Issue 6, 2023

Electronic structure regulation of halogen anion-intercalated MgAl-LDH for highly selective photothermal oxidation of CH4

Abstract

The selective oxidation of methane (CH4) into high value-added chemicals such as CO is one of the important challenges in the C1 chemical industry owing to the high bond energy of CH4 (434 kJ mol−1). Considering that Mg–O sites are the active sites for CH4 activation, we report herein the successful fabrication of a series of halogen anion-intercalated MgAl-LDHs and the as-prepared MgAl-x (x = F, Cl, Br, I) have been fully characterized by various spectroscopic studies. When applied for the photothermal oxidation of CH4, MgAl-F exhibits 86.5% selectivity for CO, while MgAl-I shows only 15.8% selectivity for CO. The O K edge XAS and XPS results show that F can significantly improve the charge density of the surface O–H bond on the MgAl-LDH laminates. In situ diffuse reflectance-infrared Fourier-transform spectroscopy (DRIFTS) demonstrates that MgAl-F can stabilize *CH3 and release *CO species during the photooxidation of CH4, which is favorable for the production of CO. DFT calculations demonstrate such a high selectivity for CO by MgAl-F can be attributed to favorable energy barriers of two key steps (*CH3 to *CH2 and *CO to *HOCO).

Graphical abstract: Electronic structure regulation of halogen anion-intercalated MgAl-LDH for highly selective photothermal oxidation of CH4

Supplementary files

Article information

Article type
Research Article
Submitted
30 Dec 2022
Accepted
03 Feb 2023
First published
08 Feb 2023

Inorg. Chem. Front., 2023,10, 1769-1774

Electronic structure regulation of halogen anion-intercalated MgAl-LDH for highly selective photothermal oxidation of CH4

X. Sun, Y. Xu, S. Bai, G. Liu, T. Shen and Y. Song, Inorg. Chem. Front., 2023, 10, 1769 DOI: 10.1039/D2QI02772K

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