RT Journal Article
T1 Covalent organic frameworks based on electroactive naphthalenediimide as active electrocatalysts toward oxygen reduction reaction
T2 Redes orgánicas covalentes basados en naftalendiimida electroactiva como electrocatalizadores activos para la reacción de reducción del oxígeno
A1 Martínez-Fernández, Marcos
A1 Martínez-Periñán, Emiliano
A1 Royuela, Sergio
A1 Martínez, José
A1 Zamora, Felix
A1 Lorenzo, Encarnación
A1 Segura Castedo, José Luis
AB 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.
PB Elsevier
SN 2352-9407
YR 2022
FD 2022
LK https://hdl.handle.net/20.500.14352/100578
UL https://hdl.handle.net/20.500.14352/100578
LA eng
NO Martínez-Fernández, M.; Martínez-Periñán, E.; Royuela, S.; Martínez, J. I.; Zamora, F.; Lorenzo, E.; Segura, J. L. Covalent organic frameworks based on electroactive naphthalenediimide as active electrocatalysts toward oxygen reduction reaction. Applied Materials Today 2022, 26, 101384 DOI:10.1016/j.apmt.2022.101384.
NO Martínez-Fernández, Marcos, et al. «Covalent Organic Frameworks Based on Electroactive Naphthalenediimide as Active Electrocatalysts toward Oxygen Reduction Reaction». Applied Materials Today, vol. 26, marzo de 2022, p. 101384. https://doi.org/10.1016/j.apmt.2022.101384.
DS Docta Complutense
RD 25 jul 2024