Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 144, Issue 22, Pages 9695-9706Publisher
AMER CHEMICAL SOC
DOI: 10.1021/jacs.2c01169
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Funding
- Academia Sinica [AS-GCS-107-07, AS-TP-108-ML07, AS-KPQ-106-DDPP]
- Ministry of Science and Technology, Taiwan [MOST 109-2113-M-001-003, 110-2113-M-001-038]
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This study presents a strategy for the electrocatalysis of selective methane oxidation by immobilizing tricopper catalysts on the cathodic surface. The technology achieves significant enhancements in performance of the catalysts toward methane oxidation, leading to high product throughputs and turnover frequencies. It is of great importance for the on-site direct conversion of methane into methanol.
Selective methane oxidation is difficult chemistry. Here we describe a strategy for the electrocatalysis of selective methane oxidation by immobilizing tricopper catalysts on the cathodic surface. In the presence of dioxygen and methane, the activation of these catalysts above a threshold cathodic potential can initiate the dioxygen chemistry for O atom transfer to methane. The catalytic turnover is completed by facile electron injections into the tricopper catalysts from the electrode. This technology leads to dramatic enhancements in performance of the catalysts toward methane oxidation. Unprecedented turnover frequencies (>40 min(-1)) and high product throughputs (turnover numbers >30 000 in 12 h) are achieved for this challenging chemical transformation in water under ambient conditions. The technology is green and suitable for on-site direct conversion of methane into methanol.
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