Rapid and Efficient Redox Processes within 2D Covalent Organic Framework Thin Films

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-act...

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Bibliographic Details
Published in:ACS nano 2015-03, Vol.9 (3), p.3178-3183
Main Authors: DeBlase, Catherine R, Hernández-Burgos, Kenneth, Silberstein, Katharine E, Rodríguez-Calero, Gabriel G, Bisbey, Ryan P, Abruña, Héctor D, Dichtel, William R
Format: Article
Language:English
Subjects:
Capacitance
Covalence
covalent organic framework
electrochemistry
Electrodes
Energy storage
energy storage supercapacitors
INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
nanoporous materials
Nanostructure
Organizing
polymer films
surface science
Thin films
Two dimensional
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Summary: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.
ISSN:1936-0851
1936-086X
DOI:10.1021/acsnano.5b00184