1. Sholl, D. S. \& Lively, R. P. Seven chemical separations to change the world. Nature 532, 435–437 (2016).

Article 
ADS 
PubMed 
Google Scholar
2. Zhou, S. et al. Asymmetric pore windows in MOF membranes for natural gas valorization. Nature 606, 706–712 (2022).

Article 
ADS 
CAS 
PubMed 
Google Scholar
3. Qian, Q. et al. MOF-based membranes for gas separations. Chem. Rev. 120, 8161–8266 (2020).

Article 
CAS 
PubMed 
Google Scholar
4. Jiang, H., Alezi, D. \& Eddaoudi, M. A reticular chemistry guide for the design of periodic solids. Nat. Rev. Mater. 6, 466–487 (2021).

Article 
CAS 
Google Scholar
5. Lin, R.-B. et al. Molecular sieving of ethylene from ethane using a rigid metal–organic framework. Nat. Mater. 17, 1128–1133 (2018).

Article 
ADS 
CAS 
PubMed 
Google Scholar
6. Knebel, A. \& Caro, J. Metal–organic frameworks and covalent organic frameworks as disruptive membrane materials for energy-efficient gas separation. Nat. Nanotechnol. 17, 911–923 (2022).

Article 
ADS 
CAS 
PubMed 
Google Scholar
7. Zhou, S. et al. Electrochemical synthesis of continuous metal–organic framework membranes for separation of hydrocarbons. Nat. Energy 6, 882–891 (2021).

Article 
ADS 
CAS 
Google Scholar
8. Knebel, A. et al. Solution processable metal–organic frameworks for mixed matrix membranes using porous liquids. Nat. Mater. 19, 1346–1353 (2020).

Article 
CAS 
PubMed 
Google Scholar
9. Cadiau, A., Adil, K., Bhatt, P. M., Belmabkhout, Y. \& Eddaoudi, M. A metal-organic framework–based splitter for separating propylene from propane. Science 353, 137–140 (2016).

Article 
ADS 
CAS 
PubMed 
Google Scholar
10. Lai, H. W. H. et al. Hydrocarbon ladder polymers with ultrahigh permselectivity for membrane gas separations. Science 375, 1390–1392 (2022).

[Article](https://doi.org/10.1126%2Fscience.abl7163) 
[ADS](http://adsabs.harvard.edu/cgi-bin/nph-data_query?link_type=ABSTRACT&bibcode=2022Sci...375.1390L) 
[CAS](/articles/cas-redirect/1:CAS:528:DC%2BB38XpvVyguro%3D) 
[PubMed](http://www.ncbi.nlm.nih.gov/entrez/query.fcgi?cmd=Retrieve&db=PubMed&dopt=Abstract&list_uids=35324307) 
[Google Scholar](http://scholar.google.com/scholar_lookup?&title=Hydrocarbon%20ladder%20polymers%20with%20ultrahigh%20permselectivity%20for%20membrane%20gas%20separations&journal=Science&doi=10.1126%2Fscience.abl7163&volume=375&pages=1390-1392&publication_year=2022&author=Lai%2CHWH)
  1. Luo, X. et al. Wrinkled metal-organic framework thin films with tunable Turing patterns for pliable integration. Science 385, 647–651 (2024).

    Article 
    ADS 
    CAS 
    PubMed 
    Google Scholar
    12. Peng, Y. et al. Metal-organic framework nanosheets as building blocks for molecular sieving membranes. Science 346, 1356–1359 (2014).

    Article 
    ADS 
    CAS 
    PubMed 
    Google Scholar
    13. Xu, L.-H. et al. Highly flexible and superhydrophobic MOF nanosheet membrane for ultrafast alcohol-water separation. Science 378, 308–313 (2022).

    Article 
    ADS 
    CAS 
    PubMed 
    Google Scholar
    14. Ma, X. et al. Zeolitic imidazolate framework membranes made by ligand-induced permselectivation. Science 361, 1008–1011 (2018).

    Article 
    ADS 
    CAS 
    PubMed 
    Google Scholar
    15. Zhou, S. et al. Paralyzed membrane: current-driven synthesis of a metal-organic framework with sharpened propene/propane separation. Sci. Adv. 4, eaau1393 (2018).

    Article 
    ADS 
    CAS 
    PubMed 
    PubMed Central 
    Google Scholar
    16. Hou, Q., Zhou, S., Wei, Y., Caro, J. \& Wang, H. Balancing the grain boundary structure and the framework flexibility through bimetallic metal–organic framework (MOF) membranes for gas separation. J. Am. Chem. Soc. 142, 9582–9586 (2020).

    CAS 
    PubMed 
    Google Scholar
    17. Zhao, Y. et al. Flexible polypropylene-supported ZIF-8 membranes for highly efficient propene/propane separation. J. Am. Chem. Soc. 142, 20915–20919 (2020).

    Article 
    ADS 
    CAS 
    PubMed 
    Google Scholar
    18. Liang, Y. et al. Large-area ultrathin metal–organic framework membranes fabricated on flexible polymer supports for gas separations. Angew. Chem. Int. Ed. 63, e202404058 (2024).

    Article 
    CAS 
    Google Scholar
    19. Ma, Q. et al. Ultrafast semi-solid processing of highly durable ZIF-8 membranes for propylene/propane separation. Angew. Chem. Int. Ed. 132, 22093–22098 (2020).

    Article 
    Google Scholar
    20. Shu, L., Peng, Y., Zhu, C., Li, K. \& Yang, W. Metal-organic framework membranes with scale-like structure for efficient propylene/propane separation. Nat. Commun. 15, 10437 (2024).

    Article 
    ADS 
    CAS 
    PubMed 
    PubMed Central 
    Google Scholar
    21. Dakhchoune, M. et al. Gas-sieving zeolitic membranes fabricated by condensation of precursor nanosheets. Nat. Mater. 20, 362–369 (2021).

    Article 
    CAS 
    PubMed 
    Google Scholar
    22. Chen, G. et al. Solid-solvent processing of ultrathin, highly loaded mixed-matrix membrane for gas separation. Science 381, 1350–1356 (2023).

    Article 
    ADS 
    CAS 
    PubMed 
    Google Scholar
    23. Datta, S. J. et al. Rational design of mixed-matrix metal-organic framework membranes for molecular separations. Science 376, 1080–1087 (2022).

    Article 
    ADS 
    CAS 
    PubMed 
    Google Scholar
    24. Tan, X. et al. Truly combining the advantages of polymeric and zeolite membranes for gas separations. Science 378, 1189–1194 (2022).

    Article 
    ADS 
    CAS 
    PubMed 
    Google Scholar
    25. Koros, W. J. \& Zhang, C. Materials for next-generation molecularly selective synthetic membranes. Nat. Mater. 16, 289–297 (2017).

    Article 
    CAS 
    PubMed 
    Google Scholar
    26. Napper, D. H. Polymeric Stabilization of Colloidal Dispersions (Academic Press, 1983).
    27. de Gennes, P. G. Polymers at an interface; a simplified view. Adv. Colloid Interface Sci. 27, 189–209 (1987).

    Article 
    Google Scholar
    28. Lin, J.-B. et al. A scalable metal-organic framework as a durable physisorbent for carbon dioxide capture. Science 374, 1464–1469 (2021).

    Article 
    ADS 
    CAS 
    PubMed 
    Google Scholar
    29. Rodenas, T. et al. Metal–organic framework nanosheets in polymer composite materials for gas separation. Nat. Mater. 14, 48–55 (2015).

    Article 
    CAS 
    PubMed 
    Google Scholar
    30. Wei, R. et al. Carbon nanotube supported oriented metal organic framework membrane for effective ethylene/ethane separation. Sci. Adv. 8, eabm6741 (2022).

    Article 
    CAS 
    PubMed 
    PubMed Central 
    Google Scholar
    31. Li, G., Zhang, H. \& Han, Y. Applications of transmission electron microscopy in phase engineering of nanomaterials. Chem. Rev. 123, 10728–10749 (2023).

    Article 
    CAS 
    PubMed 
    Google Scholar
    32. Zhang, D. et al. Atomic-resolution transmission electron microscopy of electron beam–sensitive crystalline materials. Science 359, 675–679 (2018).

    Article 
    ADS 
    CAS 
    PubMed 
    Google Scholar
    33. Zhang, H. et al. Three-dimensional inhomogeneity of zeolite structure and composition revealed by electron ptychography. Science 380, 633–638 (2023).

    Article 
    ADS 
    CAS 
    PubMed 
    Google Scholar
    34. Zhu, Y. et al. Unravelling surface and interfacial structures of a metal–organic framework by transmission electron microscopy. Nat. Mater. 16, 532–536 (2017).

    Article 
    CAS 
    PubMed 
    Google Scholar
    35. Ozcan, A. et al. Tuning MOF/polymer interfacial pore geometry in mixed matrix membrane for upgrading CO2 separation performance. Sci. Adv. 10, eadk5846 (2024).

    Article 
    CAS 
    PubMed 
    PubMed Central 
    Google Scholar
    36. Wegst, U. G. K., Bai, H., Saiz, E., Tomsia, A. P. \& Ritchie, R. O. Bioinspired structural materials. Nat. Mater. 14, 23–36 (2015).

    Article 
    CAS 
    PubMed 
    Google Scholar
    37. Batatia, I. et al. A foundation model for atomistic materials chemistry. J. Chem. Phys. 163, 184110 (2025).

    Article 
    ADS 
    CAS 
    PubMed 
    Google Scholar
    38. Hjorth Larsen, A. et al. The atomic simulation environment—a Python library for working with atoms. J. Phys. Condens. Matter 29, 273002 (2017).

    Article 
    PubMed 
    Google Scholar
    39. Hafner, J. Ab-initio simulations of materials using VASP: density-functional theory and beyond. J. Comput. Chem. 29, 2044–2078 (2008).

    Article 
    ADS 
    CAS 
    PubMed 
    Google Scholar
    40. Grimme, S. Density functional theory with London dispersion corrections. Wiley Interdiscip. Rev. Comput. Mol. Sci. 1, 211–228 (2011).

    Article 
    CAS 
    Google Scholar
    41. Dudarev, S. L., Botton, G. A., Savrasov, S. Y., Humphreys, C. J. \& Sutton, A. P. Electron-energy-loss spectra and the structural stability of nickel oxide: an LSDA+U study. Phys. Rev. B 57, 1505–1509 (1998).

    Article 
    ADS 
    CAS 
    Google Scholar
    42. Limas, N. G. \& Manz, T. A. Introducing DDEC6 atomic population analysis: part 2. Computed results for a wide range of periodic and nonperiodic materials. RSC Adv. 6, 45727–45747 (2016).

    Article 
    ADS 
    CAS 
    Google Scholar
    43. Rappé, A. K., Casewit, C. J., Colwell, K. S., Goddard, W. A. III \& Skiff, W. M. UFF, a full periodic table force field for molecular mechanics and molecular dynamics simulations. J. Am. Chem. Soc. 114, 10024–10035 (1992).

    Article 
    ADS 
    Google Scholar
    44. Boyd, P. G., Moosavi, S. M., Witman, M. \& Smit, B. Force-field prediction of materials properties in metal-organic frameworks. J. Phys. Chem. Lett. 8, 357–363 (2017).

    Article 
    CAS 
    PubMed 
    PubMed Central 
    Google Scholar
    45. Thompson, A. P. et al. LAMMPS - a flexible simulation tool for particle-based materials modeling at the atomic, meso, and continuum scales. Comput. Phys. Commun. 271, 108171 (2022).

    Article 
    CAS 
    Google Scholar
    46. Abbott, L. J., Hart, K. E. \& Colina, C. M. Polymatic: a generalized simulated polymerization algorithm for amorphous polymers. Theor. Chem. Acc. 132, 1334 (2013).

    Article 
    Google Scholar
    47. Wang, J., Wolf, R. M., Caldwell, J. W., Kollman, P. A. \& Case, D. A. Development and testing of a general amber force field. J. Comput. Chem. 25, 1157–1174 (2004).

    Article 
    ADS 
    CAS 
    PubMed 
    Google Scholar
    48. Semino, R., Ramsahye, N. A., Ghoufi, A. \& Maurin, G. Microscopic model of the metal–organic framework/polymer interface: a first step toward understanding the compatibility in mixed matrix membranes. ACS Appl. Mater. Interfaces 8, 809–819 (2016).

    Article 
    CAS 
    PubMed 
    Google Scholar
    49. Fan, D. et al. Is porosity at the MOF/polymer interface necessarily an obstacle to optimal gas-separation performances in mixed matrix membranes? ACS Mater. Lett. 3, 344–350 (2021).

    Article 
    CAS 
    Google Scholar
    50. Diaz-Marquez, A., Naskar, S., Fan, D., Eddaoudi, M. \& Maurin, G. MOF surface morphology governs interfacial pore architecture and CO2 dynamics in mixed matrix membranes. Chem. Sci. 16, 19519–19531 (2025).

    Article 
    CAS 
    PubMed 
    Google Scholar
    51. Yang, Q. \& Zhong, C. Molecular simulation of carbon dioxide/methane/hydrogen mixture adsorption in metal−organic frameworks. J. Phys. Chem. B. 110, 17776–17783 (2006).

    Article 
    CAS 
    PubMed 
    Google Scholar
    52. Martin, M. G. \& Siepmann, J. I. Transferable potentials for phase equilibria. 1. United-atom description of n-alkanes. J. Phys. Chem. B 102, 2569–2577 (1998).

    Article 
    CAS 
    Google Scholar
    53. Wells, B. A. \& Chaffee, A. L. Ewald summation for molecular simulations. J. Chem. Theory Comput. 11, 3684–3695 (2015).

    Article 
    CAS 
    PubMed 
    Google Scholar
    54. Peng, D.-Y. \& Robinson, D. B. A new two-constant equation of state. Ind. Eng. Chem. Fundam. 15, 59–64 (1976).

    Article 
    CAS 
    Google Scholar
    55. Nosé, S. A unified formulation of the constant temperature molecular dynamics methods. J. Chem. Phys. 81, 511–519 (1984).

    Article 
    ADS 
    Google Scholar
    56. Essmann, U. et al. A smooth particle mesh Ewald method. J. Chem. Phys. 103, 8577–8593 (1995).

    Article 
    ADS 
    CAS 
    Google Scholar
    57. Song, S. et al. Supplementary data for the paper “Scalable quasi-pure MOF membranes for energy-efficient gas separations”. Zenodo https://doi.org/10.5281/zenodo.20067808 (2026).