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Surface-Tension-Governed Nanoconfinement for Tunable Hydrogen-Isotope Transport

Liu Tianqi1,2,3,*, Liang Wenbin1,3,*, Li Hong1,3, Lv Zixiao1,3, Liang Xiaoye4, Hao Jianguo4, Ding Youqian5, Wu Wangsuo1,3, Chen Ximeng1,3,† et al.

Li Zhan1,3,‡

  • *These authors contributed equally to this work.
  • †Contact author: chenxm@lzu.edu.cn
  • ‡Contact author: liz@lzu.edu.cn
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PRX Energy 4, 043010 – Published 5 December, 2025

DOI: https://doi.org/10.1103/fbh1-z24h

Abstract

Interfacial forces and nanoconfined environments play crucial roles in transport phenomena within low-dimensional materials. In this study, we propose a photothermally regulated surface-tension mechanism for hydrogen-isotope fractionation, in which light-induced changes in the surface tension of gallium (Ga) dynamically modulate the confined environment between graphene oxide (GO) layers. Under near-infrared irradiation, the surface tension of Ga decreases, altering its wettability within the interlayer galleries and inducing a reversible contraction of the GO interlayer spacing. In situ temperature-dependent transmission electron microscopy confirmed this dynamic modulation, showing that confined Ga nanoparticles undergo fully reversible expansion-contraction and display surface-energy-driven extension behavior analogous to macroscopic particles. Such confinement-induced structural responsiveness regulates the local arrangement of water molecules, leading to distinct molecular aggregation states for H2O and D2O. Due to stronger intermolecular attraction, D2O diffusion is more restricted in confinement, leading to pronounced isotope selectivity. Experimentally, the membrane achieved a separation factor of 70.53 for H2O:D2O and demonstrated selective removal of tritium water (T2O). Our study elucidates the interplay between photothermally driven interfacial energy modulation and confined molecular transport, offering new insights into tunable separation processes and interfacial physics.

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Popular Summary

Efficiently separating hydrogen isotopes remains a major challenge for applications ranging from nuclear wastewater treatment to advanced energy systems. This study introduces a photothermally regulated approach that uses light to control molecular transport within nanometer-scale channels. By lowering the surface tension of liquid gallium confined between graphene oxide layers, near-infrared irradiation triggers reversible contractions in the interlayer spacing, as confirmed by in situ temperature-dependent transmission electron microscopy. These dynamic changes reshape the local environment to regulate distinct molecular aggregations states for H2O and D2O. The stronger intermolecular attraction in D2O leads to more restricted diffusion under confinement, producing distinct aggregation states and exceptionally high isotope selectivity. Leveraging this mechanism, the membrane achieves a separation factor of 70.53 for H2O/D2O and can selectively remove tritiated water, demonstrating how photothermally modulated interfacial forces can enable tunable and energy-efficient isotope separation.

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PRX Energy 4, 043010– Published 5 December, 2025
  • Received 1 March 2025
  • Revised 12 July 2025
  • Accepted 5 November 2025
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