scholarly journals Evaluation of a Catalyst Durability in Absence and Presence of Toluene Impurity: Case of the Material Co2Ni2Mg2Al2 Mixed Oxide Prepared by Hydrotalcite Route in Methane Dry Reforming to Produce Energy

Materials ◽  
2019 ◽  
Vol 12 (9) ◽  
pp. 1362
Author(s):  
Carole Tanios ◽  
Cédric Gennequin ◽  
Madona Labaki ◽  
Haingomalala Lucette Tidahy ◽  
Antoine Aboukaïs ◽  
...  
Keyword(s):  
Catalytic Activity ◽  
Mixed Oxide ◽  
Active Sites ◽  
Dry Reforming ◽  
Dry Reforming Of Methane ◽  
Side Reactions ◽  
Commercial Catalyst ◽  
Catalytic Sites ◽  
Catalyst Durability ◽  
Catalytic Performances

Ni, Co, Mg, and Al mixed-oxide solids, synthesized via the hydrotalcite route, were investigated in previous works toward the dry reforming of methane for hydrogen production. The oxide Co2Ni2Mg2Al2 calcined at 800 °C, Co2Ni2Mg2Al2800, showed the highest catalytic activity in the studied series, which was ascribable to an interaction between Ni and Co, which is optimal for this Co/Ni ratio. In the present study, Co2Ni2Mg2Al2800 was compared to a commercial catalyst widely used in the industry, Ni(50%)/Al2O3, and showed better activity despite its lower number of active sites, as well as lower amounts of carbon on its surface, i.e. less deactivation. In addition to this, Co2Ni2Mg2Al2800 showed stability for 20 h under stream during the dry reforming of methane. This good durability is attributed to a periodic cycle of carbon deposition and removal as well as to the strong interaction between Ni and Co, preventing the deactivation of the catalyst. The evaluation of the catalytic performances in the presence of toluene, which is an impurity that exists in biogas, is also a part of this work. In the presence of toluene, the catalytic activity of Co2Ni2Mg2Al2800 decreases, and higher carbon formation on the catalyst surface is detected. Toluene adsorption on catalytic sites, side reactions performed by toluene, and the competition between toluene and methane in the reaction with carbon dioxide are the main reasons for such results.

scholarly journals Atomically dispersed nickel as coke-resistant active sites for methane dry reforming

2019 ◽  
Vol 10 (1) ◽  
Author(s):  
Mohcin Akri ◽  
Shu Zhao ◽  
Xiaoyu Li ◽  
Ketao Zang ◽  
Adam F. Lee ◽  
...  
Keyword(s):  
Active Sites ◽  
Large Scale ◽  
Low Cost ◽  
Coke Formation ◽  
Dry Reforming ◽  
Dry Reforming Of Methane ◽  
Highly Active ◽  
Catalytic Sites ◽  
Earth Abundant ◽  
Poor Stability

AbstractDry reforming of methane (DRM) is an attractive route to utilize CO2 as a chemical feedstock with which to convert CH4 into valuable syngas and simultaneously mitigate both greenhouse gases. Ni-based DRM catalysts are promising due to their high activity and low cost, but suffer from poor stability due to coke formation which has hindered their commercialization. Herein, we report that atomically dispersed Ni single atoms, stabilized by interaction with Ce-doped hydroxyapatite, are highly active and coke-resistant catalytic sites for DRM. Experimental and computational studies reveal that isolated Ni atoms are intrinsically coke-resistant due to their unique ability to only activate the first C-H bond in CH4, thus avoiding methane deep decomposition into carbon. This discovery offers new opportunities to develop large-scale DRM processes using earth abundant catalysts.

scholarly journals Performance Analysis of TiO2-Modified Co/MgAl2O4 Catalyst for Dry Reforming of Methane in a Fixed Bed Reactor for Syngas (H2, CO) Production

Energies ◽  
2021 ◽  
Vol 14 (11) ◽  
pp. 3347
Author(s):  
Arslan Mazhar ◽  
Asif Hussain Khoja ◽  
Abul Kalam Azad ◽  
Faisal Mushtaq ◽  
Salman Raza Naqvi ◽  
...  
Keyword(s):  
Catalytic Activity ◽  
Fixed Bed ◽  
Catalytic Performance ◽  
Dry Reforming ◽  
Fixed Bed Reactor ◽  
Dry Reforming Of Methane ◽  
Catalyst Stability ◽  
Feed Ratio ◽  
Catalyst Loading ◽  
Impregnation Method

Co/TiO2–MgAl2O4 was investigated in a fixed bed reactor for the dry reforming of methane (DRM) process. Co/TiO2–MgAl2O4 was prepared by modified co-precipitation, followed by the hydrothermal method. The active metal Co was loaded via the wetness impregnation method. The prepared catalyst was characterized by XRD, SEM, TGA, and FTIR. The performance of Co/TiO2–MgAl2O4 for the DRM process was investigated in a reactor with a temperature of 750 °C, a feed ratio (CO2/CH4) of 1, a catalyst loading of 0.5 g, and a feed flow rate of 20 mL min−1. The effect of support interaction with metal and the composite were studied for catalytic activity, the composite showing significantly improved results. Moreover, among the tested Co loadings, 5 wt% Co over the TiO2–MgAl2O4 composite shows the best catalytic performance. The 5%Co/TiO2–MgAl2O4 improved the CH4 and CO2 conversion by up to 70% and 80%, respectively, while the selectivity of H2 and CO improved to 43% and 46.5%, respectively. The achieved H2/CO ratio of 0.9 was due to the excess amount of CO produced because of the higher conversion rate of CO2 and the surface carbon reaction with oxygen species. Furthermore, in a time on stream (TOS) test, the catalyst exhibited 75 h of stability with significant catalytic activity. Catalyst potential lies in catalyst stability and performance results, thus encouraging the further investigation and use of the catalyst for the long-run DRM process.

Kinetic Assessment of the Dry Reforming of Methane over a Solid Solution Ni–La Oxide Catalyst

2021 ◽  
Author(s):  
Victor Stivenson Sandoval-Bohorquez ◽  
Edgar M. Morales-Valencia ◽  
Carlos Omar Castillo-Araiza ◽  
Luz Marina Ballesteros Rueda ◽  
Víctor Gabriel Baldovino Medrano
Keyword(s):  
Solid Solution ◽  
Active Sites ◽  
Oxide Catalyst ◽  
Bond Cleavage ◽  
Scale Up ◽  
Active Surface ◽  
Dry Reforming ◽  
Dry Reforming Of Methane ◽  
Nickel Surface ◽  
Kinetics Of

The dry reforming of methane is a promising technology for the abatement of CH<sub>4</sub> and CO<sub>2</sub>. Solid solution Ni–La oxide catalysts are characterized by their long–term stability (100h) when tested at full conversion. The kinetics of dry reforming over this type of catalysts has been studied using both power law and Langmuir–Hinshelwood based approaches. However, these studies typically deal with fitting the net CH<sub>4</sub> rate hence disregarding competing and parallel surface processes and the different possible configurations of the active surface. In this work, we synthesized a solid solution Ni–La oxide catalyst and tested six Langmuir–Hinshelwood mechanisms considering both single and dual active sites for assessing the kinetics of dry reforming and the competing reverse water gas shift reaction and investigated the performance of the derived kinetic models. In doing this, it was found that: (1) all the net rates were better fitted by a single–site model that considered that the first C–H bond cleavage in methane occurred over a <a>metal−oxygen </a>pair site; (2) this model predicted the existence of a nearly saturated nickel surface with chemisorbed oxygen adatoms derived from the dissociation of CO<sub>2</sub>; (3) the dissociation of CO<sub>2</sub> can either be an inhibitory or an irrelevant step, and it can also modify the apparent activation energy for CH<sub>4</sub> activation. These findings contribute to a better understanding of the dry reforming reaction's kinetics and provide a robust kinetic model for the design and scale–up of the process.

scholarly journals Ce- and Y-Modified Double-Layered Hydroxides as Catalysts for Dry Reforming of Methane: On the Effect of Yttrium Promotion

Catalysts ◽  
2019 ◽  
Vol 9 (1) ◽  
pp. 56 ◽  
Author(s):  
Katarzyna Świrk ◽  
Magnus Rønning ◽  
Monika Motak ◽  
Patricia Beaunier ◽  
Patrick Da Costa ◽  
...  
Keyword(s):  
Textural Properties ◽  
Dry Reforming ◽  
Dry Reforming Of Methane ◽  
Side Reactions ◽  
X Ray Diffraction ◽  
X Ray ◽  
Transmission Electron ◽  
Temperature Programmed ◽  
Nickel Species

Ce- and Y-promoted double-layered hydroxides were synthesized and tested in dry reforming of methane (CH4/CO2 = 1/1). The characterization of the catalysts was performed using X-ray fluorescence (XRF), X-ray diffraction (XRD), N2 sorption, temperature-programmed reduction in H2 (TPR-H2), temperature-programmed desorption of CO2 (TPD-CO2), H2 chemisorption, thermogravimetric analysis coupled by mass spectrometry (TGA/MS), Raman, and high-resolution transmission electron microscopy (HRTEM). The promotion with cerium influences textural properties, improves the Ni dispersion, decreases the number of total basic sites, and increases the reduction temperature of nickel species. After promotion with yttrium, the increase in basicity is not directly correlated with the increasing Y loading on the contrary of Ni dispersion. Dry reforming of methane (DRM) was performed as a function of temperature and in isothermal conditions at 700 °C for 5 h. For catalytic tests, a slight increase of the activity is observed for both Y and Ce doped catalysts. This improvement can of course be explained by Ni dispersion, which was found higher for both Y and Ce promoted catalysts. During DRM, the H2/CO ratio was found below unity, which can be explained by side reactions occurrence. These side reactions are linked with the increase of CO2 conversion and led to carbon deposition. By HRTEM, only multi-walled and helical-shaped carbon nanotubes were identified on Y and Ce promoted catalysts. Finally, from Raman spectroscopy, it was found that on Y and Ce promoted catalysts, the formed C is less graphitic as compared to only Ce-based catalyst.

Combined partial oxidation and dry reforming of methane to synthesis gas over noble metals supported on Mg–Al mixed oxide

2004 ◽  
Vol 275 (1-2) ◽  
pp. 149-155 ◽  
Author(s):  
Andrey I. Tsyganok ◽  
Mieko Inaba ◽  
Tatsuo Tsunoda ◽  
Kunio Suzuki ◽  
Katsuomi Takehira ◽  
...  
Keyword(s):  
Partial Oxidation ◽  
Synthesis Gas ◽  
Mixed Oxide ◽  
Noble Metals ◽  
Dry Reforming ◽  
Dry Reforming Of Methane

Influence of method of preparation on the activity of La–Ni–Ce mixed oxide catalysts for dry reforming of methane

RSC Advances ◽  
2014 ◽  
Vol 4 (91) ◽  
pp. 50226-50232 ◽  
Author(s):  
T. V. Sagar ◽  
N. Sreelatha ◽  
G. Hanmant ◽  
M. Surendar ◽  
N. Lingaiah ◽  
...  
Keyword(s):  
Mixed Oxide ◽  
Dry Reforming ◽  
Oxide Catalysts ◽  
Dry Reforming Of Methane ◽  
Mixed Oxide Catalysts

scholarly journals A Short Review on the Catalytic Activity of Hydrotalcite-Derived Materials for Dry Reforming of Methane

Catalysts ◽  
2017 ◽  
Vol 7 (12) ◽  
pp. 32 ◽  
Author(s):  
Radosław Dębek ◽  
Monika Motak ◽  
Teresa Grzybek ◽  
Maria Galvez ◽  
Patrick Da Costa
Keyword(s):  
Catalytic Activity ◽  
Short Review ◽  
Dry Reforming ◽  
Dry Reforming Of Methane
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