Promotion Mechanism of CaSO4 and Au in the Plasma-Assisted Catalytic Oxidation of Diesel Particulate Matter.

Abstract

Plasma-assisted catalysis has been demonstrated to be an innovative technology for eliminating diesel particulate matter (DPM) efficiently at low temperature (≤200 °C). Moreover, past studies have demonstrated that CaSO4, which exists in small concentrations (<2%) in DPM and is toxic in thermal catalytic oxidation processes, actually enhances DPM oxidation during plasma-assisted catalytic processes. However, the role CaSO4 plays in this promotion of DPM oxidation still remains unclear. The present study addresses this issue by investigating the underlying mechanisms of DPM oxidation during plasma-assisted catalytic processes using graphitic carbon as a surrogate DPM material in conjunction with CaSO4- and Au-impregnated γ-Al2O3 catalysts. The results of mass spectrometry and in situ diffuse reflectance infrared Fourier transform spectroscopy, which employs an in situ cell with a small dielectric barrier discharge space over the catalyst bed, demonstrate that CaSO4 can save and release O atoms contributing to graphite oxidation via the −S=O units of CaSO4 through a reversible surface reaction (−S=O + O → −S(−O)2). The results are employed to propose a formal mechanism of graphite oxidation catalyzed by CaSO4 and Au. These findings both improve our understanding of the plasma-assisted catalytic oxidation mechanisms of DPM and support the development of efficient plasma-assisted catalysts.