Cold Plasma Synthesis and Testing of NiO<sub>X</sub>-Based Thin-Film Catalysts for CO<sub>2</sub> Methanation
An essential problem in managing CO<sub>2</sub> and transforming it into methane as a useful fuel is the quest for adequately efficient and cheap catalysts. Another condition is imposed by the new designs of structured reactors, which require catalysts in the form of the thinnest possibl...
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2021-07-01
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author | Martyna Smolarek Hanna Kierzkowska-Pawlak Ryszard Kapica Maciej Fronczak Maciej Sitarz Magdalena Leśniak Jacek Tyczkowski |
author_facet | Martyna Smolarek Hanna Kierzkowska-Pawlak Ryszard Kapica Maciej Fronczak Maciej Sitarz Magdalena Leśniak Jacek Tyczkowski |
author_sort | Martyna Smolarek |
collection | DOAJ |
description | An essential problem in managing CO<sub>2</sub> and transforming it into methane as a useful fuel is the quest for adequately efficient and cheap catalysts. Another condition is imposed by the new designs of structured reactors, which require catalysts in the form of the thinnest possible films. The aim of this work was to produce Ni-based thin-film catalysts by the cold plasma deposition method (PECVD) from a volatile metal complex (Ni(CO)<sub>4</sub>) and to study their structure and catalytic properties in the CO<sub>2</sub> methanation process. We tested three basic types of films: as-deposited, calcined in Ar, and calcined in air. The nanostructure and molecular structure of the films were investigated by electron microscopy (SEM), X-ray diffraction (XRD), and X-ray photoelectron spectroscopy (XPS). The catalytic activity was evaluated in the methanation process (CO<sub>2</sub> + H<sub>2</sub>), which was performed in a tubular reactor operating in the temperature range of 300–400 °C. The films calcined in air showed the highest activity in this process but behaved unstably. However, their regeneration by recalcination in air restored the initial catalytic activity. An important conclusion emerged from the obtained results, namely that the active phase in the tested films is Ni<sup>3+</sup> (most likely in the form of Ni<sub>2</sub>O<sub>3</sub>), contrary to the common opinion that this phase is metallic Ni<sup>0</sup>. In our case, Ni<sup>0</sup> quenches the catalytic activity. |
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spelling | doaj.art-df6f95a3db53488ca4fb6569a62fac582023-11-22T07:06:31ZengMDPI AGCatalysts2073-43442021-07-0111890510.3390/catal11080905Cold Plasma Synthesis and Testing of NiO<sub>X</sub>-Based Thin-Film Catalysts for CO<sub>2</sub> MethanationMartyna Smolarek0Hanna Kierzkowska-Pawlak1Ryszard Kapica2Maciej Fronczak3Maciej Sitarz4Magdalena Leśniak5Jacek Tyczkowski6Department of Molecular Engineering, Faculty of Process and Environmental Engineering, Lodz University of Technology, Wolczanska 213, 90-924 Lodz, PolandDepartment of Molecular Engineering, Faculty of Process and Environmental Engineering, Lodz University of Technology, Wolczanska 213, 90-924 Lodz, PolandDepartment of Molecular Engineering, Faculty of Process and Environmental Engineering, Lodz University of Technology, Wolczanska 213, 90-924 Lodz, PolandDepartment of Molecular Engineering, Faculty of Process and Environmental Engineering, Lodz University of Technology, Wolczanska 213, 90-924 Lodz, PolandDepartment of Silicates and Macromolecular Compounds, Faculty of Materials Science and Ceramics, AGH University of Science and Technology, 30-059 Kraków, PolandDepartment of Silicates and Macromolecular Compounds, Faculty of Materials Science and Ceramics, AGH University of Science and Technology, 30-059 Kraków, PolandDepartment of Molecular Engineering, Faculty of Process and Environmental Engineering, Lodz University of Technology, Wolczanska 213, 90-924 Lodz, PolandAn essential problem in managing CO<sub>2</sub> and transforming it into methane as a useful fuel is the quest for adequately efficient and cheap catalysts. Another condition is imposed by the new designs of structured reactors, which require catalysts in the form of the thinnest possible films. The aim of this work was to produce Ni-based thin-film catalysts by the cold plasma deposition method (PECVD) from a volatile metal complex (Ni(CO)<sub>4</sub>) and to study their structure and catalytic properties in the CO<sub>2</sub> methanation process. We tested three basic types of films: as-deposited, calcined in Ar, and calcined in air. The nanostructure and molecular structure of the films were investigated by electron microscopy (SEM), X-ray diffraction (XRD), and X-ray photoelectron spectroscopy (XPS). The catalytic activity was evaluated in the methanation process (CO<sub>2</sub> + H<sub>2</sub>), which was performed in a tubular reactor operating in the temperature range of 300–400 °C. The films calcined in air showed the highest activity in this process but behaved unstably. However, their regeneration by recalcination in air restored the initial catalytic activity. An important conclusion emerged from the obtained results, namely that the active phase in the tested films is Ni<sup>3+</sup> (most likely in the form of Ni<sub>2</sub>O<sub>3</sub>), contrary to the common opinion that this phase is metallic Ni<sup>0</sup>. In our case, Ni<sup>0</sup> quenches the catalytic activity.https://www.mdpi.com/2073-4344/11/8/905Ni-based catalyststhin-film nanocatalystscold plasma deposition (PECVD)CO<sub>2</sub> methanationnickel oxides |
spellingShingle | Martyna Smolarek Hanna Kierzkowska-Pawlak Ryszard Kapica Maciej Fronczak Maciej Sitarz Magdalena Leśniak Jacek Tyczkowski Cold Plasma Synthesis and Testing of NiO<sub>X</sub>-Based Thin-Film Catalysts for CO<sub>2</sub> Methanation Catalysts Ni-based catalysts thin-film nanocatalysts cold plasma deposition (PECVD) CO<sub>2</sub> methanation nickel oxides |
title | Cold Plasma Synthesis and Testing of NiO<sub>X</sub>-Based Thin-Film Catalysts for CO<sub>2</sub> Methanation |
title_full | Cold Plasma Synthesis and Testing of NiO<sub>X</sub>-Based Thin-Film Catalysts for CO<sub>2</sub> Methanation |
title_fullStr | Cold Plasma Synthesis and Testing of NiO<sub>X</sub>-Based Thin-Film Catalysts for CO<sub>2</sub> Methanation |
title_full_unstemmed | Cold Plasma Synthesis and Testing of NiO<sub>X</sub>-Based Thin-Film Catalysts for CO<sub>2</sub> Methanation |
title_short | Cold Plasma Synthesis and Testing of NiO<sub>X</sub>-Based Thin-Film Catalysts for CO<sub>2</sub> Methanation |
title_sort | cold plasma synthesis and testing of nio sub x sub based thin film catalysts for co sub 2 sub methanation |
topic | Ni-based catalysts thin-film nanocatalysts cold plasma deposition (PECVD) CO<sub>2</sub> methanation nickel oxides |
url | https://www.mdpi.com/2073-4344/11/8/905 |
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