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Article Dans Une Revue Plasma Sources Science and Technology Année : 2023

High-pressure CO 2 dissociation with nanosecond pulsed discharges

Résumé

Abstract We investigate the conversion of CO 2 into CO and O 2 with nanosecond repetitively pulsed (NRP) discharges in a high-pressure batch reactor. Stable discharges are obtained at up to 12 bar. By-products are measured with gas chromatography. The energy efficiency is determined for a range of processing times, pulse energy, and fill pressures. It is only weakly sensitive to the plasma operating parameters, i.e the extent of CO 2 conversion is almost linearly-dependent on the specific energy invested. A conversion rate as high as 14% is achieved with an energy efficiency of 23%. For long processing times, saturation in the yield and a drop in efficiency are observed, due to the increasing role of three-body recombination reactions, as described by zero-dimensional detailed kinetic modeling. The modeling reveals the presence of three-stage kinetics between NRP pulses, controlled by electron-impact CO 2 dissociation, vibrational relaxation, and neutral elementary kinetics. Transport effects are shown to be important for CO 2 conversion at high pressures. For fill pressures beyond 10 bar, CO 2 may locally transit into supercritical states. The supercritical plasma kinetics may bypass atomic oxygen pathways and directly convert CO 2 into O 2 . This work provides a detailed analysis of plasma-based high-pressure CO 2 conversion, which is of great relevance to future large-scale sustainable carbon capture, utilization, and storage.

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Plasmas
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Dates et versions

hal-04563780 , version 1 (30-04-2024)

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Taemin Yong, Hongtao Zhong, Erwan Pannier, Christophe Laux, Mark Cappelli. High-pressure CO 2 dissociation with nanosecond pulsed discharges. Plasma Sources Science and Technology, 2023, 32 (11), pp.115012. ⟨10.1088/1361-6595/ad066e⟩. ⟨hal-04563780⟩
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