In scope of the declining oil production in the future, methane becomes an important alternative as an energy source and feedstock for the chemical industry. The usage of methane is however hampered by its high chemical inertness.This research focuses on oxygen-activated Cu-ZSM-5 which selectively oxidizes methane to methanol. The active site in copper exchanged zeolites has unique spectroscopic features reflecting novel geometric and electronic structures that are essential to the reactivity. The active oxygen core in Cu-ZSM-5 has indeed a characteristic absorption band in the UV-vis spectrum, and we unambiguously assigned it to a mono (�-oxo)dicopper core. In our recent work a new precursor to the reactive oxygen species in Cu-ZSM-5 was identified by monitoring their formation and disappearance in a combined operando UV-vis and resonance Raman study. Based on the vibrational frequencies and isotope perturbation pattern this precursor is assigned as a �-(?2:?2)peroxo dicopper(II) species.While the mechanism is not yet fully understood, we believe that the discovery of the active Cu core could serve as a new biomimetic model towards new synthetic designs, as well as a tool to better understand the working mechanism of the Cu containing MMOs.

Reactive intermediates in methane to methanol conversion over Cu containing zeolites

243rd National Meeting (2012)

The official archive and repository for all ACS Meetings & Expositions abstracts and select posters or presentations.