Selective anaerobic oxidation of methane enables direct synthesis of methanol

Vitaly L. Sushkevich*, Dennis Palagin, Marco Ranocchiari, Jeroen A. Van Bokhoven

*Corresponding author for this work

Research output: Contribution to journalArticleScientificpeer-review

485 Citations (Scopus)


Direct functionalization of methane in natural gas remains a key challenge. We present a direct stepwise method for converting methane into methanol with high selectivity (∼97%) over a copper-containing zeolite, based on partial oxidation with water. The activation in helium at 673 kelvin (K), followed by consecutive catalyst exposures to 7 bars of methane and then water at 473 K, consistently produced 0.204 mole of CH3OH per mole of copper in zeolite. Isotopic labeling confirmed water as the source of oxygen to regenerate the zeolite active centers and renders methanol desorption energetically favorable. On the basis of in situ x-ray absorption spectroscopy, infrared spectroscopy, and density functional theory calculations, we propose a mechanism involving methane oxidation at CuII oxide active centers, followed by CuI reoxidation by water with concurrent formation of hydrogen.

Original languageEnglish
Pages (from-to)523-527
Number of pages5
Issue number6337
Publication statusPublished - 5 May 2017
Externally publishedYes


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