scholarly journals Effect of Operating Temperature, Pressure and Potassium Loading on the Performance of Silica-Supported Cobalt Catalyst in CO2 Hydrogenation to Hydrocarbon Fuel

Catalysts ◽  
2019 ◽  
Vol 9 (10) ◽  
pp. 807 ◽  
Author(s):  
Iloy ◽  
Jalama

Potassium (1–5 wt.%)-promoted and unpromoted Co/SiO2 catalysts were prepared by impregnation method and characterized by nitrogen physisorption, temperature-programmed reduction (TPR), CO2 temperature-programmed desorption (TPD), X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS) techniques. They were evaluated for CO2 hydrogenation in a fixed bed reactor from 180 to 300 °C within a pressure range of 1–20 bar. The yield for hydrocarbon products other than methane (C2+) was found to increase with an increase in the operating temperature and went through a maximum of approximately 270 °C. It did not show any significant dependency on the operating pressure and decreased at potassium loadings beyond 1 wt.%. Potassium was found to enhance the catalyst ability to adsorb CO2, but limited the reduction of cobalt species during the activation process. The improved CO2 adsorption resulted in a decrease in surface H/C ratio, the latter of which enhanced the formation of C2+ hydrocarbons. The highest C2+ yield was obtained on the catalyst promoted with 1 wt.% of potassium and operated at an optimal temperature of 270 °C and a pressure of 1 bar.

Catalysts ◽  
2021 ◽  
Vol 11 (5) ◽  
pp. 553
Author(s):  
Mansurbek Urol ugli Abdullaev ◽  
Sungjune Lee ◽  
Tae-Wan Kim ◽  
Chul-Ung Kim

Among the zeolitic catalysts for the ethylene-to-propylene (ETP) reaction, the SSZ-13 zeolite shows the highest catalytic activity based on both its suitable pore architecture and tunable acidity. In this study, in order to improve the propylene selectivity further, the surface of the SSZ-13 zeolite was modified with various amounts of tungsten oxide ranging from 1 wt% to 15 wt% via a simple incipient wetness impregnation method. The prepared catalysts were characterized with several analysis techniques, specifically, powder X-ray diffraction (PXRD), Raman spectroscopy, temperature-programmed reduction of hydrogen (H2-TPR), temperature-programmed desorption of ammonia (NH3-TPD), inductively coupled plasma-atomic emission spectroscopy (ICP-AES), and N2 sorption, and their catalytic activities were investigated in a fixed-bed reactor system. The tungsten oxide-modified SSZ-13 catalysts demonstrated significantly improved propylene selectivity and yield compared to the parent H-SSZ-13 catalyst. For the tungsten oxide loading, 10 wt% loading showed the highest propylene yield of 64.9 wt%, which was 6.5 wt% higher than the pristine H-SSZ-13 catalyst. This can be related to not only the milder and decreased strong acid sites but also the diffusion restriction of bulky byproducts, as supported by scanning transmission electron microscopy-energy dispersive X-ray spectroscopy (STEM-EDS) observation.


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 (11) ◽  
pp. 541 ◽  
Author(s):  
Haiping Xiao ◽  
Chaozong Dou ◽  
Hao Shi ◽  
Jinlin Ge ◽  
Li Cai

A series of poisoned catalysts with various forms and contents of sodium salts (Na2SO4 and Na2S2O7) were prepared using the wet impregnation method. The influence of sodium salts poisoned catalysts on SO2 oxidation and NO reduction was investigated. The chemical and physical features of the catalysts were characterized via NH3-temperature programmed desorption (NH3-TPD), H2-temperature programmed reduction (H2-TPR), X-ray photoelectron spectroscopy (XPS), Brunauer–Emmett–Teller (BET), X-ray diffraction (XRD), and Fourier Transform Infrared Spectroscopy (FT-IR). The results showed that sodium salts poisoned catalysts led to a decrease in the denitration efficiency. The 3.6% Na2SO4 poisoned catalyst was the most severely deactivated with denitration efficiency of only 50.97% at 350 °C. The introduction of SO42− and S2O72− created new Brønsted acid sites, which facilitated the adsorption of NH3 and NO reduction. The sodium salts poisoned catalysts significantly increased the conversion of SO2–SO3. 3.6%Na2S2O7 poisoned catalyst had the strongest effect on SO2 oxidation and the catalyst achieved a maximum SO2–SO3-conversion of 1.44% at 410 °C. Characterization results showed sodium salts poisoned catalysts consumed the active ingredient and lowered the V4+/V5+ ratio, which suppressed catalytic performance. However, they increased the content of chemically adsorbed oxygen and the strength of V5+=O bonds, which promoted SO2 oxidation.


Author(s):  
Fahim Fayaz ◽  
Ahmad Ziad Sulaiman ◽  
Sharanjit Singh ◽  
Sweeta Akbari

The effect of CO2 partial pressure on ethanol dry reforming was evaluated over 5%Ce-10%Co/Al2O3 catalyst at = PCO2 = 20-50 kPa, PC2H5OH = 20 kPa, reaction temperature of 973 K under atmospheric pressure. The catalyst was prepared by using impregnation method and tested in a fixed-bed reactor. X-ray diffraction measurements studied the formation of Co3O4, spinel CoAl2O4 and CeO2, phases on surface of 5%Ce-10%Co/Al2O3 catalyst. CeO2, CoO and Co3O4 oxides were obtained during temperature–programmed calcination. Ce-promoted 10%Co/Al2O3 catalyst possessed high BET surface area of 137.35 m2 g-1. C2H5OH and CO2 conversions was improved with increasing CO2 partial pressure from 20-50 kPa whilst the optimal selectivity of H2 and CO was achieved at 50 kPa.


2019 ◽  
Vol 19 (2) ◽  
pp. 86-94
Author(s):  
R. G. Moqadam ◽  
A. Tavasoli ◽  
M. Salimi

Manganese and nickel co-modified K/Co/MoS2 catalysts supported on graphene were prepared by incipient wetness impregnation method for application in higher alcohol synthesis (HAS). All catalysts were characterized by X-ray diffraction (XRD), nitrogen adsorptiondesorption, temperature-programmed reduction (TPR) and transmission electron microscopy (TEM). The effect of promoters, as well as supports on higher alcohol synthesis production from syngas, was investigated in a fixed bed reactor. The process was performed with an molar ratio H2 : CO = 1 : 1, operating pressure and temperature of 4 MPa and 330 °C, respectively, and gas hourly space velocity (GHSV) 3.84 m3 (STP)/(kgcat.·h) as reaction conditions (STP – standard temperature and pressure). Results originated from practical works showed that the addition of Ni to the graphene-based catalyst increased HAS production and decreased methanol formation. The total alcohols space-time yield (STY) and alcohol selectivity on Ni/Mn/Co/Mo/K/graphene catalyst reached a maximum at 0.41 galc./(gcat.·h) and 63.51 %, respectively, which is higher than the same composition over alumina supported catalyst.


2017 ◽  
Vol 23 (1) ◽  
pp. 49-56 ◽  
Author(s):  
Yajing Zhang ◽  
Yu Zhang ◽  
Fu Ding ◽  
Kangjun Wang ◽  
Wang Xiaolei ◽  
...  

A series of La2O3-modified CuO-ZnO-ZrO2/HZSM-5 catalysts were prepared by an oxalate co-precipitation method. The catalysts were fully characterized by X-ray diffraction (XRD), N2 adsorption-desorption, hydrogen temperature pro-grammed reduction (H2-TPR), ammonia temperature programmed desorption (NH3-TPD), and X-ray photoelectron spectroscopy (XPS) techniques. The effect of the La2O3 content on the structure and performance of the catalysts was thoroughly investigated. The catalysts were evaluated for the direct synthesis of dimethyl ether (DME) from CO2 hydrogenation. The results displayed that La2O3 addition enhanced catalytic performance, and the maximal CO2 conversion (34.3%) and DME selectivity (57.3%) were obtained over the catalyst with 1% La2O3, which due to the smaller size of Cu species and a larger ratio of Cu+/Cu.


Author(s):  
Haoran Ding ◽  
Yongqing Xu ◽  
Linyi Xiang ◽  
Qiyao Wang ◽  
Cheng Shen ◽  
...  

In order to reduce the hotspots in partial oxidation of methane, CeO2 supported BaCoO3 perogvskite-type oxides were synthesized using a sol-gel method and applied in chemical-looping steam methane reforming (CL-SMR). The synthesized BaCoO3-CeO2 was characterized by X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS). XRD and XPS results suggested that the obtained BaCoO3 was pure crystalline perovskite, its crystalline structure and lattice oxygen could regenerate after calcining. The reactivity of perovskite-type oxides in CL-SMR was evaluated using a fixed-bed reactor. Gas production rates and H2/CO ratios showed that the optimal reaction temperature was about 860 °C and the properly reaction time in fuel reactor was about 180s when Weight Hourly Space Velocity (WHSV) was 23.57 h−1. The syngas production in fuel reactor were 265.11 ml/g, hydrogen production in reforming reactor were 82.53 ml/g. (CSPE)


2018 ◽  
Author(s):  
Riikka Puurunen ◽  
Pauline Voigt ◽  
Eero Haimi ◽  
Jouko Lahtinen ◽  
You Wayne Cheah ◽  
...  

Atomic layer deposition (ALD) is gaining attention as a catalyst preparation method able to produce metal (oxide, sulphide, etc.) nanoparticles of uniform size down to single atoms. This work reports our initial experiments to support nickel on mesoporous zirconia. Nickel (2,2,6,6-tetramethyl-3,5-heptanedionato)2 [Ni(thd)2] was reacted in a fixed-bed ALD reactor with zirconia, characterised with BET surface area of 72 m2/g and mean pore size of 14 nm. According to X-ray fluorescence measurements, the average nickel loading on the top part of the support bed was on the order of 1 wt-%, corresponding to circa one nickel atom per square nanometre. Cross-sectional scanning electron microscopy combined with energy-dispersive spectroscopy confirmed that in the top part of the fixed support bed, nickel was distributed throughout the zirconia particles. X-ray photoelectron spectroscopy indicated the nickel oxidation state to be two. Organic thd ligands remained complete on the surface after the Ni(thd)2 reaction with zirconia, as followed with diffuse reflectance infrared Fourier transform spectroscopy. The ligands could be fully removed by oxidation at 400 °C. These initial results indicate that nickel catalysts on zirconia can likely be made by ALD. Before catalytic testing, in addition to increasing the nickel loading by repeated ALD cycles, optimization of the process parameters is required to ensure uniform distribution of nickel throughout the support bed and within the zirconia particles.


Catalysts ◽  
2019 ◽  
Vol 9 (10) ◽  
pp. 847 ◽  
Author(s):  
Seyed Moeini ◽  
Chiara Battocchio ◽  
Stefano Casciardi ◽  
Igor Luisetto ◽  
Paolo Lupattelli ◽  
...  

In the present study, the catalytic activity of palladium oxide (PdOx) supported on ceria nanorods (CeO2-NR) for aerobic selective oxidation of benzyl alcohol (BnOH) to benzaldehyde (PhCHO) was evaluated. The CeO2-NR was synthesized hydrothermally and the Pd(NO3)2 was deposited by a wet impregnation method, followed by calcination to acquire PdOx/CeO2-NR. The catalysts were characterized by X-ray diffraction (XRD), temperature programmed reduction (TPR), transmission electron microscopy (TEM), Brunauer–Emmet–Teller (BET) surface area analysis, and X-ray photoelectron spectroscopy (XPS). In addition, the TPR-reduced PdOx/CeO2-NR (PdOx/CeO2-NR-Red) was studied by XRD, BET, and XPS. Characterizations showed the formation of CeO2-NR with (111) exposed plane and relatively high BET surface area. PdOx (x > 1) was detected to be the major oxide species on the PdOx/CeO2-NR. The activities of the catalysts in BnOH oxidation were evaluated using air, as an environmentally friendly oxidant, and various solvents. Effects of temperature, solvent nature and palladium oxidation state were investigated. The PdOx/CeO2-NR showed remarkable activity when protic solvents were utilized. The best result was achieved using PdOx/CeO2-NR and boiling ethanol as solvent, leading to 93% BnOH conversion and 96% selectivity toward PhCHO. A mechanistic hypothesis for BnOH oxidation with PdOx/CeO2-NR in ethanol is presented.


Catalysts ◽  
2018 ◽  
Vol 8 (9) ◽  
pp. 380 ◽  
Author(s):  
Pawel Mierczynski ◽  
Agnieszka Mierczynska ◽  
Radoslaw Ciesielski ◽  
Magdalena Mosinska ◽  
Magdalena Nowosielska ◽  
...  

Herein, we report monometallic Ni and bimetallic Pd–Ni catalysts supported on CeO2–Al2O3 binary oxide which are highly active and selective in oxy-steam reforming of methanol (OSRM). Monometallic and bimetallic supported catalysts were prepared by an impregnation method. The physicochemical properties of the catalytic systems were investigated using a range of methods such as: Brunauer–Emmett–Teller (BET), X-ray Powder Diffraction (XRD), Temperature-programmed reduction (TPR–H2), Temperature-programmed desorption (TPD–NH3), X-ray photoelectron spectroscopy (XPS) and Scanning Electron Microscope equipped with an energy dispersive spectrometer (SEM–EDS). We demonstrate that the addition of palladium facilitates the reduction of nickel catalysts. The activity tests performed for all catalysts confirmed the promotion effect of palladium on the catalytic activity of nickel catalyst and their selectivity towards hydrogen production. Both nickel and bimetallic palladium–nickel supported catalysts showed excellent stability during the reaction. The reported catalytic systems are valuable to make advances in the field of fuel cell technology.


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