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

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.

SUBMITTER: Kim J

PROVIDER: S-EPMC10404228 | biostudies-literature | 2023 Aug

REPOSITORIES: biostudies-literature

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

Kim Jiwon J Kim Jae Hyung JH Oh Cheoulwoo C Yun Hyewon H Lee Eunchong E Oh Hyung-Suk HS Park Jong Hyeok JH Hwang Yun Jeong YJ

Nature communications 20230805 1

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-as ...[more]

PMID: 37543676

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Project description:Formic acid oxidation reaction (FAOR) at anode counterpart incurs at substantial high overpotential, limiting the power output efficiency of direct formic acid fuel cells (DFAFCs). Despite intense research, the lack of high-performance nanocatalysts (NCs) for FAOR remains a challenge in realizing DFAFC technologies. To surmount the overpotential losses, it is desirable to have NCs to trigger the FAOR as close to the reversible conditions (i.e. with over-potential loss as close to zero as possible). Herein, Pd-based binary and ternary NCs consisting of PdPt and PdRuPt have been synthesized via the polyol reduction method on the carbon support. As prepared PdPt and PdRuPt NCs were further subjected to heat treatment (annealed) in CO (namely PdPt-CO and PdRuPt-CO) and O2 (namely PdPt-O2 and PdRuPt-O2) atmosphere at 473 K temperature. By cross-referencing results of electron microscopy and X-ray spectroscopy together with electrochemical analysis, the effects of heat treatment under CO-reductive and O2-oxidative conditions towards FAOR were schematically elucidated. Of special relevance, the mass activity (MA) of PdPt-CO, PdPt-O2, PdRuPt-CO, and PdRuPt-O2 NCs is 1.7/2.0, 1.3/2.2, 1.1/5.5, and 0.9/4.7 Amg-1 in the anodic/cathodic scan, respectively, which is 2~4-folds improved comparative to of as-prepared PdPt (1.0/1.9 Amg-1 in anodic/cathodic scan, respectively) and PdRuPt (0.9/1.4 Amg-1 in anodic/cathodic scan, respectively) NCs. Meanwhile, after chronoamperometric (CA) stability test up to 2000 s, PdPt-CO (72 mAmg-1) and PdRuPt-CO (213 mAmg-1) NCs exhibit higher MA compared to as-prepared PdPt (54 mAmg-1) and PdRuPt (62 mAmg-1) NCs, which is attributed to the increase of surface Pt composition, especially for PdRuPt-CO NC. Besides, the stability of PdPt-O2 (15 mAmg-1) and PdRuPt-O2 (22 mAmg-1) NCs is deteriorated as compared to that of as-prepared NCs due to severe oxidation in O2 atmosphere. Of utmost importance, we developed a ternary PdRuPt catalyst with ultra-low Pt content (~2 wt.%) and significantly improved FAOR performance than pure Pt catalysts. Moreover, we demonstrated that the FAOR performance can be further enhanced by more than 30% via a unique CO annealing treatment.

Dataset Information

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

Publications

Electro-assisted methane oxidation to formic acid via in-situ cathodically generated H<sub>2</sub>O<sub>2</sub> under ambient conditions.

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