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<p>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 <i>d</i>-band center of Fe 3<i>d</i> 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.</p>

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Fe-(μ-O)-Zn dual-atom boosting C-C coupling for direct oxidation of methane to acetic acid using O2

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年10月27日

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  • Baiyang Yu,
  • Wenlong Li,
  • Xuan Tang,
  • Lu Cheng,
  • Jiawei Zhang,
  • Shuobing Yang,
  • Fudong Liu,
  • Jing Xu,
  • Ying Zhang,
  • Chengsi Pan,
  • Xiao-Ming Cao,
  • Yongfa Zhu,
  • Yang Lou

摘要

Direct oxidation of methane (DOM) into high-value C2+ products using molecular oxygen (O2) 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 (Fe1-Zn1/ZSM-5), which achieves the DOM by O2 to acetic acid under ambient temperature and pressure. The Fe-(μ-O)-Zn dual-atom sites yield an acetic acid productivity of 3006 μmol•gcat−1•h−1 with 86.8% selectivity (total C2+ products selectivity of 93.0%) for at least 20 hours at 25 oC 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 O2 photodissociation and thereby enhances the C-H bond activation of CH4. The Fe-(μ-O)-Zn dual-atom reaction sites (spatial distance of 2.7 Å) boost the C-C coupling of key CH3 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.