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Mobility and Reactivity of 4-Substituted TEMPO Derivatives in Metal-Organic Framework MIL-53(Al) Научная публикация

Журнал Journal of Physical Chemistry C
ISSN: 1932-7447
Вых. Данные Год: 2016, Том: 120, Номер: 19, Страницы: 10698-10704 Страниц : DOI: 10.1021/acs.jpcc.6b02966
Авторы Poryvaev A. S. 1,2 , Sheveleva A. M. 1,2 , Kolokolov D. I. 2,3 , Stepanov A. G. 2,3 , Bagryanskaya E. G. 2,4 , Fedin M. V. 1,2
Организации
1 (Данные Web of science) RAS, Int Tomog Ctr, SB, Novosibirsk 630090, Russia
2 (Данные Web of science) Novosibirsk State Univ, Novosibirsk 630090, Russia
3 (Данные Web of science) RAS, Boreskov Inst Catalysis, SB, Lavrentiev Av 5, Novosibirsk 630090, Russia
4 (Данные Web of science) RAS, NN Vorozhtsov Novosibirsk Inst Organ Chem, SB, Novosibirsk 630090, Russia

Реферат: 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 mu(2)-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.
Библиографическая ссылка: Poryvaev A.S. , Sheveleva A.M. , Kolokolov D.I. , Stepanov A.G. , Bagryanskaya E.G. , Fedin M.V.
Mobility and Reactivity of 4-Substituted TEMPO Derivatives in Metal-Organic Framework MIL-53(Al)
Journal of Physical Chemistry C. 2016. V.120. N19. P.10698-10704. DOI: 10.1021/acs.jpcc.6b02966 WOS Scopus РИНЦ OpenAlex
Даты:
Опубликована online: 9 мая 2016 г.
Опубликована в печати: 19 мая 2016 г.
Идентификаторы БД:
Web of science: WOS:000376417500064
Scopus: 2-s2.0-84971233968
РИНЦ: 27158015
OpenAlex: W2346758998
Цитирование в БД:
БД Цитирований
Web of science 29
Scopus 26
РИНЦ 27
OpenAlex 28
Альметрики: