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Oxidative Methane Conversion to Ethane on Highly Oxidized Pd/CeO 2 Catalysts Below 400 °C
Author(s) -
Kwon Gihun,
Shin Dongjae,
Jeong Hojin,
Sahoo Suman Kalyan,
Lee Jaeha,
Kim Gunjoo,
Choi Juhyuk,
Kim Do Heui,
Han Jeong Woo,
Lee Hyunjoo
Publication year - 2020
Publication title -
chemsuschem
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 2.412
H-Index - 157
eISSN - 1864-564X
pISSN - 1864-5631
DOI - 10.1002/cssc.201903311
Subject(s) - oxidative coupling of methane , dehydrogenation , methane , catalysis , chemistry , density functional theory , inorganic chemistry , anaerobic oxidation of methane , atmospheric pressure , oxidative phosphorylation , photochemistry , organic chemistry , computational chemistry , biochemistry , oceanography , geology
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 (<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.