Volume 1, 2023

ZSM-5-confined Cr1–O4 active sites boost methane direct oxidation to C1 oxygenates under mild conditions

Abstract

Direct oxidation of methane (DOM) to value-added chemicals is of great significance but is still challenging under mild conditions. Herein, we report that Cr1–O4 as an active site in a ZSM-5 anchored Cr single atom catalyst (Cr1/ZSM-5 SAC) can efficiently catalyse the DOM to form value-added C1 oxygenated products with a productivity of 21 100 μmol gcat−1 h−1 and a selectivity of 99.8% at 50 °C within 30 min, which outperforms most reported state-of-the-art catalysts. Density functional theory (DFT) calculations and experimental results show that Cr1 atoms anchored on the wall of ZSM-5 micropores form the Cr1–O4 active sites, which boosts the formation of the reactive oxygen species (adsorbed OH species) and the activation of a C–H bond in CH4. We believe that our atomic-level design strategy on a non-noble metal offers an approach to rationally design efficient catalysts for methane conversion.

Graphical abstract: ZSM-5-confined Cr1–O4 active sites boost methane direct oxidation to C1 oxygenates under mild conditions

Supplementary files

Article information

Article type
Paper
Submitted
28 10月 2022
Accepted
28 11月 2022
First published
28 11月 2022
This article is Open Access
Creative Commons BY-NC license

EES. Catal., 2023,1, 153-161

ZSM-5-confined Cr1–O4 active sites boost methane direct oxidation to C1 oxygenates under mild conditions

M. Zeng, L. Cheng, Q. Gu, B. Yang, B. Yu, J. Xu, Y. Zhang, C. Pan, X. Cao, Y. Lou and Y. Zhu, EES. Catal., 2023, 1, 153 DOI: 10.1039/D2EY00080F

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