Abstract

Because of its unique properties, plasma technology has gained much prominence in the microelectronics industry. Recently, environmental and energy applications of plasmas have gained a lot of attention. In this area, the focus is on converting CO2 and reforming hydrocarbons, with the goal of developing an efficient single-step ‘gas-to-liquid’ (GTL) process. Here we show that applying tri-reforming principles to plasma—further called ‘plasma-based multi-reforming’—allows us to better control the plasma chemistry and thus the formed products. To demonstrate this, we used chemical kinetics calculations supported by experiments and reveal that better control of the plasma chemistry can be achieved by adding O2 or H2O to a mixture containing CH4 and CO2 (diluted in N2). Moreover, by adding O2 and H2O simultaneously, we can tune the plasma chemistry even further, improving the conversions, thermal efficiency and methanol yield. Unlike thermocatalytic reforming, plasma-based reforming is capable of producing methanol in a single step; and compared with traditional plasma-based dry reforming, plasma-based multi-reforming increases the methanol yield by more than seven times and the thermal efficiency by 49%, as revealed by our model calculations. Thus, we believe that by using plasma-based multi-reforming, ‘gas-to-liquid’ conversion may be made efficient and scalable.

Highlights

  • The world needs an scalable gas reforming technology more than ever

  • We modelled a DBD operating at an Specific Energy Input (SEI) of 3 kJ/L, with a dry reforming of methane (DRM) mixture of 10% CH4 and 10% CO2 diluted in 80% N2

  • We have demonstrated that ‘plasma-based multi-reforming’ is a novel concept that can be successfully applied to improve the gas-to-liquid process

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Summary

Combining Experiments and Chemical Kinetics Calculations

To investigate the possibilities of plasma-based multi-reforming, we performed chemical kinetics calculations supported by experiments. We further explore the plasma-based multi-reforming process relying on extensive model calculations only, in which we extrapolate the validated range up to 32% O2 or H2O added, as well as for the combined addition of O2 and H2O These results should be qualitatively evaluated (rather than quantitatively) as an indication of the possibilities the addition of specific compounds has on tuning the chemistry. When H2O (or O2) is added to a CH4:CO2:N2 mixture, plasma-based multi-reforming allows us to control the chemistry to increase the yield(s) of the desired products(s) (in this case, methanol), but it allows us to achieve higher conversion rates and thermal efficiencies than standard plasma-based DRM does. It appeared that the oxidising character of O2 remains so dominant that the further enhancement of the plasma chemistry occurs only when a very small amount of O2 is added (Table 1)

Thermal efficiency
Conclusion and Outlook
Selectivity Yield
Author Contributions
Findings
Additional Information
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