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

Fanle Bu, Jiayu Yan, Lu Qi, Shuya Zhao and Yurui Xue ()
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Fanle Bu: Shandong University
Jiayu Yan: Shandong University
Lu Qi: Shandong University
Shuya Zhao: Jilin University
Yurui Xue: Shandong University

Nature Communications, 2025, vol. 16, issue 1, 1-10

Abstract: Abstract 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.

Date: 2025
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DOI: 10.1038/s41467-025-64248-7

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