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Polyarylether-Based 2D Covalent-Organic Frameworks with In-Plane D-A Structures and Tunable Energy Levels for Energy Storage.

ABSTRACT: The robust fully conjugated covalent organic frameworks (COFs) are emerging as a novel type of semi-conductive COFs for optoelectronic and energy devices due to their controllable architectures and easily tunable the highest occupied molecular orbital (HOMO) and the lowest occupied molecular orbital (LUMO) levels. However, the carrier mobility of such materials is still beyond requirements due to limited π-conjugation. In this study, a series of new polyarylether-based COFs are rationally synthesized via a direct reaction between hexadecafluorophthalocyanine (electron acceptor) and octahydroxyphthalocyanine (electron donor). These COFs have typical crystalline layered structures, narrow band gaps as low as ≈0.65 eV and ultra-low resistance (1.31 × 10^-6 S cm^-1 ). Such COFs can be composed of two different metal-sites and contribute improved carrier mobility via layer-altered staking mode according to density functional theory calculation. Due to the narrow pore size of 1.4 nm and promising conductivity, such COFs and electrochemically exfoliated graphene based free-standing films are fabricated for in-plane micro-supercapacitors, which demonstrate excellent volumetric capacitances (28.1 F cm^-3 ) and excellent stability of 10 000 charge-discharge cycling in acidic electrolyte. This study provides a new approach toward dioxin-linked COFs with donor-acceptor structure and easily tunable energy levels for versatile energy storage and optoelectronic devices.

SUBMITTER: Li N

PROVIDER: S-EPMC8867148 | biostudies-literature | 2022 Feb

REPOSITORIES: biostudies-literature

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Polyarylether-Based 2D Covalent-Organic Frameworks with In-Plane D-A Structures and Tunable Energy Levels for Energy Storage.

Li Nana N Jiang Kaiyue K Rodríguez-Hernández Fermín F Mao Haiyan H Han Sheng S Fu Xiaobin X Zhang Jichao J Yang Chongqing C Ke Changchun C Zhuang Xiaodong X

Advanced science (Weinheim, Baden-Wurttemberg, Germany) 20211226 6

The robust fully conjugated covalent organic frameworks (COFs) are emerging as a novel type of semi-conductive COFs for optoelectronic and energy devices due to their controllable architectures and easily tunable the highest occupied molecular orbital (HOMO) and the lowest occupied molecular orbital (LUMO) levels. However, the carrier mobility of such materials is still beyond requirements due to limited π-conjugation. In this study, a series of new polyarylether-based COFs are rationally synthe ...[more]

PMID: 34957678

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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

Polyarylether-Based 2D Covalent-Organic Frameworks with In-Plane D-A Structures and Tunable Energy Levels for Energy Storage.

Publications

Polyarylether-Based 2D Covalent-Organic Frameworks with In-Plane D-A Structures and Tunable Energy Levels for Energy Storage.

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