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Molecular modeling, multinuclear NMR, and diffraction studies in the templated synthesis and characterization of the aluminophosphate molecular sieve STA-2

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Molecular modeling, multinuclear NMR, and diffraction studies in the templated synthesis and characterization of the aluminophosphate molecular sieve STA-2. / Castro, Maria; Seymour, Valerie R.; Carnevale, Diego; Griffin, John M.; Ashbrook, Sharon E.; Wright, Paul A.; Apperley, David C.; Parker, Julia E.; Thompson, Stephen P.; Fecant, Antoine; Bats, Nicolas.

In: The Journal of Physical Chemistry C, Vol. 114, No. 29, 29.07.2010, p. 12698-12710.

Research output: Contribution to journalJournal articlepeer-review

Harvard

Castro, M, Seymour, VR, Carnevale, D, Griffin, JM, Ashbrook, SE, Wright, PA, Apperley, DC, Parker, JE, Thompson, SP, Fecant, A & Bats, N 2010, 'Molecular modeling, multinuclear NMR, and diffraction studies in the templated synthesis and characterization of the aluminophosphate molecular sieve STA-2', The Journal of Physical Chemistry C, vol. 114, no. 29, pp. 12698-12710. https://doi.org/10.1021/jp104120y

APA

Castro, M., Seymour, V. R., Carnevale, D., Griffin, J. M., Ashbrook, S. E., Wright, P. A., Apperley, D. C., Parker, J. E., Thompson, S. P., Fecant, A., & Bats, N. (2010). Molecular modeling, multinuclear NMR, and diffraction studies in the templated synthesis and characterization of the aluminophosphate molecular sieve STA-2. The Journal of Physical Chemistry C, 114(29), 12698-12710. https://doi.org/10.1021/jp104120y

Vancouver

Castro M, Seymour VR, Carnevale D, Griffin JM, Ashbrook SE, Wright PA et al. Molecular modeling, multinuclear NMR, and diffraction studies in the templated synthesis and characterization of the aluminophosphate molecular sieve STA-2. The Journal of Physical Chemistry C. 2010 Jul 29;114(29):12698-12710. https://doi.org/10.1021/jp104120y

Author

Castro, Maria ; Seymour, Valerie R. ; Carnevale, Diego ; Griffin, John M. ; Ashbrook, Sharon E. ; Wright, Paul A. ; Apperley, David C. ; Parker, Julia E. ; Thompson, Stephen P. ; Fecant, Antoine ; Bats, Nicolas. / Molecular modeling, multinuclear NMR, and diffraction studies in the templated synthesis and characterization of the aluminophosphate molecular sieve STA-2. In: The Journal of Physical Chemistry C. 2010 ; Vol. 114, No. 29. pp. 12698-12710.

Bibtex

@article{65df2a76f2994caa8d777bcb065f3b9e,
title = "Molecular modeling, multinuclear NMR, and diffraction studies in the templated synthesis and characterization of the aluminophosphate molecular sieve STA-2",
abstract = "Molecular modeling has been used to assist in the design of a new structure directing agent (SDA) for the synthesis of the AlPO(4) form of STA-2, bis-cliazabicyclooctane-butane (BDAB). This is incorporated as a divalent cation within the large cages of STA-2, as determined via a combination of solid-state (13)C and (15)N MAS NMR, supported by (14)N and (1)H-(15)N HMQC solution NMR and density functional calculations. As prepared AlPO4 STA-2 containing cationic SDA molecules achieves neutrality by the inclusion of hydroxide ions bridging between 5-fold coordinated framework Al atoms. Synchrotron X-ray powder diffraction data of the dehydrated as-prepared form indicates triclinic symmetry (Al(12)P(12)O(48)(OH)(2)center dot BDAB, P1, a = 12.3821(2) angstrom, b = 12.3795(2) angstrom, c = 12.3797(3) angstrom, alpha = 63.3585(8)degrees, 63.4830(7)degrees, gamma = 63.4218(7)) with the distortion from rhombohedral R (3) over bar symmetry resulting from the partial order of hydroxide ions in bridging Al-OH-Al sites within cancrinite cages. Upon calcination in oxygen, the organic SDA is removed, leaving AlPO(4) STA-2 with a pore volume of 0.22 cm(3) g(-1) (R (3) over bar, Al(36)P(36)O(144), a = 12.9270(2) angstrom, c = 30.7976(4) angstrom). Dehydrated calcined AlPO(4) STA-2 has two crystallographically distinct P and Al sites: (31)P MAS NMR resolves the two distinct P sites, and although 27AI MAS NMR only partially resolves the two Al sites, they are separated by MQMAS. Furthermore, 2D (27)Al -> (31)P MQ-J-HETCOR correlation spectroscopy confirms that each framework Al is linked to the two different P sites via AI-O-P connections in a 3:1 ratio (and vice versa for P linked to different Al). The (27)Al and (31)P resonances are assigned to the crystallographic Al and P sites by calculation of the NMR parameters using the CASTEP DFT program for an energy-minimized AlPO(4)(SAT) framework.",
keywords = "UNIVERSAL FORCE-FIELD, CRYSTALLINE INORGANIC SOLIDS, QUANTUM MAS NMR, 1ST-PRINCIPLES CALCULATIONS, MICROCRYSTAL DIFFRACTION, QUADRUPOLAR NUCLEI, RESOLUTION, CATALYSTS, ASSIGNMENT, PARAMETERS",
author = "Maria Castro and Seymour, {Valerie R.} and Diego Carnevale and Griffin, {John M.} and Ashbrook, {Sharon E.} and Wright, {Paul A.} and Apperley, {David C.} and Parker, {Julia E.} and Thompson, {Stephen P.} and Antoine Fecant and Nicolas Bats",
year = "2010",
month = jul,
day = "29",
doi = "10.1021/jp104120y",
language = "English",
volume = "114",
pages = "12698--12710",
journal = "The Journal of Physical Chemistry C",
issn = "1932-7447",
publisher = "American Chemical Society",
number = "29",

}

RIS

TY - JOUR

T1 - Molecular modeling, multinuclear NMR, and diffraction studies in the templated synthesis and characterization of the aluminophosphate molecular sieve STA-2

AU - Castro, Maria

AU - Seymour, Valerie R.

AU - Carnevale, Diego

AU - Griffin, John M.

AU - Ashbrook, Sharon E.

AU - Wright, Paul A.

AU - Apperley, David C.

AU - Parker, Julia E.

AU - Thompson, Stephen P.

AU - Fecant, Antoine

AU - Bats, Nicolas

PY - 2010/7/29

Y1 - 2010/7/29

N2 - Molecular modeling has been used to assist in the design of a new structure directing agent (SDA) for the synthesis of the AlPO(4) form of STA-2, bis-cliazabicyclooctane-butane (BDAB). This is incorporated as a divalent cation within the large cages of STA-2, as determined via a combination of solid-state (13)C and (15)N MAS NMR, supported by (14)N and (1)H-(15)N HMQC solution NMR and density functional calculations. As prepared AlPO4 STA-2 containing cationic SDA molecules achieves neutrality by the inclusion of hydroxide ions bridging between 5-fold coordinated framework Al atoms. Synchrotron X-ray powder diffraction data of the dehydrated as-prepared form indicates triclinic symmetry (Al(12)P(12)O(48)(OH)(2)center dot BDAB, P1, a = 12.3821(2) angstrom, b = 12.3795(2) angstrom, c = 12.3797(3) angstrom, alpha = 63.3585(8)degrees, 63.4830(7)degrees, gamma = 63.4218(7)) with the distortion from rhombohedral R (3) over bar symmetry resulting from the partial order of hydroxide ions in bridging Al-OH-Al sites within cancrinite cages. Upon calcination in oxygen, the organic SDA is removed, leaving AlPO(4) STA-2 with a pore volume of 0.22 cm(3) g(-1) (R (3) over bar, Al(36)P(36)O(144), a = 12.9270(2) angstrom, c = 30.7976(4) angstrom). Dehydrated calcined AlPO(4) STA-2 has two crystallographically distinct P and Al sites: (31)P MAS NMR resolves the two distinct P sites, and although 27AI MAS NMR only partially resolves the two Al sites, they are separated by MQMAS. Furthermore, 2D (27)Al -> (31)P MQ-J-HETCOR correlation spectroscopy confirms that each framework Al is linked to the two different P sites via AI-O-P connections in a 3:1 ratio (and vice versa for P linked to different Al). The (27)Al and (31)P resonances are assigned to the crystallographic Al and P sites by calculation of the NMR parameters using the CASTEP DFT program for an energy-minimized AlPO(4)(SAT) framework.

AB - Molecular modeling has been used to assist in the design of a new structure directing agent (SDA) for the synthesis of the AlPO(4) form of STA-2, bis-cliazabicyclooctane-butane (BDAB). This is incorporated as a divalent cation within the large cages of STA-2, as determined via a combination of solid-state (13)C and (15)N MAS NMR, supported by (14)N and (1)H-(15)N HMQC solution NMR and density functional calculations. As prepared AlPO4 STA-2 containing cationic SDA molecules achieves neutrality by the inclusion of hydroxide ions bridging between 5-fold coordinated framework Al atoms. Synchrotron X-ray powder diffraction data of the dehydrated as-prepared form indicates triclinic symmetry (Al(12)P(12)O(48)(OH)(2)center dot BDAB, P1, a = 12.3821(2) angstrom, b = 12.3795(2) angstrom, c = 12.3797(3) angstrom, alpha = 63.3585(8)degrees, 63.4830(7)degrees, gamma = 63.4218(7)) with the distortion from rhombohedral R (3) over bar symmetry resulting from the partial order of hydroxide ions in bridging Al-OH-Al sites within cancrinite cages. Upon calcination in oxygen, the organic SDA is removed, leaving AlPO(4) STA-2 with a pore volume of 0.22 cm(3) g(-1) (R (3) over bar, Al(36)P(36)O(144), a = 12.9270(2) angstrom, c = 30.7976(4) angstrom). Dehydrated calcined AlPO(4) STA-2 has two crystallographically distinct P and Al sites: (31)P MAS NMR resolves the two distinct P sites, and although 27AI MAS NMR only partially resolves the two Al sites, they are separated by MQMAS. Furthermore, 2D (27)Al -> (31)P MQ-J-HETCOR correlation spectroscopy confirms that each framework Al is linked to the two different P sites via AI-O-P connections in a 3:1 ratio (and vice versa for P linked to different Al). The (27)Al and (31)P resonances are assigned to the crystallographic Al and P sites by calculation of the NMR parameters using the CASTEP DFT program for an energy-minimized AlPO(4)(SAT) framework.

KW - UNIVERSAL FORCE-FIELD

KW - CRYSTALLINE INORGANIC SOLIDS

KW - QUANTUM MAS NMR

KW - 1ST-PRINCIPLES CALCULATIONS

KW - MICROCRYSTAL DIFFRACTION

KW - QUADRUPOLAR NUCLEI

KW - RESOLUTION

KW - CATALYSTS

KW - ASSIGNMENT

KW - PARAMETERS

U2 - 10.1021/jp104120y

DO - 10.1021/jp104120y

M3 - Journal article

VL - 114

SP - 12698

EP - 12710

JO - The Journal of Physical Chemistry C

JF - The Journal of Physical Chemistry C

SN - 1932-7447

IS - 29

ER -