Influence of calcination temperature on CuO–CeO2/SiC catalysts for SO3 decomposition in the sulfur–iodine cycle for hydrogen production

Abstract

The copper-cerium composite oxides supported on silicon carbide (SiC) catalysts (CuO–CeO2/SiC) for sulfuric acid decomposition were studied in sulfur-iodine (SI or IS) cycle. The influence of calcination temperatures (800 °C–1000 °C) of CuO–CeO2/SiC catalysts on their activities and morphology were investigated in this study. The activity of CuO–CeO2/SiC was prominently higher than that of CuO–CeO2 composite oxides catalyst. The SO3 conversion ratio of CuO–CeO2/SiC catalyst increased with calcination temperature from 800 °C to 900 °C, while decreased with calcination temperature at 900 °C–1000 °C. XRD pattern, TEM (HRTEM) images and Energy Dispersive X-ray (EDX) spectra revealed that copper–cerium composite oxides were well dispersed and immobilized on the surface of SiC grains. XRD pattern showed that the accelerated transformation of SiC crystals to amorphous SiO2 and the rapid expansion of CeO2 sub-grains at the calcination temperature of 900 °C–1000 °C, as well as the accelerated amorphization of CuO crystals at 800 °C–900 °C. The agglomeration of catalysts with sintering temperature was also proven by the BET test. At a higher calcination temperature, X-ray photoelectron spectroscopy (XPS) of Cu2p spectra revealed the reduction of more Cu2+ in the process of SiC oxidation. According to TEM (HRTEM), XPS, and infrared radiation, the amorphous SiO2 was produced by the oxidation of superficial SiC particles, and the thickness of the SiO2 layers on SiC grains increased with the calcination temperature. A simple mechanism depicted the oxidation of CuO–CeO2/SiC was created.