Acid Exfoliation of Imine-linked Covalent Organic Frameworks Enables Solution Processing into Crystalline Thin Films

David W Burke; Chao Sun; Ioannina Castano; Nathan C Flanders; Austin M Evans; Edon Vitaku; David C McLeod; Robert H Lambeth; Lin X Chen; Nathan C Gianneschi; William R Dichtel

doi:10.1002/anie.201913975

Acid Exfoliation of Imine-linked Covalent Organic Frameworks Enables Solution Processing into Crystalline Thin Films

David W Burke, Chao Sun, Ioannina Castano, Nathan C Flanders, Austin M Evans, Edon Vitaku, David C McLeod, Robert H Lambeth, Lin X Chen, Nathan C Gianneschi, William R Dichtel

Research output: Contribution to journal/Conference contribution in journal/Contribution to newspaper › Journal article › Research › peer-review

Abstract

Covalent organic frameworks (COFs) are highly modular porous crystalline polymers that are of interest for applications such as charge-storage devices, nanofiltration membranes, and optoelectronic devices. COFs are typically synthesized as microcrystalline powders, which limits their performance in these applications, and their limited solubility precludes large-scale processing into more useful morphologies and devices. We report a general, scalable method to exfoliate two-dimensional imine-linked COF powders by temporarily protonating their linkages. The resulting suspensions were cast into continuous crystalline COF films up to 10 cm in diameter, with thicknesses ranging from 50 nm to 20 μm depending on the suspension composition, concentration, and casting protocol. Furthermore, we demonstrate that the film fabrication process proceeds through a partial depolymerization/repolymerization mechanism, providing mechanically robust films that can be easily separated from their substrates.

Original language	English
Journal	Angewandte Chemie International Edition
Volume	59
Issue	13
Pages (from-to)	5165-5171
Number of pages	7
ISSN	1433-7851
DOIs	https://doi.org/10.1002/anie.201913975
Publication status	Published - 23 Mar 2020

Keywords

covalent organic frameworks
exfoliation
nanosheets
polymers
solution processing

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10.1002/anie.201913975

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Burke, D. W., Sun, C., Castano, I., Flanders, N. C., Evans, A. M., Vitaku, E., McLeod, D. C., Lambeth, R. H., Chen, L. X., Gianneschi, N. C., & Dichtel, W. R. (2020). Acid Exfoliation of Imine-linked Covalent Organic Frameworks Enables Solution Processing into Crystalline Thin Films. Angewandte Chemie International Edition, 59(13), 5165-5171. https://doi.org/10.1002/anie.201913975

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abstract = "Covalent organic frameworks (COFs) are highly modular porous crystalline polymers that are of interest for applications such as charge-storage devices, nanofiltration membranes, and optoelectronic devices. COFs are typically synthesized as microcrystalline powders, which limits their performance in these applications, and their limited solubility precludes large-scale processing into more useful morphologies and devices. We report a general, scalable method to exfoliate two-dimensional imine-linked COF powders by temporarily protonating their linkages. The resulting suspensions were cast into continuous crystalline COF films up to 10 cm in diameter, with thicknesses ranging from 50 nm to 20 μm depending on the suspension composition, concentration, and casting protocol. Furthermore, we demonstrate that the film fabrication process proceeds through a partial depolymerization/repolymerization mechanism, providing mechanically robust films that can be easily separated from their substrates.",

keywords = "covalent organic frameworks, exfoliation, nanosheets, polymers, solution processing",

author = "Burke, {David W} and Chao Sun and Ioannina Castano and Flanders, {Nathan C} and Evans, {Austin M} and Edon Vitaku and McLeod, {David C} and Lambeth, {Robert H} and Chen, {Lin X} and Gianneschi, {Nathan C} and Dichtel, {William R}",

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year = "2020",

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doi = "10.1002/anie.201913975",

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Acid Exfoliation of Imine-linked Covalent Organic Frameworks Enables Solution Processing into Crystalline Thin Films. / Burke, David W; Sun, Chao; Castano, Ioannina et al.
In: Angewandte Chemie International Edition, Vol. 59, No. 13, 23.03.2020, p. 5165-5171.

Research output: Contribution to journal/Conference contribution in journal/Contribution to newspaper › Journal article › Research › peer-review

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T1 - Acid Exfoliation of Imine-linked Covalent Organic Frameworks Enables Solution Processing into Crystalline Thin Films

AU - Burke, David W

AU - Sun, Chao

AU - Castano, Ioannina

AU - Flanders, Nathan C

AU - Evans, Austin M

AU - Vitaku, Edon

AU - McLeod, David C

AU - Lambeth, Robert H

AU - Chen, Lin X

AU - Gianneschi, Nathan C

AU - Dichtel, William R

PY - 2020/3/23

Y1 - 2020/3/23

N2 - Covalent organic frameworks (COFs) are highly modular porous crystalline polymers that are of interest for applications such as charge-storage devices, nanofiltration membranes, and optoelectronic devices. COFs are typically synthesized as microcrystalline powders, which limits their performance in these applications, and their limited solubility precludes large-scale processing into more useful morphologies and devices. We report a general, scalable method to exfoliate two-dimensional imine-linked COF powders by temporarily protonating their linkages. The resulting suspensions were cast into continuous crystalline COF films up to 10 cm in diameter, with thicknesses ranging from 50 nm to 20 μm depending on the suspension composition, concentration, and casting protocol. Furthermore, we demonstrate that the film fabrication process proceeds through a partial depolymerization/repolymerization mechanism, providing mechanically robust films that can be easily separated from their substrates.

AB - Covalent organic frameworks (COFs) are highly modular porous crystalline polymers that are of interest for applications such as charge-storage devices, nanofiltration membranes, and optoelectronic devices. COFs are typically synthesized as microcrystalline powders, which limits their performance in these applications, and their limited solubility precludes large-scale processing into more useful morphologies and devices. We report a general, scalable method to exfoliate two-dimensional imine-linked COF powders by temporarily protonating their linkages. The resulting suspensions were cast into continuous crystalline COF films up to 10 cm in diameter, with thicknesses ranging from 50 nm to 20 μm depending on the suspension composition, concentration, and casting protocol. Furthermore, we demonstrate that the film fabrication process proceeds through a partial depolymerization/repolymerization mechanism, providing mechanically robust films that can be easily separated from their substrates.

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Acid Exfoliation of Imine-linked Covalent Organic Frameworks Enables Solution Processing into Crystalline Thin Films

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