Issue 8, 2024

High conversion of methane to methyl ester at 298 K

Abstract

To establish an aerobic oxidation of methane to produce methanol with a high yield under ambient conditions is one of the dreams of researchers in academia and industry. However, although a lot of progress has been made on methane functionalization for several decades, it is still a great challenge to break through the selectivity-conversion limit in the aerobic oxidation of methane to methanol or methyl ester especially at room temperature. Herein, we report a simple visible-light driven reaction of CH4/O2 with CF3CO2H (HTFA) to CH3–O–COCF3 (MTFA) at 298 K, just using catalytic NaNO2 in an aqueous HCl/HTFA solution. In a batch reaction of CH4/O2 (1 : 5, 0.4 MPa), the yield of MTFA is over 90%. In a 7-day continuous experiment using CH4/O2 (2 : 1, 0.1 MPa), the MTFA selectivity and methane conversion are over 90% based on the methane input. The turnover frequency (TOF) is 2.5 molMTFA molNaNO2−1 h−1, and the turnover number (TON) is over 400. A reasonable reaction mechanism is suggested and partially confirmed by experiments, involving NOCl as a crucial species in the two-phase aerobic oxidation of methane to methyl ester. Methanol could be obtained with a commonly used hydrolysis of MTFA at 298 K. Neither metal catalysts nor special reagents are necessary in this two-step conversion of methane to methanol.

Graphical abstract: High conversion of methane to methyl ester at 298 K

Supplementary files

Article information

Article type
Paper
Submitted
12 Jan 2024
Accepted
11 Mar 2024
First published
11 Mar 2024
This article is Open Access
Creative Commons BY-NC license

Catal. Sci. Technol., 2024,14, 2244-2249

High conversion of methane to methyl ester at 298 K

L. Xu, C. Mei, M. Zhao and W. Lu, Catal. Sci. Technol., 2024, 14, 2244 DOI: 10.1039/D4CY00048J

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