Soluble methane monooxygenases (sMMO) enable the biological conversion of methane to methanol. Nature’s ability to directly affect this conversion under ambient conditions is a subject of great interest in energy research, particularly for the economic utilization of natural gas. To enable this conversion, biology employs a dinculear iron active site, in which the key intermediate, known as “Q”, is able to directly cleave the strong non-polar C–H bonds of methane. The nature of Q has been the subject of intense research for more than two decades, with arguments made for both “open” or “closed” Fe2O2 core confirmation. Most recently, resonance Raman studies have argued that Q is best described as a symmetric closed diamond core structure. However, additional spectroscopic evidence is desirable in order to corroborate this finding. Recently, we have utilized high energy resolution fluorescence detected x-ray absorption spectroscopy (HERFD XAS) to study MMO-Q and related model complexes. The results of these studies are correlated with time-dependent density functional (TDDFT) calculations of the HERFD XAS pre-edge features. The implications of these results for the electronic and geometric structure of MMO-Q will be discussed.

High resolution x-ray spectroscopic studies of soluble methane monooxygenase

253rd National Meeting (2017)

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