Identifying key mononuclear Fe species for low-temperature methane oxidation

Tao Yu, Zhi Li, Wilm Jones, Yuanshuai Liu, Qian He, Weiyu Song, Pengfei Du, Bing Yang, Hongyu An, Daniela M. Farmer, Chengwu Qiu, Aiqin Wang, Bert M. Weckhuysen*, Andrew M. Beale, Wenhao Luo

*Corresponding author for this work

Research output: Contribution to journalArticleAcademicpeer-review

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 H2O2at 50 °C. The 0.1% Fe/ZSM-5 catalyst with dominant mononuclear Fe species possess an excellent turnover rate (TOR) of 66 molMeOHmolFe−1h−1, approximately 4 times higher compared to the state-of-the-art dimer-containing Fe/ZSM-5 catalysts. Based on a series of advancedin situspectroscopic studies and1H- and13C- 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.

Original languageEnglish
Pages (from-to)3152-3160
Number of pages9
JournalChemical Science
Volume12
Issue number9
DOIs
Publication statusPublished - 7 Mar 2021

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