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Ambient methane functionalization initiated by electrochemical oxidation of a vanadium (V)-oxo dimer.


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 CH4 to methyl bisulfate (CH3OSO3H) 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?1) and a high turnover frequency (483 and 1336?hr-1 at 1-bar and 3-bar pure CH4, 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 d0 early transition metal species and represents a new scalable approach that helps mitigate the flaring or direct emission of natural gas at remote locations.

SUBMITTER: Deng J 

PROVIDER: S-EPMC7378254 | biostudies-literature | 2020 Jul

REPOSITORIES: biostudies-literature

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Ambient methane functionalization initiated by electrochemical oxidation of a vanadium (V)-oxo dimer.

Deng Jiao J   Lin Sheng-Chih SC   Fuller Jack J   Iñiguez Jesus A JA   Xiang Danlei D   Yang Di D   Chan Gary G   Chen Hao Ming HM   Chen Hao Ming HM   Alexandrova Anastassia N AN   Liu Chong C  

Nature communications 20200723 1


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 activ  ...[more]

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