Spectroscopic Investigation of the Role of Water in Copper Zeolite Methane Oxidation.

ABSTRACT

Methane is one of the most potent greenhouse gases; developing technology for its abatement is essential for combating climate change. Copper zeolites can activate methane at low temperatures and pressures, demonstrating promise for this technology. However, a barrier to industrial implementation is the inability to recycle the Cu(II) active site. Anaerobic active site regeneration has been reported for copper-loaded mordenite, where it is proposed that water oxidizes Cu(I) formed from the methane reaction, producing H2 gas as a byproduct. However, this result has been met with skepticism given the overall reaction is thermodynamically unfavorable. In this study, we use X-ray absorption and electron paramagnetic resonance spectroscopies to study the role of water in copper zeolite methane oxidation. We find that water does not oxidize Cu(I) to Cu(II) in CH4-reacted Cu-MOR. Further, using isotope label mass spectrometry, we detail an alternate source of the hydrogen byproduct. We uncover that, although water does not oxidize Cu(I), it has the potential to facilitate low temperature methane abatement through promotion of product decomposition to carbon dioxide and H2.