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Catalytic CO2 Methanation Reactors and Processes
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Catalytic CO2 Methanation Reactors and Processes

A special issue of Catalysts (ISSN 2073-4344). This special issue belongs to the section "Catalytic Reaction Engineering".

Deadline for manuscript submissions: closed (20 December 2022) | Viewed by 24064

Special Issue Editors

Dr. Son Ich Ngo

E-Mail Website
Guest Editor
Center of Sustainable Process Engineering (CoSPE), Department of Chemical Engineering, Hankyong National University, Gyeonggi-do, Anseong-si 17579, Jungang-ro 327, Republic of Korea
Interests: multiphase flows; chemical engineering; computational fluid dynamics; multiscale modeling; high-performance computing; machine learning in CFD
Special Issues, Collections and Topics in MDPI journals
Prof. Dr. Enrique García-Bordejé

E-Mail Website
Guest Editor
CSIC, Inst Carboquim ICB, Miguel Luesma Castan 4, E-50018 Zaragoza, Spain
Interests: CO2 methanation; carbon nanotubes; carbon nanofibers; grapheme; structured catalytic reactos

Special Issue Information

Dear Colleagues,

CO2 methanation plays an important role in balancing the time-variant supply and demand of electrical energy from intermittent nature renewable sources such as wind and solar.

Methane is easier to store and transport than electrical energy and has a good storage capacity combined with high charge/discharge periods. The excess energy from renewable sources can be converted to methane via catalytic CO2 methanation reactors. Commercial and environmental benefits have made CO2 methanation one of the most important research projects all over the world today.

Unlike biological methanation, catalytic or thermochemical CO2 methanation (CCM) operates at high temperatures between 200 and 550 °C and pressures up to 100 bar due to thermodynamic equilibrium. Therefore, CCM is characterized by a high production rate and methane selectivity. The reaction is highly exothermic, and proper heat management is necessary to avoid hot spots which are detrimental to catalyst performance.

To date, although great efforts have been made to investigate the reactor and process design for CCM, commercial CCM plants are still rare as commercial CCM requires a proper process design and reactors considering both economic feasibility and environmental regulation on a specific country.

Here, we aim to gather contributions from researchers and engineers to examine the issues of a flexible process and reactor design for CCM that is suitable for commercialization in many different countries.

Dr. Son Ich Ngo
Prof. Dr. Enrique García-Bordejé
Guest Editors

Manuscript Submission Information

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Keywords

  • Catalytic CO2 methanation
  • Modeling and simulation of catalytic CO2 methanation reactors
  • Reactor design for CO2 methanation
  • Power-to-gas
  • Energy storage

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Published Papers (7 papers)

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Editorial

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4 pages, 232 KiB  
Editorial
Catalytic CO2 Methanation Reactors and Processes
by Son Ich Ngo and Enrique García-Bordejé
Catalysts 2023, 13(11), 1422; https://doi.org/10.3390/catal13111422 - 7 Nov 2023
Cited by 1 | Viewed by 2712
Abstract
CO2 methanation is a chemical process that involves the conversion of carbon dioxide (CO2) and hydrogen (H2) gases into methane (CH4) and water (H2O) [...] Full article
(This article belongs to the Special Issue Catalytic CO2 Methanation Reactors and Processes)

Research

Jump to: Editorial

15 pages, 2592 KiB  
Article
Biogas Upgrading by CO2 Methanation with Ni-, Ni–Fe-, and Ru-Based Catalysts
by Andrés Sanz-Martínez, Paul Durán, Víctor D. Mercader, Eva Francés, José Ángel Peña and Javier Herguido
Catalysts 2022, 12(12), 1609; https://doi.org/10.3390/catal12121609 - 8 Dec 2022
Cited by 7 | Viewed by 2790
Abstract
This piece of work dealt with the concept of ‘biogas upgrading’ or enrichment of the CH4 contained in a sweetened biogas to proportions and features comparable to those of synthetic natural gas (SNG). For this, the behavior of three lab made catalysts [...] Read more.
This piece of work dealt with the concept of ‘biogas upgrading’ or enrichment of the CH4 contained in a sweetened biogas to proportions and features comparable to those of synthetic natural gas (SNG). For this, the behavior of three lab made catalysts (Ni/Al2O3, Ru/Al2O3, and Ni–Fe/Al2O3) was tested in a CO2 methanation reaction (Sabatier reaction) under different feeding conditions (with and without methane). In the first set of experiments (without methane), the good catalytic behavior of the solids was validated. All three catalysts offered similar and increasing CO2 conversions with increasing temperature (range studied from 250 to 400 °C) at a constant WHSV of 30 × 103 STPmL·gcat−1·h−1. The CH4 selectivity remained close to one in all cases. Considering their total metallic load, the Ru (3.7 wt%)-based catalyst stood out remarkably, with TOF values that reached up to 5.1 min−1, this being six or three times higher, than those obtained with the Ni (10.3 wt%) and Ni–Fe (7.4–2.1 wt%) catalysts, respectively. In the second set (cofeeding methane), and also for the three catalysts, a high correspondence between the conversions (and selectivities) obtained with both types of feeds was observed. This indicated that the addition of CH4 to the system did not severely modify the reaction mechanism, resulting in the possibility of taking advantage of the ‘biogas upgrading’ process by using H2 produced off-peak by electrolysis. In order to maximize the CH4 yield, temperatures in the range from 350–375 °C and a H2:CO2 molar ratio of 6:1 were determined as the optimal reaction conditions. Full article
(This article belongs to the Special Issue Catalytic CO2 Methanation Reactors and Processes)
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16 pages, 5281 KiB  
Article
Reaction Characteristics of Ni-Based Catalyst Supported by Al2O3 in a Fluidized Bed for CO2 Methanation
by Byungwook Hwang, Son Ich Ngo, Young-Il Lim, Myung Won Seo, Sung Jin Park, Ho-Jung Ryu, Hyungseok Nam and Doyeon Lee
Catalysts 2022, 12(11), 1346; https://doi.org/10.3390/catal12111346 - 2 Nov 2022
Cited by 5 | Viewed by 2336
Abstract
CO2 methanation is a promising technology to store renewable energy by converting carbon dioxide with green hydrogen into methane, which is known as power to gas (PtG). In this study, CO2 methanation performance of a Ni/Al2O3 catalyst was [...] Read more.
CO2 methanation is a promising technology to store renewable energy by converting carbon dioxide with green hydrogen into methane, which is known as power to gas (PtG). In this study, CO2 methanation performance of a Ni/Al2O3 catalyst was investigated in a bubbling fluidized bed (BFB) and the axial gas concentration, temperature, and CO2 conversion were densely analyzed. Moreover, a modified reaction kinetic model was proposed, and the results were compared with experimental data. The bed temperature increased by 11 °C from 340 °C to 351 °C within the first 30 mm of the fluidized bed. The CO2 conversion was approximately 90% within 50 mm from the bottom of the reactor and was maintained above this height. The Ni/Al2O3 catalyst exhibited the highest CO2 conversion (95%) at 320 °C. Using a simple plug-flow reactor model, three optimized kinetic modification factors (1.5094, 0.0238, and 0.2466) were used to fit the experimental data. The hydrodynamic effects significantly influenced the chemical reaction kinetics of the BFB. Full article
(This article belongs to the Special Issue Catalytic CO2 Methanation Reactors and Processes)
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11 pages, 1337 KiB  
Article
Comparing the Performance of Supported Ru Nanocatalysts Prepared by Chemical Reduction of RuCl3 and Thermal Decomposition of Ru3(CO)12 in the Sunlight-Powered Sabatier Reaction
by Daria Burova, Jelle Rohlfs, Francesc Sastre, Pau Martínez Molina, Nicole Meulendijks, Marcel A. Verheijen, An-Sofie Kelchtermans, Ken Elen, An Hardy, Marlies K. Van Bael and Pascal Buskens
Catalysts 2022, 12(3), 284; https://doi.org/10.3390/catal12030284 - 2 Mar 2022
Cited by 5 | Viewed by 3463
Abstract
The preparation of Ru nanoparticles supported on γ-Al2O3 followed by chemical reduction using RuCl3 as a precursor is demonstrated, and their properties are compared to Ru nanoparticles supported on γ-Al2O3 prepared by impregnation of γ-Al2 [...] Read more.
The preparation of Ru nanoparticles supported on γ-Al2O3 followed by chemical reduction using RuCl3 as a precursor is demonstrated, and their properties are compared to Ru nanoparticles supported on γ-Al2O3 prepared by impregnation of γ-Al2O3 with Ru3(CO)12 and subsequent thermal decomposition. The Ru nanoparticles resulting from chemical reduction of RuCl3 are slightly larger (1.2 vs. 0.8 nm). In addition, Ru nanoparticles were deposited on Stöber SiO2 using both deposition techniques. These particles were larger than the ones deposited on γ-Al2O3 (2.5 and 3.4 nm for chemical reduction and thermal decomposition, respectively). Taking into account the size differences between the Ru nanoparticles, all catalysts display similar activity (0.14–0.63 mol·gRu−1·h−1) and selectivity (≥99%) in the sunlight-powered Sabatier reaction. Ergo, the use of toxic and volatile Ru3(CO)12 can be avoided, since catalysts prepared by chemical reduction of RuCl3 display similar catalytic performance. Full article
(This article belongs to the Special Issue Catalytic CO2 Methanation Reactors and Processes)
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11 pages, 2296 KiB  
Article
Continuous-Flow Sunlight-Powered CO2 Methanation Catalyzed by γ-Al2O3-Supported Plasmonic Ru Nanorods
by Jelle Rohlfs, Koen W. Bossers, Nicole Meulendijks, Fidel Valega Mackenzie, Man Xu, Marcel A. Verheijen, Pascal Buskens and Francesc Sastre
Catalysts 2022, 12(2), 126; https://doi.org/10.3390/catal12020126 - 21 Jan 2022
Cited by 12 | Viewed by 3408
Abstract
Plasmonic CO2 methanation using γ-Al2O3-supported Ru nanorods was carried out under continuous-flow conditions without conventional heating, using mildly concentrated sunlight as the sole and sustainable energy source (AM 1.5, irradiance 5.5–14.4 kW·m−2 = 5.5–14.4 suns). Under 12.5 [...] Read more.
Plasmonic CO2 methanation using γ-Al2O3-supported Ru nanorods was carried out under continuous-flow conditions without conventional heating, using mildly concentrated sunlight as the sole and sustainable energy source (AM 1.5, irradiance 5.5–14.4 kW·m−2 = 5.5–14.4 suns). Under 12.5 suns, a CO2 conversion exceeding 97% was achieved with complete selectivity towards CH4 and a stable production rate (261.9 mmol·gRu−1·h−1) for at least 12 h. The CH4 production rate showed an exponential increase with increasing light intensity, suggesting that the process was mainly promoted by photothermal heating. This was confirmed by the apparent activation energy of 64.3 kJ·mol−1, which is very similar to the activation energy obtained for reference experiments in dark (67.3 kJ·mol−1). The flow rate influence was studied under 14.4 suns, achieving a CH4 production plateau of 264 µmol min−1 (792 mmol·gRu−1·h−1) with a constant catalyst bed temperature of approximately 204 °C. Full article
(This article belongs to the Special Issue Catalytic CO2 Methanation Reactors and Processes)
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20 pages, 7598 KiB  
Article
Solution and Parameter Identification of a Fixed-Bed Reactor Model for Catalytic CO2 Methanation Using Physics-Informed Neural Networks
by Son Ich Ngo and Young-Il Lim
Catalysts 2021, 11(11), 1304; https://doi.org/10.3390/catal11111304 - 28 Oct 2021
Cited by 27 | Viewed by 4958
Abstract
In this study, we develop physics-informed neural networks (PINNs) to solve an isothermal fixed-bed (IFB) model for catalytic CO2 methanation. The PINN includes a feed-forward artificial neural network (FF-ANN) and physics-informed constraints, such as governing equations, boundary conditions, and reaction kinetics. The [...] Read more.
In this study, we develop physics-informed neural networks (PINNs) to solve an isothermal fixed-bed (IFB) model for catalytic CO2 methanation. The PINN includes a feed-forward artificial neural network (FF-ANN) and physics-informed constraints, such as governing equations, boundary conditions, and reaction kinetics. The most effective PINN structure consists of 5–7 hidden layers, 256 neurons per layer, and a hyperbolic tangent (tanh) activation function. The forward PINN model solves the plug-flow reactor model of the IFB, whereas the inverse PINN model reveals an unknown effectiveness factor involved in the reaction kinetics. The forward PINN shows excellent extrapolation performance with an accuracy of 88.1% when concentrations outside the training domain are predicted using only one-sixth of the entire domain. The inverse PINN model identifies an unknown effectiveness factor with an error of 0.3%, even for a small number of observation datasets (e.g., 20 sets). These results suggest that forward and inverse PINNs can be used in the solution and system identification of fixed-bed models with chemical reaction kinetics. Full article
(This article belongs to the Special Issue Catalytic CO2 Methanation Reactors and Processes)
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10 pages, 2545 KiB  
Article
Deactivation and Regeneration Method for Ni Catalysts by H2S Poisoning in CO2 Methanation Reaction
by Jeongyoon Ahn, Woojin Chung and Soonwoong Chang
Catalysts 2021, 11(11), 1292; https://doi.org/10.3390/catal11111292 - 27 Oct 2021
Cited by 8 | Viewed by 2472
Abstract
The carbon dioxide (CO2) methanation reaction is a process that produces methane (CH4) by reacting CO2 and H2. Many studies have been conducted on this process because it enables a reduction of greenhouse gases and the [...] Read more.
The carbon dioxide (CO2) methanation reaction is a process that produces methane (CH4) by reacting CO2 and H2. Many studies have been conducted on this process because it enables a reduction of greenhouse gases and the production of energy with carbon neutrality. Moreover, it also exhibits a higher efficiency at low temperatures due to its thermodynamic characteristics; thus, there have been many studies, particularly on the catalysts that are driven at low temperatures and have high durability. However, with regards to employing this process in actual industrial processes, studies on both toxic substances that can influence catalyst performance and regeneration are still insufficient. Therefore, in this paper, the activity of a Ni catalyst before and after hydrogen sulfide (H2S) exposure was compared and an in-depth analysis was conducted to reveal the activity performance through the regeneration treatment of the poisoned catalyst. This study observed the reaction activity changes when injecting H2S during the CO2 + H2 reaction to evaluate the toxic effect of H2S on the Ni-Ce-Zr catalyst, in which the results indicate that the reaction activity decreases rapidly at 220 °C. Next, this study also successfully conducted a regeneration of the Ni-Ce-Zr catalyst that was poisoned with H2S by applying H2 heat treatment. It is expected that the results of this study can be used as fundamental data in an alternative approach to performance recovery when a small amount of H2S is included in the reaction gas of industrial processes (landfill gas, fire extinguishing tank gas, etc.) that can be linked to CO2 methanation. Full article
(This article belongs to the Special Issue Catalytic CO2 Methanation Reactors and Processes)
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