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Photocatalytic oxidative coupling of methane to C3+ hydrocarbons via nanopore-confined microenvironments

Nature Energy volume 10, pages 1095–1106 (2025)Cite this article

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Abstract

Photocatalytic oxidative coupling of methane (POCM) enables the production of value-added fuels and chemicals using renewable solar energy. Unfortunately, despite recent advances in the production of C2 chemicals (for example, ethane), POCM systems that selectively produce industrially useful and transportable C3+ hydrocarbons remain elusive. Here we report that Au-embedded porous TiO2, activated by steam during the POCM process, enables efficient and selective flow synthesis of propane with a productivity of 1.4 mmol h−1. At this productivity, we achieve a high propane selectivity of 91.3% and an apparent quantum efficiency of 39.7% at a wavelength of 365 nm. Mechanistic studies reveal that the tensile-strained Au and the nanopore-confined catalytic microenvironment jointly stabilize key ethane intermediates, boosting deeper C2–C1 coupling to form propane. Meanwhile, the steam-activated surface lattice oxygen on TiO2 accelerates hydrogen species transfer, thus enhancing POCM kinetics. This approach is economically feasible for practical application under concentrated solar light.

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Fig. 1: Design, fabrication and POCM performance of the highly porous Au/TiO2(P) catalyst.
Fig. 2: POCM performance of steam-activated Au/TiO2(P) catalyst.
Fig. 3: Characterizations of the lattice tensile strain in AuNPs induced by steam activation.
Fig. 4: Investigation of the promotion effects of steam-activated lattice oxygen in POCM.
Fig. 5: Theoretical calculations for the effect of steam-activation-induced reconstruction of the Au–TiO2 interface on the POCM energetics.

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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. Source data are provided with this paper.

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Acknowledgements

We acknowledge the financial support from the National Natural Science Foundation of China (grant nos 22405069, 51972094, 52371220, 22322101 and 22375017), the National Key Research and Development Program of China (grant no. 2020YFB1506300), the Beijing Institute of Technology Research Fund Program, the Hebei Provincial Department of Science and Technology (grant no. 236Z4403G), the Science Research Project of Hebei Education Department (grant no. JZX2024008), the Hebei Province Optoelectronic Information Materials Laboratory Performance Subsidy Fund Project (grant no. 22567634H), Hebei Education Department (grant no. BJ2025011) and the Research Innovation Team Project of Hebei University (grant nos 150000321008 and IT2023A04).

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  1. These authors contributed equally: Wenfeng Nie, Liwei Chen, Yuchen Hao.

Authors and Affiliations

  1. Research Center for Solar Driven Carbon Neutrality, School of Physics Science and Technology, Institute of Life Science and Green Development, Hebei University, Baoding, People’s Republic of China

    Wenfeng Nie, Yuchen Hao, Xiangjie Ge, Haodong Liu, Jialin Wang, Zhao Wang, Cuncai Lv, Shangbo Ning, Linjie Gao, Yaguang Li, Shufang Wang & Jinhua Ye

  2. College of Biological and Chemical Engineering, Qilu Institute of Technology, Jinan, People’s Republic of China

    Liwei Chen

  3. Ministry of Education Key Laboratory of Cluster Science, Beijing Key Laboratory of Photoelectronic/Electrophotonic Conversion Materials, School of Chemistry and Chemical Engineering, Beijing Institute of Technology, Beijing, People’s Republic of China

    Jiani Li, Hui-Zi Huang, Chao Sun & Bo Wang

  4. Sinopec Beijing Research Institute of Chemical Industry, Beijing, People’s Republic of China

    Jiani Li

  5. TJU-NIMS International Collaboration Laboratory, School of Materials Science and Engineering, Tianjin University, Tianjin, People’s Republic of China

    Jinhua Ye

Authors
  1. Wenfeng Nie
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Contributions

Y.H., B.W. and J.Y. designed the research. W.N., L.C. and Y.H. performed the catalyst preparation, characterization, photocatalytic tests and data analysis. H.L., X.G., Z.W., H.-Z.H., J.L., J.W., C.S., S.N., L.G., Y.L., C.L. and S.W. assisted with the material synthesis, characterizations and catalysis measurements. W.N., Y.H., L.C., B.W. and J.Y. wrote the paper. Y.H., S.W, B.W. and J.Y. supervised the research. All authors discussed the results and assisted during paper preparation.

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Correspondence to Yuchen Hao, Bo Wang or Jinhua Ye.

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Nie, W., Chen, L., Hao, Y. et al. Photocatalytic oxidative coupling of methane to C3+ hydrocarbons via nanopore-confined microenvironments. Nat Energy 10, 1095–1106 (2025). https://doi.org/10.1038/s41560-025-01834-5

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