High-Pressure CO$_2$ Dissociation with Nanosecond Pulsed Discharges

TL;DR

This study investigates CO$_2$ splitting into CO using nanosecond pulsed discharges at high pressure, revealing an energy efficiency of around 20% and identifying key reaction pathways affecting conversion rates.

Contribution

It provides new insights into CO$_2$ dissociation efficiency and reaction mechanisms under high-pressure nanosecond pulsed plasma conditions, with experimental data on conversion rates and efficiencies.

Findings

Energy efficiency of ~20% at high pressure

Conversion rate up to 14% with 23% efficiency

Recombination reactions reduce efficiency over time

Abstract

The efficiency of the conversion of CO$_2$ into CO with nanosecond repetitively pulsed discharges (NRP) is investigated in a high pressure batch reactor. Stable discharges are obtained at up to 12~bar. By-products of CO$_2$ splitting are measured with gas chromatography. The energy efficiency is determined for a range of processing times, pulse energy, and fill pressures. The energy efficiency is found to be approximately 20% and 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 input. A conversion rate of up to 14% is achieved with an energy efficiency of 23%. For long processing times, a drop in efficiency is observed, due to the increasing significance of recombination reactions, as described by a macroscopic kinetic mechanism. Reaction pathways that are believed to play an important role in nanosecond pulsed discharges are discussed. It appears that vibrational excitation does not play a significant role in CO$_2$ conversion in these types of short-pulse discharge. Results also draw attention to the relative importance of two particular electronic excitation reactions.