Abstract
Helium (He) recovery via conventional cryogenic distillation is highly energy-intensive and costly. Membrane separation features modularity and efficiency, but mixed-matrix membranes (MMMs) often suffer from discontinuous channels and poor filler–polymer compatibility, which impair separation performance. Here, we report an MMM platform by embedding a continuous 3D nanoporous ZIF-67-NH2 gel within a polyimide matrix. The gel functions as a dual-functional crosslinker, forming covalent amide linkages and hydrogen bonds with the polymer to eliminate interfacial voids, while creating interconnected, selective nanochannels through its intrinsic nanoporosity. This yields He/CH4 performance: 549 Barrer He permeability and 110.3 selectivity, surpassing the benchmark membranes. The membrane retains over 95% performance in mixed-gas tests over 180 h. Process simulations show that a hybrid membrane–cryogenic system achieves >93% He recovery and 74% energy savings. This work provides an energy-efficient platform for critical gas separations.
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Acknowledgements
The authors thank the Analytical Instrumentation Center of Hunan University for assistance with TEM and DSC measurements. The authors gratefully acknowledge the financial support from the Open Project Program of State Key Laboratory of Petroleum Pollution Control (Grant No. PPC2023003, recipient S.W.), CNPC Research Institute of Safety and Environmental Technology, the Natural Science Foundation of Changsha, China (kq2402057, recipient S.W.), Guangdong Basic and Applied Basic Research Foundation (2024A1515011066, recipient S.W.), Hunan Provincial Innovation Foundation For Postgraduate (CX20240454, recipient X.T.) and the Fundamental Research Funds for the Central Universities.
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K.Z. and S.W. are inventors on a patent application filed by Hunan University (no. CN202510044823.2) that covers the synthesis and application of the MOF gels described in this paper. The remaining authors declare no competing interests.
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Zhang, K., Huan, H., Tian, X. et al. MOF gel network crosslinked mixed matrix membranes with engineered interface for high-efficiency Helium recovery. Nat Commun (2026). https://doi.org/10.1038/s41467-026-72867-x
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DOI: https://doi.org/10.1038/s41467-026-72867-x
