Plasmachemical and heterogeneous processes in ozonizers with oxygen activation by a dielectric barrier discharge

Abstract

Plasmachemical and heterogeneous processes of generation and loss of ozone in the atmosphericpressure dielectric barrier discharge in oxygen are studied theoretically. Plasmachemical and electronic kinetics in the stage of development and decay of a single plasma filament (microdischarge) are calculated numerically with and without allowance for the effects of ozone vibrational excitation and high initial ozone concentration. The developed analytical approach is applied to determine the output ozone concentration taking into account ozone heterogeneous losses on the Al₂O₃ dielectric surface. Using the results of quantummechanical calculations by the method of density functional theory, a multistage catalytic mechanism of heterogeneous ozone loss based on the initial passivation of a pure Al₂O₃ surface by ozone and the subsequent interaction of O₃ molecules with the passivated surface is proposed. It is shown that the conversion reaction 2O₃ → 3O₂ of a gas-phase ozone molecule with a physically adsorbed ozone molecule can result in the saturation of the maximum achievable ozone concentration at high specific energy depositions, the nonstationarity of the output ozone concentration, and its dependence on the prehistory of ozonizer operation.