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

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Synthesis, isotopic enrichment and solid-state NMR characterization of zeolites derived from the assembly, disassembly, organisation, reassembly process. / Bignami, Giulia P. M.; Dawson, Daniel M.; Seymour, Valerie R.; Wheatley, Paul S.; Morris, Russell E.; Ashbrook, Sharon E. .

In: Journal of the American Chemical Society, Vol. 139, No. 14, 12.04.2017, p. 5140-5148.

Research output: Contribution to journalArticlepeer-review

Harvard

Bignami, GPM, Dawson, DM, Seymour, VR, Wheatley, PS, Morris, RE & Ashbrook, SE 2017, 'Synthesis, isotopic enrichment and solid-state NMR characterization of zeolites derived from the assembly, disassembly, organisation, reassembly process', Journal of the American Chemical Society, vol. 139, no. 14, pp. 5140-5148. https://doi.org/10.1021/jacs.7b00386

APA

Bignami, G. P. M., Dawson, D. M., Seymour, V. R., Wheatley, P. S., Morris, R. E., & Ashbrook, S. E. (2017). Synthesis, isotopic enrichment and solid-state NMR characterization of zeolites derived from the assembly, disassembly, organisation, reassembly process. Journal of the American Chemical Society, 139(14), 5140-5148. https://doi.org/10.1021/jacs.7b00386

Vancouver

Bignami GPM, Dawson DM, Seymour VR, Wheatley PS, Morris RE, Ashbrook SE. Synthesis, isotopic enrichment and solid-state NMR characterization of zeolites derived from the assembly, disassembly, organisation, reassembly process. Journal of the American Chemical Society. 2017 Apr 12;139(14):5140-5148. https://doi.org/10.1021/jacs.7b00386

Author

Bignami, Giulia P. M. ; Dawson, Daniel M. ; Seymour, Valerie R. ; Wheatley, Paul S. ; Morris, Russell E. ; Ashbrook, Sharon E. . / Synthesis, isotopic enrichment and solid-state NMR characterization of zeolites derived from the assembly, disassembly, organisation, reassembly process. In: Journal of the American Chemical Society. 2017 ; Vol. 139, No. 14. pp. 5140-5148.

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@article{2b56599316794a7cbcb875aad9bced02,
title = "Synthesis, isotopic enrichment and solid-state NMR characterization of zeolites derived from the assembly, disassembly, organisation, reassembly process",
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.",
author = "Bignami, {Giulia P. M.} and Dawson, {Daniel M.} and Seymour, {Valerie R.} and Wheatley, {Paul S.} and Morris, {Russell E.} and Ashbrook, {Sharon E.}",
note = "We would like to thank the ERC (EU FP7 Consolidator Grant 614290 “EXONMR”), the Leverhulme Trust (IN-2012-094), and EPSRC (EP/K025112/1, EP/L014475/1, and EP/M506631/1 (for GPMB)). S.E.A. would like to thank the Royal Society and the Wolfson Foundation for a merit award. The research data (and/or materials) supporting this publication can be accessed at DOI: 10.17630/d66d1146-5892-4f14-8e41-dfc075a8cd91.",
year = "2017",
month = apr,
day = "12",
doi = "10.1021/jacs.7b00386",
language = "English",
volume = "139",
pages = "5140--5148",
journal = "Journal of the American Chemical Society",
issn = "0002-7863",
publisher = "AMER CHEMICAL SOC",
number = "14",

}

RIS (suitable for import to EndNote) - Download

TY - JOUR

T1 - Synthesis, isotopic enrichment and solid-state NMR characterization of zeolites derived from the assembly, disassembly, organisation, reassembly process

AU - Bignami, Giulia P. M.

AU - Dawson, Daniel M.

AU - Seymour, Valerie R.

AU - Wheatley, Paul S.

AU - Morris, Russell E.

AU - Ashbrook, Sharon E.

N1 - We would like to thank the ERC (EU FP7 Consolidator Grant 614290 “EXONMR”), the Leverhulme Trust (IN-2012-094), and EPSRC (EP/K025112/1, EP/L014475/1, and EP/M506631/1 (for GPMB)). S.E.A. would like to thank the Royal Society and the Wolfson Foundation for a merit award. The research data (and/or materials) supporting this publication can be accessed at DOI: 10.17630/d66d1146-5892-4f14-8e41-dfc075a8cd91.

PY - 2017/4/12

Y1 - 2017/4/12

N2 - 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.

AB - 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.

U2 - 10.1021/jacs.7b00386

DO - 10.1021/jacs.7b00386

M3 - Article

VL - 139

SP - 5140

EP - 5148

JO - Journal of the American Chemical Society

JF - Journal of the American Chemical Society

SN - 0002-7863

IS - 14

ER -

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