Drawing boundaries between feasible and unfeasible zeolite intergrowths using high-throughput computational screening with synthesis validation

Nature Materials (2025)Cite this article 481 Accesses16 AltmetricMetrics detailsZeolites are a class of porous crystalline silicate-based materials with applications such as catalysis and separation. Zeolite intergrowths can have superior performance compared with conventional single-phase zeolites in these applications. This study develops a computational workflow to evaluate ~1.03 trillion atomistic structures to identify promising zeolite intergrowths through geometrical analysis and atomistic simulations. We find that interfacial energy is an excellent descriptor to distinguish hydrothermally synthesized zeolite intergrowths from the others, showing almost-perfect classification performance (area under the curve of 0.995). Computational screening workflow saves 100% of hydrothermally synthesized zeolite pairs and successfully rejects 99.3% of hypothetical pairs. Network analyses reveal that hypothetical pairs comparable to experimentally proven ones show substantial topological and chemical similarities, although such information is not directly used in the screening workflow. One of the hypothetical candidates that passed the criteria is experimentally realized by direct and seed-assisted hydrothermal syntheses, thereby broadening the applicable scope of zeolite intergrowths to zincosilicates with three and nine rings.This is a preview of subscription content, access via your institution Access Nature and 54 other Nature Portfolio journals Get Nature+, our best-value online-access subscription $32.99 / 30 days cancel any timeSubscribe to this journal Receive 12 print issues and online access $259.00 per yearonly $21.58 per issueBuy this articlePrices may be subject to local taxes which are calculated during checkoutOptimized crystal structures of known and promising zeolite intergrowths and the structure for the electron diffraction patterns are provided in the Supplementary Information. Source data are provided with this paper.The code to generate the zeolite intergrowth models is provided in its supplementary information file.Sun, W. et al. The thermodynamic scale of inorganic crystalline metastability. Sci. Adv. 2, e1600225 (2016).Article PubMed PubMed Central Google Scholar Aykol, M., Dwaraknath, S. S., Sun, W. & Persson, K. A. Thermodynamic limit for synthesis of metastable inorganic materials. Sci. Adv. 4, eaaq0148 (2018).Article PubMed PubMed Central Google Scholar Li, Y., Yu, J. & Xu, R. Criteria for zeolite frameworks realizable for target synthesis. Angew. Chem. Int. Ed. 52, 1673–1677 (2013).Article CAS Google Scholar Lee, A. et al. Machine learned synthesizability predictions aided by density functional theory. Commun. Mater. 3, 73 (2022).Article Google Scholar Wang, Y., Tong, C., Liu, Q., Han, R. & Liu, C. Intergrowth zeolites, synthesis, characterization, and catalysis. Chem. Rev. 123, 11664–11721 (2023).Article CAS PubMed Google Scholar Raclariu, A.-M. et al. A fast method for predicting the formation of crystal interfaces and heterocrystals. Comput. Mater. Sci. 108, 88–93 (2015).Article CAS Google Scholar Davis, M. E. Ordered porous materials for emerging applications. Nature 417, 813–821 (2002).Article CAS PubMed Google Scholar Arita, R. et al. Electronic properties of alkali-metal loaded zeolites: supercrystal Mott insulators. Phys. Rev. B 69, 195106 (2004).Article Google Scholar Villaescusa, L. A., Li, J., Mayoral, A., Gao, Z. R. & Camblor, M. A. Sandwich-type zeolite intergrowths with MFI and the novel extra-large pore IDM-1 as ordered end-members. Chem. Mater. 33, 7869–7877 (2021).Article CAS Google Scholar Chen, N. Y., Schlenker, J. L., Garwood, W. E. & Kokotailo, G. T. TMA-offretite. Relationship between structural and catalytic properties. J. Catal. 86, 24–31 (1984).Article CAS Google Scholar Conte, M. et al. Enhanced selectivity to propene in the methanol to hydrocarbons reaction by use of ZSM-5/11 intergrowth zeolite.

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C 115, 443–446 (2011).Article CAS Google Scholar Röhrig, C. & Gies, H. A new zincosilicate zeolite with nine-ring channels. Angew. Chem. Int. Ed. 34, 63–65 (1995).Article Google Scholar Download referencesThis work is primarily funded by JSPS KAKENHI (22K14751 to K.M.) and JST PRESTO (JPMJPR2378 to K.M.). Part of the calculations were performed on supercomputers at CCMS, IMR (Tohoku University, proposal number 202312-SCKXX-0006). K.O. thanks JST SPRING, grant number JPMJSP2108, for financial support. K.I. thanks ERCA (JPMEERF20242M01) for financial support. N.S., T.S. and S.T. acknowledge support from JST ERATO (JPMJER2202). T.S. acknowledges support from JST PRESTO (JPMJPR21AA). S.T. acknowledges support from JST PRESTO (JPMJPR24J7). We acknowledge K. Nayuki and Y. Omori at JEOL for their assistance with the TEM measurements.Department of Chemical System Engineering, The University of Tokyo, Bunkyo-ku, Tokyo, JapanKota Oishi, Koki Muraoka, Kenta Iyoki, Toru Wakihara, Tatsuya Okubo & Akira NakayamaInstitute of Engineering Innovation, The University of Tokyo, Bunkyo-ku, Tokyo, JapanSatoko Toyama, Takeshi Iwata, Takehito Seki, Naoya Shibata & Toru WakiharaDepartment of Environment Systems, The University of Tokyo, Kashiwa-shi, Chiba, JapanKenta IyokiSearch author on:PubMed Google ScholarSearch author on:PubMed Google ScholarSearch author on:PubMed Google ScholarSearch author on:PubMed Google ScholarSearch author on:PubMed Google ScholarSearch author on:PubMed Google ScholarSearch author on:PubMed Google ScholarSearch author on:PubMed Google ScholarSearch author on:PubMed Google ScholarSearch author on:PubMed Google ScholarK.M. conceived and designed the project, and K.M. and A.N. directed it. K.O. and K.M. developed the computer code and analysed the results. K.O. carried out the calculations and synthesized the zeolites. K.I., T.W. and T.O. supervised the synthesis. S.T., T.I., T.S. and N.S. performed the TEM characterization. K.O. and K.M. wrote the paper. All authors revised and approved the paper.Correspondence to Koki Muraoka or Akira Nakayama.The authors declare no competing interests.Nature Materials thanks Miguel Camblor, Russell Morris and German Sastre for their contribution to the peer review of this work.Publisher’s note Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.Supplementary Figs. 1–14 and Tables 1 and 2.Results of the lattice match. It is presented as a separate spreadsheet file. The interfacial area in the table is defined as the minimum area necessary to represent the intergrowth structures within a periodic cell.Supplementary codes, Jupyter notebooks for usage examples, optimized intergrowth structures and structures used in TEM simulations.Raw scatter data for Supplementary Fig. 1.CIF files to draw Supplementary Figs. 5–7.Raw data for ROC curves in Supplementary Fig. 4.Raw data for the XRD pattern in Supplementary Fig. 9.Raw data for the XRD pattern in Supplementary Fig. 10.Raw data for the XRD pattern in Supplementary Fig. 11.Raw scatter data for Fig. 3b,f.Raw data for the XRD pattern.Springer Nature or its licensor (e.g. a society or other partner) holds exclusive rights to this article under a publishing agreement with the author(s) or other rightsholder(s); author self-archiving of the accepted manuscript version of this article is solely governed by the terms of such publishing agreement and applicable law.Reprints and permissionsOishi, K., Muraoka, K., Toyama, S. et al. Drawing boundaries between feasible and unfeasible zeolite intergrowths using high-throughput computational screening with synthesis validation. Nat. Mater. (2025). https://doi.org/10.1038/s41563-025-02377-6Download citationReceived: 31 July 2024Accepted: 12 September 2025Published: 20 October 2025DOI: https://doi.org/10.1038/s41563-025-02377-6Anyone you share the following link with will be able to read this content:Sorry, a shareable link is not currently available for this article. Provided by the Springer Nature SharedIt content-sharing initiative