scholarly journals Methanation of CO2 Using MIL-53-Based Catalysts: Ni/MIL-53–Al2O3 versus Ni/MIL-53

Catalysts ◽  
2021 ◽  
Vol 11 (11) ◽  
pp. 1412
Author(s):  
Oana Grad ◽  
Gabriela Blanita ◽  
Mihaela D. Lazar ◽  
Maria Mihet
Keyword(s):  
Prolonged Exposure ◽  
Reaction Medium ◽  
Catalytic Performance ◽  
The Novel ◽  
Co2 Conversion ◽  
Co2 Methanation ◽  
Nanoparticle Deposition ◽  
Metallic Particles ◽  
Al2o3 Composite ◽  
Methane Selectivity

MIL-53 and the MIL-53–Al2O3 composite synthesized by a solvothermal procedure, with water as the only solvent besides CrCl3 and benzene-1,4-dicarboxylic acid (BDC), were used as catalytic supports to obtain the novel MIL-53-based catalysts Ni(10 wt.%)/MIL-53 and Ni(10 wt.%)/MIL-53–Al2O3. Ni nanoparticle deposition by an adapted double-solvent method leads to the uniform distribution of metallic particles, both smaller (≤10 nm) and larger ones (10–30 nm). MIL-53–Al2O3 and Ni/MIL-53–Al2O3 show superior thermal stability to MIL-53 and Ni/MIL-53, while MIL-53–Al2O3 samples combine the features of both MIL-53 and alumina in terms of porosity. The investigation of temperature’s effect on the catalytic performance in the methanation process (CO2:H2 = 1:5.2, GHSV = 4650 h−1) revealed that Ni/MIL-53 is more active at temperatures below 300 °C, and Ni/MIL-53–Al2O3 above 300 °C. Both catalysts show maximum CO2 conversion at 350 °C: 75.5% for Ni/MIL-53 (methane selectivity of 93%) and 88.8% for Ni/MIL-53–Al2O3 (methane selectivity of 98%). Stability tests performed at 280 °C prove that Ni/MIL-53–Al2O3 is a possible candidate for the CO2 methanation process due to its high CO2 conversion and CH4 selectivity, corroborated by the preservation of the structure and crystallinity of MIL-53 after prolonged exposure in the reaction medium.

scholarly journals Effect of Support and Chelating Ligand on the Synthesis of Ni Catalysts with High Activity and Stability for CO2 Methanation

Catalysts ◽  
2020 ◽  
Vol 10 (5) ◽  
pp. 493 ◽  
Author(s):  
Vetrivel Shanmugam ◽  
Stefan Neuberg ◽  
Ralf Zapf ◽  
Helmut Pennemann ◽  
Gunther Kolb
Keyword(s):  
Catalytic Performance ◽  
Impregnation Method ◽  
Chelating Ligands ◽  
Co2 Conversion ◽  
Ni Catalysts ◽  
Co2 Methanation ◽  
High Co2 ◽  
X Ray ◽  
Metal Support Interaction ◽  
Methane Selectivity

Carbon dioxide methanation was carried out over Ni-based catalysts on different supports and chelating ligands in microreactors. To investigate the influence of chelating ligands and supports, the Ni catalysts were prepared using different support such as CeO2, Al2O3, SiO2, and SBA-15 by a citric acid (CA)-assisted impregnation method. The properties of the developed catalysts were studied by X-ray diffraction (XRD), Transmission electron microscope (TEM), and X-ray photoelectron spectroscopy (XPS) measurement, and the results show that the addition of CA in the impregnation solution improved the dispersion, refines the particle size, and enhanced the interaction of nickel species. The catalytic performance of the developed Ni catalysts were evaluated by CO2 methanation in microreactors in the temperature range of 275 °C–375 °C under 12.5 bar pressure. All the catalysts exhibit high CO2 conversion and extremely high selectivity to methane. However, the catalysts prepared via CA-assisted method exhibited excellent activity and stability, compared with Ni catalysts prepared by a conventional impregnation method, which could be attributed to highly dispersed nickel particles with strong metal–support interaction. The activity of CO2 methanation followed the order of Ni/CeO2-CA > Ni/SBA-15-CA > Ni/Al2O3-CA > Ni/SiO2-CA > Ni/CeO2. The Ni/CeO2 catalysts have also been prepared using different chelating ligands such as ethylene glycol (EG), sucrose (S), oxalic acid (OA) and ethylene diamine tetra acidic acid (EDTA). Among the tested catalysts prepared with different support and chelating ligands, the Ni/CeO2 catalyst prepared via CA-assisted method gave superior catalytic performance and it could attain 98.6% of CO2 conversion and 99.7% methane selectivity at 325 °C. The partial reduction of the CeO2 support generates more surface oxygen vacancies and results in a high CO2 conversion and methane selectivity compared with other catalysts. The addition of CA as promoter favored the synergistic effect of Ni and support, which led to high dispersion, controls the size, and stabilizes the Ni nanoparticles. Furthermore, the Ni/CeO2-CA catalyst yields high CO2 conversion in a time-on-stream study due to the ability of preventing the carbon deposition and sintering of Ni particles under the applied reaction conditions. However, the Ni/Al2O3-CA and Ni/SBA-15-CA catalysts showed stable performance for 100 h of time on stream.

scholarly journals Enhanced CO2 Methanation Reaction in C1 Chemistry over a Highly Dispersed Nickel Nanocatalyst Prepared Using the One-Step Melt-Infiltration Method

Catalysts ◽  
2020 ◽  
Vol 10 (6) ◽  
pp. 643 ◽  
Author(s):  
Eui Hyun Cho ◽  
Woohyun Kim ◽  
Chang Hyun Ko ◽  
Wang Lai Yoon
Keyword(s):  
Catalytic Performance ◽  
High Dispersion ◽  
Co2 Conversion ◽  
Co2 Methanation ◽  
Gas Treatment ◽  
Ni Content ◽  
Melt Infiltration ◽  
One Step ◽  
The One ◽  
Infiltration Method

The Paris Agreement requires the world to put the best efforts to reduce CO2 emissions, due to the global warming problems. As a promising technology corresponding to this greenhouse gas treatment, the CO2 methanation process a.k.a power to gas (PtoG), which catalytically converts CO2 into methane, has been in the limelight. To develop an efficient catalytic process, it is necessary to design a low-cost and high-efficiency catalyst for high CO2 conversion and CH4 selectivity. In this study, we have developed Ni/γ-Al2O3 catalysts by the one-step melt-infiltration method, where both aging and calcination are done in one pot. For enhancement of the catalytic activity and selectivity, sufficient Ni content (>25 wt %) and a high dispersion (<10 nm) are simultaneously required. Thus, the aging conditions of the melt-infiltration methods, e.g., time and temperature, were optimized for the high dispersion with sufficient Ni content (15–50 wt %). The catalytic performance tests were carried out under atmospheric pressure, 275 to 400 °C and gas hourly velocity (GHSV) = 25,000 h−1. And the various characteristic analyses (Brunauer–Emmett–Teller (BET), X-ray diffraction (XRD), H2-chemisorption, temperature programmed reduction (TPR), etc.) were performed to confirm the effects on the catalytic performance. As a result, based on the experiments and the characterization data, the 30 wt %-Ni catalyst (Ni particles size = 11 nm) showed the best CO2 conversion at 300 °C and the 20 wt % one having the highest Ni dispersion (Ni particles size = 8.8 nm), which showed the best intrinsic reaction rate and CH4 selectivity in the entire temperature range.

scholarly journals CO2 Methanation over Hydrotalcite-Derived Nickel/Ruthenium and Supported Ruthenium Catalysts

Catalysts ◽  
2019 ◽  
Vol 9 (12) ◽  
pp. 1008 ◽  
Author(s):  
Joana A. Martins ◽  
A. Catarina Faria ◽  
Miguel A. Soria ◽  
Carlos V. Miguel ◽  
Alírio E. Rodrigues ◽  
...  
Keyword(s):  
Inductively Coupled Plasma ◽  
Optical Emission ◽  
Space Velocity ◽  
Catalytic Performance ◽  
Ruthenium Catalysts ◽  
Emission Spectrometry ◽  
Co2 Conversion ◽  
Co2 Methanation ◽  
Inductively Coupled ◽  
Weight Hourly Space Velocity

In this work, in-house synthesized NiMgAl, Ru/NiMgAl, and Ru/SiO2 catalysts and a commercial ruthenium-containing material (Ru/Al2O3com.) were tested for CO2 methanation at 250, 300, and 350 °C (weight hourly space velocity, WHSV, of 2400 mLN,CO2·g−1·h−1). Materials were compared in terms of CO2 conversion and CH4 selectivity. Still, their performances were assessed in a short stability test (24 h) performed at 350 °C. All catalysts were characterized by temperature programmed reduction (TPR), X-ray diffraction (XRD), N2 physisorption at −196 °C, inductively coupled plasma optical emission spectrometry (ICP-OES), and H2/CO chemisorption. The catalysts with the best performance (i.e., the hydrotalcite-derived NiMgAl and Ru/NiMgAl) seem to be quite promising, even when compared with other methanation catalysts reported in the literature. Extended stability experiments (240 h of time-on-stream) were performed only over NiMgAl, which was selected based on catalytic performance and estimated price criteria. This catalyst showed some deactivation under conditions that favor CO formation (high temperature and high WHSV, i.e., 350 °C and 24,000 mLN,CO2·g−1·h−1, respectively), but at 300 °C and low WHSV, excellent activity (ca. 90% of CO2 conversion) and stability, with nearly complete selectivity towards methane, were obtained.

scholarly journals Low Temperature Methanation of CO2 on High Ni Content Ni-Ce-ZrOδ Catalysts Prepared via One-Pot Hydrothermal Synthesis

Catalysts ◽  
2019 ◽  
Vol 10 (1) ◽  
pp. 32 ◽  
Author(s):  
Vissanu Meeyoo ◽  
Noppadol Panchan ◽  
Nat Phongprueksathat ◽  
Atsadang Traitangwong ◽  
Xinpeng Guo ◽  
...  
Keyword(s):  
Hydrothermal Synthesis ◽  
Low Temperature ◽  
High Surface ◽  
Oxygen Species ◽  
Co2 Conversion ◽  
One Pot ◽  
Co2 Methanation ◽  
Surface Areas ◽  
Ni Content ◽  
Methane Selectivity

Ni-Ce-Zr-Oδ catalysts were prepared via one-pot hydrothermal synthesis. It was found that Ni can be partially incorporated into the Ce-Zr lattice, increasing surface oxygen species. The catalysts possess high surface areas even at high Ni loadings. The catalyst with Ni content of 71.5 wt.% is able to activate CO2 methanation even at a low temperature (200 °C). Its CO2 conversion and methane selectivity were reported at 80% and 100%, respectively. The catalyst was stable for 48 h during the course of CO2 methanation at 300 °C. Catalysts with the addition of medium basic sites were found to have better catalytic activity for CO2 methanation.

scholarly journals CO2 Methanation Using Multimodal Ni/SiO2 Catalysts: Effect of Support Modification by MgO, CeO2, and La2O3

Catalysts ◽  
2021 ◽  
Vol 11 (4) ◽  
pp. 443
Author(s):  
Maria Mihet ◽  
Monica Dan ◽  
Lucian Barbu-Tudoran ◽  
Mihaela D. Lazar
Keyword(s):  
Pore Structure ◽  
Silica Matrix ◽  
Co2 Conversion ◽  
Target Concentration ◽  
Co2 Methanation ◽  
Temperature Programmed ◽  
Carbon Dioxide Co2 ◽  
Methane Selectivity ◽  
Effect Of Support ◽  
Adsorption Desorption

Ni/oxide-SiO2 (oxide: MgO, CeO2, La2O3, 10 wt.% target concentration) catalyst samples were prepared by successive impregnation of silica matrix, first with supplementary oxide, and then with Ni (10 wt.% target concentration). The silica matrix with multimodal pore structure was prepared by solvothermal method. The catalyst samples were structurally characterized by N2 adsorption-desorption, XRD, SEM/TEM, and functionally evaluated by temperature programmed reduction (TPR), and temperature programmed desorption of hydrogen (H2-TPD), or carbon dioxide (CO2-TPD). The addition of MgO and La2O3 leads to a better dispersion of Ni on the catalytic surface. Ni/LaSi and Ni/CeSi present a higher proportion of moderate strength basic sites for CO2 activation compared to Ni/Si, while Ni/MgSi lower. CO2 methanation was performed in the temperature range of 150–350 °C and at atmospheric pressure, all silica supported Ni catalysts showing good CO2 conversion and CH4 selectivity. The best catalytic activity was obtained for Ni/LaSi: CO2 conversion of 83% and methane selectivity of 98%, at temperatures as low as 250 °C. The used catalysts preserved the multimodal pore structure with approximately the same pore size for the low and medium mesopores. Except for Ni/CeSi, no particle sintering occurs, and no carbon deposition was observed for any of the tested catalysts.

scholarly journals Synthesis of the Novel Ligand Tris-(3,4-dimethoxylphenyl) phosphine and Its Catalytic Performance in 1-Dodecene Hydroformylation

2010 ◽  
Vol 31 (9-10) ◽  
pp. 1093-1097 ◽  
Author(s):  
Maolin YUAN ◽  
Haiyan FU ◽  
Ruixiang LI ◽  
Hua CHEN ◽  
Xianjun LI
Keyword(s):  
Catalytic Performance ◽  
The Novel

Influence of pretreatment temperature on catalytic performance of rutile TiO2-supported ruthenium catalyst in CO2 methanation

2016 ◽  
Vol 333 ◽  
pp. 227-237 ◽  
Author(s):  
Jinghua Xu ◽  
Xiong Su ◽  
Hongmin Duan ◽  
Baolin Hou ◽  
Qingquan Lin ◽  
...  
Keyword(s):  
Catalytic Performance ◽  
Ruthenium Catalyst ◽  
Co2 Methanation ◽  
Rutile Tio2 ◽  
Pretreatment Temperature

Catalytic performance for CO2 conversion to methanol of gallium-promoted copper-based catalysts: influence of metallic precursors

2001 ◽  
Vol 34 (4) ◽  
pp. 255-266 ◽  
Author(s):  
Jamil Toyir ◽  
Pilar Ramı́rez de la Piscina ◽  
José Luis G Fierro ◽  
Narcı́s Homs
Keyword(s):  
Catalytic Performance ◽  
Co2 Conversion

Pt/UiO-66 Nanocomposites as Catalysts for CO2 Methanation Process

2019 ◽  
Vol 19 (6) ◽  
pp. 3187-3196 ◽  
Author(s):  
Maria Mihet ◽  
Gabriela Blanita ◽  
Monica Dan ◽  
Lucian Barbu-Tudoran ◽  
Mihaela D Lazar
Keyword(s):  
Thermal Stability ◽  
Surface Area ◽  
Metal Organic Framework ◽  
Catalytic Performance ◽  
Molar Ratio ◽  
High Dispersion ◽  
Co2 Methanation ◽  
Preparation Methods ◽  
Good Thermal Stability ◽  
Catalytic Support

Pt/UiO-66 nanocomposites with platinum target concentration of 3 wt.% were prepared by 3 preparation methods, characterized and tested in the CO2 methanation process. Choice of the microporous UiO-66 metal-organic framework (Zr6O4(OH)4 with 1,4-benzene-dicarboxylate ligand) as catalytic support was motivated by the CO2 chemisorption capacity (proven by CO2-TPD profiles), large specific surface area (1477 m2/g) which favors a high dispersion of metal nanoparticles and good thermal stability. The preparation methods for the Pt/UiO-66 nanocomposites are: (1) wetimpregnation followed by reduction in H2 at 200 °C for 2 h; (2) wet-impregnation followed by reduction with an aqueous solution of NaBH4; and (3) “double-solvent” method, followed by reduction with NaBH4. The UiO-66 based nanocomposites were characterized by N2 adsorption–desorption (BET method), XRD, and SEM/TEM. The Pt/UiO-66 catalyst prepared by method 3 was chosen for catalytic testing due to its highest surface area, smallest platinum nanoparticles (PtNPs) size, the localization of PtNPs both on the grain’s internal and external surface and best thermal stability in the desired temperature range. Its capacity to adsorb and activate CO2 and H2 was evaluated in thermo-programmed desorption experiments (H2-TPD and CO2-TPD). Hydrogen is molecularly adsorbed, while CO2 is adsorbed both molecularly and dissociatively. The catalytic performance in the CO2 methanation process was evaluated by Temperature Programmed Reactions (TPRea, 2 °C/min, 30–350 °C), at atmospheric pressure. The best results were obtained at 350 °C, CO2:H2 molar ratio of 1:5.2 and GHSV ═ 1650 h−1. In these conditions CO2 conversion is almost 50% and CH4 selectivity is 36%, the rest of the converted CO2 being transformed in CO.

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