Affiliation:
1. School of Environmental Science and Engineering Changzhou University Changzhou 213164 P. R. China
2. School of Petrochemical Engineering Changzhou University Changzhou 213164 P. R. China
3. Key Laboratory of Advanced Plasma Catalysis Engineering for China Petrochemical Industry Changzhou 213164 P. R. China
4. School of Safety Science and Engineering Changzhou University Changzhou 213164 P. R. China
Abstract
AbstractCeO2/γ‐Al2O3, Pd/CeO2, and Pd/CeO2/γ‐Al2O3 were used for catalyzing low‐concentration CH4 oxidation. It was found that nano‐sized Pd could obviously promote CH4 oxidation on CeO2/γ‐Al2O3. The interaction between Pd and CeO2 on γ‐Al2O3 resulted in higher ratios of Ce3+/(Ce3++Ce4+), Pd2+/(Pd2++Pdδ+), and Oads/(Oads+Olatt), those benefited the formation of more oxygen vacancies and surface reactive oxygen species for CH4 oxidation. γ‐Al2O3 not only supplied a high surface area and enhanced Pd/CeO2 dispersion on γ‐Al2O3, but also simulated the formation of bicarbonate, where bicarbonate is easier to gasify to CO2 than bidentate carbonate that formed on Pd/CeO2. Operando diffuse reflectance infrared Fourier transform spectroscopy‐mass spectrometer analysis results showed that CH4 oxidation could occur at a temperature as low as 180 °C due to the reaction with surface reactive OH, this reaction was also accompanied by the formation of bicarbonate. The mechanism of CH4 oxidation promoted by bicarbonate formation on γ‐Al2O3 was proposed.
Funder
National Natural Science Foundation of China
Government of Jiangsu Province
Subject
Inorganic Chemistry,Organic Chemistry,Physical and Theoretical Chemistry,Catalysis
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