Tailoring the Gating Effect of Organic Cage via a Porous Liquid Approach

Errui Li; Arvind Ganesan; Liqi Qiu; Hongjun Liu; Alexander S. Ivanov; Lilin He; Phattananawee Nalaoh; David M. Jenkins; Tao Wang; Ellie Kim; De en Jiang; Shannon M. Mahurin; Zhenzhen Yang; Sheng Dai

doi:10.1002/adfm.202413668

Tailoring the Gating Effect of Organic Cage via a Porous Liquid Approach

Errui Li, Arvind Ganesan, Liqi Qiu, Hongjun Liu, Alexander S. Ivanov, Lilin He, Phattananawee Nalaoh, David M. Jenkins, Tao Wang, Ellie Kim, De en Jiang, Shannon M. Mahurin, Zhenzhen Yang, Sheng Dai

Research output: Contribution to journal › Article › peer-review

Abstract

Porous liquids (PLs) represent a new frontier in material design combining the merits of solid porous host and liquid phase in gas separation and catalysis. Herein, the PL construction approach is harnessed to tailor the gating effect of organic cages toward enhanced gas separation. A type-II fluorinated PL (F-PL) is developed via liquifying a fluorinated organic cage (F-cage) by a fluorinated ionic liquid (F-IL). The F-cage is featured by a small window size (≈5.1 Å), high surface area, good stability under highly ionic conditions, and abundant fluorine moieties. The F-IL possesses high steric hindrance (bulky cation) and structure similarity with the F-cage (fluorinated alkyl chain in the anion). The existing status structure integrity of F-cage in F-IL upon F-PL formation is illustrated via spectroscopy and X-ray-based techniques. The existence of rigid voids in F-PL is illustrated by positron annihilation lifetime spectroscopy (PALS) and the improved gas uptake capacity than F-IL via pressure-swing CO₂ uptake isotherms (0−40) bar. The comparison of the gas uptake behavior (CO₂, N₂, CH₄, and Xe) of F-PL and F-cage, combining the computational simulation, highlights that the PL construction can be leveraged to tune the window size of porous scaffolds, leading to enhanced gas selectivity.

Original language	English
Journal	Advanced Functional Materials
DOIs	https://doi.org/10.1002/adfm.202413668
State	Accepted/In press - 2024

Funding

The research was supported financially by the Division of Chemical Sciences, Geosciences, and Biosciences, Office of Basic Energy Sciences, US Department of Energy. SAXS and WAXS measurements were enabled by the Major Research Instrumentation program of the National Science Foundation under Award No. DMR\u20101827474. The 28\u2010ID\u20101 beamline of the National Synchrotron Light Source II was used, which is a U.S. Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Brookhaven National Laboratory under Contract No. DE\u2010SC0012704. This research used resources at the High Flux Isotope Reactor [and/or Spallation Neutron Source, a DOE Office of Science User Facility operated by the Oak Ridge National Laboratory.

Keywords

gas separation
gating effect
ionic liquids
organic cage
porous liquids

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10.1002/adfm.202413668

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title = "Tailoring the Gating Effect of Organic Cage via a Porous Liquid Approach",

abstract = "Porous liquids (PLs) represent a new frontier in material design combining the merits of solid porous host and liquid phase in gas separation and catalysis. Herein, the PL construction approach is harnessed to tailor the gating effect of organic cages toward enhanced gas separation. A type-II fluorinated PL (F-PL) is developed via liquifying a fluorinated organic cage (F-cage) by a fluorinated ionic liquid (F-IL). The F-cage is featured by a small window size (≈5.1 {\AA}), high surface area, good stability under highly ionic conditions, and abundant fluorine moieties. The F-IL possesses high steric hindrance (bulky cation) and structure similarity with the F-cage (fluorinated alkyl chain in the anion). The existing status structure integrity of F-cage in F-IL upon F-PL formation is illustrated via spectroscopy and X-ray-based techniques. The existence of rigid voids in F-PL is illustrated by positron annihilation lifetime spectroscopy (PALS) and the improved gas uptake capacity than F-IL via pressure-swing CO2 uptake isotherms (0−40) bar. The comparison of the gas uptake behavior (CO2, N2, CH4, and Xe) of F-PL and F-cage, combining the computational simulation, highlights that the PL construction can be leveraged to tune the window size of porous scaffolds, leading to enhanced gas selectivity.",

keywords = "gas separation, gating effect, ionic liquids, organic cage, porous liquids",

author = "Errui Li and Arvind Ganesan and Liqi Qiu and Hongjun Liu and Ivanov, {Alexander S.} and Lilin He and Phattananawee Nalaoh and Jenkins, {David M.} and Tao Wang and Ellie Kim and Jiang, {De en} and Mahurin, {Shannon M.} and Zhenzhen Yang and Sheng Dai",

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year = "2024",

doi = "10.1002/adfm.202413668",

language = "English",

journal = "Advanced Functional Materials",

issn = "1616-301X",

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T1 - Tailoring the Gating Effect of Organic Cage via a Porous Liquid Approach

AU - Li, Errui

AU - Ganesan, Arvind

AU - Qiu, Liqi

AU - Liu, Hongjun

AU - Ivanov, Alexander S.

AU - He, Lilin

AU - Nalaoh, Phattananawee

AU - Jenkins, David M.

AU - Wang, Tao

AU - Kim, Ellie

AU - Jiang, De en

AU - Mahurin, Shannon M.

AU - Yang, Zhenzhen

AU - Dai, Sheng

PY - 2024

Y1 - 2024

N2 - Porous liquids (PLs) represent a new frontier in material design combining the merits of solid porous host and liquid phase in gas separation and catalysis. Herein, the PL construction approach is harnessed to tailor the gating effect of organic cages toward enhanced gas separation. A type-II fluorinated PL (F-PL) is developed via liquifying a fluorinated organic cage (F-cage) by a fluorinated ionic liquid (F-IL). The F-cage is featured by a small window size (≈5.1 Å), high surface area, good stability under highly ionic conditions, and abundant fluorine moieties. The F-IL possesses high steric hindrance (bulky cation) and structure similarity with the F-cage (fluorinated alkyl chain in the anion). The existing status structure integrity of F-cage in F-IL upon F-PL formation is illustrated via spectroscopy and X-ray-based techniques. The existence of rigid voids in F-PL is illustrated by positron annihilation lifetime spectroscopy (PALS) and the improved gas uptake capacity than F-IL via pressure-swing CO2 uptake isotherms (0−40) bar. The comparison of the gas uptake behavior (CO2, N2, CH4, and Xe) of F-PL and F-cage, combining the computational simulation, highlights that the PL construction can be leveraged to tune the window size of porous scaffolds, leading to enhanced gas selectivity.

AB - Porous liquids (PLs) represent a new frontier in material design combining the merits of solid porous host and liquid phase in gas separation and catalysis. Herein, the PL construction approach is harnessed to tailor the gating effect of organic cages toward enhanced gas separation. A type-II fluorinated PL (F-PL) is developed via liquifying a fluorinated organic cage (F-cage) by a fluorinated ionic liquid (F-IL). The F-cage is featured by a small window size (≈5.1 Å), high surface area, good stability under highly ionic conditions, and abundant fluorine moieties. The F-IL possesses high steric hindrance (bulky cation) and structure similarity with the F-cage (fluorinated alkyl chain in the anion). The existing status structure integrity of F-cage in F-IL upon F-PL formation is illustrated via spectroscopy and X-ray-based techniques. The existence of rigid voids in F-PL is illustrated by positron annihilation lifetime spectroscopy (PALS) and the improved gas uptake capacity than F-IL via pressure-swing CO2 uptake isotherms (0−40) bar. The comparison of the gas uptake behavior (CO2, N2, CH4, and Xe) of F-PL and F-cage, combining the computational simulation, highlights that the PL construction can be leveraged to tune the window size of porous scaffolds, leading to enhanced gas selectivity.

KW - gas separation

KW - gating effect

KW - ionic liquids

KW - organic cage

KW - porous liquids

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DO - 10.1002/adfm.202413668

M3 - Article

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SN - 1616-301X

JO - Advanced Functional Materials

JF - Advanced Functional Materials

ER -

Tailoring the Gating Effect of Organic Cage via a Porous Liquid Approach

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