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Metal-organic frameworks to satisfy gas upgrading demands: fine-tuning the soc-MOF platform for the operative removal of H2Sстатья
Статья опубликована в высокорейтинговом журнале
Информация о цитировании статьи получена из
Web of Science,
Scopus
Статья опубликована в журнале из списка Web of Science и/или Scopus
Дата последнего поиска статьи во внешних источниках: 21 декабря 2017 г.
- Авторы: Belmabkhout Youssef, Pillai Renjith S., Alezi Dalal, Shekhah Osama, Bhatt Prashant M., Chen Zhijie, Adil Karim, Vaesen Sebastien, De Weireld Guy, Pang Maolin, Suetin Mikhail, Cairns Amy J., Solovyeva Vera, Shkurenko Aleksander, Omar El Tall, Maurin Guillaume, Eddaoudi Mohamed
- Журнал: Journal of Materials Chemistry A
- Том: 5
- Номер: 7
- Год издания: 2017
- Издательство: Royal Society of Chemistry
- Местоположение издательства: United Kingdom
- Первая страница: 3293
- Последняя страница: 3303
- DOI: 10.1039/c6ta09406f
- Аннотация: A cooperative experimental/modeling strategy was used to unveil the structure/gas separation performance relationship for a series of isostructural metal-organic frameworks (MOFs) with soc-topology (square-octahedral) hosting different extra-framework counter ions (NO3-, Cl- and Br-). In3+-, Fe3+-, Ga3+-and the newly isolated Al(III)-based isostructural soc-MOF were extensively studied and evaluated for the separation-based production of high-quality fuels (i.e., CH4, C3H8 and n-C4H10) and olefins. The structural/chemical fine-tuning of the soc-MOF platform promoted equilibrium-based selectivity toward C2+ (C2H6, C2H4, C3H6 C3H8 and n-C4H10) and conferred the desired chemical stability toward H2S. The noted dual chemical stability and gas/vapor selectivity, which have rarely been reported for equilibrium-based separation agents, are essential for the production of high-purity H-2, CH4 and C2+ fractions in high yields. Interestingly, the evaluated soc-MOF analogues exhibited high selectivity for C2H4, C3H6 and n-C4H10. In particular, the Fe, Ga and Al analogues presented relatively enhanced C2+/CH4 adsorption selectivities. Notably, the Ga and Al analogues were found to be technically preferable because their structural integrities and separation performances were maintained upon exposure to H2S, indicating that these materials are highly tolerant to H2S. Therefore, the Ga-soc-MOF was further examined for the selective adsorption of H2S in the presence of CO2-and CH4-containing streams, such as refinery-off gases (ROG) and natural gas (NG). Grand canonical Monte Carlo (GCMC) simulations based on a specific force field describing the interactions between the guest molecules and the Ga sites supported and confirmed the considerably higher affinity of the Ga-soc-MOF for C2+ (as exemplified by n-C4H10) than for CH4. The careful selection of an appropriate metal for the trinuclear inorganic molecular building block (MBB), i. e., a Ga metal center, imbues the soc-MOF platform with the requisite hydrolytic stability, H2S stability, and exceptional gas selectivity for ROG and NG upgrading. Finally, the soc-MOF was deployed as a continuous film on a porous support, and its gas permeation properties as a membrane were evaluated.
- Добавил в систему: Соловьева Вера Александровна