Journal
CHEMSUSCHEM
Volume 13, Issue 4, Pages 677-681Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/cssc.201903311
Keywords
ethane; heterogeneous catalysis; methane; oxidation; PdO
Funding
- National Research Foundation of Korea [NRF-2016M3D3A1A01913255, 2018R1A2A2A05018849]
- MSIP
- POSTECH
- National Research Foundation of Korea [2018R1A2A2A05018849, 2016M3D3A1A01913255] Funding Source: Korea Institute of Science & Technology Information (KISTI), National Science & Technology Information Service (NTIS)
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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 degrees 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 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 C-2 species.
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