Abstract
? 2022 Elsevier B.V.The direct methane (CH4) oxidation to high value-added C1 chemicals is a great promising strategy to explore the CH4 resource utilization. However, the low activity and selectivity of catalytic performance remains a great conundrum due to the difficulty to activate the C[sbnd]H bond and the unmanageable over oxidation. Herein, PdxAuy nanowires (NWs) with various Pd/Au atomic ratios are presented as ideal models to explore the atomic-level effect of PdAu atoms for the direct CH4 oxidation. The influence of reaction parameters are systematically investigated, and Pd9Au1 NWs display a maximum yield of 2890.3 μmol g?1 h?1 with 99% selectivity for the liquid C1 oxygenated products. This enhanced performance is attributed to the combination of one-dimensional structure and the synergistic effect from the suitable portion of Au on Pd sites, which regulates bond strength between adsorbed radicals (?OH, ?OOH, ?CH3) and PdAu atoms, confirmed by the density function theory calculations.
NSTL
Elsevier