Skip to content

Research at St Andrews

Synthesis, isotopic enrichment and solid-state NMR characterization of zeolites derived from the assembly, disassembly, organisation, reassembly process

Research output: Contribution to journalArticlepeer-review

DOI

Open Access permissions

Open

Author(s)

Giulia P. M. Bignami, Daniel M. Dawson, Valerie R. Seymour, Paul S. Wheatley, Russell E. Morris, Sharon E. Ashbrook

School/Research organisations

Abstract

The great utility and importance of zeolites in fields as diverse as industrial catalysis and medicine has driven considerable interest in the ability to target new framework types with novel properties and applications. The recently introduced and unconventional assembly, disassembly, organization, reassembly (ADOR) method represents one exciting new approach to obtain solids with targeted structures by selectively disassembling preprepared hydrolytically unstable frameworks and then reassembling the resulting products to form materials with new topologies. However, the hydrolytic mechanisms underlying such a powerful synthetic method are not understood in detail, requiring further investigation of the kinetic behavior and the outcome of reactions under differing conditions. In this work, we report the optimized ADOR synthesis, and subsequent solid-state characterization, of 17O- and doubly 17O- and 29Si-enriched UTL-derived zeolites, by synthesis of 29Si-enriched starting Ge-UTL frameworks and incorporation of 17O from 17O-enriched water during hydrolysis. 17O and 29Si NMR experiments are able to demonstrate that the hydrolysis and rearrangement process occurs over a much longer time scale than seen by diffraction. The observation of unexpectedly high levels of 17O in the bulk zeolitic layers, rather than being confined only to the interlayer spacing, reveals a much more extensive hydrolytic rearrangement than previously thought. This work sheds new light on the role played by water in the ADOR process and provides insight into the detailed mechanism of the structural changes involved.
Close

Details

Original languageEnglish
Pages (from-to)5140-5148
Number of pages9
JournalJournal of the American Chemical Society
Volume139
Issue number14
Early online date20 Mar 2017
DOIs
Publication statusPublished - 12 Apr 2017

Discover related content
Find related publications, people, projects and more using interactive charts.

View graph of relations

Related by author

  1. Following the unusual breathing behaviour of 17O-enriched mixed-metal (Al,Ga)-MIL-53 using NMR crystallography

    Rice, C. M., Davis, Z. H., McKay, D., Bignami, G. P. M., Chitac, R. G., Dawson, D. M., Morris, R. E. & Ashbrook, S. E., 14 Jul 2020, In: Physical Chemistry Chemical Physics. 22, 26, p. 14514-14526 13 p.

    Research output: Contribution to journalArticlepeer-review

  2. 13C pNMR of “crumple zone” Cu(II) isophthalate metal-organic frameworks

    Dawson, D. M., Sansome, C. E. F., McHugh, L. N., McPherson, M. J., McCormick McPherson, L. J., Morris, R. E. & Ashbrook, S. E., 14 May 2019, In: Solid State Nuclear Magnetic Resonance. In press

    Research output: Contribution to journalArticlepeer-review

  3. Hydrolytic stability in hemilabile metal–organic frameworks

    McHugh, L. N., McPherson, M. J., McCormick, L. J., Morris, S. A., Wheatley, P. S., Teat, S. J., McKay, D., Dawson, D. M., Sansome, C. E. F., Ashbrook, S. E., Stone, C. A., Smith, M. W. & Morris, R. E., Nov 2018, In: Nature Chemistry. 10, 11, p. 1096–1102 7 p.

    Research output: Contribution to journalArticlepeer-review

  4. Cost-effective 17O enrichment and NMR spectroscopy of mixed-metal terephthalate metal-organic frameworks

    Bignami, G. P. M., Davis, Z. H., Dawson, D. M., Morris, S. A., Russell, S. E., McKay, D., Parke, R. E., Iuga, D., Morris, R. E. & Ashbrook, S. E., 28 Jan 2018, In: Chemical Science. 9, 4, p. 850-859

    Research output: Contribution to journalArticlepeer-review

  5. In situ solid-state NMR and XRD studies of the ADOR process and the unusual structure of zeolite IPC-6

    Morris, S. A., Bignami, G. P. M., Tian, Y., Navarro-Rojas, M., Firth, D. S., Cejka, J., Wheatley, P. S., Dawson, D. M., Slawinski, W. A., Wragg, D. S., Morris, R. E. & Ashbrook, S. E., Oct 2017, In: Nature Chemistry. 9, 10, p. 1012-1018 7 p.

    Research output: Contribution to journalArticlepeer-review

Related by journal

  1. A deep blue B,N-doped heptacene emitter that shows both thermally activated delayed fluorescence and delayed fluorescence by triplet-triplet annihilation

    Madayanad Suresh, S., Duda, E., Hall, D., Yao, Z., Bagnich, S., Slawin, A. M. Z., Bässler, H., Beljonne, D., Buck, M., Olivier, Y., Köhler, A. & Zysman-Colman, E., 8 Apr 2020, In: Journal of the American Chemical Society. 142, 14, p. 6588–6599

    Research output: Contribution to journalArticlepeer-review

  2. Difluorocarbene generation from TMSCF3: kinetics and mechanism of NaI-mediated and Si-induced anionic chain reactions

    García-Domínguez, A., West, T. H., Primozic, J. J., Grant, K. M., Johnston, C. P., Cumming, G. G., Leach, A. G. & Lloyd-Jones, G. C., 26 Aug 2020, In: Journal of the American Chemical Society. 142, 34, p. 14649-14663

    Research output: Contribution to journalArticlepeer-review

  3. Encoding multiple reactivity modes within a single synthetic replicator

    Robertson, C. C., Kosikova, T. & Philp, D., 15 May 2020, In: Journal of the American Chemical Society. Just Accepted

    Research output: Contribution to journalArticlepeer-review

  4. Facile, room-temperature 17O enrichment of zeolite frameworks revealed by solid-state NMR spectroscopy

    Pugh, S. M., Wright, P. A., Law, D., Thompson, N. & Ashbrook, S. E., 15 Jan 2020, In: Journal of the American Chemical Society. 142, 2, p. 900-906 7 p.

    Research output: Contribution to journalArticlepeer-review

  5. Hydrogenative depolymerization of nylons

    Kumar, A., von Wolff, N., Rauch, M., Zou, Y-Q., Shmul, G., Ben-David, Y., Leitus, G., Avram, L. & Milstein, D., 19 Aug 2020, In: Journal of the American Chemical Society. 142, 33, p. 14267-14275

    Research output: Contribution to journalArticlepeer-review

Related by journal

  1. Journal of the American Chemical Society (Journal)

    David Trevor Richens (Editor)

    2005 → …

    Activity: Publication peer-review and editorial work typesEditor of research journal

ID: 249464908

Top