Electrochemical Reoxidation Enables Continuous Methane-to-Methanol Catalysis with Aqueous Pt Salts
Name
acscentsci.9b00273.pdf
Description
Published version
Size
1.3 MB
Format
Adobe PDF
Checksum (MD5)
a4ea86c74d2a80a703b16e13fa09859f
Author(s)
Kim, R. Soyoung
Surendranath, Yogesh
Date Issued
June 2019
Journal
ACS central science
Publisher
American Chemical Society (ACS)
Citation
Kim. R. Soyoung and Yogesh Surendranath. “Electrochemical Reoxidation Enables Continuous Methane-to-Methanol Catalysis with Aqueous Pt Salts.” ACS central science 5 (2019): 1179-1186 © 2019 The Author(s)
Version
Final published version
Abstract
The direct conversion of methane to methanol would enable better utilization of abundant natural gas resources. In the presence of stoichiometric PtIV oxidants, PtII ions are capable of catalyzing this reaction in aqueous solutions at modest temperatures. Practical implementation of this chemistry requires a viable strategy for replacing or regenerating the expensive PtIV oxidant. Herein, we establish an electrochemical strategy for continuous regeneration of the PtIV oxidant to furnish overall electrochemical methane oxidation. We show that Cl-adsorbed Pt electrodes catalyze facile oxidation of PtII to PtIV at low overpotential without concomitant methanol oxidation. Exploiting this facile electrochemistry, we maintain the PtII/IV ratio during PtII-catalyzed methane oxidation via in situ monitoring of the solution potential coupled with dynamic modulation of the electric current. This approach leads to sustained methane oxidation catalysis with 70% selectivity for methanol.
MIT Department
Massachusetts Institute of Technology. Department of Chemistry
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Article is made available in accordance with the publisher's policy and may be subject to US copyright law. Please refer to the publisher's site for terms of use.
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DOI of Published Version
https://doi.org/10.1021/ACSCENTSCI.9B00273
