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    A fine-tuned fluorinated MOF addresses the needs for trace CO2 removal and air capture using physisorption.

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    jacs2E6b05345.pdf
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    Type
    Article
    Authors
    Bhatt, Prashant
    Belmabkhout, Youssef cc
    Cadiau, Amandine cc
    Adil, Karim cc
    Shekhah, Osama cc
    Shkurenko, Aleksander cc
    Barbour, Leonard J.
    Eddaoudi, Mohamed cc
    KAUST Department
    Advanced Membranes and Porous Materials Research Center
    Chemical Science Program
    Functional Materials Design, Discovery and Development (FMD3)
    Physical Science and Engineering (PSE) Division
    KAUST Grant Number
    CCF/1/1972-02-01
    CCF/1/1972-8-01
    Date
    2016-07-19
    Online Publication Date
    2016-07-19
    Print Publication Date
    2016-07-27
    Permanent link to this record
    http://hdl.handle.net/10754/617133
    
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    Abstract
    The development of functional solid-state materials for carbon capture at low carbon dioxide (CO2) concentrations, from con-fined spaces (<0.5 %) and particularly from air (400 ppm), is of prime importance with respect to energy and environment sustainability. Herein, we report the deliberate construction of a hydrolytically stable fluorinated metal-organic framework (MOF), NbOFFIVE-1-Ni, with the proper pore system (size, shape and functionality), ideal for efficient and effective traces carbon dioxide removal. Markedly, the CO2-selective NbOFFIVE-1-Ni exhibits the highest CO2 gravimetric and volumetric uptake (ca. 1.3 mmol/g and 51.4 cm3.cm-3) for physical adsorbents at 400 ppm CO2 and 298 K. Practically, the NbOFFIVE-1-Ni affords the complete CO2 desorption at 328 K under vacuum with an associated moderate energy input of 54 kJ/mol, typical for the full CO2 desorption in reference physical adsorbents but considerably lower than the conventional chemical sorbents. Noticeably, the contracted square-like channels, affording the close proximity of the fluorine centers, permitted the enhancement of the CO2-framework interactions and subsequently the attainment of an unprecedented CO2-selectivity at very low CO2 concentrations. The precise localization of the adsorbed CO2 at the vicinity of the periodically aligned fluorine centers, promoting the selective adsorption of CO2, is evidenced by the single-crystal X-ray diffraction study on the NbOFFIVE-1-Ni hosting CO2 molecules. Cyclic CO2/N2 mixed-gas column breakthrough experiments under dry and humid conditions corroborate the excellent CO2-selectivity under practical carbon capture conditions. Pertinently, the no-table hydrolytic stability positions the NbOFFIVE-1-Ni as the new benchmark adsorbent for direct air capture and CO2 removal from confined spaces.
    Citation
    A fine-tuned fluorinated MOF addresses the needs for trace CO2 removal and air capture using physisorption. 2016 Journal of the American Chemical Society
    Sponsors
    Research reported in this publication was supported by King Abdullah University of Science and Technology (KAUST) under CCF/1/1972-02-01, CCF/1/1972-6-01 and CCF/1/1972-8-01.
    Publisher
    American Chemical Society (ACS)
    Journal
    Journal of the American Chemical Society
    DOI
    10.1021/jacs.6b05345
    PubMed ID
    27388208
    Additional Links
    http://pubs.acs.org/doi/abs/10.1021/jacs.6b05345
    Relations
    Is Supplemented By:
    • [Dataset]
      Bhatt, P. M., Belmabkhout, Y., Cadiau, A., Adil, K., Shekhah, O., Shkurenko, A., … Eddaoudi, M. (2016). CCDC 1505385: Experimental Crystal Structure Determination [Data set]. Cambridge Crystallographic Data Centre. https://doi.org/10.5517/ccdc.csd.cc1mjgtf. DOI: 10.5517/ccdc.csd.cc1mjgtf HANDLE: 10754/624595
    • [Dataset]
      Bhatt, P. M., Belmabkhout, Y., Cadiau, A., Adil, K., Shekhah, O., Shkurenko, A., … Eddaoudi, M. (2016). CCDC 1505386: Experimental Crystal Structure Determination [Data set]. Cambridge Crystallographic Data Centre. https://doi.org/10.5517/ccdc.csd.cc1mjgvg. DOI: 10.5517/ccdc.csd.cc1mjgvg HANDLE: 10754/624596
    Is Supplemented By:
    • [Dataset]
      . DOI: 10.5517/ccdc.csd.cc1klq62 HANDLE: 10754/663671
    ae974a485f413a2113503eed53cd6c53
    10.1021/jacs.6b05345
    Scopus Count
    Collections
    Articles; Advanced Membranes and Porous Materials Research Center; Physical Science and Engineering (PSE) Division; Functional Materials Design, Discovery and Development (FMD3); Chemical Science Program

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