期刊
ACS CENTRAL SCIENCE
卷 5, 期 7, 页码 1179-1186出版社
AMER CHEMICAL SOC
DOI: 10.1021/acscentsci.9b00273
关键词
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资金
- Eni S.p.A. through the MIT Energy Initiative
- Sloan Foundation
- Canadian Institute for Advanced Research
- Research Corporation for Science Advancement
The direct conversion of methane to methanol would enable better utilization of abundant natural gas resources. In the presence of stoichiometric Pt-IV oxidants, Pt-II 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 Pt-IV oxidant. Herein, we establish an electrochemical strategy for continuous regeneration of the Pt-IV oxidant to furnish overall electrochemical methane oxidation. We show that Cl-adsorbed Pt electrodes catalyze facile oxidation of Pt-II to Pt-IV at low overpotential without concomitant methanol oxidation. Exploiting this facile electrochemistry, we maintain the Pt-II/IV ratio during Pt-II-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.
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