β‐Ketoenamine‐Linked Covalent Organic Frameworks Synthesized via Gel‐to‐Gel Monomer Exchange Reaction: From Aerogel Monoliths to Electrodes for Supercapacitors

Covalent organic frameworks (COFs) possess intrinsic nanoscale pores, limiting mass transport and impacting their utility in many applications, such as catalysis, supercapacitors, and gas storage, demanding efficient diffusion throughout the material. Hierarchical porous structures, integrating larg...

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Published in:Advanced functional materials Vol. 34; no. 40
Main Authors: Martín‐Illán, Jesús Á., Sierra, Laura, Guillem‐Navajas, Ana, Suárez, José Antonio, Royuela, Sergio, Rodríguez‐San‐Miguel, David, Maspoch, Daniel, Ocón, Pilar, Zamora, Félix
Format: Journal Article
Language:English
Published: Hoboken Wiley Subscription Services, Inc 01.10.2024
Subjects:
Aerogels
Chemical synthesis
covalent organic frameworks
Electrodes
functional COF composites
Mass transport
Monomers
Porous materials
Supercapacitors
ultralight monolithic aerogels
ISSN:1616-301X, 1616-3028
Online Access:Get full text
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Summary:Covalent organic frameworks (COFs) possess intrinsic nanoscale pores, limiting mass transport and impacting their utility in many applications, such as catalysis, supercapacitors, and gas storage, demanding efficient diffusion throughout the material. Hierarchical porous structures, integrating larger macropores with inherent micro‐/meso‐pores, facilitate rapid mass transport. Recently, the fabrication of aerogel monoliths is reported exclusively from imine‐linked COFs, offering flexibility in aerogel composition. However, challenges in synthesizing robust β‐ketoenamine‐based COFs with comparable surface areas prompted innovative synthetic approaches. Leveraging the dynamic nature of COF bonds, in this work efficient monomer exchange from imine to partially β‐ketoenamine‐linked COFs within the gel phase is demonstrated. These aerogels can be transformed into electrodes using the compression technique. The new flexible electrodes‐based β‐ketoenamine‐linked COF composites with C super P exhibit superior durability and redox activity. Through supercapacitor assembly, the β‐ketoenamine‐linked COF electrodes outperform their imine‐based counterparts, showcasing enhanced capacitance (88 mF cm−2) and stability at high current densities (2.0 mA cm−2). These findings underscore the promise of β‐ketoenamine‐linked COFs for pseudocapacitor energy storage applications. The feasibility of monomer exchange to obtain β‐ketoenamine‐linked covalent organic frameworks (COFs) is shown in a monolithic gel‐to‐gel process. This allows the preparation of more robust COF aerogels and their easy processing into supercapacitor electrodes with superior performance compared to imine‐linked COFs, opening new opportunities in energy‐related applications.
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ISSN:1616-301X
1616-3028
DOI:10.1002/adfm.202403567