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Tuning the Molecular and Cationic Affinity in a Series of Multifunctional Metal–Organic Frameworks Based on Dodecanuclear Zn(II) Carboxylate Wheels Научная публикация

Журнал Journal of the American Chemical Society
ISSN: 0002-7863 , E-ISSN: 1520-5126
Вых. Данные Год: 2019, Том: 141, Номер: 43, Страницы: 17260-17269 Страниц : 10 DOI: 10.1021/jacs.9b08322
Ключевые слова Adsorption, Alcohols, Hydrocarbons, Metal-organic frameworks, Selectivity
Авторы Lysova Anna A. 1,2 , Samsonenko Denis G. 1,2 , Dorovatovskii Pavel V. 3 , Lazarenko Vladimir A. 3 , Khrustalev Victor N. 4 , Kovalenko Konstantin A. 1,2 , Dybtsev Danil N. 1,2 , Fedin Vladimir P. 1,2
Организации
1 Nikolaev Institute of Inorganic Chemistry, Siberian Branch of the Russian Academy of Sciences, Novosibirsk 630090, Russia
2 Novosibirsk State University, Novosibirsk 630090, Russia
3 National Research Center "Kurchatov Institute", Kurchatov Square 1, Moscow 123182, Russia
4 Peoples' Friendship University of Russia (RUDN University), Miklukho-Maklay Street 6, Moscow 117198, Russia

Реферат: A series of new zinc(II)–thiophene-2,5-dicarboxylate (tdc) MOFs based on novel dodecanuclear wheel-shaped building blocks has been synthesized in almost quantative yields. Single-crystal X-ray diffraction analyses reveal 3D porous frameworks with a complex composition [Zn12(tdc)6(glycolate)6(dabco)3] where glycolate is a deprotonated polyatomic alcohol (ethylene glycol, EgO2, 1; 1,2-propanediol, PrO2, 2; 1,2-butanediol, BuO2, 3; 1,2-pentanediol, PeO2, 4; glycerol, GlO2, 5) and dabco is 1,4-diazo[2.2.2.]bicyclooctane. All compounds 1–5 are isostructural except for pendant groups of the diols decorating the surface of channels. The adsorption of small gases (N2, CO2, CH4, C2H2, C2H4, C2H6) and larger hydrocarbons (benzene, cyclohexane) both in liquid and vapor phases was thoroughly investigated for all compounds. The zero-coverage adsorption enthalpies, Henry constants, and selectivity factors by various models are calculated and discussed. The versatile adsorption functionality of the title series results from the variable nature of the diol and could be tailored for a specific adsorbate system. For example, 1 shows excellent selectivity of benzene over cyclohexane (20:1 for vapors, 92:1 for liquid phase), while 4 demonstrates unprecedented adsorption preference of cyclohexane over benzene (selectivity up to 5:1). The compound 5 demonstrates great adsorption selectivity for CO2/N2 (up to 75.1), CO2/CH4 (up to 7.7), C2H2/CH4 (up to 14.2), and C2H4/CH4 (up to 9.4). Also, due to polar nature of the pores, 5 features size-selective sorption of alkaline metal cations in order Li+ > Na+ > K+ > Cs+ as well as a notable luminescent response for cesium(I) ions and urea.
Библиографическая ссылка: Lysova A.A. , Samsonenko D.G. , Dorovatovskii P.V. , Lazarenko V.A. , Khrustalev V.N. , Kovalenko K.A. , Dybtsev D.N. , Fedin V.P.
Tuning the Molecular and Cationic Affinity in a Series of Multifunctional Metal–Organic Frameworks Based on Dodecanuclear Zn(II) Carboxylate Wheels
Journal of the American Chemical Society. 2019. V.141. N43. P.17260-17269. DOI: 10.1021/jacs.9b08322 WOS Scopus OpenAlex
Даты:
Поступила в редакцию: 2 авг. 2019 г.
Опубликована online: 4 окт. 2019 г.
Опубликована в печати: 30 окт. 2019 г.
Идентификаторы БД:
Web of science: WOS:000493866300031
Scopus: 2-s2.0-85073834690
OpenAlex: W2978013965
Цитирование в БД:
БД Цитирований
Scopus 83
OpenAlex 101
Web of science 91
Альметрики: