scholarly journals Ethanol Dehydrogenation: A Reaction Path Study by Means of Temporal Analysis of Products

Catalysts ◽  
2020 ◽  
Vol 10 (10) ◽  
pp. 1151
Author(s):  
Joachim Pasel ◽  
Johannes Häusler ◽  
Dirk Schmitt ◽  
Helen Valencia ◽  
Maria Meledina ◽  
...  

Conventional fossil fuels such as gasoline or diesel should be substituted in the future by environmentally-friendly alternatives in order to reduce emissions in the transport sector and thus mitigate global warming. In this regard, iso-butanol is very promising as its chemical and physical properties are very similar to those of gasoline. Therefore, ongoing research deals with the development of catalytically-supported synthesis routes to iso-butanol, starting from renewably-generated methanol. This research has already revealed that the dehydrogenation of ethanol plays an important role in the reaction sequence from methanol to iso-butanol. To improve the fundamental understanding of the ethanol dehydrogenation step, the Temporal Analysis of Products (TAP) methodology was applied to illuminate that the catalysts used, Pt/C, Ir/C and Cu/C, are very active in ethanol adsorption. H2 and acetaldehyde are formed on the catalyst surfaces, with the latter quickly decomposing into CO and CH4 under the given reaction conditions. Based on the TAP results, this paper proposes a reaction scheme for ethanol dehydrogenation and acetaldehyde decomposition on the respective catalysts. The samples are characterized by means of N2 sorption and Scanning Transmission Electron Microscopy (STEM).

2021 ◽  
Author(s):  
Nur Sena Yüzbasi ◽  
Andac Armutlulu ◽  
Thomas Huthwelker ◽  
Paula Abdala ◽  
Christoph Müller

Chemical looping is an emerging technology to produce high purity hydrogen from fossil fuels or biomass with the simultaneous capture of the CO2 produced at the distributed scale. This process requires the availability of stable Fe2O3-based oxygen carriers. Fe2O3-Al2O3 based oxygen carriers exhibit a decay in the H2 yield with cycle number due to the formation of FeAl2O4 that cannot be re-oxidized. In this study, the addition of sodium (via a sodium salt) in the synthesis of Fe2O3-Al2O3 oxygen carriers was assessed as a means to counteract the cyclic deactivation of the oxygen carrier. Detailed insight into the oxygen carrier’s structure was gained by combined X-ray powder diffraction (XRD), X-ray absorption spectroscopy (XAS) at the Al, Na and Fe K-edges and scanning transmission electron microscopy/energy-dispersive X-ray spectroscopy (STEM/EDX) analyses. The addition of sodium prevented the formation of FeAl2O4 and stabilized the oxygen carrier via the formation of a layered structure, Na-β-Al2O3 phase. The resulting material, Na-β-Al2O3 stabilized Fe2O3, showed a very high H2 yield of ca. 13.3 mmol/g during 15 cycles.


2021 ◽  
Author(s):  
Nur Sena Yüzbasi ◽  
Andac Armutlulu ◽  
Thomas Huthwelker ◽  
Paula Abdala ◽  
Christoph Müller

Chemical looping is an emerging technology to produce high purity hydrogen from fossil fuels or biomass with the simultaneous capture of the CO2 produced at the distributed scale. This process requires the availability of stable Fe2O3-based oxygen carriers. Fe2O3-Al2O3 based oxygen carriers exhibit a decay in the H2 yield with cycle number due to the formation of FeAl2O4 that cannot be re-oxidized. In this study, the addition of sodium (via a sodium salt) in the synthesis of Fe2O3-Al2O3 oxygen carriers was assessed as a means to counteract the cyclic deactivation of the oxygen carrier. Detailed insight into the oxygen carrier’s structure was gained by combined X-ray powder diffraction (XRD), X-ray absorption spectroscopy (XAS) at the Al, Na and Fe K-edges and scanning transmission electron microscopy/energy-dispersive X-ray spectroscopy (STEM/EDX) analyses. The addition of sodium prevented the formation of FeAl2O4 and stabilized the oxygen carrier via the formation of a layered structure, Na-β-Al2O3 phase. The resulting material, Na-β-Al2O3 stabilized Fe2O3, showed a very high H2 yield of ca. 13.3 mmol/g during 15 cycles.


Author(s):  
A. V. Crewe

The high resolution STEM is now a fact of life. I think that we have, in the last few years, demonstrated that this instrument is capable of the same resolving power as a CEM but is sufficiently different in its imaging characteristics to offer some real advantages.It seems possible to prove in a quite general way that only a field emission source can give adequate intensity for the highest resolution^ and at the moment this means operating at ultra high vacuum levels. Our experience, however, is that neither the source nor the vacuum are difficult to manage and indeed are simpler than many other systems and substantially trouble-free.


Author(s):  
J. S. Wall ◽  
J. P. Langmore ◽  
H. Isaacson ◽  
A. V. Crewe

The scanning transmission electron microscope (STEM) constructed by the authors employs a field emission gun and a 1.15 mm focal length magnetic lens to produce a probe on the specimen. The aperture size is chosen to allow one wavelength of spherical aberration at the edge of the objective aperture. Under these conditions the profile of the focused spot is expected to be similar to an Airy intensity distribution with the first zero at the same point but with a peak intensity 80 per cent of that which would be obtained If the lens had no aberration. This condition is attained when the half angle that the incident beam subtends at the specimen, 𝛂 = (4𝛌/Cs)¼


Author(s):  
L. Gandolfi ◽  
J. Reiffel

Calculations have been performed on the contrast obtainable, using the Scanning Transmission Electron Microscope, in the observation of thick specimens. Recent research indicates a revival of an earlier interest in the observation of thin specimens with the view of comparing the attainable contrast using both types of specimens.Potential for biological applications of scanning transmission electron microscopy has led to a proliferation of the literature concerning specimen preparation methods and the controversy over “to stain or not to stain” in combination with the use of the dark field operating mode and the same choice of technique using bright field mode of operation has not yet been resolved.


Author(s):  
J. M. Cowley

The comparison of scanning transmission electron microscopy (STEM) with conventional transmission electron microscopy (CTEM) can best be made by means of the Reciprocity Theorem of wave optics. In Fig. 1 the intensity measured at a point A’ in the CTEM image due to emission from a point B’ in the electron source is equated to the intensity at a point of the detector, B, due to emission from a point A In the source In the STEM. On this basis it can be demonstrated that contrast effects In the two types of instrument will be similar. The reciprocity relationship can be carried further to include the Instrument design and experimental procedures required to obtain particular types of information. For any. mode of operation providing particular information with one type of microscope, the analagous type of operation giving the same information can be postulated for the other type of microscope. Then the choice between the two types of instrument depends on the practical convenience for obtaining the required Information.


Author(s):  
James F. Hainfeld ◽  
Kyra M. Alford ◽  
Mathias Sprinzl ◽  
Valsan Mandiyan ◽  
Santa J. Tumminia ◽  
...  

The undecagold (Au11) cluster was used to covalently label tRNA molecules at two specific ribonucleotides, one at position 75, and one at position 32 near the anticodon loop. Two different Au11 derivatives were used, one with a monomaleimide and one with a monoiodacetamide to effect efficient reactions.The first tRNA labeled was yeast tRNAphe which had a 2-thiocytidine (s2C) enzymatically introduced at position 75. This was found to react with the iodoacetamide-Aun derivative (Fig. 1) but not the maleimide-Aun (Fig. 2). Reaction conditions were 37° for 16 hours. Addition of dimethylformamide (DMF) up to 70% made no improvement in the labeling yield. A high resolution scanning transmission electron micrograph (STEM) taken using the darkfield elastically scattered electrons is shown in Fig. 3.


Author(s):  
H. Koike ◽  
S. Sakurai ◽  
K. Ueno ◽  
M. Watanabe

In recent years, there has been increasing demand for higher voltage SEMs, in the field of surface observation, especially that of magnetic domains, dislocations, and electron channeling patterns by backscattered electron microscopy. On the other hand, the resolution of the CTEM has now reached 1 ∼ 2Å, and several reports have recently been made on the observation of atom images, indicating that the ultimate goal of morphological observation has beem nearly achieved.


Author(s):  
E. Zeitler ◽  
M. G. R. Thomson

In the formation of an image each small volume element of the object is correlated to an areal element in the image. The structure or detail of the object is represented by changes in intensity from element to element, and this variation of intensity (contrast) is determined by the interaction of the electrons with the specimen, and by the optical processing of the information-carrying electrons. Both conventional and scanning transmission electron microscopes form images which may be considered in this way, but the mechanism of image construction is very different in the two cases. Although the electron-object interaction is the same, the optical treatment differs.


Author(s):  
A. Kosiara ◽  
J. W. Wiggins ◽  
M. Beer

A magnetic spectrometer to be attached to the Johns Hopkins S. T. E. M. is under construction. Its main purpose will be to investigate electron interactions with biological molecules in the energy range of 40 KeV to 100 KeV. The spectrometer is of the type described by Kerwin and by Crewe Its magnetic pole boundary is given by the equationwhere R is the electron curvature radius. In our case, R = 15 cm. The electron beam will be deflected by an angle of 90°. The distance between the electron source and the pole boundary will be 30 cm. A linear fringe field will be generated by a quadrupole field arrangement. This is accomplished by a grounded mirror plate and a 45° taper of the magnetic pole.


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