Activating and Converting CH4 to CH3OH via the CuPdO2/CuO Nanointerface

The activation and conversion of methane (CH4) is one of the most challenging processes, because of the high chemical inertness of CH4 and the subsequent uncontrollable overoxidation. Herein, we report that the CuPdO2/CuO interface in PdxCu1-xO/C can efficiently activate and convert CH4 to CH3OH using H2O2 or O-2 as the oxidant under mild conditions, where the CH3OH yield (4076.5 mu mol g(-1)) and selectivity (93.9%) of the optimized Pd0.3Cu0.7O/C are much higher than those of PdO/C, CuPdO2/C, and the mixture of CuPdO2/C and CuO/C. Structural characterizations and mechanism studies reveal that the highly activity of Pd0.3Cu0.7O/C is attributed to the strong synergistic effects in PdxCu1-xO/C. The formation of Pd4+ species at the interfaces of CuPdO2 and CuO, which is promoted by the electron transfer from Cu to Pd, can selectively oxidize CH4 to produce CH3OH. This work highlights the importance of controlled interface in Pd-based catalysts for heterogeneous catalysis and beyond.