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Coupling fullerene into porous aromatic frameworks for gas selective sorption.

ABSTRACT: A lot of investigations calculate that fullerene would be an excellent unit for porous adsorbents for gas sorption and separation. Although the conjugated structure and symmetrical shape of fullerene makes it an ideal building block, there is no facile strategy to achieve fullerene-based porous materials. Herein, we adopt a novel acid catalyzed coupling reaction to bind the fullerene molecules together in a one-step synthesis. After synthesizing the adducts as models, the atomic connectivity between the fullerene molecules is determined clearly. We then prepared a series of fullerene-based porous aromatic frameworks (PAFs). The targeted products adsorb H₂ and CO₂, and they exhibit some selectivity of CO₂ over N₂ and CH₄. The good performance of the PAFs indicates that we could combine the gas binding ability of the building block and the porous nature of PAF materials together to give a better adsorbent.

SUBMITTER: Yuan Y

PROVIDER: S-EPMC6008602 | biostudies-literature | 2016 Jun

REPOSITORIES: biostudies-literature

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Coupling fullerene into porous aromatic frameworks for gas selective sorption.

Yuan Ye Y Cui Peng P Tian Yuyang Y Zou Xiaoqin X Zhou Yingxi Y Sun Fuxing F Zhu Guangshan G

Chemical science 20160222 6

A lot of investigations calculate that fullerene would be an excellent unit for porous adsorbents for gas sorption and separation. Although the conjugated structure and symmetrical shape of fullerene makes it an ideal building block, there is no facile strategy to achieve fullerene-based porous materials. Herein, we adopt a novel acid catalyzed coupling reaction to bind the fullerene molecules together in a one-step synthesis. After synthesizing the adducts as models, the atomic connectivity bet ...[more]

PMID: 29997862

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Project description:Several synthetic methods have recently emerged to develop high-surface-area solid-state organic framework-based materials into free-flowing liquids with permanent porosity. The fluidity of these porous liquid (PL) materials provides them with advantages in certain storage and transport processes. However, most framework-based materials necessitate the use of cryogenic temperatures to store weakly bound gases such as H2, temperatures where PLs lose their fluidity. Covalent organic framework (COF)-based PLs that could reversibly form stable complexes with H2 near ambient temperatures would represent a promising development for gas storage and transport applications. We report here the development, characterization, and evaluation of a material with these remarkable characteristics based on Cu(I)-loaded COF colloids. Our synthetic strategy required tailoring conditions for growing robust coatings of poly(dimethylsiloxane)-methacrylate (PDMS-MA) around COF colloids using atom transfer radical polymerization (ATRP). We demonstrate exquisite control over the coating thickness on the colloidal COF, quantified by transmission electron microscopy and dynamic light scattering. The coated COF material was then suspended in a liquid polymer matrix to make a PL. CO2 isotherms confirmed that the coating preserved the general porosity of the COF in the free-flowing liquid, while CO sorption measurements using diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) confirmed the preservation of Cu(I) coordination sites. We then evaluated the gas sorption phenomenon in the Cu(I)-COF-based PLs using DRIFTS and temperature-programmed desorption measurements. In addition to confirming that H2 transport is possible at or near mild refrigeration temperatures with these materials, our observations indicate that H2 diffusion is significantly influenced by the glass-transition temperature of both the coating and the liquid matrix. The latter result underscores an additional potential advantage of PLs in tailoring gas diffusion and storage temperatures through the coating composition.

Dataset Information

Coupling fullerene into porous aromatic frameworks for gas selective sorption.

Publications

Coupling fullerene into porous aromatic frameworks for gas selective sorption.

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