Kinetics and mechanism of the hydrolysis and rearrangement processes within the assembly-disassembly-organization-reassembly synthesis of zeolites

Susan Elizabeth Henkelis; Michal Mazur; Cameron Mark Rice; Paul Stewart Wheatley; Sharon E. Ashbrook; Russell Edward Morris

doi:10.1021/jacs.9b00643

Kinetics and mechanism of the hydrolysis and rearrangement processes within the assembly-disassembly-organization-reassembly synthesis of zeolites

Susan Elizabeth Henkelis, Michal Mazur, Cameron Mark Rice, Paul Stewart Wheatley, Sharon E. Ashbrook, Russell Edward Morris

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Abstract

The hydrolysis (disassembly, D) and rearrangement (organization, O) steps of the assembly-disassembly-organization-reassembly (ADOR) process for the synthesis of zeolites have been studied. Germanium–rich UTL was subjected to hydrolysis conditions in water to understand the effects of temperature (100, 92, 85, 81, 77, and 70 °C). Samples were taken periodically over an 8–37 h period and each sample was analyzed by powder X-ray diffraction. The results show that the hydrolysis step is solely dependent on the presence of liquid water, whereas the rearrangement is dependent on the temperature of the system. The kinetics have been investigated using the Avrami-Erofeev model. With increasing temperature, an increase in rate of reaction for the rearrangement step was observed and the Arrhenius equation was used to ascertain an apparent activation energy for the rearrangement from the kinetic product of the disassembly (IPC-1P) to the thermodynamic product of the rearrangement (IPC-2P). From this information a mechanism for this transformation can be postulated.

Original language	English
Pages (from-to)	4453-4459
Number of pages	7
Journal	Journal of the American Chemical Society
Volume	141
Issue number	10
Early online date	20 Feb 2019
DOIs	https://doi.org/10.1021/jacs.9b00643
Publication status	Published - 13 Mar 2019

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Copyright © 2019 American Chemical Society. This is an open access article published under a Creative Commons Attribution (CC-BY) License, which permits unrestricted use, distribution and reproduction in any medium, provided the author and source are cited.
Final published version, 4.22 MBLicence: CC BY

H2020 ERC Advanced Grant 2017 ADOR: H2020 ERC Advanced Grant 2017 ADOR
Morris, R. E. (PI)
European Research Council
1/10/18 → 30/09/23
Project: Fellowship
Assembly Disassembly Reassembly: Assembly disassembly reassembly - New routes to extended structures and their impact
Morris, R. E. (PI)
EPSRC
1/08/13 → 31/07/18
Project: Fellowship
Hemilabile switchable metal-organic: Hemilabile and switchable metal-organic frameworks
Morris, R. E. (PI)
EPSRC
1/03/13 → 28/02/16
Project: Standard

Russell Edward Morris, FRS FRSE FRSC FLSW
- rem1st-andrews.acuk
- School of Chemistry - Bishop Wardlaw Professor
- EaSTCHEM
Person: Academic

Kinetics and mechanism of the hydrolysis and rearrangement processes within the Assembly-Disassembly-Organization-Reassembly synthesis of zeolites (dataset)
Henkelis, S. E. (Creator), Mazur, M. (Creator), Rice, C. M. (Creator), Wheatley, P. S. (Creator), Ashbrook, S. E. M. (Creator) & Morris, R. E. (Creator), University of St Andrews, 2019
DOI: 10.17630/a9b28cba-c559-4f5d-908c-ce121be5241c
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@article{f62ce154749d44b8add733c60f94ea41,

title = "Kinetics and mechanism of the hydrolysis and rearrangement processes within the assembly-disassembly-organization-reassembly synthesis of zeolites",

abstract = "The hydrolysis (disassembly, D) and rearrangement (organization, O) steps of the assembly-disassembly-organization-reassembly (ADOR) process for the synthesis of zeolites have been studied. Germanium–rich UTL was subjected to hydrolysis conditions in water to understand the effects of temperature (100, 92, 85, 81, 77, and 70 °C). Samples were taken periodically over an 8–37 h period and each sample was analyzed by powder X-ray diffraction. The results show that the hydrolysis step is solely dependent on the presence of liquid water, whereas the rearrangement is dependent on the temperature of the system. The kinetics have been investigated using the Avrami-Erofeev model. With increasing temperature, an increase in rate of reaction for the rearrangement step was observed and the Arrhenius equation was used to ascertain an apparent activation energy for the rearrangement from the kinetic product of the disassembly (IPC-1P) to the thermodynamic product of the rearrangement (IPC-2P). From this information a mechanism for this transformation can be postulated.",

author = "Henkelis, {Susan Elizabeth} and Michal Mazur and Rice, {Cameron Mark} and Wheatley, {Paul Stewart} and Ashbrook, {Sharon E.} and Morris, {Russell Edward}",

note = "The authors would like to thank the EPSRC (grants: EP/K025112/1; EP/K005499/1; EP/K503162/1; EP/N509759/1) for funding opportunities. R.E.M., and M.M. would like to acknowledge OP VVV {"}Excellent Research Teams{"}, project No. CZ.02.1.01/0.0/0.0/15_003/0000417 - CUCAM. We would like to thank the ERC (Advanced Grant 787073 “ADOR”).",

year = "2019",

month = mar,

day = "13",

doi = "10.1021/jacs.9b00643",

language = "English",

volume = "141",

pages = "4453--4459",

journal = "Journal of the American Chemical Society",

issn = "0002-7863",

publisher = "American Chemical Society (ACS)",

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Kinetics and mechanism of the hydrolysis and rearrangement processes within the assembly-disassembly-organization-reassembly synthesis of zeolites. / Henkelis, Susan Elizabeth; Mazur, Michal; Rice, Cameron Mark et al.
In: Journal of the American Chemical Society, Vol. 141, No. 10, 13.03.2019, p. 4453-4459.

Research output: Contribution to journal › Article › peer-review

TY - JOUR

T1 - Kinetics and mechanism of the hydrolysis and rearrangement processes within the assembly-disassembly-organization-reassembly synthesis of zeolites

AU - Henkelis, Susan Elizabeth

AU - Mazur, Michal

AU - Rice, Cameron Mark

AU - Wheatley, Paul Stewart

AU - Ashbrook, Sharon E.

AU - Morris, Russell Edward

N1 - The authors would like to thank the EPSRC (grants: EP/K025112/1; EP/K005499/1; EP/K503162/1; EP/N509759/1) for funding opportunities. R.E.M., and M.M. would like to acknowledge OP VVV "Excellent Research Teams", project No. CZ.02.1.01/0.0/0.0/15_003/0000417 - CUCAM. We would like to thank the ERC (Advanced Grant 787073 “ADOR”).

PY - 2019/3/13

Y1 - 2019/3/13

N2 - The hydrolysis (disassembly, D) and rearrangement (organization, O) steps of the assembly-disassembly-organization-reassembly (ADOR) process for the synthesis of zeolites have been studied. Germanium–rich UTL was subjected to hydrolysis conditions in water to understand the effects of temperature (100, 92, 85, 81, 77, and 70 °C). Samples were taken periodically over an 8–37 h period and each sample was analyzed by powder X-ray diffraction. The results show that the hydrolysis step is solely dependent on the presence of liquid water, whereas the rearrangement is dependent on the temperature of the system. The kinetics have been investigated using the Avrami-Erofeev model. With increasing temperature, an increase in rate of reaction for the rearrangement step was observed and the Arrhenius equation was used to ascertain an apparent activation energy for the rearrangement from the kinetic product of the disassembly (IPC-1P) to the thermodynamic product of the rearrangement (IPC-2P). From this information a mechanism for this transformation can be postulated.

AB - The hydrolysis (disassembly, D) and rearrangement (organization, O) steps of the assembly-disassembly-organization-reassembly (ADOR) process for the synthesis of zeolites have been studied. Germanium–rich UTL was subjected to hydrolysis conditions in water to understand the effects of temperature (100, 92, 85, 81, 77, and 70 °C). Samples were taken periodically over an 8–37 h period and each sample was analyzed by powder X-ray diffraction. The results show that the hydrolysis step is solely dependent on the presence of liquid water, whereas the rearrangement is dependent on the temperature of the system. The kinetics have been investigated using the Avrami-Erofeev model. With increasing temperature, an increase in rate of reaction for the rearrangement step was observed and the Arrhenius equation was used to ascertain an apparent activation energy for the rearrangement from the kinetic product of the disassembly (IPC-1P) to the thermodynamic product of the rearrangement (IPC-2P). From this information a mechanism for this transformation can be postulated.

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JO - Journal of the American Chemical Society

JF - Journal of the American Chemical Society

IS - 10

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Kinetics and mechanism of the hydrolysis and rearrangement processes within the assembly-disassembly-organization-reassembly synthesis of zeolites

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Projects

H2020 ERC Advanced Grant 2017 ADOR: H2020 ERC Advanced Grant 2017 ADOR

Assembly Disassembly Reassembly: Assembly disassembly reassembly - New routes to extended structures and their impact

Hemilabile switchable metal-organic: Hemilabile and switchable metal-organic frameworks

Profiles

Russell Edward Morris, FRS FRSE FRSC FLSW

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Kinetics and mechanism of the hydrolysis and rearrangement processes within the Assembly-Disassembly-Organization-Reassembly synthesis of zeolites (dataset)

Cite this