Abstract
Storage and transportation of methane (CH4) remains challenging as it cannot be liquefied at ambient temperature and instead must be stored as compressed gas at high pressures (approximately 25 MPa). Alternatively, it can be stored within nanoporous materials at moderate pressures (for example, 3.5 MPa) but this ‘adsorbed natural gas’ approach can suffer from substantial desorption with only minor temperature increases. Both methods therefore necessitate additional safety measures. Here we report graphene-coated porous carbon materials that can be charged with CH4 at high pressure and retain it at ambient pressure and temperature (below 318 K), thereby enhancing storage safety. Our data suggest that graphene serves as a thermally controllable lock that obstructs or activates pores to trap or release CH4, enabling a pressure-equivalent loading of 19.9 MPa at 298 K, and release upon heating to 473 K. The resulting reversible CH4 volumetric capacity reaches 142 v/v, exceeding that of various adsorbed natural gas materials at 3.5 MPa and 298 K when considering container space utilization.
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Acknowledgements
This work was supported by the Japan Science and Technology Agency (JST) Open Innovation Platform with Enterprise, Research Institute and Academia (OPERA), under project number JPMJOP1722 (K.K.). J.S.-A. acknowledges financial support from the Ministerio de Ciencia e Innovación (Project PID2019-108453GB-C21) and the Conselleria de Innovación, Universidades, Ciencia y Sociedad Digital (Project CIPROM/2021/022) (J.S.-A.). K.K. was also financially supported by Takagi Co. S.W. acknowledges partial support from JST funds. We thank AD’ALL Co. for providing activated carbon fibre samples. We also thank Y. Gogotsi (Drexel University) for providing valuable suggestions for the revision of the manuscript.
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S.W. and K.K. developed the study concept and designed the methodology. S.W., F.V.-B, H.T. and K.K. wrote the paper. S.W. synthesized the samples. S.W., A.F., H.O., M.N., Y.K., T.O., H.K., K.U., H.N., I.M. and T.H. contributed to sample characterization. F.V.-B. and H.T. built the simulation model. F.V.-B. performed the Grand Canonical Monte Carlo calculations. H.T. performed the MD simulations. S.W., J.P.M.-L. and J.S.-A. performed the CH4 adsorption measurements. A.F., H.O., K.U., H.T. and J.S.-A. contributed to the discussion and editing of the paper.
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Supplementary Information
Supplementary Notes 1–10, Figs. 1–38 and Tables 1–15.
Supplementary Video 1
Temperature-dependent TEM observations of graphene-coated carbon at elevated temperatures.
Supplementary Video 2
Stable graphene layer contact responsible for pore locking at 298 K.
Supplementary Video 3
Movement of the graphene coating layers corresponding to pore unlocking at 473 K.
Source data
Source Data Fig. 1
Structural characterizations of graphene-coated carbon.
Source Data Fig. 2
Methane storage performance of graphene-coated carbon and reported ANG.
Source Data Fig. 3
Temperature-dependent characterizations of pore obstruction/activation.
Source Data Fig. 4
Methane storage performance of graphene-coated carbons prepared under different conditions.
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Wang, S., Vallejos-Burgos, F., Furuse, A. et al. Ambient pressure storage of high-density methane in nanoporous carbon coated with graphene. Nat Energy (2025). https://doi.org/10.1038/s41560-025-01783-z
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DOI: https://doi.org/10.1038/s41560-025-01783-z