Abstract
Direct catalytic conversion of methane to methanol offers a pathway for transforming a potent greenhouse gas into a portable clean liquid fuel, thereby mitigating carbon emissions and supporting sustainable energy. However, this process faces challenges from thermodynamically favorable methanol overoxidation. Here, we show that spatiotemporal regulation of photogenerated charge carriers on engineered catalytic sites enables a bio-inspired ordered two-step photocatalytic process that imitates methane monooxygenase. In a platinum-loaded cadmium sulfide photocatalyst, unsaturated sulfur sites modulate hole migration while platinum sites modulate electron migration, ensuring their concurrent surface arrival within picoseconds and prolonged localization. This dynamics temporarily anchors methane at hole-enriched sulfur sites while hydroxyl radical generation occurs at electron-rich platinum sites, decoupling hydroxyl radical formation from methane dehydrogenation to suppress overoxidation. The approach achieves methane-to-methanol conversion with selectivity of 83.5%, offering a bio-inspired solar-driven strategy for C1 valorization.
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The authors declare that the data supporting the findings of this study are available within the article and its Supplementary Information files. Source data are provided as a source data file with this paper and are available from the corresponding authors upon request. Source data are provided with this paper.
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Acknowledgements
This work was supported by the National Science Fund for Distinguished Young Scholars (Grant No. 52325401, Y.Z.), the National Natural Science Foundation of China (Grant No. 22209135, Y.C.), the National Key R&D Project of China (Grant No. 2020YFA0710000, Y.Z.) and Key Research and Development Program of Sichuan Province (No. 2023ZDZX0005, Y.C.). We thank staff at the BL13SSW beamline of the Shanghai Synchrotron Radiation Facilities (SSRF) for assistance with the XAFS. This work was also supported by the User Experiment Assist System of SSRF. The group of Nano-Catalysis Group at Sum Yat-sen University and Shanghai Synchrotron Radiation Facility was thanked for sharing XAFS of standard Pt foil and PtO2. We would like to thank Analysis and Testing Center, Southwest Petroleum University for the support of EPR test.
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Y.Z. conceived and designed the study. Y.L. and C.H. conducted photocatalytic CH4 oxidation evaluation experiments. Y.L. and Y.C. guided most of characterizations and data analysis. Y.L., K.Z. and J.M. carried out the excited-state dynamics measurements and finished the data analysis. S.C carried out in-situ XPS characterizations and Y.L. finished the data analysis. Y.L. and Y.C. organized the manuscripts and co-wrote the paper. Y.Z. supervised the project and co-wrote the paper. The manuscript has been reviewed by all authors and the results are presented after the discussions.
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Li, Y., Cao, Y., Han, C. et al. Spatiotemporal photon distribution control on active sites enables bio-inspired methane-to-methanol conversion. Nat Commun (2026). https://doi.org/10.1038/s41467-026-70134-7
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DOI: https://doi.org/10.1038/s41467-026-70134-7
