Rapid and efficient redox processes within 2D covalent organic framework thin films

Catherine R. Deblase; Kenneth Hernández-Burgos; Katharine E. Silberstein; Gabriel G. Rodríguez-Calero; Ryan P. Bisbey; Héctor D. Abruña; William R. Dichtel

doi:10.1021/acsnano.5b00184

Rapid and efficient redox processes within 2D covalent organic framework thin films

Catherine R. Deblase, Kenneth Hernández-Burgos, Katharine E. Silberstein, Gabriel G. Rodríguez-Calero, Ryan P. Bisbey, Héctor D. Abruña, William R. Dichtel^*

^*Corresponding author for this work

Chemistry

Research output: Contribution to journal › Article › peer-review

278 Scopus citations

Abstract

Two-dimensional covalent organic frameworks (2D COFs) are ideally suited for organizing redox-Active subunits into periodic, permanently porous polymer networks of interest for pseudocapacitive energy storage. Here we describe a method for synthesizing crystalline, oriented thin films of a redox-Active 2D COF on Au working electrodes. The thickness of the COF film was controlled by varying the initial monomer concentration. A large percentage (80-99%) of the anthraquinone groups are electrochemically accessible in films thinner than 200 nm, an order of magnitude improvement over the same COF prepared as a randomly oriented microcrystalline powder. As a result, electrodes functionalized with oriented COF films exhibit a 400% increase in capacitance scaled to electrode area as compared to those functionalized with the randomly oriented COF powder. These results demonstrate the promise of redox-Active COFs for electrical energy storage and highlight the importance of controlling morphology for optimal performance.

Original language	English (US)
Pages (from-to)	3178-3183
Number of pages	6
Journal	ACS nano
Volume	9
Issue number	3
DOIs	https://doi.org/10.1021/acsnano.5b00184
State	Published - Mar 24 2015

Keywords

covalent organic framework
electrochemistry
energy storage
nanoporous materials
polymer films
supercapacitors
surface science

ASJC Scopus subject areas

Materials Science(all)
Engineering(all)
Physics and Astronomy(all)

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10.1021/acsnano.5b00184

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title = "Rapid and efficient redox processes within 2D covalent organic framework thin films",

abstract = "Two-dimensional covalent organic frameworks (2D COFs) are ideally suited for organizing redox-Active subunits into periodic, permanently porous polymer networks of interest for pseudocapacitive energy storage. Here we describe a method for synthesizing crystalline, oriented thin films of a redox-Active 2D COF on Au working electrodes. The thickness of the COF film was controlled by varying the initial monomer concentration. A large percentage (80-99%) of the anthraquinone groups are electrochemically accessible in films thinner than 200 nm, an order of magnitude improvement over the same COF prepared as a randomly oriented microcrystalline powder. As a result, electrodes functionalized with oriented COF films exhibit a 400% increase in capacitance scaled to electrode area as compared to those functionalized with the randomly oriented COF powder. These results demonstrate the promise of redox-Active COFs for electrical energy storage and highlight the importance of controlling morphology for optimal performance.",

keywords = "covalent organic framework, electrochemistry, energy storage, nanoporous materials, polymer films, supercapacitors, surface science",

author = "Deblase, {Catherine R.} and Kenneth Hern{\'a}ndez-Burgos and Silberstein, {Katharine E.} and Rodr{\'i}guez-Calero, {Gabriel G.} and Bisbey, {Ryan P.} and Abru{\~n}a, {H{\'e}ctor D.} and Dichtel, {William R.}",

note = "Publisher Copyright: {\textcopyright} 2015 American Chemical Society.",

year = "2015",

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doi = "10.1021/acsnano.5b00184",

language = "English (US)",

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AU - Deblase, Catherine R.

AU - Hernández-Burgos, Kenneth

AU - Silberstein, Katharine E.

AU - Rodríguez-Calero, Gabriel G.

AU - Bisbey, Ryan P.

AU - Abruña, Héctor D.

AU - Dichtel, William R.

PY - 2015/3/24

Y1 - 2015/3/24

N2 - Two-dimensional covalent organic frameworks (2D COFs) are ideally suited for organizing redox-Active subunits into periodic, permanently porous polymer networks of interest for pseudocapacitive energy storage. Here we describe a method for synthesizing crystalline, oriented thin films of a redox-Active 2D COF on Au working electrodes. The thickness of the COF film was controlled by varying the initial monomer concentration. A large percentage (80-99%) of the anthraquinone groups are electrochemically accessible in films thinner than 200 nm, an order of magnitude improvement over the same COF prepared as a randomly oriented microcrystalline powder. As a result, electrodes functionalized with oriented COF films exhibit a 400% increase in capacitance scaled to electrode area as compared to those functionalized with the randomly oriented COF powder. These results demonstrate the promise of redox-Active COFs for electrical energy storage and highlight the importance of controlling morphology for optimal performance.

AB - Two-dimensional covalent organic frameworks (2D COFs) are ideally suited for organizing redox-Active subunits into periodic, permanently porous polymer networks of interest for pseudocapacitive energy storage. Here we describe a method for synthesizing crystalline, oriented thin films of a redox-Active 2D COF on Au working electrodes. The thickness of the COF film was controlled by varying the initial monomer concentration. A large percentage (80-99%) of the anthraquinone groups are electrochemically accessible in films thinner than 200 nm, an order of magnitude improvement over the same COF prepared as a randomly oriented microcrystalline powder. As a result, electrodes functionalized with oriented COF films exhibit a 400% increase in capacitance scaled to electrode area as compared to those functionalized with the randomly oriented COF powder. These results demonstrate the promise of redox-Active COFs for electrical energy storage and highlight the importance of controlling morphology for optimal performance.

KW - covalent organic framework

KW - electrochemistry

KW - energy storage

KW - nanoporous materials

KW - polymer films

KW - supercapacitors

KW - surface science

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ER -

Rapid and efficient redox processes within 2D covalent organic framework thin films

Abstract

Keywords

ASJC Scopus subject areas

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