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    Metal–organic frameworks to satisfy gas upgrading demands: fine-tuning the soc-MOF platform for the operative removal of H2S

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    Type
    Article
    Authors
    Belmabkhout, Youssef cc
    Pillai, Renjith S. cc
    Alezi, Dalal cc
    Shekhah, Osama cc
    Bhatt, Prashant
    Chen, Zhijie cc
    Adil, Karim cc
    Vaesen, Sebastien cc
    De Weireld, Guy
    Pang, Maolin cc
    Suetin, Mikhail cc
    Cairns, Amy
    Solovyeva, Vera cc
    Shkurenko, Aleksander cc
    El Tall, Omar
    Maurin, Guillaume cc
    Eddaoudi, Mohamed cc
    KAUST Department
    Advanced Membranes and Porous Materials Research Center
    Analytical Chemistry Core Lab
    Chemical Science Program
    Functional Materials Design, Discovery and Development (FMD3)
    Physical Science and Engineering (PSE) Division
    Solids
    Technology Transfer
    KAUST Grant Number
    FCC/1/1972-8-01
    146040
    Date
    2017
    Permanent link to this record
    http://hdl.handle.net/10754/623867
    
    Metadata
    Show full item record
    Abstract
    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.
    Citation
    Belmabkhout Y, Pillai RS, Alezi D, Shekhah O, Bhatt PM, et al. (2017) Metal–organic frameworks to satisfy gas upgrading demands: fine-tuning the soc-MOF platform for the operative removal of H2S. J Mater Chem A 5: 3293–3303. Available: http://dx.doi.org/10.1039/c6ta09406f.
    Sponsors
    The authors gratefully acknowledge Internal KAUST FUND FCC/1/1972-8-01. Y. B., P. M. B. and M. E. thank the Aramco-sponsored research fund (contract. 66600024505). R. S. P. and G. M. thank KAUST for providing funding (contract 146040). We would like to acknowledge Dr Hamad Feras from Aramco R&D for his help in performing the initial evaluation of the H<INF>2</INF>S/CO<INF>2</INF>/CH<INF>4</INF> mixtures.
    Publisher
    Royal Society of Chemistry (RSC)
    Journal
    J. Mater. Chem. A
    DOI
    10.1039/c6ta09406f
    Additional Links
    http://pubs.rsc.org/en/Content/ArticleLanding/2017/TA/C6TA09406F#!divAbstract
    Relations
    Is Supplemented By:
    • [Dataset]
      Belmabkhout, Y., Pillai, R. S., Alezi, D., Shekhah, O., Bhatt, P. M., Chen, Z., Adil, K., Vaesen, S., De Weireld, G., Pang, M., Suetin, M., Cairns, A. J., Solovyeva, V., Shkurenko, A., El Tall, O., Maurin, G., & Eddaoudi, M. (2017). CCDC 1510859: Experimental Crystal Structure Determination [Data set]. Cambridge Crystallographic Data Centre. https://doi.org/10.5517/CCDC.CSD.CC1MQ5DX. DOI: 10.5517/ccdc.csd.cc1mq5dx Handle: 10754/663753
    ae974a485f413a2113503eed53cd6c53
    10.1039/c6ta09406f
    Scopus Count
    Collections
    Articles; Advanced Membranes and Porous Materials Research Center; Analytical Chemistry Core Lab; Physical Science and Engineering (PSE) Division; Functional Materials Design, Discovery and Development (FMD3); Chemical Science Program

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