scholarly journals Synthesis, Characterization and Kinetic Behavior of Supported Cobalt Catalysts for Oxidative after-Treatment of Methane Lean Mixtures

Materials ◽  
2019 ◽  
Vol 12 (19) ◽  
pp. 3174 ◽  
Author(s):  
Andoni Choya ◽  
Beatriz de Rivas ◽  
Jose Ignacio Gutiérrez-Ortiz ◽  
Juan Ramón González-Velasco ◽  
Rubén López-Fonseca

The present work addresses the influence of the support on the catalytic behavior of Co3O4-based catalysts in the combustion of lean methane present in the exhaust gases from natural gas vehicular engines. Three different supports were selected, namely γ-alumina, magnesia and ceria and the corresponding catalysts were loaded with a nominal cobalt content of 30 wt. %. The samples were characterized by N2 physisorption, wavelength dispersive X-ray fluorescence (WDXRF), X-ray diffraction (XRD), Raman spectroscopy, X-ray photoelectron spectroscopy (XPS) and temperature-programmed reduction with hydrogen and methane. The performance was negatively influenced by a strong cobalt-support interaction, which in turn reduced the amount of active cobalt species as Co3O4. Hence, when alumina or magnesia supports were employed, the formation of CoAl2O4 or Co–Mg mixed oxides, respectively, with a low reducibility was evident, while ceria showed a lower affinity for deposited cobalt and this remained essentially as Co3O4. Furthermore, the observed partial insertion of Ce into the Co3O4 lattice played a beneficial role in promoting the oxygen mobility at low temperatures and consequently the catalytic activity. This catalyst also exhibited a good thermal stability while the presence of water vapor in the feedstream induced a partial inhibition, which was found to be completely reversible.

Materials ◽  
2019 ◽  
Vol 12 (11) ◽  
pp. 1771 ◽  
Author(s):  
Stefan Neatu ◽  
Mihaela M. Trandafir ◽  
Adelina Stănoiu ◽  
Ovidiu G. Florea ◽  
Cristian E. Simion ◽  
...  

This study presents the synthesis and characterization of lanthanum-modified alumina supported cerium–manganese mixed oxides, which were prepared by three different methods (coprecipitation, impregnation and citrate-based sol-gel method) followed by calcination at 500 °C. The physicochemical properties of the synthesized materials were investigated by various characterization techniques, namely: nitrogen adsorption-desorption isotherms, X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), scanning electron microscopy (SEM) and H2–temperature programmed reduction (TPR). This experimental study demonstrated that the role of the catalytic surface is much more important than the bulk one. Indeed, the incipient impregnation of CeO2–MnOx catalyst, supported on an optimized amount of 4 wt.% La2O3–Al2O3, provided the best results of the catalytic combustion of methane on our catalytic micro-convertors. This is mainly due to: (i) the highest pore size dimensions according to the Brunauer-Emmett-Teller (BET) investigations, (ii) the highest amount of Mn4+ or/and Ce4+ on the surface as revealed by XPS, (iii) the presence of a mixed phase (Ce2MnO6) as shown by X-ray diffraction; and (iv) a higher reducibility of Mn4+ or/and Ce4+ species as displayed by H2–TPR and therefore more reactive oxygen species.


Materials ◽  
2020 ◽  
Vol 14 (1) ◽  
pp. 48
Author(s):  
Pawel Mierczynski ◽  
Magdalena Mosińska ◽  
Lukasz Szkudlarek ◽  
Karolina Chalupka ◽  
Misa Tatsuzawa ◽  
...  

Biodiesel production from rapeseed oil and methanol via transesterification reaction facilitated by various monometallic catalyst supported on natural zeolite (NZ) was investigated. The physicochemical characteristics of the synthesized catalysts were studied by X-ray diffraction (XRD), Brunauer–Emmett–Teller method (BET), temperature-programmed-reduction in hydrogen (H2-TPR), temperature-programmed-desorption of ammonia (NH3-TPD), Scanning Electron Microscope equipped with EDX detector (SEM-EDS), and X-ray photoelectron spectroscopy (XPS) methods. The highest activity and methyl ester yields were obtained for the Pt/NZ catalyst. This catalyst showed the highest triglycerides conversion of 98.9% and fatty acids methyl esters yields of 94.6%. The activity results also confirmed the high activity of the carrier material (NZ) itself in the investigated reaction. Support material exhibited 90.5% of TG conversion and the Fatty Acid Methyl Esters yield (FAME) of 67.2%. Introduction of noble metals improves the TG conversion and FAME yield values. Increasing of the metal loading from 0.5 to 2 wt.% improves the reactivity properties of the investigated catalysts.


Catalysts ◽  
2020 ◽  
Vol 10 (2) ◽  
pp. 202
Author(s):  
Long Lu ◽  
Xueman Wang ◽  
Chunhua Hu ◽  
Ying Liu ◽  
Xiongbo Chen ◽  
...  

Nanosized V-Ce oxides supported on TiO2 (VCT) were prepared and utilized in the low-temperature selective catalytic reduction (SCR) of NO with NH3. Compared with the other V-Ce oxides-based catalysts supported on Al2O3, ZrO2, and ZSM-5, VCT showed the best SCR activity in a low-temperature range. The NOx conversion of 90% could be achieved at 220 °C. Characterizations including X-ray diffraction (XRD), scanning election micrograph (SEM), transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS), temperature-programmed desorption with NH3 (NH3-TPD), and temperature-programmed reduction with H2 (H2-TPR) showed that V1.05Ce1/TiO2 exhibited a good dispersion of V2O5, enrichment of surface Ce3+ and chemical-absorbed oxygen, and excellent redox capacity and acidity, which resulted in the best SCR performance at low temperature.


2017 ◽  
Vol 2 (1) ◽  
pp. 51-61
Author(s):  
Nima Mohammadi Taher ◽  
Maedeh Mahmoudi ◽  
Seyyede Shahrzad Sajjadivand

Abstract An investigation was done to develop and characterize the alumina supported cobalt catalyst for Fischer-Tropsch Synthesis to produce biodiesel from biomass with the aim to produce alumina-supported cobalt catalysts containing 7 to 19 wt.% cobalt content. By using incipient wetness impregnation of γ-Al2O3 supports with cobalt nitrate hexahydrate with ethanol and distilled water solutions; the 14 wt.% cobalt content in catalyst was achieved. Nitrogen adsorption-desorption, X-ray diffraction (XRD), scanning electron microscopy (SEM), energy dispersive spectroscopy (EDS), X-ray fluorescence (XRF), H2temperature programmed reduction (H2-TPR), temperature programmed desorption (TPD), temperature programmed oxidation (TPO) and carbon monoxide chemisorption were used for the characterization of the catalysts to attain an appropriate cobalt catalyst. In order to investigate the effect of the impregnation on the crystalline size, surface area and cobalt content, three different impregnation methods with various durations were investigated. In addition, increasing the impregnation duration increased the cobalt content and its dispersion. Based on results, positive effect of the alumina support and impregnation duration on the crystallite size, surface area, and pore diameter, reducibility of the catalyst and cobalt dispersion were investigated. Thus, cobalt catalyst for using in fixed bed reactor to produce biodiesel from biomass through Fischer-Tropsch Synthesis was prepared and characterized.


Crystals ◽  
2020 ◽  
Vol 10 (6) ◽  
pp. 530 ◽  
Author(s):  
Chaoqun Bian ◽  
Xiao Wang ◽  
Lan Yu ◽  
Fen Zhang ◽  
Jie Zhang ◽  
...  

The incorporation of metal heteroatoms into zeolites is an effective modification strategy for enhancing their catalytic performance. Herein, for the first time we report a generalized methodology for inserting metal heteroatoms (such as Sn, Fe, Zn, and Co) into the layered zeolite precursor RUB-36 via interlayer expansion by using the corresponding metal acetylacetate salt. Through this generalized methodology, Sn-JHP-1, Fe-JHP-1, Zn-JHP-1 and Co-JHP-1 zeolites could be successfully prepared by the reaction of RUB-36 and corresponding metal acetylacetate salt at 180 °C for 24 h in the presence of HCl solution. As a typical example, Sn-JHP-1 and calcined Sn-JHP-1 (Sn-JHP-2) zeolite is well characterized by the X-ray diffraction (XRD), diffuse reflectance ultraviolet-visible (UV-Vis), inductively coupled plasma (ICP), N2 sorption, temperature-programmed-desorption of ammonia (NH3-TPD) and X-ray photoelectron spectroscopy (XPS) techniques, which confirm the expansion of adjacent interlayers and thus the incorporation of isolated Sn sites within the zeolite structure. Notably, the obtained Sn-JHP-2 zeolite sample shows enhanced catalytic performance in the conversion of glucose to levulinic acid (LA) reaction.


Catalysts ◽  
2019 ◽  
Vol 9 (1) ◽  
pp. 62 ◽  
Author(s):  
Gunugunuri K. Reddy ◽  
Torin C. Peck ◽  
Charles A. Roberts

Direct decomposition of NO into N2 and O2 (2NO→N2 + O2) is recognized as the “ideal” reaction for NOx removal because it needs no reductant. It was reported that the spinel Co3O4 is one of the most active single-element oxide catalysts for NO decomposition at higher reaction temperatures, however, activity remains low below 650 °C. The present study aims to investigate new promoters for Co3O4, specifically PdO vs. PtO. Interestingly, the PdO promoter effect on Co3O4 was much greater than the PtO effect, yielding a 4 times higher activity for direct NO decomposition at 650 °C. Also, Co3O4 catalysts with the PdO promoter exhibit higher selectivity to N2 compared to PtO/Co3O4 catalysts. Several characterization measurements, including X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), H2-temperature programmed reduction (H2-TPR), and in situ FT-IR, were performed to understand the effect of PdO vs. PtO on the properties of Co3O4. Structural and surface analysis measurements show that impregnation of PdO on Co3O4 leads to a greater ease of reduction of the catalysts and an increased thermal stability of surface adsorbed NOx species, which contribute to promotion of direct NO decomposition activity. In contrast, rather than remaining solely as a surface species, PtO enters the Co3O4 structure, and it promotes neither redox properties nor NO adsorption properties of Co3O4, resulting in a diminished promotional effect compared to PdO.


2015 ◽  
Vol 1118 ◽  
pp. 20-27
Author(s):  
Jing Yang ◽  
Bao Song Li ◽  
Xiang Huo ◽  
Hao Xu ◽  
Hai Yun Hou

Pd/SiO2 organic-inorganic hybrid materials were prepared by adding PdCl2 into methyl-modified silica sol. The Pd/SiO2 hybrid materials were characterized by X-ray diffraction (XRD), fourier transform infrared (FTIR) and X-ray photoelectron spectroscopy (XPS). The effects of calcination temperature and Pd-doping on the phase transition of Pd element and the thermal stability of CH3 group in the Pd/SiO2 organic-inorganic hybrid materials were investigated. The results showed that the reduced metallic Pd0 exhibits good thermal stability under H2 atmosphere in the calcination process. Pd element in noncalcined Pd/SiO2 materials exists in PdCl2 form, calcination at 200 °C in a H2 atmosphere produces some metallic Pd0 and calcinations at 350 °C results in the complete transformation of Pd2+ to metallic Pd0. With the increase of calcination temperature, the Pd0 particle sizes increase and the hydrophobic Si−CH3 bands decrease in intensity. As the calcination temperature is greater than or equal to 350 °C, the loading of metallic Pd0 nearly has no influence on the chemical structure but, with the increase of Pd content, the formed Pd0 particle size increases. To keep the hydrophobicity of Pd/SiO2 membrane materials, the optimal calcination temperature is about 350 °C under H2 atmosphere.


2021 ◽  
Vol 16 (1) ◽  
pp. 97-110
Author(s):  
Faris A. Jassim Al-Doghachi ◽  
Diyar M. A. Murad ◽  
Huda S. Al-Niaeem ◽  
Salam H. H. Al-Jaberi ◽  
Surahim Mohamad ◽  
...  

Co/Mg1−XCe3+XO (x = 0, 0.03, 0.07, 0.15; 1 wt% cobalt each) catalysts for the dry reforming of methane (DRM) reaction were prepared using the co-precipitation method with K2CO3 as precipitant. Characterization of the catalysts was achieved by X-ray diffraction (XRD), X-ray fluorescence spectroscopy (XRF), X-ray photoelectron spectroscopy (XPS), temperature programmed reduction (H2-TPR), Brunauer–Emmett–Teller (BET), transmission electron microscopy (TEM), and thermal gravimetric analysis (TGA). The role of several reactant and catalyst concentrations, and reaction temperatures (700–900 °C) on the catalytic performance of the DRM reaction was measured in a tubular fixed-bed reactor under atmospheric pressure at various CH4/CO2 concentration ratios (1:1 to 2:1). Using X-ray diffraction, a surface area of 19.2 m2.g−1 was exhibited by the Co/Mg0.85Ce3+0.15O catalyst and MgO phase (average crystallite size of 61.4 nm) was detected on the surface of the catalyst. H2 temperature programmed reaction revealed a reduction of CoO particles to metallic Co0 phase. The catalytic stability of the Co/Mg0.85Ce3+0.15O catalyst was achieved for 200 h on-stream at 900 °C for the 1:1 CH4:CO2 ratio with an H2/CO ratio of 1.0 and a CH4, CO2 conversions of 75% and 86%, respectively. In the present study, the conversion of CH4 was improved (75%–84%) when conducting the experiment at a lower flow of oxygen (1.25%). Finally, the deposition of carbon on the spent catalysts was analyzed using TEM and Temperature programmed oxidation-mass spectroscopy (TPO-MS) following 200 h under an oxygen stream. Better anti-coking activity of the reduced catalyst was observed by both, TEM, and TPO-MS analysis. Copyright © 2021 by Authors, Published by BCREC Group. This is an open access article under the CC BY-SA   License (https://creativecommons.org/licenses/by-sa/4.0). 


Catalysts ◽  
2018 ◽  
Vol 8 (10) ◽  
pp. 415 ◽  
Author(s):  
Lingjuan Ma ◽  
Hongbin Ma ◽  
Dawei Han ◽  
Mingyue Qiu ◽  
Yafei Guan ◽  
...  

Rod-shaped Cu1Fe9Ox precursor was successfully prepared through an aqueous precipitation method. The shape and phase composition were characterized by X-ray diffraction (XRD) and transmission electron microscopy (TEM). It was found that Cu1Fe9Ox is composed of CuFe2O4 and Fe2O3. The reduction performance of Cu1Fe9Ox was studied by in situ XRD and H2 temperature-programmed reduction (H2-TPR). Cu/Fe3O4 nanorod catalyst is obtained through the controllable reduction of Cu1Fe9Ox nanorod, and the formed Cu/Fe3O4 nanorod catalyst does not have low-temperature water gas shift (WGS) activity, but exhibits high-temperature WGS reaction activity. Ambient pressure X-ray photoelectron spectroscopy (AP-XPS) studies showed that the main species of copper is Cu+ during the WGS reaction. The interaction between Cu and Fe3O4 rod and phase evolution of Cu species are quite different from Cu/Fe3O4 nanoparticles.


Coatings ◽  
2019 ◽  
Vol 9 (3) ◽  
pp. 180 ◽  
Author(s):  
Miriam Yuste ◽  
Ramon Escobar-Galindo ◽  
Noelia Benito ◽  
Carlos Palacio ◽  
Oscar Martínez ◽  
...  

ZnO films with Ti atoms incorporated (TZO) in a wide range (0–18 at.%) have been grown by reactive co-sputtering on silicon and glass substrates. The influence of the titanium incorporation in the ZnO matrix on the structural and optical characteristics of the samples has been determined by Rutherford backscattering spectroscopy (RBS), X-ray photoelectron spectroscopy (XPS) and X-ray diffraction (XRD). The results indicate that the samples with low Ti content (<4 at.%) exhibit a wurtzite-like structure, with the Ti4+ ions substitutionally incorporated into the ZnO structure, forming Ti-doped ZnO films. In particular, a very low concentration of Ti (<0.9 at.%) leads to a significant increase of the crystallinity of the TZO samples. Higher Ti contents give rise to a progressive amorphization of the wurtzite-like structure, so samples with high Ti content (≥18 at.%) display an amorphous structure, indicating in the XPS analysis, a predominance of Ti–O–Zn mixed oxides. The energy gap obtained from absorption spectrophotometry increases from 3.2 eV for pure ZnO films to 3.6 eV for those with the highest Ti content. Ti incorporation in the ZnO samples <0.9 at.% raises both the blue (380 nm) and green (approx. 550 nm) bands of the photoluminescence (PL) emission, thereby indicating a significant improvement of the PL efficiency of the samples.


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