Special Issue "C1 Chemistry—C1-Platform Chemicals as Cornerstone for a Sustainable Energy"

A special issue of Catalysts (ISSN 2073-4344).

Deadline for manuscript submissions: closed (15 June 2017)

Special Issue Editors

Guest Editor
Dr. Benoît Louis

Directeur de Recherches CNRS, Laboratoire de Synthèse Réactivité Organiques et Catalyse –LASYROC, Institute of Chemistry, UMR 7177, University of Strasbourg, 1 rue Blaise Pascal F-67000 Strasbourg Cedex, France
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Guest Editor
Prof. Qiang Wang

Environmental Functional Nanomaterials (EFN) Lab, College of Environmental Science and Engineering, Beijing Forestry University, P.O. Box 60, 35 Qinghua East Road, Haidian District, Beijing 100083, China
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Phone: 86-13699130626
Guest Editor
Prof. Marcelo Maciel Pereira

LACES - Universidade Federal do Rio de Janeiro, Instituto de Química, Av. Athos da Silveira Ramos 149, CT Bloco A, Cidade Universitária, 21941-909 Rio de Janeiro, Brazil
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Special Issue Information

Dear Colleagues,

In the last century, life expectancy has more than doubled and most human-related activities have dramatically improved with respect to security and comfort. Unfortunately, despite the enormous benefits to modern civilization, the adopted production scheme, and consumption patterns are mostly based on non-recycled sources of energy. Additionally, less than 0.1% of CO2 produced by anthropogenic means are recycled or mitigated. Moreover, oil petroleum scarcity will affect the health system through its effects on medical supplies and equipment, transportation, energy generation, and food production.

In addition to carbon dioxide, all C1-platform chemicals appear to be cornerstones to generate a new and sustainable energy concept for the 21st century: Methane, methanol, carbon monoxide, and formic acid can all be used directly either as fuels or as storage media.

Therefore, a key to shorten the path to sustainability is to implement, in the refinery production structure:

1—green energy sources. 

2—a central C1-chemical platform. 

3—new processes for CO2 mitigation and recyclability.

These features should be designed in order to be connected to already-existing processes. Therefore, future refineries should supply our needs by proper combinations of (new or regular) processes and feedstocks. 

This Special Issue is devoted to present the central catalytic role into the aforementioned topics. For example:

- CO2 capture

- use of CO2 as reactant or process to its mitigation;

- C1-platform like formic acid, CO, methanol and methane;

- biomass or biomass-derivate feed;

- gas emissions mitigation (NOx and SOx);

- hydro-treatment process for fuel, etc.

 

Dr. Benoît Louis

Prof. Qiang Wang

Prof. Marcelo Maciel Pereira
Guest Editors

Manuscript Submission Information

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Submitted manuscripts should not have been published previously, nor be under consideration for publication elsewhere (except conference proceedings papers). All manuscripts are thoroughly refereed through a single-blind peer-review process. A guide for authors and other relevant information for submission of manuscripts is available on the Instructions for Authors page. Catalysts is an international peer-reviewed open access monthly journal published by MDPI.

Please visit the Instructions for Authors page before submitting a manuscript. The Article Processing Charge (APC) for publication in this open access journal is 1000 CHF (Swiss Francs). Submitted papers should be well formatted and use good English. Authors may use MDPI's English editing service prior to publication or during author revisions.

Keywords

  • CO2 capture and valorization
  • biomass conversion
  • gas-to-liquids
  • Methanol-To-Hydrocarbons
  • C1 chemistry
  • energy
  • biofuels

Published Papers (12 papers)

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Research

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Open AccessArticle DBD Plasma Assisted CO2 Decomposition: Influence of Diluent Gases
Catalysts 2017, 7(9), 244; doi:10.3390/catal7090244
Received: 25 June 2017 / Revised: 29 July 2017 / Accepted: 9 August 2017 / Published: 23 August 2017
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Abstract
Carbon dioxide (CO2) partial reduction to carbon monoxide (CO) and oxygen has been conducted in a dielectric barrier discharge reactor (DBD) operating a packed bed configuration and the results are compared with that of no packing condition. The effect of diluent
[...] Read more.
Carbon dioxide (CO2) partial reduction to carbon monoxide (CO) and oxygen has been conducted in a dielectric barrier discharge reactor (DBD) operating a packed bed configuration and the results are compared with that of no packing condition. The effect of diluent gas is studied to understand the influence on dielectric strength of the plasma gas on CO2 splitting, with the objective of obtaining the best CO selectivity and high energy efficiency. Typical results indicated that among N2, He and Ar gases, Ar showed the best decomposition efficiency. Glass beads packing has a strong influence on the performance, probably due to the enhanced field strength due to dielectric nature of the packed material. In a similar manner, Ar mole ratio in the gas mixture also played a significant role, where the maximum CO2 conversion of 19.5% was obtained with packed DBD at CO2:Ar ratio 1:2. The best CO yield (16.8%) was also obtained under the same conditions. The highest energy efficiency was found to be 0.945 mmol/kJ. The activated species formed inside the CO2 plasma were identified by optical emission spectroscopy. Full article
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Open AccessArticle Effect of Citric Acid on MoO3/Al2O3 Catalysts for Sulfur-Resistant Methanation
Catalysts 2017, 7(5), 151; doi:10.3390/catal7050151
Received: 6 December 2016 / Revised: 24 April 2017 / Accepted: 26 April 2017 / Published: 12 May 2017
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Abstract
A series of MoO3/Al2O3 catalysts with different amounts (molar ratio of CA/Mo = 0, 1, 1.5, and 2) of citric acid (CA) prepared by simultaneous impregnation were evaluated for sulfur-resistant methanation. Based on the evaluation results, catalytic activity
[...] Read more.
A series of MoO3/Al2O3 catalysts with different amounts (molar ratio of CA/Mo = 0, 1, 1.5, and 2) of citric acid (CA) prepared by simultaneous impregnation were evaluated for sulfur-resistant methanation. Based on the evaluation results, catalytic activity increased accompanied with the rise of citric acid amount. Combine with the analysis of N2-physisorption, XRD, H2-TPR, XPS, and TEM, the catalyst saturated loading capacity improved, resulting in increasing dispersion of Mo species on Al2O3 surface clearly. According to H2-TPR result, the Mo oxide precursors can be more easily sulfureted when citric acid is added. Moreover, based on the Raman analysis, increasingly tetrahedrally coordinated Mo6+ species with high methanation performance are generated after citric acid treatment. These factors probably together accelerate MoO3/Al2O3 catalytic activity growth for methanation. Full article
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Open AccessArticle Synthesis of SAPO-34 Molecular Sieves via Novel Intermittent Hydrothermal Treatment and Its Effect on the Crystallization and Product Properties
Catalysts 2017, 7(5), 150; doi:10.3390/catal7050150
Received: 13 March 2017 / Revised: 24 April 2017 / Accepted: 26 April 2017 / Published: 11 May 2017
PDF Full-text (6604 KB) | HTML Full-text | XML Full-text | Supplementary Files
Abstract
Intermittent hydrothermal treatment was introduced into the synthesis of SAPO-34 molecular sieves to control the nucleation and the growth in the crystallization. The effect of the crystallization time, the order of long-time and short-time crystallization in two-stage crystallization, and frequency in multi-stage crystallization
[...] Read more.
Intermittent hydrothermal treatment was introduced into the synthesis of SAPO-34 molecular sieves to control the nucleation and the growth in the crystallization. The effect of the crystallization time, the order of long-time and short-time crystallization in two-stage crystallization, and frequency in multi-stage crystallization on synthesis, physicochemical properties and catalytic performance for conversion of methanol to light olefins (MTO) has been studied. The results show that pure SAPO-34 can be obtained with increasing crystallization time. The interruption of the initial crystallization is more beneficial for improving the Si distribution and the MTO catalytic performance of SAPO-34 molecular sieves. The sample obtained by repeatedly alternating heating and cooling during crystallization shows smaller particle size, higher acidity, longer lifetimes and higher yields of ethylene than that obtained by the conventional continuous crystallization at high temperature. Full article
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Open AccessArticle Hydrothermal Fabrication of High Specific Surface Area Mesoporous MgO with Excellent CO2 Adsorption Potential at Intermediate Temperatures
Catalysts 2017, 7(4), 116; doi:10.3390/catal7040116
Received: 5 March 2017 / Revised: 10 April 2017 / Accepted: 11 April 2017 / Published: 15 April 2017
Cited by 2 | PDF Full-text (8654 KB) | HTML Full-text | XML Full-text
Abstract
In this work, we report on a novel sodium dodecyl sulfate (SDS)-assisted magnesium oxide (MgO)-based porous adsorbent synthesized by hydrothermal method for intermediate CO2 capture. For industrial MgO, its CO2 adsorption capacity is normally less than 0.06 mmol g−1,
[...] Read more.
In this work, we report on a novel sodium dodecyl sulfate (SDS)-assisted magnesium oxide (MgO)-based porous adsorbent synthesized by hydrothermal method for intermediate CO2 capture. For industrial MgO, its CO2 adsorption capacity is normally less than 0.06 mmol g−1, with a specific surface area as low as 25.1 m2 g−1. Herein, leaf-like MgO nanosheets which exhibited a disordered layer structure were fabricated by the introduction of SDS surfactants and the control of other synthesis parameters. This leaf-like MgO adsorbent showed an excellent CO2 capacity of 0.96 mmol g−1 at moderate temperatures (~300 °C), which is more than ten times higher than that of the commercial light MgO. This novel mesoporous MgO adsorbent also exhibited high stability during multiple CO2 adsorption/desorption cycles. The excellent CO2 capturing performance was believed to be related to its high specific surface area of 321.3 m2 g−1 and abundant surface active adsorption sites. This work suggested a new synthesis scheme for MgO based CO2 adsorbents at intermediate temperatures, providing a competitive candidate for capturing CO2 from certain sorption enhanced hydrogen production processes. Full article
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Open AccessArticle Environmental Benign Synthesis of Lithium Silicates and Mg-Al Layered Double Hydroxide from Vermiculite Mineral for CO2 Capture
Catalysts 2017, 7(4), 105; doi:10.3390/catal7040105
Received: 26 February 2017 / Revised: 20 March 2017 / Accepted: 31 March 2017 / Published: 3 April 2017
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Abstract
This research introduces a completely new environmental benign synthesis route for obtaining two kinds of inter-mediate and high temperature CO2 sorbents, Mg-Al layered double hydroxide (LDH) and Li4SiO4, from vermiculite. The mineral vermiculite was leached with acid, from
[...] Read more.
This research introduces a completely new environmental benign synthesis route for obtaining two kinds of inter-mediate and high temperature CO2 sorbents, Mg-Al layered double hydroxide (LDH) and Li4SiO4, from vermiculite. The mineral vermiculite was leached with acid, from which the obtained SiO2 was used for the synthesis of Li4SiO4 and the leaching waste water was used for the synthesis of Mg-Al LDH. Therefore, no waste was produced during the whole process. Both Li4SiO4 and Mg-Al LDH sorbents were carefully characterized using XRD, SEM, and BET analyses. The CO2 capturing performance of these two sorbents was comprehensively evaluated. The influence of the Li/Si ratio, calcination temperature, calcination time, and sorption temperature on the CO2 sorption capacity of Li4SiO4, and the sorption temperature on the CO2 sorption capacity of LDH, were investigated. The optimal leaching acid concentration for vermiculite and the CO2 sorption/desorption cycling performance of both the Li4SiO4 and Mg-Al LDH sorbents were determined. In sum, this demonstrated a unique and environment-friendly scheme for obtaining two CO2 sorbents from cheap raw materials, and this idea is applicable to the efficient utilization of other minerals. Full article
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Open AccessArticle Methanation of Carbon Dioxide over Ni–Ce–Zr Oxides Prepared by One-Pot Hydrolysis of Metal Nitrates with Ammonium Carbonate
Catalysts 2017, 7(4), 104; doi:10.3390/catal7040104
Received: 6 March 2017 / Revised: 28 March 2017 / Accepted: 29 March 2017 / Published: 31 March 2017
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Abstract
Ni–Ce–Zr mixed oxides were prepared through one-pot hydrolysis of mixed metal nitrates with ammonium carbonate for CO2 methanation. The effects of Ce/Zr molar ratio and Ni content on catalysts’ physical and chemical properties, reduction degree of Ni2+, and catalytic properties
[...] Read more.
Ni–Ce–Zr mixed oxides were prepared through one-pot hydrolysis of mixed metal nitrates with ammonium carbonate for CO2 methanation. The effects of Ce/Zr molar ratio and Ni content on catalysts’ physical and chemical properties, reduction degree of Ni2+, and catalytic properties were systematically investigated. The results showed that Zr could lower metallic Ni particle sizes and alter interaction between Ni and supports, resulting in enhancements in the catalytic activity for CO2 methanation. The Ni–Ce–Zr catalyst containing 40 wt % Ni and Ce/Zr molar ratio of 9:1 exhibited the optimal catalytic properties, with 96.2% CO2 conversion and almost 100% CH4 selectivity at a low temperature of 275 °C. During the tested period of 500 h, CO2 conversion and CH4 selectivity over Ni–Ce–Zr catalyst kept constant under 300 °C. Full article
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Open AccessArticle Highly Selective Solid Acid Catalyst H1−xTi2(PO4)3−x(SO4)x for Non-Oxidative Dehydrogenation of Methanol and Ethanol
Catalysts 2017, 7(3), 95; doi:10.3390/catal7030095
Received: 21 February 2017 / Revised: 13 March 2017 / Accepted: 16 March 2017 / Published: 22 March 2017
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Abstract
The conversion of alcohols towards aldehydes in the presence of catalysts by non-oxidative dehydrogenation requires special importance from the perspective of green chemistry. Sodium (Na) super ionic conductor (NASICON)-type hydrogen titanium phosphate sulfate (HTPS; H1−xTi2(PO4)3−
[...] Read more.
The conversion of alcohols towards aldehydes in the presence of catalysts by non-oxidative dehydrogenation requires special importance from the perspective of green chemistry. Sodium (Na) super ionic conductor (NASICON)-type hydrogen titanium phosphate sulfate (HTPS; H1−xTi2(PO4)3−x(SO4)x, x = 0.5–1) catalysts were synthesized by the sol-gel method, characterized by N2 gas sorption, X-ray powder diffraction (XRD), scanning electron microscopy (SEM), transmission electron microscopy (TEM), NH3 temperature-programmed desorption (NH3-TPD), ultraviolet–visible (UV-VIS) spectroscopy, and their catalytic properties were studied for the non-oxidative dehydrogenation of methanol and ethanol. The ethanol is more reactive than methanol, with the conversion for ethanol exceeding 95% as compared to methanol, where the conversion has a maximum value at 55%. The selectivity to formaldehyde is almost 100% in methanol conversion, while the selectivity to acetaldehyde decreases from 56% to 43% in ethanol conversion, when the reaction temperature is increased from 250 to 400 °C. Full article
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Open AccessArticle Two-Dimensional Layered Double Hydroxide Derived from Vermiculite Waste Water Supported Highly Dispersed Ni Nanoparticles for CO Methanation
Catalysts 2017, 7(3), 79; doi:10.3390/catal7030079
Received: 9 December 2016 / Accepted: 1 March 2017 / Published: 7 March 2017
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Abstract
Expanded multilayered vermiculite (VMT) was successfully used as catalyst support and Ni/VMT synthesized by microwave irradiation assisted synthesis (MIAS) exhibited excellent performance in our previous work. We also developed a two-dimensional porous SiO2 nanomesh (2D VMT-SiO2) by mixed-acid etching of VMT. Compared with
[...] Read more.
Expanded multilayered vermiculite (VMT) was successfully used as catalyst support and Ni/VMT synthesized by microwave irradiation assisted synthesis (MIAS) exhibited excellent performance in our previous work. We also developed a two-dimensional porous SiO2 nanomesh (2D VMT-SiO2) by mixed-acid etching of VMT. Compared with three-dimensional (3D) MCM-41, 2D VMT-SiO2 as a catalyst support provided a superior position for implantation of NiO species and the as-obtained catalyst exhibited excellent performance. In this paper, we successfully synthesized a layered double hydroxide (LDH) using the spent liquor after mixed-acid etching of VMT, which mainly contained Mg2+ and Al3+. The as-calcined layered double oxide (LDO) was used as a catalyst support for CO methanation. Compared with Ni/MgAl-LDO, Ni/VMT-LDO had smaller active component particles; therefore, in this study, it exhibited excellent catalytic performance over the whole temperature range of 250–500 °C. Ni/VMT-LDO achieved the best activity with 87.88% CO conversion, 89.97% CH4 selectivity, and 12.47 × 10−2·s−1 turn over frequency (TOF) at 400 °C under a gas hourly space velocity of 20,000 mL/g/h. This study demonstrated that VMT-LDO as a catalyst support provided an efficient way to develop high-performance catalysts for synthetic natural gas (SNG) from syngas. Full article
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Open AccessArticle The Synergy Effect of Ni-M (M = Mo, Fe, Co, Mn or Cr) Bicomponent Catalysts on Partial Methanation Coupling with Water Gas Shift under Low H2/CO Conditions
Catalysts 2017, 7(2), 51; doi:10.3390/catal7020051
Received: 6 January 2017 / Revised: 30 January 2017 / Accepted: 3 February 2017 / Published: 8 February 2017
Cited by 1 | PDF Full-text (7869 KB) | HTML Full-text | XML Full-text | Supplementary Files
Abstract
Ni-M (M = Mo, Fe, Co, Mn or Cr) bicomponent catalysts were prepared through the co-impregnation method for upgrading low H2/CO ratio biomass gas into urban gas through partial methanation coupling with water gas shift (WGS). The catalysts were characterized by
[...] Read more.
Ni-M (M = Mo, Fe, Co, Mn or Cr) bicomponent catalysts were prepared through the co-impregnation method for upgrading low H2/CO ratio biomass gas into urban gas through partial methanation coupling with water gas shift (WGS). The catalysts were characterized by N2 isothermal adsorption, X-ray diffraction (XRD), H2 temperature programmed reduction (H2-TPR), H2 temperature programmed desorption (H2-TPD), scanning electron microscopy (SEM) and thermogravimetry (TG). The catalytic performances demonstrated that Mn and Cr were superior to the other three elements due to the increased fraction of reducible NiO particles, promoted dispersion of Ni nanoparticles and enhanced H2 chemisorption ability. The comparative study on Mn and Cr showed that Mn was more suitable due to its smaller carbon deposition rate and wider adaptability to various H2/CO and H2O/CO conditions, indicating its better synergy effect with Ni. A nearly 100 h, the lifetime test and start/stop cycle test further implied that 15Ni-3Mn was stable for industrial application. Full article
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Open AccessArticle Core-Shell Structured Ni@SiO2 Catalysts Exhibiting Excellent Catalytic Performance for Syngas Methanation Reactions
Catalysts 2017, 7(1), 21; doi:10.3390/catal7010021
Received: 24 November 2016 / Revised: 17 December 2016 / Accepted: 5 January 2017 / Published: 9 January 2017
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Abstract
In this study, we prepared core-shell structured Ni@SiO2 catalysts using chemical precipitation and modified Stöber methods. The obtained Ni@SiO2 samples exhibited excellent catalysis performances, including high CO conversion of 99.0% and CH4 yield of 89.8%. Moreover, Ni@SiO2 exhibited excellent
[...] Read more.
In this study, we prepared core-shell structured Ni@SiO2 catalysts using chemical precipitation and modified Stöber methods. The obtained Ni@SiO2 samples exhibited excellent catalysis performances, including high CO conversion of 99.0% and CH4 yield of 89.8%. Moreover, Ni@SiO2 exhibited excellent catalytic stability during a 100 h lifetime test, which was superior to that of the Ni/SiO2 catalyst. The prepared samples were characterized using a series of techniques, and the results indicated that the catalytic performance for syngas methanation reaction of the Ni@SiO2 sample was markedly improved owing to its nanoreactor structure. The strong interaction between the Ni core and the SiO2 shell effectively restrained the growth of particles, and the deposition of C species. Full article
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Review

Jump to: Research

Open AccessReview Review on Copper and Palladium Based Catalysts for Methanol Steam Reforming to Produce Hydrogen
Catalysts 2017, 7(6), 183; doi:10.3390/catal7060183
Received: 4 May 2017 / Revised: 26 May 2017 / Accepted: 26 May 2017 / Published: 8 June 2017
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Abstract
Methanol steam reforming is a promising technology for producing hydrogen for onboard fuel cell applications. The methanol conversion rate and the contents of hydrogen, carbon monoxide and carbon dioxide in the reformate, significantly depend on the reforming catalyst. Copper-based catalysts and palladium-based catalysts
[...] Read more.
Methanol steam reforming is a promising technology for producing hydrogen for onboard fuel cell applications. The methanol conversion rate and the contents of hydrogen, carbon monoxide and carbon dioxide in the reformate, significantly depend on the reforming catalyst. Copper-based catalysts and palladium-based catalysts can effectively convert methanol into hydrogen and carbon dioxide. Copper and palladium-based catalysts with different formulations and compositions have been thoroughly investigated in the literature. This work summarized the development of the two groups of catalysts for methanol steam reforming. Interactions between the activity components and the supports as well as the effects of different promoters were discussed. Compositional and morphological characteristics, along with the methanol steam reforming performances of different Cu/ZnO and Pd/ZnO catalysts promoted by Al2O3, CeO2, ZrO2 or other metal oxides, were reviewed and compared. Moreover, the reaction mechanism of methanol steam reforming over the copper based and palladium based catalysts were discussed. Full article
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Open AccessFeature PaperReview Supported Catalysts for CO2 Methanation: A Review
Catalysts 2017, 7(2), 59; doi:10.3390/catal7020059
Received: 16 December 2016 / Revised: 7 February 2017 / Accepted: 8 February 2017 / Published: 13 February 2017
Cited by 9 | PDF Full-text (2171 KB) | HTML Full-text | XML Full-text
Abstract
CO2 methanation is a well-known reaction that is of interest as a capture and storage (CCS) process and as a renewable energy storage system based on a power-to-gas conversion process by substitute or synthetic natural gas (SNG) production. Integrating water electrolysis and
[...] Read more.
CO2 methanation is a well-known reaction that is of interest as a capture and storage (CCS) process and as a renewable energy storage system based on a power-to-gas conversion process by substitute or synthetic natural gas (SNG) production. Integrating water electrolysis and CO2 methanation is a highly effective way to store energy produced by renewables sources. The conversion of electricity into methane takes place via two steps: hydrogen is produced by electrolysis and converted to methane by CO2 methanation. The effectiveness and efficiency of power-to-gas plants strongly depend on the CO2 methanation process. For this reason, research on CO2 methanation has intensified over the last 10 years. The rise of active, selective, and stable catalysts is the core of the CO2 methanation process. Novel, heterogeneous catalysts have been tested and tuned such that the CO2 methanation process increases their productivity. The present work aims to give a critical overview of CO2 methanation catalyst production and research carried out in the last 50 years. The fundamentals of reaction mechanism, catalyst deactivation, and catalyst promoters, as well as a discussion of current and future developments in CO2 methanation, are also included. Full article
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