Temporal evolution of electron energy distribution function and its correlation with hydrogen radical generation in atmospheric-pressure methane needle-plane discharge plasmas

Non-thermal plasmas show great potential in low-temperature activation of methane (CH4) owing to the abundant energetic active species. Motivated by the fact that the chemical reactions in plasma-based CH4 conversion are dominated and regulated by the energetic electrons and various radicals, the temporal evolution of the electron energy distribution function (EEDF) and its relation to hydrogen (H) radical generation in an atmospheric-pressure CH4 needle-plane discharge plasma have been investigated numerically. The simulations are carried out using one-dimensional particle-in-cell Monte-Carlo collision and fluid dynamic models. It can be shown that during the formation and development of the streamer, a characteristic time exists, before and after which the evolution characteristic of the EEDF is reversed. This is mainly attributed to the competition between the energies continuously obtained from the electric field and the increasingly strong inelastic collisions and fast-growing low-energy electron population. When the amplitude of the applied voltage is increased, the fraction of electrons with high enough energy to participate in dissociation or ionization reactions of CH4 increases, leading to an increased H density. Besides, the characteristic time decreases exponentially, and the energy efficiency of the activation of CH4 molecules is decreased. An appropriate electron energy distribution and H radical density should be chosen to ensure acceptable product selectivity and conversion rate without excessive energy consumption; this will depend on the required products. The results presented in this work provide a partial theoretical basis for effectively optimizing the content of high-energy electrons and H radicals.