Hydrogen Bonding Between Ions of Like Charge in Ionic Liquids Characterized by NMR Deuteron Quadrupole Coupling Constants—Comparison with Salt Bridges and Molecular Systems | Sciact - CRIS-система Института катализа

Hydrogen Bonding Between Ions of Like Charge in Ionic Liquids Characterized by NMR Deuteron Quadrupole Coupling Constants—Comparison with Salt Bridges and Molecular Systems Обзор

Журнал

Angewandte Chemie - International Edition
ISSN: 1433-7851 , E-ISSN: 1521-3773

Вых. Данные

Год: 2019, Том: 58, Номер: 49, Страницы: 17863-17871 Страниц : 9 DOI: 10.1002/anie.201912476

Ключевые слова

DFT calculations; hydrogen bonding; ionic liquids; molecular-dynamics simulations; solid-state NMR

Авторы

Khudozhitkov Alexander E. ^1,5 , Neumann Jan ² , Niemann Thomas ² , Zaitsau Dzmitry ³ , Stange Peter ² , Paschek Dietmar ² , Stepanov Alexander G. ^1,5 , Kolokolov Daniil I. ^1,5 , Ludwig Ralf ^2,3,4

Организации

1	Boreskov Institute of Catalysis, Siberian Branch of Russian Academy of Sciences, Prospekt Akademika Lavrentieva 5, Novosibirsk 630090 (Russia)
2	Universität Rostock, Institut für Chemie, Abteilung für Physikalische Chemie, Dr.-Lorenz-Weg 2, 18059 Rostock (Germany)
3	Department LL&M, University of Rostock, Albert-Einstein-Str. 25, 18059 Rostock (Germany)
4	Leibniz-Institut für Katalyse an der Universität Rostock e.V., Albert-Einstein-Str. 29a, 18059 Rostock (Germany)
5	Novosibirsk State University, Pirogova Street 2, Novosibirsk 630090 (Russia)

Информация о финансировании (4)

1	Федеральное агентство научных организаций России	0303-2016-0003
2	Rostock University
3	German Research Foundation	LU 506/14-1
4	German Research Foundation	LU 506/14-2 (286149019)

We present deuteron quadrupole coupling constants (DQCC) for hydroxyl-functionalized ionic liquids (ILs) in the crystalline or glassy states characterizing two types of hydrogen bonding: The regular Coulomb-enhanced hydrogen bonds between cation and anion (c–a), and the unusual hydrogen bonds between cation and cation (c–c), which are present despite repulsive Coulomb forces. We measure these sensitive probes of hydrogen bonding by means of solid-state NMR spectroscopy. The DQCCs of (c–a) ion pairs and (c–c) H-bonds are compared to those of salt bridges in supramolecular complexes and those present in molecular liquids. At low temperatures, the (c–c) species successfully compete with the (c–a) ion pairs and dominate the cluster populations. Equilibrium constants obtained from molecular-dynamics (MD) simulations show van't Hoff behavior with small transition enthalpies between the differently H-bonded species. We show that cationic-cluster formation prevents these ILs from crystallizing. With cooling, the (c–c) hydrogen bonds persist, resulting in supercooling and glass formation. © 2019 The Authors. Published by Wiley-VCH Verlag GmbH & Co. KGaA.

Khudozhitkov A.E. , Neumann J. , Niemann T. , Zaitsau D. , Stange P. , Paschek D. , Stepanov A.G. , Kolokolov D.I. , Ludwig R.
Hydrogen Bonding Between Ions of Like Charge in Ionic Liquids Characterized by NMR Deuteron Quadrupole Coupling Constants—Comparison with Salt Bridges and Molecular Systems

Angewandte Chemie - International Edition. 2019. V.58. N49. P.17863-17871. DOI: 10.1002/anie.201912476 WOS Scopus РИНЦ CAPlusCA PMID OpenAlex

Полный текст от издателя

Поступила в редакцию:	30 сент. 2019 г.
Принята к публикации:	6 окт. 2019 г.
Опубликована online:	31 окт. 2019 г.
Опубликована в печати:	2 дек. 2019 г.

Web of science:	WOS:000501293400057
Scopus:	2-s2.0-85074818635
РИНЦ:	43211141
Chemical Abstracts:	2019:2082475
Chemical Abstracts (print):	172:15412
PMID (PubMed):	31588622
OpenAlex:	W2977353509

БД	Цитирований
Scopus	45
Web of science	39
РИНЦ	38
OpenAlex	41