The aerobic, selective oxidation of methane to C -oxygenates remains a challenge, due to the more facile, consecutive oxidation of formed products to CO . Here, we report on the aerobic selective oxidation of methane under continuous flow conditions, over platinum-based catalysts yielding formaldehyde with a high selectivity (reaching 90 % for Pt/TiO and 65 % over Pt/Al O ) upon co-feeding water. The presence of liquid water under reaction conditions increases the activity strongly attaining a methane conversion of 1-3 % over Pt/TiO . Density-functional theory (DFT) calculations show that the preferential formation of formaldehyde is linked to the stability of the di-σ-hydroxy-methoxy species on platinum, the preferred carbon-containing species on Pt(111) at a high chemical potential of water. Our findings provide novel insights into the reaction pathway for the Pt-catalysed, aerobic selective oxidation of CH .
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| http://www.ncbi.nlm.nih.gov/pmc/articles/PMC9541881 | PMC |
| http://dx.doi.org/10.1002/anie.202206841 | DOI Listing |
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