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Outstanding Charge Mobility by Band Transport in Two-Dimensional Semiconducting Covalent Organic Frameworks.


ABSTRACT: Two-dimensional covalent organic frameworks (2D COFs) represent a family of crystalline porous polymers with a long-range order and well-defined open nanochannels that hold great promise for electronics, catalysis, sensing, and energy storage. To date, the development of highly conductive 2D COFs has remained challenging due to the finite π-conjugation along the 2D lattice and charge localization at grain boundaries. Furthermore, the charge transport mechanism within the crystalline framework remains elusive. Here, time- and frequency-resolved terahertz spectroscopy reveals intrinsically Drude-type band transport of charge carriers in semiconducting 2D COF thin films condensed by 1,3,5-tris(4-aminophenyl)benzene (TPB) and 1,3,5-triformylbenzene (TFB). The TPB-TFB COF thin films demonstrate high photoconductivity with a long charge scattering time exceeding 70 fs at room temperature which resembles crystalline inorganic materials. This corresponds to a record charge carrier mobility of 165 ± 10 cm2 V-1 s-1, vastly outperforming that of the state-of-the-art conductive COFs. These results reveal TPB-TFB COF thin films as promising candidates for organic electronics and catalysis and provide insights into the rational design of highly crystalline porous materials for efficient and long-range charge transport.

SUBMITTER: Fu S 

PROVIDER: S-EPMC9052747 | biostudies-literature | 2022 Apr

REPOSITORIES: biostudies-literature

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Outstanding Charge Mobility by Band Transport in Two-Dimensional Semiconducting Covalent Organic Frameworks.

Fu Shuai S   Jin Enquan E   Jin Enquan E   Hanayama Hiroki H   Zheng Wenhao W   Zhang Heng H   Di Virgilio Lucia L   Addicoat Matthew A MA   Mezger Markus M   Narita Akimitsu A   Bonn Mischa M   Müllen Klaus K   Wang Hai I HI  

Journal of the American Chemical Society 20220414 16


Two-dimensional covalent organic frameworks (2D COFs) represent a family of crystalline porous polymers with a long-range order and well-defined open nanochannels that hold great promise for electronics, catalysis, sensing, and energy storage. To date, the development of highly conductive 2D COFs has remained challenging due to the finite π-conjugation along the 2D lattice and charge localization at grain boundaries. Furthermore, the charge transport mechanism within the crystalline framework re  ...[more]

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