Electro-assisted methane oxidation to formic acid via in-situ cathodically generated H2O2 under ambient conditions

Jiwon Kim, Jae Hyung Kim, Cheoulwoo Oh, Hyewon Yun, Eunchong Lee, Hyung-Suk Oh, Jong Hyeok Park () and Yun Jeong Hwang ()
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Jiwon Kim: Yonsei University
Jae Hyung Kim: Korea Institute of Energy Research
Cheoulwoo Oh: Yonsei University
Hyewon Yun: Seoul National University
Eunchong Lee: Seoul National University
Hyung-Suk Oh: Korea Institute of Science and Technology
Jong Hyeok Park: Yonsei University
Yun Jeong Hwang: Seoul National University

Nature Communications, 2023, vol. 14, issue 1, 1-10

Abstract: 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.

Date: 2023
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DOI: 10.1038/s41467-023-40415-6

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