Zn-Fe pair sites catalyst for highly selective photocatalytic oxidation of methane to formaldehyde

Shixuan Yu, Shiying Fan, Jun Duan, Dongke Zhang, Xinyong Li

Research output: Contribution to journalArticlepeer-review

2 Citations (Scopus)

Abstract

Efficient methane photooxidation into formaldehyde in H2O under mild conditions lies in C-H bond activation and intermediates coupling. Here, we report a Zn-Fe pair sites (Zn-Fex PS) photocatalyst to polarize the CH4 molecules on Zn+-O-sites and facilitate the coupling of *CH3 and *OH on Fe sites. Various in situ investigations confirm that the Zn-Fe0.2 PS promotes the generation of *CH3 and *OH. The theoretical calculations reveal that the local charge density accumulation on Zn and O atoms significantly strengthens Zn+-O- sites polarization, lowering the energy barrier for *CH3 formation from 0.87 eV to 0.36 eV. Moreover, a strong d-σ hybridization between *CH3 and Fe reduces C-H bonds steric hindrance, enhancing the coupling of *CH3 and *OH. Accordingly, the HCHO productivity over Zn-Fe0.2 PS reaches 2660.44 μmol·g−1 with a remarkable selectivity of 95.89 %. This study broadens the scope for designing cost-effective photocatalysts to selectively oxidize CH4 into value-added oxygenates.

Original languageEnglish
Article number124930
Number of pages12
JournalApplied Catalysis B: Environmental
Volume365
Early online date11 Dec 2024
DOIs
Publication statusPublished - 15 May 2025

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