Investigation of highly efficient CO₂ hydrogenation at ambient conditions using dielectric barrier discharge plasma

Abstract

The increasing utilization of CO₂ for synthesizing high-value fuels or essential chemicals is a potentially effective approach to mitigating global warming and climate change. Compared to thermal catalytic CO₂ conversion under harsh operating conditions (400∼500°C, 10 MPa), non-thermal plasma can overcome kinetic barriers and trigger reactions beyond thermal equilibrium at ambient temperature and pressure. In this study, the effects of operating conditions (discharge frequency, input power, and gas flow rate) and geometrical parameters (discharge length, discharge gap, and dielectric materials) have been extensively analyzed using typical cylindrical dielectric barrier discharge (DBD) plasma. The discharge characteristics changed by operating conditions (including waveforms of applied voltage and current) are compared, indicating higher applied voltage and lower gas flow rate can strengthen the filamentary discharges. The results demonstrate CO₂ conversion rate increases with the increase of applied voltage and the decrease of CO₂/H₂ ratio, achieving its maximum value of 43.0% at 20 mL/min. The highest energy efficiency of 3771.9 μg/kJ for CO generation is obtained at the applied voltage of 5.5 kV and gas flow rate of 40 mL/min, respectively. Besides, the structure of plasma reactor also impacts the performance of CO₂ conversion. On the one hand, the discharge gap has a significant role in the variation of CO₂ conversion and product selectivity, which is attributed to the electric field density and corresponding electron-induced reaction. On the other hand, the circulating water-cooling jacket was used to find out the influence of reaction temperature, which switched the product from CO to CH₄. This work will pave the way for a sustainable alternative towards future CO₂ conversion and utilization.

Keywords

CO₂ hydrogenation / Dielectric barrier discharge (DBD) plasma / Nonthermal equilibrium / CO₂ utilization / Ambient conditions

CRediT authorship contribution statement

Zhihao Zeng: Formal analysis, Investigation, Methodology, Writing - original draft. Yujiao Li: Data curation, Formal analysis, Investigation, Supervision, Writing - review & editing. Yunfei Ma: Investigation, Methodology. Xiaoqing Lin: Supervision. Xiangbo Zou: Methodology. Hao Zhang: Validation. Xiaodong Li: Supervision. Qingyang Lin: Supervision. Ming-Liang Qu: Investigation. Angjian Wu: Project administration, Resources, Supervision, Validation.

Declaration of competing interest

The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper.

Acknowledgements

This work is supported by the “Pioneer” and “Leading Goose” R&D Program of Zhejiang Province (2022C03016) and the Fundamental Research Funds for the Central Universities (2022ZFJH04).

Appendix A. Supplementary data

Supplementary data to this article can be found online at https://doi.org/10.1016/j.gerr.2024.100102.