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

Jiao Deng, Sheng-Chih Lin, Jack Fuller, Jesus A. Iñiguez, Danlei Xiang, Di Yang, Gary Chan, Hao Ming Chen (), Anastassia N. Alexandrova () and Chong Liu ()
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Jiao Deng: University of California, Los Angeles
Sheng-Chih Lin: National Taiwan University
Jack Fuller: University of California, Los Angeles
Jesus A. Iñiguez: University of California, Los Angeles
Danlei Xiang: University of California, Los Angeles
Di Yang: University of California, Los Angeles
Gary Chan: University of California, Los Angeles
Hao Ming Chen: National Taiwan University
Anastassia N. Alexandrova: University of California, Los Angeles
Chong Liu: University of California, Los Angeles

Nature Communications, 2020, vol. 11, issue 1, 1-10

Abstract: 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.

Date: 2020
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DOI: 10.1038/s41467-020-17494-w

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