Electro-assisted methane oxidation to formic acid via in-situ cathodically generated H<sub>2</sub>O<sub>2</sub> under ambient conditions.
basic_science · Level V
Where this comes from
- Record sourced from PubMed, PMID 37543676.
- Also identified by DOI 10.1038/s41467-023-40415-6 and PMC identifier 10404228.
- Licence recorded as CC BY.
- The licence permits redistribution, so the abstract is shown in full and the full text is available from the publisher.
Abstract
Direct partial oxidation of methane to liquid oxygenates has been regarded as a potential route to valorize methane. However, CH4 activation usually requires a high temperature and pressure, which lowers the feasibility of the reaction. Here, we propose an electro-assisted approach for the partial oxidation of methane, using in-situ cathodically generated reactive oxygen species, at ambient temperature and pressure. Upon using acid-treated carbon as the electrocatalyst, the electro-assisted system enables the partial oxidation of methane in an acidic electrolyte to produce oxygenated liquid products. We also demonstrate a high production rate of oxygenates (18.9 μmol h-1) with selective HCOOH production. Mechanistic analysis reveals that reactive oxygen species such as ∙OH and ∙OOH radicals are produced and activate CH4 and CH3OH. In addition, unstable CH3OOH generated from methane partial oxidation can be additionally reduced to CH3OH on the cathode, and so-produced CH3OH is further oxidized to HCOOH, allowing selective methane partial oxidation.