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<p>Selective CH<sub>4</sub>-to-C<sub>2</sub> oxygenates conversion under mild conditions represents a frontier challenge in catalysis science with promising commercial implications. Herein, we report the successful and controlled construction of densely distributed O<sub>2</sub>-bridged Fe diatomic (Fe<sub>1</sub>-O<sub>2</sub>-Fe<sub>1</sub>) interfaces in carbon nitride aerogel-supported Fe dual-atom catalysts (Fe-DAC/g-C<sub>3</sub>N<sub>4</sub>) for selective methane oxidation to acetic acid (CH<sub>3</sub>COOH) in aqueous solution under mild conditions. Experimental studies reveal that the Fe<sub>1</sub>-O<sub>2</sub>-Fe<sub>1</sub> atomic interfaces with tailored coordination environments and precisely modulated Fe-Fe distance (2.92 ± 0.05 Å) and oxygen-bridged coordination environment synergistically promote the activation and cleavage of C-H bond to form methyl radicals (•CH<sub>3</sub>), carboxyl intermediates (•COOH), followed by selective C-C coupling via a radical recombination pathway. This concerted mechanism achieves unprecedented performance with near 100% selectivity and a remarkable CH<sub>3</sub>COOH production rate of 0.79 mmol g<sub>cat</sub><sup>−1</sup> h<sup>−1</sup> under ambient conditions. Notably, industrially relevant pressures (1.5 MPa CH<sub>4</sub>) elevate the production rate to 1.67 mmol g<sub>cat</sub><sup>−1</sup> h<sup>−1</sup> while maintaining &gt;96% selectivity.</p>

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Coordination-tailored atomic interfaces for selective CH4-to-C2 conversion in aqueous solution

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年10月15日

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  • Fanle Bu,
  • Jiayu Yan,
  • Lu Qi,
  • Shuya Zhao,
  • Yurui Xue

摘要

Selective CH4-to-C2 oxygenates conversion under mild conditions represents a frontier challenge in catalysis science with promising commercial implications. Herein, we report the successful and controlled construction of densely distributed O2-bridged Fe diatomic (Fe1-O2-Fe1) interfaces in carbon nitride aerogel-supported Fe dual-atom catalysts (Fe-DAC/g-C3N4) for selective methane oxidation to acetic acid (CH3COOH) in aqueous solution under mild conditions. Experimental studies reveal that the Fe1-O2-Fe1 atomic interfaces with tailored coordination environments and precisely modulated Fe-Fe distance (2.92 ± 0.05 Å) and oxygen-bridged coordination environment synergistically promote the activation and cleavage of C-H bond to form methyl radicals (•CH3), carboxyl intermediates (•COOH), followed by selective C-C coupling via a radical recombination pathway. This concerted mechanism achieves unprecedented performance with near 100% selectivity and a remarkable CH3COOH production rate of 0.79 mmol gcat−1 h−1 under ambient conditions. Notably, industrially relevant pressures (1.5 MPa CH4) elevate the production rate to 1.67 mmol gcat−1 h−1 while maintaining >96% selectivity.