Zhu, Qiang, Johal, Jay, Widdowson, Daniel E 
ORCID: 0000-0002-5958-0703, Pang, Zhongfu, Li, Boyu, Kane, Christopher M, Kurlin, Vitaliy ORCID: 0000-0001-5328-5351, Day, Graeme M, Little, Marc A and Cooper, Andrew I ORCID: 0000-0003-0201-1021
(2022)
Analogy Powered by Prediction and Structural Invariants: Computationally Led Discovery of a Mesoporous Hydrogen-Bonded Organic Cage Crystal.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 144 (22).
pp. 9893-9901.
Abstract
Mesoporous molecular crystals have potential applications in separation and catalysis, but they are rare and hard to design because many weak interactions compete during crystallization, and most molecules have an energetic preference for close packing. Here, we combine crystal structure prediction (CSP) with structural invariants to continuously qualify the similarity between predicted crystal structures for related molecules. This allows isomorphous substitution strategies, which can be unreliable for molecular crystals, to be augmented by <i>a priori</i> prediction, thus leveraging the power of both approaches. We used this combined approach to discover a rare example of a low-density (0.54 g cm<sup>-3</sup>) mesoporous hydrogen-bonded framework (HOF), <b>3D-CageHOF-1</b>. This structure comprises an organic cage (<b>Cage-3-NH</b><sub><b>2</b></sub>) that was predicted to form kinetically trapped, low-density polymorphs <i>via</i> CSP. Pointwise distance distribution structural invariants revealed five predicted forms of <b>Cage-3-NH</b><sub><b>2</b></sub> that are analogous to experimentally realized porous crystals of a chemically different but geometrically similar molecule, <b>T2</b>. More broadly, this approach overcomes the difficulties in comparing predicted molecular crystals with varying lattice parameters, thus allowing for the systematic comparison of energy-structure landscapes for chemically dissimilar molecules.
| Item Type: | Article |
|---|---|
| Divisions: | Faculty of Science and Engineering > School of Electrical Engineering, Electronics and Computer Science Faculty of Science and Engineering > School of Physical Sciences |
| Depositing User: | Symplectic Admin |
| Date Deposited: | 07 Jul 2022 11:49 |
| Last Modified: | 18 Jan 2023 20:56 |
| DOI: | 10.1021/jacs.2c02653 |
| Open Access URL: | https://doi.org/10.1021/jacs.2c02653 |
| Related URLs: | |
| URI: | https://livrepository.liverpool.ac.uk/id/eprint/3157942 |
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