Fe-(μ-O)-Zn dual-atom boosting C-C coupling for direct oxidation of methane to acetic acid using O<sub>2</sub>.
basic_science · Level V
Where this comes from
- Record sourced from PubMed, PMID 41145491.
- Also identified by DOI 10.1038/s41467-025-64505-9 and PMC identifier 12559319.
- Licence recorded as CC BY-NC-ND.
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Abstract
Direct oxidation of methane (DOM) into high-value C2+ products using molecular oxygen (O<sub>2</sub>) is essential for the sustainable production of clean energy and bulk chemicals, but is still challenging due to the difficult C-H activation and uncontrollable C-C coupling process. Herein, we design and construct the Fe-(μ-O)-Zn dual-atom sites by supporting Fe and Zn atoms on ZSM-5 (Fe<sub>1</sub>-Zn<sub>1</sub>/ZSM-5), which achieves the DOM by O<sub>2</sub> to acetic acid under ambient temperature and pressure. The Fe-(μ-O)-Zn dual-atom sites yield an acetic acid productivity of 3006 μmol•g<sub>cat</sub><sup>-1</sup>•h<sup>-1</sup> with 86.8% selectivity (total C2+ products selectivity of 93.0%) for at least 20 hours at 25 <sup>o</sup>C and atmospheric pressure. The mutual electronic modulation between Fe and Zn shifts the d-band center of Fe 3d in Fe-(μ-O)-Zn dual-atom sites upwards, which promotes the formation and stabilization of highly reactive Fe=O species through O<sub>2</sub> photodissociation and thereby enhances the C-H bond activation of CH<sub>4</sub>. The Fe-(μ-O)-Zn dual-atom reaction sites (spatial distance of 2.7 Å) boost the C-C coupling of key CH<sub>3</sub> and HCHO intermediate species, which steadily produce acetic acid and other C2+ oxygenates. This work would broaden the avenue towards the sustainable conversion of methane to value-added C2+ products under ambient temperature and pressure.