Covalent organic frameworks based on electroactive naphthalenediimide as active electrocatalysts toward oxygen reduction reaction
EntityUAM. Departamento de Química Analítica y Análisis Instrumental; UAM. Departamento de Química Inorgánica
10.1016/j.apmt.2022.101384Applied Materials Today 26 (2022): 101384
ISSN2352-9407 (print); 2352-9415 (online)
Funded byThis work was financially supported by MICINN (PID2019-106268GB-C33; RED2018-102412-T; PID2020-116728RB-I00), Comunidad de Madrid (P2018/NMT-4349 TRANSNANOAVANSENS Program; SI3/PJI/2021-00341) and the UCM (INV.GR.00.1819.10759). The support provided by Álvaro Fuentes Benavides for the artwork of the graphical abstract is also acknowledged. MMF acknowledges Comunidad de Madrid for a predoctoral contract
ProjectGobierno de España. PID2019-106268GB-C33; Gobierno de España. RED2018-102412-T; Gobierno de España. PID2020-116728RB-I00
SubjectsCOF; Electrocatalysis; Napthalenediimide; Covalent Organic Frameworks; Metal-Free; Oxygen Reduction Reaction; Pyrolysis-Free; Química
Rights© 2022 Elsevier Ltd.
Esta obra está bajo una licencia de Creative Commons Reconocimiento-NoComercial-SinObraDerivada 4.0 Internacional.
Developing organic electrocatalysts toward the oxygen reduction reaction (ORR) that avoid heteroatom doping processes and high-temperature carbonization is of great significance for the maturing of fuel cell applications. Herein, a series of two-dimensional imide-based covalent organic framework (COFs) electrocatalysts toward the ORR is reported. The hydrodynamic electrochemical study reveals that 3.5 electrons are exchanged during the ORR indicating that the process catalyzed by these COFs has a clear preference for the 4-electron reduction pathway. The COFs contain conjugated electroactive napthalenediimide (NDI) moieties that provides the active sites for the electrocatalysis and promotes the formation of COFs with face-to-face π-π stacked structures to provide intrinsic porosity and large surface areas. These COFs can be essentially considered as an organized pattern of active sites embedded in the pore walls of the COF. The choice of suitable comonomers with variable distortions from planarity offers the possibility of obtaining these electroactive COFs with similar redox ability but different degrees of porosity and interlaminar spacing. This work evidences a new insight into developing novel families of electrocatalysts from COFs. Structure and stacking fashion of the COF-systems are investigated on the basis of DFT calculations, as well as the photoabsorption spectra of the representative molecular entities and a proof-of-concept rationalization of the intermediate steps of the ORR mechanism
Google Scholar:Martínez-Fernández, Marcos - Martínez Periñán, Emiliano - Royuela Collado, Sergio - Martínez, José I. - Zamora Abanades, Félix Juan - Lorenzo Abad, Encarnación - Segura, José L.
This item appears in the following Collection(s)
Showing items related by title, author, creator and subject.