Robust Amide-Linked Fluorinated Covalent Organic Framework for Long-Term Oxygen Reduction Reaction Electrocatalysis

The high energy demand of the evolving world opens the door to develop more sustainable and environmentally friendly energy sources. Oxygen reduction reaction (ORR) is a promising candidate, being the 2e− pathway of great interest for the green production of hydrogen peroxide. Metal-free covalent or...

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Bibliographic Details
Authors: Jiménez-Duro, M., Martínez-Periñán, E., Martínez-Fernández, M., Martínez, José I., Lorenzo, E., Segura, J.L.
Format: article
Status:Published version
Publication Date:2024
Country:España
Institution:Consejo Superior de Investigaciones Científicas (CSIC)
Repository:DIGITAL.CSIC. Repositorio Institucional del CSIC
OAI Identifier:oai:digital.csic.es:10261/392940
Online Access:http://hdl.handle.net/10261/392940
https://www.scopus.com/inward/record.uri?eid=2-s2.0-85193579688&doi=10.1002%2fsmll.202402082&partnerID=40&md5=4d3eb030002118f6f2efae3070ecc6c1
Access Level:Open access
Keyword:amide
COF
electrocatalyst
fluorine
H2O2
ORR
post-synthesisD
Description
Summary:The high energy demand of the evolving world opens the door to develop more sustainable and environmentally friendly energy sources. Oxygen reduction reaction (ORR) is a promising candidate, being the 2e− pathway of great interest for the green production of hydrogen peroxide. Metal-free covalent organic frameworks (COFs) electrocatalysts present a suitable alternative to substitute the noble-metals more commonly employed in this application. However, the lability of the linkages building up the framework raises an issue for their long-term use and application in aggressive media. Herein, a stable amide-linked COF is reported through post-synthetic modification of a previously reported imine-linked COF proven to be effective as an electrocatalyst, enhancing its chemical stability and electrochemical response. It is found that after the linkage transformation, the new electrocatalyst displays a higher selectivity toward the H2O2 production (98.5%) and an enhanced turnover frequency of 0.155 s−1, which is among the bests reported to date for metal-free and COF based electrocatalysts. The results represent a promising step forward for metal-free non pyrolyzed electrocatalysts, improving their properties through post-synthetic linkage modification for long-term operation. © 2024 The Author(s). Small published by Wiley-VCH GmbH.