Abstract
Industrially, hydrogen production often relies on carbon-based resources, necessitating the separation of hydrogen from impurities such as CO, CO2, hydrocarbons and N2. Traditional purification methods involve complicated and energy-intensive sequential conversion and removal of these impurities. Here we introduce a reversible catalytic cycle based on the interconversion between γ-butyrolactone and 1,4-butanediol over an inverse Al2O3/Cu catalyst, enabling efficient hydrogen separation and storage from crude hydrogen feeds. This process could transform crude hydrogen feeds containing over 50% impurities into pure hydrogen at low temperature. The low impurity affinity and high dispersion of inverse Al2O3/Cu facilitate catalytic crude and waste hydrogen separations previously considered unachievable. This approach avoids the need for expensive pressure swing adsorption or membrane systems in liquid organic hydrogen carriers, showing great potential for large-scale applications in crude hydrogen or industrial tail gas utilization processes. By providing a low-risk, energy-efficient alternative, this strategy supports the global transition from grey/blue hydrogen to green hydrogen.
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The authors declare that all data supporting the findings of this study are available within the paper and Supplementary Information files. Source data are provided with this paper.
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Acknowledgements
This work was supported by the Ministry of Science and Technology of China (2023YFA1509103, 2022YFA1503804, Yifeng Zhu; 2021YFA1501102, D.M.; 2023YFA1506602, M.P.), National Natural Science Foundation of China (22272031, 22472035, 22102033, Yifeng Zhu; 22232001, D.M.; 22402035, C.Y.), Science and Technology Commission of Shanghai Municipality (22ZR1408000, 22QA1401300, Yifeng Zhu) and the Fundamental Research Funds for the Central Universities (20720220008, Yifeng Zhu). D.M. acknowledges support from the Tencent Foundation through the XPLORER PRIZE. We are grateful for the support of BL02B01 (31124.02.SSRF.BL02B01), BL05U (31124.02.SSRF.BL05U) and BL06B (31124.02.SSRF.BL06B) at the SSRF. We acknowledge the Energy Strategy and Engineering Consulting Center at the Institute of Coal Chemistry for their support in the techno-economic assessments and X. Duan and Y. Cao from the School of Chemical Engineering, East China University of Science and Technology, for their assistance with Aspen ONE.
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Yifeng Zhu, D.M. and X.B. conceived of the idea and concept. Y. Chen, X.K., C.Y. and G.G. performed the experiments. Y. Chen, X.P., R.M., Y.L. and Yifeng Zhu performed techno-economic and life-cycle assessments. W.S., F.Y., H. Zhang and Z.L. helped with the surface characterizations. Data were discussed among all co-authors. The original draft was organized by Yifeng Zhu, X.K. and Y. Cao. The paper was reviewed and edited by H. Zheng, Yulei Zhu, H. Zhang, M.P., D.M. and X.B., with contributions from all authors.
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Chen, Y., Kong, X., Yang, C. et al. A catalytic cycle that enables crude hydrogen separation, storage and transportation. Nat Energy 10, 971–980 (2025). https://doi.org/10.1038/s41560-025-01806-9
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DOI: https://doi.org/10.1038/s41560-025-01806-9
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