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Nanomaterials
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Nanocatalysts for Methanation Reaction
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Nanocatalysts for Methanation Reaction

A special issue of Nanomaterials (ISSN 2079-4991). This special issue belongs to the section "Energy and Catalysis".

Deadline for manuscript submissions: closed (31 December 2022) | Viewed by 15493

Special Issue Editors

Prof. Dr. Maria Goula

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Guest Editor
Department of Chemical Engineering, University of Western Macedonia, GR–50100 Koila, Greece
Interests: environmental catalysis; biomass utilization; bio-oil; biogas; glycerol; hydrogen; syngas; renewable diesel; reforming; selective deoxygenation; CO2 hydrogenation; H2S adsorption
Special Issues, Collections and Topics in MDPI journals
Dr. Nikolaos D. Charisiou

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Guest Editor
Laboratory of Alternative Fuels & Environmental Catalysis (LAFEC), Department of Chemical Engineering, University of Western Macedonia, Active Urban Planning Zone (ZEP), GR-50100 Kozani, Greece
Interests: catalytic processes; biomass pyrolysis; environmental catalysis
Special Issues, Collections and Topics in MDPI journals
Prof. Dr. Kyriaki Polychronopoulou

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Guest Editor
Department of Mechanical Engineering, Khalifa University of Science and Technology, P.O. Box 127788, Abu Dhabi, United Arab Emirates
Interests: catalyst synthesis; porous materials; reforming; CO2 sequestration; H2 production and storage
Special Issues, Collections and Topics in MDPI journals

Special Issue Information

Dear Colleagues,

The CO2 methanation reaction provides an opportunity to utilize CO2 captured from air or flue gases, as well as H2 produced from renewables to produce synthetic natural gas, i.e., methane. This provides the opportunity to store the energy generated from renewables via a high energy density carrier, as well as utilize the excess anthropogenic CO2 and create a closed carbon cycle. The creation of low-cost, efficient, and highly selective catalysts able to convert the majority of CO2 into CH4 has received great research attention in recent years. Rh and especially Ru among noble metals, as well as Ni among transition metals, are the most popular active phases for CO2 methanation. Furthermore, the support type also exerts a great influence, with redox active CeO2-based supports being proven to boost low temperature catalytic activity and CH4 selectivity. Many works also focus on the effect of active metal dispersion, the texture of the metal oxide support, the synergetic effect provided by adding two active metal phases, as well as the availability of active sites for CO2 and H2 dissociation, respectively.

This Special Issue of Nanomaterials will aim to cover recent advances made in the following fields: Synthesis of nanostructured catalysts with a different texture and morphology; preparation of bimetallic catalysts with a different mix of supported metals; enhancement of defect chemistry of redox-active supports toward boosting low-temperature catalytic activity and selectivity; influence of different preparation methods on active metal dispersion.

Prof. Dr. Maria Goula
Dr. Nikolaos D. Charisiou
Prof. Dr. Kyriaki Polychronopoulou
Guest Editors

Manuscript Submission Information

Manuscripts should be submitted online at www.mdpi.com by registering and logging in to this website. Once you are registered, click here to go to the submission form. Manuscripts can be submitted until the deadline. All submissions that pass pre-check are peer-reviewed. Accepted papers will be published continuously in the journal (as soon as accepted) and will be listed together on the special issue website. Research articles, review articles as well as short communications are invited. For planned papers, a title and short abstract (about 100 words) can be sent to the Editorial Office for announcement on this website.

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. Nanomaterials is an international peer-reviewed open access semimonthly 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 2900 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 methanation
  • CO2 utilization
  • Power-to-Gas Nanocatalysts
  • Metal dispersion
  • Nickel-based catalyst
  • Bimetallic catalyst
  • Catalyst morphology
  • Redox properties
  • Oxygen lability

Published Papers (7 papers)

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Research

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13 pages, 2604 KiB  
Article
Catalytic Sabatier Process under Thermally and Magnetically Induced Heating: A Comparative Case Study for Titania-Supported Nickel Catalyst
by Sourav Ghosh, Sharad Gupta, Manon Gregoire, Thibault Ourlin, Pier-Francesco Fazzini, Edmond Abi-Aad, Christophe Poupin and Bruno Chaudret
Nanomaterials 2023, 13(9), 1474; https://doi.org/10.3390/nano13091474 - 26 Apr 2023
Cited by 2 | Viewed by 1751
Abstract
In the present paper, we compare the activity, selectivity, and stability of a supported nickel catalyst in classical heating conditions and in magnetically activated catalysis by using iron wool as a heating agent. The catalyst, 5 wt% Ni supported on titania (Degussa P25), [...] Read more.
In the present paper, we compare the activity, selectivity, and stability of a supported nickel catalyst in classical heating conditions and in magnetically activated catalysis by using iron wool as a heating agent. The catalyst, 5 wt% Ni supported on titania (Degussa P25), was prepared via an organometallic decomposition method and was thoroughly characterized by using elemental, microscopic, and diffraction techniques. In the event of magnetic induction heating, the % CO2 conversion reached a maximum of ~85% compared to ~78% for thermal conditions at a slightly lower temperature (~335 °C) than the thermal heating (380 °C). More importantly, both processes were found to be stable for 45 h on stream. Moreover, the effects of magnetic induction and classical heating over the catalyst evolution were discussed. This study demonstrated the potential of magnetic heating-mediated methanation, which is currently under investigation for the development of pilot-scale reactors. Full article
(This article belongs to the Special Issue Nanocatalysts for Methanation Reaction)
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12 pages, 2315 KiB  
Article
One-Step Synthesis of a Binder-Free, Stable, and High-Performance Electrode; Cu-O|Cu3P Heterostructure for the Electrocatalytic Methanol Oxidation Reaction (MOR)
by Alina Yarmolenko, Bibhudatta Malik, Efrat Shawat Avraham and Gilbert Daniel Nessim
Nanomaterials 2023, 13(7), 1234; https://doi.org/10.3390/nano13071234 - 30 Mar 2023
Cited by 1 | Viewed by 1298
Abstract
Although direct methanol fuel cells (DMFCs) have been spotlighted in the past decade, their commercialization has been hampered by the poor efficiency of the methanol oxidation reaction (MOR) due to the unsatisfactory performance of currently available electrocatalysts. Herein, we developed a binder-free, copper-based, [...] Read more.
Although direct methanol fuel cells (DMFCs) have been spotlighted in the past decade, their commercialization has been hampered by the poor efficiency of the methanol oxidation reaction (MOR) due to the unsatisfactory performance of currently available electrocatalysts. Herein, we developed a binder-free, copper-based, self-supported electrode consisting of a heterostructure of Cu3P and mixed copper oxides, i.e., cuprous–cupric oxide (Cu-O), as a high-performance catalyst for the electro-oxidation of methanol. We synthesized a self-supported electrode composed of Cu-O|Cu3P using a two-furnace atmospheric pressure–chemical vapor deposition (AP-CVD) process. High-resolution transmission electron microscopy analysis revealed the formation of 3D nanocrystals with defects and pores. Cu-O|Cu3P outperformed the MOR activity of individual Cu3P and Cu-O owing to the synergistic interaction between them. Cu3P|Cu-O exhibited a highest anodic current density of 232.5 mAcm−2 at the low potential of 0.65 V vs. Hg/HgO, which is impressive and superior to the electrocatalytic activity of its individual counterparts. The formation of defects, 3D morphology, and the synergistic effect between Cu3P and Cu-O play a crucial role in facilitating the electron transport between electrode and electrolyte to obtain the optimal MOR activity. Cu-O|Cu3P shows outstanding MOR stability for about 3600 s with 100% retention of the current density, which proves its robustness alongside CO intermediate. Full article
(This article belongs to the Special Issue Nanocatalysts for Methanation Reaction)
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17 pages, 7754 KiB  
Article
Performance of Cu/ZnO Nanosheets on Electrospun Al2O3 Nanofibers in CO2 Catalytic Hydrogenation to Methanol and Dimethyl Ether
by Itzhak I. Maor, Svetlana Heyte, Oren Elishav, Meirav Mann-Lahav, Joelle Thuriot-Roukos, Sébastien Paul and Gideon S. Grader
Nanomaterials 2023, 13(4), 635; https://doi.org/10.3390/nano13040635 - 05 Feb 2023
Cited by 1 | Viewed by 2097
Abstract
The synthesis of methanol and dimethyl ether (DME) from carbon dioxide (CO2) and green hydrogen (H2) offers a sustainable pathway to convert CO2 emissions into value-added products. This heterogeneous catalytic reaction often uses copper (Cu) catalysts due to [...] Read more.
The synthesis of methanol and dimethyl ether (DME) from carbon dioxide (CO2) and green hydrogen (H2) offers a sustainable pathway to convert CO2 emissions into value-added products. This heterogeneous catalytic reaction often uses copper (Cu) catalysts due to their low cost compared with their noble metal analogs. Nevertheless, improving the activity and selectivity of these Cu catalysts for these products is highly desirable. In the present study, a new architecture of Cu- and Cu/Zn-based catalysts supported on electrospun alumina nanofibers were synthesized. The catalysts were tested under various reaction conditions using high-throughput equipment to highlight the role of the hierarchical fibrous structure on the reaction activity and selectivity. The Cu or Cu/ZnO formed a unique structure of nanosheets, covering the alumina fiber surface. This exceptional morphology provides a large surface area, up to ~300 m2/g, accessible for reaction. Maximal production of methanol (~1106 gmethanolKgCu−1∙h−1) and DME (760 gDMEKgCu−1∙h−1) were obtained for catalysts containing 7% wt. Cu/Zn with a weight ratio of 2.3 Zn to Cu (at 300 °C, 50 bar). The promising results in CO2 hydrogenation to methanol and DME obtained here point out the significant advantage of nanofiber-based catalysts in heterogeneous catalysis. Full article
(This article belongs to the Special Issue Nanocatalysts for Methanation Reaction)
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18 pages, 2373 KiB  
Article
Flexible NiRu Systems for CO2 Methanation: From Efficient Catalysts to Advanced Dual-Function Materials
by Loukia-Pantzechroula Merkouri, Juan Luis Martín-Espejo, Luis Francisco Bobadilla, José Antonio Odriozola, Melis Seher Duyar and Tomas Ramirez Reina
Nanomaterials 2023, 13(3), 506; https://doi.org/10.3390/nano13030506 - 27 Jan 2023
Cited by 5 | Viewed by 2363
Abstract
CO2 emissions in the atmosphere have been increasing rapidly in recent years, causing global warming. CO2 methanation reaction is deemed to be a way to combat these emissions by converting CO2 into synthetic natural gas, i.e., CH4. NiRu/CeAl [...] Read more.
CO2 emissions in the atmosphere have been increasing rapidly in recent years, causing global warming. CO2 methanation reaction is deemed to be a way to combat these emissions by converting CO2 into synthetic natural gas, i.e., CH4. NiRu/CeAl and NiRu/CeZr both demonstrated favourable activity for CO2 methanation, with NiRu/CeAl approaching equilibrium conversion at 350 °C with 100% CH4 selectivity. Its stability under high space velocity (400 L·g−1·h−1) was also commendable. By adding an adsorbent, potassium, the CO2 adsorption capability of NiRu/CeAl was boosted, allowing it to function as a dual-function material (DFM) for integrated CO2 capture and utilisation, producing 0.264 mol of CH4/kg of sample from captured CO2. Furthermore, time-resolved operando DRIFTS-MS measurements were performed to gain insights into the process mechanism. The obtained results demonstrate that CO2 was captured on basic sites and was also dissociated on metallic sites in such a way that during the reduction step, methane was produced by two different pathways. This study reveals that by adding an adsorbent to the formulation of an effective NiRu methanation catalyst, advanced dual-function materials can be designed. Full article
(This article belongs to the Special Issue Nanocatalysts for Methanation Reaction)
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19 pages, 2882 KiB  
Article
Catalyst Design: Counter Anion Effect on Ni Nanocatalysts Anchored on Hollow Carbon Spheres
by Ryan O’Connor, Joyce B. Matsoso, Victor Mashindi, Pumza Mente, Lebohang Macheli, Beatriz D. Moreno, Bryan P. Doyle, Neil J. Coville and Dean H. Barrett
Nanomaterials 2023, 13(3), 426; https://doi.org/10.3390/nano13030426 - 20 Jan 2023
Viewed by 1527
Abstract
Herein, the influence of the counter anion on the structural properties of hollow carbon spheres (HCS) support was investigated by varying the nickel metal precursor salts applied. TEM and SEM micrographs revealed the dimensional dependence of the HCS shell on the Ni precursor [...] Read more.
Herein, the influence of the counter anion on the structural properties of hollow carbon spheres (HCS) support was investigated by varying the nickel metal precursor salts applied. TEM and SEM micrographs revealed the dimensional dependence of the HCS shell on the Ni precursor salt, as evidenced by thick (~42 nm) and thin (~23 nm) shells for the acetate and chloride-based salts, respectively. Importantly, the effect of the precursor salt on the textural properties of the HCS nanosupports (~565 m2/gNi(acet)) and ~607 m2/gNiCl), influenced the growth of the Ni nanoparticles, viz for the acetate-(ca 6.4 nm)- and chloride (ca 12 nm)-based salts, respectively. Further, XRD and PDF analysis showed the dependence of the reduction mechanism relating to nickel and the interaction of the nickel–carbon support on the type of counter anion used. Despite the well-known significance of the counter anion on the size and crystallinity of Ni nanoparticles, little is known about the influence of such counter anions on the physicochemical properties of the carbon support. Through this study, we highlight the importance of the choice of the Ni-salt on the size of Ni in Ni–carbon-based nanocatalysts. Full article
(This article belongs to the Special Issue Nanocatalysts for Methanation Reaction)
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20 pages, 6722 KiB  
Article
Optimal Icosahedral Copper-Based Bimetallic Clusters for the Selective Electrocatalytic CO2 Conversion to One Carbon Products
by Azeem Ghulam Nabi, Aman-ur-Rehman, Akhtar Hussain, Gregory A. Chass and Devis Di Tommaso
Nanomaterials 2023, 13(1), 87; https://doi.org/10.3390/nano13010087 - 24 Dec 2022
Cited by 4 | Viewed by 2331
Abstract
Electrochemical CO2 reduction reactions can lead to high value-added chemical and materials production while helping decrease anthropogenic CO2 emissions. Copper metal clusters can reduce CO2 to more than thirty different hydrocarbons and oxygenates yet they lack the required selectivity. We [...] Read more.
Electrochemical CO2 reduction reactions can lead to high value-added chemical and materials production while helping decrease anthropogenic CO2 emissions. Copper metal clusters can reduce CO2 to more than thirty different hydrocarbons and oxygenates yet they lack the required selectivity. We present a computational characterization of the role of nano-structuring and alloying in Cu-based catalysts on the activity and selectivity of CO2 reduction to generate the following one-carbon products: carbon monoxide (CO), formic acid (HCOOH), formaldehyde (H2C=O), methanol (CH3OH) and methane (CH4). The structures and energetics were determined for the adsorption, activation, and conversion of CO2 on monometallic and bimetallic (decorated and core@shell) 55-atom Cu-based clusters. The dopant metals considered were Ag, Cd, Pd, Pt, and Zn, located at different coordination sites. The relative binding strength of the intermediates were used to identify the optimal catalyst for the selective CO2 conversion to one-carbon products. It was discovered that single atom Cd or Zn doping is optimal for the conversion of CO2 to CO. The core@shell models with Ag, Pd and Pt provided higher selectivity for formic acid and formaldehyde. The Cu-Pt and Cu-Pd showed lowest overpotential for methane formation. Full article
(This article belongs to the Special Issue Nanocatalysts for Methanation Reaction)
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Review

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27 pages, 4374 KiB  
Review
Recent Application of Core-Shell Nanostructured Catalysts for CO2 Thermocatalytic Conversion Processes
by Nisa Afiqah Rusdan, Sharifah Najiha Timmiati, Wan Nor Roslam Wan Isahak, Zahira Yaakob, Kean Long Lim and Dalilah Khaidar
Nanomaterials 2022, 12(21), 3877; https://doi.org/10.3390/nano12213877 - 02 Nov 2022
Cited by 7 | Viewed by 2909
Abstract
Carbon-intensive industries must deem carbon capture, utilization, and storage initiatives to mitigate rising CO2 concentration by 2050. A 45% national reduction in CO2 emissions has been projected by government to realize net zero carbon in 2030. CO2 utilization is the [...] Read more.
Carbon-intensive industries must deem carbon capture, utilization, and storage initiatives to mitigate rising CO2 concentration by 2050. A 45% national reduction in CO2 emissions has been projected by government to realize net zero carbon in 2030. CO2 utilization is the prominent solution to curb not only CO2 but other greenhouse gases, such as methane, on a large scale. For decades, thermocatalytic CO2 conversions into clean fuels and specialty chemicals through catalytic CO2 hydrogenation and CO2 reforming using green hydrogen and pure methane sources have been under scrutiny. However, these processes are still immature for industrial applications because of their thermodynamic and kinetic limitations caused by rapid catalyst deactivation due to fouling, sintering, and poisoning under harsh conditions. Therefore, a key research focus on thermocatalytic CO2 conversion is to develop high-performance and selective catalysts even at low temperatures while suppressing side reactions. Conventional catalysts suffer from a lack of precise structural control, which is detrimental toward selectivity, activity, and stability. Core-shell is a recently emerged nanomaterial that offers confinement effect to preserve multiple functionalities from sintering in CO2 conversions. Substantial progress has been achieved to implement core-shell in direct or indirect thermocatalytic CO2 reactions, such as methanation, methanol synthesis, Fischer–Tropsch synthesis, and dry reforming methane. However, cost-effective and simple synthesis methods and feasible mechanisms on core-shell catalysts remain to be developed. This review provides insights into recent works on core-shell catalysts for thermocatalytic CO2 conversion into syngas and fuels Full article
(This article belongs to the Special Issue Nanocatalysts for Methanation Reaction)
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