Graph similarity drives zeolite diffusionless transformations and intergrowth
Name
20190812_Manuscript.pdf
Description
Accepted version
Size
3.15 MB
Format
Adobe PDF
Checksum (MD5)
5804f21299dfcaa2f58ff003281b6372
Author(s)
Schwalbe-Koda, Daniel
Jensen, Zach
Olivetti, Elsa A.
Gomez-Bombarelli, Rafael
Date Issued
October 2019
Journal
Nature Materials
Publisher
Springer Science and Business Media LLC
Citation
Schwalbe-Koda, Daniel et al., "Graph similarity drives zeolite diffusionless transformations and intergrowth" Nature Materials 18, 11 (November 2019): 1177–81 10.1038/s41563-019-0486-1 ©2019
Version
Author's final manuscript
Abstract
Predicting and directing polymorphic transformations is a critical challenge in zeolite synthesis1–3. Interzeolite transformations enable selective crystallization4–7, but are often too complex to be designed by comparing crystal structures. Here, computational and theoretical tools are combined to both exhaustively data mine polymorphic transformations reported in the literature and analyse and explain interzeolite relations. It was found that crystallographic building units are weak predictors of topology interconversion and insufficient to explain intergrowth. By introducing a supercell-invariant metric that compares crystal structures using graph theory, we show that diffusionless (topotactic and reconstructive) transformations occur only between graph-similar pairs. Furthermore, all the known instances of intergrowth occur between either structurally similar or graph similar frameworks. We identify promising pairs to realize diffusionless transformations and intergrowth, with hundreds of low-distance pairs identified among known zeolites, and thousands of hypothetical frameworks connected to known zeolite counterparts. The theory may enable the understanding and control of zeolite polymorphism. ©2019, The Author(s), under exclusive licence to Springer Nature Limited.
MIT Department
Massachusetts Institute of Technology. Department of Materials Science and Engineering
Terms of Use
Article is made available in accordance with the publisher's policy and may be subject to US copyright law. Please refer to the publisher's site for terms of use.
Persistent DSpace Link
DOI of Published Version
https://doi.org/10.1038/S41563-019-0486-1
