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Mobility and reactivity of 4-substituted TEMPO derivatives in metal-organic framework MIL-53(Al). / Poryvaev, A. S.; Sheveleva, A. M.; Kolokolov, D. I. et al.

In: Journal of Physical Chemistry C, Vol. 120, No. 19, 19.05.2016, p. 10698-10704.

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Harvard

Poryvaev, AS, Sheveleva, AM, Kolokolov, DI, Stepanov, AG, Bagryanskaya, EG & Fedin, MV 2016, 'Mobility and reactivity of 4-substituted TEMPO derivatives in metal-organic framework MIL-53(Al)', Journal of Physical Chemistry C, vol. 120, no. 19, pp. 10698-10704. https://doi.org/10.1021/acs.jpcc.6b02966

APA

Vancouver

Poryvaev AS, Sheveleva AM, Kolokolov DI, Stepanov AG, Bagryanskaya EG, Fedin MV. Mobility and reactivity of 4-substituted TEMPO derivatives in metal-organic framework MIL-53(Al). Journal of Physical Chemistry C. 2016 May 19;120(19):10698-10704. doi: 10.1021/acs.jpcc.6b02966

Author

Poryvaev, A. S. ; Sheveleva, A. M. ; Kolokolov, D. I. et al. / Mobility and reactivity of 4-substituted TEMPO derivatives in metal-organic framework MIL-53(Al). In: Journal of Physical Chemistry C. 2016 ; Vol. 120, No. 19. pp. 10698-10704.

BibTeX

@article{f17ad859083248dcb6b388b145d9947e,
title = "Mobility and reactivity of 4-substituted TEMPO derivatives in metal-organic framework MIL-53(Al)",
abstract = "Postsynthetic adsorption of stable nitroxide radical probes in diamagnetic nano/mesoporous metal-organic frameworks (MOFs) allows application of electron paramagnetic resonance (EPR) for studying structure, functions, and corresponding guest-host interactions in such MOFs. This approach was recently demonstrated using (2,2,6,6-tetramethylpiperidin-1-yl)oxyl (TEMPO) embedded in structurally flexible MIL-53(Al), with the mobility and reactivity of TEMPO reflecting structural dynamics of MOF. In the present work we embed three derivatives of TEMPO (4-oxo-TEMPO, 4-hydroxo-TEMPO, 4- acetamido-TEMPO) in MIL-53(Al) and investigate structural {"}breathing{"} of this MOF with temperature to gain deeper understanding of underlying guest-host interactions. Different substituents in the piperidine ring lead to different mobility and reactivity of corresponding nitroxides. The obtained EPR data and molecular dynamics calculations show that the efficiency of nitroxide radical reaction with μ2-hydroxo group of MIL-53(Al) strongly correlates with the character of its molecular motion, and the reversibility of this reaction upon structural {"}breathing{"} is a general phenomenon. On the basis of these findings, practical suggestions on selecting spin probes for in-MOF EPR studies are formulated.",
author = "Poryvaev, {A. S.} and Sheveleva, {A. M.} and Kolokolov, {D. I.} and Stepanov, {A. G.} and Bagryanskaya, {E. G.} and Fedin, {M. V.}",
year = "2016",
month = may,
day = "19",
doi = "10.1021/acs.jpcc.6b02966",
language = "English",
volume = "120",
pages = "10698--10704",
journal = "Journal of Physical Chemistry C",
issn = "1932-7447",
publisher = "American Chemical Society",
number = "19",

}

RIS

TY - JOUR

T1 - Mobility and reactivity of 4-substituted TEMPO derivatives in metal-organic framework MIL-53(Al)

AU - Poryvaev, A. S.

AU - Sheveleva, A. M.

AU - Kolokolov, D. I.

AU - Stepanov, A. G.

AU - Bagryanskaya, E. G.

AU - Fedin, M. V.

PY - 2016/5/19

Y1 - 2016/5/19

N2 - Postsynthetic adsorption of stable nitroxide radical probes in diamagnetic nano/mesoporous metal-organic frameworks (MOFs) allows application of electron paramagnetic resonance (EPR) for studying structure, functions, and corresponding guest-host interactions in such MOFs. This approach was recently demonstrated using (2,2,6,6-tetramethylpiperidin-1-yl)oxyl (TEMPO) embedded in structurally flexible MIL-53(Al), with the mobility and reactivity of TEMPO reflecting structural dynamics of MOF. In the present work we embed three derivatives of TEMPO (4-oxo-TEMPO, 4-hydroxo-TEMPO, 4- acetamido-TEMPO) in MIL-53(Al) and investigate structural "breathing" of this MOF with temperature to gain deeper understanding of underlying guest-host interactions. Different substituents in the piperidine ring lead to different mobility and reactivity of corresponding nitroxides. The obtained EPR data and molecular dynamics calculations show that the efficiency of nitroxide radical reaction with μ2-hydroxo group of MIL-53(Al) strongly correlates with the character of its molecular motion, and the reversibility of this reaction upon structural "breathing" is a general phenomenon. On the basis of these findings, practical suggestions on selecting spin probes for in-MOF EPR studies are formulated.

AB - Postsynthetic adsorption of stable nitroxide radical probes in diamagnetic nano/mesoporous metal-organic frameworks (MOFs) allows application of electron paramagnetic resonance (EPR) for studying structure, functions, and corresponding guest-host interactions in such MOFs. This approach was recently demonstrated using (2,2,6,6-tetramethylpiperidin-1-yl)oxyl (TEMPO) embedded in structurally flexible MIL-53(Al), with the mobility and reactivity of TEMPO reflecting structural dynamics of MOF. In the present work we embed three derivatives of TEMPO (4-oxo-TEMPO, 4-hydroxo-TEMPO, 4- acetamido-TEMPO) in MIL-53(Al) and investigate structural "breathing" of this MOF with temperature to gain deeper understanding of underlying guest-host interactions. Different substituents in the piperidine ring lead to different mobility and reactivity of corresponding nitroxides. The obtained EPR data and molecular dynamics calculations show that the efficiency of nitroxide radical reaction with μ2-hydroxo group of MIL-53(Al) strongly correlates with the character of its molecular motion, and the reversibility of this reaction upon structural "breathing" is a general phenomenon. On the basis of these findings, practical suggestions on selecting spin probes for in-MOF EPR studies are formulated.

UR - http://www.scopus.com/inward/record.url?scp=84971233968&partnerID=8YFLogxK

U2 - 10.1021/acs.jpcc.6b02966

DO - 10.1021/acs.jpcc.6b02966

M3 - Article

AN - SCOPUS:84971233968

VL - 120

SP - 10698

EP - 10704

JO - Journal of Physical Chemistry C

JF - Journal of Physical Chemistry C

SN - 1932-7447

IS - 19

ER -

ID: 23331373