Methane (CH<sub>4</sub>), the major component of natural gas, is a clean and important energy source. Direct conversion of methane to an easier-to-handle fuel, such as methanol, is both technically and economically viable. Recently, Ikuno et al. [J. Am. Chem. Soc. 139, 30, 10294-10301] synthesized a Cu-NU-1000 catalyst by deposition of Cu-oxo clusters on the nodes of the metal–organic framework NU-1000 and showed that it can catalyze the conversion of methane to methanol with a carbon selectivity of 45–60% at 150 °C. The structure of the synthesized Cu-NU-1000 prior to activation was identified by experimental and theoretical work. In the present work, we apply density functional theory to study the structures of Cu-NU-1000 catalysts after activation by O<sub>2</sub>, and we use a thermodynamic analysis to study the stabilities of these structures as functions of temperature and pressure. We investigate various reaction pathways on different catalyst structures to identify the most active sites for the selective oxidation of methane to methanol. The goal is to elucidate the mechanism of the catalytic reaction and provide guidance for the synthesis of catalysts and the optimization of reaction conditions.

Computational study of the stability and catalytic activity of a copper-oxo cluster supported on the NU-1000 metal–organic framework for methane oxidation to methanol

2019 Spring National Meeting

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