The research on CO oxidation over Ce-Mn oxides: The preparation method effects and oxidation mechanism

Abstract

A series of CeO₂-MnO_x for highly efficient catalytical oxidation of carbon monoxide were prepared by citrate sol-gel (C), hydrothermal (H) and hydrothermal-citrate complexation (CH) methods. The outcome indicates that the catalyst generated using the CH technique (CH-1:8) demonstrated the greatest catalytic performance for CO oxidation with a T₅₀ of 98 °C, and also good stability in 1400 min. Compared to the catalysts prepared by C and H method, CH-1:8 has the highest specific surface of 156.1 m² g^-1, and the better reducibility of CH-1:8 was also observed in CO-TPR. It is also observed the high ratio of adsorbed oxygen/lattice oxygen (1.5) in the XPS result. Moreover, characterizations by the TOF-SIMS method indicated that obtained catalyst CH-Ce/Mn = 1:8 had stronger interactions between Ce and Mn oxides, and the redox cycle of Mn³⁺+Ce⁴⁺ ↔ Mn⁴⁺+Ce³⁺ was a key process for CO adsorption and oxidation process. According to in-situ FTIR, the possible reaction pathway for CO was deduced in three ways. CO directly oxidize with O₂ to CO₂, CO adsorbed on Mn⁴⁺ and Ce³⁺ reacts with O to form intermediates (COO^-) (T > 50 °C) and carbonates (T > 90 °C), which are further oxidized into CO₂.

Keywords: CO oxidation; Ce–Mn redox Cycle; Hydrothermal-citrate complexation (CH); In-situ characterization.