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

Author

Listed:
  • 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
    California NanoSystems Institute)

  • Chong Liu

    (University of California, Los Angeles)

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.

Suggested Citation

  • Jiao Deng & Sheng-Chih Lin & Jack Fuller & Jesus A. Iñiguez & Danlei Xiang & Di Yang & Gary Chan & Hao Ming Chen & Anastassia N. Alexandrova & Chong Liu, 2020. "Ambient methane functionalization initiated by electrochemical oxidation of a vanadium (V)-oxo dimer," Nature Communications, Nature, vol. 11(1), pages 1-10, December.
    • Handle: RePEc:nat:natcom:v:11:y:2020:i:1:d:10.1038_s41467-020-17494-w
    DOI: 10.1038/s41467-020-17494-w
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