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Hydrogen-Bonded Water-Aminium Assemblies for Synthesis of Zeotypes with Ordered Heteroatoms

Park, Sung Hwan; Radhakrishnan, Sambhu; Choi, Wanuk; Chandran, C Vinod; Kemp, Kingsley Christian; Breynaert, Eric; Bell, Robert G; ... Hong, Suk Bong; + view all (2022) Hydrogen-Bonded Water-Aminium Assemblies for Synthesis of Zeotypes with Ordered Heteroatoms. Journal of the American Chemical Society , 144 (39) pp. 18054-18061. 10.1021/jacs.2c07661. Green open access

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Abstract

Water plays a central role in the crystallization of a variety of organic, inorganic, biological, and hybrid materials. This is also true for zeolites and zeolite-like materials, an important class of industrial catalysts and adsorbents. Water is always present during their hydrothermal synthesis, either with or without organic species as structure-directing agents. Apart from its role as a solvent or a catalyst, structure direction by water in zeolite synthesis has never been clearly elucidated. Here, we report the crystallization of phosphate-based molecular sieves using rationally designed, hydrogen-bonded water-aminium assemblies, resulting in molecular sieves exhibiting the crystallographic ordering of heteroatoms. We demonstrate that a 1:1 assembly of water and diprotonated N,N-dimethyl-1,2-ethanediamine acts as a structure-directing agent in the synthesis of a silicoaluminophosphate material with phillipsite (PHI) topology, using SMARTER crystallography, which combines single-crystal X-ray diffraction and nuclear magnetic resonance spectroscopy, as well as ab initio molecular dynamics simulations. The molecular arrangement of the hydrogen-bonded assembly matches well with the shape and size of subunits in the PHI structure, and their charge distributions result in the strict ordering of framework tetrahedral atoms. This concept of structure direction by water-containing supramolecular assemblies should be applicable to the synthesis of many classes of porous materials.

Type: Article
Title: Hydrogen-Bonded Water-Aminium Assemblies for Synthesis of Zeotypes with Ordered Heteroatoms
Open access status: An open access version is available from UCL Discovery
DOI: 10.1021/jacs.2c07661
Publisher version: https://doi.org/10.1021/jacs.2c07661
Language: English
Additional information: This version is the author accepted manuscript. For information on re-use, please refer to the publisher’s terms and conditions.
Keywords: Crystallization, Diffraction, Noncovalent interactions, Nuclear magnetic resonance spectroscopy, Supramolecular structures and assemblies
UCL classification: UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences > Dept of Chemistry
UCL > Provost and Vice Provost Offices > UCL BEAMS
UCL
URI: https://discovery.ucl.ac.uk/id/eprint/10156146
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