Abstract
Gravitationally induced stratification during self-assembly often leads to density-driven vertical segregation, resulting in an inherent density gradient that severely limits the synthesis of metastable nanofilms requiring inverted architectures. Here we show an antigravity confined interfacial self-assembly approach based on a liquid-liquid interface formed between hydrophilic and hydrophobic porous membranes, where capillary forces suppress gravitational effects to enable precise molecular organization. Experimental data, supported by quantum chemistry, density functional theory, and Fick’s first law, demonstrate that capillary forces enhance local concentration and interaction probability, yielding highly ordered, stable nanofilms. Our approach achieves a 17-fold increase in film area than gravity-limited methods and a 109-fold improvement over unconfined techniques. These nanofilms exhibit the stability and mechanical property, showing promise for green enhanced oil recovery and multifunctional material development. Furthermore, our strategy offers a paradigm for nanofilm mechanical characterization, paving the way for future advances in the design and application of nanomaterials.
Similar content being viewed by others
Data availability
The data supporting the findings of this study are available within this article and its Supplementary Information. Source data are provided with this paper. All data are available from the corresponding author upon request. Source data are provided with this paper.
References
Whitesides, G. M., Mathias, J. P. & Seto, C. T. Molecular self-assembly and nanochemistry: a chemical strategy for the synthesis of nanostructures. Science 254, 1312–1319 (1991).
Whitesides, G. M. & Grzybowski, B. Self-assembly at all scales. Science 298, 2418–2421 (2002).
Liu, Z., Wang, Y., Zhou, Y., Smith, R. L. & Qi, X. Confined interfacial self-assembly of graphene-like carbon/MXene composite electrodes for capacitive deionization. Chem. Eng. J. 498, 155717 (2024).
Wang, A., Ma, Y. & Zhao, D. Pore engineering of porous materials: effects and applications. ACS Nano 18, 22829–22854 (2024).
Zhu, Y. et al. A general strategy for synthesizing biomacromolecular ionogel membranes via solvent-induced self-assembly. Nat. Synth. 2, 864–872 (2023).
Yang, R. et al. Potential difference-modulated synthesis of self-standing covalent organic framework membranes at liquid/liquid interfaces. J. Am. Chem. Soc. 144, 11778–11787 (2022).
Sproncken, C. C. M. et al. Large-area, self-healing block copolymer membranes for energy conversion. Nature 630, 866–871 (2024).
Lehane, R. A. et al. Electrosynthesis of biocompatible free-standing PEDOT thin films at a polarized liquid/liquid interface. J. Am. Chem. Soc. 144, 4853–4862 (2022).
Ikuta, D. et al. Conformationally supple glucose monomers enable synthesis of the smallest cyclodextrins. Science 364, 674–677 (2019).
Wu, Y. et al. Mirror-image cyclodextrins. Nat. Synth. 3, 698–706 (2024).
Landman, J. et al. Inward growth by nucleation: Multiscale self-assembly of ordered membranes. Sci. Adv. 4, eaat1817 (2018).
Xu, Z. et al. Heteromultivalent peptide recognition by co-assembly of cyclodextrin and calixarene amphiphiles enables inhibition of amyloid fibrillation. Nat. Chem. 11, 86–93 (2019).
Yang, S. et al. Giant capsids from lattice self-assembly of cyclodextrin complexes. Nat. Commun. 8, 15856 (2017).
Liu, J. et al. On-liquid-gallium surface synthesis of ultrasmooth thin films of conductive metal–organic frameworks. Nat. Synth. 3, 715–726 (2024).
Liu, S. et al. Ultrathin cyclodextrin nanofilm composite membranes for efficient separation of xylene isomers. J. Membr. Sci. 644, 120165 (2022).
Zhou, L. et al. Ultrathin cyclodextrin-based nanofiltration membrane with tunable microporosity for antibiotic desalination. J. Membr. Sci. 715, 123504 (2025).
Holden, M. A., Needham, D. & Bayley, H. Functional bionetworks from nanoliter water droplets. J. Am. Chem. Soc. 129, 8650–8655 (2007).
Hwang, W. L., Chen, M., Cronin, B., Holden, M. A. & Bayley, H. Asymmetric droplet interface bilayers. J. Am. Chem. Soc. 130, 5878–5879 (2008).
Zeng, Y. et al. Reconfigurable liquid devices from liquid building blocks. Nat. Chem. Eng. 1, 149–158 (2024).
Zhang, Y. et al. Continuous air purification by aqueous interface filtration and absorption. Nature 610, 74–80 (2022).
Liu, J. et al. Liquid-gating meniscus-shaped deformable magnetoelastic membranes with self-driven regulation of gas/liquid release. Adv. Mater. 34, 2107327 (2021).
Guo, X. et al. Janus channel of membranes enables concurrent oil and water recovery from emulsions. Science 386, 654–659 (2024).
Schmidt, B. V. K. J. & Barner-Kowollik, C. Dynamic macromolecular material design-the versatility of cyclodextrin-based host–guest chemistry. Angew. Chem. Int. Ed. 56, 8350–8369 (2017).
Wankar, J. et al. Recent advances in host-guest self-assembled cyclodextrin carriers: implications for responsive drug delivery and biomedical engineering. Adv. Funct. Mater. 30, 1909049 (2020).
Zhou, C., Huang, J. & Yan, Y. Chain length dependent alkane/b-cyclodextrin nonamphiphilic supramolecular building blocks. Soft Matter 12, 1579–1585 (2016).
Hou, X., Hu, Y., Grinthal, A., Khan, M. & Aizenberg, J. Liquid-based gating mechanismwith tunable multiphase selectivity and antifouling behaviour. Nature 519, 70–73 (2015).
Sheng, Z. et al. Liquid-based porous membranes. Chem. Soc. Rev. 49, 7907–7928 (2020).
Lee, T. et al. Large-area synthesis of ultrathin, flexible, and transparent conductive metal-organic framework thin films via a microfluidic-based solution shearing process. Adv. Mater. 34, 2107696 (2022).
Ding, Z., Liu, Z., Liu, R. & Yang, C. Breakup of ultra-thin liquid films on vertical fiber enhanced by Marangoni effect. Chem. Eng. Sci. 199, 342–348 (2019).
Chatzigiannakis, E., Veenstra, P., Bosch, D. & Vermant, J. Mimicking coalescence using a pressurecontrolled dynamic thin film balance. Soft Matter 16, 9410–9422 (2020).
Wang, C. et al. Interfacial rheological behaviors of inclusion complexes of cyclodextrin and alkanes. Soft Matter 13, 8636–8643 (2017).
Wang, H. et al. Host-guest liquid gating mechanism with specific recognition interface behavior for universal quantitative chemical detection. Nat. Commun. 13, 1906 (2022).
Grimme, S., Bannwarth, C. & Shushkov, P. A robust and accurate tight-binding quantum chemical method for structures, vibrational frequencies, and noncovalent interactions of large molecular systems parametrized for all spd-block elements (Z =1-86). J. Chem. Theory Comput. 13, 1989–2009 (2017).
Bannwarth, C., Ehlert, S. & Grimme, S. GFN2-xTB-an accurate and broadly parametrized self-consistent tight-binding quantum chemical method with multipole electrostatics and density-dependent dispersion contributions. J. Chem. Theory Comput. 15, 1652–1671 (2019).
Lu, T. & Chen, Q. Interaction region indicator: a simple real space function clearly revealing both chemical bonds and weak interactions. Chem. Methods 1, 231–239 (2021).
Lu, T. & Chen, F. Multiwfn: a multifunctional wavefunction analyzer. J. Comput. Chem. 33, 580–592 (2012).
Tyne, R. L. et al. Rapid microbial methanogenesis during CO2 storage in hydrocarbon reservoirs. Nature 600, 670–674 (2021).
Nafisifar, A., Manshad, A. K. & Shadizadeh, S. R. Synergistic study of xanthan-gum based nano-composite on PELS anionic surfactant performance, and mechanism in porous media: Microfluidic & carbonate system. Fuel 348, 128510 (2023).
Hu, Z., Al-Ameri, L., Gardy, J., Alhreez, M. & Wen, D. In situ produced nanoparticles at the oil-water interface for conformance control and enhanced oil recovery. Energ. Fuel. 36, 12986–12996 (2022).
Zhang, Z., Yao, Z. & Jiang, Z. Fast self-assembled microfibrillated cellulose@MXene film with high-performance energy storage and superior mechanical strength. Chin. Chem. Lett. 32, 3575–3578 (2021).
Chen, S., Yin, L., Liu, L., Zhang, N. & Dong, D. Ion-induced white-light-emitting polymeric hydrogels with high mechanical strength and reversible stimuli-responsive properties. Chin. Chem. Lett. 32, 3133–3136 (2021).
Shi, S. et al. Self-assembly of mXene-surfactants at liquid-liquid interfaces: from structured liquids to 3D aerogels. Angew. Chem. Int. Ed. 58, 18171–18176 (2019).
Wang, F., Wu, Y. & Huang, Y. Novel application of graphene oxide to improve hydrophilicity and mechanical strength of aramid nanofiber hybrid membrane. Compos. Part A 110, 126–132 (2018).
Lyu, L. et al. Anomalously high apparent Young’s modulus of ultrathin freestanding PZT films revealed by machine learning empowered nanoindentation. Adv. Mater. 37, 2412635 (2025).
Zhao, W., Zhu, M., Mo, Y. & Bai, M. Effect of anion on micro/nano-tribological properties of ultra-thin imidazolium ionic liquid films on silicon wafer. Colloids Surf. A: Physicochem. Eng. Asp. 332, 78–83 (2009).
Humphrey, W., Dalke, A. & Schulten, K. VMD: visual molecular dynamics. J. Mol. Graph. 14, 33–38 (1996).
Acknowledgements
This work was supported by the National Natural Science Foundation of China (Nos. 52025132, U24A20205, 21621091, 22021001, 22121001 awarded to X.H., No. 52303350 awarded to Y.F., and No. 52304027 awarded to G.L.), the China National Quality Infrastructure System (NQI) Key Scientific and Technological Project (No. 2023YFF0614100-01 awarded to Z.H.Z.), the 111 Project (Nos. B17027 and B16029 awarded to X.H.), the Natural Science Foundation of Fujian Province of China (No. 2022J02059 awarded to X.H. and No. 2024J08037 awarded to J.M.L.), the Scientific Research and Technology Development Projects of PetroChina (Nos. 2021ZZ01 and 2023ZZ04 awarded to Z.H.Z.), and the New Cornerstone Science Foundation through the XPLORER PRIZE, awarded to X.H.
Author information
Authors and Affiliations
Contributions
X.H. conceived the project. X.H., J.M.L., Z.H.Z., and W.F.L. designed the research. J.M.L., Z.Y.Z., G.L., and S.J.Y. performed the experiments. J.M.L., Y.Y.C., and X.H. designed and analyzed the theoretical model. J.M.L., X.Z., Y.F., and X.H. designed the devices for the applications. Z.H.Z., J.M.L., G.L., Q.Z., L.H., N.H.J., B.Z., and W.F.L. designed and analyzed the applications. J.M.L., X.H, and Z.H.Z. wrote the manuscript. All authors edited, read, and approved the manuscript.
Corresponding authors
Ethics declarations
Competing interests
The authors declare no competing interests.
Peer review
Peer review information
Nature Communications thanks Atul Parikh, Stefan Schröder and the other, anonymous, reviewer(s) for their contribution to the peer review of this work. A peer review file is available.
Additional information
Publisher’s note Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.
Supplementary information
Source data
Rights and permissions
Open Access This article is licensed under a Creative Commons Attribution-NonCommercial-NoDerivatives 4.0 International License, which permits any non-commercial use, sharing, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons licence, and indicate if you modified the licensed material. You do not have permission under this licence to share adapted material derived from this article or parts of it. The images or other third party material in this article are included in the article’s Creative Commons licence, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons licence and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this licence, visit http://creativecommons.org/licenses/by-nc-nd/4.0/.
About this article
Cite this article
Zhou, Z., Lei, J., Zhang, Z. et al. Antigravity confined interfacial self-assembly approach for the synthesis and characterization of nanofilms. Nat Commun (2026). https://doi.org/10.1038/s41467-026-68447-8
Received:
Accepted:
Published:
DOI: https://doi.org/10.1038/s41467-026-68447-8


