期刊
CHEMICAL ENGINEERING JOURNAL
卷 405, 期 -, 页码 -出版社
ELSEVIER SCIENCE SA
DOI: 10.1016/j.cej.2020.126630
关键词
Plasma; Dielectric barrier discharge; Dry reforming of methane; Chemical equilibrium; Chemical kinetics; Partial chemical equilibrium
资金
- European Fund for Regional Development through the cross-border collaborative Interreg V program Flanders-the Netherlands (project EnOp)
- Fund for Scientific Research (FWO) [G.0254.14N]
- TOP-BOF project
- IOF-SBO (SynCO2Chem) project from the University of Antwerp
Plasma reactors are being studied for gas-based chemical conversion, with a focus on the relationship between plasma chemistry and conditions. Experiments show differences in kinetic characteristics and partial chemical equilibrium states between CO2 dissociation and CH4 reforming reactions, and how these are influenced by combining both gases in the dry reforming of methane (DRM) reaction. The addition of a packing material can also impact the conversion rate and equilibrium position, depending on the gas composition.
Plasma reactors are interesting for gas-based chemical conversion but the fundamental relation between the plasma chemistry and selected conditions remains poorly understood. Apparent kinetic parameters for the loss and formation processes of individual components of gas conversion processes, can however be extracted by performing experiments in an extended residence time range (2-75 s) and fitting the gas composition to a firstorder kinetic model of the evolution towards partial chemical equilibrium (PCE). We specifically investigated the differences in kinetic characteristics and PCE state of the CO2 dissociation and CH4 reforming reactions in a dielectric barrier discharge reactor (DBD), how these are mutually affected when combining both gases in the dry reforming of methane (DRM) reaction, and how they change when a packing material (non-porous SiO2) is added to the reactor. We find that CO2 dissociation is characterized by a comparatively high reaction rate of 0.120 s(-1) compared to CH4 reforming at 0.041 s(-1); whereas CH4 reforming reaches higher equilibrium conversions, 82% compared to 53.6% for CO2 dissociation. Combining both feed gases makes the DRM reaction to proceed at a relatively high rate (0.088 s(-1)), and high conversion (75.4%) compared to CO2 dissociation, through accessing new chemical pathways between the products of CO2 and CH4. The addition of the packing material can also distinctly influence the conversion rate and position of the equilibrium, but its precise effect depends strongly on the gas composition. Comparing different CO2:CH4 ratios reveals the delicate balance of the combined chemistry. CO2 drives the loss reactions in DRM, whereas CH4 in the mixture suppresses back reactions. As a result, our methodology provides some of the insight necessary to systematically tune the conversion process.
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