Self-sustained oscillations in oxidation of methane over palladium: The nature of “low active” and “highly active” states

Author(s):  
Vasily V. Kaichev ◽  
Zakhar S. Vinokurov ◽  
Andrey A. Saraev

The oxidation of methane was studied in a flow reactor at atmospheric pressure using palladium foil as a catalyst. It was shown that regular self-sustained reaction rate oscillations arise under...

2017 ◽  
Vol 7 (8) ◽  
pp. 1646-1649 ◽  
Author(s):  
A. A. Saraev ◽  
Z. S. Vinokurov ◽  
V. V. Kaichev ◽  
A. N. Shmakov ◽  
V. I. Bukhtiyarov

The self-sustained kinetic oscillations in the catalytic oxidation of methane over Ni foil have been studied at atmospheric pressure using an X-ray diffraction technique and mass spectrometry.


2008 ◽  
Vol 15 (06) ◽  
pp. 769-774 ◽  
Author(s):  
XIU-BIN REN ◽  
XIANG-YUN GUO

The oscillatory behavior during partial oxidation of methane was studied by the Monte Carlo simulation with Langmuir–Hinshelwood mechanism and oxide formation and removal. The well-developed reaction rate oscillations can be observed when the CH 4 adsorption probability varies in a small window. The oscillation window is very sensitive to the variation of reaction temperature. When the temperature increases, the window for sustained oscillation becomes narrow and has an obvious shift. In the meantime, the oscillation period tends to become small and the amplitude decreases. When the temperature increases to a certain value, the oscillations will disappear.


2019 ◽  
Author(s):  
Suchanuch Sachdev ◽  
Rhushabh Maugi ◽  
Sam Davis ◽  
Scott Doak ◽  
Zhaoxia Zhou ◽  
...  

<div>The interface between two immiscible liquids represent an ideal substrate for the assembly of nanomaterials. The defect free surface provides a reproducible support for creating densely packed ordered materials. Here a droplet flow reactor is presented for the synthesis and/ or assembly of nanomaterials at the interface of the emulsion. Each droplet acts as microreactor for a reaction between decamethylferrocene (DmFc) within the hexane and metal salts (Ag+/ Pd2+) in the aqueous phase. The hypothesis was that a spontaneous, interfacial reaction would lead to the assembly of nanomaterials creating a Pickering emulsion. The subsequent removal of the solvents showed how the Ag nanoparticles were trapped at the interface and retain the shape of the droplet, however the Pd nanoparticles were dispersed with no tertiary structure. To further exploit this, a one-step process where the particles are synthesised and then assembled into core-shell materials was proposed. The same reactions were performed in the presence of oleic acid stabilise Iron oxide nanoparticles dispersed within the hexane. It was shown that by changing the reaction rate and ratio between palladium and iron oxide a continuous coating of palladium onto iron oxide microspheres can be created. The same reaction with silver, was unsuccessful and resulted in the silver particles being shed into solution, or incorporated within the iron oxide micro particle. These insights offer a new method and chemistry within flow reactors for the creation of palladium and silver nanoparticles. We use the technique to create metal coated iron oxide nanomaterials but the methodology could be easily transferred to the assembly of other materials.</div><div><br></div>


1982 ◽  
Vol 47 (12) ◽  
pp. 3348-3361 ◽  
Author(s):  
Erich Lippert ◽  
Karel Mocek ◽  
Emerich Erdös

The reactivity of the anhydrous carbonates of alkaline metals with sulphur dioxide has been studied experimentally in dependence both on the nature of the cation and on the way of preparation of the anhydrous carbonate. The carbonates were prepared either by thermal decomposition of hydrogen carbonates or by thermal dehydration of carbonate hydrates. The carbonates of lithium, sodium, potassium, rubidium and caesium have been investigated. Kinetic measurements were carried out in a flow reactor in the integral regime at 423 K under atmospheric pressure, with a gas containing 0.2 vol.% of sulphur dioxide and 2.0 vol.% of water vapour in the nitrogen as a carrier gas. The reactivities have been compared on the basis of time dependence of the conversion of carbonate to sulphite.


1980 ◽  
Vol 45 (10) ◽  
pp. 2728-2741 ◽  
Author(s):  
Pavel Fott ◽  
Petr Schneider

Kinetics have been studied of the reaction system taking place during the reaction of thiophene on the cobalt-molybdenum catalyst in a gradientless circulation flow reactor at 360 °C and atmospheric pressure. Butane has been found present in a small amount in the reaction products even at very low conversion. In view of this, consecutive and parallel-consecutive (triangular) reaction schemes have been proposed. In the former scheme the appearance of butane is accounted for by rate of desorption of butene being comparable with the rate of its hydrogenation. According to the latter scheme part of the butane originates from thiophene via a different route than through hydrogenation of butene. Analysis of the kinetic data has revealed that the reaction of thiophene should be considered to take place on other active sites than that of butene. Kinetic equations derived on this assumption for the consecutive and the triangular reaction schemes correlate experimental data with acceptable accuracy.


2020 ◽  
Vol 8 (35) ◽  
pp. 13195-13205 ◽  
Author(s):  
Swathi Mukundan ◽  
Daria Boffito ◽  
Abhijit Shrotri ◽  
Luqman Atanda ◽  
Jorge Beltramini ◽  
...  

2013 ◽  
Vol 634-638 ◽  
pp. 624-627 ◽  
Author(s):  
Feng Jiang ◽  
Wei Xu ◽  
Lei Niu ◽  
Guo Min Xiao

Bulk vanadium-chromium oxide (VCrO) catalyst was prepared and characterized by N2 adsorption, XRD, NH3-TPD, H2-TPR, and Raman spectroscopy. XRD and Raman results showed that the VCrO catalyst was a kind of VV-CrIII composite oxide mainly consisted of crystalline V2O5 and CrVO4-Ⅲ (orthorhombic). NH3-TPD and H2-TPR results revealed that this catalyst had negligible surface acidity, and was easily reduced due to the formation of CrVO4-Ⅲ. Their catalytic activity was evaluated in the ammoxidation of 3-picoline to nicotinonitrile. Catalytic results showed that the bulk VCrO catalyst was highly active and selective; the nicotinonitrile selectivity and yield was up to 96.1%, 88.2% respectively at atmospheric pressure and 360 °C. The high selectivity was related closely to the low surface acidity of the catalyst.


2001 ◽  
Vol 15 (1) ◽  
pp. 44-51 ◽  
Author(s):  
Tetsuya Takemoto ◽  
Kenji Tabata ◽  
Yonghong Teng ◽  
Shuiliang Yao ◽  
Akira Nakayama ◽  
...  

Author(s):  
Jesús Andrés Tavizón Pozos ◽  
Gerardo Chávez Esquivel ◽  
Ignacio Cervantes Arista ◽  
José Antonio de los Reyes Heredia ◽  
Víctor Alejandro Suárez Toriello

Abstract The influence of Al2O3–ZrO2 and TiO2–ZrO2 supports on NiMo-supported catalysts at a different sulfur concentration in a model hydrodeoxygenation (HDO)-hydrodesulfurization (HDS) co-processing reaction has been studied in this work. A competition effect between phenol and dibenzothiophene (DBT) for active sites was evidenced. The competence for the active sites between phenol and DBT was measured by comparison of the initial reaction rate and selectivity at two sulfur concentrations (200 and 500 ppm S). NiMo/TiO2–ZrO2 was almost four-fold more active in phenol HDO co-processed with DBT than NiMo/Al2O3–ZrO2 catalyst. Consequently, more labile active sites are present on NiMo/TiO2–ZrO2 than in NiMo/Al2O3–ZrO2 confirmed by the decrease in co-processing competition for the active sites between phenol and DBT. DBT molecules react at hydrogenolysis sites (edge and rim) preferentially so that phenol reacts at hydrogenation sites (edge and edge). However, the hydrogenated capacity would be lost when the sulfur content was increased. In general, both catalysts showed similar functionalities but different degrees of competition according to the highly active NiMoS phase availability. TiO2–ZrO2 as the support provided weaker metal-support interaction than Al2O3–ZrO2, generating a larger fraction of easily reducible octahedrally coordinated Mo- and Ni-oxide species, causing that NiMo/TiO2–ZrO2 generated precursors of MoS2 crystallites with a longer length and stacking but with a higher degree of Ni-promotion than NiMo/Al2O3–ZrO2 catalyst.


Sign in / Sign up

Export Citation Format

Share Document