Abstract
Direct conversion of CH4 into liquid oxygenates under mild conditions is of great significance but remains challenging due to the high dissociation energy of inert C-H bond. Here we report the fabrication of a dual atomic Fe and Pd catalyst with periodic macroporous structure (Fe1-Pd1 OMNC) toward the direct CH4 conversion at room temperature. Mechanism studies reveal that a charge polarization region (Oδ−-Fe-Pdδ+) is formed in-situ on Fe-Pd atomic sites upon oxidant activation, wherein the electron-rich Oδ⁻ and electron-deficient Pdδ+ regions can respectively capture the Hδ⁺ and CH3δ⁻ in CH4 and lead to the activation of C-H bond. As a result, Fe1-Pd1 OMNC demonstrates attractive photothermal catalytic performance toward the selective oxidation of CH4 under Xe lamp irradiation, achieving the productivities of C1 oxygenates as high as 0.754 mmol h−1 and 0.035 mmol h−1 when using H2O2 or O2 as the oxidant, respectively.
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The data that support the findings of this study are available within the article and Supplementary Information. Source data are provided with this paper or available from the corresponding author upon request. Source data are provided with this paper.
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Acknowledgements
This work was supported by the National Natural Science Foundation of China (22138003, 22578133, 21825802, 22208107), China Postdoctoral Science Foundation (2023T160228, 2022M710051), the Natural Science Foundation of Guangdong Province (2023B1515040005, 2022A1515012575), the Guangdong Basic and Applied Basic Research Foundation (2021A1515110413), the Fundamental Research Funds for the Central Universities (2023ZYGXZR087), State Key Laboratory of Pulp and Paper Engineering (2023PY06, 202302).
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F. Wang and Y. Li developed the idea and designed experiments. D. Chen, J. Zhou and F. Wang performed experiments. W. Lyu, X. Zhao and R. Fang assisted in synthetic experiments. D. Chen conducted the theoretical calculation. F. Wang and Y. Li secured funding. D. Chen, F. Wang and Y. Li wrote the manuscript. All authors discussed the results and commented on the manuscript.
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Chen, D., Zhou, J., Lyu, W. et al. Formation of charge-polarized regions at dual single-atom sites for C-H bond activation in methane. Nat Commun (2026). https://doi.org/10.1038/s41467-026-69822-1
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DOI: https://doi.org/10.1038/s41467-026-69822-1
