Facile fabrication of three-dimensional MnO2 for trichloroethylene degradation by plasma catalysis

Abstract

Non-thermal plasma (NTP) coupled with catalyst is a cutting-edge technique for the abatement of chlorinated volatile organic compounds (Cl-VOCs), which are typically chemically stable, highly toxic and non-biodegradable. In this study, different morphologies of 3D MnO2 catalysts were fabricated facilely through a hydrothermal method and coupled with NTP for trichloroethylene (TCE) degradation. Among the various catalysts tested, MnO2 IV exhibited the highest TCE degradation performance, with removal efficiency, mineralization and energy yield ranging from 44.3% to 94.8%, 28.9% to 90.1% and 5.76 to 2.31 g/kWh, respectively, at voltage levels between 7 and 11 kV. The relationship between the physicochemical properties of the catalysts and their degradation performance was established through various characterization methods. The exceptional catalytic efficiency of MnO2 IV can be ascribed to its hierarchical flower-like structure, the greatest specific surface area (120 m2/g), the weakest Mn-O bonds, increased lattice defects and oxygen vacancies, and lower H2 reduction temperature. These characteristics facilitate enhanced transfer, adsorption, and utilization of reactive oxygen species in NTP on the surface of MnO2 IV, promoting the deep oxidation of TCE. The optimization of operational parameters was achieved using response surface methodology, with results indicating that the applied voltage exerted the greatest influence on both the mineralization rate and energy yield. The optimal operating conditions were determined, with initial TCE concentration, applied voltage, and gas flow rate values identified as 393 ppm, 7.3 kV, and 0.83 L/min, respectively. Lastly, the TCE degradation mechanism in the NTP-MnO2 catalyst system was hypothesized based on the identification of various plasma reactive species and organic intermediates. This study provides new insights for the improvement of the VOCs oxidation performance in plasma catalytic system.