Aqueous-Phase Partial Oxidation of Methane over Pd−Fe/ZSM-5 with O2 in the Presence of H2

Abstract

The selective oxidation of methane into methane oxygenates such as CH3OH and HCOOH with O2 is a promising technology for direct methane conversion. This study successfully demonstrates the partial oxidation of methane over Pd−Fe/ZSM-5 catalysts in water, where H2O2 was generated in situ from H2 and O2. A low Pd content is essential for preventing agglomeration of Pd nanoparticles, and intimate contact between Pd and Fe species is beneficial for achieving high yields of methane oxygenates. This one-body catalyst showed better catalytic performance than that of previously reported ones, especially at low temperatures. 0.28 %Pd–0.56 %Fe/ZSM-5 exhibited a stable catalytic performance in a continuous flow reactor.