초록 |
Methane upgrading into more valuable chemicals has received enormous attention. In this work, we show oxidative methane conversion to ethane using gaseous O2 at low temperatures (< 400 ºC) and atmospheric pressure in a continuous reactor. A highly oxidized Pd deposited on ceria could produce ethane with the productivity as high as 0.84 mmol/gcat/h. The Pd-O-Pd sites, not Pd-O-Ce, were the active sites for selective ethane production at low temperatures. Density functional theory (DFT) calculations identified that Pd-O-Pd sites are energetically more advantageous for C-C coupling, while Pd-O-Ce prefers CH4 dehydrogenation. The ceria helped Pd maintain oxidic state in reductive CH4 flow. This work can give new insight for methane upgrading into C2 species. |