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Issue 9, 2021
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Identifying key mononuclear Fe species for low-temperature methane oxidation

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Abstract

The direct functionalization of methane into platform chemicals is arguably one of the holy grails in chemistry. The actual active sites for methane activation are intensively debated. By correlating a wide variety of characterization results with catalytic performance data we have been able to identify mononuclear Fe species as the active site in the Fe/ZSM-5 zeolites for the mild oxidation of methane with H2O2 at 50 °C. The 0.1% Fe/ZSM-5 catalyst with dominant mononuclear Fe species possess an excellent turnover rate (TOR) of 66 molMeOH molFe−1 h−1, approximately 4 times higher compared to the state-of-the-art dimer-containing Fe/ZSM-5 catalysts. Based on a series of advanced in situ spectroscopic studies and 1H- and 13C- nuclear magnetic resonance (NMR), we found that methane activation initially proceeds on the Fe site of mononuclear Fe species. With the aid of adjacent Brønsted acid sites (BAS), methane can be first oxidized to CH3OOH and CH3OH, and then subsequently converted into HOCH2OOH and consecutively into HCOOH. These findings will facilitate the search towards new metal-zeolite combinations for the activation of C–H bonds in various hydrocarbons, for light alkanes and beyond.

Graphical abstract: Identifying key mononuclear Fe species for low-temperature methane oxidation

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Article information


Submitted
04 Nov 2020
Accepted
07 Jan 2021
First published
08 Jan 2021

This article is Open Access
All publication charges for this article have been paid for by the Royal Society of Chemistry

Chem. Sci., 2021,12, 3152-3160
Article type
Edge Article

Identifying key mononuclear Fe species for low-temperature methane oxidation

T. Yu, Z. Li, W. Jones, Y. Liu, Q. He, W. Song, P. Du, B. Yang, H. An, D. M. Farmer, C. Qiu, A. Wang, B. M. Weckhuysen, A. M. Beale and W. Luo, Chem. Sci., 2021, 12, 3152
DOI: 10.1039/D0SC06067D

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