemical adsorption could be used to fabricate novel molecular electronic devices or to construct small, “smart”, unobtrusive sensors with the potential to detect a wide variety of preselected species at the molecular level. These might include a particular carcinogen in the environment, a specific type of explosive, a chemical agent, a virus, or even a tumor in the human body.


Author(s):  
W. Chiu ◽  
M.F. Schmid ◽  
T.-W. Jeng

Cryo-electron microscopy has been developed to the point where one can image thin protein crystals to 3.5 Å resolution. In our study of the crotoxin complex crystal, we can confirm this structural resolution from optical diffractograms of the low dose images. To retrieve high resolution phases from images, we have to include as many unit cells as possible in order to detect the weak signals in the Fourier transforms of the image. Hayward and Stroud proposed to superimpose multiple image areas by combining phase probability distribution functions for each reflection. The reliability of their phase determination was evaluated in terms of a crystallographic “figure of merit”. Grant and co-workers used a different procedure to enhance the signals from multiple image areas by vector summation of the complex structure factors in reciprocal space.


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