Ambient methane functionalization initiated by electrochemical oxidation of a vanadium (V)-oxo dimer.
basic_science · Level V
Where this comes from
- Record sourced from PubMed, PMID 32703955.
- Also identified by DOI 10.1038/s41467-020-17494-w and PMC identifier 7378254.
- 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
The abundant yet widely distributed methane resources require efficient conversion of methane into liquid chemicals, whereas an ambient selective process with minimal infrastructure support remains to be demonstrated. Here we report selective electrochemical oxidation of CH<sub>4</sub> to methyl bisulfate (CH<sub>3</sub>OSO<sub>3</sub>H) at ambient pressure and room temperature with a molecular catalyst of vanadium (V)-oxo dimer. This water-tolerant, earth-abundant catalyst possesses a low activation energy (10.8 kcal mol<sup>‒1</sup>) and a high turnover frequency (483 and 1336 hr<sup>-1</sup> at 1-bar and 3-bar pure CH<sub>4</sub>, respectively). The catalytic system electrochemically converts natural gas mixture into liquid products under ambient conditions over 240 h with a Faradaic efficiency of 90% and turnover numbers exceeding 100,000. This tentatively proposed mechanism is applicable to other d<sup>0</sup> early transition metal species and represents a new scalable approach that helps mitigate the flaring or direct emission of natural gas at remote locations.