Abstract
Deoxygen is a crucial step for landfill gas (LFG) recycling and purification. Pt/γ-Al2O3 is the most active catalyst for LFG deoxygen via catalytic methane oxidation. It is challenging but significant to further improve the performance of this type of catalyst. In regard of homogeneous and heterogeneous activation of methane by superacids, here we demonstrate LFG deoxygen via catalytic methane oxidation using a solid superacid catalyst, Pt/SO42-/Al2O3, synthesized using pre-sulfated γ-Al2O3 support by impregnated with sulfuric acid. In comparison to Pt/γ-Al2O3, Pt/SO42-/Al2O3 catalysts exhibit exceptionally improved activity and minimum complete O2 conversion at a temperature of 264 ℃, a decrease of about 51 ℃. This value is superior to the state-of-the-art Pt-based deoxygen catalysts. Characterizations and theoretical calculations indicate that sulfation enhances the amount of acid sites on γ-Al2O3 support and induces electron deficiency of the supported Pt species (+0.28|e|), thus boosting the low-temperature activity. Furthermore, the Pt/SO42-/Al2O3 catalyst maintained its initial activity after six runs without any detectable coke deposition. This discovery offers simple and effective strategies to precisely design higher performance application-oriented Pt based deoxygen catalysts.
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