A fine-tuned fluorinated MOF addresses the needs for trace CO2 removal and air capture using physisorption.
Type
ArticleAuthors
Bhatt, PrashantBelmabkhout, Youssef
Cadiau, Amandine
Adil, Karim
Shekhah, Osama
Shkurenko, Aleksander
Barbour, Leonard J.
Eddaoudi, Mohamed
KAUST Department
Advanced Membranes and Porous Materials Research CenterChemical Science Program
Functional Materials Design, Discovery and Development (FMD3)
Physical Science and Engineering (PSE) Division
KAUST Grant Number
CCF/1/1972-02-01CCF/1/1972-8-01
Online Publication Date
2016-07-19Print Publication Date
2016-07-27Date
2016-07-19Abstract
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 SocietyAcknowledgements
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 SocietyDOI
10.1021/jacs.6b05345PubMed ID
27388208Additional Links
http://pubs.acs.org/doi/abs/10.1021/jacs.6b05345Relations
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
- [Dataset]
. DOI: 10.5517/ccdc.csd.cc1klq62 HANDLE: 10754/663671