scholarly journals One-Pot Synthesis of Ni0.05Ce0.95O2−δ Catalysts with Nanocubes and Nanorods Morphology for CO2 Methanation Reaction and in Operando DRIFT Analysis of Intermediate Species

Processes ◽  
2021 ◽  
Vol 9 (11) ◽  
pp. 1899
Author(s):  
Igor Luisetto ◽  
Stefano Stendardo ◽  
Sakkarapalayam Murugesan Senthil Kumar ◽  
Karuppiah Selvakumar ◽  
Jagadesh Kopula Kesavan ◽  
...  
Keyword(s):  
Reaction Pathway ◽  
Renewable Energy Sources ◽  
Main Reaction ◽  
One Pot ◽  
Co2 Methanation ◽  
Methanation Reaction ◽  
Drift Analysis ◽  
In Operando ◽  
Direct Hydrogenation ◽  
Diffuse Reflectance Infrared

The valorization of CO2 via renewable energy sources allows one to obtain carbon-neutral fuels through its hydrogenation, like methane. In this study, Ni0.05Ce0.95O2−δ catalysts were prepared using a simple one-pot hydrothermal method yielding nanorod and nanocube particles to be used for the methanation reaction. Samples were characterized by XRD, BET, TEM, H2-TPR, and H2-TPD experiments. The catalytic activity tests revealed that the best performing catalyst was Ni0.05Ce0.95O2−δ, with nanorod morphology, which gave a CO2 conversion of 40% with a selectivity of CH4 as high as 93%, operating at 325 °C and a GHSV of 240,000 cm3 h−1 g−1. However, the lower activation energy was found for Ni0.05Ce0.95O2−δ catalysts with nanocube morphology. Furthermore, an in operando diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) analysis was performed flowing CO2:H2 or CO:H2 mixture, showing that the main reaction pathway, for the CO2 methanation, is the direct hydrogenation of formate intermediate.

scholarly journals Comparative analysis of carbon dioxide methanation technologies for low carbon society development

2020 ◽  
Author(s):  
Gheorghe Lazaroiu ◽  
Dana-Alexandra Ciupageanu ◽  
Lucian Mihaescu ◽  
Rodica-Manuela Grigoriu
Keyword(s):  
Carbon Dioxide ◽  
Conversion Rate ◽  
Renewable Energy Sources ◽  
Clean Energy ◽  
Detailed Comparison ◽  
Co2 Conversion ◽  
Low Carbon ◽  
Co2 Methanation ◽  
Synthetic Natural Gas ◽  
Methanation Reaction

Conversion technologies able to transform renewable energy sources (RES) based electricity in gaseous fuels, which can be stored over long timeframes, represent a key focus point considering the low carbon society development. Thus, Power-to-Gas technologies emerge as a viable solution to mitigate the variability of RES power generation, enabling spatial and temporal balancing of production vs. demand mismatches. An additional benefit in this context is brought by the decarbonization facilities, employing polluting carbon dioxide (CO2) emissions and RES-based electricity to produce synthetic natural gas with high methane (CH4) concentration. The fuel obtained can be stored or injected in the gas distribution infrastructure, becoming a clean energy vector. This paper investigates the functional parameters of such technologies, aiming to comparatively analyze their suitability for further integration in hybrid and ecofriendly energy systems. Given the stability of CO2 molecule, a catalyst must be used to overcome the methanation reaction kinetics limitations. Therefore, the required conditions (in terms of pressure and temperature) for CO2 methanation reaction unfolding are analyzed first. Further, CO2 conversion rate and CH4 selectivity are investigated in order to provide a detailed comparison of available technologies in the field, addressing moreover the particularities of catalyst preparation processes. It is found that Nickel (Ni) based catalysts are performing well, achieving good performances even at atmospheric pressure and low temperatures. It is remarkable that, within a [300,500]℃ temperature range, Ni-based catalysts enable a CO2 conversion rate over 78% with a CH4 selectivity of up to 100%. Last, integration perspectives and benefits are discussed, highlighting the crucial importance of the results presented in this paper.

Study of the role of chemical support and structured carrier on the CO2 methanation reaction

2019 ◽  
Vol 377 ◽  
pp. 120461 ◽  
Author(s):  
Antonio Ricca ◽  
Livia Truda ◽  
Vincenzo Palma
Keyword(s):  
Co2 Methanation ◽  
Methanation Reaction

Synthesis of novel N-functionalized 4-aryl-tetrahydrobiquinoline-2,5-(1H,3H)-diones via one-pot three-component reaction: a joint experimental and computational study

2018 ◽  
Vol 96 (12) ◽  
pp. 1071-1078
Author(s):  
Vahideh Zadsirjan ◽  
Sayyed Jalil Mahdizadeh ◽  
Majid M. Heravi ◽  
Masumeh Heydari
Keyword(s):  
Density Functional Theory ◽  
Density Functional ◽  
Computational Study ◽  
Reaction Pathway ◽  
Deep Insight ◽  
One Pot ◽  
Functional Theory ◽  
Three Component Reaction ◽  
High Yields ◽  
Mechanism Of The Reaction

A novel series of N-functionalized 4-aryl-tetrahydrobiquinoline-2,5-(1H,3H)-diones were synthesized in high yields by a one-pot three-component reaction involving 2-chloroquinoline-3-carbaldehydes, Meldrum’s acid, and enaminones (dimedone-based enaminones) in the presence of K2CO3 in CH3CN under reflux condition. To gain a deep insight on the mechanism of the reaction, an extensive series of quantum mechanics calculations in the framework of density functional theory (DFT) were carried out for supporting the suggested reaction pathway.

Elucidating the mechanism of the CO2 methanation reaction over Ni–Fe hydrotalcite-derived catalysts via surface-sensitive in situ XPS and NEXAFS

2020 ◽  
Vol 22 (34) ◽  
pp. 18788-18797 ◽  
Author(s):  
Gianfranco Giorgianni ◽  
Chalachew Mebrahtu ◽  
Manfred Erwin Schuster ◽  
Alexander Ian Large ◽  
Georg Held ◽  
...  
Keyword(s):  
Co2 Methanation ◽  
Promotion Effect ◽  
Methanation Reaction ◽  
In Situ Xps

In situ surface sensitive XPS and NEXAFS clarify the promotion effect of Fe in Ni–Fe/hydrotalcite-derived catalysts for the CO2 methanation reaction.

scholarly journals CO2 Methanation over Rh/CeO2 Studied with Infrared Modulation Excitation Spectroscopy and Phase Sensitive Detection

Catalysts ◽  
2020 ◽  
Vol 10 (6) ◽  
pp. 601
Author(s):  
Felix Hemmingsson ◽  
Andreas Schaefer ◽  
Magnus Skoglundh ◽  
Per-Anders Carlsson
Keyword(s):  
Reaction Pathway ◽  
Sensitive Detection ◽  
Side Reactions ◽  
Co2 Methanation ◽  
Individual Contributions ◽  
Phase Sensitive ◽  
Phase Sensitive Detection ◽  
Modulation Excitation Spectroscopy ◽  
Modulation Excitation

Methane is a well-established fuel molecule whose production from CO 2 through methanation garners increasing interest as an energy storage solution. While often produced with Ni based catalysts, other metals are of interest thanks to higher robustness and activity-selectivity numbers. The Rh/CeO 2 catalyst has shown appreciable properties for CO 2 methanation and its structural dynamics has been studied in situ. However, the reaction pathway is unknown. Here, we present infrared modulation excitation spectroscopy measurements with phase sensitive detection of a Rh/CeO 2 catalyst adsorbate composition during H 2 pulsing (0–2 vol.%) to a constant CO 2 (0.5 vol.%) feed. Various carbonyl (CO) and carbonate (b-CO 3 /p-CO 3 ) ad-species clearly respond to the hydrogen stimulus, making them potential reaction intermediates. The different CO ad-species are likely intermediates for product CO and CH 4 but their individual contributions to the respective formations are not unambiguously ascertained. As for the carbonate dynamics, it might be linked to the reduction/oxidation of the CeO 2 surface upon H 2 pulsing. Formate (HCOO) ad-species are clearly visible but appear to be, if not spectators, linked to slow side reactions possibly also affected by CeO 2 redox processes.

Enhanced low-temperature activity for CO2 methanation over Ru doped the Ni/CexZr(1−)O2 catalysts prepared by one-pot hydrolysis method

2018 ◽  
Vol 43 (14) ◽  
pp. 7179-7189 ◽  
Author(s):  
Xingfu Shang ◽  
Digu Deng ◽  
Xueguang Wang ◽  
Weidong Xuan ◽  
Xiujing Zou ◽  
...  
Keyword(s):  
Low Temperature ◽  
One Pot ◽  
Co2 Methanation ◽  
Hydrolysis Method

scholarly journals UV-Catalyzed Persulfate Oxidation of an Anthraquinone Based Dye

Catalysts ◽  
2020 ◽  
Vol 10 (4) ◽  
pp. 456 ◽  
Author(s):  
Kamil Krawczyk ◽  
Stanisław Wacławek ◽  
Edyta Kudlek ◽  
Daniele Silvestri ◽  
Tomasz Kukulski ◽  
...  
Keyword(s):  
Textile Industry ◽  
Membrane Filtration ◽  
Lemna Minor ◽  
Reaction Pathway ◽  
Main Reaction ◽  
Synthetic Dyes ◽  
Quantum Chemical Analysis ◽  
Substantial Impact ◽  
Anthraquinone Dye ◽  
Persulfate Oxidation

Wastewater from the textile industry has a substantial impact on water quality. Synthetic dyes used in the textile production process are often discharged into water bodies as residues. Highly colored wastewater causes various of problems for the aquatic environment such as: reducing light penetration, inhibiting photosynthesis and being toxic to certain organisms. Since most dyes are resistant to biodegradation and are not completely removed by conventional methods (adsorption, coagulation-flocculation, activated sludge, membrane filtration) they persist in the environment. Advanced oxidation processes (AOPs) based on hydrogen peroxide (H2O2) have been proven to decolorize only some of the dyes from wastewater by photocatalysis. In this article, we compared two very different photocatalytic systems (UV/peroxydisulfate and UV/H2O2). Photocatalyzed activation of peroxydisulfate (PDS) generated sulfate radicals (SO4•−), which reacted with the selected anthraquinone dye of concern, Acid Blue 129 (AB129). Various conditions, such as pH and concentration of PDS were applied, in order to obtain an effective decolorization effect, which was significantly better than in the case of hydroxyl radicals. The kinetics of the reaction followed a pseudo-first order model. The main reaction pathway was also proposed based on quantum chemical analysis. Moreover, the toxicity of the solution after treatment was evaluated using Daphnia magna and Lemna minor, and was found to be significantly lower compared to the toxicity of the initial dye.

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