Oxidative Methane Conversion to Ethane on Highly Oxidized Pd/CeO2 Catalysts Below 400 °C. Issue 4 (30th January 2020)

• Record Type: Journal Article
• Authors: Kwon, Gihun; Shin, Dongjae; Jeong, Hojin; Sahoo, Suman Kalyan; Lee, Jaeha; Kim, Gunjoo; Choi, Juhyuk; Kim, Do Heui; Han, Jeong Woo; Lee, Hyunjoo
• Is Part Of: ChemSusChem. Volume 13:Issue 4(2020)
• Page Start: 677
• Page End: 681
• Publication Date: 2020-01-30
• Subjects: ethane -- heterogeneous catalysis -- methane -- oxidation -- PdO; Green chemistry -- Periodicals; Sustainable engineering -- Periodicals; Chemistry -- Periodicals; Chemical engineering -- Periodicals; 660
• DOI: 10.1002/cssc.201903311
• Languages: English
• ISSNs: 1864-5631

Abstract

Abstract: Methane upgrading into more valuable chemicals has received much attention. Herein, we report oxidative methane conversion to ethane using gaseous O2 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 gcat −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 CH4 dehydrogenation. The ceria helped Pd maintain a highly oxidic state despite reductive CH4 flow. This work can provide new insight for methane upgrading into C2 species. Abstract : Continuous methane upgrading : A highly oxidized Pd deposited on ceria can oxidize methane directly to ethane in a stable manner using gaseous O2 below 400 °C. The Pd−O−Pd sites, not Pd−O−Ce, enables the oxidative methane coupling.