Selective CO2 adsorption by a new metal-organic framework: synergy between open metal sites and a charged imidazolinium backbone

Dalton Transactions : an International Journal of Inorganic Chemistry
Ilia KochetygovWendy L Queen

Abstract

Metal-organic frameworks (MOFs) are porous, tunable crystalline materials that are attracting widespread scientific attention for their potential use in post-combustion CO2 capture. In this work, we report the synthesis of a new ligand, 1,3-bis(4-carboxyphenyl)-4,5-dihydro-1H-imidazol-3-ium tetrafluoroborate, H2Sp5-BF4, that is subsequently used for the construction of a novel MOF, Cu-Sp5-EtOH. This highly crystalline material has a charged framework that is expected to give rise to high CO2/N2 selectivity. However, the pores of the parent structure could not be accessed due to the presence of strongly coordinated ethanol molecules. After solvent exchange with methanol and subsequently heating Cu-Sp5-MeOH under vacuum, we are able to liberate the solvent providing other small molecules like CO2 access to the inside of the now porous structure, Cu-Sp5. The combination of open metal sites and framework charge leads to an exceptionally high CO2/N2 selectivity, as determined by Ideal Adsorbed Solution Theory (IAST) calculations performed on single-component adsorption isotherms. The CO2/N2 selectivity of Cu-Sp5 reaches a value of over 200 at pressures typically found in post-combustion flue gas (0.15 bar CO2/0.85 bar N2), a value t...Continue Reading

References

Oct 10, 2009·Inorganic Chemistry·Jeong Yong LeeJoseph T Hupp
Apr 16, 2010·Physical Chemistry Chemical Physics : PCCP·Nikola DrenchevKonstantin Hadjiivanov
Dec 7, 2011·Chemical Society Reviews·Jian LiuJun Liu
Feb 23, 2012·Physical Chemistry Chemical Physics : PCCP·Janos SzanyiCharles H F Peden
Apr 24, 2013·Journal of the American Chemical Society·Dong-Xu XueMohamed Eddaoudi
Dec 30, 2014·Acta Crystallographica. Section A, Foundations and Advances·George M Sheldrick
Jan 9, 2015·Acta Crystallographica. Section C, Structural Chemistry·George M Sheldrick
Sep 24, 2015·Physical Chemistry Chemical Physics : PCCP·Cheng-Yu WangAngela D Lueking
Mar 7, 2018·The Journal of Organic Chemistry·Safak Bulut, Wendy L Queen

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Citations

Apr 3, 2020·Chemical Society Reviews·Ülkü Kökçam-DemirChristoph Janiak
Sep 4, 2019·Chemistry, an Asian Journal·Rahul MaityRamanathan Vaidhyanathan
Dec 12, 2020·Frontiers in Chemistry·Tiago J FerreiraIsabel A A C Esteves
Apr 22, 2020·Journal of the American Chemical Society·Francoise M Amombo NoaLars Öhrström
Feb 15, 2019·Langmuir : the ACS Journal of Surfaces and Colloids·Tingting ZhouDawen Zeng

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Methods Mentioned

BETA
NMR
X-ray

Software Mentioned

2013
PerkinElmer
Bruker Topspin
ShelXL
ShelXT
SAINT
SADABS
Olex2
HFIX
pyIAST

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