A kinetic study of nonthermal plasma pyrolysis of methane: Insights into hydrogen and carbon material production

作者：Xuchu Yuan, Jintao Sun, Yichen Ma, Yaolin Wang, Bowen Liu, Yuxiang Cai, Xue Yong, Xin Tu · 发表于：Chemical Engineering Journal · 年份：2024 · DOI：10.1016/j.cej.2024.156396 · 被引用次数：22 · 研究领域：Plasma Applications and Diagnostics、Diamond and Carbon-based Materials Research、Carbon Nanotubes in Composites

• Methane pyrolysis using a gliding arc yields H 2 and valuable carbon materials. • A 0D chemical kinetics model was developed to elucidate the reaction mechanism. • The reaction pathways for carbon formation during this process were investigated. • The reaction between CH 4 and H significantly contributes to hydrogen production. • Electron-impact dissociation of C 2 H 2 greatly contributes to solid carbon formation. Nonthermal plasma-assisted methane pyrolysis has emerged as a promising approach for hydrogen production under mild conditions while simultaneously yielding valuable carbon materials. Herein, we develop a plasma chemical kinetic model to elucidate the underlying reaction mechanisms involved in methane pyrolysis to hydrogen and solid carbon within a gliding arc (GA) reactor. A zero-dimensional (0D) chemical kinetics model was developed to simulate the plasma chemistry during the GA-based methane pyrolysis process, incorporating reactions involving electrons, excited species, ions, and heavy species. The model accurately predicted methane conversion and product selectivity in agreement with the experimental data. A strong correlation between hydrogen production and methane conversion was observed, primarily driven by the reaction CH 4 + H → CH 3 + H 2, contributing 44.2% to hydrogen formation and 37.7% to methane depletion. Electron impact collisions with hydrocarbons play a secondary role, accounting for 31.1% of H 2 formation. This work provides a detailed invest...