Nonthermal plasma catalysis for toluene decomposition over BaTiO3-based catalysts by Ce doping at A-sites: The role of surface-reactive oxygen species
The insights on the primary surface-reactive oxygen species and their relation with lattice defects is essential for designing catalysts for plasma-catalytic reactions. Herein, a series of Ba 1−x Ce x TiO 3 perovskite catalysts with high specific surface areas (68.6–85.6 m 2 g −1 ) were prepared by a facile in-situ Ce-doping strategy and investigated to catalytically decompose toluene. Combining the catalysts with a nonthermal plasma produced a significant synergy effect . The highest decomposition efficiency (100%), CO x selectivity (98.1%), CO 2 selectivity (63.9%), and the lowest O 3 production (0 ppm) were obtained when BC 4 T (Ce/Ti molar ratio = 4:100) was packed in a coaxial dielectric barrier discharge reactor at a specific input energy of 508.8 J L −1 . The H 2 -TPR, temperature-programmed Raman spectra , EPR and OSC results suggested that superoxides ( • O 2 − ) were the primary reactive oxygen species and were reversibly generated on the perovskite surface. Molecular O 2 was adsorbed and activated at the active sites (Ti 3+ -V O ) via an electron transfer process to form • O 2 − . Surface-adsorbed • O 2 − had a greater effect on the heterogeneous surface plasma reactions than the dielectric constant , and enhanced the toluene decomposition and intermediate oxidation . A possible reaction path of toluene decomposition was also proposed.
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