Coupling effect of reaction conditions on the catalytic activity of Cu-Mn composite oxide catalysts for toluene

Abstract

Volatile organic compounds (VOCs) are one of the major components of air pollution. Catalytic combustion is a promising technology for the treatment of VOCs and at its center is the preparation of efficient and cheap catalysts. In this study, by loading copper (Cu) and manganese (Mn) on Santa Barbara Amorphous-15 (SBA-15) molecular sieve, the Cu_x-Mn_y/SBA-15 (x = 1, 2; y = 1, 2) composite metal oxide catalyst was prepared using the equal volume impregnation method. Their performance in the toluene catalytic combustion reaction was investigated by adjusting the molar ratio (x : y), and the loading of Cu and Mn. The results of the Brunner-Emmett-Teller (BET), X-ray diffraction (XRD), scanning electron microscopy (SEM), and X-ray photoelectron spectroscopy (XPS) analyses show that the CuMnO spinel phase can be detected in the Cu-Mn composite metal oxide catalyst doped with a low concentration of Cu. The overall rod-like structure of the fibrous network structure provides a large specific surface area, and the particle crystallinity is low and the dispersion is good. Due to the synergistic effect of Cu and Mn, the greater the amount of Mn³⁺ and adsorbed oxygen species (O_ads) that are available, and the higher the turnover frequency (TOF) value, the better and more superior catalytic performance and excellent stability is obtained, when compared with the single-component oxides used in toluene catalytic combustion. After a continuous catalytic reaction for 12 h, the toluene conversion rate remained above 95%. The coupling effect of the catalytic reaction temperature and concentration of oxygen on the catalytic combustion of toluene was also studied. At a low reaction temperature (<250 °C), the increase of the concentration of oxygen played a superior role in promoting the conversion of toluene. The kinetic analysis of the toluene catalytic combustion process showed that the catalytic combustion of toluene by Cu-Mn/SBA-15 followed both the Mars-Van Krevelen (MVK) and Langmuir-Hinshelwood (L-H) reaction mechanisms. With the increase of the O_ads amount caused by the decrease of the Cu ratio, the proportion of the L-H reaction mechanism increases.