Study on activity, stability limit and reaction mechanism of CO self-sustained combustion over the LaMnO3, La0.9Ce0.1MnO3 and La0.9Sr0.1MnO3 perovskite catalysts using sugar agent

Abstract

The LaMnO3, La0.9Ce0.1MnO3 and La0.9Sr0.1MnO3 catalysts are synthesized using sugar agent, and the CO self-sustained combustion is investigated, where the catalytic performance is decided by temperature with CO conversions of 10% (T10), 50% (T50), and 90% (T90). The results show that self-sustaining combustion is successfully realized on the catalyst, and the order of activity decrease is as follows: La0.9Ce0.1MnO3 (with sugar) > La0.9Sr0.1MnO3 (with sugar) > LaMnO3 (with sugar) > LaMnO3 (without sugar) > La0.9Sr0.1MnO3 (without sugar) > La0.9Ce0.1MnO3 (without sugar). Combined with the results of XPS, H2-TPR, O2-TPD and CO-TPD techniques, the excellent activity of La0.9Ce0.1MnO3 (with sugar) can be attributed to the high content of Mn4+ ions and reactive oxygen vacancies enriched on the catalyst surface, sound low-temperature reduction, and uniform dispersion. Besides, in situ IR spectroscopy results indicate that the catalytic combustion of CO over manganese-based perovskite catalysts follows the L-H mechanism: the chemisorption of CO and O2 takes place to produce monodentate carbonates and bicarbonate species, which then decompose to yield CO2 release. The high-temperature stability test provides evidence that the La0.9Ce0.1MnO3 (with sugar) gives 100% CO conversion and that the activities remain almost unchanged after reaction for 12 h, where the temperature of catalyst bed reaches about 717 °C. The results obtained are helpful to accept this technology on efficient and clean energy utilization in iron and steel industry.