Room-Temperature Methane Conversion by Graphene-Confined Single Iron Atoms

By Xiaoju Cui, Haobo Li, Yan Wang, Yuanli Hu, Lei Hua, Haiyang Li, Xiuwen Han, Qingfei Liu, Fan Yang, Limin He and 5 more. Chem, 2018

387 citations recorded by the source corpus.

Summary Direct conversion of methane to high-value-added chemicals is a major challenge in catalysis, which usually requires high-energy input to overcome the reaction barrier. We report that graphene-confined single Fe atoms can be used as an efficient non-precious catalyst to directly convert methane to C1 oxygenated products at room temperature. A series of graphene-confined 3d transition metals (Mn, Fe, Co, Ni, and Cu) were screened, yet only single Fe atoms could catalyze the methane conversion. Combining in operando time-of-flight mass spectrometry, 13C nuclear magnetic resonance, and density functional theory calculations, we found that methane conversion proceeds on the O–FeN4–O active site along a radical pathway to produce CH3OH and CH3OOH first, and then the generated CH3OH can be further catalyzed to form HOCH2OOH and HCOOH at room temperature.

Subfields: Catalysis, Materials Chemistry

View Paper: https://www.semanticscholar.org/paper/92d147b10d78cee1fe94bc7c932e8e9ef106299d