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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.

Authors:
 [1];  [1];  [1];  [1];  [1];  [1];  [1]
  1. Department of Chemistry and Chemical Biology, Cornell University, Baker Laboratory, Ithaca, New York 14853-1301, United States
Publication Date:
Research Org.:
Energy Frontier Research Centers (EFRC) (United States). Energy Materials Center at Cornell (EMC2)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1386645
DOE Contract Number:  
SC0001086
Resource Type:
Journal Article
Resource Relation:
Journal Name: ACS Nano; Journal Volume: 9; Journal Issue: 3; Related Information: Emc2 partners with Cornell University (lead); Lawrence Berkeley National Laboratory
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; catalysis (homogeneous), catalysis (heterogeneous), energy storage (including batteries and capacitors), hydrogen and fuel cells, defects, charge transport, membrane, materials and chemistry by design, synthesis (novel materials), synthesis (self-assembly), synthesis (scalable processing)

Citation Formats

DeBlase, Catherine R., Hernández-Burgos, Kenneth, Silberstein, Katharine E., Rodríguez-Calero, Gabriel G., Bisbey, Ryan P., Abruña, Héctor D., and Dichtel, William R.. Rapid and Efficient Redox Processes within 2D Covalent Organic Framework Thin Films. United States: N. p., 2015. Web. doi:10.1021/acsnano.5b00184.
DeBlase, Catherine R., Hernández-Burgos, Kenneth, Silberstein, Katharine E., Rodríguez-Calero, Gabriel G., Bisbey, Ryan P., Abruña, Héctor D., & Dichtel, William R.. Rapid and Efficient Redox Processes within 2D Covalent Organic Framework Thin Films. United States. doi:10.1021/acsnano.5b00184.
DeBlase, Catherine R., Hernández-Burgos, Kenneth, Silberstein, Katharine E., Rodríguez-Calero, Gabriel G., Bisbey, Ryan P., Abruña, Héctor D., and Dichtel, William R.. Tue . "Rapid and Efficient Redox Processes within 2D Covalent Organic Framework Thin Films". United States. doi:10.1021/acsnano.5b00184.
@article{osti_1386645,
title = {Rapid and Efficient Redox Processes within 2D Covalent Organic Framework Thin Films},
author = {DeBlase, Catherine R. and Hernández-Burgos, Kenneth and Silberstein, Katharine E. and Rodríguez-Calero, Gabriel G. and Bisbey, Ryan P. and Abruña, Héctor D. and Dichtel, William R.},
abstractNote = {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.},
doi = {10.1021/acsnano.5b00184},
journal = {ACS Nano},
number = 3,
volume = 9,
place = {United States},
year = {Tue Feb 17 00:00:00 EST 2015},
month = {Tue Feb 17 00:00:00 EST 2015}
}