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

Journal Article · · ACS Nano

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. Currently, 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 findings demonstrate the promise of redox-active COFs for electrical energy storage and highlight the importance of controlling morphology for optimal performance.

Research Organization:
Energy Frontier Research Centers (EFRC) (United States). Energy Materials Center at Cornell (EMC2)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)
Grant/Contract Number:
SC0001086; FG02-87ER45298; PHY-936384; DMR-1332208
OSTI ID:
1370446
Journal Information:
ACS Nano, Vol. 9, Issue 3; Related Information: Emc2 partners with Cornell University (lead); Lawrence Berkeley National Laboratory; ISSN 1936-0851
Publisher:
American Chemical Society (ACS)Copyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 279 works
Citation information provided by
Web of Science

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Nanoscale Engineering of Graphene‐Viologen Based 3D Covalent Organic Polymer Interfaces Leading to Efficient Charge‐Transfer for Pseudocapacitive Energy Storage journal July 2019
Catalysis and CO 2 Capture by Palladium-Incorporated Covalent Organic Frameworks journal October 2017
Stable Covalent Organic Frameworks for Photochemical Applications journal June 2019
Combined effect of nitrogen and oxygen heteroatoms and micropores of porous carbon frameworks from Schiff-base networks on their high supercapacitance journal January 2018
Covalent Organic Frameworks: Structures, Synthesis, and Applications journal July 2018
Preparation and energy storage application of a long-life and high rate performance pseudocapacitive COF material linked with –NH– bonds journal January 2018
Efficient Supercapacitor Energy Storage Using Conjugated Microporous Polymer Networks Synthesized from Buchwald-Hartwig Coupling journal January 2018
Catecholamine-functionalized graphene as a biomimetic redox shuttle for solar water oxidation journal January 2017
Bringing Porous Organic and Carbon-Based Materials toward Thin-Film Applications journal August 2018
A redox-active 2D covalent organic framework with pyridine moieties capable of faradaic energy storage journal January 2016
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Porous Polymers as Multifunctional Material Platforms toward Task-Specific Applications journal October 2018
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