Abstract
Tritiated water emissions from nuclear facilities pose significant environmental risks and threaten the sustainability of nuclear energy. However, deep detritiation remains a major challenge due to the nearly indistinguishable physicochemical properties among water isotopologues. Here we present an efficient hydrogen isotope separation process based on catalytic proton exchange. The unique catalysis-promoted proton-transfer pathway found in a metal–organic framework (MIL-101(Cr)) significantly lowers the isotope exchange energy barrier to a previously unachieved level. Incorporating MIL-101(Cr) into a water distillation (WD) system enables a solid–liquid–gas triphasic mass transfer that overcomes the thermodynamic constraints of traditional WD, which relies on a liquid–gas biphasic isotope exchange. The height equivalent to the theoretical plate of the established WD prototype fell by half compared to the existing WD systems, thus increasing the separation efficiency by over four orders of magnitude in a 10-m distillation tower. This work offers an industrially viable and scalable option for cleaning up tritiated water.
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Data availability
The data supporting the findings of this study are available within the article and its Supplementary Information. Further information and answers to questions about the data and modelling approach are available from the corresponding author on request. Source data are provided with this paper.
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Acknowledgements
We would like to acknowledge the support from the following funding sources: the National Natural Science Foundation of China (Grant Nos. 22425061 to S.W., 22276132 to H.L., 22206144 to L.C., 22406135 to T.W., 22125602 and 22076078 to L.M. and 22306139 to A.J.), the National Natural Key R&D Program of China (Grant No. 2022YFE0105300 to S.W.), the New Cornerstone Science Foundation through the Xplorer Prize, a project funded by the Priority Academic Program Development of Jiangsu Higher Education Institutions and the Postdoctoral Fellowship Program of CPSF (GZC 20231888 to T.W.). We also thank C. Zhang from Anhui University of Science and Technology for his help with the theoretical calculations.
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S.W. conceived and supervised the project. H.L., Q.Y. and S.Z. completed the experiments and collected and analysed the data. N.L. and X.D. contributed to the theoretical calculations. L.C. was involved in data analysis and writing of the paper. J.S. analysed the ssNMR data. T.W., N.S., J.X., J.L., L.H., A.J., Z.X., G.Z., C.G., H.Y., J.C., L.M., S.G., K.L., P.L., X.L., X.O., Y.P., X.Z. and Z.C. participated in project discussions and provided valuable insights. All authors contributed to refining the paper before submission.
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S.W., H.L., Q.Y., S.Z., A.J., T.W. and J.L. and Soochow University have filed a patent based on the results presented. The other authors declare no competing interests.
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Nature Sustainability thanks Zhan Li, Ken-ichi Otake and Sheng Zhang for their contribution to the peer review of this work.
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The PDF file includes supplementary materials, namely text, Supplementary Figs. 1–46, Tables 1–3 and References 1–34.
Supplementary Video 1
H/D exchange path for MIL-101(Al). As MIL-101(Al) and MIL-101(Cr) are isomorphic systems, the spin complexity of the Cr atoms needs to be considered. Thus, MIL-101(Al) was chosen as the simulation object to speed up the calculations. The kinetic simulation of proton transfer in the water bridge of MIL-101(Al) shows that a stable structure of three H2O molecules can be formed between Al–OH2 and Al–OH−. Protons are repeatedly transferred back and forth in the hydrogen bonding lattice of this water bridge to realize the H/D exchange process, which is very rapid. The ultrafast exchange rate was at the femtosecond level. The kinetic results show that the proton exchange process was fast and frequent at 350 K. Colour code: Al, purple; O, red; C, grey; H, white.
Source data
Source Data Fig. 3
Water vapour adsorption data, ssNMR processing data, etc.
Source Data Fig. 4
Tritium WD data.
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Liu, H., Yang, Q., Luan, N. et al. Catalytic proton exchange in water distillation for efficient tritiated water clean-up. Nat Sustain 8, 553–561 (2025). https://doi.org/10.1038/s41893-025-01537-5
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DOI: https://doi.org/10.1038/s41893-025-01537-5
