A Close View of the Organic Linker in a MOF: Structural Insights from a Combined 1H NMR Relaxometry and Computational Investigation | Sciact - CRIS-система Института катализа

A Close View of the Organic Linker in a MOF: Structural Insights from a Combined 1H NMR Relaxometry and Computational Investigation Научная публикация

Журнал

PCCP: Physical Chemistry Chemical Physics
ISSN: 1463-9076 , E-ISSN: 1463-9084

Вых. Данные

Год: 2020, Том: 22, Номер: 27, Страницы: 15222-15230 Страниц : 9 DOI: 10.1039/d0cp01863e

Ключевые слова

TEREPHTHALATE PHENYLENES; ROTATIONAL-DYNAMICS; HEAT TRANSFORMATION; FRAMEWORKS; N-14; RELAXATION; MOBILITY; SEPARATION; STORAGE

Авторы

Pizzanelli Silvia ¹ , Monti Susanna ¹ , Gordeeva Larisa G. ^2,3 , Solovyeva Marina V. ^2,3 , Freni Angelo ¹ , Forte Claudia ¹

Организации

1	CNR-ICCOM, Institute of the Chemistry of Organometallic Compounds, via G. Moruzzi 1, 56124 Pisa, Italy
2	Boreskov Institute of Catalysis, Ac. Lavrentiev av. 5, Novosibirsk 630090, Russia
3	Novosibirsk State University, Pirogova str. 1, Novosibirsk 630090, Russia

Информация о финансировании (4)

1	Российский фонд фундаментальных исследований	18-29-04033
2	European Cooperation in Science and Technology	CA15209
3	Tuscany Region	2014-2020 FELIX project
4	BENEFICENTIA Stiftung

The organic linker in a metal organic framework (MOF) affects its adsorption behavior and performance, and its structure and dynamics play a role in the modulation of the adsorption properties. In this work, the combination of 1H nuclear magnetic resonance (NMR) longitudinal relaxometry and theoretical calculations allowed details of the structure and dynamics of the organic linker in the NH2-MIL-125 MOF to be obtained. In particular, fast field cycling (FFC) NMR, applied here for the first time on MOFs, was used to disclose the dynamics of the amino group and its electronic environment through the analysis of the 14N quadrupole relaxation peaks, observed in the frequency interval 0.5–5 MHz, at different temperatures from 25 to 110 °C. The line width of the peaks allowed a lower boundary on the rotational correlation time of the N–H bonds to be set, whereas relevant changes in the amplitudes were interpreted in terms of a change in the orientation of the 14N averaged electric field gradient tensor. The experimental findings were complemented by quantum chemistry calculations and classical molecular dynamics simulations.

Pizzanelli S. , Monti S. , Gordeeva L.G. , Solovyeva M.V. , Freni A. , Forte C.
A Close View of the Organic Linker in a MOF: Structural Insights from a Combined 1H NMR Relaxometry and Computational Investigation

PCCP: Physical Chemistry Chemical Physics. 2020. V.22. N27. P.15222-15230. DOI: 10.1039/d0cp01863e WOS Scopus РИНЦ CAPlus PMID OpenAlex

Полный текст от издателя

Поступила в редакцию:	6 апр. 2020 г.
Принята к публикации:	17 июн. 2020 г.
Опубликована online:	17 июн. 2020 г.
Опубликована в печати:	21 июл. 2020 г.

Web of science:	WOS:000549894000005
Scopus:	2-s2.0-85088246709
РИНЦ:	45401345
Chemical Abstracts:	2020:1179533
PMID (PubMed):	32601632
OpenAlex:	W3036639434

БД	Цитирований
Web of science	6
Scopus	8
РИНЦ	6
OpenAlex	9