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

Nature Materials volume 24, pages 1978–1984 (2025)Cite this article

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Abstract

Zeolites 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.

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Fig. 1: Structural models and similarities of zeolites.
Fig. 2: Workflow to match lattices and atoms.
Fig. 3: Screening of potential zeolite intergrowths.
Fig. 4: Network representation of zeolite pairs that can form intergrowths.
Fig. 5: Ex silico synthesis of a predicted zeolite intergrowth.

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Data availability

Optimized 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.

Code availability

The code to generate the zeolite intergrowth models is provided in its supplementary information file.

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Acknowledgements

This 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.

Author information

Authors and Affiliations

  1. Department of Chemical System Engineering, The University of Tokyo, Bunkyo-ku, Tokyo, Japan

    Kota Oishi, Koki Muraoka, Kenta Iyoki, Toru Wakihara, Tatsuya Okubo & Akira Nakayama

  2. Institute of Engineering Innovation, The University of Tokyo, Bunkyo-ku, Tokyo, Japan

    Satoko Toyama, Takeshi Iwata, Takehito Seki, Naoya Shibata & Toru Wakihara

  3. Department of Environment Systems, The University of Tokyo, Kashiwa-shi, Chiba, Japan

    Kenta Iyoki

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  1. Kota Oishi
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Contributions

K.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.

Corresponding authors

Correspondence to Koki Muraoka or Akira Nakayama.

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Nature Materials thanks Miguel Camblor, Russell Morris and German Sastre for their contribution to the peer review of this work.

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Supplementary information

Supplementary Information (download PDF )

Supplementary Figs. 1–14 and Tables 1 and 2.

Supplementary Table 3 (download XLSX )

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 Software 1 (download ZIP )

Supplementary codes, Jupyter notebooks for usage examples, optimized intergrowth structures and structures used in TEM simulations.

Supplementary Data 1 (download CSV )

Raw scatter data for Supplementary Fig. 1.

Supplementary Data 2 (download ZIP )

CIF files to draw Supplementary Figs. 5–7.

Supplementary Data 3 (download CSV )

Raw data for ROC curves in Supplementary Fig. 4.

Supplementary Data 4 (download CSV )

Raw data for the XRD pattern in Supplementary Fig. 9.

Supplementary Data 5 (download CSV )

Raw data for the XRD pattern in Supplementary Fig. 10.

Supplementary Data 6 (download CSV )

Raw data for the XRD pattern in Supplementary Fig. 11.

Source data

Source Data Fig. 3 (download XLSX )

Raw scatter data for Fig. 3b,f.

Source Data Fig. 5 (download XLSX )

Raw data for the XRD pattern.

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Oishi, 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. 24, 1978–1984 (2025). https://doi.org/10.1038/s41563-025-02377-6

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