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Energy-storage covalent organic frameworks: improving performance via engineering polysulfide chains on walls.

ABSTRACT: The aligned one-dimensional channels found in covalent organic frameworks offer a unique space for energy storage. However, physical isolation of sulfur in the channels is not sufficient to prevent the shuttle of lithium-sulfide intermediates that eventually results in a poor performance of lithium-sulfur energy storage. Herein, we report a strategy based on imine-linked frameworks for addressing this shuttle issue by covalently engineering polysulfide chains on the pore walls. The imine linkages can trigger the polymerization of sulfur to form polysulfide chains and anchor them on the channel walls. The immobilized polysulfide chains suppress the shuttle effect and are highly redox active. This structural evolution induces multifold positive effects on energy storage and achieves improved capacity, sulfur accessibility, rate capability and cycle stability. Our results suggest a porous platform achieved by pore wall engineering for tackling key issues in energy storage.

SUBMITTER: Xu F

PROVIDER: S-EPMC6566448 | biostudies-literature | 2019 Jun

REPOSITORIES: biostudies-literature

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Energy-storage covalent organic frameworks: improving performance <i>via</i> engineering polysulfide chains on walls.

Xu Fei F Yang Shuhao S Chen Xiong X Liu Qianhui Q Li Hejun H Wang Hongqiang H Wei Bingqing B Jiang Donglin D

Chemical science 20190507 23

The aligned one-dimensional channels found in covalent organic frameworks offer a unique space for energy storage. However, physical isolation of sulfur in the channels is not sufficient to prevent the shuttle of lithium-sulfide intermediates that eventually results in a poor performance of lithium-sulfur energy storage. Herein, we report a strategy based on imine-linked frameworks for addressing this shuttle issue by covalently engineering polysulfide chains on the pore walls. The imine linkage ...[more]

PMID: 31360408

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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

Energy-storage covalent organic frameworks: improving performance via engineering polysulfide chains on walls.

Publications

Energy-storage covalent organic frameworks: improving performance <i>via</i> engineering polysulfide chains on walls.

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