Carbon dioxide valorisation with partial oxidation of methane in a water cooled DBD plasma

The valorisation of carbon dioxide in chemical plasmas implies as a principal reaction step its energy efficient dissociation into carbon monoxide. For hydrogen production, the reaction carbon monoxide with water (WGS) may lead to the generation of green hydrogen and reusable carbon dioxide. Beyond hydrogen, most valorisation processes require the removal of O 2 to avoid its recombination with CO on any downstream hot catalytic surface. Moreover, if the oxygen scavenging is performed directly inside the plasma volume, it can also shift the dissociation equilibrium that is responsible for the well-known trade-off between energy efficiency and conversion, thus improving efficiency when larger specific energy densities are applied. In this paper we first report on the plasma dissociation of pure CO 2 in a water cooled, high power(<2 kW), Dielectric Barrier Discharge with high gas flow regime (<3600sccm), and then we explore the synergistic oxygen removal by the partial oxidation of methane for syngas production. The presence of CH 4 , even in small amounts, removes oxygen from the outstream and from the discharge region, as confirmed by mass and optical emission spectroscopies, and enhances the process in two ways: it allows to feed the system with gas having a low CH 4 to CO 2 ratio (0.1–0.3) instead of pure CO 2 , where landfill and waste gases are undesired climate altering emissions with a similar composition that currently require flaring; it will allow to use directly the reactor outstream into a WGS reactor, or any other CO valorisation process without the necessity to remove downstream O 2 . • Removing oxygen from dissociated carbon dioxide is vital for downstream conversion of carbon monoxide in hydrogen by WGS. • The reaction of carbon dioxide and methane in a high-power water cooled DBD plasma system is investigated when methane is less than 1/3 of carbon dioxide • Very small methane amounts remove oxygen but also depress plasma dissociation of carbon dioxide • The plasma dissociation of carbon dioxide and the partial oxidation of methane act synergistically and may allow the electric valorisation of waste or landfill gases that are instead flared • The investigation was performed in a dielectric barrier discharge reactor that allows a plasma power above 2 kW

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Publication Details

Journal
Journal of CO2 Utilization
Published
2024-09-19
DOI
https://doi.org/10.1016/j.jcou.2024.102931
Citations
4
Primary Topic
Plasma Applications and Diagnostics
Type
article
Field-Weighted Citation Impact
1.62
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article

Carbon dioxide valorisation with partial oxidation of methane in a water cooled DBD plasma

Nicola Lisi, Umberto Pasqual Laverdura
4 citations
Journal of CO2 Utilization
Plasma Applications and Diagnostics
1.62
article

Carbon dioxide valorisation with partial oxidation of methane in a water cooled DBD plasma

Nicola Lisi, Umberto Pasqual Laverdura
article en
4 citations

Abstract

The valorisation of carbon dioxide in chemical plasmas implies as a principal reaction step its energy efficient dissociation into carbon monoxide. For hydrogen production, the reaction carbon monoxide with water (WGS) may lead to the generation of green hydrogen and reusable carbon dioxide. Beyond hydrogen, most valorisation processes require the removal of O 2 to avoid its recombination with CO on any downstream hot catalytic surface. Moreover, if the oxygen scavenging is performed directly inside the plasma volume, it can also shift the dissociation equilibrium that is responsible for the well-known trade-off between energy efficiency and conversion, thus improving efficiency when larger specific energy densities are applied. In this paper we first report on the plasma dissociation of pure CO 2 in a water cooled, high power(<2 kW), Dielectric Barrier Discharge with high gas flow regime (<3600sccm), and then we explore the synergistic oxygen removal by the partial oxidation of methane for syngas production. The presence of CH 4 , even in small amounts, removes oxygen from the outstream and from the discharge region, as confirmed by mass and optical emission spectroscopies, and enhances the process in two ways: it allows to feed the system with gas having a low CH 4 to CO 2 ratio (0.1–0.3) instead of pure CO 2 , where landfill and waste gases are undesired climate altering emissions with a similar composition that currently require flaring; it will allow to use directly the reactor outstream into a WGS reactor, or any other CO valorisation process without the necessity to remove downstream O 2 . • Removing oxygen from dissociated carbon dioxide is vital for downstream conversion of carbon monoxide in hydrogen by WGS. • The reaction of carbon dioxide and methane in a high-power water cooled DBD plasma system is investigated when methane is less than 1/3 of carbon dioxide • Very small methane amounts remove oxygen but also depress plasma dissociation of carbon dioxide • The plasma dissociation of carbon dioxide and the partial oxidation of methane act synergistically and may allow the electric valorisation of waste or landfill gases that are instead flared • The investigation was performed in a dielectric barrier discharge reactor that allows a plasma power above 2 kW

Journal of CO2 UtilizationVol. 88
National Agency for New Technologies, Energy and Sustainable Economic Development (IT)
Clean water and sanitation
Openalex Percentile: Top 16%
Plasma Applications and Diagnostics
1.62
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