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Oxidative Methane Conversion to Ethane on Highly Oxidized Pd/CeO<sub>2</sub> Catalysts Below 400 °C

Gihun Kwon, Dongjae Shin, Hojin Jeong, Suman Kalyan Sahoo, Jaeha Lee, Gunjoo Kim, Juhyuk Choi, Do Heui Kim, Jeong Woo Han, Hyunjoo Lee

2020ChemSusChem17 citationsDOI

Abstract

Abstract Methane upgrading into more valuable chemicals has received much attention. Herein, we report oxidative methane conversion to ethane using gaseous O 2 at low temperatures (&lt;400 °C) and atmospheric pressure in a continuous reactor. A highly oxidized Pd deposited on ceria could produce ethane with a productivity as high as 0.84 mmol g cat −1 h −1 . The Pd−O−Pd sites, not Pd−O−Ce, were the active sites for the selective ethane production at low temperatures. Density functional theory calculations confirmed that the Pd−O−Pd site is energetically more advantageous for C−C coupling, whereas Pd−O−Ce promotes CH 4 dehydrogenation. The ceria helped Pd maintain a highly oxidic state despite reductive CH 4 flow. This work can provide new insight for methane upgrading into C 2 species.

Topics & Concepts

CatalysisMethaneChemistryOxidative phosphorylationOxidative coupling of methaneInorganic chemistryAnaerobic oxidation of methaneMaterials sciencePhotochemistryChemical engineeringOrganic chemistryEngineeringBiochemistryCatalytic Processes in Materials ScienceCatalysis and Oxidation ReactionsCatalysts for Methane Reforming
Oxidative Methane Conversion to Ethane on Highly Oxidized Pd/CeO<sub>2</sub> Catalysts Below 400 °C | Litcius